A review of transition metal dichalcogenides for supercapacitor applications: materials, performance, and challenges

Meenakshia, Gaurav Pandeyab, Shiv Dutta Lawaniyaa, Prashanth W. Menezescd and Kamlendra Awasthi*a
aDepartment of Physics, Malaviya National Institute of Technology, Jaipur-302017, Rajasthan, India. E-mail: kawasthi.phy@mnit.ac.in
bInstitute of Inorganic and Materials Chemistry, University of Cologne, Greinstr. 6, 50939, Cologne, Germany
cDepartment of Materials Chemistry for Catalysis, Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-Einstein-Str. 15, 12489 Berlin, Germany
dCentre for Future Materials, University of Southern Queensland, Toowoomba, Queensland, Australia

Received 17th February 2026 , Accepted 21st April 2026

First published on 23rd April 2026


Abstract

Supercapacitors (SCs) are environmentally friendly and sustainable innovations in energy transformation and storage. SCs provide a promising solution to fossil fuel depletion on account of their impressive power density (Pd) together with durable cycling lifespan, which makes them vital for modern electronic and electrical applications. However, they still face challenges, such as enhancing energy density (Ed) values, which remain a critical issue for the SC community that needs to be comprehensively tackled to meet the growing need for clean energy technologies. Significant attention has been garnered by two-dimensional (2D) transition metal dichalcogenides (TMDs) owing to their promise as key electrode materials in SCs. The excellent surface tunability, large electrochemically active exposed surface, and elevated electrical charge transport ability featuring adjustable oxidation levels facilitate efficient energy storage through pseudo-capacitive and electrical double-layer charge storage mechanisms. This review covers SC fundamentals, key components influencing Ed, and electrochemical evaluation techniques like galvanostatic charge–discharge (GCD), electrochemical impedance spectroscopy (EIS), and cyclic voltammetry (CV). It also provides a detailed analysis of the structural properties and synthesis routes of TMD-based electrodes, highlighting how doping, defect modulation, and composite engineering synergistically improve the electrochemical performance of TMD-based SCs. However, to fully unlock and optimise their capabilities, future research should be focused on integrating in situ characterisation, surface functionalization, and morphological engineering to enhance understanding of material behaviour. Additionally, integrating Density Functional Theory (DFT) simulations with machine learning-assisted calculations can accelerate the discovery and optimisation of high-performance materials for next-generation energy storage applications.


1. Introduction

Energy is a critical area of focus because energy resources are vital for both residential and industrial applications. Currently, fossil fuels are the dominant energy source and a major contributor to global warming. The progressive reduction in fossil fuel usage, as well as the ecological impact of greenhouse gas releases, has driven the worldwide development of sustainable energy supplies.1,2 The risks tied to the exploitation of fossil fuels might be addressed by utilising alternative renewable energy sources, including tidal, thermal, wind, hydro, and solar energy, which are environmentally friendly, and their associated technologies have been globally competitive.3,4 However, renewable energy conversion technologies are confronted with a critical challenge due to intermittent energy production, leading to interruptions in energy supply. As a result, the electrical energy produced by these sources is intermittent and does not reliably provide a continuous supply for domestic and commercial utilisation. Consequently, electrical energy storage systems have gained significant attention from researchers as a solution to overcome the barriers of continuous energy production and distribution, ensuring a stable and on-demand energy supply.3,4

Batteries5 and supercapacitors (SCs)6 are vital energy storage devices (ESDs) recognised for their superior energy density (Ed), power density (Pd), mobility, and optimal life cycles.7 Among batteries, rechargeable systems have become the backbone of modern energy infrastructure, owing to their ability to store and deliver energy efficiently, making them key enablers of the renewable energy revolution.8 However, the growing demand for rapid energy delivery and high-power performance has drawn increasing attention to SCs. In this context, SCs have become essential due to their exceptional Pd and seamless integration with diverse energy conversion systems.9,10 Whether it's enabling electric vehicles to charge within minutes or accelerate beyond 60 mph in seconds, SCs are increasingly being adopted for specialised applications worldwide.9 SCs offer a significant advantage over other contemporary energy retention technologies by virtue of their exceptional storage properties as well as excellent Pd. Due to these distinct characteristics, including high Pd, longer life cycles, high specific capacitance (Cs), superior low-temperature performance, and non-hazardous waste management, they can be considered environmentally sustainable. Along with this, SCs can be charged rapidly with quick power delivery, making them a viable intermediary between a battery and conventional capacitor, as can be seen in Fig. 1(a).11–13 Although SCs store less charge than batteries, they can provide a thousand times more power than batteries.14,15 Furthermore, unlike batteries, SCs are safer, posing no explosion risk even when overcharged.11,12


image file: d6ta01482h-f1.tif
Fig. 1 (a) Comparison of Ed and Pd in different energy storage technologies, represented through a Ragone plot; (b) number of publications on TMDs and SCs by year, based on Web of Science searches in April 2026, using keywords “transition metal dichalcogenides” or “TMDs” and “supercapacitors” or “SCs”.

Generally, SCs can be categorised into three distinct types based on their charge storage mechanisms: electric double layer capacitance, which occurs through charge segregation at the electrolyte/electrode junction; and faradaic pseudo-capacitance, which results from rapid, reversible absorption/desorption or reduction–oxidation reactions on or around the electrode face, besides asymmetric SCs.15,16 Among these, asymmetric SCs can be generally categorised into two categories: configurations with two capacitive electrodes or hybrid capacitors. Furthermore, hybrid capacitors are recognised as a system where charge accumulation occurs at a single electrode through battery-style faradaic reactions, while the counterpart electrode utilises a capacitive-type storage method.4,17 SCs are predominantly found in current fields, including electronic gadgets, voltage regulation devices, minimal-power device buffers, motorised tools, and hybrid automobiles, alongside industrial and medical use instruments. They may be used independently or in conjunction with batteries to enhance the lifespan of the latter and achieve a balanced power and Ed as needed. A well-designed SC system can provide this balance, making it ideal for current applications where improving the operational life of batteries and optimising the energy-power balance is crucial.15,18 Electrode materials as well as electrolytes have a vital involvement in advancing SC capability and enabling their commercialisation.11,19,20 These components directly impact key characteristics such as Cs, operating voltage, Ed, and Pd values.

Addressing the increasing worldwide need for efficient, high-performance, and eco-friendly energy storage has led to extensive research into advanced electrode materials for supercapacitors. These are crucial for use in portable electronics, electric vehicles, and large-scale energy storage systems.21 Traditional SC electrodes based on activated carbon typically use binders, which serve as inert components that reduce the functional area of the electroactive material and add unwanted weight, resulting in bulkier devices.22,23 The discovery of graphene, a remarkable material, has paved the way for significant advancements in energy retention enabled by its vast surface area, superior electrical conductivity, and robust physical stability.24–28 Despite extensive studies, graphene-based SCs still exhibit lower Ed than lithium-ion batteries.29,30 Owing to the fact that graphene primarily stores charge via the EDL (i.e. electrochemical double layer) on the electrolyte/electrode junction, its capacitance is primarily governed by surface area and ion accessibility, rather than by faradaic reactions. In order to enhance efficiency, redox materials, including transition metal oxides (for example, MnO2 and RuO2) and polymers that show electrical conductivity (for example, polyaniline (PANI) and polypyrrole (PPy)), are incorporated; however, this compromises the cycle life.31–34 Transition metal-derived materials, excluding graphene-based composites, have been largely explored as materials for electrodes due to their excellent capacitance, high-rate capability, and cost-effectiveness.35,36 Nevertheless, challenges such as constrained surface area, short cycling lifespan, and inadequate electrical conductivity hinder their efficiency. Therefore, several approaches can be employed to overcome these limitations, including (1) morphology control, (2) composite formation of electrode materials to achieve synergistic effects, (3) doping elements into electrode materials to boost redox activity, and (4) manipulation of defects.9,11,37,38

Recently, advances in materials science have highlighted metal-based two-dimensional (2D) layered materials, such as transition metal dichalcogenides (TMDs), beyond conventional graphene, as highly promising electrode candidates for advanced supercapacitors (Fig. 1(b)). Nonetheless, recent advances in materials science indicate that 2D layered materials have secured noteworthy popularity as electrode materials in advanced capacitors, owing to their extensive surface area resulting from the full accessibility of surface atoms.39,40 The edge sites in thin 2D nanosheets are more chemically active than the basal plane, and the exposed van der Waals voids facilitate ion intercalation from the electrolyte, further enhancing their performance. Additionally, their high mechanical strength and atomic-scale dimension flexibility make them suitable for next-generation wearable electronics.41 Apart from graphene, there exist numerous types of 2D materials, such as layered transition metal dichalcogenides (TMDs), that have become highly promising candidates for SC electrodes.26–28 TMDs consist of layered inorganic materials containing transition metals (M) and chalcogens (X: S, Se, and Te) arranged in an X–M–X structure with the chemical formula MX2. They possess a wide array of physicochemical properties, making them very attractive for both fundamental studies and practical applications.9 Nowadays, various 2D TMDs are employed for SC electrodes, including molybdenum disulfide (MoS2), molybdenum diselenide (MoSe2), tantalum disulfide (TaS2), tantalum diselenide (TaSe2), niobium disulfide (NbS2), tungsten disulfide (WS2), tungsten ditelluride (WTe2), tungsten diselenide (WSe2), titanium disulfide (TiS2), vanadium disulfide (VS2), vanadium diselenide (VSe2), zirconium disulfide (ZrS2), etc.9 Furthermore, MoS2, MoSe2, WS2, and WSe2 have emerged as the most studied TMDs for their crucial role in augmenting electrochemical efficiency within energy retention and conversion technologies.42 Major TMDs exhibit a layered structure featuring weak interlayer bonding through van-der Waal force (for example, group 4–7 TMDs), while some are non-layered (for example, group 9–10 TMDs).43,44 They can exist in either the 1T/2H structure (for example, group 5 TMDs) and typically favour 1T (for example, groups 4 and 7) or 2H (for example, group 6), each with distinct physical properties, i.e. the 2H phase, characterised as semiconducting with an inadequate electrical conductivity, and the 1T phase, which is normally metallic and highly conductive.44–48 The extraordinary electrical, optical, and catalytic properties of 2H-TMDs have positioned them as a leading choice for a wide range of energy-related applications. Conversely, T-phases usually display metallic properties, greatly improving charge transfer efficiency in different energy-related applications. Nonetheless, 1T meta-stable materials, such as MoS2, can undergo a spontaneous transition to the H-phase. Controlling the preparation of the metallic phase continues to be a major challenge. TMDs can be used as electrodes in SCs in their bulk state, but their properties change significantly when reduced to single- or few-layer thicknesses. A significant limitation of bulk TMDs is their low surface area.42,43,49 However, the nano-optimisation of TMDs into zero-, one-, and three-dimensional structures offers a compelling technique to overcome their natural shortcomings. Moreover, the transition of phases in TMDs, from 2H semiconducting to 1T metallic, has ignited significant interest in developing a novel category of metallic TMDs exhibiting significant potential to achieve enhanced Ed (Fig. 2).9


image file: d6ta01482h-f2.tif
Fig. 2 Classification of TMDs based on their dimensionality, electronic properties, and structures.

Numerous reviews delved into different aspects of TMDs, along with their fabrication methods, intrinsic characteristics, and SC applications.50–55 Thomas et al. explored the crystal structure and synthesis methods of only tin disulfide (SnS2), a TMD material, and provided a detailed analysis of the electrochemical performance of both pristine SnS2 and SnS2-based nanocomposites in SC applications.53 In another review, Song et al. thoroughly examined how element doping, morphology, structure, phase, composite and hybrid configurations, and the electrolyte, impact the overall performance of 2D TMD-based SCs from the perspective of device optimisation.54 In a subsequent review, Philip et al. examined recent progress in TMD-based compounds aimed at improving electrochemical energy storage devices, highlighting material properties, device performance, and key challenges, including stability, conductivity, and cost. They stressed the importance of optimised synthesis methods, innovative heterostructures, and advanced electrolytes to create flexible, stable, and high-performance SCs for future use.56 Another study by Debbarma et al. reviewed the transition metal tellurides (TMTes), covering their composition, crystal structure, physical properties, and synthesis methods. They also examined factors influencing the charge storage mechanism in TMTes, the impact of morphology on electrochemical performance, and the role of various transition metal-based tellurides in SC applications.57 Apart from these, Sowbakkiyavathi et al. reviewed the fundamentals and recent progress in SCs, concentrating on TMD materials and their synthesis methods. They underscored the role of doping with CNTs, MWCNTs, reduced graphene oxide, metal-based compounds, and polymers in enhancing electrochemical performance.55 In a distinct review, Mohan et al. investigated tungsten disulfide-based nanomaterials, covering their structural characteristics, synthesis approaches, and an in-depth analysis of the electrochemical performance of WS2-based electrode systems.58 In another review, Khan et al. discussed graphene/TMSe composites and explored the synergistic effects between them, like structural stability and charge transfer kinetics. Along with this, they explored the challenges based on the graphene/TMSe hybrid SC.59

While existing reviews on TMDs for supercapacitor applications have largely focused on specific materials or on modification strategies and interface engineering, a comprehensive understanding that connects supercapacitor fundamentals with the electrochemical performance of TMDs, particularly in light of recent progress, remains insufficiently addressed. In this context, the aim of this review is to provide an in-depth, structured, and up-to-date overview of high Ed SCs employing TMD-based electrode nanomaterials for energy storage applications. It explores the use of 2D/3D TMDs to enhance SC performance. The review begins with an in-depth explanation of SCs, covering their fundamental principles and various performance enhancement techniques. It then highlights the distinctive merits of ultrathin 2D/3D nanomaterials, focusing on their electronic and crystal structures. A variety of TMDs and their composites utilised in SCs are introduced. Subsequently, the structural parameters and inherent engineering aspects that influence capacitance performance are elaborated. Additionally, the review describes the design and future development of TMD-derived materials tailored for next-generation energy storage technologies. Finally, based on recent advancements, we conclude by offering insights into the current challenges and future outlook of this rapidly evolving field. This review serves as a valuable resource, offering a clear and concise explanation of SCs, making it accessible even to scholars with limited prior exposure to electrochemical energy storage.

2. Supercapacitor fundamentals

SCs have attracted significant interest as ESDs over the last few decades due to their ability to store and release energy quickly, providing high current in a short time.60,61 Here, we present the historical progression of the development of SCs, as depicted in Fig. 3.62
image file: d6ta01482h-f3.tif
Fig. 3 Historical timeline of the development of SCs. Reproduced from ref. 4 with permission from American Chemical Society, copyright 2018.

The SCs mainly have three components: electrolytes, electrodes (positive or negative), and separators. The electrolyte can be liquid, solid, or in the gel form, and it allows ions to move for the charge–discharge process.63–65 The electrodes store electric charge by accumulating ions from the electrolyte. A separator is employed to prevent direct contact with the electrodes.

2.1 Working principle of SCs

The principles underlying energy storage are based on two mechanisms:66

• The EDL capacitance originates through the adsorption of coulombic charge on the interfacial region between the electrode and the electrode–electrolyte.

• Pseudo capacitance originates from surface redox reactions that are related to their respective potential.

• The combination of both forms the storage principle of hybrid SCs.

2.2 Supercapacitor classification based on charge storage mechanisms

SCs are classified into three distinct classes based on their energy-storage mechanisms, as outlined and discussed in detail below.
2.2.1 Electric double layer capacitors (EDLCs). An EDLC is considered a promising high-power energy storage solution for both electric transport and wireless communication devices.67 EDLCs offer advantages, including higher rate efficiency and longer cycle life, compared with modern secondary batteries.67 In EDLCs, energy is stored through the separation of charges at the interface between the electrode and electrolyte, as illustrated in Fig. 4(b). Most EDLCs use liquid electrolytes, typically consisting of aprotic solvents such as aqueous electrolytes (salts dissolved in water), propylene carbonate (PC), diethyl carbonate (DEC), dimethyl carbonate (DME), or ethylene carbonate (EC).68 These EDLC SCs store energy via electrostatic interactions in Helmholtz double layers, which develop amid the electrode–electrolyte interfaces. In addition, for EDLC SCs, graphene, activated carbon (AC), carbon nanotubes (CNTs), carbon aerogels, metal oxides, and conducting polymers are frequently employed as electrode materials owing to their large specific surface areas, which enhance capacitance.68
image file: d6ta01482h-f4.tif
Fig. 4 (a) Classification of SCs. Reproduced from ref. 4 with permission from American Chemical Society, copyright 2018. (b) Schematics of different charge-storage principles underlying EDLCs, pseudocapacitors, and hybrid SCs. Reproduced from ref. 64 with permission from Royal Society of Chemistry, copyright 2019.
2.2.2 Pseudo-capacitors. A pseudo-capacitor represents a category of SCs that fall between batteries and EDLCs. The pseudo-capacitor forms an SC when combined with a double layer.67 It stores energy via rapid, reversible faradaic reactions (such as redox reactions, electro-sorption, or intercalation) at the electrode–electrolyte interface, as shown in Fig. 4(b). This results in a capacitance exceeding that of EDLCs, attributed to the presence of faradaic charge-storage mechanisms.69
2.2.3 Hybrid supercapacitors. The hybrid supercapacitor is primarily governed by a combination of EDLC and pseudo-capacitor mechanisms as depicted in Fig. 4.66,70 The ideal hybrid SCs would offer superior Pd and prolonged cycle life, along with an Ed comparable to that of batteries, as shown in the Ragone plot (Fig. 1(a)). The limitations of EDLCs are absent in pseudo capacitors, and vice versa. Their combination (hybrid SCs) overcomes the shortcomings of each individual component, resulting in enhanced capacitance. The combination offers a higher working potential and carries capacitance that is two to three times greater relative to conventional capacitors, along with EDLCs and pseudo-capacitors. Hybrid SCs are synthesised by integrating various redox and electric double-layer capacitor (EDLC) materials, including graphene, graphite, metal oxides, conductive polymers, and activated carbon.71–73

2.3 Components of supercapacitors

A SC is composed of four primary components (Fig. 5): electrode materials, electrolytes, a current collector for charge collection, and a separator that isolates the cathode and anode, and their selection largely influences the SC performance.74,75 To build insight into how these components affect the SC performance, we discuss each component in detail below.
image file: d6ta01482h-f5.tif
Fig. 5 Different components of the SCs.
2.3.1 Electrode materials. Choosing the appropriate electrode material is essential for optimising SC performance, as it directly impacts energy storage, power delivery, and overall efficiency. The typically utilised electrode materials in SCs include (i) TMDs like molybdenum disulfide (MoS2); (ii) porous carbon materials, like graphene, carbon nanotubes (CNTs), and activated carbon (AC); (iii) metal nitrides, like vanadium nitride (VN) and titanium nitride (TiN); (iv) metal oxides, including ruthenium oxide (RuO2), manganese oxide (MnO2), vanadium pentoxide (V2O5), and molybdenum trioxide (MoO3); (v) other materials that have gained attention in recent years, including MXenes, conductive polymers, like polypyrrole (PPy), polyaniline (PANI), and poly(phenylene diimine) (PPdi), and conductive metal–organic frameworks (MOFs).62 Additionally, it is crucial to consider the material's compatibility with electrolytes, cost-effectiveness, and manufacturability. For this purpose, optimising the pore size and structure is vital, as it facilitates easier ion movement, which boosts overall efficiency. Furthermore, surface functionalization of electrode materials improves electrolyte compatibility, while the use of thin, uniform electrodes helps minimise resistance.76–78
2.3.2 Electrolytes. The electrolyte in an SC plays a vital role in facilitating ion movement between electrodes. The electrolyte is basically composed of cations, anions, and a solvent (except in ionic liquid (IL) electrolytes), and serves as the charge transfer medium. The electrolytes can be categorised into several types: (i) basic electrolytes, including potassium hydroxide (KOH) and sodium hydroxide (NaOH); (ii) acidic electrolytes, including sulfuric acid (H2SO4) and hydrochloric acid (HCl); (iii) strongly concentrated electrolytes, including hydrate-melt electrolytes and water-in-salt (WIS); (iv) neutral electrolytes, such as metal sulphate salts (e.g., sodium sulphate, Na2SO4).62 Crucially, the electrolyte selection is basically determined by the required balance of performance, stability, and cost.
2.3.3 Current collectors. The current collector facilitates electronic transfer and ensures uniform charge distribution at the surface of faradaic reactions, and defines the characteristics of the SC.79 Over the past few decades, metallic (foil and porous) and carbon-based current collectors have been widely used in SCs.75 However, fundamental criteria for selecting current collectors apply regardless of the properties of SCs, ensuring high efficiency and stable operation.
2.3.4 Separators. In an SC, the separator maintains a uniform gap between the anode and cathode, preventing short circuits caused by direct electrode contact. It is usually a microporous film composed of polymers such as polyethylene (PE) or polypropylene (PP). It should be chemically stable and resistant to high voltages and environmental conditions to ensure longevity and safety. Its function also ensures the proper transport of ions between electrodes through the electrolyte during charging and discharging cycles.

2.4 Different parameters and their influence on the efficiency of supercapacitors

The SC performance is determined based on several key criteria including (1) high Cs, (2) significantly superior Pd, (3) relatively superior Ed, (4) excellent cycle stability, (5) rapid charge–discharge capability, (6) operating voltage, (7) equivalent series resistance, (8) time constant and (9) cost-effectiveness.42,80 These parameters are described below:
2.4.1 Capacitance. The device's capacitance (C) is the amount of charge (ΔQ) stored per unit of applied voltage (ΔV).81
 
image file: d6ta01482h-t1.tif(1)

Moreover, in SCs, capacitance is typically defined in terms of specific capacitance (Cs), as:82

 
image file: d6ta01482h-t2.tif(2)
where m represents the mass, area, or volume.

Furthermore, under constant current conditions during charging and discharging, eqn (2) can be rewritten as:83

 
image file: d6ta01482h-t3.tif(3)
where Δt represents the discharging time.84

2.4.2 Energy and power density. The electrochemical efficiency of SCs is primarily assessed through their Ed and Pd and can be determined using eqn (4) and (5), respectively.85
 
image file: d6ta01482h-t4.tif(4)
 
image file: d6ta01482h-t5.tif(5)
 
image file: d6ta01482h-t6.tif(6)
Here, ν represents the scan rate, and t represents the time span of the GCD discharge curve. Using eqn (4) and (5), the Ed and Pd were calculated via the CV method, while eqn (4) and (6) were used to calculate the Ed and Pd, using the GCD method, and these techniques are discussed in the following Section 2.5.42
2.4.3 Equivalent series resistance (ESR). The combined resistance of the SC configuration, including the electrolyte, electrode, electrode-collector interface, and separator, is referred to as the ESR (Resr) as given below.86
 
image file: d6ta01482h-t7.tif(7)
where I represents the current and V denotes the voltage.
2.4.4 Operating voltage (Vo). Ideal capacitors are assumed to operate without voltage limit restrictions. In contrast, real capacitors have specific upper and lower voltage limits that describe their “voltage window”. Exceeding this voltage range may trigger electrolyte decomposition, damaging the device. Capacitor electrolytes are classified into two kinds: aqueous and nonaqueous. Aqueous electrolytes are easier to grip and harmless in operation in a narrow potential window, while nonaqueous electrolytes provide a wider voltage window. Diverse SC materials can enhance the operating voltage (Vo) in asymmetric configurations by creating an electrochemical potential difference between the electrodes.42
2.4.5 Time constant and cycle life. The time constant is a crucial parameter in SC performance evaluation and is determined by the SC capacitance and equivalent series resistance (ESR). It is the product of the capacitance (Cs) and ESR (R), expressed by using the formula τ = R × Cs. In practical applications, SCs are used for short-term energy bursts, with time constants typically ranging from seconds to minutes. The time constant varies based on the capacitance and ESR of SCs.42 Apart from this, another crucial parameter is the cycling life of the SC. The cycle life of SCs is chiefly influenced by the capacitance retention of the electrode materials. Key factors like applied voltage, operating temperature, and charge/discharge current also play a role in determining their longevity. Activated carbon electrodes, with their chemical and electrochemical stability, help extend the lifespan of SCs.42

2.5 Techniques used to measure the electrochemical performance of supercapacitors

Electrochemical performance of materials is determined using two configurations: the two-electrode and three-electrode systems. Various analytical techniques, including CV, GCD, and EIS are utilised to systematically determine the performance characteristics of SCs.87
2.5.1 Cyclic voltammetry (CV). CV is a highly advanced, pervasively utilised electrochemical procedure that comprehensively characterises a system's thermodynamic and kinetic properties.88 It provides valuable insights into reaction kinetics, electrochemical reversibility, and diffusion-controlled transport phenomena, and distinguishes between capacitive and faradaic charge storage mechanisms. The current–potential plot, called the voltammogram, serves as a diagnostic tool for understanding electrochemical behaviour, especially in materials such as TMDs and hybrid structures.89,90 Theoretically, the presence of a rectangular CV curve indicates ideal capacitive behaviour, while an EDLC electrode shows a distorted shape due to non-ideal behaviour. In contrast, faradaic reactions in pseudo-capacitors produce reduction and oxidation peaks. From the CV curve, a range of parameters, including Cs, Ed, and Pd, charge retention mechanisms, stability, and operational lifetime, can be calculated to evaluate the performance of SCs and other electrochemical devices.91–93

To further analyse the electrochemical processes involved, the concentrations of redox species on the electrode surface are assessed using the Nernst equation (eqn (8)).

 
image file: d6ta01482h-t8.tif(8)
where ET represents the reversible cell voltage at temperature T, E0 denotes the standard-state reversible cell voltage, R is the gas constant, F is Faraday's constant, Cred signifies the concentration of the reductive species, and Cox indicates the concentration of the oxidative species.

Moreover, Randles–Ševčík eqn (9) provides a theoretical expression for the peak current in a reversible CV concerning the scanning speed, which is crucial for studying electrochemical mechanisms.93 Peak current (ip) in redox reaction cycles is influenced by several factors, including the concentration (C′), diffusion coefficient (D), scan rate (ϑ), number of electrons embedded in the redox reaction (n), electrode surface area (A) of the redox-active species and Faraday constant (F).

 
image file: d6ta01482h-t9.tif(9)

Calculating peak currents using this equation and plotting them against the square root of the scanning rate reveals a direct correlation, indicating that diffusion-controlled processes are the primary mechanism for charge storage.94 Moreover, for reversible electrochemical reactions, the anodic and cathodic peak potentials can be used to determine the number of electrons involved in the electrode reaction.

Apart from these, Dunn's power law is another general formula relating the peak current to the scan rate, providing insights into the charge storage dynamics of the electrodes, as outlined in eqn (10).

 
ip = b (10)
In this equation, ip represents the current response corresponding to a specific voltage (relative to the reference electrode), and ϑ denotes the scan rate. The diffusion and capacitive contributions are assessed via the b value, obtained from the slope of log[thin space (1/6-em)]i vs. log(ϑ); it ranges from 0.5 to 1.0 in the power-law relation. A b value of 0.5 indicates a diffusion-controlled (intercalation/deintercalation) process, while b = 1.0 reflects a capacitive-controlled current response.95

Besides, the relative contributions of diffusion-controlled charge storage and capacitive processes (including EDLC and pseudo capacitance) might be distinguished by deconvoluting the Voltammetric current response (eqn (10)) via two mechanisms:

 
image file: d6ta01482h-t10.tif(11)
where the k1ϑ and image file: d6ta01482h-t11.tif term correspond to the capacitive current, and the diffusion-limited current, respectively.

Derived from the profile of the obtained CV plot, its mechanism of charge storage, whether it is electrical double layer capacitance or pseudo-capacitance, can be predicted.96 This prediction is mathematically supported by the relationship, as shown in the following eqn (12):

 
image file: d6ta01482h-t12.tif(12)
where I(t) = current response, C = capacitance (F), and image file: d6ta01482h-t13.tif.

Now to determine the Cs (F g−1) of the electroactive material, eqn (12) can be modified as eqn (13), by assuming that the auxiliary electrode's capacitance is much larger than the working electrode's, due to the potentiostats enabling effective system analysis,

 
image file: d6ta01482h-t14.tif(13)
where image file: d6ta01482h-t15.tif is calculated by integrating the area beneath the CV, m represents the mass of the electrode material (g), ϑ denotes the scan rate (mV s−1), and the voltage range (V) is ΔV. Moreover, the specific energy (Wh kg−1) and specific power (W kg−1) of the electrode material can be determined using the following eqn (14) and (15).97
 
image file: d6ta01482h-t16.tif(14)
 
image file: d6ta01482h-t17.tif(15)

2.5.2 Galvanostatic charge–discharge (GCD). GCD is a critical electrochemical technique used to evaluate SC performance.87 In a typical GCD experiment, a constant current density is applied, and the resulting potential variations are recorded with time.

The various parameters, including Cs, Ed, and Pd of an electrode material, are evaluated from the GCD curves using the subsequent eqn (16)–(18), respectively:60

 
image file: d6ta01482h-t18.tif(16)
 
image file: d6ta01482h-t19.tif(17)
 
image file: d6ta01482h-t20.tif(18)
where i denotes the applied constant current (A), t represents the charge–discharge duration (s), m refers to the mass of the electrode material (g), and ΔV indicates the potential window.94,98 Additionally, GCD provides valuable insights into other important electrochemical properties, such as:

• Rate capability: variation in capacitance at diverse current densities.

• Cycling stability: retention of capacitance over multiple charging and discharging cycles.

• Coulombic efficiency: ratio of stored charge to delivered charge during the charge–discharge cycles.

2.5.3 Electrochemical impedance spectroscopy (EIS). EIS is an operational method that yields critical insights into series resistance (Rs), charge-transfer resistance (Rct), double-layer capacitance (Cdl), and Warburg's impedance (Zw) due to diffusion.99 The impedance (Z) is measured across spanning frequencies from 0.01 Hz to 1 MHz, incorporating the extent of measurement precision achievable by most EIS instruments represented by a specific value of Z (Ω).95

Within a Nyquist plot, the real part of impedance (Z′ = Z0(cos[thin space (1/6-em)]θ + i[thin space (1/6-em)]sin[thin space (1/6-em)]θ)) is represented along the horizontal axis, whereas the reactive component (Z″) appears on the vertical axis. This plot typically displays semicircles in the high-frequency region, indicative of faradaic redox reactions or electronic conduction.100 The 45° linear segment observed at medium frequencies is indicative of molecular diffusion, commonly referred to as the Warburg region, with a 90° line observed at lower frequencies indicating the development of an electric double layer on the electrode's surface. The equivalent series resistance (Rs) is represented by the semicircle's intercept on the real axis, and charge transfer resistance (Rct) is estimated from the low-frequency region, where a low value signifies a fast charge transfer process.101 Fitting the Nyquist plot using the Randles circuit model (Fig. 6(b)) allows for the extraction of additional parameters, including capacitance owing to the development of double-layer (Cdl) and Warburg's impedance (Zw). The slope of the Warburg line in the lower-frequency area elucidates the charge storage mechanism of electrode materials. In contrast, the Bode plot represents angular frequency (ω) plotted along the horizontal axis against the shift in phase (θ = arg[thin space (1/6-em)]Z) or log impedance (log[thin space (1/6-em)]Z) along the vertical axis.102 This representation provides insights into faradaic impedance related to charge transfer and diffusional processes, enhancing understanding of the system's behaviour across different frequency ranges.103 Faradaic impedance (Rf) related to charge transfer, along with diffusional phenomena, is examined by using the following eqn (19):

 
Rf = Rct + Rw (19)
where image file: d6ta01482h-t21.tif and σ denote the Warburg coefficient (ohm rad1/2 per s) and Warburg impedance image file: d6ta01482h-t22.tif.


image file: d6ta01482h-f6.tif
Fig. 6 (a) Characteristic CV and GCD profiles for EDLCs, and pseudocapacitive, and battery-type materials, (b) schematic of a general circuit model for EIS with Bode and Nyquist plots. Reproduced from ref. 107 with permission from Wiley, copyright 2019. (c) Combining material results in asymmetric and hybrid configurations, each exhibiting unique CV characteristics. Reproduced from ref. 87 with permission from Elsevier, copyright 2023.

Theoretically, the phase shift in a Bode plot is represented as the phase angle, determined by image file: d6ta01482h-t23.tif.

For a reversible process, Rct = 0 and the phase angle is ≤45° and for a quasi-reversible process, Rct > 0 and the phase angle is <45°.

The capacitance of the electrical double layer, Cdl, is determined by using eqn (20):

 
image file: d6ta01482h-t24.tif(20)
where ω = angular frequency in units of rad s−1.

Within the Nyquist plot, Warburg's impedance (Zw) appears as a diagonal line inclined at 45°. The Bode plot shows a phase shift of 45°.104 Minimal Rs and Rct values are crucial for minimising IR drop, which enables larger output power and energy in energy storage systems. Therefore, the charge-transfer behaviour of the prepared electrodes is examined using EIS.105,106

3. Transition metal dichalcogenides

3.1 Structural characteristics and their properties

TMDs can typically be denoted by the molecular formula, MX2 (with M representing transition metals from groups IVB to VIII and X denoting elements such as S, Se, and Te from group VIA) (Fig. 7(a)).51,108 Macroscopic TMDs have been extensively researched for an extended period due to their ability to create compounds with diverse electronic structures. In their bulk form, MX2 compounds are layered materials (or van-der Waals solids) displaying significant intralayer bonding and weak interlayer bonding. Every layer of TMDs contains three atomic layers, with a transition metal atom lying within two chalcogen atoms. The chalcogen atoms are fully saturated, making them relatively non-reactive. These characteristics allow for the isolation of individual TMD layers through techniques like exfoliation or vapor deposition. When TMDs are reduced to monolayers, their properties change significantly, mainly because charge carriers are confined to two dimensions (x- and y-directions) and do not interact in the z-direction. As a result, single-layered nanosheets exhibit fundamentally different properties compared to their bulk forms, rendering them highly suitable for numerous applications in catalysis, electronics, and photonics. Moreover, this has sparked considerable interest in these materials.109 TMDs feature a tunable band-gap (direct/indirect) with a structure analogous to graphite.110 When considering the bonding in TMDs, metal atoms (M) supply the electrons. The metal (M) atoms in TMDs usually exhibit a +4 oxidation state, while the chalcogen (X) atoms have an oxidation state of −2.111 The characteristics of macro-TMDs span a wide range, from insulators like HfS2 to semiconductors including WS2 and MoS2, true metals like VSe2 and NbS2 and semi-metals like WTe2 and TiSe2.43 TMDs exist in different structural phases (Fig. 7(b)). Among them, three well-known polytypic structures arise from varying coordination geometries of the transition metal atoms: 2H (hexagonal or trigonal prismatic), 1T (tetragonal or octahedral), and 1T′ (distorted octahedral).108,112 The stacking configurations of the X–M–X atomic trilayers also differ. In 2H-TMDs, the atomic planes follow a Bernal (ABA) stacking arrangement, while in 1T-TMDs, the stacking is rhombohedral (ABC). This variation in structure gives rise to distinct electronic properties. For instance, the 2H phase of MoS2 exhibits semiconducting characteristics, while the 1T phase of MoS2 demonstrates metallic behaviours.108 To gain a better understanding of TMD materials, we have discussed their diverse properties below in detail.
image file: d6ta01482h-f7.tif
Fig. 7 Composition and crystal phases of TMDs: (a) the composition of TMDs and (b) schematic diagrams of different TMD phases, including hexagonal (2H), octahedral (1T), and distorted octahedral (1T′). The top view shows the atomic arrangement of a single layer (top panel), while the side view depicts the typical packing sequences (bottom panel). Reproduced from ref. 108 with permission from Wiley, copyright 2023.
3.1.1 Electronic properties. The unique dispersion of electronic states across the 2D plane gives rise to many remarkable properties of 2D materials. A comprehensive description of their electronic structure often requires detailed density functional theory (DFT) calculations. However, fundamental electrical properties for TMDs can be predicted from the ligand field-induced electronic splitting of the nonbonding transition metal d-orbitals and the filling of these orbitals.113 All layered TMDs crystallise in either octahedral or trigonal prismatic coordination, with group 6 compounds typically adopting the latter in their most stable form, known as the 2H phase. In this 2H phase, the ligand field splitting of the d-orbitals results in the formation of dz2 (a1′), dx2y2,xy (e′), and dxz,yz (e″) bands, which are separated by an energy gap. The two d-electrons of the transition metal fill the a1′ orbital, giving the material semiconducting properties. Octahedrally coordinated TMDs, commonly known as the 1T phase, feature degenerate dxy,yz,zx (t2g) and dz2,x2y2 (eg) orbitals. Group 6 TMDs are typically unstable in the octahedral coordination; however, the phase can be induced through alkali metal intercalation or high-dose electron irradiation. Since the lower-lying t2g orbitals are only partially filled, group 6 TMDs in the 1T phase exhibit metallic electronic behaviour.113

2D TMDs show distinctive optical and electrical properties because of quantum confinement and face phenomena, notably arising from the transition of the bandgap, undergoing a transition from indirect to direct as the material is reduced to monolayers. The tunable bandgap of 2D TMDs, along with their robust photoluminescence (PL) coupled with high exciton binding energy, positioned them as optimistic materials for diverse areas of optoelectronic applications, including solar cells, photodetectors, LEDs, phototransistors, etc.114–116 MoS2, for example, displays inimitable assets like a direct bandgap ∼1.8 eV, high mobility (around 700 cm2 V−1 s−1), a large current on/off ratio (∼107–108), significant optical absorption (∼107 m−1 in the visible range), and strong photoluminescence (PL) due to the direct bandgap in the monolayer. These remarkable characteristics have made MoS2 widely studied for electronic and optoelectronic applications.117

3.1.2 Transport properties. The progression from 3D to 2D brings about significant changes in material properties. Key characteristics of TMD monolayers, including a stable structure, electron mobility, and bandgap, make them ideal for semiconductor fabrication. Thin-layer TMDs generally exhibit lower electron mobility than their bulk counterparts. However, this carrier mobility can be enhanced by coating the TMDs with materials such as HfO2 and hexagonal boron nitride (hBN).51
3.1.3 Mechanical properties. The properties of TMDs are largely governed by their band gap. Monolayers of 2D materials were more challenging to deform uniformly, so AFM (atomic force microscopy) was employed for identifying mechanically exfoliated monolayer flakes without defects. For instance, MoS2 exhibits a Young's modulus of approximately 270 GPa for monolayer flakes (200 GPa for bilayer flakes), with a strain tolerance of up to 10% before failure. As the number of layers increases, Young's modulus of multilayer flakes (ranging from 5 to 25 layers) increases to around 330 GPa. As strain increases, both the direct and indirect band gaps of the material decrease, with the indirect band gap decreasing more rapidly than the direct band gap. This results in a reduced emission efficiency in monolayer TMDs under high strain.51

3.2 Merits, demerits, and mitigation strategies

Owing to their unique properties and beneficial features, TMDs hold significant promise as electrode materials for advanced energy storage devices, such as supercapacitors.
3.2.1 Merits. (a) High specific surface area: the large specific surface area of TMDs greatly benefits their electrochemical performance. Increased surface area provides more active sites, improving ion adsorption and charge transfer, which facilitates faster ion diffusion. This directly impacts their rate capability and overall performance, particularly in monolayer TMDs where the surface area is the greatest. Thanks to their high surface area, TMD electrode materials are ideal for more efficient, high-response energy storage devices.118–120 (b) Tunable layered structure: TMDs possess a distinctive layered architecture, with neighbouring layers held together by van der Waals forces. This characteristic enables them to rearrange their layers in response to external stimuli, facilitating safer, easier exfoliation and restacking.121 By modifying the number of layers and the interlayer distance, one can easily tune electronic conductivity, ion mobility, and mechanical properties. Typically, monolayer and few-layer TMDs offer enhanced conductivity and quicker ion transport, thereby improving supercapacitor efficiency.122 (c) Tunable band gap: the range of TMDs depends on their band-gap thickness and phase, due to quantum-confinement effects that enhance carrier mobility.123 For example, in 2H-MoS2, the bulk band gap is 0.88 eV, while the monolayer's band gap can reach 1.71 eV, enabling tunable indirect-to-direct band-gap transitions.124 Meanwhile, monolayer 1T-MoS2 exhibits metallic conductivity with a negligible bandgap, whereas the 1T′ phase features a narrow bandgap and quasi-metallic properties.125 Hence, by varying the band gaps of TMDs, their electronic properties can be customised. (d) Chemical stability: the valence electrons of transition metals interact with the p-orbitals of chalcogens, forming a stable electronic configuration. d–p hybridisation boosts the strength and stability of the TMD crystal lattice. Consequently, TMDs exhibit consistent performance over long electrochemical cycles with little degradation, even under harsh conditions. The strong M–X bonds also provide corrosion resistance in acidic and alkaline environments, rendering TMDs ideal for energy storage applications.126
3.2.2 Demerits. (a) Restacking of layers: interlayer aggregation and restacking hinder the energy storage of TMDs by reducing surface area and ion transport. Weak van der Waals forces cause these materials to aggregate or restack under external forces or in solution, leading to structural damage and lower performance in supercapacitors.127 (b) Structural collapse: during charge–discharge cycling, TMDs undergo volume expansion and mechanical strain, which can damage the lattice, disrupt interlayer interactions, and lead to structural collapse, thereby affecting cycling stability.128 (c) Low conductivity: covalent bonding between transition metals and chalcogen atoms leads to electron localisation, limiting charge delocalisation and electronic conductivity. The low conductivity of TMDs mainly results from weak interlayer bonding that restricts electron mobility and alters their electronic structure, making charge excitation or transport difficult. Defects and impurities introduced during synthesis can scatter charge carriers, further reducing conductivity.129 (d) Susceptibility to oxidation: TMDs are prone to oxidation when exposed to air, as oxygen molecules adsorb on their surfaces, altering the oxidation state of the metal centres and accelerating oxidation. This results in oxides with poor conductivity and low electrochemical activity. The surface's tendency to adsorb oxygen alters the oxidation states of metal ions, damaging the lattice and reducing stability.130,131

Surface modification and heterojunction engineering enhance conductivity and reduce interfacial resistance. Creating nanostructures with specific arrangements improves electron transport. Organic molecules, polymers, or chemical modifications prevent restacking. External electric or magnetic fields can alter interlayer interactions. Designing nanostructures with strong interlayer forces, like porous or heterostructures, stabilises TMDs. Surface treatments like carbon coating or doping decrease oxidation. Combining TMDs with stable materials like metal oxides or nitrides forms heterostructures or composites to further prevent oxidation. Approaches such as doping, forming composites, or using confined structures strengthen interlayer bonds and prevent degradation and collapse.132–134

3.3 Synthesis routes for TMDs

The synthesis of TMDs typically follows two principal routes: top-down and bottom-up methods.135–137 The bottom-up procedure involves building nanomaterials formed using atomic or molecular building blocks, which allows for precise control over their properties at the nanoscale. In contrast, the top-down method involves controlled downscaling of bulk materials to nanoscale forms, often used in top-down fabrication processes for the generation of thin sheets using diverse physicochemical processes. Each approach presents unique advantages and can be chosen according to the desired characteristics and applications of the TMDs (Table 1).138,139
Table 1 Different synthesis methods of TMDsa
Material Synthesis route Precursors Preparative parameters Morphologies Ref.
a Hydro: hydrothermal, LPE: liquid-phase exfoliation, Oxi: oxidation, CVD: chemical vapour deposition, MW: microwave-assisted, TR: thermal reduction, VF: vacuum filtration, DCS: DC sputtering, Li-SE: Li-intercalation and sonication-assisted exfoliation, CBD: chemical bath deposition, Solvo: solvothermal, BM: ball milling, SCM: soft chemical method, BS-DC: bath sonication followed by dip-coating, LE: liquid exfoliation, PAS: polyquaternary ammonium salt, MSE: mixed solvent exfoliation, PEG-800: polyethylene glycol-800, VGCNF: vapor grown carbon nanofibers, T-S: target to substrate, and Soni: sonication.
FeNi2S4-g-MoSe2 Hydro (FeCl3·6H2O, NiCl3·6H2O), thiourea, and exfoliated TMDs (MoSe2 or MoS2) 180 °C, 24 h Hierarchical nanostructure 103
1Td WTe2 LPE Single crystals of 1Td WTe2 (type-II Weyl semimetal) Soni: 600 W, 8 h, cooling Few-layer nanosheets (2–7 layers) 180
h-WO3/WS2 Oxi/CVD WO3 nanowires Vacuum (10−3 mTorr), Ar, 850 °C, 20 °C min, 40 min Nanowires 181
rGO/TMD composite papers (MoS2, MoSe2, or MoTe2) LPE/TD/VF TMD powders and super acids (chlorosulfonic acid and methanesulfonic acid) Soni: 30 min, Ar (glovebox), RT Nanosheets 182
MoS2-rGO/PGE LPE; refluxing MoS2 powder; rGO and aq. MoS2 Soni: 100 W, 80 kHz, 90 min; 100 °C, 6 h (reflux) Heterostructure 183
MoS2 DCS MoS2 and copper foil Bias (MoS2 target), 6 cm (T-S), 45 W, 300 °C, 30 min Nanoworms 184
1T-2H-hybrid MoS2 Solvo MoS2 powder and n-butyllithium solution in hexane 90 °C, several h Well-packed layered structure with wrinkles 185
Edge-oriented MoS2 CVD Sulphur powder 200–300 °C, 50 mTorr, Ar (100 sccm), 0.5–2 h, natural cooling Sponge-like films 186
1T-MoS2 Li-SE Bulk MoS2 powder and n-butyllithium in n-hexane 187
MoS2 Hydro Sodium molybdate and thioacetamide 200 °C, 24 h Mesoporous morphology 188
MoS2 Two-step hydro Molybdenum trioxide and thiourea 180 °C, 40 h Uniform 3D flower-like nanostructures 189
MoS2 Hydro-PAS Sodium molybdate and thiourea 220 °C, 24 h Microflower 190
MoS2 SDBS assisted hydro Ammonium molybdate tetrahydrate and thiourea 220 °C, 18 h Nanosheets 191
Yolk–shell MoS2 Hydro Ammonium molybdate, thioacetamide, and PEG-800 180 °C, 3 h Microspheres 192
2D-MoS2 Hydro Ammonium molybdate and thiourea 220 °C, 24 h Spherical rose-flower-like structures 193
MoS2 CBD Ammonium molybdate, sulfuric acid, and sodium sulfide RT, 1 h Nanoflakes 194
MoS2 Hydro Sodium molybdate dihydrate and thioacetamide 200 °C, 24 h Nanosheets 195
MoS2 thin film SCM Ammonium heptamolybdate, sulfuric acid, and thioacetamide Water bath (303 K), 5 h Nanograins 196
3D-MoS2 BS-DC Ammonium tetrathiomolybdate 600 °C, 2 h, Ar (tube furnace) Nanodots 197
1T-2H-hybridised MoS2 monolayers Solvo MoS2 powder; n-butyllithium 90 °C, several h Nanosheets 185
MoS2; WS2; TiS2; MoSe2 LE MoS2; WS2; TiS2; MoSe2 powders Soni: 37 kHz, 40% amp., 12 h ‘Paper’ like structure for all 198
MoS2 BM Bulk MoS2 300 rpm, 48 h Nanosheets 199
Ex-MoS2 LE Commercial MoS2 powder and n-butyllithium Expanded layer 200
IE-MoS2 (IE = interspace-expanded) LE Sodium molybdate dihydrate, and thiourea Soni: 2 h Nanoflower 201
Freestanding MoS2 hydrogel LE 1T phase MoS2 and sulfuric acid 202
MoS2 MSE Bulk MoS2 Soni: 8 h Nanoflake-like morphology 203
1T-MoS2 Hydro Molybdenum trioxide and thioacetamide 200 °C, 12 h Nanoflowers 204
3DG-VS2 In situ hydro Graphene oxide, ammonium metavanadate, and thioacetamide 180 °C, 24 h Nanosheets 205
MoS2/Mn Hydro MnCl2, MoO3, potassium thiocyanate, and sodium dodecyl sulphate 180 °C, 24 h Flower-like hierarchical 3D structure 206
MoS2 nanowall/VGCNF MW hydro Na2MoO4·2H2O and thiourea 100 W, 200 °C, 30 min, 15 °C min Nanowalls 207
VS2 CVD Sulphur (S) and vanadium(III) chloride (VCl3) 600 °C, 25 min, Ar Nanosheets (thickness 10 nm) 208


3.3.1 Bottom-up approach. The technique is effective for producing ultrathin, high-quality nanocomposites with large lateral dimensions, and large-scale production costs are typically low, as nanoscale materials are assembled using bottom-up processes that start from atomic or molecular sources.135,140 The methods include hydrothermal, solvothermal, electrodeposition, sol–gel, and many more. Some of them are discussed below.
3.3.1.1 Hydrothermal method. The hydrothermal process serves as a standard technique for synthesising high-quality materials with precise control over their morphology.141 Conducting synthesis at high pressure and temperature in an aqueous or non-aqueous solution within an autoclave makes this method scalable, cost-effective, and effective at producing materials with fewer defects, suitable for applications in electronics, energy storage, and catalysis.142,143 By heating a precursor solution in an autoclave, the hydrothermal method facilitates the creation of materials with diverse sizes and shapes. As shown in Fig. 8(A and B), J. Zhao et al. prepared a particular nanostructure consisting of Ni3Se2 nanosheets (NSs) grown on the surface of NiSe nanowire assembly (NWAs), which were successfully synthesised and deposited onto nickel foam through a one-step in situ hydrothermal approach, coupling with an electrodeposition route.144 Bogale et al. synthesised MoS2@CuCo2O4 with a palm-leaf morphology for a bottom-up approach and demonstrated it as a highly effective electrode for asymmetric supercapacitors, showcasing significant advancements in energy storage technology.145 The hydrothermal approach is a commonly used technique for the synthesis of TMD-supported rGO heterostructures. Abdullah et al. (Fig. 8(C and D)) created a MoTe2 supported on rGO nanocomposite using this approach, which involves a chemical reaction in a sealed container at high temperature and pressure, with water as the solvent. The morphology analysis revealed that MoTe2 has an irregular nanoparticle structure with porous features, which enhances ion accessibility, and rGO exhibits a diffused nanosheet architecture with high surface area and flexibility. In the MoTe2/rGO composite, MoTe2 particles were embedded in overlapping rGO sheets, which form a conductive network and also highlight the strong bonding between MoTe2 and rGO, showing a suitable SC performance. The presence of molybdenum (Mo) and tellurium (Te), and high carbon content from rGO can be confirmed by EDS analysis.146
image file: d6ta01482h-f8.tif
Fig. 8 (A) Schematic illustration of the synthesis of NiSe NAs@Ni3Se2 NS composites. (B) SEM images at different magnifications of (a–c) NiSe NWAs and (d) NiSe NWAs@Ni3Se2 NSs. Reproduced from ref. 144 with permission from Elsevier, copyright 2021. (C) Graphical illustration of a synthetic scheme for the MoTe2/rGO nanocomposite, (D) SEM micrograph of (a) MoTe2, (b) rGO and (c) the MoTe2/rGO nanohybrid and (d) EDX spectrum of the MoTe2/rGO nanohybrid. Reproduced from ref. 146 with permission from Elsevier, copyright 2023.

3.3.1.2 Solvothermal method. The solvothermal method is a popular synthesis technique where precursors like metal salts and sulfur sources are dissolved in an organic solvent (like ethanol, ethylene glycol, etc.). Now, the mixture is then heated in a sealed autoclave under elevated temperature and pressure conditions.147 This process not only allows for controlled growth of nanostructures with a specific size, shape, and thickness but also enhances crystallinity and reduces impurities in the final product.148 Using this method, materials generally showcased increased surface area, better conductivity, and stable morphologies, allowing their application in areas like energy storage and SCs.143,149 Kumar et al. synthesised a Ni-MoS2@SnS2 flower-like nanocomposite via a facile one-step solvothermal method as shown in Fig. 9(a–d).150 Karuppasamy et al. successfully synthesised a composite of iron sulfide/reduced graphene oxide (Fe3S4/rGO) using a standard solvothermal approach. FESEM showed that Fe3S4 nanoparticles possessing an average diameter of <50 nm are distributed evenly across the surface of rGO.151 Singh et al. synthesised a layered 2H-WSe2 structure through a single-step solvothermal method. SEM micrographs of WSe2 reveal a highly porous network of layered nanostructures with a 40 nm thickness of the WSe2 nanosheets.152
image file: d6ta01482h-f9.tif
Fig. 9 (a) Scheme route of Ni-MoS2@SnS2, (b) FESEM image of 10% Ni-MoS2@SnS2, (c and d) TEM & HRTEM image of 10% Ni-MoS2@SnS2. Reproduced from ref. 150 with permission from Wiley, copyright 2025. (e) Characterisation of as-grown single-crystalline T-VS2 nanosheets on SrTiO3 (100) substrates, schematic of the CVD setup for T-VS2 synthesis, and (f) AFM and SEM images of T-VS2/SrTiO3 (100), respectively; the inset shows the thickness of an individual T-VS2 nanosheet. Reproduced from ref. 153 with permission from Elsevier, copyright 2025.

3.3.1.3 Chemical vapor deposition (CVD). CVD is a key technique for fabricating thin and high-quality layers. This method utilises vapor-phase precursors that chemically react on a heated substrate, ensuring precise deposition of material layers. In this synthesis technique, using high temperature facilitates the production of materials characterised by uniform thickness and large surface area, leading to better crystallisation and electrical efficiency while eliminating harsh chemical treatments.135,154 Common precursors include metal oxides like MoO3 and WO3, along with chalcogen sources such as sulphur, selenium, and tellurium. Carrier gases like argon and nitrogen are used to transport precursor materials into the reaction zone and are often mixed with hydrogen gas to establish a reducing environment. Through precise regulation of reaction temperature (typically 600–900 °C), pressure, and gas flow rate, CVD ensures the controlled deposition of uniform and scalable layers of TMD materials. Depending on synthesis requirements, various CVDs such as atmospheric pressure CVD (APCVD), low-pressure CVD (LPCVD), and metal–organic CVD (MOCVD) are utilised.155 Jin et al. thoroughly examined how various growth parameters in a CVD process influence T-VS2 nanosheet synthesis, as shown in Fig. 9(e). They observed that lowering the growth temperature tends to increase sheet size, while higher vanadium precursor concentrations effectively control the nanosheets' thickness. Longer reaction durations can lead to nanosheet flipping. Additionally, the shape of T-VS2 is affected by temperature, V source supply, and H2 supply, resulting in a shift among trapezoidal, truncated triangular, and hexagonal forms. By carefully tuning these factors, a precise growth strategy for T-VS2 can be established. SEM and AFM (Fig. 9(f)) analyses confirm the production of well-defined 2D VS2 nanosheets with controllable size and thickness, whose morphology is influenced by growth conditions.153
3.3.1.4 Microwave-assisted synthesis. The microwave-assisted method provides a highly efficient and rapid route for the fabrication of TMDs, which are widely used in SC applications.156,157 This method involves dissolving metal salts and chalcogen sources in a solvent and then irradiating them with microwave radiation. The microwave energy heats the precursor materials rapidly, enabling the formation of TMDs like MoS2 and WS2 in less time than conventional methods, and this energy ensures the uniform heating of materials, by which the crystallinity and consistency of the TMDs can be improved. Also, this process offers faster synthesis, higher yields, and the ability to modify material properties for enhanced SC performance. Sahoo et al. presented a swift, cost-effective microwave technique to synthesise a nanocomposite composed of graphitic C3N4, reduced graphene oxide (rGO), and MoS2 using ultrafast MW irradiation (see Fig. 10(A)). The FESEM image (Fig. 10(B)) reveals commercial MoS2 with a nanoflake structure, characterised by random orientation and agglomeration. In contrast, the rGO/MoS2 nanocomposite shows MoS2 nanoflakes that are more ordered, mostly hexagonal, and grown on exfoliated rGO nanosheets that serve as templates. The g-C3N4/rGO/MoS2 flakes appear distorted yet interconnected. These differences are due to the templating effects of rGO versus g-C3N4-coated rGO. The interconnected flakes on conductive nanosheets likely improve electron transport.158
image file: d6ta01482h-f10.tif
Fig. 10 (A) Schematic representation of the synthesis routes for GM (rGO/MoS2) and CNGM (g-C3N4/rGO/MoS2), (B) FESEM images at various magnifications of (a and b) commercial MoS2, (c and d) GM, and (e and f) CNGM. Reproduced from ref. 158 with permission from Elsevier, copyright 2025. (C) Electrodeposition of composites, (a) particle addition to the electrolyte, (b) particle entrapment by the metal, and (c) composite coating. Particles are encircled in red. Reproduced from ref. 160 with permission from Elsevier, copyright 2022. (D) (a) Top surface FE-SEM image, (b) FE-SEM cross-sectional view, and (c and d) TEM visualisation of a prepared sample. Reproduced from ref. 162 with permission from Elsevier, copyright 2025.

3.3.1.5 Electrochemical deposition. Electrochemical deposition is an important method for fabricating TMDs for SCs. In this process, metal ions from an electrolyte are reduced and deposited onto a conductive electrode by applying an electric current, where they react with sulphur or selenium to form TMD nanostructures and films.159 Here, a three-electrode system is utilised, enabling precise control over shape, thickness, and properties by adjusting parameters like voltage, temperature, and duration.160 This scalable and cost-effective technique is ideal for producing materials like MoS2 or WS2, which enhance SC efficiency because of their excellent surface area and conductivity.161 Najafi et al. electrochemically deposited Mn–Ni–Co–S on annealed flexible titanium oxide (TiO2) nanotube arrays (synthesised via anodization of titanium sheets) and ITO using CV, sweeping from −1.2 to 0.2 V at 5 mV s−1 for 5 cycles in a metal nitrate–thiourea electrolyte. The synthesised sample reveals nanoflower-like formations growing on the titanium oxide nanotubes, and the close arrangement of the nanotubes and their perpendicular positioning to the substrate are indicated in the magnified cross-sectional views as depicted in Fig. 10(C)(a–c). Furthermore, TEM images (Fig. 10(D)) showed individual TiO2 nanotubes with a straight hollow channel structure, with the wall thickness, inner diameter, and outer diameter measuring 32.98 nm, 111.1 nm, and 174.4 nm, respectively.162
3.3.1.6 Sol–gel method. The sol–gel technique is employed to synthesise various TMDs (e.g. MoS2), and this process involves dissolving metal precursors like ammonium molybdate and chalcogen sources like thiourea in a solvent to form a uniform solution. Then the solution undergoes chemical reactions and forms a gel, after which it is dried and subjected to heat treatment to yield materials.163 The sol–gel method provides control over the material's composition, shape, and purity.164 Materials made using this method offer a large surface area and better conductivity, along with strong electrochemical performance, making them ideal for use in SCs. It is also cost-effective, scalable, and adaptable for performance enhancement.165
3.3.2 Top-down approach.
3.3.2.1 Scotch-tape method. The scotch-tape technique is recognised as the least complex and most time-effective approach for synthesising 2D TMDs.166 It involves using a bulk material (e.g. MoS2) as the starting material and peeling off sections with sticky tape.167 Due to van der Waals forces, some portions stay adhered to the substrate when the tape is removed. Repeating this process produces MoS2 flakes in various shapes, sizes, and layers.168,169 Also referred to as micromechanical exfoliation, this method is a quick and versatile approach that allows easy transfer of single-layer MoS2 to the desired substrate.170
3.3.2.2 Liquid phase exfoliation (LPE). This process involves dispersing bulk TMD crystals into a solvent and exfoliating them using mechanical forces like sonication or high-shear mixing and leads to the formation of nanosheets or few-layer flakes, which remain stable in the liquid phase.171,172 While liquid-phase exfoliation (LPE) can generate TMDs having good surface area as well as strong electrochemical characteristics, issues with dispersion stability and achieving high monolayer yields still exist.173
3.3.2.3 Ball milling. Ball milling is employed as a top-down approach for synthesising nanoscale materials by grinding bulk materials with grinding media.174 The mechanical forces reduce the material size, exfoliate bulk TMDs into thin nanosheets or nanoparticles, and improve the surface area, leading to better charge storage and electrical conductivity.175,176 This scalable method enables precise tailoring of material behaviour, but challenges such as agglomeration as well as inconsistent size distribution necessitate careful optimisation of milling parameters.177,178 As shown in Fig. 11(B), Dong et al. employed ball milling to synthesise and modify the electrode material by mechanically blending precursor components. This process uses high-energy impacts between balls and powders, ensuring thorough mixing and inducing structural changes. As a result, the material exhibited smaller particle sizes and improved homogeneity, thereby enhancing its electrochemical performance. The benefits stem from the mechanochemical effect of ball milling, which increases contact between components and modifies their structural properties. SEM analyses (Fig. 11(B)) validate the creation of a clearly defined and structurally altered material following ball milling.179
image file: d6ta01482h-f11.tif
Fig. 11 (A) Schematic illustration of the synthesis process of the MoS2/FLG (FLG: few-layer graphene) composite and (B) SEM images of MoS2/FLG@1 h, MoS2/FLG@3 h, and MoS2/FLG@10 h, highlighting the evolution of surface morphology with reaction time. Reproduced from ref. 179 with permission from Elsevier, copyright 2025.

4. Supercapacitors based on pristine TMDs

TMDs gained significant attention as promising electrode materials for SCs owing to their exceptional specific power, superior electrical conductivity, as well as structurally adaptable nature. Their bandgap, ranging from 0 to 2 eV, can be precisely tuned by modulating factors such as the elemental composition, atomic arrangement, and layer thickness. The adjustable nature of these materials enhances their electrochemical characteristics while also enabling the development of optimised transition architectures for high-performance energy storage applications, making them highly significant for industrial implementation. Among various nanomaterials utilised for electrochemical SC applications, both layered and non-layered transition metal sulfides (TMSs) have garnered increasing focus stemming from their widespread availability, cost-effectiveness, eco-friendliness, and elevated theoretical capacity.209

4.1 TiX2 (X: S, Se, and Te)

Limited studies have explored the potential of layered TiS2 for electrochemical SC applications despite its advantageous properties, including a fast ion transport rate, high electrical conductivity (1.4 × 103 Ω−1 cm−1),210 and remarkable theoretical capacitance (239 mAh g−1 for sodium storage).211,212 Additionally, it offers excellent stability due to its minimal volume expansion during reversible charging–discharging cycles. Ucar et al. recently produced self-standing, binder-free, electrically conductive 2D 1T-TiS2 flakes via organolithium exfoliation. The obtained 2D structure enhanced interlayer spacing for easy intercalation and excellent conductivity, enabling binder-free self-standing films.213 The single electrode exhibited a Cs of 128 F g−1 at 10 mV s−1. Furthermore, the symmetric SC stored 96.1% capacity after 10[thin space (1/6-em)]000 cycles and 85.5% after 18[thin space (1/6-em)]000 cycles. In another study, Wang et al. fabricated a new Zn-ion hybrid SC (ZHSC) using a TiS2 battery-like anode, an AC capacitor-type cathode, and ZnSO4 electrolyte to address challenges like slow zinc-ion diffusion and dendrite formation. The TiS2 fragments are prepared via liquid-phase exfoliation, and Fig. 12 shows the TiS2//AC ZHSC, which stores energy through zinc-ion intercalation in the TiS2 anode and SO42− adsorption on the AC cathode. It delivers a high Cs of 249 F g−1, Ed of 112 Wh kg−1, and Pd of 3600 W kg−1, and it stores 92% C after 5000 cycles. This eco-friendly design grants access to advanced, superior energy storage systems.214
image file: d6ta01482h-f12.tif
Fig. 12 (a) Electrochemical performances of the TiS2//AC ZHSC, (b) CV of TiS2, the AC electrode, and TiS2//AC ZHSC @ 5 mV s−1, (c) Cs versus current density, (d) cycling performance (inset shows an LED lit by a TiS2//AC ZHSC), and (e) Nyquist plots (inset shows the fitting equivalent circuits) of the TiS2//AC ZHSC. Reproduced from ref. 214 with permission from Wiley, copyright 2020.

4.2 ZrX2 (X: S, Se, and Te)

ZrS2 is highly preferred for SCs and various other energy storage systems due to its superior stability, minimal diffusion path, enhanced electron transport capacity, abundant availability, ease of synthesis, cost-effectiveness, and ability to exhibit multiple oxidation states.215,216 Habib et al. synthesised zirconium disulfide/diselenide (ZrX2, X = S, Se) single crystals via the chemical vapour transport process and studied them for SC applications. ZrS2 achieved a Cs of 18.8 F g−1, while ZrSe2 showed 18 F g−1 at 10 mV s−1. ZrSe2 demonstrated robust charge–discharge endurance (>90%), and ZrS2 benefited from higher layer spacing for better capacitance. These materials exhibit high conductivity as well as reliability, rendering them excellent candidates for SC electrodes without requiring carbon additives.217 Using a chemical bath deposition technique, Gokulsaswath et al. fabricated zirconium disulfide (ZrS2) quantum dots; CV analysis of ZrS2 QDs demonstrated faradaic charge storage, evident from distinct anodic and cathodic peaks. With an increasing scan rate (5–100 mV s−1), a progressive reduction in the CV area was observed, attributed to diffusion-limited ion transport, which consequently altered the electrolyte-ion dynamics at the electrode interface. Furthermore, the GCD curves of the ZrS2 QD-based electrode show symmetric charge/discharge behaviour, signifying stable electron transport and material reliability. The faradaic process improves electron access, prolonging discharge time and leading to a Cs of 101.75 F g−1 at 1 A g−1, slipping to 5.11 F g−1 at 10 A g−1, showing strong electrochemical activity and reversibility and providing a Ed of 45.78 Wh kg−1 with Pd of 14.99 W kg−1. EIS analysis reveals an incomplete semicircle in the Nyquist plot, indicating pseudocapacitance with low resistance and high conductivity at high frequencies, and the material shows lower electrochemical conductivity (solution resistance is 97 Ω). Based on these findings, ZrS2 QDs show potential for use in energy storage applications.218

4.3 VX2 (X: S, Se, and Te)

Metallic VX2 stands out among TMDs owing to its excellent physical properties, including superconductivity, electrical conductivity, charge density wave, optical behaviour, and magnetism, making it an ideal candidate for applications within condensed-matter science, materials physics, and device technology.219 Nandana et al. examined VS2 nanosheets as an electrode material for supercapacitors and synthesised them through a single-step hydrothermal process at 220 °C for 24 hours. The resulting electrode was further tested using symmetric supercapacitors made with these VS2 nanosheets (Fig. 13(a and b)), which exhibited a Cs of 106 F g−1 at a current density of 1 A g−1. This setup achieved an Ed of 34[thin space (1/6-em)]Wh kg−1 at a Pd of 800 W kg−1, as shown in Fig. 13(c). Additionally, the supercapacitor retained 94% of its capacitance after 9000 charge–discharge cycles at 5 A g−1 (Fig. 13(d)), demonstrating the promising potential of VS2 nanosheets as effective electrode materials for supercapacitor applications. The improved electrochemical performance is driven by the high surface area, metallic conductivity, fast ion diffusion, and reversible redox activity of VS2 nanosheets, which enhance charge storage and cycling stability.220
image file: d6ta01482h-f13.tif
Fig. 13 (a) CV, (b) GCD, (c) Ragone plot, ans (d) capacitance retention profile for 9000 cycles at 5 A g−1 of VS2 nanosheets. Reproduced from ref. 220 with permission from Wiley, copyright 2025.

Feng et al. highlighted the potential of VS2 as an advanced material for ultrathin, a flexible energy retention tool by introducing an innovative ammonia-assisted exfoliation technique to synthesise VS2 nanosheets through an ultrathin structure of less than five S–V–S layers, leveraging their metallic properties and high conductivity for in-plane SC electrodes. The resulting VS2 thin films demonstrated exceptional performance, achieving a Cs of 4760 µF cm−2 in a 150 nm configuration with excellent cycling stability (no significant degradation after 1000 cycles).221

4.4 MoX2 (X: S, Se, and Te)

MoS2 distinguishes itself among TMDs due to their unique physical characteristics exhibited in mono-layer, multi-layer, and restacked configurations, which can be obtained through chemical exfoliation. The surface morphology of MoS2 nanosheets can be tailored to improve their electrochemical efficiency.222 Nardekar et al. synthesised exfoliated MoS2 quantum sheets (5 to 10 nm) via a salt-assisted ball-milling technique because it reduces MoS2 size and layers more effectively than wet milling due to shear stress from NaCl crystals. It is clear that MoS2 QDs show superior electrochemical properties compared to bulk MoS2 due to their quasi-rectangular CV profile and minor redox peak, with the reduction in MoS2 sheet size and layer count facilitating ion transport and intercalation, while the metallic 1T phase transition contributes to higher quantum capacitance. A flexible symmetric SC based on MoS2 QSs fabricated with the MoS2 QS-coated carbon cloth electrode along with PVA/H2SO4 electrolyte shows a Cs of 162 F g−1 @ 1 mA, and exhibited high coulombic efficiency (>90%) with good rate reliability, having an Ed of 14.46 Wh kg−1 @ 1 mA and 6 Wh kg−1 @ 10 mA, even though Pd increased from 200 W kg−1 to 2000 W kg−1.223 Mishra et al. reported three-dimensional 2H-phase MoS2 nanoflowers targeting SC-based applications. The 2H-MoS2 nanoflower-derived electrodes exhibited a superior Cs of 382 F g−1 @ 1 A g−1 in 1 M Na2SO4 aqueous electrolytic solution. An asymmetric solid-state SC having 2H-MoS2 nanoflowers or PVA-Na2SO4 electrolyte demonstrates an Ed of 16.4 Wh kg−1 @ 0.2 A g−1 and outstanding retention of 97.5% after 4000 cycles.224 Abraham et al. impregnated 5 nm MoS2 nanodots (NDs) on a 3D nickel substrate via utilising a dip-coating technique without binder electrodes. MoS2 NDs were synthesised through controlled sonication of MoS2 nanosheets. The electrode showed good results, delivering a Cs of 395 F g−1 @ 1.5 A g−1 in a three-electrode setup. For a symmetric SC, the MoS2 NDs exhibited 122 F g−1 at 1 A g−1 and 86% capacitance retention after 1000 cycles, along with a gravimetric power and Ed of 10[thin space (1/6-em)]000 W kg−1 and 22 Wh kg−1, respectively.197 Although research on molybdenum selenide (MoSe2) is limited, it holds potential for superior electrochemical and energy storage properties compared to other molybdenum chalcogenides. In contrast, MoS2 and MoO3 have been extensively studied. MoS2, a widely researched TMD, is favoured in energy-saving applications owing to its unique and diverse properties. While MoS2 exhibits strong electrochemical performance, MoSe2 is known for its better cycling stability.15 Vattikuti et al. synthesised a uniform MoSe2 nanostructure using a microwave-assisted process, achieving a Cs of 257.38 F g−1 @ 1 A g−1 along with good cyclic reliability up to 5000 cycles.225 Upadhyay et al. synthesised layered 2H-MoSe2 nanosheets (Fig. 14(a and b)) via in situ selenization and evaluated SC performance in KOH electrolyte. The MoSe2 electrode exhibits battery-like faradaic behaviour, with Mo4+/Mo3+ redox transitions and K+ ion intercalation/extraction. Its hexagonal structure enables efficient ion diffusion, while minimal peak shifts indicate low polarisation and high reversibility. GCD measurements (Fig. 14(c)) reveal a capacity of 46.22 mAh g−1 @ 2 A g−1, decreasing to 30 mAh g−1 at 10 A g−1. An endurance test showed a 25% capacity loss after 1000 cycles, stabilising at 56.5 mAh g−1 (64% of the initial capacity). Coulombic efficiency improved from 88% to 90% after 2000 cycles. EIS measurements indicated consistent resistance (∼0.85 Ω) and decreasing charge transfer resistance (Rct), confirming efficient charge transfer. An asymmetric SC using MoSe2 operated effectively up to 0–0.6 V and showed excellent performance, with CV curves indicating strong capacitive properties and pseudocapacitive behaviour at 10–90 mV s−1. The charge–discharge curve demonstrates high reversibility, with Cs ranging from 4.1 to 0.5 F g−1 at 0.5 to 1 A g−1. The Ragone curve (Fig. 14(d)) reveals a maximum Ed of 184.5 mWh kg−1 at 74.6 mW kg−1. It maintains 22.6 mWh kg−1 at 155.6 mW kg−1, indicating good rate capability. Cycling stability tests (Fig. 14(e)) show a retention of 105% up to 10[thin space (1/6-em)]000 cycles and CE increasing from 98% to 100%, confirming the strong performance and stability of the MoSe2 SSC. These properties highlight the potential of MoSe2 nanosheets as efficient electrodes for SCs.226
image file: d6ta01482h-f14.tif
Fig. 14 (a) Crystal structure of monolayered hexagonal MoSe2 showing the plane of Mo (blue) sandwiched in Se (red), (b) digital photograph of MoSe2 SSC, (c) current density versus Cs estimated from GCD curves, (d) Ragone plot for MoSe2 SSC, and (e) cyclic response & CE @ 1 A g−1. Reproduced from ref. 226 with permission from Elsevier, copyright 2021. (f) Capacitance variations for MoTe2, MoSe2, and MoS2 nanostructure electrodes, (g) EIS profiles of MoTe2, MoSe2, and MoS2 nanostructures, (h) asymmetric device construction, (i) asymmetric capacitances for the MoTe2 device, (j) capacitance retention profiles over 5000 continuous cycles for the MoTe2 asymmetric device at 10 A g−1 applied current, and (k) Ragone plots for the MoTe2 asymmetric device and various reported literature results. Reproduced from ref. 227 with permission from Wiley, copyright 2022.

Bahadursha et al. synthesised MoTe2 nanosheets (NSs) via a facile and cheap liquid-phase exfoliation method to fabricate an electrode. The MoTe2 NSs demonstrated meaningfully enhanced electrochemical response, exhibiting a Cs of 859 F g−1, over threefold that of bulk MoTe2 (271 F g−1) @ 1 A g−1. The MoTe2-based electrode additionally exhibited excellent cycling stability, retaining 92.7% of initial Cs after 1000 cycles @ 10 A g−1.228 Hussain et al. studied and synthesised MoTe2, MoS2, and MoSe2 nanoarrays. Fig. 14(f and g) shows that the MoTe2 electrode achieves 416 F g−1 @ 2 A g−1, outperforming MoS2 (173 F g−1) and MoSe2 (283 F g−1), and retention of 97.1% respectively. An asymmetric SC device was constructed with activated carbon as the negative electrode along with MoTe2 as the positive electrode, separated by 1 M KOH-dipped Whatman filter paper (Fig. 14(h)). The CVdemonstrates that the device has high-rate capability and consistent performance over 100 cycles at 100 mV s−1, and the GCD reveals a nonlinear profile that indicates a prolonged charge/discharge span, and Cs was measured to be 138 F g−1 @ 2 A g−1 (Fig. 14(i)). These superior storage properties result from the unique surface nanoarray properties of MoTe2. Additionally, the device retained 95.5% of its initial Cs after 5000 cycles at 10 A g−1 (Fig. 14(j)), demonstrating better durability. Ed and Pd calculations revealed an enhanced specific energy of 49 Wh kg−1 at various power levels (Fig. 14(k)). This improved performance is linked to the optimised nanoarray morphology that facilitates ion diffusion. Practical applications, including lighting different colour LEDs, confirmed the device's efficiency in accommodating electrolyte ions.227

4.5 WX2 (X: S, Se, and Te)

Properties like superior surface areas, higher theoretical capacitance as well as surface-confined redox processes contribute to the high efficiency of 2D WS2 TMDs, leading to materials intended for energy storage purposes.229 Owing to its distinctive structural and electrical properties, WS2 is considered a promising candidate among 2D TMDs for next-generation electrochemical ESDs.77,230,231 WS2 consists of 2D covalently bonded S–W–S planes isolated through the van-der Waals gap, which is closely related to the active site for charge accumulation.232 Additionally, WS2 is of great interest because of the wide range of oxidation states of tungsten (W) atoms, ranging from +2 to +6, and its ability to store charge via an intercalation mechanism, making it a unique pseudocapacitive material. Mohan et al. synthesised WS2 nanoflowers using a simple hydrothermal method and fabricated a flexible symmetric SC by depositing two 2 mg active electrodes on a carbon fabric substrate, and using a Celgard 3400 separator, and 6 M KOH electrolyte, which was then assembled in a SC test cell (EL-Cell). The CV curves shown in Fig. 15(a) suggests a mixed charge storage mechanism involving both pseudocapacitance and double-layer capacitance. Additionally, the non-ideal triangular shape of the GCD curves (Fig. 15(b)) confirms the pseudocapacitive behaviour of WS2, driven by redox reactions. The identical Cs values of 119 F g−1 from CV (20 mV s−1) and GCD (1 A g−1) validate the accuracy of the electrochemical data. The device retains nearly 100% capacitance after 10[thin space (1/6-em)]000 cycles (Fig. 15(c)), ensuring long-term stability. Additionally, EIS analysis (Fig. 15(d and e)) confirms the low Rs (0.4 Ω) and Rct (5.2 Ω), indicating good conductivity. The Nyquist plot shows capacitive behaviour, and the Ragone plot (Fig. 15(f)) shows an Ed of 10.57 Wh kg−1.229
image file: d6ta01482h-f15.tif
Fig. 15 (a) CV of WS2, (b) GCD curve of WS2, (c) cycling stability at 5 A g−1 current density, (d) Nyquist plot, (e) equivalent circuit model employed to fit the Nyquist plot, and (f) Ragone plot of the flexible symmetric SC. Reproduced from ref. 229 with permission from Wiley, copyright 2021. (g) Specific capacity versus current density for different electrodes, (h) illustrative schematic of NiSe2-200//AC HSC, (i) Cs vs. current density of the device, (j) Ragone curve, (k) cycle stability, and (l) photos related to a clock driven by a NiSe2-200//AC device. Reproduced from ref. 233 with permission from Elsevier, copyright 2024.

Although WSe2 features a layered atomic structure and inherently favourable electrical properties, studies on WSe2-based SC electrodes remain relatively scarce.234–236 Therefore, it is essential to develop an effective pathway to augment the performance of WSe2 and strengthen its implementation in energy storage technologies.237 Sruthi et al. studied chemically modified WSe2 monolayers using ad-atom adsorption, showing high quantum capacitance (>1000 µF cm−2). DFT calculations revealed that doping shifts the Fermi level and creates new electronic states near the band edge, enhancing capacitance. These results highlight the potential of WSe2 for energy storage.238 A WSe2 thin-film SC electrode on graphite, fabricated using DC magnetron sputtering, was investigated by Tomar et al. and unveiled a significant areal capacitance of 149.75 mF cm−2, a 7.7-fold increase compared to that of bare graphite, with 86.15% retention after 2000 cycles. Using 1 M Na2SO4, the symmetric SC achieved an areal Ed of 5.54 mWh cm−2 and a Pd of 1197 mW cm−2.239

4.6 CoX2 (X: S, Se, and Te)

Octahedron-shaped CoS2 crystals were fabricated by Xing et al. through a simple hydrothermal process. These crystals exhibit a Cs of 236.5 F g−1 @ 1 A g−1 along with admirable cycling reliability, retaining 92.6% of Cs after 2000 cycles.240 Furthermore, Ren et al. directly synthesised metallic CoS2 nanowires (NWs) on current collectors like carbon cloth or graphite discs. Electrochemical responses were investigated using the three-electrode setup with KOH serving as electrolyte. CV and GCD revealed that CoS2 NWs on carbon cloth and graphite discs, respectively, particularly on graphite discs, demonstrate strong potential as high-performance SC electrodes, offering high capacitance, stable charge–discharge performance, and improved electrolyte infiltration due to their open structure. CoS2 nanowires on graphite discs gain a higher Cs 828.2 F g−1 than CoS2 nanowires on carbon cloth with a Cs of 174.1 F g−1 at 10 mV s−1 and exceptional cycling stability, with minimal capacity loss (0–2.5%) after 4250 cycles @ 5 A g−1. Ragone plots revealed good rate performance, with an Ed of 7.2 Wh kg−1 @ 0.18 kW kg−1 or 5.0 Wh kg−1 @ 0.16 kW kg−1 for CoS2 NWs on graphite discs. The relatively low Ed is attributed to the small potential range limited by the aqueous electrolyte, with higher Ed potentially achievable with organic solvents.241 Han et al. developed CoSe2 quantum dots with selenium vacancies and hollow cages using MOF templates. The optimised structure enhances active sites, reduces volumetric expansion, and improves electroactivity. The CoSe2/NC-350 electrode shows 12.13 F cm−2 capacitance at 2 mA cm−2, 90.6% retention up to 5000 cycles, an an Ed of 0.581 mW cm−2 with 92.74% retention after 10[thin space (1/6-em)]000 cycles.242 CoTe2 nanoflowers (NFs) were prepared by Mao et al. by utilising a simple solvothermal method. Their 20 nm thickness enhances exposure to the electrolyte and improves ion/charge movement. The CoTe2 NF electrode demonstrates an admirable electrochemical capacitance of 460 F g−1 @ 1.5 A g−1 and retains 91% Cs after 5000 cycles, demonstrating good durability.243

4.7 NiX2 (X: S, Se, and Te)

NiS2 hollow nanoprisms produced by Dai et al. via a cost-efficient sacrificial template technique, offer efficient ion and electron pathways due to their unique hollow structure. The prisms achieved a high Cs of 1725 F g−1 @ 5 A g−1 & 1193 F g−1 @ 40 A g−1 with LiOH electrolyte, with exceptional cycling stability, showing a 22.9% capacitance increase after 10[thin space (1/6-em)]000 cycles.244 NiS2 microflowers fabricated by Dai et al. using hydrothermal and sulphidation processes, feature a unique nano/microstructure with superior conductivity. They delivered capacities of 813 C g−1 @ 1 A g−1 & 580 C g−1 @ 20 A g−1 in LiOH, retaining 93% capacity up to 10[thin space (1/6-em)]000 cycles. A hybrid SC composed of NiS2 microflowers and activated carbon achieved an Ed of 39.8 Wh kg−1 @ 900 W kg−1.245 Arul et al. synthesised hexapod-like nickel diselenide (NiSe2) structures via the hydrothermal method and studied SC electrode materials for the first time. Characterisation confirmed the orthorhombic phase of NiSe2 in the synthesised structures. The NiSe2 electrode on graphite foil unveiled a Cs of 75 F g−1 @ 1 mA cm−2, also showing excellent cycling stability with 94% capacitance retention after 5000 cycles. The data reveal the potential of hexapod-like NiSe2 serving as a prospective option for energy storage applications.246 NiSe2 single crystals with a truncated cubic morphology were fabricated by Wang et al. and deployed as an electrode material in SC systems. The NiSe2 electrode shows a Cs of 1044 F g−1 @ 3 A g−1 (4.07 F cm−2) and admirable current rate tolerance (601 F g−1 @ 30 A g−1). An asymmetric SC based on NiSe2//activated-carbon achieved an Ed of 44.8 Wh kg−1 @ 969.7 W kg−1, along with 87.4% retention later 20[thin space (1/6-em)]000 cycles, showing great potential for practical applications.247 Porous NiSe2 nanowires (NWs) were synthesised by Li et al. by treating α-Ni(OH)2 NWs with Se powder and among the investigated electrodes, NiSe2-200 exhibited superior CV area, demonstrating the best energy storage behaviour. The CV profile of NiSe2 NWs at various sweep rates shows consistent shapes and excellent charge/discharge stability, whereas the GCD displayed nonlinear characteristics, indicating Faraday reactions for energy storage and good charge/discharge reversibility. NiSe2-200 showed a superior discharge time at 1.0 A g−1 and achieved a Cs of 653.3 C g−1 at 0.25 A g−1, maintaining 408.0 C g−1 at 10 A g−1 (Fig. 15(g)), with a 62.5% capacity retention rate. The decrease in Cs at high current densities is ascribed to the electrode's internal resistance and underutilisation of electroactive materials. Fig. 15(h and i) shows that the NiSe2-200//activated carbon hybrid SC showed excellent performance, including 88.3 F g−1 Cs, 35.4 Wh kg−1 Ed, and 74.6% retention after 21[thin space (1/6-em)]000 cycles.233 Zhang et al. synthesised hollow NiTe2 nanotubes through a low-cost hydrothermal method and evaluated them for SC applications. Their unique hollow structure, rich in defects, provides an extensive surface area coupled with effective ion transport channels, enhancing electrochemical performance. The nanotube electrodes display a superior Cs of 566 F g−1 at 1.5 A g−1 with admirable stability, rendering them attractive materials for energy storage systems.248 Nickel telluride nanorods (NiTe NRs) produced by Manikandan et al. through the hydrothermal technique using ascorbic acid acting as a reducing agent and CTAB as a surfactant, exhibit a hexagonal structure with excellent properties. Electrochemical measurements revealed a high Cs of 618 F g−1 @ 1 A g−1 as well as notable cycling, retaining 75% of capacitance after 5000 cycles with a CE above 99%. The marked conductivity, porous structure, and nickel's synergistic effects contribute to the superior performance.249

5. Supercapacitors based on modified TMDs

5.1 Doped TMDs

The incorporation of dopants into a material induces significant changes in its structural framework and physicochemical properties. Doping generally occurs through two primary mechanisms: substitutional and interstitial doping. In the substitutional doping process, dopant atoms directly replace host lattice atoms. The success of substitution depends on key factors such as the similarity in atomic or ionic radii, matching valence states, and the compatibility of coordination environments between the dopant and host atoms. In the interstitial doping mechanism, dopant atoms occupy the interstitial voids embedded in the crystal lattice instead of replacing existing atoms. This alters the material's electronic as well as structural properties while maintaining the overall lattice framework.250 Doping is a fundamental technique for tailoring the electronic properties of semiconductors by precisely regulating charge carrier concentration, shifting the Fermi level position, and amending the band gap energy. The controlled incorporation of dopants enables the fabrication of semiconductors with specific conductivity types (P-type or N-type), which is essential for optimising their efficiency in advanced electronic and optoelectronic applications.42

Hence, by doping in an SC, one can increase conductivity and surface area and attain improved structural stability as well as ion mobility. Vikraman et al. doped transition metals (Ni, Cu, and Fe) within the MoS2 nanoarrays by facile chemical precipitation and found that highly porous structured Cu doped MoS2 nanostructures show better performance for SCs by achieving a maximum Cs of 353 F g−1 at 1 A g−1 current density along with a remarkable retention of ∼94% later 5000 cycles. Furthermore, symmetric devices with Cu doped MoS2 electrodes achieved a specific energy of 5.58[thin space (1/6-em)]Wh kg−1 at 6 kW kg−1 specific power, maintaining 94% of their initial symmetric capacitance after 5000 cycles.251 Doping MoS2 with transition metals, for instance Ni, Cu, and Fe, activates additional active sites, enhancing its electrochemical performance for SCs. The doping modifies the morphology, resulting in vertically aligned nanoarrays with an expanded surface area and enhanced exposure of active edges. Overall, doping enhances conductivity, surface area, and both catalytic (for the HER) and capacitive performance (for SCs).251 Furthermore, Kour et al. showed the consequence of Cr doping in MoS2 suggesting that due to the superior conductivity offered by Cr atoms (because it has the highest number of unpaired valence electrons among all the 3d transition metals), the hybrid SC made out of this electrode, CrMoS2//AC, shows an impressive Ed and Pd of 40.14 Wh kg−1 and 2.4 kW kg−1, respectively. It demonstrated outstanding stability, retaining 83% of its capacity after 6000 cycles.252 Bello I. T. et al. synthesised non-modulated cobalt doped molybdenum sulfide (MoS2) nanoflowers through a facile hydrothermal method. The electrode materials underwent electrochemical evaluation to determine their energy storage efficiency. The materials display a Cs of 164 F g−1 at 1 A g−1. Also, the energy and Pd are 3.67 Wh kg−1 and 3279.97 W kg−1, respectively.253 Isacfranklin et al. doped MoS2 with neodymium and gadolinium (lanthanide metals) and found that sheet-like Gd doped MoS2 nanostructures unveiled the maximum 357 F g−1 @ 10 mV s−1 Cs from CV and 231.38 F g−1 @ 1 A g−1 as revealed by GCD analysis with an extended cycling life of 81.5% over 5000 cycles.254 Singha et al. showed that a SC electrode made of low-Mn incorporated MoS2 nanoflowers exhibits a maximum Cs of 430 F g−1, an Ed of 48.9 Wh kg−1, and a Pd of 5 kW kg−1. It also exhibits excellent capacitance retention over 5000 cycles at 10 A g−1. Additionally, its performance was validated by lighting four LED bulbs in series, displaying an extended discharge time.206

Similarly, Shree Raj et al. demonstrated how Mn incorporation improves the electrochemical charge storage capacity of VSe2 sheets. For this synthesis, a one-pot hydrothermal reaction is used, and it was found that 6% Mn doped VSe2 exhibited enhanced energy storage properties, with a Cs of 250 F g−1 at 1 A g−1. An asymmetric SC using 6% Mn VSe2 and red phosphorus as electrodes achieved 21.3 Wh kg−1 Ed and 25.6 kW kg−1 Pd, with 95% capacitance retention after 5000 cycles. Mn doping in VSe2 boosts its electrochemical performance by superior active sites, enhancing ion transport, and preventing structural collapse. This results in smaller grain sizes and thinner sheets, which, in turn, increase surface area. However, Mn concentrations higher than 6% can impair performance. 6% Mn doped VSe2 demonstrates the best performance, combining these effects to provide enhanced charge storage and cycling stability.255 Two samples using magnetron sputtering, Type I (WS2 directly sputtered on nickel foam) and Type II (WS2 with a 150 nm chromium (Cr) interfacial layer between WS2 and nickel foam), were fabricated by Iqbal et al., and then electrochemical testing was conducted through CV, GCD, and EIS in three- and two-electrode setups. Fig. 16(a–d) confirms that the addition of the Cr layer significantly enhanced performance, with Type II achieving a higher specific capacity (1600 C g−1 vs. 661.79 C g−1 for Type I), better capacity retention (83.04% vs. 61.37%), and lower resistance (ESR: 0.1 Ω). By taking Type II as a positive electrode and AC as a negative electrode, a hybrid SC (WS2/Cr//AC) (Fig. 16(e)) was prepared, which delivered an Ed of 81 Wh kg−1, with a Pd of 1750 W kg−1, and maintained 87.3% capacity after 5000 cycles as shown in Fig. 16(f–h). So, introducing the Cr layer enhances conductivity and energy storage performance.256


image file: d6ta01482h-f16.tif
Fig. 16 (a) Specific capacity of WS2 and WS2/Cr through GCD. (b) Nyquist plots of WS2 and WS2/Cr. (c and d) Stability of both samples, (e) schematic of the real device, (f) specific capacity of the real device through GCD, (g) Ed and Pd of WS2/Cr//AC, and (h) capacity retention of WS2/Cr//AC. Reproduced from ref. 256 with permission from Elsevier, copyright 2024. (i) Cs of pure and Mn doped WSe2, (j) Ed and Pd of pure and Mn doped WSe2, (k) EIS, (l) CV stability of Mn doped WSe2, and (m) chronoamperometry of WSe2 pure and Mn doped WSe2. Reproduced from ref. 237 with permission from Elsevier, copyright 2024.

Furthermore, doping of Mn into WSe2 was done by Faisal et al. via a hydrothermal technique. Mn doped WSe2 has enhanced electrochemical performance due to higher Cs, improved ion intercalation, and better ionic conductivity, leading to a high Cs of 1908 F g−1 at 1 A g−1, surpassing pure WSe2 (593 F g−1) as shown in Fig. 16(i). As shown in Fig. 16(j), the electrode showed an Ed of 210 Wh kg−1, Pd of 846 W kg−1, and stability after 5000 cycles, respectively. Mn doped WSe2 has a lower charge transfer resistance (Rct = 0.1 Ω) than pure WSe2 (Rct = 0.18 Ω) (Fig. 16(k)), suggesting enhanced charge transport and ion diffusion at the electrode–electrolyte interface. Fig. 16(l) illustrates that Mn doped WSe2 retained its redox activity with negligible structural changes even after 5000 CV cycles. Fig. 16(m) presents chronoamperometry results showing that Mn doped WSe2 maintained stable performance over 45 hours, whereas pure WSe2 experienced a slight decline in stability. These results make Mn doped WSe2 a promising material for efficiency and durability.237 Samal et al. illustrated a convenient method for defect engineering by incorporating transition metals, which helps to generate active sites that are efficient. For which synthesised Metal (Mn, Zn, Cr, Fe, Ni) doped CoSe2 samples were investigated. The electrochemical performance of the asymmetric SC was first tested in a three-electrode system, and then in a two-electrode setup using different metal doped cobalt selenides as the positive electrode and titanium carbide (Mxene) as the negative electrode along with a PVA/KOH gel electrolyte with a maximum potential window of 1.5 V. The gravimetric capacitance values reported were 38.4 F g−1 for pristine, and it increased to 92.11 F g−1 for iron doped systems (a 2-fold increase), with the values being 73.38 F g−1 for manganese, 86.87 F g−1 for nickel, 49.33 F g−1 for zinc, and 42.65 F g−1 for chromium doped systems. Impedance analysis showed the best device had a low impedance of 2 Ω, indicating excellent conductivity. The Ragone plot and cycling stability verify that the Ed achieved was 28.78 Wh kg−1 at a Pd of 778.6 W kg−1 and 5000 cycles at 10 A g−1 revealed a capacitance decay to 90.56% and a coulombic efficiency of ∼97.86%. Overall, the use of MXenes as the negative electrode improved performance, expanded the potential window, and enhanced stability, while doping provided active sites and robustness to the materials.257 Sial et al. prepared cobalt doped NiVSe via a solvothermal method on a nickel foam substrate. The material exhibited an exceptional specific capacity of 2863.38 mAh g−1 at 3 A g−1, along with a high Ed and Pd of 38.73 Wh kg−1 and 1909.788 W kg−1, respectively. It exhibited remarkable stability, retaining its capacitance over 10[thin space (1/6-em)]000 cycles.206,258,259 Mahajan et al. demonstrated a superior performance SC based on biocarbon-supported MoS2 (Bio-C/MoS2) nanoparticles synthesised via a simple hydrothermal method utilising date fruits. They reported high Cs for this carbon-based nanocomposite, derived through pyrolysis of agricultural biowaste, highlighting its potential as a cost-effective energy source. The biocompatible Bio-C/MoS2 nanospheres showed a superior capacitance of 945 F g−1 at a current density of 0.5 A g−1 and demonstrated admirable cycling stability, retaining 92% of their capacitance after 10[thin space (1/6-em)]000 charge/discharge cycles. Additionally, the Bio-C/MoS2 nanospheres exhibited an outstanding Pd ranging from 3800 to 8000 W kg−1 and an Ed between 74.9 and 157 Wh kg−1. These results offer a promising pathway for the development of eco-friendly materials for high-performance energy storage technologies.260 Kishore et al. introduced an innovative method for developing high-performance SCs by using a banana peel, an eco-friendly and affordable biomass waste, as a precursor for heteroatom doped carbon (H-PC) electrodes. The electrochemical performance of MoS2@H-PC exhibits notable faradaic reactions and electrostatic adsorption, resulting in an outstanding Cs of 408 F g−1 at a current density of 1 A g−1. Furthermore, the composite demonstrates exceptional cycling stability, maintaining 90% of its capacitance after more than 10[thin space (1/6-em)]000 cycles.261 Vikraman et al. arranged an asymmetrically SeMoTe layered structure, synthesised via a one-pot reaction, demonstrating that the SeMoTe electrode achieves a symmetric capacitance of 367 F g−1 at 1 A g−1, with an Ed of 41.3 Wh kg−1 at a Pd of 4.0 kW kg−1.262

Various studies indicate that doping TMDs, such as MoS2 and WSe2, is employed not only to enhance electrochemical performance but also to enable deep modifications. Dopants alter the charge distribution by transforming inactive sites into active ones and can modify the shape and structure of the materials. However, the efficacy of a particular dopant depends on the specific material and context. For instance, Mn doping in MoS2 and WSe2 improves redox behaviour; however, at certain concentrations, elements such as Fe and Co, and rare earth metals like Gd and Nd influence conductivity and structural attributes differently, owing to their electronic properties. Doping can also induce changes in the electronic structure: the d-band shifts toward the centre, and the density of electron states near the Fermi level increases, facilitating electron mobility. Additionally, interlayer spacing enlarges, easing ion movement and promoting the formation of multiple oxidation states. During this process, nanosheets become thinner, which may lead to the formation of nanoflowers. Nevertheless, increased doping concentration can introduce instability in morphology, reduce conductivity, or alter the original phase of the material. To mitigate such issues, hybrid approaches such as interfacial doping, exemplified by surface doping with chromium and the utilisation of bio-carbon scaffolds, have been proposed, allowing similar improvements without compromising the crystal structure. Substantial doping is thus not the sole solution. These insights underscore the necessity for a sophisticated system to identify the optimal dopant for each TMD, considering factors such as band alignment, defect tolerance, and dopant-host compatibility. Future research should extend beyond experimental investigations to incorporate theoretical models, thereby developing a comprehensive understanding that cohesively bridges diverse observations.

5.2 Different composites with TMDs

5.2.1 Carbon/TMDs. Carbon-based materials predominantly store charge via the electric double layer mechanism. Carbon nanotubes (CNTs) are valued for their high conductivity and stability, and the integration of nanostructures with multi-walled CNTs (MWCNTs) provides robust electrochemical activity. The combination of TMDs with conductive carbon materials (such as CNTs or graphene) increases surface area and facilitates charge transfer, thereby improving electrochemical performance. Graphene, characterised by its high surface area and excellent conductivity, serves as an ideal medium for electron transport. Nonetheless, addressing issues related to restacking and low intrinsic conductivity through the development of TMD-carbon hybrid materials remains an effective strategy.263,264 Nabi et al. synthesised TiS2/g-C3N4 and achieved a high Cs of 546 F g−1, outperforming TiS2 due to its smaller size, extra active sites, and synergistic effects. It also retained 87% of its capacitance after 2500 cycles, showcasing admirable stability. This makes TiS2/g-C3N4 a promising material for SC electrodes with enhanced charge transfer and durability.265 Tang et al. prepared sodium-ion capacitors (SICs) using carbon-coated TiS2 nanosheets (TiS2@Cpvp) to deliver excellent performance due to their ultrathin structure and carbon modification. They achieve 448 mAh g−1, a superior retention (387 mAh g−1 @ 10 A g−1), and also 92.5% retention after 5000 cycles. Combined with an activated carbon cathode, the SIC offers an Ed of 101.7 Wh kg−1 with Pd of 200 W kg−1, demonstrating potential of 2D hybrid materials for advanced energy storage.266 Iqbal et al. developed chromium sulfide and rGO-based supercapacitor electrodes and examined their structure, morphology, and electrochemical properties. Both materials display pseudocapacitive behaviour in CV curves, with a maximum Cs of 522.84 F g−1 and 3.77 F g−1 at 5 mV s−1. GCD results reveal chromium sulfide's capacitance of 710.90 F g−1, an Ed of 24.68 Wh kg−1 at 3 mA cm−2, and a Pd of 1028.81 W kg−1 at 6 mA cm−2. An asymmetric system combining chromium sulfide and rGO exhibits pseudocapacitive traits, with a CV Cs of 24.53 F g−1 at 10 mV s−1 and a GCD capacitance of 26.41 F g−1 at 4 µA cm−2. Its Pd of 780.35 W kg−1 demonstrates its potential for supercapacitor applications.267 Hence, integrating chromium sulfide nanoparticles with a conductive rGO network boosts charge transport, provides electroactive sites, and improves stability. This leads to higher capacitance, power, and cycling durability in supercapacitors. Furthermore, Rana et al. demonstrated a straightforward hydrothermal method to synthesise reduced graphene oxide (rGO)-wrapped chromium sulfide (rGO/Cr2S3/NF). The rGO/Cr2S3/NF nanocomposite has a Cs of 2563.12 F g−1 from CV curves at 5 mV s−1, with an Ed of 87.50 Wh kg−1 and a Pd of 1607.14 W kg−1 at 2.0 mA cm−2. It remains stable over 1000 cycles thanks to the excellent electrical conductivity of rGO between the porous Ni foam collector and Cr2S3.268 The author states that the rGO/Cr2S3/NF nanocomposite's porous structure as a binder-free electrode improves electrolyte diffusion and boosts electrochemical performance. Both studies emphasise the synergistic benefits of rGO and chromium sulfide. Nevertheless, the binder-free, directly grown structure on nickel foam greatly surpasses standard composites by offering improved charge transport, lower resistance, and better electrochemical performance. A cost-effective sonochemical technique is used by Imtiaz et al. to fabricate the ZrS2@rGO nanohybrid. The electrochemical results for the three electrodes show that ZrS2@rGO nanohybrids outperform ZrS2 alone, offering Cs 1011.4 F g−1 @ 10 mV s−1 and 351.8 F g−1 @ 40 mV s−1. This excellent performance is due to the synergistic effects of sulfides and rGO, which improve ion diffusion and slow faradaic reactions. At 40 mV s−1, 81% of the charge is retained. Additionally, the GCD of the ZrS2@rGO composite shows a Cs of 1237.9 F g−1 @ 1 A g−1, well beyond the ZrS2 Cs of 813.5 F g−1. This demonstrates good durability, and 57.89% retention up to 10[thin space (1/6-em)]000 cycles at 3 A g−1. These outcomes position it as a viable material for superior-performance SC application. Furthermore, the ZrS2@rGO composite shows excellent electrochemical performance in a symmetric SC, giving Cs of 274.99 F g−1 @ 10 mV s−1 and Cs of 327.57 F g−1, and also attains a 16.86 Wh kg−1 Ed at a Pd of 303.5 W kg−1.269 Haider et al. reported a high-performance on-chip micro-supercapacitor using pyrolysed carbon/vanadium disulfide (C/VS2) microelectrodes. Fabricated through photolithography and pyrolysis, Fig. 17(a and b) shows a comparative analysis of CV and GCD curves of C/VS2-MSC and C-MSC. The layered VS2 nanosheets embedded in carbon enhance ion diffusion and charge storage, yielding a volumetric capacitance as high as 86.4 F cm−3 (Fig. 17(c)), revealing admirable cycling stability, and retaining 97.7% of their capacitance after 10[thin space (1/6-em)]000 cycles (Fig. 17(d)). The MSC also has an Ed of 15.6 mWh cm−3, with a Pd of 2.88 W cm−3 within a wide potential window (0–1.2 V) as shown in (Fig. 17(e)). This approach showcases the potential of layered TMDs for compact and efficient energy storage applications.270
image file: d6ta01482h-f17.tif
Fig. 17 (a and b) Comparative analysis of CV and GCD measurements of C/VS2-MSC and C-MSC, (c) specific volumetric capacitances of C/VS2-MSC and C-MSC at various current densities, (d) EIS of C/VS2-MSC and C-MSC, inset shows the Nyquist plot in the higher-frequency region, (e) cycling performance of C/VS2-MSC @ 0.5 V s−1, (f) Ragone curve of the C/VS2-MSC, and comparative analysis with different reported devices. Reproduced from ref. 270 with permission from [Elsevier], copyright [2020]. (g) CV curves at 50 mV s−1, (h) GCD curves at 1 A g−1, (i) EIS curves of CoS2@C and Co3S4@C, (j) schematic diagram of the asymmetrical SC, (k) CV curves of CoS2@C//RGO in different potential ranges at 50 mV s−1, (l) CV curves of the CoS2@C//RGO device, (m) GCD curves of CoS2@C//RGO, and (n) cycling performance & CE of CoS2@C//RGO. Reproduced from ref. 271 with permission from Elsevier, copyright 2023.

The study by Koudahi et al. developed hybrid electrodes combining 3D graphene-like (3DG) and VS2 to enhance Ed in electrochemical capacitors (ECs). By reducing electrode roughness, optimising VS2 content, and using a specialised electrolyte, the cell achieved a wide operating voltage of 1.8 V. It demonstrated 80% retention up to 7500 cycles with an Ed of 18 Wh kg−1 @ 430 W kg−1, and 12 Wh kg−1 at 31[thin space (1/6-em)]000 W kg−1. The hybrid EC offers stable, high-performance energy storage with rapid charge/discharge capability, making it ideal for advanced energy storage applications.205 Tobis et al. reported a hydrothermal 1-cysteine-assisted synthesis method for producing two MoS2-based composites using distinct carbon materials: multiwalled carbon nanotubes (NTs) and carbon black (Black Pearl-BP2000). MoS2 nanolayers were deposited onto these carbon materials, and the resulting composites were utilised as electrode materials in symmetric electrochemical capacitors (ECs). Their electrochemical performance was assessed and compared to that of the pristine carbon substrates. Among the two, the NTs/MoS2 composite exhibited superior electrochemical characteristics, achieving a Cs of 150 F g−1, attributed to enhanced conductivity and charge storage. In comparison, the BP2000/MoS2 composite achieved 110 F g−1 at a current density of 0.2 A g−1.272 Kapse et al. analysed 2H, 1T, and 1T′ phases of MoS2 and their carbon-based heterostructures as SC electrodes via utilising density functional theory. The underlying CNT drives a phase transition from 1T to 1T′ in MoS2, resulting in a high quantum capacitance (500 µF cm−2 at 0.6 V) because of increased DOS around the Fermi level. Nitrogen doping along with defects in CNTs further enhances capacitance over a wider potential range, making 1T′-MoS2/N doped CNT a promising electrode for next-generation SCs.273 Using a 3D rGO hydrogel network, Magdum et al. engineered a superior-performance SC electrode with VS2 and WS2 nanoparticles, synthesised via two routes (V-W-1 with ammonium metavanadate and V-W-2 with VS2), followed by hydrothermal and chemical reduction to form rGO/VW hydrogels. The rGO-VS2-WS2 hydrogel showed superior Cs (220 F g−1 at 1 A g−1), Ed (30.55 Wh kg−1), and Pd (355 W kg−1) compared to rGO and rGO-VS2. The uniform anchoring of VS2 and WS2 nanoparticles on rGO improved conductivity, ion transport, and electrochemical utilisation, enabling excellent performance and stability.274 Lin et al., using a simple chemical method, developed an rGO-MoS2-WS2 heterostructure for SCs. The composite showed a Cs of 365 F g−1 @ 1 A g−1, superior to that of single TMD-based materials, due to improved conductivity, lower resistance, and the synergistic effects of MoS2, WS2, and rGO. Operating as the positive electrode in an asymmetric SC along with rGO as the negative electrode, it achieved an Ed of 15 Wh kg−1 at a Pd of 373 W kg−1 and retained 70% capacitance over 3000 cycles, demonstrating superior performance and stability for SCs.275 Wei et al. prepared CoS2@C and Co3S4@C nanoparticles using a ZIF-67 precursor through calcination and sulphuration. The CV curves (Fig. 17(g)) and GCD curves (Fig. 17(h)) demonstrate that CoS2@C outperforms Co3S4@C, with a larger integral area, better redox reversibility, longer charge/discharge times, and higher capacitance, giving an inimitable hierarchical structure that enhances the surface area and active sites. CoS2@C gives a high Cs 1151 F g−1 @ 1 A g−1, and also retained 85.58% capacity after 10[thin space (1/6-em)]000 cycles, respectively. Fig. 17(i) shows the EIS curves of both electrodes. For an asymmetric SC with redox graphene (RGO) for the negative electrode and CoS2@C for the positive electrode in a 2 M aqueous KOH solution (Fig. 17(j)), CV tests (Fig. 17(k)) showed no significant polarisation or shapeshift in the 0–1.6 V voltage window, indicating stability. The CV profiles obtained at different scan rates (Fig. 17(l)) revealed the excellent redox activity of CoS2@C, with observable redox peaks. GCD curves (Fig. 17(m)) showed a Cs of 130.6 F g−1 at 1 A g−1 and 87.8 F g−1 at 10 A g−1. The device demonstrated an Ed of 46.52 Wh kg−1 at 800 W kg−1 and 33.28 Wh kg−1 at 6400 W kg−1, highlighting its high Pd with minimal energy loss. The CoS2@C//RGO device maintained 81.12% capacitance retention as well as 91.7% Coulombic efficiency over 10[thin space (1/6-em)]000 cycles at 10 A g−1 (Fig. 17(n)).271 Zhao et al. used a self-sacrificing template strategy to construct uniform carbon-modified NiS/NiS2 yolk–shell spheres from a Ni-based metal organic framework (Ni-MOF) precursor. The NiS/NiS2@C nanocomposites demonstrate a high specific capacity of 1082 C g−1 at 1 A g−1 and maintain excellent cycling stability with 85% capacity retention after 5000 cycles. Additionally, a hybrid supercapacitor using this nanocomposite and porous carbon can achieve a high Ed of 56.2 Wh kg−1 at 800 W kg−1 and retain 86% capacity after 10[thin space (1/6-em)]000 charge/discharge cycles, as shown in Fig. 18(a–d). The authors state that the improved electrochemical performance results from the yolk–shell structure, which provides internal voids to accommodate volume changes while preserving integrity. The carbon coating enhances conductivity, facilitates electron flow, and strengthens stability. Additionally, the combination of NiS and NiS2 phases enhances redox activity, thereby improving charge storage.276


image file: d6ta01482h-f18.tif
Fig. 18 (a) Electrochemical performance of NiS/NiS2@C and NiSx: CV curves at 20 mV s−1, (b) GCD curves at 1 A g−1, (c) capacity at various current densities, and (d) cycling stability. (e) Schematic of the NiS/NiS2@C//PAC device, (f) cycling stability and coulombic efficiency, (g) Ragone plots, and (h) LED lighting images powered by two HSCs. Reproduced from ref. 276 with permission from Springer Nature, copyright 2025.

Han et al. incorporated MoSe2 nanosheets into carbon aerogel microspheres (MoSe2 NSs/CRF) via a solvent-thermal method, enhancing both specific surface area as well as electrical conductivity. The MoSe2 NSs/CRF electrode achieved a Cs of 498 F g−1 at 1 A g−1, three times higher than that of pristine MoSe2 (136 F g−1). At 5 A g−1, it retained 278 F g−1 with 127.2% capacitance retention at 100 mV s−1 over 2500 cycles. The symmetric SC fabricated with the composite showed a capacitance of 124 F g−1, an Ed of 8.5 Wh kg−1, and a Pd of 264.8 W kg−1 at 1 A g−1.277 Furthermore, Tanwar et al. synthesised the MoSe2@AC composite using a simple hydrothermal method and methods employed for the preparation of the electrodes and the six-day-aged M6AC exhibited superior electrochemical performance. The symmetric cell fabricated with M6AC achieved a Cs of 394 F g−1 at 1 A g−1 in 6 M KOH electrolyte as shown in Fig. 19(a). It delivered an Ed of 55 Wh g−1 and a Pd of 845 W kg−1 at 1 A g−1 (Fig. 19(b)). The M6AC-based devices demonstrated 85% cycling stability and 100% coulombic efficiency following 3000 cycles, as presented in Fig. 19(c). Fig. 19(d) shows the GCD profiles recorded before and after 3000 cycles of the stability test at 2 A g−1. Fig. 19(e) shows the charge storage mechanism before and after charging. To test practical usability, the M6AC symmetric cell powered 26 red LEDs connected in parallel for approximately 32 minutes as shown in Fig. 19(f).278 Li et al. grew ultrathin MoSe2 nanosheets (MoSe2 NSs) on multi-walled carbon nanotubes (MWCNTs) via a hydrothermal method. The MoSe2/MWCNT composite exhibited a maximum Cs of 927.25 F g−1 and retained 70.08% of its initial capacity after 3000 cycles at 1 A g−1. An asymmetric SC using MoSe2/MWCNT as the anode and activated carbon (AC) as the cathode showed a Cs of 233.3 mF cm−2 at 1 mA cm−2, 101 mF cm−2 at 10 mA cm−2, and a specific energy of 72.9 µWh cm−2 at 849.3 mW cm−2, with 67.4% capacitance retention after 3000 cycles. At 10 mA cm−2, it achieved a Pd of 5980 mW cm−2.279 Gao et al. synthesised CNT@NiCo-Se using Ni-Co PBA with an etching and isolation technique, resulting in CNTs with smaller diameters and larger interlayer spacing. This structure enhanced charge transfer and –OH binding energy, leading to superior SC performance. The electrode achieved a specific capacity of 105.1 mAh g−1 at 1 A g−1, and the ASC device delivered an Ed of 46.3 Wh kg−1 at 801 W kg−1 with 80.4% capacitance retention after 10[thin space (1/6-em)]000 cycles. This approach provides a novel way to optimise CNT-based materials for energy storage.280


image file: d6ta01482h-f19.tif
Fig. 19 (a) GCD curves at several current densities, (b) Ragone plot comparing the performance, with the inset showing the variation of Cs with current density, (c) capacitance retention and coulombic efficiency over an increasing number of cycles, with the inset highlighting the GCD curves of the final 25 cycles, (d) GCD profiles recorded before and after 3000 stability cycles under constant conditions of 100 mV s−1 and 2 A g−1 respectively, (e) proposed charge storage mechanism during: (a) the charging process and; (b) the discharging process, and (f) practical demonstration of the M6AC-based SC powering multiple LEDs, including various colors and a display panel of 26 red LEDs. Reproduced from ref. 278 with permission from Elsevier, copyright 2023. (g) Plot illustrating Cs as a function of current density for all the composite materials, (h) EIS profile of all materials, (i) stability cycle of the MoTe2/rGO nanocomposite, and (j) CV cycling stability. Reproduced from ref. 146 with permission from Elsevier, copyright 2023.

Li et al. reported that 1T′-MoTe2 nanoparticles on reduced graphene oxide (1T′-MoTe2 NPs/rGO), synthesised via in situ tellurization of MoO2, exhibit excellent electrochemical performance. The 1T′-MoTe2 NPs/rGO SC achieves 98.8 F g−1 at 1 A g−1, excellent rate capacitance, and high stability, owing to enhanced conductivity and increased surface area.281 Sarwar et al. used microwave-initiated synthesis of MoTe2/graphene nanosheets to yield a high-performance energy storage material. It shows a Cs of 434 ± 37.5 F g−1 at 1 A g−1, 125% retention after 5000 cycles, and excellent stability up to 10[thin space (1/6-em)]000 cycles in 1 M Na2SO4. The symmetric device achieves an Ed of 43.2 Wh kg−1 at 3000 W kg−1.282 Furthermore, as shown in Fig. 19(g–j), Abdullah et al. showed that the MoTe2/rGO nanocomposite, synthesised via a cost-effective hydrothermal method, exhibits exceptional SC performance in a 2 M KOH electrolyte. It achieves a Cs of 1196 F g−1 (GCD) and 757.40 F g−1 (CV), a specific energy of 83.06 Wh kg−1, and a specific power of 353.5 W kg−1. With 94.23% capacitance retention after 5000 cycles, its superior performance is attributed to the synergy between MoTe2 and rGO nanosheets. This simple, scalable material is highly promising for green energy SCs.146 Zhang et al. presented a strategy using MOF-derived carbon materials to enhance Co-based nanoparticle anodes. By sequential carbonisation, oxidation, and tellurization of ZIF-67, CoTe2@N-C composites were developed, demonstrating superior Li+ storage, high-rate capacity, and excellent cycling stability. The resulting lithium-ion capacitor achieved a high Ed of 144.5 Wh kg−1 and a Pd of 10 kW kg−1, and retained 90.95% capacity after 1000 cycles. The carbon coating effectively stabilised the structure, preventing collapse and active material loss, showcasing the potential of MOF-derived materials for high-performance ESDs.283

5.2.2 Conductive polymer/TMDs. Conductive polymers such as polypyrrole (PPy), polyaniline (PANI), polythiophene (PTh), and poly(3,4-ethylenedioxythiophene) (PEDOT) exhibit high conductivity, capacitance, and flexibility, and are environmentally friendly, which renders them suitable for SC applications.284 When combined with 2D TMDs, these polymers facilitate shorter ion/electron diffusion pathways. The presence of 2D TMDs enhances the cycle life of polymer-based electrodes and improves mechanical stability. Such hybrid structures are typically fabricated through in situ polymerisation. Chen et al. prepared a similar urchin-like MoS2@PANI; electrostatic and hydrogen bond interactions between MoS2 and PANI enhance the structural integrity and surface area of the hybrids. MoS2@PANI (25 wt% MoS2) achieved a Cs pf 645 F g−1 @ 0.5 A g−1, also 89% retention after 2000 cycles. Compared to pure PANI (335 F g−1), these hybrids show improved energy storage, making them promising materials for hybrid SCs.285 Moghaddam et al. explored group 6 TMDs (MX2; M = Mo, W; X = S, Se, Te) as advanced electrode materials for SCs. MoTe2 nanosheets demonstrate good gravimetric Cs (45 F g−1 @ 0.4 A g−1), followed by WS2 (32 F g−1) & MoS2 (25 F g−1). Combining MX2 with polyaniline (PANI) significantly enhanced capacitance. The MoTe2/PANI composite exhibited the best performance with 499 F g−1, a 76% improvement over that of pure PANI (283 F g−1). This enhancement is due to the increased active surface area, making MX2/PANI hybrids promising for energy storage applications.286
5.2.3 Metal oxide (/hydroxides)/TMDs. TMD and TMO composites synergistically combine the excellent conductivity and flexibility of TMDs with the high capacitance of TMOs, leading to significantly enhanced electrochemical performance.287 Nabi et al. reported that the NiMoO4/TiS2 (NT-1) composite, prepared via hydrothermal synthesis, shows excellent SC performance with a high Cs of 1257.14 F g−1 at 1 A g−1 and 92% retention after 5000 cycles. Its mesoporous structure, large surface area, and efficient charge transfer contribute to enhanced durability, making it highly effective for advanced SC applications.288 Choudhary et al. developed h-WO3/WS2 core/shell nanowires for SCs, combining 1D nanowires and 2D TMD layers with robust interfaces. The design achieved excellent performance, including long-term stability over 30[thin space (1/6-em)]000 cycles and high capacitance.181 Gao et al. prepared CoSe2@NiCo-LDH composite electrodes with high conductivity and abundant redox sites. They achieved 6.06 F cm−2 at 6 mA cm−2 and excellent ion adsorption in KOH. Asymmetric SCs showed 0.183 mWh cm−2 Ed, 40 mW cm−2 Pd, and 97.82% capacitance retention over 5000 cycles, demonstrating high stability and performance.289
5.2.4 MXene/TMDs. In recent years, 2D transition metal carbides and nitrides (MXenes), such as Ti3C2Tx, have gained popularity as electrode materials for SCs owing to their lamellar structure, high electrical conductivity, and active sites. However, their limited Cs presents a challenge. To address this, MXenes are often decorated with pseudocapacitive materials. The synthesis of MXenes involves etching and exfoliation of MAX phases (for example, Ti3AlC2) in strong etchant solutions. Surface functionalization is employed to improve compatibility and dispersion. MXene composites are subsequently fabricated using methods such as solution mixing, hydrothermal synthesis, chemical vapor deposition (CVD), or physical vapor deposition (PVD), to enhance performance tailored to specific applications.290–292 Raj KA et al. developed VSe2/MXene hybrid materials for enhanced SC performance. The VSe2/MXene heterostructure achieved a Cs of 144 F g−1 @ 1 A g−1, along with 92.8% retention after 5000 cycles. DFT simulations revealed improved electronic properties, enhanced states near the Fermi level, and lower diffusion barriers due to charge transfer from Ti 3d orbitals of MXenes to V 3d orbitals of VSe2. An asymmetric SC with VSe2/MXene//MoS2/MWCNT electrodes delivered an Ed of 42 Wh kg−1 at 2316 W kg−1, retaining 90% C up to 5000 cycles.293 Furthermore, Xiao et al. presented a solvothermal method to produce CoSe2@Ti3C2Tx heterostructures by confining CoSe2 within MXene-Ti3C2Tx layers. The Schottky heterostructures enhance Na+ ion adsorption, fast ion transport, and cycling stability. As an anode, it achieves 600.1 mAh g−1 capacity, excellent rate performance, and long durability. The sodium-ion capacitor with CoSe2@Ti3C2Tx and activated carbon shows high energy (125 Wh kg−1) and Pd (22.5 kW kg−1) with 86.3% retention over 15[thin space (1/6-em)]300 cycles.294
5.2.5 TMDs/TMDs. Another composite synthesised by Gul et al., i.e. the ZrS:BaS:Ni9S8 thin film via a resistive heating method, shows a 21 nm crystallite size and a 2.5 eV optical band gap. It achieved a Cs of 540.7 F g−1 with excellent cycling stability, making it a promising material for high-performance SC applications.295 Wang et al. prepared MoS2/CoS2 NSTAs, and these arrays, grown directly on Ti plates, enhance electrical conductivity and simplify electrode preparation. The MoS2/CoS2 NSTAs demonstrated a Cs of 142.5 mF cm−2 @ 1 mA cm−2, almost twice that of MoS2 nanosheets and 50 times that of CoS2 arrays. They also exhibited outstanding long-term reliability, with 92.7% retention up to 1000 cycles. Synergistic effects from MoS2 and CoS2 make MoS2/CoS2 NSTAs promising electrode materials for SCs.296 Also, the MoS2@CoS2 material was prepared by Iqbal et al. through the one-step hydrothermal method, combining flower-like MoS2 and square-shaped CoS2 for enhanced SC performance. It achieves a Cs of 199 F g−1 @ 2 A g−1, Ed of 27.74 Wh kg−1, and Pd of 494.46 W kg−1. Their unique structure prevents MoS2 restacking, improves ion dynamics, and enhances conductivity. Additionally, it powered an LED for over 3 minutes, demonstrating its practical potential.297

Patel et al. presented a MoSe2@WSe2 nanohybrid heterostructure (HS) electrocatalyst, synthesised via liquid-phase exfoliation of nanocrystals. Better electrocatalytic performance led to increased availability of active edge spots following exfoliation, along with the synergistic interactions at the heterostructure interfaces between MoSe2 and WSe2. FSSC, depending upon an HS catalyst, showed admirable electrochemical performance, with a Cs of 401 F g−1 @ 1 A g−1 and 97.20% retained up to 5000 cycles, with good flexibility, and stability maintained after 1000 bend cycles.298 MoSe18Se24 and Mg3Mo18Se24 (MoSe/MMSe) composite electrodes were synthesised by Nagaraju et al. on Ni foam (NF) via hydrothermal synthesis. The MoSe/MMSe composite showed superior areal capacity (1154.4 µAh cm−2) and specific capacity (250.9 mAh g−1) compared to individual electrodes. The electrochemical properties of MoSe and MgSe were also analysed. An OAC/NF (OAC onion-derived activated carbon) negative electrode was used, showing high capacitance. The MoSe/MMSe/NF (positive)//OAC/NF (negative) hybrid SC delivered an Ed of 28.5 Wh kg−1 and Pd of 2353.8 W kg−1, with 74.3% retained after 45[thin space (1/6-em)]000 cycles.299

Shamami et al. introduced CoTe@CoFeTe double-shelled nanocubes as advanced SC materials, synthesised through anion exchange, annealing, and tellurization processes. The unique porous structure and incorporation of tellurium enhance conductivity, ion diffusion, and electron transport. These nanocubes achieve an extraordinary specific capacity of 1312 C g−1 at 1 A g−1 and retain 92.35% capacity after 10[thin space (1/6-em)]000 cycles. A HSC (AC//CoTe@CoFeTe) exhibits high Ed (64.66 Wh kg−1) and excellent cycling stability (88.25% retained up to 10[thin space (1/6-em)]000 cycling).300 Liu et al. synthesised NiSe/NiTe2 nanocomposites via a microwave method on nickel foam, demonstrating exceptional performance for SCs. It achieved a Cs of 1782.7 F g−1 @ 1 A g−1, surpassing individual NiSe and NiTe2 electrodes. The composite shows excellent cycling stability, and retained 81.5% up to 30[thin space (1/6-em)]000 cycles. Additionally, the NiSe/NiTe2//AC ASC delivered an Ed of 23.26 Wh kg−1 and retained 84.8% after 20[thin space (1/6-em)]000 cycles. The data emphasise the viability of the NiSe/NiTe2 composite for high-performance and durable SCs.301

5.2.6 Mixed composites. Mixed composites, involving the integration of TMDs with other materials such as metal oxides, carbon-based materials (like graphene and CNTs), or conductive polymers, aim to harness the optimal properties of each constituent. This approach is particularly pertinent to SC applications, as it markedly improves overall capacitance, electrical conductivity, and cycle stability. For example, Vinodhini et al. designed a mixed electrode by combining TiO2 and CNTs (i.e. MoS2/TiO2/CNTs) that outperformed and achieved 1252.57 mAh g−1 at 20 mV s−1 in 1 M KOH, with significantly lower impedance (Rct 1.7 Ω cm2, Rf 2.1 Ω cm2). It demonstrated excellent cycling stability, retaining 98.83% capacitance after 10[thin space (1/6-em)]000 cycles @ 1 A g−1. The Ed was 757.80 Wh kg−1, and the Pd was 4546.80 W kg−1.302 Siddu et al. prepared a 3D hybrid structure of VSe2, Ti3C2Tx MXene, and CNTs to overcome challenges like oxidation and sheet restacking in SCs. The VSe2/e-MXene/CNT_30 electrode exhibits excellent electrochemical performance, with high capacitance and improved rate capability. It shows the largest CV area, indicating superior activity, delivers a higher Cs of 151 F g−1 @ 1 mA, and maintains 98.1% capacitance retention and nearly 100% CE up to 5000 cycles. An ASC with this hybrid achieved 35.91 Wh kg−1 Ed, 1280 W kg−1 Pd, and retained 24.17 Wh kg−1 at 6350 W kg−1, demonstrating strong rate capability. The device maintained ∼99% capacitance retention and nearly 100% coulombic efficiency after 5000 cycles, confirming its stability and efficiency.303 Gao et al. developed CNTs with NiSe2/CoSe2 nanoparticles (CNT@NiCo-Se) using an etching and isolation technique, achieving smaller tube diameters and larger interlayer spacing. These enhancements improve charge transfer and binding energy, resulting in a 375% higher specific capacity (105.1 mAh g−1 at 1 A g−1). The CNT@NiCo-Se//AC SC delivers 46.3 Wh kg−1 Ed and 8000 W kg−1 Pd, and retains 80.4% capacitance after 10[thin space (1/6-em)]000 cycles, showcasing a new method for optimising PBA-derived materials.280

In the meantime, Su et al. synthesised a Ni2P/NiSe2/MoSe2 (NNM) hybrid to address MoSe2 restacking issues in SCs. Embedding Ni2P and NiSe2 nanoparticles within MoSe2 nanosheets increased interlayer spacing, enhanced active sites, and improved electron transfer. The NNM electrode achieved a Cs 607.5 F g−1 @ 0.5 A g−1, and also retention of 87.9% up to 1000 cycles. An NNM//AC hybrid SC delivered 23.5 Wh kg−1 @ 400 W kg−1 with exceptional durability, retaining 116.6% up to 45[thin space (1/6-em)]000 cycles, showcasing feasibility for advanced energy storage.304 Farshadnia et al. studied a NiTe2-Co2Te2@rGO nanocomposite successfully using a two-step hydrothermal method, and the electrochemical tests demonstrate excellent performance, with a specific capacity of 223.6 mAh g−1 at 1 A g−1 and 89.3% stability after 3000 cycles. The hybrid SC, with NiTe2-Co2Te2@rGO as the cathode, and activated carbon as the anode, gave an Ed of 51 Wh kg−1 and Pd of 800 W kg−1. This electrode also powers LEDs for 20 minutes, validating its performance for future next-generation storage platforms in devices and vehicles.11

5.2.7 Others. Qadeer et al. produced a Bi2WO6/TiS2 (BW/T@40%) composite by the hydrothermal process, achieving a high Cs of 1153.3 F g−1 because of increased surface area, pore size, and also synergistic effects. It also demonstrated excellent stability, retaining 92% capacitance after 4500 cycles.305 The overall conclusion of the recent study indicates that the integration of TMDs with various materials through compositing serves not only to enhance their inherently low electrical conductivity and limited surface area but also as a strategic approach to regulate charge transfer, redox reactions (electron exchange), and voltage stability. Notably, when TMDs such as VSe2 are combined with MXenes, orbital interactions occur between them, resulting in increased electron flow and equilibrium in redox processes. Structural design is equally crucial; for instance, vertically aligned, porous hollow materials facilitate ion mobility, prevent material degradation, and provide abundant active sites. An additional consideration pertains to aqueous systems, where the voltage window is typically constrained due to the rapid onset of the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). However, this limitation can be mitigated by controlling the edge sites of the material, selecting appropriate electrolytes, and meticulously designing the interface. The synthesis method employed, whether solvothermal or metal–organic framework (MOF)-based techniques, not only determines the morphology but also influences the phase formation, defect density, and overall stability of the material. In conclusion, the creation of composites is a deliberate and strategic process rather than an arbitrary mixture. This process involves a comprehensive balance of TMD quantity, structural features, and the electrolyte environment to produce an energy storage system that is efficient, evidencing a purposeful electrochemical design rather than a random material combination. The integration of electronic behaviour, structural design, and electrochemical performance establishes a new paradigm for future TMD composites. Moving forward, research should extend beyond merely discovering new materials to focusing on how existing materials can be engineered into intelligent, integrated, and functional systems, wherein each component supports the others. A comparison table indication the supercapacitor performance of all type of TMD-based electrodes have been compared in Table 2.
Table 2 TMD-based electrodes' performance for SCsa
Electrode materials Device technique Cs @ current density/scan rate Cycles Capacitance retention Ed Pd Ref.
a PEI@ACWPANI HCFMs: flexible silver-anchored polyetherimide@CNP/WS2/polyaniline coaxial fibrous membranes.
Pristine TMDs
1T-TiS2 Symmetric 10[thin space (1/6-em)]000 96.1% 2000 W kg−1 213
TiS2 Symmetric 68.62 mF cm−2 @ 0.375 mA cm−2 5000 4% loss 34.35 mWh cm−2 675.1 mW cm−2 306
TiSe2 Asymmetric 60.6 F g−1 @ 0.2 A g−1 38.1[thin space (1/6-em)]Wh kg−1 176.4 W kg−1 307
TaS2 Three electrodes 151.11 F cm−2 @ 0.3 A g−1 5000 81% 308
TaSe2 Three electrodes 102.6 F cm−2 @ 0.3 A g−1 5000 98% 308
WS2 Three electrodes 116.1 F cm−2 @ 0.3 A g−1 5000 98% 308
WSe2 Three electrodes 152.3 F cm−2 @ 0.3 A g−1 5000 98% 308
ZrS2 Three electrodes 141.8 F cm−2 @ 0.3 A g−1 5000 92% 308
ZrSe2 Three electrodes 127.3 F cm−2 @ 0.3 A g−1 5000 92% 308
VS2 Asymmetric 155 F g−1 @ 1 A g−1 5000 99% 42 Wh kg−1 700 W kg−1 309
2D-pristine VS4 Three electrodes 215 F g−1 @ 5 mV s−1 2000 82% 310
Hierarchical NbS2 Three electrodes 221.4 F g−1 @ 1 A g−1 10[thin space (1/6-em)]000 78.9% 311
Ultrathin NbS2 Three electrodes 175.6 F g−1 @ 1 A g−1 311
Mesoporous MoS2 Three electrodes 403 F g−1 @ 1 mV s−1 2000 80% 188
1T-2H WS2 Hybrid 240.7 F g−1 @ 1 A g−1 95.7% 65.5 Wh kg−1 784 W kg−1 312
WSe2 nanoflakes thin-film Symmetric 88 mF cm−2 5000 75.36% 27.5 µWh−1 cm−2 3000 µW cm−2 313
CoSe2 Asymmetric 90.5 F g−1 @ 10 mA cm−2 32.2 Wh kg−1 1914.7 W kg−1 314
[thin space (1/6-em)]
Modified TMDs
TiS2/MoS2 Three electrodes 709 F g−1 @ 10 mV s−1 4000 91% 315
rGO/TiS2/MoO3 Three electrodes 1100 mAh g−1 @ 1 A g−1 8000 98.83% 882 Wh kg−1 5773 W kg−1 316
3D patterned MoS2/TiS2 Two electrodes 448.16 mF cm−2 @ 90 mg cm−2 100[thin space (1/6-em)]000 99.1% 3.89 µWh cm−2 250 µW cm−2 317
PPT/ZrO2/ZrS2 Three electrodes 1326 F g−1 @ 5 A g−1 10[thin space (1/6-em)]000 96% 166 Wh kg−1 664 W kg−1 318
VS2/MWCNT Symmetric 182 F g−1 @ 2 mV s−1 5000 93.2% 42 Wh kg−1 2.8 kW kg−1 319
NiCo2S4@VS2 Asymmetric 299.5 C g−1 @ 1 A g−1 4000 31.2 Wh kg−1 775 W kg−1 320
2D VS2-black phosphorus-50 Symmetric 203.25 mF cm−2 @ 1 mA cm−2 10[thin space (1/6-em)]000 87% 28.22 µWh cm−2 596.09 mW cm−2 321
VSe2/SWCNTs/rGO Symmetric 450 F g−1 @ 1 A g−1 5000 91% 131.4 Wh kg−1 27.49 kW kg−1 322
S-VSe2/CNT Asymmetric 96 mF cm−2 @ 4 mA cm−2 5000 87.2% 36.3 µWh cm−2 3.2 mW cm−2 323
N doped V4C3/C//VO2/VSe2 Asymmetric 50.6 F g−1 @ 0.25 A g−1 5000 78% 21.4 Wh kg−1 4.5 kW kg−1 324
VSe2/MWCNT Symmetric 233.33 F g−1 @ 2 A g−1 5000 87% 46.66 Wh kg−1 4.8 kW kg−1 325
VSe2/RGO Coin cell 680 F g−1 @ 1 A g−1 10[thin space (1/6-em)]000 81% 212 Wh kg−1 3.3 kW kg−1 326
VSe2@N-doping carbon Asymmetric 313.8 F g−1 @ 1 A g−1 2000 90% 85.41 Wh kg−1 701.99 W kg−1 327
3D VSe2/e-MXene/CNT Asymmetric 101 F g−1 @ 1.6 A g−1 5000 99% 35.91 Wh kg−1 1280 W kg−1 303
3D VTe2/MXene/CNT Symmetric 34.2 mF cm−2 @ 0.25 mA cm−2 10[thin space (1/6-em)]000 78% 6.84 µWh cm−2 304.7 µW cm−2 328
NiCu-MOF/NbS2 Asymmetric 194 C g−1 @ 1 A g−1 20[thin space (1/6-em)]000 97% 83 Wh kg−1 970 W kg−1 329
NbSe2@PPy Asymmetric 401 mF cm−2 @ 0.5 mA cm−2 10[thin space (1/6-em)]000 98.2% 11.9 mWh cm−3 29.6 mW cm−3 330
NbTe2@rGO Symmetric 498 F g−1 @ 1 A g−1 22 Wh kg−1 285 W kg−1 331
PEDOT:PSS/WS2 Three electrodes 118 mF cm−2 @ 0.5 mA cm−2 5000 95.7% 14.75 µWh cm−2 249.31 µW cm−2 332
Ni@Cu/WS2 Asymmetric 265.42 F g−1 @ 0.5 A g−1 4500 98.1% 43.9 Wh kg−1 425 W kg−1 333
1T-WS2/Gr Three electrodes 2964 mF cm−2 @ 4 mA cm−2 1000 86% 334
WS2/carbon composite (WS2/Z8-800) Asymmetric 88 F g−1 @ 1 A g−1 3000 78.3% 25 Wh kg−1 801 W kg−1 335
W2C/WS2 Symmetric 328 F g−1 @ 1 A g−1 45.5 Wh kg−1 0.5 kW kg−1 336
WS2-WO3/rGO Three electrodes 728 F g−1 @ 1.25 A g−1 3000 91% 337
WS2/FeCoTeZr Asymmetric 150 F g−1 @ 1 A g−1 3000 97.9% 55 Wh kg−1 4250 W kg−1 338
MXene/WS2 Three electrodes 373 F g−1 @ 0.4 A g−1 1000 91.2% 339
h-BN-WS2 Asymmetric 142.1 C g−1 @ 1 A g−1 10[thin space (1/6-em)]000 81.6% 33.37 Wh kg−1 844.9 W kg−1 340
PEI@ACWPANI HCFMs Symmetric 1381.2 mF cm−2 @ 0.5 mA cm−2 10[thin space (1/6-em)]000 76.3% 122.78 µWh cm−2 0.24 mW cm−2 341
MnSe/WSe2 Three electrodes 1326 F g−1 @ 1 A g−1 5000 92% 37 Wh kg−1 225 W kg−1 342
MXene/WSe2 Symmetric 246 F g−1 @ 2 A g−1 5000 97% 12.3 Wh kg−1 600 W kg−1 343
2H-WSe2@rGO Asymmetric 145 F g−1 @ 2 A g−1 3000 82% 51.5 Wh kg−1 2133.3 W kg−1 344
1T-WSe2/graphene Symmetric 323.3 F g−1 @ 0.5 A g−1 5000 86.7% 48.2 Wh kg−1 250 W kg−1 345
WSe2@rGO Three electrodes 1337 F g−1 @ 1 A g−1 5000 53 Wh kg−1 261 W kg−1 346
MoSe2@WSe2 Symmetric 401 F g−1 @ 1 A g−1 5000 97.2% 14.44 Wh kg−1 397 W kg−1 298
WSe2/MoS2 Three electrodes 1169.53 F g−1 @ 1 A g−1 5000 82.80% 161.8 Wh kg−1 950.2 W kg−1 347
WSe2@ReSnSe2 Symmetric 175 F g−1 @ 1 A g−1 5000 84.6% 3.88 Wh kg−1 411 W kg−1 348
WSe2/NiCo-MOF nanocomposites Asymmetric 270.5 C g−1 @ 1.5 A g−1 5000 86.7% 38.8 Wh kg−1 1791.4 W kg−1 349
CoS2/MWCNT Three electrodes 1486 F g−1 @ 1 A g−1 10[thin space (1/6-em)]000 80% 350


6. Conclusion and future perspectives

6.1 Conclusion

Energy is essential for human needs and development. The search for renewable energy sources has intensified, with SCs gaining attention as a promising solution for the depletion of fossil fuels. SCs offer high Pd, fast charge/discharge rates, and longer lifespans than batteries and fuel cells, making them suitable for electric vehicles, hybrid systems, and emergency power applications. An SC cell has two electrodes and an electrolyte; the electrode is vital for storing charge and determining performance. Ideal electrode features include high surface area, conductivity, porosity, low cost, and stability. In the last few decades, TMDs have been promising electrode materials for SC applications. Hence, in this review article, we present an in-depth analysis of the structure and properties of TMDs, along with an exploration of various synthesis routes for TMD-based materials. Thereafter, the supercapacitive behaviour of TMDs in energy storage applications has also been thoroughly discussed, with emphasis on the critical roles of defects, morphology, surface area, doping, pore size, and compositional variations in optimising their performance. TMDs exhibit attractive features like a broad exposed area, adjustable band gap, and enhanced physical robustness, thus allowing them to serve as ideal candidates for layered geometries. Nevertheless, their weak electron transport efficiency restricts their effectiveness in energy conservation, prompting the development of several strategies to enhance their conductivity. The key strategies highlighted in this review to tackle this challenge are mixing, wrapping, or depositing TMDs with a range of organic/inorganic capacitive materials. However, some challenges remain that need to be addressed to meet the current energy demand.

6.2 Future perspectives

Although optimized 2D TMD-based SCs show great potential, acknowledging current problems and challenges is important. Addressing these issues should guide future research. We emphasize the following points, as illustrated in Fig. 20 and discussed in detail below:
image file: d6ta01482h-f20.tif
Fig. 20 Exploring challenges and emerging trends in TMDs for SCs.
6.2.1 Surface functionalization. Surface functionalization addresses the inherent drawbacks of TMD-based SC electrodes, including restacking, slow ion diffusion, and limited conductivity. Adding heteroatoms (N, O, snf S), functional groups, and conducting polymers to their surface increases the electroactive sites and enhances charge transfer. Also, controlled functionalisation methods, such as atomic-level doping, defect engineering, and hybridisation with carbon frameworks, can enhance structural stability and minimise volume changes during long-term cycling. Furthermore, incorporating redox-active groups and metal oxides onto the TMD surface provides additional pseudocapacitance without affecting conductivity. In addition, the heterojunction design that combines different 2D TMD materials, such as MoS2, WS2, and TiS2, generates built-in electric fields. This enhances charge storage and transfer capabilities and helps prevent electrode collapse. With surface doping, ion and electron migration improve, and the kinetics of the electrochemical reaction are optimised. By making protective films, oxidation resistance and chemical stability improve. The biggest challenge is ensuring that the functionalization is scalable, uniform, and durable, enabling practical device fabrication. If these hurdles can be overcome, then TMD-based electrodes for SCs offer high Ed, fast charge and discharge, and, along with excellent durability, can provide a strong foundation for next-generation SCs.
6.2.2 Morphological engineering and nanoscale confinement. Future research on TMD-based electrodes for SCs should strongly focus on advanced morphological engineering combined with nanoscale confinement strategies to unlock their full electrochemical potential, enabling high Ed, Pd, and long-term cycling stability. Designing advanced nanoscale structures, including nanosheets, nanotubes, nanorods, and hierarchical networks with controlled porosity, can greatly increase surface area and reduce ion diffusion paths, thereby improving charge storage and transfer kinetics. Additionally, accurately controlling ultrathin or few-layer structures can leverage quantum confinement effects, boosting electrical conductivity and redox activity. Also, in the future, modulating interlayer spacing and using conductive nanomaterials and molecular spacers can optimise ion accessibility and mitigate volumetric expansion during repeated cycles. Apart from these, multi-scale morphological design, which combines nanoscale engineering with meso and macroscale architectures, will be crucial for simultaneously achieving high Ed and Pd. The synergistic optimisation of porosity, layer alignment, and surface functionalisation will unlock superior cycling stability and long-term durability.
6.2.3 AI and machine learning assisted material calculations. In the future, the design and development of 2D TMDs are anticipated to progress more rapidly through the integration of Artificial Intelligence (AI) and Machine Learning (ML). The existing experimental and computational databases can aid AI–ML algorithms in predicting and optimising synthesis parameters, processing conditions, and defect engineering. AI–ML models can help identify enhanced specific design factors for TMD electrode materials, such as mass ratios, charge–discharge modes, potential ranges, and fabrication methodologies. The integration of AI–ML has not only facilitated material synthesis but has also conserved resources and time. Furthermore, AI–ML is highly valuable for analysing electrochemical behaviour, enabling the prediction of SC performance.
6.2.4 DFT and multiscale simulations. In the near future, DFT and multiscale simulations will become the cornerstone tools for the rational design of TMD-based SC electrodes. With the help of DFT, the atomic-level electronic structure, orbital hybridisation, defect states, edge vs. basal-plane activity, and ion-intercalation energetics can be predicted with high fidelity. This allows the redox site activation, charge redistribution, local strain effects and conductivity pathways to be engineered on the atomic scale. In particular, the effects of vacancy defects, heteroatom doping, and functional group modifications on electrochemical potential, Fermi-level tuning, and adsorption energies are quantified accurately, which influence the electrode's performance. Multiscale simulations (molecular dynamics, reactive force fields, coarse-grained modelling, kinetic Monte Carlo, and continuum electrochemical simulations) can couple atomic-scale phenomena with mesoscale morphology and device-level electrochemical behaviour, enabling the prediction of ion transport kinetics, electrolyte penetration, and electrode porosity optimisation.
6.2.5 Advanced in situ characterisation. In future studies, the advanced in situ characterisation techniques have facilitated a comprehensive understanding of reaction mechanisms, material behaviours, and hidden phenomena under realistic conditions.351 Techniques such as in situ Raman spectroscopy, infrared (IR) spectroscopy, in situ transmission electron microscopy (TEM), in situ scanning electron microscopy (SEM), in situ X-ray diffraction (XRD), in situ X-ray absorption spectroscopy (XAS), and in situ X-photoelectron spectroscopy (XPS) enable real-time observation of structural, compositional, and electronic changes during reactions.352 These methods are instrumental in directly tracking material transformations in both equilibrium and non-equilibrium states.353 They contribute to improving interfacial phenomena, enhancing battery stability, and supporting practical applications. Such tools are vital for understanding the intrinsic properties of 2D TMDs and their dynamic alterations, which are crucial for the development of energy-related technologies.
6.2.6 Techno-economic optimization of TMD-based SCs. TMDs provide high Cs and Ed but face commercialization challenges due to low conductivity, restacking, and high synthesis costs. From a techno-economic perspective, the synthesis routes discussed in this review are largely compatible with scalable processes such as hydrothermal, solution-phase, and gas-phase methods, although further optimization is required to reduce processing complexity and energy consumption. Economically, the cost of raw materials, use of costly precursors, and multi-step fabrication procedures remain key cost drivers that may hinder large-scale commercialization. Therefore, future efforts should focus on low-cost precursors, simplified synthesis strategies, and improved material utilization to enhance cost-effectiveness. Overall, while the reviewed materials demonstrate promising performance at the laboratory scale, targeted techno-economic optimization will be essential to translate these advances into commercially viable energy storage devices, thereby strengthening their application prospects.

Conflicts of interest

There are no conflicts to declare.

Data availability

This manuscript is a review article and does not report any new primary data. All information discussed in this review has been obtained from previously published literature, which has been appropriately cited within the manuscript.

Acknowledgements

Meenakshi gratefully acknowledges the Ministry of Education, India, for financial assistance. P. W. M. gratefully acknowledges funding from the German Federal Ministry of Education and Research under the funding code 03EW0015A/B.

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