CNT-based electrodes for flexible aqueous zinc-ion batteries: progress and opportunities

Abstract

The advancement of wearable electronics requires flexible power sources with durable electrodes to withstand dynamic operational conditions. Among diverse materials for electrodes, carbon nanotubes (CNTs) emerge as an ideal material due to their unique structure, high aspect ratio, and tunable surface chemistry, enabling versatile architectures from fibers to films and sponges. This review systematically examines CNT-based flexible electrodes for zinc-ion batteries (ZIBs), highlighting recent breakthroughs in multifunctional wearable applications achieved through optimized CNT architectures. Key strategies in component engineering and structural design are discussed to enhance mechanical–electrochemical performance. Furthermore, critical correlations between material properties, electrode design, and practical applications are established. By providing methodological insights and technological roadmaps, this comprehensive analysis advances the development of CNT-based flexible electrodes for next-generation electrochemical energy storage systems.

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Tao Sun

Tao Sun is a professor in the School of Chemistry & Chemical Engineering at Jiangsu University. He obtained his PhD from Changchun Institute of Applied Chemistry, Chinese Academy of Sciences in 2019. Then, he worked as a postdoctoral research fellow at Nanyang Technological University (NTU), Singapore. His research focuses on the design and development of novel materials for battery applications, with a particular emphasis on elucidating the reaction mechanisms of high-performance organic electrode materials for rechargeable batteries.

Qichun Zhang

Prof. Qichun Zhang holds the position of Full Professor at City University of Hong Kong (CityU, Hong Kong, China). Prior to joining CityU, he served as a tenured Associate Professor at Nanyang Technological University of Singapore (NTU, Singapore). Currently, he has been recognized as one of Clarivate Analytics' top 1% highly cited researchers in cross-field from 2018 to 2024. His research focuses on carbon-rich conjugated materials and their potential applications. To date, he has published over 600 papers with citations of more than 47 000 and an H-index of 119.

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1. Introduction

The scarcity of global fossil energy resources and associated environmental challenges have intensified research efforts toward developing novel clean energy technologies.^1–3 The advancement of efficient electrochemical energy storage devices is critical for addressing the intermittent nature of renewable energy sources.^4–6 Recent safety concerns surrounding lithium-ion batteries, including explosion risks, have spurred the search for cost-effective, environmentally benign, and stable alternatives.^7–10 Aqueous batteries offer significant advantages, such as low cost, abundant reserves, high safety, environmental friendliness, and high energy density.^11–14 They show promising application prospects in large-scale energy storage areas, as well as in flexible electronics.^15–18 The rapid advancement of flexible wearable electronics has created growing demands for power sources with enhanced safety and flexibility.^19–22 Owing to their intrinsic advantages including cost-effectiveness, operational safety, and eco-friendliness, aqueous zinc-ion batteries (ZIBs) are well-suited for such applications. Utilizing non-flammable and non-volatile aqueous electrolytes, ZIBs eliminate the risks of thermal runaway, fire, and leakage, making them ideal for close-contact wearable devices.^23,24 They avoid toxic organic solvents and reliance on rare metals, reducing both environmental impact and manufacturing complexity.^25,26 Importantly, aqueous ZIBs can be manufactured using scalable techniques to produce flexible or fiber-shaped batteries. Their lightweight and thin profiles further enable seamless integration into smart fabrics or flexible substrates, supporting the next generation of wearable electronics.²⁷

Current research on aqueous ZIBs focuses on three key areas: electrolyte engineering, zinc anode protection, and the development of novel electrode materials.^28–31 Optimizing electrode architectures and fabrication techniques, alongside material innovations, can enhance energy density without compromising performance. Thus, precise microstructural design and controllable synthesis of electrodes have become pivotal research topics. Conventional electrodes typically consist of active materials, conductive additives, and binders coated onto conductive current collectors to form porous structures.^32,33 However, weak interfacial adhesion between electrode materials and current collectors can lead to material delamination during long-term cycling, reducing electrode lifespan.^34–37 Self-supporting electrodes can overcome these limitations by eliminating powder-based materials.^38–41 Among potential self-supporting matrices, carbon nanotubes (CNTs) are particularly attractive due to their unique one-dimensional (1D) structure, high aspect ratio, and tunable surface chemistry, enabling assembly into diverse architectures, including 1D fibers, two-dimensional (2D) films, and three-dimensional (3D) sponges or aerogels.^42–45

The rise of wearable electronics imposes stringent requirements on flexible power sources, particularly for electrodes. Wearable devices demand current collectors with exceptional bendability and stretchability. During operation, mechanical stresses (e.g., bending, stretching, and twisting) and environmental factors (e.g., moisture, pressure, and chemical exposure) can induce microcracks and active material detachment, severely degrading battery performance.^46–49 Addressing these challenges requires advanced flexible conductive substrates. CNTs, with their high conductivity, mechanical flexibility, and chemical stability, are ideal for flexible electrodes (Fig. 1), maintaining structural integrity and efficient charge/mass transport even under harsh conditions.^50–53 Developing CNT-based flexible substrates and elucidating their influence on electrode performance will advance their macroscopic utilization in next-generation electrochemical devices.^54–57

Fig. 1 Overview of various applications of CNTs for flexible aqueous ZIBs. Reprinted with permission from ref. 119, Copyright 2025, Reprinted with permission from ref. 122, Copyright 2025, Wiley. Elsevier; with permission from ref. 129 Copyright 2019, American Chemical Society; with permission from ref. 130, Copyright 2022, American Chemical Society; with permission from ref. 131, Copyright 2024, American Chemical Society; with permission from ref. 140, Copyright 2024, Wiley; with permission from ref. 142, Copyright 2024, Wiley; with permission from ref. 153, Copyright 2025, Elsevier.

This review provides a comprehensive and systematic summary of recent advancements in CNT-based flexible electrodes for ZIBs. First, we elucidate the energy storage mechanisms and flexibility principles of flexible zinc-ion batteries (FZIBs). Next, we systematically examine their component composition, structural configurations, and design strategies. Subsequently, we review recent advancements and practical applications of FZIBs in wearable electronics, focusing on multifunctional scenarios. Finally, we present forward-looking perspectives on this field, offering directional guidance for their practical applications of CNT-based flexible electrodes in wearable electronics.

2. The preparation of CNT-based electrodes

As one of the core members of carbon-based nanomaterials, CNTs have been drawing significant attention since their discovery. CNTs possess unique structures and properties such as a high aspect ratio, exceptional tensile strength, and unusual electronic transport characteristics.^58–61 In recent years, with the continuous improvement in preparation technology of CNTs, production costs have significantly decreased. CNTs synthesized through different methods exhibit distinct performance characteristics (Fig. 2a).⁶² Generally, CNTs can be categorized into powder-form and array-form configurations. Powder-form CNTs typically demonstrate random orientation, morphological heterogeneity, and entanglement issues, often accompanied by amorphous carbon by-products that complicate purification processes, thereby limiting practical applications. In contrast, array-form CNTs maintain controlled growth orientation with uniform alignment and consistent length distribution, effectively addressing agglomeration issues while minimizing surface contaminant formation through high-density packing.^63,64 Generally, the preparation methods for CNT-based flexible electrodes can be divided into the chemical vapor deposition (CVD) method, utilizing self-supporting substrates, and the powder self-assembly method:^65,66

Fig. 2 The preparation methods for CNT-based electrodes. (a) Applications of CNTs with diverse morphologies in electrode materials. Reprinted with permission from ref. 62, Copyright 2020, Oxford University Press. (b) The synthesis of CNTs and fabrication of films and fibers. Reprinted with permission from ref. 67, Copyright 2018, Elsevier; ref. 68, Copyright 2025, Wiley.

(i) The CVD method enables the preparation of CNT arrays that can be processed into self-supporting materials like films and yarns through mechanical treatments such as pulling and twisting (Fig. 2b).^67,68 These materials maintain the intrinsic high conductivity of CNTs while demonstrating exceptional mechanical properties, including high tensile strength and Young's modulus.

(ii) Conventional metal foils (e.g., copper or titanium) function effectively as growth substrates, offering direct contact with active materials and efficient charge transfer pathways. To reduce mass contribution from substrates, carbon-based alternatives such as carbon paper, carbon fiber cloth, and 3D graphene networks have been adopted as both current collectors and CNT growth platforms. CVD-grown CNTs on these substrates typically exhibit strong interfacial adhesion, which minimizes contact resistance and enhances charge and mass transport.^69–72

(iii) Under the influence of strong π–π interactions, CNT suspensions can form CNT films through methods like vacuum filtration, printing, or spraying.^73,74 The hydrophilicity of the film can be adjusted by regulating the surface functional groups of raw CNTs.^75–77 While this approach offers advantages in cost-effectiveness, operational simplicity, and scalability for mass production, it requires uniform CNT dispersion typically achieved through acid treatment and ultrasonication.^78,79 These processing steps may compromise CNT quality, potentially affecting their conductive and mechanical properties.

Printed electronics based on conductive ink demonstrate advantages including flexibility, large-area production, lightweight design, cost-effectiveness, and environmental friendliness, showing promising market prospects.^80–83 Among them, conductive inks using CNTs as fillers exhibit unique advantages in fabricating flexible electronic devices.^84,85 However, higher aspect ratios of CNTs lead to greater dispersion challenges, as they tend to entangle and agglomerate, increasing processing difficulty and compromising composite performance.^86–89 Achieving uniform dispersion of CNTs in a medium is crucial for preparing CNT-based conductive inks and forms the foundation for flexible electronics manufacturing.

Given the dispersion challenges of CNT powders, increasing research focuses on one-dimensional CNT fibers (CNTFs) (Fig. 2b). As macroscopic assemblies of axially aligned individual CNTs, CNTFs inherit properties like high conductivity, lightweight, and flexibility, making them particularly suitable for smart wearables, intelligent textiles, and flexible energy storage devices.^90–92 Current preparation methods include wet spinning (dispersing CNT powder in solvent followed by coagulation), array spinning (directly drawing fibers from vertically aligned CNTs arrays), and floating catalyst chemical vapor deposition (FCCVD) spinning.^93–96 Nowadays, CNTFs demonstrate exceptional mechanical and electrical properties. They can also be twisted into more wearable CNT yarns using traditional spinning techniques. In recent years, a growing interest has been witnessed in macroscopic CNT assemblies as self-supporting conductive substrates for cathodes in flexible battery systems. Key research directions include enhancing inter-tube connections to reduce contact resistance, enhancing specific surface area, and improving mechanical stability and flexibility for practical applications.

3. Configurations and design principles of FZIBs

Current strategies for achieving battery flexibility primarily focus on replacing rigid electrodes and liquid electrolytes with flexible electrodes and solid-state electrolytes.^97–100 Flexible structural designs are categorized into two types: stacked configurations and fiber-shaped architecture. Stacked configurations have been widely investigated due to their structural simplicity, ease of fabrication, and excellent performance. These systems typically involve flexible cathode and anode layers separated by planar solid-state or semi-solid electrolyte interlayers, forming a layer-by-layer stacked FZIBs.¹⁰¹ The planar design enables series or parallel assembly configurations, making it suitable for powering various bendable devices. However, current stacked FZIBs assemblies predominantly rely on weak physical adhesion between components, which fails to meet operational requirements under prolonged or complex mechanical deformations. Achieving stable battery performance during repeated mechanical stress necessitates robust interfacial contact stability and mechanical robustness. Consequently, developing advanced methodologies to construct durable stacked architecture remains a pivotal challenge in advancing FZIB technology. Additionally, stacked batteries often rely on external encapsulation (e.g., polymer films) to prevent electrolyte leakage. However, repeated mechanical deformation can cause packaging cracks or tears, leading to electrolyte leakage and device failure.

Compared to stacked FZIBs, 1D fiber-shaped configurations not only exhibit superior mechanical properties but can also be woven into energy storage textiles via conventional textile techniques, offering advantages such as lightweight design, enhanced flexibility, breathability, and comfort, thereby enabling broader potential applications.^102–104 Fiber-shaped configurations utilize coaxial or twisted geometries, where electrodes are helically wrapped or core–shell structured. This design enables uniform stress distribution during bending due to its radial symmetry and intrinsic flexibility of fibrous components.^105,106 Current fiber-shaped zinc battery designs predominantly adopt coaxial architectures, which are further classified into two types: (i) inner-anode structures with zinc anodes at the innermost layer, sequentially coated with electrolyte, cathode, and encapsulation materials; and (ii) inner-cathode structures with reversed component arrangements.

Fiber-shaped zinc batteries endure more complex deformation modes (e.g., stretching, bending, and twisting) than stacked configurations, necessitating flexible design strategies for cathodes, zinc anodes, and electrolytes to ensure both mechanical durability and electrochemical performance. The ideal architecture for 1D fiber-shaped aqueous zinc batteries involves compact structures with high aspect ratios and curvature radii, requiring flexible cathodes with high specific capacity, mechanical resilience, flexibility, and structural stability.¹⁰⁷ However, current fabrication methods for flexible cathodes – primarily spraying/coating-casting techniques – involve depositing active materials onto conductive flexible substrates. These methods inevitably require binders (e.g., PVDF and PTFE) and conductive additives to prepare coating slurries. Unfortunately, such additives often exhibit instability during charge/discharge cycles, leading to intermittent contact between active materials and conductive substrates, thereby degrading interfacial stability.^108–111 Additionally, the coating and binding processes significantly impair battery performance under twisting, stretching, or bending stresses.

Consequently, increasing attention has been directed toward constructing self-supporting flexible cathodes through in situ growth of active materials on substrates.^112–114 Direct growth of active materials on conductive substrates enhances interfacial stability and facilitates efficient reaction kinetics. Although significant progress has been made in structural design and component optimization of fiber-shaped zinc batteries, achieving 1D configurations that simultaneously deliver exceptional mechanical stability, flexibility, electrochemical durability, and high energy density remains a critical challenge requiring further research.

4. The application of CNTs in composite cathode design

Electrodes play a pivotal role in determining battery performance. Conventional battery electrodes often rely on rigid substrates (e.g., metal current collectors), which are prone to cracking or structural degradation under repeated bending, stretching, or compression. CNTs inherently possess excellent mechanical flexibility and robustness, enabling them to form self-supporting, ultra-thin, and highly deformable electrode architectures. Their 1D tubular structure and high tensile strength allow the electrode to withstand significant mechanical stress without compromising structural integrity, even after thousands of cycles. Traditional electrodes suffer from weak interfacial adhesion between active materials and rigid current collectors, leading to delamination and performance loss during deformation. CNT-based self-supporting electrodes eliminate the need for separate current collectors by acting as both the conductive scaffold and the active material support. The high electronic conductivity of CNTs ensures efficient electron transport, while their porous network facilitates uniform dispersion of active materials, minimizing interfacial resistance and enhancing electrochemical stability. CNT-based electrodes address this through their porous 3D network structure, which acts as a buffer to accommodate volume changes. Meanwhile, the intrinsic flexibility of CNTs allows them to adapt mechanical deformations, preventing crack propagation and maintaining electrode stability even under dynamic conditions. Additionally, flexible electrodes often face limitations in active material loading due to the use of bulky or rigid substrates. CNTs, with their high specific surface area and lightweight nature, enable high-density integration of active materials. This enhances energy density while maintaining flexibility, as the CNT network provides a compact and scalable platform for material deposition.¹¹⁵

Extensive studies have focused on enhancing the structural stability of freestanding matrices, optimizing interfacial contacts among components, and improving overall electrode capacity. Zheng and coworkers utilize a CNT sheet sheath to wrap the electrode, inducing turbulence effects that accelerate ion mixing between the electrolyte and electrode interface, further tuning charge storage kinetics.¹¹⁶ Synergistic material-structural design enables high-performance flexible batteries by optimizing charge storage kinetics and ion transport. Co-intercalation of Na⁺ and polyaniline expands NH₄V₄O₁₀ interplanar spacing to 13.5 Å, facilitating rapid ion diffusion and contributing to exceptional capacity (346.9 mAh g⁻¹) and energy density (255.2 Wh kg⁻¹).¹¹⁷ The core-sheath yarn architecture combines flexibility and compactness, enabling seamless textile integration for wearable energy systems (Fig. 3a). CNT integration addresses sluggish Zn²⁺ kinetics while improving structural stability, establishing a scalable pathway for self-powering energy solutions in wearable electronics.

Fig. 3 Flexible batteries through synergistic material–structural optimization and wearable integration. (a) Schematic of the fabrication process for core-sheath CNT/NaNVO-PANI cathode yarn. Reprinted with permission from ref. 117, Copyright 2024, Elsevier. (b) Illustration of the photovoltaic-integrated yarn-electrode architecture. Reprinted with permission from ref. 118, Copyright 2025, Elsevier.

Manganese-based materials (e.g., MnO₂) are promising cathodes for aqueous ZIBs but suffer from low conductivity and Mn dissolution. To address these problems, a novel cone-spinning strategy was developed by Zheng and coworkers to fabricate carbon nanotube/manganese dioxide (CNT/MnO₂) composite yarns.¹¹⁸ Unique yarn architecture enhances interfacial electrochemical characteristics, mitigating MnO₂ dissolution and conductivity issues. Compared to Fermat-spun yarns, cone-spun CNT/MnO₂ composite yarns exhibit superior electrochemical performance. By integrating these yarn-shaped batteries with polycrystalline solar cells, the study also demonstrates the feasibility of creating self-powered systems suitable for portable electronics. The integrated wearable self-powered system (combining ZIBs with solar cells) achieves efficient solar energy harvesting-storage synergy. This work redefines the structure-design principles of flexible energy storage devices and paves the way for practical applications in wearable electronics (Fig. 3b).

Serving as 3D conductive scaffolds, CNT-based current collectors create continuous electron transport networks throughout the electrode architecture. Their inherent hierarchical porosity not only ensures homogeneous distribution of active species and suppresses particle aggregation, but also accommodates mechanical strain induced by cyclic volume expansion/contraction. Pendashteh and colleagues introduced composite electrodes made from vanadium oxide embedded with a conducting network of CNTs¹¹⁹ (Fig. 4a). The use of CNT fabrics as built-in percolated current collectors not only alleviates the adverse effects of heavier metallic current collectors but also significantly enhances the specific energy of batteries, especially when compared to titanium (Ti) and stainless steel (SS) foils. As a result, the binder-free CNT-embedded composite cathodes achieved 96 wt% active material content by eliminating metallic foil/binders, enabling ultra-lightweight electrode architecture.

Fig. 4 Structural innovation in flexible ZIBs. (a) Synthetic route of conformally coated CNTFs. Reprinted with permission from ref. 119, Copyright 2025, Elsevier. (b) Illustration of an air-rechargeable aqueous ZIB and its incorporation in wearable systems. Reprinted with permission from ref. 120, Copyright 2021, Royal Society of Chemistry. (c) Schematic of the N-VO₂@NC@CNTF fabrication process with corresponding GCD and CV curves. Reprinted with permission from ref. 122, Copyright 2025, Wiley. (d) Schematic of ZIMB fabrication via 3D printing and photos of the resulting printed structure. Reprinted with permission from ref. 123, Copyright 2025, Elsevier.

Innovating the application scenarios of flexible zinc-based batteries and developing their functional applications under specific conditions are also key directions for advancing FZIB technology. Peng and coworkers developed high-capacity fiber-shaped ZIBs that can self-recharge using ambient oxygen, enabling direct conversion between chemical and electrical energy.¹²⁰ This air-enabled energy harvesting relies on freestanding fiber with nano-structured V₆O₁₃/aligned CNT heterostructures. Such hierarchical architecture ensures an efficient reaction area, enabling spontaneous oxygen redox reactions in discharged fibers for capacity restoration (Fig. 4b). The air-recharging process is chemically reversible and operates synergistically with constant–current charge/discharge. This makes the solution particularly suitable for remote areas or resource-limited applications where conventional charging facilities are unavailable.

Developing flexible electrodes/devices with innovative architectures to enable higher active material loading while mitigating stress concentration is key for future progress. In this regard, a self-standing, binder-free cathode material was developed by Mahmoud and colleagues by combining polydopamine (PDA)-coated V₂O₅ particles with CNTs.¹²¹ The PDA coating inhibits V₂O₅ dissolution and side reactions, significantly boosting stability in aqueous ZIBs. Partial reduction of V⁵⁺ to V⁴⁺ induced by PDA enhances redox activity and accelerates ion diffusion kinetics. The active components are anchored within the highly conductive network constructed by CNTs, endowing the composite material with both high specific capacity and superior rate capability. The binder-free design simplifies electrode fabrication processes and reduces production costs, enabling scalable energy storage solutions.

Li and colleagues proposed a simple yet effective approach for constructing fiber-shaped devices through the design of N-doped VO₂/N-doped carbon (N-VO₂@NC) heterojunction electrodes. The synthesis involves electrochemical deposition of polypyrrole (PPy) on CNTFs, followed by solvothermal growth of vanadium oxide precursors and thermal treatment.¹²² The resulting architecture features a nitrogen-doped 3D conductive carbon scaffold derived from PPy carbonization, which enhances ion transport and active material loading (Fig. 4c). The in situ nitrogen doping of VO₂ reduces its bandgap, significantly improving electronic conductivity. The N-VO₂@NC@CNTF electrodes demonstrate exceptional electrochemical performance in both all-solid-state fiber-shaped supercapacitors and aqueous ZIBs, addressing critical challenges of low specific capacitance, sluggish ion diffusion, and poor conductivity in wearable energy storage.

3D printing enables direct fabrication of complex functional structures through layer-by-layer deposition of nanomaterials, with its core advantage lying in micro-scale precision control. This technology has emerged as a novel approach for fabricating flexible electrode microstructures, offering unique benefits including high design freedom, customizability, and multi-material integration potential that may overcome existing limitations. By strategically controlling material distribution through optimized microstructure design, 3D printing allows performance enhancement at the microscopic level, thereby improving energy conversion efficiency. Jin and coworkers fabricated innovative zinc-ion microbatteries (ZIMBs) via direct ink writing using 3D-printable inks.¹²³ Vat photopolymerization (VP)-based 3D printing is developed for microbattery packaging, enabling efficient integration of ZIMBs into wearable monoliths (Fig. 4d). This method allows for precise control over microelectrode design and 3D structure prototyping. The cathode is calcium vanadate nanoribbons, while the anode is Cu-modified Zn nanosheets, which suppress dendrite growth and reduce polarization during Zn plating/stripping. The 3D-printed ZIMBs deliver an outstanding device capacity of 8.9 mAh cm⁻² (surpassing previous ZIMBs and even Li-ion microbatteries). By optimizing printing parameters, capacity is further enhanced to 14.9 mAh cm⁻². This work provides a universal approach for developing free-standing fiber electrodes, advancing the practical implementation of next-generation wearable energy storage systems.

Capitalizing on the complementary merits of battery-type energy storage and capacitor-type power delivery, zinc-ion hybrid capacitors (ZIHCs) represent a frontier technology in advanced energy storage systems. Their unique working mechanism endows simultaneous achievement of supercapacitor-level power density and battery-comparable energy density. Li and coworkers reported a novel zinc-ion hybrid micro-supercapacitor configuration based on a carboxylated CNT cathode and electrodeposited Zn anode.¹²⁴ The study employs advanced yet simple and effective techniques such as electrodeposition and electrophoretic methods to fabricate electrodes without the use of binders. Vertically aligned Zn nanoflakes were grown on graphite paper to construct a 3D interconnected Zn anode, ensuring stable stripping/deposition behavior. The device maintains its performance with minimal degradation even when bent at angles ranging from 0 to 120 degrees, demonstrating its potential for use in wearable energy storage electronics.

The stability of FZIBs, particularly their electrochemical and mechanical stability, is a critical determinant of cycle life. Electrochemical stability depends on electrode materials, nanostructures, and electrode–electrolyte interfaces.^125–128 Effective solutions include constructing interfacial modification layers with excellent ionic and electronic conductivity on the electrode surface, as well as carefully designing highly stable micro-nano structures for the electrodes. Wei and coworkers fabricated coaxial fiber-structured flexible aqueous batteries (CARZIBs).¹²⁹ This design achieves a remarkable specific capacity and energy density, surpassing reported flexible aqueous batteries. This coaxial-structured battery configuration possesses unique structural advantages, with zinc nanosheet arrays (Zn-NSAs) grown on CNTFs serving as the inner core electrode, and ZnHCF/CNT composites on aligned carbon nanotube sheets (ACNTSs) acting as the outer electrode (Fig. 5a). The CARZIB exhibits exceptional flexibility, retaining 93.2% of its capacity after 3000 bending cycles at 90°, making it ideal for wearable applications. This design enables efficient charge transport and low contact resistance, significantly improving electrochemical performance and mechanical stability.

Fig. 5 Fabrication process and application demonstrations of fiber-structured flexible aqueous batteries. (a) Schematic of the CARZIB assembly process and its corresponding electrochemical behavior under different bending conditions. Reprinted with permission from ref. 129, Copyright 2019, American Chemical Society. (b) Fabrication process of the fiber-shaped battery and its resistance variation during hand movement. Reprinted with permission from ref. 130, Copyright 2022, American Chemical Society.

Integrated multifunctional flexible smart electronic devices are emerging as a pivotal trend in the electronics industry. These innovations facilitate ubiquitous intelligent applications in daily life, demonstrating vast application prospects in human health monitoring, activity tracking, and beyond. In this regard, a multifunctional battery was developed by integrating a fiber-shaped ZIB with a strain sensor. By coating the battery with carbon nanotube/polydimethylsiloxane (CNT/PDMS) nanocomposites, it can function as a strain sensor with good sensitivity for monitoring body motions like wrist, finger, elbow, and knee movements¹³⁰ (Fig. 5b). The integration of these functionalities in a flexible form factor makes it highly suitable for wearable devices, where both compactness and functionality are critical. The battery successfully powers an electronic watch and five LEDs, demonstrating its practical usability in real-world applications. After bending 2000 times, the battery retains 90% of its original capacity, indicating excellent mechanical flexibility and durability. This multifunctional battery represents a significant step forward in wearable electronics by combining energy storage and sensing capabilities into a single device.

Effectively integrating display functionalities into fiber battery textiles while maintaining stable power supply, remains a major challenge in the field of smart electronic textiles. Addressing this, Zhi et al. developed high-performance, waterproof, stretchable, and tailorable yarn-based ZIBs (Fig. 6a).¹³¹ This double-helix structured yarn electrode, combined with a polyacrylamide (PAM) electrolyte, enables the battery to achieve exceptional specific capacity and long-term cycling stability. PAM-based hydrogels exhibit excellent flexibility and ductility, capable of stretching up to 300% of their original length without breaking. Under various deformation conditions (bending, knotting, twisting), the yarn battery retains over 95% of its capacity, recovering to its original shape with over 95.8% initial capacity remaining. Interestingly, even when cut, short yarn-structured ZIBs can still function properly and be woven into textiles to power LED and electroluminescent panels (Fig. 6b). By overcoming traditional electrolyte weaknesses through optimized polymer–metal salt compatibility, this work establishes a scalable manufacturing protocol for next-generation smart textiles, fundamentally advancing the field of deformable energy devices for IoT and wearable applications (Fig. 6c–f).

Fig. 6 Double-helix yarn electrodes and PAM electrolyte-driven stretchable ZIBs for stable power supply in display-integrated smart textiles. (a) Schematic of the fabrication and encapsulation process for yarn-structured ZIBs. (b) Schematic diagram of a flexible battery display unit system. (c) SEM images of the pristine CNT fibers, (d) and (e) SEM images of the CNT@Zn yarn, and (f) TEM image of the MnO₂ nanorods. Reprinted with permission from ref. 131, Copyright 2024, American Chemical Society.

5. The application of CNTs in the structure design of zinc anodes

The practical application of zinc metal batteries faces significant challenges due to the incompatibility between zinc metal and aqueous electrolytes, including zinc dendrite growth and various side reactions (e.g., passivation, corrosion, and hydrogen evolution reaction, HER).^132–135 Notably, the persistent formation of zinc dendrites not only reduces the Coulombic efficiency (CE) during zinc deposition/stripping but also diminishes zinc electrode utilization and drastically shortens battery lifespan. To enhance the durability and reversibility of zinc metal, researchers have developed multiple strategies, such as anode structural optimization, interface regulation (e.g., modifying the electrochemical double layer or introducing artificial protective layers), and electrolyte engineering (e.g., incorporating organic co-solvents, polymer electrolytes, or functional additives).^136–139

Zhang et al. presents a novel strategy for dendrite-free zinc anodes in aqueous ZIBs through a cationic surfactant-functionalized 3D carbon nanotube (C-CNT) host.¹⁴⁰ The CNT framework serves as a highly conductive network, providing abundant nucleation sites for Zn²⁺ deposition (Fig. 7a). The entangled CTA⁺ cations form a conformal shielding layer around zinc protrusions, effectively suppressing dendrite growth. Density functional theory (DFT) calculations further confirm the efficacy of this electrostatic repulsion shielding mechanism. Cationic surfactants selectively adsorb onto active sites of the zinc anode, forming a self-assembled electrostatic shielding layer. This layer physically separates the Zn surface from free water molecules in the electrolyte, significantly reducing hydrogen evolution reactions (HERs) and other parasitic side reactions. The cations in the surfactant preferentially occupy high-curvature regions (e.g., tips of dendritic growth or surface irregularities), creating localized electrostatic repulsion that homogenizes Zn²⁺ flux distribution. Additionally, the electrostatic shielding layer acts as a dynamic barrier that redirects Zn²⁺ ion flux away from high-current–density zones (e.g., dendritic tips) toward smooth, low-curvature regions of the anode. The cationic surfactant layer is self-repairing and adaptive to mechanical/chemical changes during cycling. As dendrites form or the anode surface deforms, the surfactant cations reorient to maintain electrostatic shielding at newly exposed active sites. Meanwhile, CNTs provide a high-surface-area scaffold for surfactant anchoring, enhancing the coverage and stability of the electrostatic shielding layer. The C-CNT host outperforms conventional approaches (e.g., heterogeneous interphases or electrolyte additives) by integrating nucleation control and dynamic growth regulation into a single scalable platform. This work advances practical ZIBs by addressing both fundamental and engineering challenges in Zn anode design. Lu et al. introduces a flexible 3D CNT network as a conductive scaffold for zinc deposition¹⁴¹ (Fig. 7b). This structure effectively lowers the zinc nucleation overpotential, homogenizes electric field distribution, and promotes reversible Zn plating/stripping, thereby inhibiting dendrite formation and byproduct generation. The 3D porous CNT network enables uniform Zn nanosheet growth with minimal aggregation. The Zn/CNT symmetric cell achieves a low voltage hysteresis of 27 mV at 2 mA cm⁻² and 28% depth of discharge, cycling stably for 200 hours.

Fig. 7 Dendrite-free zinc anodes enabled by 3D CNT hosts: cationic shielding and conductive scaffolds for high-performance aqueous ZIBs. (a) Schematic illustration of a self-adaptive hierarchical host achieved by cationic functionalization of CNT films. Reprinted with permission from ref. 140, Copyright 2024, Wiley. (b) Schematic illustrations of Zn deposition on CC and CNT electrodes and voltage profiles of symmetric cells. Reprinted with permission from ref. 141, Copyright 2019, Wiley.

Coating technology can significantly enhance the stability of zinc anodes. By carefully selecting and designing coating materials, the corrosion resistance of zinc anodes can be improved, thereby greatly extending the battery's lifespan. Liu and coworkers present a novel PVDF/CNTs-PT@Zn protective layer for zinc anodes, fabricated via a facile phase transfer method to address dendrite growth and side reactions in aqueous ZIBs¹⁴² (Fig. 8a). The composite structure combines a chemically stable PVDF matrix (utilizing –F groups to repel H₂O and guide Zn²⁺ deposition) with a conductive CNT network, forming a 3D porous architecture that ensures uniform ion flux and electric field distribution. The synergistic design enables suppressed Zn dendrite formation and hydrogen evolution, along with reduced interfacial current density. Additionally, it provides tolerance to volume changes during cycling, ensuring structural stability. Symmetrical cells with PVDF/CNTs-PT@Zn exhibit exceptional stability, while full cells paired with V₂O₅ cathodes demonstrate practical viability. Notably, the phase transfer method is scalable and equipment-free, coating directly onto untreated Zn foil. In situ CT imaging confirms homogeneous Zn deposition, highlighting the layer's dynamic protection mechanism. This work provides an industrially feasible strategy to enhance ZIB performance through interfacial engineering.

Fig. 8 3D CNT-based strategies for scalable and stable aqueous ZIBs. (a) PVDF/CNTs-PT@Zn preparation process, and corresponding linear polarization curves and nucleation overpotential. Reprinted with permission from ref. 142, Copyright 2024, Wiley. (b) Schematic of the fabrication process for the self-supporting zinc anode. Reprinted with permission from ref. 143, Copyright 2021, Royal Society of Chemistry. (c) Schematic of Zn²⁺ deposition and corresponding confocal laser microscopy images of Zn²⁺ deposition on different substrates. Reprinted with permission from ref. 149, Copyright 2024, Elsevier.

Zhou and coworkers presented a flexible, free-standing Zn anode fabricated via a simple spin-coating technique for high-performance ZIBs.¹⁴³ The anode was prepared by integrating commercial Zn paste with CNTs and poly(vinylidene fluoride)-co-hexafluoropropylene (PVDF-HFP), forming a robust 3D interconnected network (Fig. 8b). CNTs enhance electrical conductivity, while PVDF-HFP improves mechanical strength and flexibility via its 3D interconnected network and hexafluoropropylene groups. The anode achieves exceptional flexibility (e.g., foldable without damage) and high electrical conductivity due to CNT percolation, leading to ZIBs with high capacity, rate capability, and mechanical flexibility. Compared to conventional zinc foil, this design significantly improves electrochemical performance while maintaining safety and cost-effectiveness. The free-standing design not only overcomes limitations of conventional Zn foil but also simplifies device architecture, making it ideal for flexible electronics. This work highlights the potential of binder/CNT-engineered Zn anodes for next-generation portable and wearable energy storage.

Carbon materials (e.g., nitrogen-doped carbon nanotubes) act as protective layers, minimizing direct contact between the Zn anode and electrolytes to inhibit side reactions. The high conductivity of carbon accelerates charge transfer, reduces interfacial impedance, and improves the reversibility of zinc deposition/stripping. Introducing nitrogen atoms into the carbon matrix modulates interactions, increasing nucleation sites and blocking dendrite propagation, thereby reducing short-circuit risks. Additionally, the N-doped carbon matrix will homogenize electric field distribution and provide nucleation sites, guiding uniform Zn²⁺ deposition to suppress dendrite growth. Ou and coworkers highlighted the value and significance of nitrogen-doped carbon nanotubes (N-CNTs) in enhancing the stability of zinc anodes.¹⁴⁴ Nitrogen doping introduces surface defects and vacancies on carbon nanotubes, providing more nucleation sites for uniform zinc deposition. The high dielectric constant of nitrogen-doped layers shields external electric fields, promoting uniform Zn²⁺ distribution and inhibiting dendrite growth. The N-CNT@Zn anode enables zinc–manganese batteries to operate stably at 40 °C, expanding their usability in high-temperature environments. The application of nitrogen-doped carbon nanotubes as a protective layer on zinc anodes offers a promising approach to achieve dendrite-free growth. This not only suppresses dendritic growth but also reduces side reactions that can lead to battery short circuits.

Under repeated bending conditions of FZIBs, interfacial slippage between the electrode and electrolyte can lead to loss of contact at the interface and trigger non-uniform zinc deposition at both bent and flat regions. Consequently, interfacial slippage may cause electric field accumulation at edges and peak positions due to edge effects and geometric deformation, thereby facilitating the formation of excess zinc dendrites. To address the zinc dendrite issue in FZIBs, several promising strategies have been proposed. Quasi-solid-state electrolytes with excellent mechanical properties can act as protective sheaths to prevent zinc dendrite penetration, though their superior mechanical performance may compromise ionic conductivity. Designing quasi-solid-state electrolytes with high adhesive strength can help avoid interfacial slippage, ensuring robust interfacial contact.^145–148 Additionally, incorporating additives into the electrolyte that can in situ form protective layers on the zinc anode surface may also serve as an effective solution to the dendrite problem. By leveraging these strategies, the formation of zinc dendrites in FZIBs can be suppressed, making the batteries more reliable and efficient. He and colleagues fabricated a flexible membrane (CNT/PAN/Ag) with uniformly interwoven pores using a one-step phase inversion method (Fig. 8c).¹⁴⁹ This membrane features a complex woven pore structure that effectively disperses Zn²⁺ ions, reduces nucleation site current density, and prevents aggregated deposition of Zn²⁺. Additionally, the Janus membrane designed with different electrolyte affinities on each side further optimizes battery performance. The upper surface's high wettability facilitates rapid Zn²⁺ flux transfer into the membrane, while the lower surface's low wettability helps isolate the zinc anode from the electrolyte, minimizing side reactions. The Ag active sites within the membrane enhance Zn²⁺ dispersion and induce Zn²⁺ deposition within the membrane, balancing and reducing current density at the deposition interface.

In wearable electronics, quasi-solid-state electrolytes (QSSEs) address critical challenges such as electrolyte leakage, electrode corrosion, and mechanical instability. By combining robust mechanical resilience with electrochemical stability, QSSEs enable ZIBs to endure repeated deformations while maintaining stable voltage profiles and high energy density. This makes them a viable solution for next-generation flexible and stretchable energy storage systems. Firstly, QSSEs exhibit superior mechanical strength and flexibility compared to conventional liquid electrolytes. This is achieved through a tough, flexible matrix, which prevents electrolyte leakage and maintains structural integrity under repeated mechanical deformation (e.g., bending, stretching, or compression). For wearable devices, this ensures stable operation even during dynamic movements. Secondly, QSSEs act as a physical barrier to inhibit zinc dendrite penetration. The rigid yet flexible matrix restricts ion flux heterogeneity at the zinc anode, reducing localized current densities that drive dendrite formation. This mitigates risks of internal short circuits and electrode degradation, thereby extending cycle life and enhancing safety in flexible or fiber-shaped ZIBs. Thirdly, the non-leakage nature of QSSEs eliminates risks associated with liquid electrolyte spills, making them ideal for wearable and portable devices. Additionally, their self-healing or adaptive interfaces maintain consistent electrochemical contact between electrodes and electrolytes, even after repeated mechanical stress. This ensures reliable performance under extreme conditions. Finally, QSSEs can be integrated into fiber-shaped or compressible architecture without compromising performance. Their processability aligns with emerging techniques like wet-spinning or electrospinning, enabling mass production of flexible ZIBs for energy textiles or smart fabrics.

Constructing multifunctional quasi-solid-state electrolytes is a prerequisite for achieving FZIBs with diverse capabilities, such as compressibility, stretchability, freeze resistance, self-healing, thermal protection, and luminescence. For QSSEs with compression or stretching capabilities, the designed polymer matrix must exhibit high elasticity and superior mechanical strength. Niu and coworkers present compressible ZIBs based on a micro-nano structured polyaniline-single-walled carbon nanotube-sponge (PANI-SWCNT-sponge) cathode, enabling stable electrochemical performance under extreme mechanical deformation (up to 60% strain)¹⁵⁰ (Fig. 9a). The quasi-solid-state battery design incorporates a PANI/SWCNT-coated sponge cathode, a PVA/Zn(CF₃SO₃)₂ gel electrolyte, and a Zn foil anode. The SWCNT network's high fault tolerance ensures continuous current pathways even under compression. The quasi-solid-state design eliminates liquid electrolyte leakage issues, making it compatible with highly compressible electronics. The 3D porous sponge scaffold, reinforced by a conductive SWCNT network, ensures structural integrity, fault tolerance, and maintained conductivity even under repeated compression. This advancement opens possibilities for elastic energy storage devices that can be integrated with flexible or compressible electronics, overcoming limitations associated with conventional electrode materials and liquid–electrolyte configurations. It highlights the potential for developing compression-tolerant energy-storage solutions compatible with next-generation electronic devices.

Fig. 9 Quasi-solid electrolytes and deformable anodes enabling robust wearable energy storage. (a) Schematic of electron/ion transport in compressible ZIBs. Reprinted with permission from ref. 150. Copyright 2019, Royal Society of Chemistry. (b) Schematic of the wet-spinning fabrication process for fiber-shaped flexible ZIBs and their application in wearable energy storage textiles. Reprinted with permission from ref. 153, Copyright 2025, Elsevier.

In the early stages, zinc metal rods or wires were commonly used as anodes in fiber-shaped zinc batteries due to their inherent flexibility. However, their limited bending performance made it difficult to meet the increasingly demanding conditions for the application of fiber-type zinc batteries. Therefore, flexible design of zinc anodes has attracted growing attention and research interest from scholars. By introducing flexible substrates to construct 1D composite flexible anodes, the original flexibility of the substrate can be preserved, enabling the anode to withstand complex stress-deformation conditions in fiber-shaped zinc batteries.^27,151,152 For instance, a flexible yet robust fibrous metal anode was fabricated by first uniformly coating copper onto cotton yarn via electroless plating, followed by zinc deposition. When assembled into a fiber-shaped zinc battery, this anode maintained stable and excellent performance even under severe bending and twisting. Another effective solution for improving flexibility through macroscopic design of the anode structure involves forming spring-like zinc anodes by winding zinc wires or rods. This macroscopic structural design not only enhances the tensile properties of the zinc anode under stress but also increases the contact area between the electrolyte and the anode, thereby promoting electrochemical reactions. Guo and coworkers fabricated all-fiber ZIBs via wet-spinning technology.¹⁵³ MnO₂ nanowire-based cathodes and Zn powder-based anodes are processed into fiber electrodes using wet-spinning (Fig. 9b). The slurry formulation mimics conventional battery electrode pastes, enabling industrial-scale production. A binary percolation network of 1D carbon nanofibers (CNFs) and CNTs ensures uniform dispersion of active materials (MnO₂/Zn) and optimal conductive pathways. Fiber electrodes are wrapped in hydrophobic cotton cloth and encapsulated with heat-shrink tubing to form 1D flexible batteries. The cotton cloth acts as both a separator and electrolyte reservoir, simplifying the battery architecture. Furthermore, the fiber batteries are integrated with flexible sensors, demonstrating stable operation in toxic gas environments and during dynamic human motion.

6. Conclusions

In summary, this review provides a comprehensive and systematic summary on the design strategies, recent research progress, and future development directions of CNT-based flexible electrodes for FZIBs. With the rapid development of wearable electronics, extensive research efforts have focused on developing FZIBs with high electrochemical performance and excellent mechanical flexibility to meet the demands of wearable devices across diverse application scenarios. Nevertheless, current research on CNT-based composite electrodes faces challenges as summarized below.

(i) Poor structural stability of the matrix: for CNT-based energy storage composites, the dispersion and structural stability of the CNT matrix are critical factors determining active material loading and electrochemical performance. Achieving in situ structural modification during CNT preparation without compromising its quality remains key to optimizing self-supporting CNT-based composite electrodes.

(ii) Weak interfacial contact between matrix and active components: the interfacial stability and impedance between components critically determine rate performance. In CNT-based composite electrodes, the electrochemical response differences between CNTs and active components are significant. For example, transition metal oxides undergo phase transitions during charge/discharge cycles accompanied by ion intercalation and chemical state changes – processes characterized by slow reaction rates and large volume variations. In contrast, CNT matrices exhibit rapid electrochemical responses and structural stability. This mismatch leads to high interfacial impedance and fracture risks that accumulate over long-term cycling, particularly under high-rate conditions where interfacial failure causes active material detachment and performance degradation. Although carbon coating designs can enhance interfacial bonding strength, they introduce additional impedance. Therefore, rational interfacial engineering to improve rate capability and cycling stability is crucial for boosting electrochemical performance.

(iii) Limited overall performance of composite electrodes: the complex electrode reaction process involves multi-scale influencing factors. The intrinsic capacity of active components and the effective mass of composite electrodes collectively determine device performance. Interface engineering can enhance component compatibility, while multi-approach synergistic modifications may unlock the full potential of composites. The success of CNT-based FZIBs depends on the combination of softness and strength through multi-scale design. Currently, CNT-based FZIBs urgently require the development of cross-dimensional integration strategies to address the challenges of functional integration. Multi-scale engineering bridges this gap by combining atomic-scale material properties, mesoscale interface dynamics, and macroscale structural responses into a unified platform. For instance, machine learning can integrate material genomic data (e.g., electronic properties of CNTs) with device-level functional parameters (e.g., energy/power density, cycle life) to build a “performance requirements–structural features” reverse design model. This allows researchers to predict optimal material compositions and structural designs for specific applications, accelerating the development of practical devices. Next-generation energy textiles require not only material and structural innovations but also organic integration of multi-dimensional manufacturing techniques. This highlights the need for scalable processes like wet-spinning technology, which embeds CNT networks and active materials into all-fiber electrodes. Multi-scale engineering ensures that these processes align with the designed microstructures and interfacial properties. By coupling computational models (e.g., phase-field simulations) with experimental validation, researchers can optimize manufacturing parameters to maintain the designed multi-scale features during large-scale production.

(iv) Recent advances in FZIBs have focused on integrating multifunctional features beyond basic flexibility and energy supply to address the diverse demands of wearable electronics. For compressibility in flexible devices, 3D porous structures (e.g., sponges, foams, aerogels, and hydrogels) can be utilized as core components to uniformly distribute compressive stress. These structures serve as internal free spaces that accommodate mechanical deformation while maintaining stable electrode–electrolyte contact, ensuring reliable electrochemical performance under repeated compression. This design makes FZIBs particularly suitable for wearable applications that undergo dynamic pressure changes. Stretchability represents another crucial development direction for flexible devices. This can be achieved by designing reversible elongation mechanisms through novel architectures with large shape deformation, combined with depositing active materials on stretchable current collectors. Such approaches enable the battery to withstand tensile stress without structural failure – a critical requirement for applications demanding skin-like flexibility or stretchable garment integration.

(v) Multifunctional integration represents a crucial future trend in flexible device development. For instance, the reversible oxidation/reduction of electrochromic active materials during charge/discharge cycles alters their optical properties, creating an intelligent visual indicator of energy status. State-of-charge-dependent color variations provide immediate feedback, offering significant user experience advantages over conventional transparent batteries. Special application scenarios impose more demanding requirements on flexible batteries. Taking extreme cold environments as an example, this necessitates optimization of electrolyte formulations and material selection (e.g., employing low-viscosity, freeze-resistant electrolytes) to maintain ionic conductivity at subzero temperatures. Such cold-resistant battery designs significantly expand application possibilities to harsh climates – including outdoor winter sports equipment and military operations in frost-prone regions – while guaranteeing reliable power output even under extreme low-temperature conditions. Self-healing capability represents a fascinating and promising research direction for batteries. By integrating self-healing polymers into critical components – which utilize mechanisms such as hydrogen bonding, metal–ligand coordination, or reversible crosslinking to reconstruct damaged interfaces – these systems can autonomously repair mechanical failures. This innovative approach effectively mitigates performance degradation caused by repeated mechanical stress, thereby extending device lifespan and enhancing safety for long-term wearable applications, particularly in demanding environments where battery failure would otherwise occur.

To date, only a few FZIBs have been manually integrated into textiles. Future energy textiles must prioritize washability, comfort, breathability, flexibility and absolute safety. Advanced industrial spinning/knitting technologies offer a viable pathway for weaving fiber-shaped FZIBs into garments. However, challenges such as poor stability and large diameters of fiber-shaped FZIBs hinder progress. By integrating matrix structural modification, interfacial optimization, and comprehensive multi-scale engineering, it is reasonable to fabricate FZIBs with favorable mechanical flexibility and maintaining outstanding electrochemical performance. It is anticipated that this systematic, objectively evaluative, and inspirationally suggestive review will provide researchers with timely references for designing high-performance FZIBs and accelerate their scalable applications in the rapidly growing field of wearable electronics.

Author contributions

Tao Sun: writing – original draft, investigation, funding acquisition, conceptualization. Jiaxu Yang: writing – original draft, writing – review & editing. Fangyuan Kang: writing – review & editing, validation. Wenyong Zhang: writing – review & editing, validation. Jianing Hui: data curation, visualization, validation. Xu Li: supervision, validation. Qichun Zhang: supervision, project administration.

Conflicts of interest

The authors declare that they have no known competing financial interests or personal relationships that could influence the work reported in this paper.

Data availability

No primary research results, software or code have been included and no new data were generated or analysed as part of this review.

Acknowledgements

This work was supported by the National Natural Science Foundation of China (22305103), the China Postdoctoral Science Foundation (2024M761186), the Natural Science Foundation of Jiangsu Province (BK20230520), the Program for Jiangsu Specially-Appointed Professors (RC20240920), the General Program of Natural Science Foundation for Higher Education in Jiangsu Province (23KJB150006), and the Young Talent Support Fund from Jiangsu University. Q. Z. acknowledges the financial support from the City University of Hong Kong (7020148; 9239116; 9240189; 9380117; 9678403; 9680375; R-IND26401 and R-IND26402) and the Hong Kong Branch of National Precious Metals Material Engineering Research Center (NPMM), Hong Kong, P. R. China.

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