Porous materials fabricated using carbon dots

Abstract

Porous materials (PMs) are a class of special materials characterized by their internal pore network structures, which afford them a larger specific surface area and a greater number of accessible active sites. Consequently, they find widespread applications in catalysis, energy storage and conversion, etc. Carbon dots (CDs), an emerging class of zero-dimensional carbon nanomaterials, possess highly cross-linked or carbonized cores along with abundant surface functional groups. The precursors of CDs are diverse and cost-effective, allowing for the tailoring of specific structures through controlled reaction conditions. Initially, CDs were extensively utilized in bioimaging and fluorescence detection due to their characteristic photoluminescence properties. However, in recent years, a substantial body of research has focused on employing CDs as fundamental building blocks or modifying species to fabricate various PMs, with experimental evidence underscoring their significant role. In this review, PMs are categorized into porous carbons, porous inorganic materials, and porous gel materials based on their fundamental constituents. We summarize recent advances in PMs constructed using CDs, with a particular emphasis on the influence of CDs regarding the morphology and pore structure of these materials, as well as the underlying mechanisms. This systematic overview aims to provide new insights into the design of porous materials and the multifunctional applications of CDs.

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1. Introduction

Porous materials (PMs) are generally defined as a class of solid materials featuring internal pore network structures, where the pores are interconnected or isolated, forming multiscale spatial systems ranging from the microscopic to the macroscopic scale.^1–3 PMs are typically designed with hierarchical structures, which allow chemical reactions to proceed in a controlled manner both temporally and spatially. Therefore, the size and distribution of pores are critical for PM performance.⁴ According to the International Union of Pure and Applied Chemistry (IUPAC) classification, pore sizes are categorized into three types: micropores (<2 nm), mesopores (2–50 nm), and macropores (>50 nm).⁵ PMs typically exhibit significantly higher specific surface areas (SSAs) compared to dense solids, enabling more extensive interaction with the surrounding environment.^6,7 This characteristic imparts PMs with considerable research value across various fields, particularly in adsorption and separation,^8,9 catalysis^10,11 and energy storage and conversion.^12,13 Under identical conditions, PMs offer faster mass transport rates, more accessible active sites, and performance that often surpasses that of dense bulk materials by several orders of magnitude.¹⁴ Since the recognition of the critical role of the pore structure, an expanding range of PMs have been developed and widely applied. In this work, we categorize PMs based on their fundamental composition into three groups: porous carbon materials (PCMs), porous inorganic materials (PIMs, such as g-C₃N₄, metal oxides, and metal sulfides), and porous gel materials (PGMs).

Carbon dots (CDs) are an emerging class of fluorescent carbon nanomaterials characterized by their ultrasmall size, typically not exceeding 10 nm.^15,16 Most studies agree that the structure of CDs consists of two components: a highly cross-linked or carbonized core and a shell enriched with surface functional groups and defects.¹⁷ Compared to the core, the surface states exert a more profound influence on the properties of CDs, particularly their photoluminescence behavior.^18–20 CDs are generally synthesized from precursors containing conjugated structures or readily cross-linkable organic molecules. The abundance and low cost of such precursors allow for flexible modulation of the CD structure.^21–23 Owing to their unique characteristics, CDs have been extensively employed as fundamental building blocks or functional modifiers in the construction of various materials, exerting significant influence on the morphology and pore structures of the resulting products.

While previous reviews have summarized composite strategies and host–guest interactions between CDs and porous materials,^24,25 it is increasingly recognized that CDs also play a crucial role in pore formation and morphology control. Therefore, this review specifically emphasizes the role of CDs in regulating material morphology, pore structures, and SSA. It covers three main aspects: (i) porous carbon materials engineered by CDs; (ii) porous inorganic materials constructed using CDs; and (iii) porous polymer materials induced by CDs (Fig. 1). In the end, we provide a summary and discuss the primary challenges and future opportunities for CDs in building innovative materials.

Fig. 1 The various roles of CDs in fabrication of PMs.

2. Structure and properties of CDs

CDs are a novel class of zero-dimensional (0D) carbon-based nanomaterials, following the emergence of one-dimensional (1D) carbon nanotubes, two-dimensional (2D) graphene, and molecular fullerenes.²⁶ In 2004, Xu et al. discovered a type of fluorescent carbon nanoparticle during the purification of crude arc-discharge soot via electrophoresis, marking the debut of CDs as a new category of photoluminescent nanomaterials.²⁷ Subsequently, Sun et al. coined the term “carbon dots” to describe these materials.²⁸ CDs typically exhibit ultra-small sizes below 10 nm and a quasi-spherical morphology.²⁹

As illustrated in Fig. 2a, after nearly two decades of development, CDs are generally classified into four types: graphene quantum dots (GQDs), carbon nanodots (CNDs), carbon quantum dots (CQDs), and carbonized polymer dots (CPDs), which are generally regarded as possessing a core–shell structure.^30–33 GQDs are made up of single layers of graphene, which exhibit a high degree of graphitization, extensive sp² domains, and lattice spacings ranging from 0.18 to 0.24 nm—values that are comparable to those of bulk graphite.³⁴ In contrast, CQDs are quasi-spherical carbon nanoparticles which exhibit a crystalline core based on a mixture of sp² and sp³ carbons.³⁵ Compared to GQDs, CQDs have a greater abundance of surface functional groups and higher defect densities. Due to their high crystallinity, the optical bandgaps of both GQDs and CQDs are significantly influenced by their size.³⁶ Due to their high crystallinity, GQDs and CQDs are often prepared via top-down approaches, such as chemical oxidation or arc discharge, which exfoliate them from bulk carbon materials. CNDs are often confused with CQDs. However, some researchers distinguish CNDs as quasi-spherical carbon nanoparticles characterized by an amorphous core, as opposed to the more crystalline core found in CQDs.^37,38 In recent years, an increasing number of studies have adopted bottom-up approaches to synthesize CDs, whereby organic small molecules undergo polymerization and cross-linking to form distinctive core–shell structures (Fig. 2b).^39–41 The majority of CDs prepared via this method are classified as CPDs, a term proposed by Yang et al. in 2018.⁴² Due to incomplete carbonization, CPDs exhibit low crystallinity and possess typical polymeric characteristics.⁴³ CPDs are characterized by the highest abundance of surface functional groups among CD types, enabling facile functionalization or interaction with other materials through tailored precursor selection and reaction conditions.^19,44,45

Fig. 2 (a) Four categories of CDs and their respective characteristics.⁴⁹ Reproduced with permission from ref. 49. Copyright 2022 Springer Nature. (b) Diagram to describe the reaction process of hydrothermal cross-linking polymerization to prepare CPDs by the “bottom-up” route. Reprinted with permission from ref. 39. Copyright 2019 American Chemical Society.

Owing to their unique array of properties, CDs have been increasingly utilized by researchers as fundamental building blocks or additives in material synthesis. Experimental results demonstrate that CDs exert a significant influence on the morphological features of materials, particularly their pore structures.^46–48 (Unless otherwise specified, the term “CDs” in the subsequent discussion refers specifically to CPDs.)

3. PCMs fabricated using carbon dots

As the most predominant category within the PMs family, PCMs have found extensive applications in many domains. Given their structural advantages, CDs have emerged as a logical choice for constructing PCMs. Here, we comprehensively summarize the multifaceted roles of CDs in the fabrication processes of PCMs. It is worth emphasizing that similar synthetic approaches may be categorized under different sub-classifications, as our criterion is based on the primary role of CDs in the formation of PCMs, without causing any conceptual confusion.

3.1. CDs as porous carbon frameworks

CDs generally possessing an intrinsic carbon content exceeding 80% and graphitized cores serve as ideal primary carbon precursors for constructing PCMs. Alkalis (e.g., KOH) or salts (e.g., ZnCl₂) have been widely employed as porogens at both laboratory and industrial scales, functioning through following mechanisms: (i) as chemical activators that etch carbon frameworks to create pores, and (ii) as hard templates to direct morphology. The combination of CDs with porogens represents a universal strategy for tailored PCMs synthesis.

In 2015, Hou et al. developed a novel strategy for the large-scale synthesis of carbon dots via an aldol condensation reaction.⁵⁰ Without any purification (retaining residual NaOH), the as-prepared products were annealed at 800 °C for 2 hours under an argon atmosphere. Under such high temperature and Na catalysis effects, the solid products were rapidly decomposed to produce abundant carbon atoms which then gradually self-assembled to form carbon nanosheets. The rapid decomposition of abundant surface functional groups on CDs generates transient high internal pressure, which effectively suppresses the stacking of carbon nanosheets during their self-assembly process. Finally, with the linkage of numerous O-rich functional groups, the as-grown nanosheets exhibited a cross-linked 3D framework structure (Fig. 3a and b). In subsequent work, the researchers purified as prepared CDs and pyrolyzed them with sodium dihydrogen phosphate (NaH₂PO₄), yielding phosphorus-doped, large-area porous carbon nanosheets.⁵¹ It confirmed that the method possesses universality and allows for facile heteroatom doping. The resulting anode material for sodium-ion batteries (SIBs) delivered a remarkable specific capacity of 108 mAh g⁻¹ even at 20 A g⁻¹, attributed to its abundant micropores (1.2 nm) and expanded interlayer spacing.

Fig. 3 (a) SEM and (b) nitrogen adsorption–desorption isotherms of 3D PCFs. Reproduced with permission from ref. 50. Copyright 2015, Wiley-VCH. (c) General synthetic route of the ultra microporous carbons. Reprinted with permission from ref. 52. Copyright 2018, Wiley-VCH. SEM images of the samples at different reactant ratios (NaOH : acetylacetone): (d) and (g) 1 : 10, (e) and (h) 3 : 10, (f) and (i) 5 : 10. Reprinted with permission from ref. 54. Copyright 2020, Elsevier. (j) Schematic illustrations of the ice templated assembly strategy for fabricating 3D porous carbon. Reprinted with permission from ref. 56. Copyright 2023, Elsevier.

To emphasize the advantages of CDs over conventional carbon sources as precursors for PMs, Zhang et al. compared and analysed the structure and properties of PCMs derived from coal and coal-derived GQDs.⁵² As illustrated in Fig. 3c, the coal-derived GQDs were prepared via chemical oxidation. Benefiting from their ultrasmall size, minimal amounts of KOH could be uniformly dispersed at the edges or interlayers of GQDs. Subsequent high-temperature treatment enabled in situ activation of GQDs by KOH from the interior to the exterior, yielding ultra microporous carbon (CoDCs) with both a high SSA (1730 m² g⁻¹) and an exceptional packing density (0.97 g cm⁻³). In contrast, direct use of coal as the carbon precursor not only consumed significantly more KOH (eightfold higher than that for GQDs) but also resulted in PCMs with heterogeneous pore size distribution and a markedly lower packing density (0.4 g cm⁻³). When CoDCs were employed as electrode materials, the optimized PCMs achieved an ultrahigh areal capacitance of 5.70 F cm⁻² at 1 A g⁻¹ under a high mass loading of 25 mg cm⁻². Similarly, Huang et al. systematically compared sulfur-doped hard carbon derived from CDs (2SC-600), glucose, and carbon fibers.⁵³ The results demonstrated that CDs not only facilitated pore generation but, more critically, provided abundant sulfur-binding sites on their surfaces. The formed C–S bonds decomposed into H₂S, generating more micropores. Benefiting from the selective substitution of oxygen atoms in the carbon framework by sulfur, 2SC-600 exhibits a high initial coulombic efficiency of 68%.

Beyond their role as chemical porogens, alkalis can serve as crystalline templates. As demonstrated by Qiu et al., hollow carbon microboxes were synthesized through precise control of NaOH concentration and carbonization temperature.⁵⁴ Under critical thermal conditions, NaOH underwent transformation into Na₂CO₃ crystalline templates (eqn (1)), which directed the assembly of carbon layers into polyhedral architectures via synergistic electrostatic and van der Waals interactions. The template-precursor balance proved essential: insufficient NaOH led to incomplete template formation, while excess NaOH generated oversized crystals that prevented uniform carbon coating on polyhedral units, ultimately causing structural fragmentation into sharp-edged carbon nanosheets (Fig. 3d–i).

6NaOH + 2C → 2Na + 3H₂ + 2Na₂CO₃ (1)

Notably, benefiting from abundant heteroatom doping, CDs can form PCMs without porogens. In 2014, Zhou et al. fabricated mesoporous carbons (MCs) with a high surface area (183.6 m² g⁻¹) by simply drop-casting CQD solutions onto silicon wafers followed by direct pyrolysis.⁵⁵ Remarkably, MCs demonstrated outstanding catalytic selectivity (84.67%) in the oxidation of cyclooctene to epoxy cyclooctane with 17.37% conversion. As a clearer example, Shi et al. employed a mild chemical oxidation method to prepare CQDs from coal tar pitch.⁵⁶ Subsequently, ice-template induced assembly coupled with the carbonization strategy reveals a transition from 0D CQDs to 3D porous carbon frameworks (PCF-800) composed of cross-linked and twisted nanosheets (Fig. 3j). Through comparative analysis of different pyrolysis stages, the authors proposed that the thermal decomposition of surface functional groups on CQDs and small molecules generates trace gases at high temperatures, thereby creating additional pores in the carbon skeleton.

3.2. CDs as structural modulators

CDs also serve as structural modulators in the fabrication of PCMs. When incorporated into other polymeric or carbon-based matrices, they can effectively induce the formation of unique pore architectures. Two representative strategies have been widely reported: (i) the incorporation of CDs into gel-based polymer networks; and (ii) CD-assisted etching or assembly of carbonaceous materials (e.g., graphene).

The sol–gel method is a commonly employed approach for synthesizing PCMs. However, during pyrolysis, polymer chains are converted into a carbonaceous framework, often leading to issues such as pore collapse or structural inhomogeneity. Fortunately, these challenges can be mitigated by introducing CDs, which act as pore-directing agents and stabilize the porous network during carbonization. For instance, Zhang et al. synthesized Co₉S₈/CD@NSC by oxidizing a mixture of aniline, CDs, and CoCl₂·6H₂O to form a polyaniline hydrogel, followed by freeze-drying and dual-step annealing.⁵⁷ The resulting material exhibited a high SSA of 745.2 m² g⁻¹, with both CDs and CoCl₂ contributing to pore formation. Notably, the SSA increased with the amount of CDs added (Fig. 4a and b), attributed to the crosslinking between CDs and polyaniline nanofibers, as well as the role of CD surface functional groups in dispersing CoCl₂. Similarly, Xu et al. introduced CDs into a starch-based hydrogel (CDSA), where the oxygen-containing functional groups on the CDs formed hydrogen bonds with hydroxyl groups on starch chains, promoting polymerization and crosslinking.⁵⁸ As illustrated in Fig. 4c–h, CDs acted as structural stabilizers, preventing pore collapse during both freeze-drying and carbonization. As a result, PCMs derived from CDSA (C-CDSA) exhibited a higher SSA and a more developed porous structure compared to the CD-free counterpart (C-SA).

Fig. 4 (a) Nitrogen adsorption–desorption isotherms and (b) pore size distribution of Co₉S₈/CD@NSC with different amounts of CD addition. Reprinted with permission from ref. 57. Copyright 2019, American Chemical Society. Photographs and SEM images of the cross-section of (c)–(e) C-SA and (f)–(h) C-CDSA. Reprinted with permission from ref. 58. Copyright 2022, Royal Society of Chemistry. (i) Nitrogen adsorption–desorption isotherms of PD/GS composites and GS. FESEM of (j) GS and (k) PDs/GS-0.5. Reprinted with permission from ref. 60. Copyright 2017, Elsevier. The TEM image of the (l) N,P-PCNFs and (m) PCNFs. Reprinted with permission from ref. 62. Copyright 2024, Royal Society of Chemistry. (n) Nitrogen adsorption/desorption isotherms; (o) pore size distributions of CDs@rGO composites treated with HI vapor for various reduction times. Reprinted with permission from ref. 64. Copyright 2019, Elsevier.

Graphene is a remarkable material composed of carbon atoms arranged in a two-dimensional honeycomb lattice through sp² hybridization. This unique structure grants it exceptional optical, electrical, and mechanical properties, positioning it as a revolutionary material for future technologies.⁵⁹ However, a significant challenge arises from its tendency to restack due to strong π–π interactions between its sheets, which reduces SSA and limits its practical applications. Fortunately, as 0D carbon materials, CDs can readily integrate with graphene, effectively mitigating this issue. Wei et al. employed a sol–gel approach to fabricate composites of CDs and graphene nanosheets (PDs/GS-0.5).⁶⁰ The incorporation of CDs effectively transformed the initially smooth and planar graphene into fractured and wrinkled morphologies, accompanied by a significant increase in SSA (Fig. 4i–k). Meanwhile, this morphology introduces various microporous structures, which is highly beneficial for enhancing the specific capacitance. Heteroatom doping of graphene is a common strategy to enhance its properties. Zhang et al. employed N,S co-doped CDs (N,S-CDs) in a hydrothermal reaction with reduced graphene oxide, achieving not only effective heteroatom incorporation but also inducing the assembly of a morphology with a significantly enlarged SSA.⁶¹

In recent years, porous carbon nanofibers (PCNFs) have emerged as novel 1D carbon materials, which can be synthesized via methods such as chemical vapor deposition or electrospinning. PCNFs not only inherit the excellent electrical conductivity and mechanical flexibility characteristic of 1D nanostructures, but their porous features further expand their potential applications. To achieve this goal, Yuan et al. introduced polytetrafluoroethylene and N,P-co-doped CDs (N,P-CDs) into the precursor solution used for electrospinning.⁶² The resulting fibrous membrane was annealed at 900 °C for 2 hours, yielding N,P-PCNFs with a distinct bubble-like porous morphology. Compared to PCNFs prepared without the addition of N,P-CDs, the N,P-PCNFs exhibited uniform porosity and no observable fiber breakage, indicating that the incorporation of N,P-CDs significantly enhanced the structural stability of CNFs (Fig. 4l and m). In 2025, Qin et al. employed a similar approach to fabricate CoOx-loaded porous CNFs (CNF@CDs@CoOx), in which CDs also played a crucial role in enhancing the mechanical flexibility of the fibers.⁶³ When used as an anode material for SIBs, the resulting CNF@CDs@CoOx demonstrated promising potential for application in flexible energy storage devices.

In some circumstances, the insufficient surface functional groups on CDs fail to contribute to the formation or modulation of the pore structure. However, CDs possess a highly stable structure, enabling them to serve as “nano-buttresses” that physically reinforce the carbon framework. Hoang et al. synthesized CDs@rGO composites via a hydrothermal method and found that during the HI-mediated reduction of GO, CDs served as nanofillers to effectively inhibit the restacking of graphene sheets, thereby preserving the porous architecture to a significant extent (Fig. 4n and o).⁶⁴ Metal–organic frameworks (MOFs), with their intrinsic porosity and highly tunable elemental composition, are considered ideal precursors for porous carbon materials. However, under extreme temperatures, the framework structure of MOFs tends to collapse, leading to pore blockage. Tang et al. reported PCMs derived from MOF-5, in which GQDs with abundant carboxyl groups and rigid structure could uniformly distribute in the MOF-5 precursor by coordinating with [Zn₄O]⁶⁺ clusters and effectively reinforce the carbon skeleton during pyrolysis (Fig. 5a).⁶⁵ As a result, the SSA of the obtained PCMs was 500 m² g⁻¹ higher than that of PCMs derived from pristine MOF-5.

Fig. 5 (a) The preparation and structural transformation process of MPC and GMPC-0.35. Reprinted with permission from ref. 65. Copyright 2022, Elsevier. (b) Pore size distribution of PNDCs-500CDs-y °C with different carbonization temperatures. (c) TEM of PNDCs-500CDs-1200 °C. (d) SAXS patterns of PNDCs, PNDCs-500CDs, and PNDCs-500CDs-1200 °C. Reprinted with permission from ref. 66. Copyright 2024, Wiley-VCH. (e) Schematic representation of the synthesis of hollow N-doped carbon. (f) and (g) TEM and HRTEM images of p-HNCs. Reprinted with permission from ref. 67. Copyright 2019, Elsevier.

Closed pores represent a distinct type of pore structure compared to open pores. Although they are isolated from the external environment, they play a crucial role in anode material SIBs. Huang et al. synthesized composite nanosheets of polyimide and CDs (PI-xCDs) via a solvothermal method.⁶⁶ During subsequent high-temperature carbonization, the surface functional groups on the CDs decomposed and released gases, leading to the formation of flower-like porous carbon nanosheets (PNDCs-xCDs-y °C). Interestingly, although BET measurements failed to detect porosity when the carbonization temperature exceeded 1000 °C, TEM observations revealed the presence of abundant mesopores (Fig. 5b and c). Furthermore, small-angle X-ray scattering (SAXS) analysis of PNDCs-500CDs-1200 °C displayed distinct peaks in Q = 0.1–1 Å⁻¹, indicating a large number of closed pores (Fig. 5d). These findings suggest a transformation from micropores to closed pores with increasing carbonization temperature. The presence of such closed-pore structures provides additional sodium storage sites in the plateau region for the high storage capacity.

3.3. CDs as templates

The template method is a widely adopted strategy for the synthesis of PMs, typically categorized into hard-template and soft-template methods. The hard-template method employs the inner or outer surfaces of solid materials as structural frameworks, into which monomers are filled and reacted, followed by template removal to yield porous structures. In contrast, the soft-template method relies on the self-assembly of amphiphilic molecules into ordered aggregates (e.g., micelles or reverse microemulsions), which serve as dynamic scaffolds during material formation. Notably, recent studies have demonstrated that CDs can also function as effective templates for the fabrication of PCMs.

Hong et al. dispersed CDs in a water/ethanol mixed solvent to form micelles, which were then coated with a polypyrrole shell via chemical oxidative polymerization.⁶⁷ As shown in Fig. 5e, the abundant functional groups on the CDs provide ample reactive sites for the polymerization of pyrrole, leading to the formation of a uniform shell layer. Subsequently, CDs were removed by repeated washing with ethanol and water, followed by annealing at 650 °C for 5 h to obtain w-HNCs. Samples in which CDs were not removed were denoted as p-HNCs. Both p-HNCs and w-HNCs possess hollow structures (Fig. 5f and g), but p-HNCs exhibit more micropores, which originates from the internal pressure and gas release generated during the decomposition of CDs. The enhanced porosity was advantageous for electrolyte infiltration and ion adsorption. As a result, anode materials constructed using p-HNCs for potassium-ion batteries delivered high reversible specific capacities of 254 mAh g⁻¹ at 0.1 A g⁻¹ after 100 cycles and 160 mAh g⁻¹ at 1.0 A g⁻¹ after 800 cycles.

For partially carbonized CDs, a substantial number of active chemical bonds remain within their structure. These residual bonds can serve as targets for directional etching, enabling precise modulation of pore size and uniformity. Huang et al. demonstrated that CDs can serve as hard templates for the fabrication of PCMs with highly uniform pore sizes.⁶⁸ In this work, coal tar-derived CPDs were reacted with melamine to form a hyper-crosslinked polymer (HCP). Acting as sacrificial templates, the CPDs underwent targeted “excavation” by KOH, producing pores that closely matched CPD dimensions (Fig. 6a). As a result, the carbonized product exhibited a highly developed porous structure dominated by small mesopores (2–10 nm accounting for 92.07%) and an ultrahigh SSA of 4241 m² g⁻¹. In 2024, Zhang et al. reported the synthesis of sub-nanometer PCMs using CDs prepared from citric acid and diethylenetriamine (DETA), which contained a large number of amide bonds in its interior structure.⁴⁶ These CDs were crosslinked into a gel via reaction between surface amine groups and poly(ethylene glycol) diglycidyl ether (PEGDGE), followed by immersion in KOH. As shown in Fig. 6b, the internal amide bonds within the CDs were selectively cleaved, leading to their fragmentation into small pieces. After carbonization, the resulting PCMs exhibited numerous sub-nanopores (0.64–0.8 nm), which are favourable for K⁺ desolvation and rapid ion transport (Fig. 6c). As a result, the optimal sample with a high packing density (0.81 g cm⁻³) displays outstanding capacitances (gravimetric 515.5 F g⁻¹, areal 5.16 F cm⁻², and volumetric 417.6 F cm⁻³ respectively at 1 A g⁻¹) at the commercial-level mass-loading of 10 mg cm⁻².

Fig. 6 (a) Schematic diagram showing the transformation of CCPD@HCPM(CC). Reprinted with permission from ref. 68. Copyright 2023, Elsevier. (b) Schematic diagram of the synthetic procedure for CPDHs. (c) Schematics of K⁺ residing in pores with different sizes. Reprinted with permission from ref. 46. Copyright 2025, Wiley-VCH.

4. PIMs constructed using carbon dots

Most pristine inorganic materials possess dense structures and relatively low SSA, which result in limited exposure of active sites and consequently restrict their performance in various applications. As a result, increasing research efforts have been devoted to engineering morphology of inorganic materials, particularly toward enlarging their SSA and introducing well-defined porous architectures—to significantly enhance their performance. As an organic–inorganic hybrid nanomaterial, CDs readily form composites with a wide range of inorganic materials. It has been proved that the incorporation of CDs often induces significant structural changes in the inorganic host materials. The mechanisms underlying pore formation in inorganic materials mediated by CDs can be classified into two primary categories: (i) CDs-induced self-assembly of the inorganic components, and (ii) gas evolution from the decomposition of surface functional groups on CDs during thermal treatment.

4.1. Decomposition of CDs induces porosity in inorganic materials

A polymeric semiconductor, namely graphitic carbon nitride (g-C₃N₄), has elicited ripples of excitement in the research communities as the next generation photocatalyst, due to its facile synthesis, appealing electronic band structure, high physicochemical stability, and “earth-abundant” nature. However, bulk g-C₃N₄ suffers from rapid recombination of photogenerated charge carriers and limited visible-light utilization.⁶⁹ To address these issues, Xu et al. synthesized a porous S-doped g-C₃N₄/C-dot composite (S-C₃N₄/C-dot) via a simple stirring process followed by thermal treatment.⁷⁰ During pyrolysis, CDs were oxidized into gases at high temperatures, creating pores within the S-C₃N₄ framework (Fig. 7a and b). The pore formation also accelerated the thermal polymerization of the S-C₃N₄ precursor, and further facilitated its crystallization.

Fig. 7 (a) TEM images of S-C₃N₄/C-dot. (b) Pore size distribution of S-C₃N₄/C-dot with addition of different C-dots. Reprinted with permission from ref. 70. Copyright 2019, Elsevier. (c) and (d) High-resolution SEM image of CDs@P-Eu-MNs. Reprinted with permission from ref. 71. Copyright 2022, Elsevier. (e) The role of CDs in modified Mxene. Reprinted with permission from ref. 47. Copyright 2023, Springer Nature. (f) Different morphologies resulting from different concentrations of CDs (From left to right, the concentrations of CDs are respectively 0, 0.25, 0.5, and 1 mg mL⁻¹). Reprinted with permission from ref. 72. Copyright 2016, Wiley-VCH.

Wang et al. synthesized CDs via a hydrothermal reaction using citric acid and cysteine, and subsequently reacted them with citric acid and Eu(NO₃)₃·6H₂O to fabricate CD-based porous europium micro-networks (CDs@P-Eu-MNs).⁷¹ As shown in Fig. 7c and d, CDs not only serve as excellent nucleation and growth platforms for the initial nanostructures, but also contribute to the generation of abundant pores through dehydration reactions between their surface functional groups and Eu-MNs. The construction of CDs@P-Eu-MNs not only extends light absorption into the visible region but also enhances the separation and transport of photogenerated charge carriers. Similarly, Wang et al. introduced CDs into layered Ti₃CNT_x MXene via simple stirring, followed by annealing at 350 °C for 1h to obtain porous MXene.⁴⁷ As illustrated in Fig. 7e, on one hand, CDs act as interlayer spacers to prevent restacking of MXene nanosheets, and on the other, CDs partially decompose to release NH₃ which in situ etches the MXene to form a 3D interconnected porous network. The resulting flexible film electrodes achieve excellent gravimetric capacitance (688.9 F g⁻¹ at 2 A g⁻¹) and outstanding rate capability.

4.2. CD-induced self-assembly of inorganic materials

As one of the simplest and most widely adopted strategies, incorporating CDs into inorganic precursors has been extensively employed to tailor the growth of inorganic materials. Remarkably, CDs often interact with inorganic species during synthesis, regulating their nucleation and growth processes, thereby affording optimized morphologies and enhanced performance.

As early as 2016, Wei et al. utilized CDs to modulate the morphology of NiCo₂O₄ grown on Ni foam.⁷² By increasing the concentration of CDs in the precursor solution from 0 mg mL⁻¹ to 1 mg mL⁻¹, the NiCo₂O₄ morphology evolved from sea urchin-like to flower-like, and eventually to bayberry-like structures, accompanied by significant changes in SSA and the pore structure (Fig. 7f). By simply tuning the reaction conditions, PIMs with diverse morphologies can be readily obtained, which has attracted significant attention from researchers. In 2017, Wei et al. introduced CQDs into M_xO_y (M = Co, Ni) precursor solutions for hydrothermal synthesis, followed by annealing the resulting powders at 300 °C for 3 h.⁷³ Compared to M_xO_y, CQDs/M_xO_y exhibit distinctly different morphologies. It was found that CQDs could induce the self-assembly of M_xO_y nanosheets or nanowires into flower-like or sea urchin-like architectures (Fig. 8a–f) through electrostatic interactions with metal ions, leading to a substantial increase in both SSA and specific capacitance.

Fig. 8 FESEM images of M_xO_y: (a) Co₃O₄, (c) NiCo₂O₄, (e) NiO and the CQDs/M_xO_y: (b) CQDs/Co₃O₄, (d) CQDs/NiCo₂O₄, (f) CQDs/NiO. Reprinted with permission from ref. 73. Copyright 2017, Elsevier. TEM images of CT-500 products synthesized at different reaction time: (g) 0.5 h, and (h) 1.5 h of hydrolysis reaction at room temperature, (i) 1 h, (j) 3 h, (k) 6 h, and (l) 12 h of hydrothermal time at 180 °C. Reprinted with permission from ref. 74. Copyright 2020, Elsevier. (m) Schematic illustration of Bi₂Se₃ self-assembly induced by CDs. Reprinted with permission from ref. 76. Copyright 2022, Elsevier.

Although the modulation of inorganic materials by CDs is a commonly observed phenomenon, a more detailed investigation into their morphological evolution is still required. In 2020, Wu et al. reported the use of CQDs to regulate the growth of TiO₂.⁷⁴ Specifically, TiO₂ nanorods were mixed with CQDs under stirring, followed by hydrothermal treatment, resulting in flower-like architectures rich in mesopores. The morphological evolution process is shown in Fig. 8g–l: after CQDs incorporation, the originally dense TiO₂ nanorods became loose and uneven (Fig. 8h). Following just 1 hour of hydrothermal treatment, the morphology rapidly transformed into oval-shaped structures with burr-like surfaces. The results suggest that the incorporation of CQDs can decrease the surface energy of the system, then promoting the formation of mesoporous TiO₂ nanostructure. With further increasing the hydrothermal reaction time, the product showed a spherical morphology, where more nanosheets grew onto the surface of nanospheres. The obtained CT-500 exhibited a SSA of 197.7 m² g⁻¹ along with abundant mesopores. Song et al. has also synthesized TiO₂ spheres with flower-like surfaces via a solvothermal reaction between nitrogen-doped CDs (N-CDs) and TiO₂.⁷⁵ They found that the amount of NCDs plays a critical role in determining the final morphology. The optimized TiO₂/NCDs₅ sample, featuring ideal morphology and pore size distribution, was employed as a protective layer for zinc-ion battery anodes, which facilitated ion transport, suppressed dendrite growth, and significantly improved cycling stability. Wang et al. synthesized uniform rod-like Bi₂Se₃/CDs composites using ZnSe(DETA)_0.5 microbelts as a substrate via an ion-exchange method.⁷⁶ Through detailed morphological evolution studies, the authors proposed a CDs-induced self-assembly growth mechanism (Fig. 8m): when sufficient CDs are incorporated in the reaction, firstly, they will coat on the ZnSe(DETA)_0.5 microbelts due to the coordination effects. After adding BiCl₃, the CDs will interact with Bi³⁺ by electrostatic interaction, which drives the CDs to act as active sites for ion exchange process between Bi³⁺ and Zn²⁺, yielding the formation of Bi₂Se₃ nanosheets tightly bound with CDs and distributed along the nanobelts. The crosslinked Bi₂Se₃ nanosheets form a robust 3D framework for fast-kinetics lithium storage, providing efficient pathways for electron and ion transport.

Notably, beyond guiding the assembly of inorganic materials, CDs impart additional functions. For instance, Liu et al. also prepared SnS₂/CDs composites via hydrothermal synthesis, which were applied as fillers in polymer electrolytes for lithium-ion batteries (LIBs).⁷⁷ The incorporation of CDs not only induced the transformation of SnS₂ from a stacked hexagonal structure into a flower-like morphology but also promoted the generation of abundant sulfur vacancies, which significantly facilitate dissociation of lithium salt and accelerate migration of Li⁺. Furthermore, CDs dotted on the surface of SnS₂ have rich organic functional groups, which can serve as the bridging agent to enhance the compatibility of filler and polymer, leading to superior mechanical performance and fast ion transport pathway.

In summary, CDs have been demonstrated to effectively direct the growth of inorganic materials, preventing their excessive aggregation and thereby generating higher SSA and well-defined pores. Moreover, CDs can also be simply composited with inorganic materials followed by calcination, where their nanoscale dispersibility and the thermal decomposition of surface functional groups contribute to the formation of uniform pores.

5. PGMs constructed using carbon dots

PGMs are a class of porous soft materials characterized by a 3D crosslinked polymer network infused with a filling medium, such as water, organic solvents, or gases. Owing to their high SSA, low density, excellent stability, and uniform pore size distribution, PGMs form a distinct subset of porous materials. Typically, GPMs are derived from flexible molecular chains with polymerizable double bonds or reactive functional groups. CDs, with their abundant surface functional groups, can be readily incorporated into gel networks via crosslinking reactions. This integration not only enables composite formation but also modulates the pore architecture of the resulting gels.

5.1. CDs as crosslinkers

In 2017, Lee et al. reported the fabrication of a photoluminescent C-dot-incorporated keratin/poly(vinyl alcohol) (keratin/PVA) hydrogel via an electron beam irradiation technique.⁷⁸ The keratin/PVA hydrogel without C-dots (0% C-dots) exhibited a network structure composed of randomly oriented fibrous structures. In contrast, the hydrogels incorporating C-dots displayed a more pronounced fibrous morphology along with a well-developed porous architecture. Importantly, the hydrogel retained the quantum confinement effect of C-dots, endowing the material with excellent photoluminescent properties. As a further demonstration of CDs functioning as crosslinkers, Wu et al. polymerized CDs with egg white (EW) to form hydrogels.⁴⁸ Notably, the EW hydrogel fabricated without CDs exhibited a dense, non-porous morphology, whereas the introduction of CDs led to the formation of distinct pores, with the pore size decreasing progressively as the CD content increased (Fig. 9a–e). The proposed mechanism is illustrated in Fig. 9f: during heating of the EW + CDs solution, the EW proteins unfolded, exposing functional groups, such as amino, carbonyl and carboxyl groups. These groups then bonded with surface functional groups on the CDs via non-covalent or covalent bonds, including intermolecular hydrogen bonding or dehydration reactions. CDs served as crosslinking agents, facilitating the formation of a robust 3D and porous network structure by connecting the unfolded protein chains.

Fig. 9 (a)–(e) SEM images of hydrogels: 1CDs@EW, 4CDs@EW, CEWH (8CDs@EW), and 12CDs@EW (the numbers represent the concentration of CDs added.). Scale bars: 20 μm. (f) A proposed mechanism for the formation of a stretchable and transparent network structure using CDs and EW peptide chains. Reprinted with permission from ref. 48. Copyright 2023, American Association for the Advancement of Science. SEM images of (g1) and (g2) TAC0 without ACDs and ACDs-loaded nanocomposite hydrogels: (g3) and (g4) TAC100 with 100, (g5) and (g6) TAC500, (g7) and (g8) TAC1000 (the numbers indicate the amount of ACDs added, in μL). Reprinted with permission from ref. 79. Copyright 2022, American Chemical Society. (h) The schematic comparison between the GPEs derived from three polymers: the cast PVDF-HFP (solid polymer), the phase inversion derived PVDF-HFP (stacked polymer dots), and the PVDF-HFP/CDs (polymer-CDs columns). Reprinted with permission from ref. 103. Copyright 2024, Elsevier.

In fact, some functional groups on the CDs do not participate in crosslinking with the monomers. Instead, they may interact with the side groups of the polymer chains, leading to a reduction in the original pore size of PGMs. However, this effect is not necessarily detrimental. Das et al. synthesized Apium graveolens-derived carbon dots (ACDs) and subsequently prepared thermoplastic starch/poly(acrylic acid)/ACD hydrogels via thermal polymerization.⁷⁹ As shown in Fig. 9g1–g8, with the gradual increase of ACD addition from 0 μL to 1000 μL, the pore size of the hydrogel progressively decreased. This effect is attributed to the formation of additional physical crosslinks through hydrogen bonding between ACDs and the polymer chains. Moreover, the room-temperature self-healing behaviour was observed for the ACDs-reinforced hydrogels, with a healing efficacy of more than 45%. Similarly, Alzahrani prepared CDs via a thermal coupling reaction between polyethyleneimine and L-cysteine, followed by their incorporation into a precursor solution to fabricate the chitosan/poly(acrylamide-co-2-aminoethyl methacrylate) hydrogels.⁸⁰ The introduction of CDs led to a reduction in pore size and a denser gel network. This phenomenon can be explained by the formation of broad secondary interactions between the polarities on the surface of CDs and the additional groups attached to the hydrogel polymer chains. The resulting hydrogel not only inherits the antibacterial and antioxidant properties of CDs but also effectively prevents the penetration of moisture and gases, demonstrating excellent potential in food preservation applications.

5.2. Others

In certain cases, CDs cannot effectively crosslink with polymer monomers; however, their unique intrinsic properties can still be harnessed to construct PGMs. In 2024, Ni et al. proposed a strategy for constructing uniform ion transport channels within gel polymer matrices using CDs as structural modulators.¹⁰³ Specifically, a cast PVDF-HFP/U-CDs membranes was first prepared in N-methyl-2-pyrrolidone (NMP) via a mild phase inversion method, resulting in a dense, closed-surface structure. After the membranes generating procedure, the solvent exchange is conducted between water and NMP, which helps form vertical channels in the polymer matrix. It is noteworthy that a portion of the U-CDs spontaneously migrated from the membrane into the aqueous phase due to their high water solubility. Consequently, the resulting PVDF-HFP/U-CD membranes featured oriented polymer arrays perpendicular to the lithium metal surface, with CDs embedded along the channel walls (Fig. 9h). After absorbing substantial amounts of liquid electrolyte, the obtained gel polymer electrolytes exhibited vertically aligned Li⁺ transport pathways. Additionally, the presence of CDs facilitated lithium salt dissociation, thereby increasing the Li⁺ transference number. In 2025, Huang et al. further optimized this approach by employing a more aggressive boiling treatment to remove CDs from the PVDF-HFP membrane, yielding a membrane with an even richer porous structure.¹⁰⁷ Notably, the porosity was found to correlate positively with the initial CD loading amount.

To provide readers with a clear and systematic overview, we have summarized in Table 1 the key information and application of CD-fabricated PMs.

Table 1 The key information and application of CD-fabricated PMs

Sort	Material	Precursors of CDs	Fabrication methods of PMs	SSA (m^2 g^−1)	Application	Ref.
PCMs	MCs	Graphite	Direct calcination of CDs	183.6	Selective oxidation of hydrocarbons	55
	3D PCFs	Acetone	Direct calcination of CDs	467	Sodium-ion batteries (SIBs)	50
	PDs/GS	Polyethyleneimine (PEI)	Ultrasonic compounding of CDs with graphene nanosheets	407.2	Supercapacitor	60
	1D CNF, 2D CNS, and 3D CFW	Acetone	Calcination of CDs and salt mixtures	429.5	SIBs	81
	NPOCD/HPC	Phytic acid, PEI	Calcination of CDs@Polyacrylamide hydrogel	1025	Supercapacitor	82
	PS–BC	Benzenesulfonic acid, phenylphosphonic acid, acetone	Direct calcination of CDs	671.6	Na- and Li-ion batteries (LIBs)	83
	p-HNCs	Acetaldehyde	Calcination of CDs-assisted hollow polypyrrole	68.78	Na- and K-ion batteries (KIBs)	67
	3@10–600 °C	Acetylacetone	Na2CO3-assisted templating method	60.6	SIBs	54
	CCPD@HCPM(CC)	Coal tar	Oriented etching of CDs by KOH	4241	Supercapacitor	68
	PNDCs-500CDs-1200 °C	Acetaldehyde	Calcination of CDs@polyimide	—	SIBs	66
	CPDHs	Citric acid (CA), diethylenetriamine	CDs gelation followed by calcination	1020.4	Supercapacitor	46
	N-PCFs	CA, urea	Direct calcination of CDs	483.7	LIBs	84
	CDs/NSPC	Bovine serum albumin	Direct calcination of CDs	1172.54	Zn–air batteries(ZABs)	85
	PC-CDs	P-nitroaniline	Ultrasonic compounding of CDs with p-nitroaniline derived PCMs	2462	Supercapacitor	86
	DAEC	Yolks	Calcination of CDs and egg white mixtures	1999.3	Supercapacitor	87
	GMPC-0.35	Coal powder	CDs encapsulated in MOF-5 followed by calcination	1841	Supercapacitor	65
	PCF-700	Coal tar pitch	Direct calcination of CDs	65.21	LIBs	56
	CQDs/HPC	CA, urea	Calcination of CDs with camellia oleifera shell powder and urea	1750	Supercapacitor	88
	ACD	Glucose	Direct calcination of CDs	1246	Supercapacitor	89
	rGO/CDs	CA	Ultrasonic-assisted blending of CDs with rGO	44.52	Supercapacitor	90
PIMs	S-C3N4/C-dot	Glucose	Calcination of S-C3N4/C-dot composite	98	Photocatalysis	70
	Ni9PCN	CA, urea	Calcination of CDs with urea	47.603	Photocatalysis	91
	CDs-MnO2	Ammonium citrate, sodium dihydrogen phosphate	Microwave-assisted hydrothermal reaction of CDs and KMnO4	254.83	Oxygen evolution reaction (OER)	92
	Ni(OH)2/af-GQDs	Graphite	Homogeneous blending of CDs with Ni(OH)2 nanosheets	84.6	Supercapacitor	93
	Black ZnO Nano Clusters	CA, ethylenediamine(EDA)	Reaction of CDs with ZnO precursors	49.8	Nickel-zinc alkaline batteries	94
	Bi2Se3/CDs	Acetaldehyde	CD-assisted hydrothermal growth of Bi2Se3 on ZnSe(DETA)0.5 substrates	59.89	LIBs	76
	Mn3O4/NCDs	CA, EDA	Hydrothermal reaction of CDs with Mn3O4 precursors followed by calcination	45.5	Zinc-ion batteries (ZIBs)	95
	SnO2/CDs-300	Acetaldehyde	Solvothermal reaction of CDs with SnO2 precursors in ethanol	77.61	LIBs	96
	LDH/CD@CC	Cetylpyridinium chloride monohydrate	Electrodeposition using mixed electrolyte containing Ni(NO3)2, Co(NO3)2, and CDs	—	Supercapacitor	97
	Bi2O3/NCDs	CA, EDA	Solvothermal reaction of CDs with Bi(NO3)3·9H2O followed by calcination	—	Supercapacitor	98
	NCDs@g-C3N4	p-phenylenediamine	Hydrothermal reaction of CDs with g-C3N4	60.9	Photocatalysis	99
PGMs	PLLA/CQD	Corn stalks	Gelation of CDs and poly(L-lactic acid) followed by solvent evaporation	—	Cell culture	100
	FH-5	CA, polyvinyl alcohol	Synthesis of carboxymethylated carbon nanofibers grafted with CDs and free radical copolymerization with acrylic acid monomer	—	Contaminant treatment	101
	PCCEs	CA, EDA	Polymerization of PVDF and PEG-CDs by solvent evaporation method	—	Gel electrolytes of LIBs	102
	CEWH	CA, urea	Thermal polymerization of CDs and egg white	—	Wound dressing	48
	PVDF-HFP/U-CDs	CA, urea	Polymerization of PVDF and CDs by a mild phase inversion process	—	Gel electrolytes of LIBs	103
	GCDs-PAA	Garlic	Thermal polymerization of CDs, acrylic acid, pectin and polyethylene glycol dimethacrylate	—	Wound dressing	104
	CD-HY	Chitosan, poly(ethyleneimine)	Gelation of chitosan–CD–glycerol mixture induced by NaOH	—	Cell monitoring	105
	CDs/HD	Tartaric acid, triethylenetetramine	Thermal polymerization of CDs, polyvinyl alcohol, polyvinylpyrrolidone and citric acid	—	Contaminant treatment	106

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6. Conclusions and outlook

In summary, CDs have demonstrated remarkable potential in the construction and performance enhancement of PMs, with wide-ranging applications in energy storage and conversion, catalysis, and adsorption. This review highlights the influence of CDs on the morphology and pore structure of materials, systematically summarizing various PMs synthesized with CDs. Numerous studies have explored the evolution of PMs by modulating the type and amount of CDs, revealing a range of material growth mechanisms and underscoring the pivotal role of surface functional groups on CDs. Despite past research confirming the role of CDs in constructing PMs, several challenges remain before their practical application.

(i) The true structure of CDs remains unclear, and existing structural models are primarily derived from indirect evidence obtained through various characterization techniques. A more accurate understanding of the structural features of CDs would facilitate deeper insights into their role in the synthesis of PMs and enable a clearer analysis of structure–property relationships. Employing structurally well-defined precursors in combination with advanced characterization methods may offer a promising strategy to address this challenge.

(ii) The large-scale and precise synthesis of CDs remains a critical challenge that directly impacts their potential for industrial application. Currently, solvothermal methods dominate CD synthesis in the laboratory, offering good particle uniformity. However, the high energy consumption and stringent safety requirements limit large scale production. In recent years, the salt-assisted solid-state pyrolysis method has emerged as a promising alternative, eliminating the hazards of high-pressure conditions and enabling kilogram-scale production.

(iii) Most of the research on PMs constructed using CDs is application-oriented, ignoring the underlying reaction mechanisms and structure–property relationships. Although some studies have investigated the intermediate products at various reaction stages, the overall synthesis process remains a “black box,” as ex situ characterization techniques frequently miss critical transient information. Advanced in situ characterization and real-time observation techniques may be helpful. A more comprehensive understanding of the mechanisms would facilitate the broader application of CDs across diverse materials.

(iv) Although the potential of CDs in constructing porous materials has been well established in recent years, only a few studies have investigated the influence of CDs on other features of PMs, such as the electronic structure, which is also critical for PM performance. Moreover, CDs possess unique properties, including fluorescence, catalytic activity, and bioactivity. Integrating these properties with PMs to create multifunctional materials is therefore highly meaningful.

Nevertheless, CDs have demonstrated excellent potential in constructing PMs. We believe that in the near future, these challenges will be conquered by researchers, and CDs will make greater contributions to the preparation and application of PMs.

Author contributions

H. S. was responsible for writing the review and conducting the literature search and compilation. X. Z. contributed to the conceptual development and preparation of the manuscript. B. W. and T. H. arranged and organized the figures and assisted with manuscript revision. H. X. supervised all stages of the project, from defining the review topic to finalizing the manuscript, to ensure scientific rigor.

Conflicts of interest

There are no conflicts to declare.

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 financially supported by the National Natural Science Foundation of China (U24A20565 and 22575057) and the Science and Technology Commission of Shanghai Municipality (25ZR1401024).

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