先进电催化功能碳基材料研究新进展

doi:10.1016/S1872-2067(25)64749-8

催化学报 ›› 2025, Vol. 76: 10-36.DOI: 10.1016/S1872-2067(25)64749-8

先进电催化功能碳基材料研究新进展

翁应龙^b^,^d, 张建平^b, 张坤^a^,^*(), 路亦通^a^,^b, 黄婷婷^b, 康英博^d, 韩晓彤^b^,^*(), 邱介山^c^,^*()

^a东北电力大学化学工程学院, 吉林吉林 132012
^b重庆大学化学化工学院, 重庆 401331
^c北京化工大学化学工程学院, 化工资源有效利用国家重点实验室, 北京 100029
^d辽宁工业大学化学与环境工程学院, 辽宁锦州 121001

收稿日期:2025-04-10 接受日期:2025-04-26 出版日期:2025-09-18 发布日期:2025-09-10
通讯作者: 张坤,韩晓彤,邱介山
基金资助:
国家自然科学基金(22208035);重庆自然科学基金(2024NSCQ-MSX1402);留学生回国创业创新(cx2024115)

Recent progress in functional carbon-based materials for advanced electrocatalysis

Yinglong Weng^b^,^d, Jianping Zhang^b, Kun Zhang^a^,^*(), Yitong Lu^a^,^b, Tingting Huang^b, Yingbo Kang^d, Xiaotong Han^b^,^*(), Jieshan Qiu^c^,^*()

^aSchool of Chemical Engineering, Northeast Electric Power University, Jilin 132012, Jilin, China
^bSchool of Chemistry and Chemical Engineering, Chongqing University, Chongqing 401331, China
^cState Key Laboratory of Chemical Resource Engineering, College of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China
^dSchool of Chemical and Environmental Engineering, Liaoning University of Technology, Jinzhou 121001, Liaoning, China

Received:2025-04-10 Accepted:2025-04-26 Online:2025-09-18 Published:2025-09-10
Contact: Kun Zhang, Xiaotong Han, Jieshan Qiu
About author:Kun Zhang (School of Chemical Engineering, Northeast Electric Power University) received his Ph.D. degree from Dalian University of Technology in 2020. In the same year, he joined the Guangzhou Branch of Sinopec Corporation. Since 2022, he has been working at Northeast Electric Power University. His research focuses on energy materials and electrocatalysis, with an emphasis on the design of novel electrocatalysts for hydrogen production. His recent work includes the synthesis of hollow-structured materials with superior electrocatalytic performance and the development of metal- and nonmetal-ion-doped electrocatalysts derived from metal organic frameworks (MOFs) with excellent overall water splitting activity. To date, he has published more than 20 peer-reviewed papers.
Xiaotong Han (School of Chemistry and Chemical Engineering, Chongqing University) received his B.A. degree from Nanjing Tech University (P. R. China) in 2013, and Ph.D. degree from Dalian University of Technology in 2019. He carried out postdoctoral research at Sungkyunkwan University (Republic of Korea) from 2019 to 2022. Since May of 2022, he has been working in School of Chemistry and Chemical Engineering, Chongqing University. His research interests focus on surface/interface engineering of energy materials and their applications in water splitting, organic electrosynthesis, biomass electrooxidation, electrocatalytic epoxidation of olefins, and zinc-air batteries. To date, he has published more than 70 peer-reviewed papers.
Jieshan Qiu (College of Chemical Engineering, Beijing University of Chemical Technology) received his Ph.D. degree in Organic Chemical Engineering in 1990 from Dalian University of Technology. Currently, he is Cheung-Kong Distinguished Professor of Carbon Science and Chemical Engineering. He is an internationally recognized research and thought leader in carbon science and chemical engineering. His research encompasses both fundamental and applied aspects of carbon materials and science, with a focus on the methodologies for producing carbon materials and their applications in catalysis, energy storage and conversion. He has published more than 800 peer-reviewed papers.
Supported by:
National Natural Science Foundation of China(22208035);Natural Science Foundation of Chongqing(2024NSCQ-MSX1402);Support Plan for Overseas Students to Return to China for Entrepreneurship and Innovation(cx2024115)

摘要/Abstract

摘要：

随着能源危机和环境污染问题日益严重, 开发绿色、可持续的能源转换与存储技术已成为全球研究的热点. 电催化技术, 特别是在水分解、二氧化碳还原、氮气还原等反应中的应用, 已被广泛认为是实现绿色能源转换和存储的关键技术. 然而, 现有的贵金属催化剂虽然具有出色的催化性能, 但由于其稀缺性、高成本及长期稳定性差, 限制了它们在大规模应用中的推广. 因此, 开发低成本、高效、稳定且资源丰富的替代电催化剂, 特别是非贵金属和功能碳基材料, 已成为当前科研的重点. 功能碳基材料因其优异的化学稳定性、高导电性和较大的比表面积, 成为研究人员关注的焦点. 通过对碳基材料的结构设计和功能化改性, 可以显著提升其在电催化反应中的性能. 因此, 基于碳的电催化剂的研究不仅为绿色能源技术提供了新的解决方案, 也推动了电催化领域的发展.

本文总结了近年来碳基材料在先进电催化领域中的研究进展, 特别是它们在多种电催化反应中的应用. 首先介绍了碳基材料在电催化中的优势, 包括其大比表面积、优异的导电性和良好的化学稳定性. 与传统贵金属催化剂相比, 碳基材料具有较低的成本和较好的可调性, 使其成为实现高效电催化反应的理想选择. 在功能化方面, 详细介绍了不同维度碳材料(如零维碳量子点、二维石墨烯、三维碳纳米材料)的设计与改性策略. 通过引入不同的官能团、掺杂异质原子等手段, 可以调节材料的电子结构、提高其催化活性和稳定性. 例如, 碳量子点通过掺入金属元素或有机分子, 可增强催化反应中的电子交换能力, 从而提高电催化性能. 碳纳米管和石墨烯等一维和二维碳材料通过表面修饰和异质原子掺杂, 可以进一步改善催化性能, 特别是在氧还原反应、析氧反应和析氢反应等重要电催化反应中. 此外还重点讨论了碳基材料在双功能和三功能催化中的应用, 特别是在氧还原反应与析氧反应的双功能催化, 以及析氧反应与析氢反应的三功能催化方面的进展. 通过合理设计多功能催化剂, 能够实现电催化过程的高效性和经济性, 为未来的能源转换和存储技术提供了新的解决思路. 最后, 本文还提出了未来研究的方向, 包括精确调节碳基材料的功能化策略、发展可再生碳材料、采用先进表征技术以及促进智能制造和响应性催化等方面的展望. 这些方向的研究不仅能提升碳基催化剂的性能, 也能推动绿色能源技术的发展.

综上, 本文全面回顾了碳基材料在电催化领域的最新研究进展, 突出了其结构设计、电子工程和功能化改性对催化性能的影响, 旨在为碳基电催化材料的开发与应用提供理论依据和技术指导.

关键词: 碳材料, 功能化, 电催化

Abstract:

abstract:Functional carbon-based materials have become a key research direction in the field of advanced electrocatalysis due to their unique structure and properties. Various strategies have been proposed to design and synthesize high-performance carbon-based electrocatalysts. In this review, we comprehensively summarize the latest developments in carbon-based materials for advanced electrocatalysis, with particular emphasis on the structure design strategies and the intrinsic relationship between structure, activity, and performance. The functionalization of multi-dimensional carbon-based materials with enhanced electrocatalytic performance is first addressed. Next, the impact of electronic and structural engineering on the performance of carbon-based materials for electrocatalysis is discussed in terms of the advantages of different types of carbon-based materials in electrocatalytic applications. Finally, the prospects in areas such as precise tuning of functional carbon-based materials, the development of renewable carbon materials, the use of advanced characterization techniques and the promotion of smart manufacturing and responsiveness are highlighted.

Key words: Carbon materials, Functionalization, Electrocatalysis

翁应龙, 张建平, 张坤, 路亦通, 黄婷婷, 康英博, 韩晓彤, 邱介山. 先进电催化功能碳基材料研究新进展[J]. 催化学报, 2025, 76: 10-36.

Yinglong Weng, Jianping Zhang, Kun Zhang, Yitong Lu, Tingting Huang, Yingbo Kang, Xiaotong Han, Jieshan Qiu. Recent progress in functional carbon-based materials for advanced electrocatalysis[J]. Chinese Journal of Catalysis, 2025, 76: 10-36.

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Fig. 1. (A) Main gaps in existence between doing fundamental research and making practical applications of carbon-based materials for advanced electrocatalysis. Configurations of water electrolyzer (B), fuel cell (C), biomass oxidation coupled water electrolyzer (D).

Fig. 2. Multi-dimensional carbon supports. (A1) Schematic illustration of CQDs confining Zn and Cu species. TEM image of ZnCu-CQDs. Structure model of an active metal dopant from ZnCu-CQDs. Reproduced with permission from Ref. [23]. Copyright 2018, American Chemical Society. (A2) The schematic diagram for the surface grafting of CQDs. Reproduced with permission from Ref. [17]. Copyright 2015, Elsevier B.V. (B1) Schematic illustration for the preparation of CNRs. TEM images of pristine CNTs and CNRs. Reproduced with permission from Ref. [21]. Copyright 2015, Wiley-VCH. (B2) TEM images of carbon nanorods encapsulated cobalt nanoparticles. Reproduced with permission from Ref. [24]. Copyright 2016, Elsevier. (C1) Schematic illustration of the few-layer graphene sheets with the anchoring of Ni single atom. SEM and TEM images of the as-exfoliated graphite foil. Reproduced with permission from Ref. [19]. Copyright 2020, American Chemical Society. (C2) SEM and TEM images of the NiCo2O4 grown on the polyaniline modified graphene surface. Reproduced with permission from Ref. [18]. Copyright 2016, American Chemical Society. (D1) SEM and TEM images of TiO2 on carbon nanofibers. Reproduced with permission from Ref. [25]. Copyright 2013, Wiley-VCH. (D2) Schematic illustration of the superhydro philic “nanoglue” stabilizing guest nanomaterials in a vertical orientation onto carbon cloth, SEM images of the functionalized carbon cloth without and with guest nanomaterials. Reproduced with permission from Ref. [26]. Copyright 2017, The Royal Society of Chemistry.

Fig. 3. (A) Position of the heteroatoms of interest in the periodic table and electron arrangement, electronegativity, and atomic size of the heteroatoms. (B) Comparison of the electronic states, active sites, and activation energies between BPC and NPC. (C) Solid-state 31P NMR spectra. (D) TDOS plots of the BPC. (E) DFT studies on the catalytic reaction mechanism of the oxidation of BA. Reproduced with permission from Ref. [47]. Copyright 2022, Wiley-VCH.

Fig. 4. (A) Schematic illustration of the synthetic procedure of CBNO. HR-TEM image (B) and fast Fourier transform pattern (C) of CBNO. The blue and yellow areas respectively represent h-BN and graphene, forming a heterojunction. (D) Schematic configuration models of representative CBNO fragments. The carbon, nitrogen, boron, and oxygen atoms are represented by gray, blue, pink, and red spheres. (E) Tafel plots of CBNO, CBN, CNO, CBO, and AC. Reproduced with permission from Ref. [54]. Copyright 2023, Wiley-VCH. (F) Schematic diagram of the two-layer stacking model in cell units. (G) Schematic illustration of the synthetic procedure of SWNTs. (H) SEM image of the dried hydrogel of poly (acrylic acid) containing pyridine-modified SWNTs. Reproduced with permission from Ref. [59]. Copyright 2010, American Chemical Society.

Fig. 5. (A) Illustration of the synthesis route of CoNG-MC. (B) The proposed mechanism for nonradical phenol oxidation on CoNG-MC. (C) Comparation of PMS dosages and specific activity (k/mPMS) for different catalysts. (D) The crystal field splitting of d orbitals in octahedron structure and electronic arrangement of Co3+ in different orbitals under CoNG-C and CoNG-MC. (E) Dark green represents electron-acquiring capability and purple represents electron-supplying capability. (F) Temperature-dependent inverse susceptibilities fitted by the Curie-Weiss law for CoNG-MC and CoNG-C. Reproduced with permission from Ref. [70]. Copyright 2024, Wiley-VCH. (G) Bader charge and differential charge density of a Ag55 cluster supported on defective graphene Ag55/d-C. (H) CO2RR. (I) HER on Ag55/d-C. Reproduced with permission from Ref. [66]. Copyright 2023, American Chemical Society.

Fig. 6. (A) The active edge sites of multi-walled carbon nanotubes and the mechanism of heteroatom doping on ORR. (B) TEM images of unzipped MWCNTs with incremental unzipping degree. Reproduced with permission from Ref. [73]. Copyright 2019, Elsevier B.V. (C) Oxygen reduction reaction/oxygen evolution reaction (ORR/OER) catalytic activities. (D) Schematic of the X-doped graphene nanoribbons, showing the possible positions ofdopants. (E) Measured limiting current density from the LSV curves, normalized by Pt/C electrode current density at 0.5 V (SCE, saturated calomel electrode) under the same conditions in the same experiment, and the predictions. (F) Fluorine doped graphene sheets. (G) Free energy diagram of X-doped graphene nanoribbons with the best catalytic performance at the equilibrium potential (U0 = 0.402 V) for ORR in alkaline medium. Repro duced with permission from Ref. [74]. Copyright 2015, Wiley-VCH.

Fig. 7. (A) Illustration of sample preparations for vacancy-free N-doped graphene upon mild nitrogen plasma, vacancy-rich graphene upon strong nitrogen plasma, and vacancy-rich graphene without nitrogen dopants upon argon plasma. (B) Mechanistic diagram of N-doped graphene containing vacancy defects. (C) Current density for N-doped graphene, N-doped graphene containing vacancy defects, and graphene containing vacancy defects at the voltage of −0.2, −0.1, 0, 0.1, and 0.2 V, obtained from the LSV curves, vs the corresponding defect distance Ld. Reproduced with permission fromRef. [78]. Copyright 2024, American Chemical Society. (D) E1/2 of different sp3-hybridized carbon content. (E) sp3-hybridized carbon content versus power density. (F) LSV curves (5 mV s−1 and 1600 rpm). (G) Difference in charge density and Bader charge analysis of oxygenated intermediates in the AB-N-P models during ORR. Reproduced with permission from Ref. [80]. Copyright 2023, Elsevier B.V. (H,I) SEM images of NSHOPC. TEM image (J) and scanning TEM image and corresponding elemental maps (K) of NSHOPC. (L) Polarization curves of catalysts in 0.1 mol L−1 KOH at 1600 rpm. Reproduced with permission from Ref. [81]. Copyright 2023, Elsevier B.V.

Fig. 8. (A) Illustration of the synthetic route to the preparation of biomass-derived N-self-doped defect-rich porous carbon nanosheets. (B) and (C) TEM and SEM of KOH-II ABC nanosheets. Reproduced with permission from Ref. [85]. Copyright 2023, Elsevier B.V. (D) Comparison of the Gibbs free energy of formation after corrosion, accompanied by the removal of one carbon atom, for each carbon structure. (E) Proposed reaction pathways of electrochemical carbon corrosion obtained from DFT calculations. (F) Stability of the MEAs containing NiFe/C and NiFe electrocatalysts at 80 °C under a constant current density of 200 mA cm-2. Reproduced with permission from Ref. [86]. Copyright 2024, American Chemical Society.

Fig. 9. (A) Schematic illustration for the synthesis of NiW-CNT/PC/CC. (B) LSV curves. Reproduced with permission from Ref. [92]. Copyright 2021, Wiley-VCH. (C,D) The H+ concentration of Mo2C and CD@Mo2C. (E) TDOS of Mo2C and CD@Mo2C. (F) Charge-density distribution of CD@Mo2C. Reproduced with permission from Ref. [93]. Copyright 2024, Elsevier B.V. (G,H) SEM and TEM images of CoP/N-CNT/CC. Raman spectra of the N-CNT/CC irradiated at 532 nm with the increasing (I) and decreasing (J) laser power, respectively. Reproduced with permission from Ref. [94]. Copyright 2021, Elsevier B.V.

Fig. 10. (A) Synthetic procedure of FePc@N,P-DC catalyst. (B) LSV curves of ORR in O2-saturated 0.1 mol L-1 KOH at 1600?rpm for different catalysts. Inset is amplifying picture at onset potential. (C) ORR polarization LSV of FePc@N,P-DC measurement before and after 5000 and 10000 cycles at the scan rate of 50?mV s-1 with the rotation speed of 1600?rpm. Reproduced with permission from Ref. [99]. Copyright 2019, Elsevier B.V. (D) LSV curves of different catalysts for both ORR and OER in 0.1 mol L-1 KOH at 1600?rpm (scan rate: 5?mV s-1). (E) Polarization and power density curves of the liquid ZABs using FePc@N,P-DC and Pt/C catalysts. (F) ORR polarization curves. (G) OER polarization curves. (H) TEM image of CoFe-FeNC. (I) HR-TEM image of CoFe-FeNC. (J) Absorbate evolution mechanism for ORR/OER on Fe-N-C active site. (K) Projected density of state. Reproduced with permission from Ref. [100]. Copyright 2019, Elsevier B.V.

Fig. 11. (A) HR-TEM image of ZnCoNi/(Ppy/CNTs)4. (B) The charge density distribution illustrates the change in electron distribution. (C) Free energy diagrams at the U of 1.23 V. Reproduced with permission from Ref. [101]. Copyright 2022, Elsevier B.V. (D) LSV curves for HER. (E) Schematic illustration of hydrogen generation processes on P-NiSe2 in 1 mol L-1 KOH. (F) Calculated water dissociation energy and hydrogen adsorption free energy during alkaline-HER process on NiSe2 and P-NiSe2. Reproduced with permission from Ref. [102]. Copyright 2022, Elsevier B.V.

Fig. 12. (A) AFM images of NCN-1000-5. (B) Doped graphene monolayer and doped graphene nanoribbons. (C) The volcano plot for the ORR and OER by plotting the overpotential as a function of ΔG(*O) at various possible active sites, The top and side views of the active site. Reproduced with permission from Ref. [105]. Copyright 2014, Royal Society of Chemistry. (D) LSV curves of C-1000, NCN-800-5, NCN-900-5, NCN-1000-1, NCN-1000-2.5, NCN-1000-5, RuO2 and IrO2 in O2-saturated 0.1 mol L-1 KOH electrolyte (1600 rpm, 5 mV s−1). (E) The overall LSV curves for the ORR and OER of various catalysts at 1600 rpm. (F) HER polarization curves of Co/NC, Fe3C/NC, Fe3C-Co/NC, and Pt/C in 0.5 mol L-1 H2SO4. (G) OER polarization curves of Co/NC, Fe3C/NC, Fe3C-Co/NC, and RuO2 in 1 mol L-1 KOH. (H) RRDE voltammograms of Co/NC, Fe3C/NC, Fe3C-Co/NC, and Pt/C. (I) TEM images of Fe3C-Co/NC. (J) Schematic presentation of the bond length around C-N6 sites on Fe3C-Co/NC. (K) Relative energy diagram for ORR on C-N6 sites on Fe3C-Co/NC and NC. Reproduced with permission from Ref. [106]. Copyright 2019, Wiley-VCH.

Fig. 13. (A) Possible reaction pathways for the electrochemical oxidation of glycerol to various value-added products in alkaline solution. (B) SEM images of the cobalt-based spinel oxide (MCo2O4, M = Mn, Fe, Co, Ni, Cu, and Zn) nanostructures. (C) General crystal structure of MCo2O4 spinel oxides. (D) XRD patterns of MCo2O4 arrays on three-dimensional carbon fiber paper support. (E) The intrinsic glycerol electrooxidation activity trend within the series of MCo2O4 catalysts (in the order of increasing atomic number of M from left to right). (F) Concentrations of glycerol and its oxidation products as a function of the total charge passed after the glycerol electrooxidation using CuCo2O4 as electrocatalyst at 1.30 V vs. RHE at pH = 13 in 0.1 mol L-1 KOH solution containing 0.1 mol L-1 glycerol. Reproduced with permission from Ref. [20]. Copyright 2020, American Chemical Society.

Fig. 14. (A) Possible reaction pathways for the electrochemical oxidation of HMF to various value-added products in alkaline solution. (B) SEM image of the NiFe LDH nanosheets on 3D carbon fiber paper. (C) Schematic diagram of the electrochemical cell used for HMF electrooxidation. (D) Polarization curves of the NiFe-LDH nanosheets and pristine carbon fiber paper in 1 mol L-1 of KOH with and without 10 mmol L-1 of HMF. (E) The capacitive currents at 0.975 V vs. RHE as a function of scan rate for NiFe LDH with and without HMF. (F) Concentration changes of HMF and its oxidation products with the time of chronoamperometric tests at 1.33 V vs. RHE using NiFe LDH as electrocatalyst. (G) HMF concentration changes during four successive cycles using NiFe LDH as electrocatalyst. Reproduced with permission from Ref. [117]. Copyright 2018, American Chemical Society.

Fig. 15. (A) The proposed reaction pathways for CO2RR on Ni-N4-C doped graphene. (B) TEM image of the NiSAs@?3D-INCT. (C) Fourier transformed curves of Ni K-edge EXAFS spectra. (D) Steady-state polarization curves. Reproduced with permission from Ref. [120]. Copyright 2023, Elsevier B.V. (E) Aberration-corrected HAADF-STEM image of D-FeN/C. (F) XANES spectra of Fe K-edge for Fe foil, Fe2O3, FePc, and D-FeN/C. (G) FE values and NH3 yields. (H) calculated partial current densities of D-FeN/C, FeN/C, and D-N/C at given potentials. (I) Diagram of the alternative pathway on D-FeN4-C sites. Reproduced with permission from Ref. [121]. Copyright 2022, Wiley-VCH.

Fig. 16. (A) Illustration of the intercalation of secondary species into the layered graphite structure via the staging mechanism according to Rüdorff-Hofmann (RH) theory (top pathway) and Daumas-Herold theory (bottom pathway). Reproduced with permission from Ref. [122]. Copyright 2014, Royal Society of Chemistry. (B) Schematic illustration for the coexistence of two types. (C) The three main end products (pyro-gases, bio-oils (liquid), and biocarbons (solid)) obtained from thermochemical conversion process of different organic waste biomass and the current important applications for biocarbon. Reproduced with permission from Ref. [123]. Copyright 2023, Elsevier B.V. (D) Schematic representation of the workflow for the guided setup of ML frameworks toward electrocatalyst discovery from theoretical and experimental feed data. Reproduced with permission from Ref. [91]. Copyright 2019, Wiley-VCH. (E) 4D-STEM experiment. Reproduced with permission from Ref. [124]. Copyright 2021, American Chemical Society. (F) The diagram of operando in-situ Raman device. Reproduced with permission from Ref. [125]. Copyright 2024, Elsevier B.V. (G) Dynamic electron microscopy STEM/TEM observations. Reproduced with permission from Ref. [126]. Copyright 2025, Elsevier B.V. (H) Direct patterning of carbon nanotube aerosols for high-performance flexible electronics. Reproduced with permission from Ref. [127]. Copyright 2025, Elsevier B.V.

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先进电催化功能碳基材料研究新进展

Recent progress in functional carbon-based materials for advanced electrocatalysis

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