Research Progress of Graphene‑Based Catalysts in Electrochemistry
DOI: https://doi.org/10.62517/jiem.202603305
Author(s)
Zhiming Wang
Affiliation(s)
School of Chemistry and Chemical Engineering, Tianjin University of Technology, Tianjin, China
Abstract
The energy crisis and CO₂ emissions caused by excessive fossil fuel consumption urgently need to be addressed. Electrocatalytic technologies (ORR, OER, HER, CO₂RR) are central to clean energy conversion but are limited by high cost and low efficiency. Graphene, owing to its large specific surface area, high electrical conductivity, and tunable surface chemistry, has become an ideal catalyst support. This review systematically summarizes the research progress of graphene‑based catalysts in the above reactions, discusses the advantages and disadvantages of preparation methods such as high‑temperature pyrolysis, microwave, and spray drying, and classifies the structure–activity relationships of noble metal, non‑noble metal, heteroatom‑doped, and three‑dimensional graphene catalysts. Studies show that through defect engineering, heteroatom co‑doping, and morphological design, certain graphene-based catalysts have outperformed commercial Pt/C in terms of functionality and stability, demonstrating kilogram‑scale production potential. The review serves as a guide for the logical creation of high-efficiency electrocatalysts based on graphene.
Keywords
Graphene; Electrocatalysis; Preparation Methods; Oxygen Reduction Reaction; Carbon Dioxide Reduction
References
[1] Chu, S., & Majumdar, A. (2012). Opportunities and challenges for a sustainable energy future. Nature, 488(7411), 294–303.
[2] Gao, M. (2023). Morphology engineering of graphene‑based catalysts for tuning the catalytic performance toward the oxygen reduction reaction (Master’s thesis). Hunan University, Changsha, China.
[3] Wu, Z. L., Wang, C. W., Zhang, X. X., Guo, Q. G., & Wang, J. Y. (2024). Graphene‑based CO₂ reduction electrocatalysts: A review. New Carbon Materials, 39(1), 100–130.
[4] Du, Y. D., Meng, X. T., Wang, Z., Zhao, X., & Qiu, J. S. (2022). Graphene‑based catalysts for CO₂ electroreduction. Acta Physico‑Chimica Sinica, 38(2), 2101009.
[5] Yan, R., Wang, K., Wang, C. W., Guo, Q. G., & Wang, J. Z. (2020). A review of graphene‑based catalysts for oxygen reduction reaction. New Carbon Materials, 35(5), 508–514.
[6] Chen, S., Sun, L. Z., Shu, X. X., & Zhang, J. T. (2018). Graphene‑based catalysts for efficient electrocatalytic applications. Chinese Journal of Applied Chemistry, 35(3), 272–285.
[7] Mou, K., Chen, Z., Zhang, X., et al. (2019). Highly efficient electroreduction of CO₂ on nickel single‑atom catalysts: Atom trapping and nitrogen anchoring. Small, 15(49), 1903668.
[8] Li, X., Chai, G., Xu, X., et al. (2020). Electrocatalytic reduction of CO₂ to CO over iron phthalocyanine‑modified graphene nanocomposites. Carbon, 167, 658–667.
[9] Chen, L. L., & Zhao, Z. H. (2025). Research progress in graphene catalyst carriers for fuel cells. Contemporary Chemical Industry, 54(9), 2196–2200.
[10] Wang, J., Huang, X., Xi, S., et al. (2019). Linkage effect in the heterogenization of cobalt complexes by doped graphene for electrocatalytic CO₂ reduction. Angewandte Chemie International Edition, 58(38), 13532–13539.
[11] Liu, X. J., Wang, J., Liu, J., Mao, H. S., Han, W. J., & Li, W. (2026). Application and challenges of graphene‑based catalysts in vanadium redox flow batteries. Fine Chemicals. Advance online publication.
[12] Wu, J., Liu, M., Sharma, P. P., et al. (2016). Incorporation of nitrogen defects for efficient reduction of CO₂ via two‑electron pathway on three‑dimensional graphene foam. Nano Letters, 16(1), 466–470.
[13] Cheng, Y., Zhao, S., Li, H., et al. (2019). Unsaturated edge‑anchored Ni single atoms on porous microwave exfoliated graphene oxide for electrochemical CO₂ reduction. Applied Catalysis B: Environmental, 243, 294–303.
[14] Zhang, H., Wang, H., Jia, S., et al. (2022). CoN₄ active sites in a graphene matrix for the highly efficient electrocatalysis of CO₂ reduction. New Carbon Materials, 37(4), 732–733.
[15] Wang, Y., Wang, D. S., & Li, Y. (2021). A fundamental comprehension and recent progress in advanced Pt‑based ORR nanocatalysts. SmartMat, 2(1), 56–75.
[16] Meng, X. H., Guo, R. H., Tian, X., Huang, Y. R., Guan, L. L., & Zhang, G. F. (2025). Preparation and electrocatalytic performance of graphene‑supported Pt‑Co high‑efficiency catalyst. Chinese Journal of Rare Metals, 49(7), 1011–1021.
[17] Liu, Y. H. (2021). Theoretical study on the hydrogen oxidation activity of graphene‑supported non‑noble metal catalysts (Master’s thesis). China University of Petroleum (East China), Qingdao, China.
[18] Guo, S., Wen, D., Zhai, Y., et al. (2010). Platinum nanoparticle ensemble‑on‑graphene hybrid nanosheet: One‑pot, rapid synthesis, and used as new electrode material for electrochemical sensing. ACS Nano, 4(7), 3959–3968.
[19] Zheng, Y., Qiao, J., Yuan, J., et al. (2018). One‑pot synthesis of a PtPd dendritic nanocube cage superstructure on graphenes as advanced catalysts for oxygen reduction. Nanotechnology, 29(10), 10LT01.
[20] Fu, T., Huang, J. X., Lai, S. B., et al. (2017). Pt skin coated hollow Ag‑Pt bimetallic nanoparticles with high catalytic activity for oxygen reduction reaction. Journal of Power Sources, 365, 17–25.
[21] Yoo, T. Y., Yoo, J. M., Sinha, A. K., et al. (2020). Direct synthesis of intermetallic platinum‑alloy nanoparticles highly loaded on carbon supports for efficient electrocatalysis. Journal of the American Chemical Society, 142(33), 14190–14200.
[22] Yan, Y., Xia, B. Y., Zhao, B., et al. (2016). A review on noble‑metal‑free bifunctional heterogeneous catalysts for overall electrochemical water splitting. Journal of Materials Chemistry A, 4(45), 17587–17603.
[23] Qin, R. J., Zhang, Z. N., & Wang, Y. X. (2017). MoS₂‑Ni₂P nanoparticles supported on graphene as electrocatalyst towards hydrogen evolution reaction. Chemical Industry and Engineering, 34(2), 21–26.
[24]Yuan, F. Y. (2024). Research on the oxygen reduction reaction performance of graphene‑loaded non‑precious metals (Master’s thesis). Hangzhou Dianzi University, Hangzhou, China.
[25] Bayeh, A. W., Ou, Y. Y., Ou, Y. T., et al. (2021). MoO₂‑graphene nanocomposite as an electrocatalyst for high‑performance vanadium redox flow battery. Journal of Energy Storage, 40, 102795.
[26] Yang, M. W. (2024). Design of graphene catalyst based on theoretical calculation and study of tetracycline degradation mechanism (Master’s thesis). North China Electric Power University, Beijing, China.
[27] Liu, S., Yang, H., Huang, X., et al. (2018). Identifying active sites of nitrogen‑doped carbon materials for the CO₂ reduction reaction. Advanced Functional Materials, 28(21), 1800499.
[28] Liu, Z. W., Peng, F., Wang, H. J., et al. (2011). Phosphorus‑doped graphite layers with high electrocatalytic activity for the O₂ reduction in an alkaline medium. Angewandte Chemie International Edition, 50(14), 3257–3261.
[29] Jeon, I. Y., Zhang, S., Zhang, L., et al. (2013). Edge‑selectively sulfurized graphene nanoplatelets as efficient metal‑free electrocatalysts for oxygen reduction reaction: The electron spin effect. Advanced Materials, 25(42), 6138–6145.
[30] Sreekanth, N., Nazrulla, M. A., Vineesh, T. V., Sailaja, K., & Phani, K. L. (2015). Chemical Communications, 51, 16061.
[31] Ding, W., Wei, Z. D., Chen, S. G., et al. (2013). Space‑confinement‑induced synthesis of pyridinic‑ and pyrrolic‑nitrogen‑doped graphene for the catalysis of oxygen reduction. Angewandte Chemie International Edition, 52(45), 11755–11759.
[32] Li, Q., Bai, A. Y., Xue, Z. C., et al. (2020). Nitrogen and sulfur co‑doped graphene composite electrode with high electrocatalytic activity for vanadium redox flow battery application. Electrochimica Acta, 362, 137223.
[33] Zhao, Y., Yuan, Q., Fan, M., et al. (2023). Fabricating pyridinic N‑B sites in porous carbon as efficient metal‑free electrocatalyst in conversion CO₂ into CH₄. Chinese Chemical Letters, 34(8), 108120.
[34] Qu, K. G., Zheng, Y., Dai, S., et al. (2016). Graphene oxide‑polydopamine derived N,S‑codoped carbon nanosheets as superior bifunctional electrocatalysts for oxygen reduction and evolution. Nano Energy, 19, 373–381.
[35] Zhang, J. T., & Dai, L. M. (2016). Nitrogen, phosphorus, and fluorine tri‑doped graphene as a multifunctional catalyst for self‑powered electrochemical water splitting. Angewandte Chemie International Edition, 55(42), 13296–13300.
[36]Liu, Y. N. (2024). Structural design of nitrogen‑doped graphene‑supported metal single atoms and theoretical study on their electroreduction of carbon dioxide (Master’s thesis). Zhejiang University, Hangzhou, China.
[37] Wu, Z. L., Wang, H. B., Meng, X. Q., Wen, H., Zhao, Z. Y., Wang, C. W., Guo, Q. G., Song, Y., & Wang, J. Y. (2025). Simple synthesis of a graphene‑supported bismuth single‑atom catalyst for the improved electrochemical reduction of CO₂. New Carbon Materials, 40(6). (no page numbers)
[38] Zu, X., Li, X., Liu, W., et al. (2019). Efficient and robust carbon dioxide electroreduction enabled by atomically dispersed Snᵟ⁺ sites. Advanced Materials, 31(15), 1808135.
[39] Hu, C., Mu, Y., Bai, S., et al. (2019). Polyvinyl pyrrolidone mediated fabrication of Fe, N‑codoped porous carbon sheets for efficient electrocatalytic CO₂ reduction. Carbon, 153, 609–616.
[40] Zhi, W.‑Y., Liu, Y.‑T., Shan, S.‑L., Jiang, C.‑J., Wang, H., & Lu, J.‑X. (2021). Efficient electroreduction of CO₂ to C₂–C₃ products on Cu/Cu₂O@N‑doped graphene. Journal of CO₂ Utilization, 50, 101594.
[41] Gadipelli, S., Zhao, T., Shevlin, S. A., et al. (2016). Switching effective oxygen reduction and evolution performance by controlled graphitization of a cobalt nitrogen carbon framework system. Energy & Environmental Science, 9(5), 1661–1667.
[42] Gu, H., Shi, G., Zhong, L., et al. (2022). A two‑dimensional van der Waals heterostructure with isolated electron‑deficient cobalt sites toward high‑efficiency CO₂ electroreduction. Journal of the American Chemical Society, 144(47), 21502–21511.
[43] Feng, T., Zhao, X. R., Dong, C. K., et al. (2018). Boosting reversible oxygen electrocatalysis with enhanced interfacial pyridinic‑N‑Co bonding in cobalt oxide/mesoporous N‑doped graphene hybrids. Nanoscale, 10(47), 22140–22147.
[44] Zhang, T. W., Li, T. C., Diao, Q. P., & Luo, W. W. (2024). Synthesis and properties of spinel cobalt iron oxide supported on N‑doped graphene catalysts for oxygen reduction reaction. Journal of Anshan Normal University, 26(6), 37–42.
[45] Bu, D. C., & Zhao, B. (2023). Preparation and electrocatalytic properties of graphene‑supported S‑doped NiFe LDH materials. Guangzhou Chemistry, 48(6), 1–5.
[46] Zhang, X., Zhu, Y., Liu, Z., et al. (2022). Perforated nitrogen‑rich graphene‑like carbon nanolayers supported Cu‑In catalyst for boosting CO₂ electroreduction to CO. Journal of Energy Chemistry, 75, 383–390.
[47] Zeng, L., Shi, J., Luo, J., et al. (2018). Silver sulfide anchored on reduced graphene oxide as a high‑performance catalyst for CO₂ electroreduction. Journal of Power Sources, 398, 83–90.
[48] Tong, Y., Chen, P. Z., Zhou, T. P., et al. (2017). A bifunctional hybrid electrocatalyst for oxygen reduction and evolution: Cobalt oxide nanoparticles strongly coupled to B,N‑decorated graphene. Angewandte Chemie International Edition, 56(25), 7121–7125.
[49] Zhang, T., Li, W., Huang, K., et al. (2021). Regulation of functional groups on graphene quantum dots directs selective CO₂ to CH₄ conversion. Nature Communications, 12(1), 5265.
[50] Yadav, R. M., Li, Z., Zhang, T., et al. (2022). Amine‑functionalized carbon nanodot electrocatalysts converting carbon dioxide to methane. Advanced Materials, 34(2), 2105690.
[51] Wu, J., Ma, S., Sun, J., et al. (2016). A metal‑free electrocatalyst for carbon dioxide reduction to multi‑carbon hydrocarbons and oxygenates. Nature Communications, 7, 13869.
[52] Fu, J., Wang, Y., Liu, J., Huang, K., Chen, Y., Li, Y., & Zhu, J. J. (2018). Graphene quantum dots supported by graphene nanoribbons with ultrahigh electrocatalytic performance for oxygen reduction. ACS Energy Letters, 3, 946.
[53] Xu, F. (2025). The assembly of graphene quantum dots for electrocatalytic oxygen reduction reaction (Master’s thesis). Yangzhou University, Yangzhou, China.
[54] Hu, S. Q., & Li, Z. A. (2023). Facile synthesis of PtCo nanoparticles/three‑dimensional graphene hybrid material as a highly active and stable electrocatalyst for oxygen reduction reaction. Chemical Engineering Journal, 471, 144828.