Citation: Qianqing Xu, Qu Jiang, Haoyue Zhang, Fang Song. Deciphering the active species of anodically activated carbon-based electrocatalysts for oxygen evolution reaction[J]. Chinese Chemical Letters, ;2025, 36(11): 111417. doi: 10.1016/j.cclet.2025.111417 shu

Deciphering the active species of anodically activated carbon-based electrocatalysts for oxygen evolution reaction

State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China

jiangqu@sjtu.edu.cn

songfang@sjtu.edu.cn

Received Date: 18 February 2025
Revised Date: 29 May 2025
Accepted Date: 6 June 2025
Available Online: 6 June 2025

Figures(4)

Metal-free electrocatalysts for the oxygen evolution reaction (OER) are gaining attention for their low cost, high conductivity, and moderate catalytic performance. While trace metal interference in as-synthesized catalysts has been ruled out, the impact of trace metal contamination during electrochemical activation remains unexplored. This study demonstrates that anodic pretreatment in alkaline electrolytes enhances the catalytic performance of carbon cloth. Specifically, carbon cloth activated in 8 mol/L NaOH achieves a current density of 10 mA/cm² with an overpotential of only 338 mV, comparable to metal-based OER catalysts. Electrochemical and spectroscopic analyses show the deposition of FeNiO_xH_y oxyhydroxides (0.19 ± 0.06 µg/cm²) on specific sites of the carbon substrate during activation. These nanoparticles contribute significantly to the catalytic activity, with a synergistic effect between FeNiO_xH_y and the carbon substrate. The turnover frequency (TOF) for Fe correlates with the amount of C=O groups on the carbon substrate, providing evidence for an interfacial synergistic effect. This work emphasizes the importance of considering trace metal effects in metal-free catalyst evaluation and offers insights for the design of more efficient carbon-based hybrid OER catalysts.
- Metal-free electrocatalysts,
- Anodic activation,
- Electrocatalysis,
- Synergistic effect,
- Oxygen evolution reaction,
- Oxygen-containing groups
1. [1]
  S.J. Davis, N.S. Lewis, M. Shaner, et al., Science 360 (2018) eaas9793. doi: 10.1126/science.aas9793
2. [2]
  X. Yang, C.P. Nielsen, S. Song, M.B. McElroy, Nat. Energy 7 (2022) 955–965. doi: 10.1038/s41560-022-01114-6
3. [3]
  J. Lei, Z. Wang, Y. Zhang, et al., Carbon Neutrality 3 (2024) 25. doi: 10.1007/s43979-024-00101-y
4. [4]
  J. Song, C. Wei, Z.F. Huang, et al., Chem. Soc. Rev. 49 (2020) 2196–2214. doi: 10.1039/c9cs00607a
5. [5]
  S.Z. Oener, A. Bergmann, B.R. Cuenya, Nat. Synth. 2 (2023) 817–827. doi: 10.1038/s44160-023-00376-6
6. [6]
  Y. Jiao, Y. Zheng, M.T. Jaroniec, S.Z. Qiao, Chem. Soc. Rev. 44 (2015) 2060–2086. doi: 10.1039/C4CS00470A
7. [7]
  C.G. Morales-Guio, L. Liardet, X. Hu, J. Am. Chem. Soc. 138 (2016) 8946–8957. doi: 10.1021/jacs.6b05196
8. [8]
  N.T. Suen, S.F. Hung, Q. Quan, et al., Chem. Soc. Rev. 46 (2017) 337–365. doi: 10.1039/C6CS00328A
9. [9]
  Y. Zheng, A. Serban, H. Zhang, et al., ACS Energy Lett. 8 (2023) 5018–5024. doi: 10.1021/acsenergylett.3c01866
10. [10]
  Q. Zhang, Y. Hu, H. Wu, et al., ACS Nano 17 (2023) 1485–1494. doi: 10.1021/acsnano.2c10247
11. [11]
  J.J. Duan, S. Chen, M. Jaroniec, S.Z. Qiao, ACS Catal. 5 (2015) 5207–5234. doi: 10.1021/acscatal.5b00991
12. [12]
  X.Y. Lu, W.L. Yim, B.H.R. Suryanto, C. Zhao, J. Am. Chem. Soc. 137 (2015) 2901–2907. doi: 10.1021/ja509879r
13. [13]
  X. Liu, L.M. Dai, Nat. Rev. Mater. 1 (2016) 16064. doi: 10.1038/natrevmats.2016.64
14. [14]
  L.Q. Li, H.B. Yang, J.W. Miao, et al., ACS Energy Lett. 2 (2017) 294–300. doi: 10.1021/acsenergylett.6b00681
15. [15]
  B. Wang, X. Cui, J. Huang, et al., Chin. Chem. Lett. 29 (2018) 1757–1767. doi: 10.1016/j.cclet.2018.11.021
16. [16]
  F. Liu, R. Shi, Z. Wang, et al., Angew. Chem. Int. Ed. 58 (2019) 11791–11795. doi: 10.1002/anie.201906416
17. [17]
  S. Sahani, K. Malika Tripathi, T.Il Lee, et al., Energy Convers. Manag. 252 (2022) 115133. doi: 10.1016/j.enconman.2021.115133
18. [18]
  Z. Zhang, Y. Lei, W. Huang, Chin. Chem. Lett. 33 (2022) 3623–3631. doi: 10.1016/j.cclet.2021.11.041
19. [19]
  X. Ren, H. Liu, J. Wang, J. Yu, Chin. Chem. Lett. 35 (2024) 109282. doi: 10.1016/j.cclet.2023.109282
20. [20]
  L. Lin, Z. Yu, X. Wang, Angew. Chem. Int. Ed. 58 (2019) 6164–6175. doi: 10.1002/anie.201809897
21. [21]
  H. Lin, J. Wu, F. Zhou, et al., J. Environ. Sci. 124 (2023) 570–590. doi: 10.1016/j.jes.2021.11.017
22. [22]
  D.A. Corrigan, J. Electrochem. Soc. 134 (1987) 377. doi: 10.1149/1.2100463
23. [23]
  A. Ambrosi, S.Y. Chee, B. Khezri, et al., Angew. Chem. Int. Ed. 51 (2012) 500–503. doi: 10.1002/anie.201106917
24. [24]
  L. Trotochaud, S.L. Young, J.K. Ranney, S.W. Boettcher, J. Am. Chem. Soc. 136 (2014) 6744–6753. doi: 10.1021/ja502379c
25. [25]
  J. Masa, A.Q. Zhao, W. Xia, et al., Electrochim. Acta 128 (2014) 271–278. doi: 10.1016/j.electacta.2013.11.026
26. [26]
  I. Roger, M.D. Symes, J. Am. Chem. Soc. 137 (2015) 13980–13988. doi: 10.1021/jacs.5b08139
27. [27]
  N.Y. Cheng, Q. Liu, J.Q. Tian, et al., Chem. Commun. 51 (2015) 1616–1619. doi: 10.1039/C4CC07120D
28. [28]
  Y. Zhao, R. Nakamura, K. Kamiya, et al., Nat. Commun. 4 (2013) 2390. doi: 10.1038/ncomms3390
29. [29]
  M. Gong, Y. Li, H. Wang, et al., J. Am. Chem. Soc. 135 (2013) 8452–8455. doi: 10.1021/ja4027715
30. [30]
  H.L. Wang, H.J. Dai, Chem. Soc. Rev. 42 (2013) 3088. doi: 10.1039/c2cs35307e
31. [31]
  X. Long, J.K. Li, S. Xiao, et al., Angew. Chem. Int. Ed. 53 (2014) 7584–7588. doi: 10.1002/anie.201402822
32. [32]
  D. Tang, J. Liu, X.Y. Wu, et al., ACS Appl. Mater. Interfaces 6 (2014) 7918–7925. doi: 10.1021/am501256x
33. [33]
  T.Y. Ma, S. Dai, M. Jaroniec, S.Z. Qiao, J. Am. Chem. Soc. 136 (2014) 13925–13931. doi: 10.1021/ja5082553
34. [34]
  W. Ma, R. Ma, C. Wang, et al., ACS Nano 9 (2015) 1977–1984. doi: 10.1021/nn5069836
35. [35]
  L. Wang, H. Chen, Q.T. Daniel, et al., Adv. Energy Mater. 6 (2016) 1600516. doi: 10.1002/aenm.201600516
36. [36]
  X.J. Cui, P.J. Ren, D.H. Deng, et al., Energy Environ. Sci. 9 (2016) 123–129. doi: 10.1039/C5EE03316K
37. [37]
  Q. Mou, X. Wang, Z. Xu, et al., Chin. Chem. Lett. 33 (2022) 562–566. doi: 10.1016/j.cclet.2021.08.028
38. [38]
  L. Lv, B. Tang, Q. Ji, et al., Chin. Chem. Lett. 34 (2023) 107524. doi: 10.1016/j.cclet.2022.05.038
39. [39]
  C. Wang, K. Zhang, B. Yang, Chin. Chem. Lett. 36 (2025) 110538. doi: 10.1016/j.cclet.2024.110538
40. [40]
  J. Zhang, J. Liu, J. Ran, et al., Chin. Chem. Lett. 36 (2025) 110403. doi: 10.1016/j.cclet.2024.110403
41. [41]
  L. Wang, Y. Yan, R. Li, et al., Chin. Chem. Lett. 35 (2024) 110011. doi: 10.1016/j.cclet.2024.110011
42. [42]
  D. Friebel, M.W. Louie, M. Bajdich, et al., J. Am. Chem. Soc. 137 (2015) 1305–1313. doi: 10.1021/ja511559d
43. [43]
  F. Song, X. Hu, Nat. Commun. 5 (2014) 4477–4485. doi: 10.1038/ncomms5477
44. [44]
  A.S. Batchellor, S.W. Boettcher, ACS Catal. 5 (2015) 6680–6689. doi: 10.1021/acscatal.5b01551
45. [45]
  B.S. Yeo, A.T. Bell, J. Am. Chem. Soc. 133 (2011) 5587–5593. doi: 10.1021/ja200559j
46. [46]
  Y. Gorlin, C.J. Chung, J.D. Benck, et al., J. Am. Chem. Soc. 136 (2014) 4920–4926. doi: 10.1021/ja407581w
47. [47]
  R. Frydendal, M. Busch, N.B. Halck, et al., ChemCatChem 7 (2015) 149–154. doi: 10.1002/cctc.201402756
48. [48]
  Y. Yi, J. Tornow, E. Willinger, et al., ChemElectroChem 2 (2015) 1929–1937. doi: 10.1002/celc.201500268
1. [1]
  Tengjia Ni , Xianbiao Hou , Huanlei Wang , Lei Chu , Shuixing Dai , Minghua Huang . Controllable defect engineering based on cobalt metal-organic framework for boosting oxygen evolution reaction. Chinese Journal of Structural Chemistry, 2024, 43(1): 100210-100210. doi: 10.1016/j.cjsc.2023.100210
2. [2]
  Shaojie Ding , Henan Wang , Xiaojing Dai , Yuru Lv , Xinxin Niu , Ruilian Yin , Fangfang Wu , Wenhui Shi , Wenxian Liu , Xiehong Cao . Mn-modulated Co–N–C oxygen electrocatalysts for robust and temperature-adaptative zinc-air batteries. Chinese Journal of Structural Chemistry, 2024, 43(7): 100302-100302. doi: 10.1016/j.cjsc.2024.100302
3. [3]
  Weibin Shen , Jie Liu , Gongyu Wen , Shuai Li , Binhui Yu , Shuangyu Song , Bojie Gong , Rongyang Zhang , Shibao Liu , Hongpeng Wang , Yao Wang , Yujing Liu , Huadong Yuan , Jianming Luo , Shihui Zou , Xinyong Tao , Jianwei Nai . Formation of FeNi-based nanowire-assembled superstructures with tunable anions for electrocatalytic oxygen evolution reaction. Chinese Chemical Letters, 2025, 36(7): 110184-. doi: 10.1016/j.cclet.2024.110184
4. [4]
  Guan-Nan Xing , Di-Ye Wei , Hua Zhang , Zhong-Qun Tian , Jian-Feng Li . Pd-based nanocatalysts for oxygen reduction reaction: Preparation, performance, and in-situ characterization. Chinese Journal of Structural Chemistry, 2023, 42(11): 100021-100021. doi: 10.1016/j.cjsc.2023.100021
5. [5]
  Lin Zhang , Jianlong Li , Maoyuan Hu , Yao Xu , Xiaoli Xiong , Zhaoyu Jin . MOF-derived beaded stream-like nitrogen and phosphorus-codoped carbon-coated Fe₃O₄ nanocomposites via lattice-oxygen-mediated mechanism for efficient water oxidation. Chinese Chemical Letters, 2025, 36(8): 111123-. doi: 10.1016/j.cclet.2025.111123
6. [6]
  Fenglin Wang , Chengwei Kuang , Zhicheng Zheng , Dan Wu , Hao Wan , Gen Chen , Ning Zhang , Xiaohe Liu , Renzhi Ma . Noble metal clusters substitution in porous Ni substrate renders high mass-specific activities toward oxygen evolution reaction and methanol oxidation reaction. Chinese Chemical Letters, 2025, 36(6): 109989-. doi: 10.1016/j.cclet.2024.109989
7. [7]
  Yanan Zhou , Li Sheng , Lanlan Chen , Wenhua Zhang , Jinlong Yang . Axial coordinated iron-nitrogen-carbon as efficient electrocatalysts for hydrogen evolution and oxygen redox reactions. Chinese Chemical Letters, 2025, 36(1): 109588-. doi: 10.1016/j.cclet.2024.109588
8. [8]
  Jing Cao , Dezheng Zhang , Bianqing Ren , Ping Song , Weilin Xu . Mn incorporated RuO₂ nanocrystals as an efficient and stable bifunctional electrocatalyst for oxygen evolution reaction and hydrogen evolution reaction in acid and alkaline. Chinese Chemical Letters, 2024, 35(10): 109863-. doi: 10.1016/j.cclet.2024.109863
9. [9]
  Jiayu Xu , Meng Li , Baoxia Dong , Ligang Feng . Fully fluorinated hybrid zeolite imidazole/Prussian blue analogs with combined advantages for efficient oxygen evolution reaction. Chinese Chemical Letters, 2024, 35(6): 108798-. doi: 10.1016/j.cclet.2023.108798
10. [10]
  Junan Pan , Xinyi Liu , Huachao Ji , Yanwei Zhu , Yanling Zhuang , Kang Chen , Ning Sun , Yongqi Liu , Yunchao Lei , Kun Wang , Bao Zang , Longlu Wang . The strategies to improve TMDs represented by MoS₂ electrocatalytic oxygen evolution reaction. Chinese Chemical Letters, 2024, 35(11): 109515-. doi: 10.1016/j.cclet.2024.109515
11. [11]
  Genxiang Wang , Linfeng Fan , Peng Wang , Junfeng Wang , Fen Qiao , Zhenhai Wen . Efficient synthesis of nano high-entropy compounds for advanced oxygen evolution reaction. Chinese Chemical Letters, 2025, 36(4): 110498-. doi: 10.1016/j.cclet.2024.110498
12. [12]
  Jiawei Ge , Xian Wang , Heyuan Tian , Hao Wan , Wei Ma , Jiangying Qu , Junjie Ge . Iridium-based catalysts for oxygen evolution reaction in proton exchange membrane water electrolysis. Chinese Chemical Letters, 2025, 36(5): 109906-. doi: 10.1016/j.cclet.2024.109906
13. [13]
  Chupeng Luo , Keying Su , Shan Yang , Yujia Liang , Yawen Tang , Xiaoyu Qiu . Ultrathin NiS₂ nanocages with hierarchical-flexible walls and rich grain boundaries for efficient oxygen evolution reaction. Chinese Chemical Letters, 2025, 36(5): 109940-. doi: 10.1016/j.cclet.2024.109940
14. [14]
  Ming Yue , Yi-Rong Wang , Jia-Yong Weng , Jia-Li Zhang , Da-Yu Chi , Mingjin Shi , Xiao-Gang Hu , Yifa Chen , Shun-Li Li , Ya-Qian Lan . Multi-metal porous crystalline materials for electrocatalysis applications. Chinese Chemical Letters, 2025, 36(6): 110049-. doi: 10.1016/j.cclet.2024.110049
15. [15]
  Xuyun Lu , Yanan Chang , Shasha Wang , Xiaoxuan Li , Jianchun Bao , Ying Liu . Hydrogen peroxide electrosynthesis via two-electron oxygen reduction: From pH effect to device engineering. Chinese Chemical Letters, 2025, 36(5): 110277-. doi: 10.1016/j.cclet.2024.110277
16. [16]
  Yi Zhang , Biao Wang , Chao Hu , Muhammad Humayun , Yaping Huang , Yulin Cao , Mosaad Negem , Yigang Ding , Chundong Wang . Fe–Ni–F electrocatalyst for enhancing reaction kinetics of water oxidation. Chinese Journal of Structural Chemistry, 2024, 43(2): 100243-100243. doi: 10.1016/j.cjsc.2024.100243
17. [17]
  Lanlan Zong , Yuxin Dai , Jiahao Xu , Chaofeng Qiao , Yao Qi , Chengyuan Ma , Hong Li , Xiaobin Pang , Xiaohui Pu . Luteolin and glycyrrhetinic exert cooperative effect on liver cancer by selfassembling into carrier-free nanostructures. Chinese Chemical Letters, 2025, 36(10): 111325-. doi: 10.1016/j.cclet.2025.111325
18. [18]
  Da Yue , Tanglue Feng , Zhicheng Zhu , Mingcheng Zhang , Liyuan Chen , Xiao Han , Haizhu Sun , Bai Yang . Carbonized polymer dots confined active Ru-O sites for boosting electrocatalytic oxygen evolution. Chinese Chemical Letters, 2025, 36(11): 111393-. doi: 10.1016/j.cclet.2025.111393
19. [19]
  Jinqiang Gao , Haifeng Yuan , Xinjuan Du , Feng Dong , Yu Zhou , Shengnan Na , Yanpeng Chen , Mingyu Hu , Mei Hong , Shihe Yang . Methanol steam mediated corrosion engineering towards high-entropy NiFe layered double hydroxide for ultra-stable oxygen evolution. Chinese Chemical Letters, 2025, 36(1): 110232-. doi: 10.1016/j.cclet.2024.110232
20. [20]
  Bin Zhao , Heping Luo , Jiaqing Liu , Sha Chen , Han Xu , Yu Liao , Xue Feng Lu , Yan Qing , Yiqiang Wu . S-doped carbonized wood fiber decorated with sulfide heterojunction-embedded S, N-doped carbon microleaf arrays for efficient high-current-density oxygen evolution. Chinese Chemical Letters, 2025, 36(5): 109919-. doi: 10.1016/j.cclet.2024.109919

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(22)
HTML views(3)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142