Citation: Mingliang Wu, Yehui Zhang, Zhanzhao Fu, Zhiyang Lyu, Qiang Li, Jinlan Wang. Structure-Activity Relationship of Atomic-Scale Cobalt-Based N-C Catalysts in the Oxygen Evolution Reaction[J]. Acta Physico-Chimica Sinica, ;2023, 39(1): 220700. doi: 10.3866/PKU.WHXB202207007 shu

Structure-Activity Relationship of Atomic-Scale Cobalt-Based N-C Catalysts in the Oxygen Evolution Reaction

1.
School of Physics, Southeast University, Nanjing, 211189, China
2.
Jiangsu Key Laboratory for Design and Manufacture of Micro-Nano Biomedical Instruments, School of Mechanical Engineering, Southeast University, Nanjing 211189, China

Corresponding author: Qiang Li, qiang.li@seu.edu.cn Jinlan Wang, jlwang@seu.edu.cn
Received Date: 5 July 2022
Revised Date: 31 July 2022
Accepted Date: 31 July 2022
Available Online: 9 August 2022
Fund Project: the National Key Research and Development Program of China 2021YFA1500700National Natural Science Foundation of China 22033002National Natural Science Foundation of China 22173018

Understanding the origin of the active site activity in the oxygen evolution reaction (OER) electrocatalysts is key for developing efficient electrocatalysts. However, crucial challenges remain due to the complexity of catalyst structure-activity relationships. Herein, various Co-N-C configurations, including single atoms, diatoms, and clusters, were designed to establish structure-activity relationships by first-principles calculations. It was revealed that the Co-N₄ exhibited the best reactivity due to the high coordination number of the metal center and moderate adsorption energies for all reaction intermediates. The diatom and cluster activities originate from the highly coordinated structures formed with reaction intermediates, which serve as coordination ligands. Furthermore, other factors influencing the OER activity based on the Co-N₄ configuration are discussed. For example, the weak metal-metal interaction can further optimize the adsorption of oxygen-containing intermediates by tuning antibonding energy levels of Co-O. Subsequently, an ultralow overpotential of 0.23 V for the OER in CoNi-type4 systems can be obtained by extrapolation of the volcano plot derived from the established structure-adsorption-activity relationships. This work uncovers the underlying OER activity mechanisms of Co-N-C catalysts, which helps to further understanding of high-performance of M-N-C base catalysts and will aid in the future design of high-efficiency OER catalysts.
- Electrocatalysis,
- Oxygen evolution reaction,
- First-principles calculations,
- Structure-activity relationship,
- Weak metal-metal interaction
1. [1]
  Li, Y.; Wang, H.; Priest, C.; Li, S.; Xu, P.; Wu, G. Adv. Mater. 2021, 33, e2000381. doi: 10.1002/adma.202000381 doi: 10.1002/adma.202000381
2. [2]
  Seh, Z. W.; Kibsgaard, J.; Dickens, C. F.; Chorkendorff, I.; Norskov, J. K.; Jaramillo, T. F. Science 2017, 355, eaad4998. doi: 10.1126/science.aad4998 doi: 10.1126/science.aad4998
3. [3]
  Ding, Y.; Cai, P.; Wen, Z. Chem. Soc. Rev. 2021, 50, 1495. doi: 10.1039/d0cs01239d doi: 10.1039/d0cs01239d
4. [4]
  Yan, Z.; Hitt, J. L.; Turner, J. A.; Mallouk, T. E. Proc. Natl. Acad. Sci. USA 2020, 117, 12558. doi: 10.1073/pnas.1821686116 doi: 10.1073/pnas.1821686116
5. [5]
  Wang, J.; Cui, W.; Liu, Q.; Xing, Z.; Asiri, A. M.; Sun, X. Adv. Mater. 2016, 28, 215. doi: 10.1002/adma.201502696 doi: 10.1002/adma.201502696
6. [6]
  Song, J.; Wei, C.; Huang, Z. -F.; Liu, C.; Zeng, L.; Wang, X.; Xu, Z. J. Chem. Soc. Rev. 2020, 49, 2196. doi: 10.1039/c9cs00607a doi: 10.1039/c9cs00607a
7. [7]
  Xia, B. Y.; Yan, Y.; Li, N.; Wu, H. B.; Lou, X. W.; Wang, X. Nat. Energy 2016, 1, 15006. doi: 10.1038/nenergy.2015.6 doi: 10.1038/nenergy.2015.6
8. [8]
  Zhang, L.; Jia, Y.; Gao, G.; Yan, X.; Chen, N.; Chen, J.; Soo, M. T.; Wood, B.; Yang, D.; Du, A.; et al. Chem 2018, 4, 285. doi: 10.1016/j.chempr.2017.12.005 doi: 10.1016/j.chempr.2017.12.005
9. [9]
  Zhao, C. X.; Liu, J. N.; Wang, J.; Ren, D.; Li, B. Q.; Zhang, Q. Chem. Soc. Rev. 2021, 50, 7745. doi: 10.1039/d1cs00135c doi: 10.1039/d1cs00135c
10. [10]
  Zhang, W.; Cao, R. Chem 2021, 7, 1981. doi: 10.1016/j.chempr.2021.07.012 doi: 10.1016/j.chempr.2021.07.012
11. [11]
  Zhang, J. -Y.; Yan, Y.; Mei, B.; Qi, R.; He, T.; Wang, Z.; Fang, W.; Zaman, S.; Su, Y.; Ding, S.; et al. Energy Environ. Sci. 2021, 14, 365. doi: 10.1039/d0ee03500a doi: 10.1039/d0ee03500a
12. [12]
  Fei, H.; Dong, J.; Feng, Y.; Allen, C. S.; Wan, C.; Volosskiy, B.; Li, M.; Zhao, Z.; Wang, Y.; Sun, H.; et al. Nat. Catal. 2018, 1, 63. doi: 10.1038/s41929-017-0008-y doi: 10.1038/s41929-017-0008-y
13. [13]
  Liu, J.; Xiao, J.; Luo, B.; Tian, E.; Waterhouse, G. I. N. Chem. Eng. J. 2022, 427, 132038. doi: 10.1016/j.cej.2021.131686 doi: 10.1016/j.cej.2021.131686
14. [14]
  Zhao, C. X.; Li, B. Q.; Liu, J. N.; Zhang, Q. Angew. Chem. Int. Ed. 2021, 60, 4448. doi: 10.1002/anie.202003917 doi: 10.1002/anie.202003917
15. [15]
  Li, X.; Yang, X.; Liu, L.; Zhao, H.; Li, Y.; Zhu, H.; Chen, Y.; Guo, S.; Liu, Y.; Tan, Q.; Wu, G. ACS Catal. 2021, 11, 7450. doi: 10.1021/acscatal.0c05446 doi: 10.1021/acscatal.0c05446
16. [16]
  Wu, Y. -J.; Wu, X. -H.; Tu, T. -X.; Zhang, P. -F.; Li, J. -T.; Zhou, Y.; Huang, L.; Sun, S. -G. Appl. Catal. B Environ. 2020, 278, 119259. doi: 10.1016/j.apcatb.2020.119259 doi: 10.1016/j.apcatb.2020.119259
17. [17]
  Ban, J. J.; Wen, X. H.; Xu, H. J.; Wang, Z.; Liu, X. H.; Cao, G. Q.; Shao, G. S.; Hu, J. H. Adv. Funct. Mater. 2021, 31, 2010472. doi: 10.1002/adfm.202010472 doi: 10.1002/adfm.202010472
18. [18]
  Huang, Q. E.; Wang, B.; Ye, S.; Liu, H.; Chi, H.; Liu, X.; Fan, H.; Li, M.; Ding, C.; Li, Z.; et al. ACS Catal. 2021, 12, 491. doi: 10.1021/acscatal.1c04644. doi: 10.1021/acscatal.1c04644
19. [19]
  Li, X. Y.; Rong, H. P.; Zhang, J. T.; Wang, D. S.; Li, Y. D. Nano Res. 2020, 13, 1842. doi: 10.1007/s12274-020-2755-3 doi: 10.1007/s12274-020-2755-3
20. [20]
  Liu, J. ACS Catal. 2016, 7, 34. doi: 10.1021/acscatal.6b01534 doi: 10.1021/acscatal.6b01534
21. [21]
  Zhang, Q.; Duan, Z.; Li, M.; Guan, J. Chem. Commun. 2020, 56, 794. doi: 10.1039/c9cc09007j doi: 10.1039/c9cc09007j
22. [22]
  Xu, H.; Cheng, D.; Cao, D.; Zeng, X. C. Nat. Catal. 2018, 1, 339. doi: 10.1038/s41929-018-0063-z doi: 10.1038/s41929-018-0063-z
23. [23]
  Lu, J.; Zeng, Y.; Ma, X.; Wang, H.; Gao, L.; Zhong, H.; Meng, Q. Polymers 2019, 11, 828. doi: 10.3390/polym11050828 doi: 10.3390/polym11050828
24. [24]
  Wang, J.; Huang, Z.; Liu, W.; Chang, C.; Tang, H.; Li, Z.; Chen, W.; Jia, C.; Yao, T.; Wei, S.; et al. J. Am. Chem. Soc. 2017, 139, 17281. doi: 10.1021/jacs.7b10385 doi: 10.1021/jacs.7b10385
25. [25]
  Zhang, L.; Fischer, J.; Jia, Y.; Yan, X.; Xu, W.; Wang, X.; Chen, J.; Yang, D.; Liu, H.; Zhuang, L.; et al. J. Am. Chem. Soc. 2018, 140, 10757. doi: 10.1021/jacs.8b04647 doi: 10.1021/jacs.8b04647
26. [26]
  Zhou, Y.; Yang, W.; Utetiwabo, W.; Lian, Y. M.; Yin, X.; Zhou, L.; Yu, P.; Chen, R.; Sun, S. J. Phys. Chem. Lett. 2020, 11, 1404. doi: 10.1021/acs.jpclett.9b03771 doi: 10.1021/acs.jpclett.9b03771
27. [27]
  Kresse, G.; Hafner, J. Phys. Rev. B 1993, 48, 13115. doi: 10.1103/PhysRevB.48.13115 doi: 10.1103/PhysRevB.48.13115
28. [28]
  Kresse, G.; Furthmüller, J. Phys. Rev. B 1996, 54, 11169. doi: 10.1103/PhysRevB.54.11169 doi: 10.1103/PhysRevB.54.11169
29. [29]
  Kresse, G.; Joubert, D. Phys. Rev. B 1999, 59, 1758-1775. doi: 10.1103/PhysRevB.59.1758 doi: 10.1103/PhysRevB.59.1758
30. [30]
  Perdew, J. P.; Burke, K.; Ernzerhof, M. Phys. Rev. Lett. 1996, 77, 3865. doi: 10.1103/PhysRevLett.77.3865 doi: 10.1103/PhysRevLett.77.3865
31. [31]
  Grimme, S.; Antony, J.; Ehrlich, S.; Krieg, H. J. Chem. Phys. 2010, 132, 154104. doi: 10.1063/1.3382344 doi: 10.1063/1.3382344
32. [32]
  Grimme, S.; Ehrlich, S.; Goerigk, L. J. Comput. Chem. 2011, 32, 1456. doi: 10.1002/jcc.21759 doi: 10.1002/jcc.21759
33. [33]
  Henkelman, G.; Arnaldsson, A.; Jónsson, H. Comput. Mater. Sci. 2006, 36, 354. doi: 10.1016/j.commatsci.2005.04.010 doi: 10.1016/j.commatsci.2005.04.010
34. [34]
  Sanville, E.; Kenny, S. D.; Smith, R.; Henkelman, G. J. Comput. Chem. 2007, 28, 899. doi: 10.1002/jcc.20575 doi: 10.1002/jcc.20575
35. [35]
  Henkelman, G.; Uberuaga, B. P.; Jónsson, H. J. Chem. Phys. 2000, 113, 9901. doi: 10.1063/1.1329672 doi: 10.1063/1.1329672
36. [36]
  Maintz, S.; Deringer, V. L.; Tchougréeff, A. L.; Dronskowski, R. J. Comput. Chem. 2013, 34, 2557. doi: 10.1002/jcc.23424 doi: 10.1002/jcc.23424
37. [37]
  Maintz, S.; Deringer, V. L.; Tchougréeff, A. L.; Dronskowski, R. J. Comput. Chem. 2016, 37, 1030. doi: 10.1002/jcc.24300 doi: 10.1002/jcc.24300
38. [38]
  Hansen, H. A.; Viswanathan, V.; Nørskov, J. K. J. Phys. Chem. C 2014, 118, 6706. doi: 10.1021/jp4100608 doi: 10.1021/jp4100608
39. [39]
  Zhang, X.; Yang, Z.; Lu, Z.; Wang, W. Carbon 2018, 130, 112. doi: 10.1016/j.carbon.2017.12.121 doi: 10.1016/j.carbon.2017.12.121
40. [40]
  Sun, X.; Sun, S.; Gu, S.; Liang, Z.; Zhang, J.; Yang, Y.; Deng, Z.; Wei, P.; Peng, J.; Xu, Y.; et al. Nano Energy 2019, 61, 245. doi: 10.1016/j.nanoen.2019.04.076 doi: 10.1016/j.nanoen.2019.04.076
41. [41]
  Zhao, J.; Zhang, J. -J.; Li, Z. -Y.; Bu, X. -H. Small 2020, 16, 2003916. doi: 10.1002/smll.202003916 doi: 10.1002/smll.202003916
42. [42]
  Vinogradov, I.; Singh, S.; Lyle, H.; Paolino, M.; Mandal, A.; Rossmeisl, J.; Cuk, T. Nat. Mater. 2022, 21, 88. doi: 10.1038/s41563-021-01118-9 doi: 10.1038/s41563-021-01118-9
43. [43]
  Tahir, M.; Pan, L.; Idrees, F.; Zhang, X.; Wang, L.; Zou, J. -J.; Wang, Z. L. Nano Energy 2017, 37, 136. doi: 10.1016/j.nanoen.2017.05.022 doi: 10.1016/j.nanoen.2017.05.022
44. [44]
  Betley, T. A.; Wu, Q.; Van Voorhis, T.; Nocera, D. G. Inorg. Chem. 2008, 47, 1849. doi: 10.1021/ic701972n doi: 10.1021/ic701972n
45. [45]
  He, Y. H.; Guo, H.; Hwang, S.; Yang, X. X.; He, Z. Z.; Braaten, J.; Karakalos, S.; Shan, W. T.; Wang, M. Y.; Zhou, H.; et al. Adv. Mater. 2020, 32, 2003577. doi: 10.1002/adma.202003577 doi: 10.1002/adma.202003577
46. [46]
  Zhang, N.; Zhou, T.; Ge, J.; Lin, Y.; Du, Z.; Zhong, C. A.; Wang, W.; Jiao, Q.; Yuan, R.; Tian, Y.; et al. Matter 2020, 3, 509. doi: 10.1016/j.matt.2020.06.026 doi: 10.1016/j.matt.2020.06.026
47. [47]
  Bajdich, M.; Garcia-Mota, M.; Vojvodic, A.; Norskov, J. K.; Bell, A. T. J. Am. Chem. Soc. 2013, 135, 13521. doi: 10.1021/ja405997s doi: 10.1021/ja405997s
48. [48]
  Qiu, Z.; Tai, C. W.; Niklasson, G. A.; Edvinsson, T. Energy Environ. Sci. 2019, 12, 572. doi: 10.1039/c8ee03282c doi: 10.1039/c8ee03282c
49. [49]
  Mefford, J. T.; Akbashev, A. R.; Kang, M.; Bentley, C. L.; Gent, W. E.; Deng, H. D.; Alsem, D. H.; Yu, Y. S.; Salmon, N. J.; Shapiro, D. A.; et al. Nature 2021, 593, 67. doi: 10.1038/s41586-021-03454-x doi: 10.1038/s41586-021-03454-x
50. [50]
  Suntivich, J.; May, K. J.; Gasteiger, H. A.; Goodenough, J. B.; Shao-Horn, Y. Science 2011, 334, 1383. doi: 10.1126/science.1212858 doi: 10.1126/science.1212858
51. [51]
  Li, Q. K.; Li, X. F.; Zhang, G.; Jiang, J. J. J. Am. Chem. Soc. 2018, 140, 15149. doi: 10.1021/jacs.8b07816 doi: 10.1021/jacs.8b07816
52. [52]
  Jin, Z.; Li, P.; Meng, Y.; Fang, Z.; Xiao, D.; Yu, G. Nat. Catal. 2021, 4, 615. doi: 10.1038/s41929-021-00650-w doi: 10.1038/s41929-021-00650-w
53. [53]
  Li, Z.; Wang, Z.; Xi, S.; Zhao, X.; Sun, T.; Li, J.; Yu, W.; Xu, H.; Herng, T. S.; Hai, X.; et al. ACS Nano 2021, 15, 7105. doi: 10.1021/acsnano.1c00251 doi: 10.1021/acsnano.1c00251
54. [54]
  Exner, K. S. Chem Catal. 2021, 1, 258. doi: 10.1016/j.checat.2021.06.011 doi: 10.1016/j.checat.2021.06.011
55. [55]
  Govindarajan, N.; Koper, M. T. M.; Meijer, E. J.; Calle-Vallejo, F. ACS Catal. 2019, 9, 4218. doi: 10.1021/acscatal.9b00532 doi: 10.1021/acscatal.9b00532
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