Citation: Yaoyu Liu, Yuchen Wang, Biying Liu, Mahmoud Amer, Kai Yan. Cobalt-Vanadium Layered Double Hydroxides Nanosheets as High-Performance Electrocatalysts for Urea Oxidation Reaction[J]. Acta Physico-Chimica Sinica, ;2023, 39(2): 220502. doi: 10.3866/PKU.WHXB202205028 shu

Cobalt-Vanadium Layered Double Hydroxides Nanosheets as High-Performance Electrocatalysts for Urea Oxidation Reaction

Yaoyu Liu ¹ ,
Yuchen Wang ^1,, ,
Biying Liu ¹ ,
Mahmoud Amer ² ,
Kai Yan ^1,,

1.
School of Environmental Science and Engineering, Sun Yat-sen University, Guangzhou 510275, China
2.
Mechanical Engineering Department, Faculty of Engineering, Alexandria University, Alexandria 21544, Egypt

Corresponding author: Yuchen Wang, wangych235@mail.sysu.edu.cn Kai Yan, yank9@mail.sysu.edu.cn
Received Date: 12 May 2022
Revised Date: 6 June 2022
Accepted Date: 9 June 2022
Available Online: 6 July 2022
Fund Project: the National Natural Science Foundation of China 22078374the National Key R & D Program of China 2020YFC1807600the Key-Area Research and Development Program of Guangdong Province 2019B110209003the Guangdong Basic and Applied Basic Research Foundation 2019B1515120058the Scientific and Technological Planning Project of Guangzhou 202206010145

Hydrogen is considered as a desirable clean energy source for supporting human life in the future. Electrochemical water splitting is a promising method for generating carbon-free hydrogen. However, the relatively high overpotential of anodic oxygen evolution reaction (OER) is the main obstacle hindering the widespread popularity of water electrocatalysis technology. Recently, urea oxidation reaction (UOR) has gained significant attention as a potential alternative to OER for hydrogen production since the equilibrium potential of UOR is 0.86 V lower than that of OER. Transition metal-based layered double hydroxides (TM-LDHs) have been explored as promising UOR electrocatalysts, with the advantages of diversified metal species, stable two-dimensional layered structure and exchangeability of interlayer anions. To date, most studies have focused on TM-LDHs of late transition metals (e.g., Ni, Co, and Fe). In this work, by combining early and late transition metals, CoV-LDHs nanosheets were fabricated via a simple one-step coprecipitation method as high-performance UOR electrocatalysts. Additionally, cobalt hydroxide (Co(OH)₂), with a similar lamellar structure, was synthesized via the same method. When compared with Co(OH)₂, CoV-LDHs nanosheets exhibited better UOR performance owing to the following advantages: 1) The nanosheet structure of the as-fabricated CoV-LDHs electrocatalyst exposed a high number of active sites for the electrocatalytic conversion of urea. 2) The introduction of V enhanced the wettability of the CoV-LDHs electrocatalyst; thus, increasing its intrinsic electrocatalytic kinetics. 3) The d-electron compensation effect between Co (3d⁷4s²) and V (3d³4s²) was conducive to promoting the adsorption of urea. Therefore, the CoV-LDHs electrocatalyst exhibited a low electrochemical potential (1.52 V vs. the reversible hydrogen electrode, RHE) to achieve a current density of 10 mA∙cm⁻² in 1 mol∙L⁻¹ of potassium hydroxide containing 0.33 mol∙L⁻¹ urea, which was 70 mV less than that of Co(OH)₂. The Tafel slope value of the CoV-LDHs electrocatalyst (99.9 mV∙dec⁻¹) was lower than that of Co(OH)₂ (115.9 mV∙dec⁻¹), indicating faster UOR kinetics over the CoV-LDHs electrocatalyst. Furthermore, the CoV-LDHs electrocatalyst displayed high stability, with a negligible potential increase after a 10-h chronopotentiometry test by maintaining the current density of 10 mA∙cm⁻². In conclusion, the present work not only shows that the d-electron compensation effect between early and late transition metals could adjust the local electronic structure of TM-LDHs to improve the UOR efficiency, but also provides a feasible route to design dedicated nanostructured TM-LDHs as high-performance UOR electrocatalysts.
- Urea oxidation,
- Layered double hydroxide,
- Nanosheet,
- d-Electron compensation,
- Wettability
1. [1]
  Lagadec, M. F.; Grimaud, A. Nat. Mater. 2020, 19, 1140. doi: 10.1038/s41563-020-0788-3 doi: 10.1038/s41563-020-0788-3
2. [2]
  Rausch, B.; Symes Mark, D.; Chisholm, G.; Cronin, L. Science 2014, 345, 1326. doi: 10.1126/science.1257443 doi: 10.1126/science.1257443
3. [3]
  He, Y.; Wang, T. L.; Zhang, M.; Wang, T. W.; Wu, L. F.; Zeng, L. Y.; Wang, X. P.; Boubeche, M.; Wang, S.; Yan, K.; et al. Small 2021, 17, 2006153. doi: 10.1002/smll.202006153 doi: 10.1002/smll.202006153
4. [4]
  Yu, J.; Yu, F.; Yuen, M.-F.; Wang, C. J. Mater. Chem. A 2021, 9, 9389. doi: 10.1039/D0TA11910E doi: 10.1039/D0TA11910E
5. [5]
  Xu, B. Y.; Zhang, Y.; Pi, Y. C.; Shao, Q.; Huang, X. Q. Acta Phys. -Chim. Sin. 2021, 37, 2009074. doi: 10.3866/PKU.WHXB202009074
6. [6]
  Zhu, B. J.; Liang, Z. B.; Zou, R. Q. Small 2020, 16, 1906133. doi: 10.1002/smll.201906133 doi: 10.1002/smll.201906133
7. [7]
  Hu, S. A.; Tan, Y.; Feng, C. Q.; Wu, H. M.; Zhang, J. J.; Mei, H. J. Power Sources 2020, 453, 227872. doi: 10.1016/j.jpowsour.2020.227872 doi: 10.1016/j.jpowsour.2020.227872
8. [8]
  Xie, J. F.; Qu, H. C.; Lei, F. G.; Peng, X.; Liu, W. W.; Gao, L.; Hao, P.; Cui, G. W.; Tang, B. J. Mater. Chem. A 2018, 6, 16121. doi: 10.1039/C8TA05054F doi: 10.1039/C8TA05054F
9. [9]
  Wang, Z. L.; Liu, W. J.; Hu, Y. M.; Guan, M.; Xu, L.; Li, H. P.; Bao, J.; Li, H. M. Appl. Catal. B: Environ. 2020, 272, 118959. doi: 10.1016/j.apcatb.2020.118959 doi: 10.1016/j.apcatb.2020.118959
10. [10]
  Wang, K. L.; Hou, M. M.; Huang, W.; Cao, Q. H.; Zhao, Y. J.; Sun, X. J.; Ding, R.; Lin, W. W.; Liu, E. H.; Gao, P. J. Colloid Interf. Sci. 2022, 615, 309. doi: 10.1016/j.jcis.2022.01.151 doi: 10.1016/j.jcis.2022.01.151
11. [11]
  Wang, Z. L.; Liu, W. J.; Bao, J.; Song, Y. J.; She, X. J.; Hua, Y. J.; Lv, G. A.; Yuan, J. J.; Li, H. M.; Xu, H. Chem. Eng. J. 2022, 430, 133100. doi: 10.1016/j.cej.2021.133100 doi: 10.1016/j.cej.2021.133100
12. [12]
  Sun, H. C.; Zhang, W.; Li, J. G.; Li, Z. S.; Ao, X.; Xue, K. H.; Ostrikov, K. K.; Tang, J.; Wang, C. D. Appl. Catal. B: Environ. 2021, 284, 119740. doi: 10.1016/j.apcatb.2020.119740 doi: 10.1016/j.apcatb.2020.119740
13. [13]
  Zhang, R.; Wei, Z. H.; Ye, G. Y.; Chen, G. J.; Miao, J. J.; Zhou, X. H.; Zhu, X. W.; Cao, X. Q.; Sun, X. N. Adv. Energy Mater. 2021, 11, 2101758. doi: 10.1002/aenm.202101758 doi: 10.1002/aenm.202101758
14. [14]
  Cao, Q. H.; Yuan, Y. H.; Wang, K. L.; Huang, W.; Zhao, Y. J.; Sun, X. J.; Ding, R.; Lin, W. W.; Liu, E. H.; Gao, P. J. Colloid Interf. Sci. 2022, 618, 411. doi: 10.1016/j.jcis.2022.03.054 doi: 10.1016/j.jcis.2022.03.054
15. [15]
  Ma, T. F.; Xu, W. W.; Li, B. R.; Chen, X.; Zhao, J. J.; Wan, S. S.; Jiang, K.; Zhang, S. X.; Wang, Z. F.; Tian, Z. Q.; et al. Angew. Chem. Int. Ed. 2021, 60, 22740. doi: 10.1002/anie.202110355 doi: 10.1002/anie.202110355
16. [16]
  Jakšić, M. M. J. Mol. Catal. 1986, 38, 161. doi: 10.1016/0304-5102(86)87056-0 doi: 10.1016/0304-5102(86)87056-0
17. [17]
  Zhou, L.; Zhang, C.; Zhang, Y. Q.; Li, Z. H.; Shao, M. F. Adv. Funct. Mater. 2021, 31, 2009743. doi: 10.1002/adfm.202009743 doi: 10.1002/adfm.202009743
18. [18]
  Gong, W. Z.; Wang, M. J.; An, Y.; Wang, J. L.; Zhou, L. X.; Xia, Y.; Wang, C. J.; Dong, K.; Pan, C.; Zhou, R. F. J. Energy Storage 2021, 38, 102579. doi: 10.1016/j.est.2021.102579 doi: 10.1016/j.est.2021.102579
19. [19]
  Lee, S. C.; Kim, M.; Park, J.-H.; Kim, E. S.; Liu, S. D.; Chung, K. Y.; Seong, C. J. J. Power Sources 2021, 486, 229341. doi: 10.1016/j.jpowsour.2020.229341 doi: 10.1016/j.jpowsour.2020.229341
20. [20]
  Wang, Y. C.; Chen, Z.; Zhang, M.; Liu, Y. Y.; Luo, H. X.; Yan, K. Green Energy Environ. 2022, 7, 1053. doi: 10.1016/j.gee.2021.01.019 doi: 10.1016/j.gee.2021.01.019
21. [21]
  Eisa, T.; Park, S.-G.; Mohamed, H. O.; Abdelkareem, M. A.; Lee, J.; Yang, E.; Castaño, P.; Chae, K.-J. Energy 2021, 228, 120584. doi: 10.1016/j.energy.2021.120584 doi: 10.1016/j.energy.2021.120584
22. [22]
  Liu, J. Z.; Ji, Y. F.; Nai, J. W.; Niu, X. G.; Luo, Y.; Guo, L.; Yang, S. H. Energy Environ. Sci. 2018, 11, 1736. doi: 10.1039/C8EE00611C doi: 10.1039/C8EE00611C
23. [23]
  Huang, G. Q.; Zhao, L.; Yuan, S. S.; Li, N.; Jing, S. B. Int. J. Hydrogen Energy 2022, 47, 14767. doi: 10.1016/j.ijhydene.2022.02.223 doi: 10.1016/j.ijhydene.2022.02.223
24. [24]
  Wang, Z. P.; Chen, L.; Xu, S. D.; Zhang, D.; Zhou, X. X.; Wu, X.; Xie, X. M.; Qiu, X. Y. Compos. Commun. 2021, 27, 100780. doi: 10.1016/j.coco.2021.100780 doi: 10.1016/j.coco.2021.100780
25. [25]
  He, D. Y.; Cao, L. Y.; Huang, J. F.; Kajiyoshi, K.; Wu, J. P.; Wang, C. C.; Liu, Q. Q.; Yang, D.; Feng, L. L. J. Energy Chem. 2020, 47, 263. doi: 10.1016/j.jechem.2020.02.010 doi: 10.1016/j.jechem.2020.02.010
26. [26]
  Li, C. F.; Xie, L. J.; Zhao, J. W.; Gu, L. F.; Wu, J. Q.; Li, G. R. Appl. Catal. B: Environ. 2022, 306, 121097. doi: 10.1016/j.apcatb.2022.121097 doi: 10.1016/j.apcatb.2022.121097
27. [27]
  Zhang, B. J.; Pan, C. T.; Liu, H. J.; Wu, X. S.; Jiang, H. L.; Yang, L.; Qi, Z. M.; Li, G.; Shan, L.; Lin, Y. X.; et al. Chem. Eng. J. 2022, 439, 135768. doi: 10.1016/j.cej.2022.135768 doi: 10.1016/j.cej.2022.135768
28. [28]
  Geng, S. K.; Zheng, Y.; Li, S. Q.; Su, H.; Zhao, X.; Hu, J.; Shu, H. B.; Jaroniec, M.; Chen, P.; Liu, Q. H.; et al. Nat. Energy 2021, 6, 904. doi: 10.1038/s41560-021-00899-2 doi: 10.1038/s41560-021-00899-2
29. [29]
  Chen, W.; Xu, L. T.; Zhu, X. R.; Huang, Y.-C.; Zhou, W.; Wang, D. D.; Zhou, Y. Y.; Du, S. Q.; Li, Q. L.; Xie, C.; et al. Angew. Chem. Int. Ed. 2021, 60, 7297. doi: 10.1002/anie.202015773 doi: 10.1002/anie.202015773
30. [30]
  Chen, W.; Xie, C.; Wang, Y. Y.; Zou, Y. Q.; Dong, C.-L.; Huang, Y.-C.; Xiao, Z. H.; Wei, Z. X.; Du, S. Q.; Chen, C.; et al. Chem 2020, 6, 2974. doi: 10.1016/j.chempr.2020.07.022 doi: 10.1016/j.chempr.2020.07.022
31. [31]
  Ji, Z. J.; Song, Y. J.; Zhao, S. H.; Li, Y.; Liu, J.; Hu, W. P. ACS Catal. 2022, 12, 569. doi: 10.1021/acscatal.1c05190 doi: 10.1021/acscatal.1c05190
32. [32]
  Yan, H. J.; Xie, Y.; Wu, A. P.; Cai, Z. C.; Wang, L.; Tian, C. G.; Zhang, X. M.; Fu, H. G. Adv. Mater. 2019, 31, 1901174. doi: 10.1002/adma.201901174 doi: 10.1002/adma.201901174
33. [33]
  Li, S. D.; Fan, J. C.; Li, S. Y.; Ma, Y.; Wu, J. H.; Jin, H. G.; Chao, Z. S.; Pan, D.; Guo, Z. H. J. Nanostruct. Chem. 2021, 11, 735. doi: 10.1007/s40097-021-00441-6 doi: 10.1007/s40097-021-00441-6
34. [34]
  Ge, J. H.; Liu, Z. F.; Guan, M. H.; Kuang, J.; Xiao, Y. H.; Yang, Y.; Tsang, C. H.; Lu, X. Y.; Yang, C. Z. J. Colloid Interf. Sci. 2022, 620, 442. doi: 10.1016/j.jcis.2022.03.152 doi: 10.1016/j.jcis.2022.03.152
35. [35]
  Wei, S.; Wang, X. X.; Wang, J. M.; Sun, X. P.; Cui, L.; Yang, W. R.; Zheng, Y. W.; Liu, J. Q. Electrochim. Acta 2017, 246, 776. doi: 10.1016/j.electacta.2017.06.068 doi: 10.1016/j.electacta.2017.06.068
36. [36]
  Hu, Q.; Zhu, B.; Li, G. M.; Liu, X. F.; Yang, H. P.; Sewell, C. D.; Zhang, Q. L.; Liu, J. H.; He, C. X.; Lin, Z. Q. Nano Energy 2019, 66, 104194. doi: 10.1016/j.nanoen.2019.104194 doi: 10.1016/j.nanoen.2019.104194
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