Citation: Lei Chen, Chaozheng He, Ran Wang, Qian Li, Jian Zeng, Wei Liu, Yuchao Wang, Qichen Wang, Tong Ye, Yougen Tang, Yongpeng Lei. Potential active sites of Mo single atoms for electrocatalytic reduction of N₂[J]. Chinese Chemical Letters, ;2021, 32(1): 53-56. doi: 10.1016/j.cclet.2020.11.013 shu

Potential active sites of Mo single atoms for electrocatalytic reduction of N₂

Lei Chen ^{a, 1} ,
Chaozheng He ^{b, d, 1} ,
Ran Wang ^{b, 1} ,
Qian Li ^{a, e} ,
Jian Zeng ^a ,
Wei Liu ^c ,
Yuchao Wang ^{a, e} ,
Qichen Wang ^a ,
Tong Ye ^a ,
Yougen Tang ^a ,
Yongpeng Lei ^{a, *,}

a.
State Key Laboratory of Powder Metallurgy, Hunan Provincial Key Laboratory of Chemical Power Sources, College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, China
b.
Institute of Environmental and Energy Catalysis, School of Materials Science and Chemical Engineering, Xi'an Technological University, Xi'an 710021, China
c.
State Key Laboratory of Fine Chemicals, Department of Chemistry, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China
d.
Shaanxi Key Laboratory of Optoelectronic Functional Materials and Devices, School of Materials Science and Chemical Engineering, Xi'an Technological University, Xi'an 710021, China
e.
School of Material Science and Engineering, Central South University of Forestry and Technology, Changsha 410004, China

ypkd@163.com

Received Date: 16 October 2020
Revised Date: 2 November 2020
Accepted Date: 5 November 2020
Available Online: 5 November 2020

Figures(4)

Single atom catalysts (SACs) with isolated metal atoms dispersed on supports exhibit distinctive performances for electrocatalysis reactions. The designable realization of well-dispersed single metal atoms is still a great challenge owing to their ease of aggregation. Here, Mo single atomic sites (Mo-N₃C) combined with some ultrasmall Mo₂C/MoN clusters (Mo-SA/Mo₂C-MoN-Cs, mean diameter < 2 nm) on nitrogen-doped porous carbon were synthesized via a simple pyrolysis of bimetallic Zn/Mo metal-organic frameworks. X-ray absorption near edge spectra (XANES) in combination with various characterizations show that most of Mo species in sample exist in the form of single sites and the exact structure is Mo-N₃C. Density functional theory (DFT) calculation further shows that as the number of N-coordination in the Mo-N_xC moieties increases, the positive charge of Mo atoms increases. The single Mo atoms in Mo-N₃C have the best capability of N₂ adsorption, which may serve as main active sites for further electrochemical N₂ reduction.
- Single atom catalysts,
- N₂ reduction reaction,
- Electrocatalysis,
- Density functional theory,
- Active sites
1. [1]
  C. Zhao, X. Dai, T. Yao, et al., J. Am. Chem. Soc. 139(2017) 8078-8081. doi: 10.1021/jacs.7b02736
2. [2]
  J. Liu, ACS Catal. 7(2017) 34-59. doi: 10.1021/acscatal.6b01534
3. [3]
  L. Han, L.J. Zhang, H. Wu, et al., Adv. Sci. 6(2019) 1900006. doi: 10.1002/advs.201900006
4. [4]
  Y. Cheng, S. He, S.F. Lu, et al., Adv. Sci. 6(2019) 1802066. doi: 10.1002/advs.201802066
5. [5]
  X. Li, H. Rong, J. Zhang, D. Wang, Y. Li, Nano Res. 13(2020) 1842-1855. doi: 10.1007/s12274-020-2755-3
6. [6]
  J. Yang, W. Li, D. Wang, Y. Li, Small Struct. (2020), doi:http://dx.doi.org/10.1002/sstr.202000051. doi: 10.1002/sstr.202000051
7. [7]
  J. Zhang, C. Zheng, M. Zhang, et al., Nano Res. 13(2020) 3082-3087. doi: 10.1007/s12274-020-2977-4
8. [8]
  W. Peng, M. Luo, X. Xu, et al., Adv. Energy Mater. 10(2020) 2001364. doi: 10.1002/aenm.202001364
9. [9]
  J.J. Guo, T. Tadesse Tsega, I. Ul Islam, et al., Chin. Chem. Lett. 31(2020) 2487-2490. doi: 10.1016/j.cclet.2020.02.019
10. [10]
  Y. Hang, W. Qiang, L. Wei, S.P. Cheng, Chin. Chem. Lett. 31(2020) 1768-1772. doi: 10.1016/j.cclet.2020.01.010
11. [11]
  J. Sun, W.H. Kong, Z.Y. Jin, et al., Chin. Chem. Lett. 31(2020) 953-960. doi: 10.1016/j.cclet.2020.01.035
12. [12]
  W. Xiong, X. Cheng, T. Wang, et al., Nano Res. 13(2020) 1008-1012. doi: 10.1007/s12274-020-2733-9
13. [13]
  T. Wu, H. Zhao, X. Zhu, et al., Adv. Mater. 32(2020) 2000299. doi: 10.1002/adma.202000299
14. [14]
  X. Lv, F. Wang, J. Du, et al., Sustain. Energy Fuels 4(2020) 4469-4472. doi: 10.1039/D0SE00828A
15. [15]
  S. Zhang, M. Jin, T. Shi, et al., Angew. Chem. Int. Ed. 59(2020) 13423-13429. doi: 10.1002/anie.202005930
16. [16]
  Y. Chen, R. Guo, X. Peng, et al., ACS Nano 14(2020) 6938-6946. doi: 10.1021/acsnano.0c01340
17. [17]
  F. Lü, S. Zhao, R. Guo, et al., Nano Energy 61(2019) 420-427. doi: 10.1016/j.nanoen.2019.04.092
18. [18]
  C. Tang, Y. Jiao, B. Shi, et al., Angew. Chem. Int. Ed. 59(2020) 9171-9176. doi: 10.1002/anie.202003842
19. [19]
  Y.P. Lei, Y.C. Wang, Y. Liu, et al., Angew. Chem. Int. Ed. 59(2020) 20794-20812. doi: 10.1002/anie.201914647
20. [20]
  W. Chen, J. Pei, C.T. He, et al., Angew. Chem. Int. Ed. 56(2017) 16086-16090. doi: 10.1002/anie.201710599
21. [21]
  L. Han, X. Liu, J. Chen, et al., Angew. Chem. Int. Ed. 58(2019) 2321-2325. doi: 10.1002/anie.201811728
22. [22]
  G. Gao, Q. Xi, Y. Zhang, et al., Nanoscale 11(2019) 1169-1176. doi: 10.1039/C8NR07739H
23. [23]
  P. Zhang, F. Sun, Z. Xiang, et al., Energy Environ. Sci. 7(2014) 442-450. doi: 10.1039/C3EE42799D
24. [24]
  P. Yin, T. Yao, Y. Wu, et al., Angew. Chem. Int. Ed. 55(2016) 10800-10805. doi: 10.1002/anie.201604802
25. [25]
  X.F. Lu, L. Yu, J. Zhang, X.W. Lou, Adv. Mater. 31(2019) 1900699.
26. [26]
  Y. Liu, C.Y. Song, Y.C. Wang, et al., Chem. Eng. J. 401(2020) 126038. doi: 10.1016/j.cej.2020.126038
27. [27]
  Y. Lei, F. Yang, H. Xie, et al., J. Mater. Chem. A 8(2020) 20629-20636. doi: 10.1039/D0TA06022D
28. [28]
  Y. Ma, T. Yang, H. Zou, et al., Adv. Mater. 32(2020) 2002177. doi: 10.1002/adma.202002177
29. [29]
  Y. Wang, J. Wang, D. Wei, M. Li, ACS Appl. Mater. Interfaces 11(2019) 35755-35763. doi: 10.1021/acsami.9b12638
30. [30]
  J. Yang, F. Zhang, X. Wang, et al., Angew. Chem. Int. Ed. 55(2016) 12854-12858. doi: 10.1002/anie.201604315
31. [31]
  M. Xiang, D. Li, W. Li, B. Zhong, Y. Sun, Catal. Commun. 8(2007) 513-518. doi: 10.1016/j.catcom.2006.07.028
32. [32]
  J. Jiang, Q. Liu, C. Zeng, L. Ai, J. Mater. Chem. A 5(2017) 16929-16935. doi: 10.1039/C7TA04893A
33. [33]
  Y. Wang, Z. Shi, Q. Mo, et al., ChemElectroChem 4(2017) 2169-2177. doi: 10.1002/celc.201700378
34. [34]
  Q.C. Wang, Y.J. Ji, Y. Lei, et al., ACS Energy Lett. 3(2018) 1183-1191. doi: 10.1021/acsenergylett.8b00303
35. [35]
  Q.C. Wang, K. Ye, L. Xu, et al., Chem. Commun. 55(2019) 14801-14804. doi: 10.1039/C9CC08439H
36. [36]
  S. Li, C. Cheng, A. Sagaltchik, et al., Adv. Funct. Mater. 29(2019) 1807419. doi: 10.1002/adfm.201807419
37. [37]
  L. Zeng, S. Chen, J. van der Zalm, X. Li, A. Chen, Chem. Commun. 55(2019) 7386-7389. doi: 10.1039/C9CC02607J
38. [38]
  L. Zhang, Z. Su, F. Jiang, et al., Nanoscale 6(2014) 6590-6602. doi: 10.1039/C4NR00348A
39. [39]
  A.M. Gänzler, M. Casapu, A. Boubnov, et al., J. Catal. 328(2015) 216-224. doi: 10.1016/j.jcat.2015.01.002
40. [40]
  Q. Liu, Q. Wang, J. Wang, et al., Adv. Funct. Mater. (2020) 2000593.
41. [41]
  Q.C. Wang, Y. Lei, Y.C. Wang, et al., Energy Environ. Sci. 13(2020) 1593-1616. doi: 10.1039/D0EE00450B
42. [42]
  Y.C. Wang, Y. Liu, W. Liu, et al., Energy Environ. Sci. 13(2020) 4609-4624. doi: 10.1039/D0EE02833A
43. [43]
  J. Zhao, Z. Chen, J. Am. Chem. Soc. 139(2017) 12480-12487. doi: 10.1021/jacs.7b05213
44. [44]
  C. Yao, R. Wang, Z. Wang, et al., J. Mater. Chem. A 7(2019) 27547-27559. doi: 10.1039/C9TA09201C
45. [45]
  C. He, R. Wang, H. Yang, S. Li, L. Fu, Appl. Surf. Sci. 507(2020) 145076. doi: 10.1016/j.apsusc.2019.145076
46. [46]
  Y. Sun, Z.Z. Deng, X.M. Song, et al., Nano Micro Lett. 12(2020) 133. doi: 10.1007/s40820-020-00444-y
47. [47]
  Q.C. Wang, Y. Lei, D.S. Wang, Y.D. Li, Energy Environ. Sci. 12(2019) 1730-1750. doi: 10.1039/C8EE03781G
48. [48]
  Y.C. Wang, B. Liu, Y. Liu, et al., Chem. Commun. 56(2020) 14019-14022. doi: 10.1039/D0CC05656A
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Potential active sites of Mo single atoms for electrocatalytic reduction of N2

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通讯作者: 陈斌, bchen63@163.com

Potential active sites of Mo single atoms for electrocatalytic reduction of N₂