Citation: Jiajun Wang, Chen Sun, Li Sheng, Zhiwen Zhuo, Shujuan Li, Jiayao Wang, Weiyi Wang, Jinbo Sun, Juqian Yang, Ke Xu, Shulai Lei. Unveiling the electrocatalytic potential of main-group metal-embedded BC₃ monolayer for highly efficient NO reduction to NH₃[J]. Chinese Chemical Letters, ;2026, 37(5): 110974. doi: 10.1016/j.cclet.2025.110974 shu

Unveiling the electrocatalytic potential of main-group metal-embedded BC₃ monolayer for highly efficient NO reduction to NH₃

Jiajun Wang ^a ,
Chen Sun ^a ,
Li Sheng ^b ,
Zhiwen Zhuo ^c ,
Shujuan Li ^{d, *,} ,
Jiayao Wang ^d ,
Weiyi Wang ^{c, *,} ,
Jinbo Sun ^d ,
Juqian Yang ^d ,
Ke Xu ^d ,
Shulai Lei ^{d, e, *,}

a.
Tianjin Key Laboratory of Structure and Performance for Functional Molecules, College of Chemistry, Tianjin Normal University, Tianjin 300387, China
b.
Hefei Metrology and Testing Center, Hefei 230088, China
c.
Department of Chemical Physics & Hefei National Laboratory for Physical Sciences at Microscale, University of Science and Technology of China, Hefei 230026, China
d.
School of Physics and Electronic Engineering, Hubei Key Laboratory of Low Dimensional Optoelectronic Materials and Devices, Hubei University of Arts and Science, Xiangyang 441053, China
e.
Hubei Longzhong Laboratory, Xiangyang 441053, China

11724@hbuas.edu.cn

dancingw@ustc.edu.cn

sllei@hbuas.edu.cn

Received Date: 16 October 2024
Revised Date: 4 February 2025
Accepted Date: 18 February 2025
Available Online: 18 February 2025

Figures(5)

Electrochemical NO reduction reaction (NORR) has gained extensive attention as a promising approach to achieve both harmful NO removal and ambient NH₃ production. Main-group metal-based single-atom catalysts (SACs) hold great promise for electrocatalysis but still lack adequate investigation. Herein, by means of the first-principles calculations, we systematically explore the potential of main-group metal-embedded BC₃ monolayer (denoted as M@V_B and M@V_C, M = Mg, Ca, Al, Ga, In, Ge, Sn, Sb, and Bi) as highly efficient SACs for the NORR toward NH₃ synthesis. After examining the structural stability, NO adsorbability, NORR catalytic performance, and NH₃ selectivity, we screen Al@V_B, Ga@V_B, and Ge@V_C out of 18 candidate systems. Remarkably, NO can be adsorbed and activated on them with moderate ΔG_^*NO of -1.27~-1.90 eV, and spontaneously reduced into NH₃ without any limiting potential. Moreover, the three screened candidates can effectively inhibit the production of N₂O/N₂ byproducts under high NO converge, as well as the competing hydrogen evolution reaction (HER). Our work not only offers several high-efficiency NORR electrocatalysts, but also guides the rational design of potential main-group metal-based SACs.
- BC₃ monolayer,
- Single-atom catalysts,
- Main-group metals,
- Electrocatalytic NO reduction,
- First-principles calculations
1. [1]
  T.Y. Dai, T.H. Wang, Z. Wen, et al., Adv. Funct. Mater. 34 (2024) 2400773. doi: 10.1002/adfm.202400773
2. [2]
  Y. Yang, J. Wang, Y. Shu, et al., Phys. Chem. Chem. Phys. 24 (2022) 8591–8603. doi: 10.1039/d1cp05442b
3. [3]
  C. He, J. Wang, L. Fu, et al., Chin. Chem. Lett. 35 (2024) 109037. doi: 10.1016/j.cclet.2023.109037
4. [4]
  G. Qing, R. Ghazfar, S.T. Jackowski, et al., Chem. Rev. 120 (2020) 5437–5516. doi: 10.1021/acs.chemrev.9b00659
5. [5]
  J. Wang, M. Shi, G. Yi, et al., Mol. Catal. 511 (2021) 111726.
6. [6]
  J. Wu, L. Yang, X. Liu, et al., Chin. Chem. Lett. 34 (2023) 107659. doi: 10.1016/j.cclet.2022.07.002
7. [7]
  J. Wang, M. Shi, G. Yi, et al., Chin. Chem. Lett. 33 (2022) 4623–4627. doi: 10.1016/j.cclet.2021.12.040
8. [8]
  Y. Ren, S. Li, C. Yu, et al., J. Am. Chem. Soc. 146 (2024) 6409–6421. doi: 10.1021/jacs.3c11676
9. [9]
  D. Wang, X.F. Lu, D. Luan, et al., Adv. Mater. 36 (2024) 2312645. doi: 10.1002/adma.202312645
10. [10]
  Y. Zang, Q. Wu, S. Wang, et al., Adv. Energy Mater. 14 (2024) 2303953. doi: 10.1002/aenm.202303953
11. [11]
  X. Sun, Y. Dai, B. Huang, et al., J. Phys. Chem. Lett. 14 (2023) 11684–11690. doi: 10.1021/acs.jpclett.3c03105
12. [12]
  C. He, J. Wang, L. Fu, et al., Chin. Chem. Lett. 33 (2022) 1051–1057. doi: 10.1016/j.cclet.2021.09.009
13. [13]
  S. Zhao, Y. Li, Z. Guo, et al., J. Mater. Chem. A 10 (2022) 25201–25211. doi: 10.1039/d2ta06354a
14. [14]
  C. He, R. Sun, L. Fu, et al., Chin. Chem. Lett. 33 (2022) 527–532. doi: 10.1016/j.cclet.2021.05.072
15. [15]
  Z. Wu, Y. Liu, D. Wang, et al., Adv. Mater. 36 (2024) 2309470. doi: 10.1002/adma.202309470
16. [16]
  L. Xiao, S. Mou, W. Dai, et al., Angew. Chem. Int. Ed. 63 (2024) e202319135. doi: 10.1002/anie.202319135
17. [17]
  K. Chen, J. Xiang, Y. Guo, et al., Nano Lett. 24 (2024) 541–548. doi: 10.1021/acs.nanolett.3c02259
18. [18]
  B. Qiao, A. Wang, X. Yang, et al., Nat. Chem. 3 (2011) 634–641. doi: 10.1038/nchem.1095
19. [19]
  F. Kraushofer, G.S. Parkinson, Chem. Rev. 122 (2022) 14911–14939. doi: 10.1021/acs.chemrev.2c00259
20. [20]
  S. Wang, X.T. Min, B. Qiao, et al., Chin. J. Catal. 52 (2023) 1–13.
21. [21]
  J. Wang, G. Yi, S. Guo, et al., Chin. Chem. Lett. 35 (2024) 109050. doi: 10.1016/j.cclet.2023.109050
22. [22]
  G. Xue, S. Ping, H. Ce, et al., Energy Mater. 3 (2023) 300016.
23. [23]
  R. Cheng, C.N. Cui, Z.X. Luo, Rare Met. 43 (2024) 3810–3818. doi: 10.1007/s12598-024-02680-2
24. [24]
  G. Song, R. Gao, Z. Zhao, et al., Appl. Catal. B: Environ. 301 (2022) 120809. doi: 10.1016/j.apcatb.2021.120809
25. [25]
  W. Zhang, M. Xu, T. Wang, et al., Sep. Purif. Technol. 354 (2025) 129536. doi: 10.1016/j.seppur.2024.129536
26. [26]
  S. Peng, Y. Rao, T. Li, et al., Chin. Chem. Lett. 35 (2024) 109219. doi: 10.1016/j.cclet.2023.109219
27. [27]
  X. Yao, L. Huang, E. Halpren, et al., J. Am. Chem. Soc. 145 (2023) 26249–26256. doi: 10.1021/jacs.3c08936
28. [28]
  L. Kong, X. Liang, M. Wang, et al., J. Colloid Interf. Sci. 647 (2023) 375–383. doi: 10.1016/j.jcis.2023.05.158
29. [29]
  H. Niu, Z. Zhang, X. Wang, et al., Small 17 (2021) 2102396. doi: 10.1002/smll.202102396
30. [30]
  L. Lin, L. Yan, L. Fu, et al., Fuel 308 (2022) 122068. doi: 10.1016/j.fuel.2021.122068
31. [31]
  R. Zhao, Z. Ma, Y. Yu, et al., Nano Res. 16 (2023) 8533–8541. doi: 10.1007/s12274-023-5619-9
32. [32]
  Y. Zang, Q. Wu, S. Wang, et al., Mater. Horiz. 10 (2023) 2160–2168. doi: 10.1039/d2mh01440h
33. [33]
  Y. Wu, J. Lv, F. Xie, et al., J. Colloid Interf. Sci. 656 (2024) 155–167. doi: 10.3847/1538-4357/ad509f
34. [34]
  L. Kong, M. Wang, C.M.L. Wu, ACS Mater. Lett. 6 (2024) 1711–1721. doi: 10.1021/acsmaterialslett.3c01604
35. [35]
  H. Li, D. Wu, J. Wu, et al., Nanoscale 16 (2024) 7058–7067. doi: 10.1039/d4nr00028e
36. [36]
  G.F. Chen, S. Ren, L. Zhang, et al., Small Methods 3 (2019) 1800337. doi: 10.1002/smtd.201800337
37. [37]
  S. Liu, Z. Li, C. Wang, et al., Nat. Commun. 11 (2020) 938. doi: 10.1038/s41467-020-14565-w
38. [38]
  T. Liu, X. Qu, Y. Zhang, et al., Chem. Eng. J. 457 (2023) 141187. doi: 10.1016/j.cej.2022.141187
39. [39]
  F. Luo, A. Roy, L. Silvioli, et al., Nat. Mater. 19 (2020) 1215–1223. doi: 10.1038/s41563-020-0717-5
40. [40]
  Q. Wang, M. Dai, H. Li, et al., Adv. Mater. 35 (2023) 2300695. doi: 10.1002/adma.202300695
41. [41]
  L. Zhang, H. Zhou, X. Yang, et al., Angew. Chem. Int. Ed. 62 (2023) e202217473. doi: 10.1002/anie.202217473
42. [42]
  K. Chen, Y. Zhang, J. Xiang, et al., ACS Energy Lett. 8 (2023) 1281–1288. doi: 10.1021/acsenergylett.2c02882
43. [43]
  X. Li, G. Zhang, P. Shen, et al., Inorg. Chem. Front. 10 (2023) 280–287. doi: 10.1039/d2qi02118h
44. [44]
  K. Chen, N. Zhang, F. Wang, et al., J. Mater. Chem. A 11 (2023) 6814–6819. doi: 10.1039/d3ta00606a
45. [45]
  Q. Wu, B. Huang, Y. Dai, et al., npj 2D Mater. Appl. 6 (2022) 52. doi: 10.1038/s41699-022-00326-4
46. [46]
  L. Zhao, Y. Li, G. Zhou, et al., Chin. Chem. Lett. 32 (2021) 900–905. doi: 10.1016/j.cclet.2020.07.016
47. [47]
  H. Yanagisawa, T. Tanaka, Y. Ishida, et al., Phys. Rev. Lett. 93 (2004) 177003. doi: 10.1103/PhysRevLett.93.177003
48. [48]
  Z. Yang, J. Ni, Appl. Phys. Lett. 100 (2012) 183109. doi: 10.1063/1.4711038
49. [49]
  J. Li, Y. Guo, S. Ma, et al., Int. J. Hydrogen Energy 47 (2022) 24004–24013. doi: 10.1016/j.ijhydene.2022.05.154
50. [50]
  H. Yang, C. He, L. Fu, et al., Chin. Chem. Lett. 32 (2021) 3202–3206. doi: 10.1016/j.cclet.2021.03.038
51. [51]
  Y. Guo, X. Kang, S. Gao, et al., Phys. Chem. Chem. Phys. 25 (2023) 12420–12425. doi: 10.1039/d3cp00653k
52. [52]
  R.P. Joshi, B. Ozdemir, V. Barone, et al., J. Phys. Chem. Lett. 6 (2015) 2728–2732. doi: 10.1021/acs.jpclett.5b01110
53. [53]
  J. Ou, X. Kang, X. Duan, Nanoscale 14 (2022) 12823–12829. doi: 10.1039/d2nr02796h
54. [54]
  W. Guo, S. Wang, H. Wang, et al., J. Energy Chem. 96 (2024) 336–344. doi: 10.1016/j.jechem.2024.05.002
55. [55]
  C. Chen, B. Xiao, Z. Qin, et al., ACS Appl. Mater. Interfaces 15 (2023) 40538–40548. doi: 10.1021/acsami.3c07790
56. [56]
  Y. Wang, N. Zhou, Y. Li, Chem. Eng. J. 425 (2021) 130631. doi: 10.1016/j.cej.2021.130631
57. [57]
  Y. Zhou, G. Gao, W. Chu, et al., Nanoscale 13 (2021) 1331–1339. doi: 10.1039/d0nr07580a
58. [58]
  D. McGlamery, C. McDaniel, D.M. Ladd, et al., Chem. Sci. 15 (2024) 4358–4363. doi: 10.1039/d3sc06837d
59. [59]
  G. Kresse, J. Furthmuller, Phys. Rev. B 54 (1996) 11169. doi: 10.1103/PhysRevB.54.11169
60. [60]
  P.E. Blöchl, Phys. Rev. B 50 (1994) 17953. doi: 10.1103/PhysRevB.50.17953
61. [61]
  J.P. Perdew, K. Burke, M. Ernzerhof, Phys. Rev. Lett. 77 (1996) 3865. doi: 10.1103/PhysRevLett.77.3865
62. [62]
  S. Grimme, J. Comput. Chem. 27 (2006) 1787–1799. doi: 10.1002/jcc.20495
63. [63]
  H.J. Monkhorst, J.D. Pack, Phys. Rev. B 13 (1976) 5188. doi: 10.1103/PhysRevB.13.5188
64. [64]
  L. Pan, X. Kang, S. Gao, et al., Phys. Chem. Chem. Phys. 26 (2024) 1011–1016. doi: 10.1039/d3cp04660e
65. [65]
  G. Xing, S. Liu, J.Y. Liu, Mol. Catal. 553 (2024) 113771.
66. [66]
  S. Li, M. Shi, J. Yu, et al., Chin. Chem. Lett. 32 (2021) 1977–1982. doi: 10.1016/j.cclet.2020.09.056
67. [67]
  Y. Zhou, W. Chu, F. Jing, et al., Appl. Surf. Sci. 410 (2017) 166–176. doi: 10.1089/scd.2016.0162
68. [68]
  D.H. Lim, J. Wilcox, J. Phys. Chem. C 115 (2011) 22742–22747. doi: 10.1021/jp205244m
69. [69]
  L.J. Ma, J. Wang, J. Jia, et al., Int. J. Hydrogen Energy 47 (2022) 28423–28433. doi: 10.1016/j.ijhydene.2022.06.152
70. [70]
  S.J. Qian, H. Cao, Y.G. Wang, et al., J. Am. Chem. Soc. 146 (2024) 12530–12537. doi: 10.1021/jacs.4c00827
71. [71]
  M. He, X. Chen, Y. Zhou, et al., J. Phys. Chem. Lett. 14 (2023) 7100–7107. doi: 10.1021/acs.jpclett.3c01576
72. [72]
  C. Ling, X. Niu, Q. Li, et al., J. Am. Chem. Soc. 140 (2018) 14161–14168. doi: 10.1021/jacs.8b07472
73. [73]
  Y. Zang, Q. Wu, S. Wang, et al., J. Phys. Chem. Lett. 13 (2022) 527–535. doi: 10.1021/acs.jpclett.1c03938
74. [74]
  Y. Sun, Z. Wang, Y. Liu, et al., Inorg. Chem. Front. 10 (2023) 2677–2688. doi: 10.1039/d3qi00225j
75. [75]
  K. Mathew, R. Sundararaman, K. Letchworth-Weaver, et al., J. Chem. Phys. 140 (2014) 084106. doi: 10.1063/1.4865107
76. [76]
  S. Liu, G. Xing, J.Y. Liu, Appl. Surf. Sci. 611 (2023) 155764. doi: 10.1016/j.apsusc.2022.155764
77. [77]
  M. Tursun, C. Wu, Inorg. Chem. 61 (2022) 17448–17458. doi: 10.1021/acs.inorgchem.2c02247
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Unveiling the electrocatalytic potential of main-group metal-embedded BC3 monolayer for highly efficient NO reduction to NH3

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通讯作者: 陈斌, bchen63@163.com

Unveiling the electrocatalytic potential of main-group metal-embedded BC₃ monolayer for highly efficient NO reduction to NH₃