Citation: Yue Zhang, Xiaoya Fan, Xun He, Tingyu Yan, Yongchao Yao, Dongdong Zheng, Jingxiang Zhao, Qinghai Cai, Qian Liu, Luming Li, Wei Chu, Shengjun Sun, Xuping Sun. Ambient electrosynthesis of urea from carbon dioxide and nitrate over Mo₂C nanosheet[J]. Chinese Chemical Letters, ;2024, 35(8): 109806. doi: 10.1016/j.cclet.2024.109806 shu

Ambient electrosynthesis of urea from carbon dioxide and nitrate over Mo₂C nanosheet

Yue Zhang ^a ,
Xiaoya Fan ^b ,
Xun He ^b ,
Tingyu Yan ^a ,
Yongchao Yao ^b ,
Dongdong Zheng ^b ,
Jingxiang Zhao ^{a, *,} ,
Qinghai Cai ^a ,
Qian Liu ^c ,
Luming Li ^c ,
Wei Chu ^c ,
Shengjun Sun ^d ,
Xuping Sun ^{b, d, *,}

a.
College of Chemistry and Chemical Engineering, and Key Laboratory of Photonic and Electronic Bandgap Materials, Ministry of Education, Harbin Normal University, Harbin 150025, China
b.
Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
c.
Institute for Advanced Study, Chengdu University, Chengdu 610106, China
d.
College of Chemistry, Chemical Engineering and Materials Science, Shandong Normal University, Ji'nan 250014, China

zhaojingxiang@hrbnu.edu.cn

xpsun@uestc.edu.cn

Received Date: 15 January 2024
Revised Date: 20 March 2024
Accepted Date: 20 March 2024
Available Online: 22 March 2024

Figures(4)

Electrocatalytic synthesis of urea through CN bond formation, converting carbon dioxide (CO₂) and nitrate (NO₃^–), presents a promising, less energy-intensive alternative to industrial urea production process. In this communication, we report the application of Mo₂C nanosheets-decorated carbon sheets (Mo₂C/C) as a highly efficient electrocatalyst for facilitating CN coupling in ambient urea electrosynthesis. In CO₂-saturated 0.2 mol/L Na₂SO₄ solution containing 0.05 mol/L NO₃^–, the Mo₂C/C catalyst achieves an impressive urea yield of 579.13 µg h^–1 mg^–1 with high Faradaic efficiency of 44.80% at –0.5 V versus the reversible hydrogen electrode. Further theoretical calculations reveal that the multiple Mo active sites enhance the formation of *CO and *NH₂ intermediates and facilitate their CN coupling. This research propels the use of Mo₂C-based electrodes in electrocatalysis and accentuates the capabilities of binary metal-based catalysts in CN coupling reactions.
- Mo₂C,
- Multiple active sites,
- C-N coupling,
- Electrocatalysis,
- Urea synthesis,
- Density functional theory calculation
1. [1]
  S. Kim, S.H. Ye, A. Adamo, et al., J. Mater. Chem. B 8 (2020) 8305–8314. doi: 10.1039/D0TB01220C
2. [2]
  P.M. Glibert, J. Harrison, C. Heil, S. Seitzinger, Biogeochem 77 (2006) 441–463. doi: 10.1007/s10533-005-3070-5
3. [3]
  A. Yapicioglu, I. Dincer, Renew. Sustain. Energy Rev. 103 (2019) 96–108. doi: 10.1016/j.rser.2018.12.023
4. [4]
  F. Barzagli, F. Mani, M. Peruzzini, Green Chem. 13 (2011) 1267–1274. doi: 10.1039/c0gc00674b
5. [5]
  J.G. Chen, R.M. Crooks, L.C. Seefeldt, et al., Science 360 (2018) 6391.
6. [6]
  S. Li, Y. Zou, C. Chen, S. Wang, Z.Q. Liu, Chin. Chem. Lett. 35 (2024) 109147. doi: 10.1016/j.cclet.2023.109147
7. [7]
  C. Chen, X. Zhu, X. Wen, et al., Nat. Chem. 12 (2020) 717–724. doi: 10.1038/s41557-020-0481-9
8. [8]
  Y. Huang, Y. Wang, Y. Wu, et al., Sci. China Chem. 65 (2022) 204–206. doi: 10.1007/s11426-021-1173-8
9. [9]
  X. Liu, Y. Jiao, Y. Zheng, et al., Nat. Commun. 13 (2022) 5471. doi: 10.1038/s41467-022-33258-0
10. [10]
  Z. Zhang, D. Li, Y. Tu, et al., SusMat 4 (2024) e193.
11. [11]
  X. Fan, C. Liu, X. He, et al., Adv. Mater. (2024), https://doi.org/10.1002/adma.202401221. doi: 10.1002/adma.202401221
12. [12]
  M. Yuan, J. Chen, Y. Bai, et al., Chem. Sci. 12 (2021) 6048–6058. doi: 10.1039/D1SC01467F
13. [13]
  X. Chen, S. Lv, J. Kang, et al., Proc. Natl. Acad. Sci. U. S. A. 120 (2023) e2306841120.
14. [14]
  M. Yuan, J. Chen, H. Zhang, et al., Energy Environ. Sci. 15 (2022) 2084–2095. doi: 10.1039/D1EE03918K
15. [15]
  X. Zhu, Y, Li, ACS Catal. 13 (2023) 15322–15330. doi: 10.1021/acscatal.3c03491
16. [16]
  J. Liu, X. Lv, Y. Ma, et al., ACS Nano 17 (2023) 25667–25678. doi: 10.1021/acsnano.3c10451
17. [17]
  J. Liang, Q. Liu, A.A. Alshehri, X. Sun, Nano Res. Energy 1 (2022) e9120010.
18. [18]
  H.Q. Yin, L.L. Yang, H. Sun, et al., Chin. Chem. Lett. 34 (2023) 107337. doi: 10.1016/j.cclet.2022.03.060
19. [19]
  D. Chen, M. Luo, S. Ning, et al., Small 18 (2022) 2104043. doi: 10.1002/smll.202104043
20. [20]
  D. Chen, J. Lan, F. Xie, et al., Chem. Eng. J. 475 (2023) 146137. doi: 10.1016/j.cej.2023.146137
21. [21]
  J. Lan, M. Luo, J. Han, et al., Small 17 (2021) 2102814. doi: 10.1002/smll.202102814
22. [22]
  W. Peng, M. Luo, X. Xu, et al., Adv. Energy Mater. 10 (2020) 2001364. doi: 10.1002/aenm.202001364
23. [23]
  X. He, J. Li, R. Li, et al., Inorg. Chem. 62 (2023) 25–29. doi: 10.1021/acs.inorgchem.2c03640
24. [24]
  J. Leverett, T. Tran-Phu, J.A. Yuwono, et al., Adv. Energy Mater. 12 (2022) 2201500. doi: 10.1002/aenm.202201500
25. [25]
  Y. Mao, Y. Jiang, H. Liu, et al., Chin. Chem. Lett. 35 (2024) 108540. doi: 10.1016/j.cclet.2023.108540
26. [26]
  Y. Luo, K. Xie, P. Ou, et al., Nat. Catal. 6 (2023) 939–948. doi: 10.1038/s41929-023-01020-4
27. [27]
  X. He, T. Xie, K. Dong, et al., Sci. China Mater. (2024), doi:10.1007/s40843-024-2798-5. doi: 10.1007/s40843-024-2798-5
28. [28]
  Y. Zhao, Y. Ding, W. Li, et al., Nat. Commun. 14 (2023) 4491. doi: 10.1038/s41467-023-40273-2
29. [29]
  C. Chen, S. Li, X. Zhu, et al., Carbon Energy 5 (2023) e345.
30. [30]
  H. Song, D.A. Chipoco Haro, P.W. Huang, et al., Acc. Chem. Res. 56 (2023) 2944–2953. doi: 10.1021/acs.accounts.3c00424
31. [31]
  C. Tang, Y. Zheng, M. Jaroniec, S.Z. Qiao, Angew. Chem. Int. Ed. 133 (2021) 2–21. doi: 10.1002/ange.202014556
32. [32]
  C. Lv, L. Zhong, C. Yan, et al., Nat. Sustain. 4 (2021) 868–876. doi: 10.1038/s41893-021-00741-3
33. [33]
  Y. Mao, Y. Jiang, Q. Gou, et al., Appl. Catal. B: Environ. 340 (2024) 123189. doi: 10.1016/j.apcatb.2023.123189
34. [34]
  Z. Li, P. Zhou, M. Zhou, et al., Appl. Catal. B: Environ. (338) (2023) 122962.
35. [35]
  J. Qin, N. Liu, L. Chen, et al., ACS Sustainable Chem. Eng. 10 (2022) 15869–15875. doi: 10.1021/acssuschemeng.2c05110
36. [36]
  C. Liu, H. Tong, P. Wang, et al., Appl. Catal. B: Environ. 336 (2023) 122917. doi: 10.1016/j.apcatb.2023.122917
37. [37]
  X. Zhu, X. Yuan, Y. Wang, M. Ge, Y. Tang, J. Catal. 429 (2024) 115218. doi: 10.1016/j.jcat.2023.115218
38. [38]
  Y. Wang, S. Xia, J. Zhang, et al., ACS Energy Lett. 8 (2023) 3373–3380. doi: 10.1021/acsenergylett.3c00824
39. [39]
  S. Shin, S. Sultan, Z.X. Chen, et al., Energy Environ. Sci. 16 (2023) 2003–2013. doi: 10.1039/D3EE00008G
40. [40]
  N. Meng, X. Ma, C. Wang, et al., ACS Nano 16 (2022) 9095–9104. doi: 10.1021/acsnano.2c01177
41. [41]
  F.Y. Chen, Z.Y. Wu, S. Gupta, et al., Nat. Nanotechnol. 17 (2022) 759–767. doi: 10.1038/s41565-022-01121-4
42. [42]
  Y. Wang, W. Zhou, R. Jia, Y. Yu, B. Zhang, Angew. Chem. Int. Ed. 59 (2020) 5350–5354. doi: 10.1002/anie.201915992
43. [43]
  J. Liang, Z. Li, L. Zhang, et al., Chem 9 (2023) 1768–1827. doi: 10.1016/j.chempr.2023.05.037
44. [44]
  T. Zhao, K. Chen, X. Xu, et al., Appl. Catal. B: Environ. 339 (2023) 123156. doi: 10.1016/j.apcatb.2023.123156
45. [45]
  R.D. Milton, S.D. Minteer, ChemPlusChem 82 (2017) 513–521. doi: 10.1002/cplu.201600442
46. [46]
  E. Murphy, Y. Liu, I. Matanovic, et al., ACS Catal. 12 (2022) 6651–6662. doi: 10.1021/acscatal.2c01367
47. [47]
  P. Huang, M. Cheng, H. Zhang, et al., Nano Energy 61 (2019) 428–434. doi: 10.1016/j.nanoen.2019.05.003
48. [48]
  M. Sun, G. Wu, J. Jiang, et al., Angew. Chem. Int. Ed. 62 (2023) e202301957.
49. [49]
  J. Yu, W. Yu, B. Chang, et al., Chin. Chem. Lett. 33 (2023) 3231–3235.
50. [50]
  Z. Nie, Z. Tang, D. Jiao, et al., ChemCatChem 14 (2022) e202101885.
51. [51]
  Y. Wu, K. Yao, Z. Zhao, et al., Chem. Eng. J. 479 (2024) 147602. doi: 10.1016/j.cej.2023.147602
52. [52]
  X. Ye, J. Ma, W. Yu, et al., J. Energy Chem. 67 (2022) 184–192. doi: 10.1016/j.jechem.2021.10.017
53. [53]
  N.H. Attanayake, H.R. Banjade, A.C. Thenuwara, et al., Chem. Commun. 57 (2021) 1675–1678. doi: 10.1039/D0CC05822J
54. [54]
  J. Li, C. Zhang, C. Wu, et al., Chin. Chem. Lett. 35 (2024) 108782. doi: 10.1016/j.cclet.2023.108782
55. [55]
  Y. Wan, M. Zheng, R. Lv, Mater. Today Energy 32 (2023) 101240. doi: 10.1016/j.mtener.2022.101240
56. [56]
  X. Ren, J. Zhao, Q. Wei, et al., ACS Cent. Sci. 5 (2019) 116–121. doi: 10.1021/acscentsci.8b00734
57. [57]
  X. Liu, W. Sun, J. Chen, Z. Wen, Angew. Chem. Int. Ed. 136 (2023) e202317313.
58. [58]
  X. He, X. Li, X. Fan, et al., ACS Appl. Nano Mater. 5 (2022) 14246–14250. doi: 10.1021/acsanm.2c03720
59. [59]
  Z. Nie, L. Zhang, Q. Zhu, et al., J. Energy Chem. 88 (2024) 202–212. doi: 10.1016/j.jechem.2023.09.009
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沈阳化工大学材料科学与工程学院沈阳 110142

Ambient electrosynthesis of urea from carbon dioxide and nitrate over Mo2C nanosheet

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Ambient electrosynthesis of urea from carbon dioxide and nitrate over Mo₂C nanosheet