Citation: Lanxin Wang, Kaiwei Liang, Xuelian Yu, Guocheng Lv, Libing Liao. Facile method for creating frustrated Lewis pairs in g-C₃N₄ to enhance photocatalytic nitrogen fixation performance[J]. Chinese Chemical Letters, ;2026, 37(1): 110572. doi: 10.1016/j.cclet.2024.110572 shu

Facile method for creating frustrated Lewis pairs in g-C₃N₄ to enhance photocatalytic nitrogen fixation performance

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Engineering Research Center of Ministry of Education for Geological Carbon Storage and Low Carbon Utilization of Resources, Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes, National Laboratory of Mineral Materials, School of Materials Science and Technology, China University of Geosciences (Beijing), Beijing 100083, China

xlyu@cugb.edu.cn

guochenglv@cugb.edu.cn

Received Date: 3 July 2024
Revised Date: 17 September 2024
Accepted Date: 22 October 2024
Available Online: 22 October 2024

Figures(7)

The rate-limited activation of NN triple bonds with high bond energies has been a bottleneck in photoctalytic nitrogen fixation. Here, polymeric carbon nitride with frustrated Lewis pairs (FLPs) was constructed by inserting electron-deficient magnesium into g-C₃N₄ (CN). The synergistic interactions between Mg and amino groups in CN led to a 7.2 fold increase in the photoreactivity of nitrogen (N₂) fixation by carbon nitride.
- N₂ fixation,
- Photocatalytic,
- FLPs,
- Ammonia,
- g-C₃N₄
1. [1]
  R. Wu, S. Gao, C. Jones, et al., Adv. Funct. Mater. 34 (2024) 2314051.
2. [2]
  T. Bao, Y. Xi, C. Zhang, et al., Natl. Sci. Rev. 11 (2024) nwae093.
3. [3]
  N. Zhang, A. Jalil, D. Wu, et al., J. Am. Chem. Soc. 140 (2018) 9434–9443. doi: 10.1021/jacs.8b02076
4. [4]
  Y. Liu, X. Ye, R. Li, et al., Chin. Chem. Lett. 33 (2022) 5162–5168.
5. [5]
  Y. Xia, Y. Xu, X. Yu, et al., J. Mater. Chem. A 10 (2022) 17377–17394. doi: 10.1039/d2ta03977j
6. [6]
  B. Li, Y. Si, B. Zhou, et al., ACS Appl. Mater. Interfaces 11 (2019) 17341–17349. doi: 10.1021/acsami.8b22366
7. [7]
  Y. Tan, L. Yan, C. Huang, et al., Small. 17 (2021) 2100372.
8. [8]
  S. Wang, X. Hai, X. Ding, et al., Adv. Mater. 29 (2017) 1701774.
9. [9]
  X. Feng, W. Meng, H. Du, Chem. Soc. Rev. 52 (2023) 858–8598.
10. [10]
  A. Dai, S. Li, T. Wang, et al., Chin. Chem. Lett. 34 (2023) 107559–107562.
11. [11]
  G.A. Russell-Parks, T. Gennett, B.G. Trewyn, Int. J. Hydrog. Energy 48 (2023) 18612–18633.
12. [12]
  L. Ma, Y. Gao, B. Wei, et al., ACS Catal. 14 (2024) 2775–2786. doi: 10.1021/acscatal.3c05360
13. [13]
  J.A. Buss, D.G. VanderVelde, T. Agapie, J. Am. Chem. Soc. 140 (2018) 10121–10125. doi: 10.1021/jacs.8b05874
14. [14]
  Y. Ran, X. Yu, J. Liu, et al., J. Mater. Chem. A 8 (2020) 13292–13298. doi: 10.1039/d0ta03914d
15. [15]
  J. Zhang, G. Zhang, X. Chen, et al., Angew. Chem. Int. Ed. 51 (2012) 3183–3187. doi: 10.1002/anie.201106656
16. [16]
  H. Zhang, Y. Tang, Z. Liu, et al., Chem. Phys. Lett. 51 (2020) 137467.
17. [17]
  C. Yuan, S. Liang, Z. Lu, W. Hao, F. Teng, Energy Fuels 35 (2021) 16232–16240. doi: 10.1021/acs.energyfuels.1c02590
18. [18]
  E. Vesali-Kermani, A. Habibi-Yangjeh, S. Ghosh, J. Ind. Eng. Chem. 84 (2020) 185–195.
19. [19]
  M. Gao, Z. Li, X. Su, et al., Chemosphere 343 (2023) 140285.
20. [20]
  S. Yang, Y. Gong, J. Zhang, et al., Adv. Mater. 25 (2013) 2452–2456. doi: 10.1002/adma.201204453
21. [21]
  J.L. Chen, J.H. Zhu, Res. Chem. Intermed. 45 (2019) 947–950. doi: 10.1007/s11164-018-3654-z
22. [22]
  R.C. Dante, Int. J. Hydrog. Energy 44 (2019) 21030–21036.
23. [23]
  J. Li, B. Zhang, Q. Song, X. Xu, W. Hou, Ceram. Int. 46 (2020) 14178–14187.
24. [24]
  D. Hong, T. Kawanishi, Y. Tsukakoshi, et al., J. Am. Chem. Soc. 141 (2019) 20309–20317. doi: 10.1021/jacs.9b10597
25. [25]
  X. Xie, P. Xiao, W. Fang, G. Cui, W. Thiel, ACS Catal. 9 (2019) 9178–9187. doi: 10.1021/acscatal.9b01551
26. [26]
  Y. Dong, K.K. Ghuman, R. Popescu, et al., Adv. Sci. 5 (2018) 1700732.
27. [27]
  M. Liu, G. Lv, H. Liu, et al., Chin. Chem. Lett. 35 (2024) 108459–108463.
28. [28]
  W. Lin, H. Chen, G. Lin, et al., Angew. Chem. Int. Ed. 134 (2022) e202207807.
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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

Facile method for creating frustrated Lewis pairs in g-C3N4 to enhance photocatalytic nitrogen fixation performance

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通讯作者: 陈斌, bchen63@163.com

Facile method for creating frustrated Lewis pairs in g-C₃N₄ to enhance photocatalytic nitrogen fixation performance