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

.
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.
1. [1]
  Kai Han , Guohui Dong , Ishaaq Saeed , Tingting Dong , Chenyang Xiao . Morphology and photocatalytic tetracycline degradation of g-C3N4 optimized by the coal gangue. Chinese Journal of Structural Chemistry, 2024, 43(2): 100208-100208. doi: 10.1016/j.cjsc.2023.100208
2. [2]
  Zheng Liu , Yuqing Bian , Graham Dawson , Jiawei Zhu , Kai Dai . Rational constructing of Zn_0.5Cd_0.5S-diethylenetriamine/g-C₃N₄ S-scheme heterojunction with enhanced photocatalytic H₂O₂ production. Chinese Chemical Letters, 2025, 36(9): 111272-. doi: 10.1016/j.cclet.2025.111272
3. [3]
  Xuejiao Wang , Suiying Dong , Kezhen Qi , Vadim Popkov , Xianglin Xiang . Photocatalytic CO₂ Reduction by Modified g-C₃N₄. Acta Physico-Chimica Sinica, 2024, 40(12): 2408005-0. doi: 10.3866/PKU.WHXB202408005
4. [4]
  Haitao Wang , Lianglang Yu , Jizhou Jiang , Arramel , Jing Zou . S-Doping of the N-Sites of g-C₃N₄ to Enhance Photocatalytic H₂ Evolution Activity. Acta Physico-Chimica Sinica, 2024, 40(5): 2305047-0. doi: 10.3866/PKU.WHXB202305047
5. [5]
  Pengkun Li , Runjie Wu , Shuai Gao , Zeping Qin , Mingming Sun , Changzheng Wang , Wenming Sun , Qiang Wang . Bi-Bi₂Ti₂O₇ ohmic junction: Dual electron channels driving efficient photocatalytic nitrogen fixation. Chinese Chemical Letters, 2026, 37(1): 111116-. doi: 10.1016/j.cclet.2025.111116
6. [6]
  Guangming YIN , Huaiyao WANG , Jianhua ZHENG , Xinyue DONG , Jian LI , Yi'nan SUN , Yiming GAO , Bingbing WANG . Preparation and photocatalytic degradation performance of Ag/protonated g-C₃N₄ nanorod materials. Chinese Journal of Inorganic Chemistry, 2024, 40(8): 1491-1500. doi: 10.11862/CJIC.20240086
7. [7]
  Jianyu Qin , Yuejiao An , Yanfeng Zhang . In Situ Assembled ZnWO₄/g-C₃N₄ S-Scheme Heterojunction with Nitrogen Defect for CO₂ Photoreduction. Acta Physico-Chimica Sinica, 2024, 40(12): 2408002-0. doi: 10.3866/PKU.WHXB202408002
8. [8]
  Yingqi BAI , Hua ZHAO , Huipeng LI , Xinran REN , Jun LI . Perovskite LaCoO₃/g-C₃N₄ heterojunction: Construction and photocatalytic degradation properties. Chinese Journal of Inorganic Chemistry, 2025, 41(3): 480-490. doi: 10.11862/CJIC.20240259
9. [9]
  Min WANG , Dehua XIN , Wei ZHANG , Haiying YANG , Yuchun WANG , Zhaorong LIU , Meng SHI , Le SHI . Preparation and full-spectrum catalytic degradation performance of nitrogen vacancy g-C₃N₄/Bi/BiOBr/BiOI heterojunction material. Chinese Journal of Inorganic Chemistry, 2025, 41(11): 2283-2298. doi: 10.11862/CJIC.20250109
10. [10]
  Hui Wang , Abdelkader Labidi , Menghan Ren , Feroz Shaik , Chuanyi Wang . Recent Progress of Microstructure-Regulated g-C₃N₄ in Photocatalytic NO Conversion: The Pivotal Roles of Adsorption/Activation Sites. Acta Physico-Chimica Sinica, 2025, 41(5): 100039-0. doi: 10.1016/j.actphy.2024.100039
11. [11]
  Guixu Pan , Zhiling Xia , Ning Wang , Hejia Sun , Zhaoqi Guo , Yunfeng Li , Xin Li . Preparation of high-efficient donor-π-acceptor system with crystalline g-C3N4 as charge transfer module for enhanced photocatalytic hydrogen evolution. Chinese Journal of Structural Chemistry, 2024, 43(12): 100463-100463. doi: 10.1016/j.cjsc.2024.100463
12. [12]
  Yanghanbin Zhang , Dongxiao Wen , Wei Sun , Jiahe Peng , Dezhong Yu , Xin Li , Yang Qu , Jizhou Jiang . State-of-the-art evolution of g-C3N4-based photocatalytic applications: A critical review. Chinese Journal of Structural Chemistry, 2024, 43(12): 100469-100469. doi: 10.1016/j.cjsc.2024.100469
13. [13]
  Tianjun Ni , Hui Zhang , Liping Zhou , Roujie Ma , Yanyu Wang , Zhijun Yang , Dan Luo , Nithima Khaorapapong , Xingtao Xu , Yusuke Yamauchi , Dong Liu . Atomic cobalt catalysts on 3D interconnected g-C₃N₄ support for activation of peroxymonosulfate: The importance of Co-N coordination effect. Chinese Chemical Letters, 2025, 36(9): 110659-. doi: 10.1016/j.cclet.2024.110659
14. [14]
  Jiayao Wang , Guixu Pan , Ning Wang , Shihan Wang , Yaolin Zhu , Yunfeng Li . Preparation of donor-π-acceptor type graphitic carbon nitride photocatalytic systems via molecular level regulation for high-efficient H₂O₂ production. Acta Physico-Chimica Sinica, 2025, 41(12): 100168-0. doi: 10.1016/j.actphy.2025.100168
15. [15]
  Hualin Jiang , Wenxi Ye , Huitao Zhen , Xubiao Luo , Vyacheslav Fominski , Long Ye , Pinghua Chen . Novel 3D-on-2D g-C₃N₄/AgI._x._y heterojunction photocatalyst for simultaneous and stoichiometric production of H₂ and H₂O₂ from water splitting under visible light. Chinese Chemical Letters, 2025, 36(2): 109984-. doi: 10.1016/j.cclet.2024.109984
16. [16]
  Chao-Long Chen , Rong Chen , La-Sheng Long , Lan-Sun Zheng , Xiang-Jian Kong . Anchoring heterometallic cluster on P-doped carbon nitride for efficient photocatalytic nitrogen fixation in water and air ambient. Chinese Chemical Letters, 2024, 35(4): 108795-. doi: 10.1016/j.cclet.2023.108795
17. [17]
  Yueying Wang , Jianming Xiong , Linwei Xin , Yuanyuan Li , He Huang , Wenjun Miao . Photosensitizer-synergized g-carbon nitride nanosheets with enhanced photocatalytic activity for eradicating drug-resistant bacteria and promoting wound healing. Chinese Chemical Letters, 2025, 36(4): 110003-. doi: 10.1016/j.cclet.2024.110003
18. [18]
  Qiang Feng , Jindong Hao , Ya Hu , Rong Fu , Wei Wei , Dong Yi . Photocatalytic multi-component synthesis of ester-containing quinoxalin-2(1H)-ones using water as the hydrogen donor. Chinese Chemical Letters, 2025, 36(6): 110582-. doi: 10.1016/j.cclet.2024.110582
19. [19]
  Sajid Mahmood , Haiyan Wang , Fang Chen , Yijun Zhong , Yong Hu . Recent progress and prospects of electrolytes for electrocatalytic nitrogen reduction toward ammonia. Chinese Chemical Letters, 2024, 35(4): 108550-. doi: 10.1016/j.cclet.2023.108550
20. [20]
  Hong-Rui Li , Xia Kang , Rui Gao , Miao-Miao Shi , Bo Bi , Ze-Yu Chen , Jun-Min Yan . Interfacial interactions of Cu/MnOOH enhance ammonia synthesis from electrochemical nitrate reduction. Chinese Chemical Letters, 2025, 36(2): 109958-. doi: 10.1016/j.cclet.2024.109958

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(7)
HTML views(1)

通讯作者: 陈斌, bchen63@163.com

1.
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

Metrics

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