Study on the Nitrogen Vacancy in Carbon Nitride Photocatalysts for Visible-Light-Driven H2O2 Production

doi:10.6023/A26020041

Abstract

Photocatalytic H₂O₂ production is a green, safe, efficient and low-cost synthesis process, and carbon nitride is considered one of the most promising photocatalysts for this purpose. However, its high recombination rate of photogenerated electron-hole pairs and weak O₂ adsorption capacity result in poor performance in H₂O₂ production. In this study, three carbon nitrides of C₃N₄, C₂N₃ and C₃N₅ were synthesized via a one-step calcination route with different precursors and calcination parameters. Among them, the C₂N₃ photocatalyst was obtained by adding 1 g of 3-amino-1,2,4-triazole into a covered crucible, heating to 550 ℃ in a muffle furnace at a heating ramp of 5 ℃•min⁻¹ and maintaining this temperature for 3 h. It was found that C₂N₃ exhibited excellent capability of photocatalytic H₂O₂ production. Under ambient oxygen atmosphere and visible light (λ>420 nm) irradiation, the production yield of H₂O₂ reached 247.31 μmol•g⁻¹ after 3 h of irradiation, which was 3.29 times that of C₃N₄ and 2.33 times that of C₃N₅. Specific surface area analyzer and electron paramagnetic resonance (EPR) confirmed that the C₂N₃ catalyst possessed a large specific surface area, and was rich in nitrogen vacancies. Theoretical calculations revealed that nitrogen vacancy could serve as active site, enhancing the O₂ adsorption capacity of the catalyst, thereby promoting photocatalytic H₂O₂ production. Additionally, UV-Vis diffuse reflectance spectroscopy (UV-Vis DRS), photoluminescence (PL), electrochemical impedance spectroscopy (EIS), and photocurrent response tests indicated that C₂N₃ had a suitable band gap of 1.98 eV, which not only facilitated visible light absorption, but also effectively suppressed the recombination of photogenerated carriers, thus improving the efficiency of visible-light-driven photocatalytic reactions. Mechanistic analysis demonstrated that the adsorbed O₂ was reduced by photogenerated electrons to form •O₂⁻, which could subsequently be converted into H₂O₂ through two distinct pathways. This research provides new insights into the design and fabrication of low-cost, high-performance photocatalysts, and sheds fresh light on the exploration and development of clean-energy fields.

Key words: carbon nitride, visible-light photocatalysis, H₂O₂ production, nitrogen vacancy, dual-channel mechanism

Cite this article

Zijie Zeng, Ziling Peng, Chen Wang, Fatang Tan, Xinyun Wang, Po Keung Wong, Wei Wang. Study on the Nitrogen Vacancy in Carbon Nitride Photocatalysts for Visible-Light-Driven H₂O₂ Production[J]. Acta Chimica Sinica, 2026, 84(6): 879-887.

Export EndNote|Reference Manager|ProCite|BibTeX|RefWorks

share this article

Fig. & Tab. 7

Figure 1. Preparation processes and SEM images of C3N4, C2N3 and C3N5

Figure 2. EPR spectra of C3N4, C2N3 and C3N5

Figure 3. XRD patterns (a), FT-IR spectra (b), C 1s XPS spectra (c) and N 1s XPS spectra (d) of C3N4、C2N3和C3N5

Figure 4. UV-Vis DRS spectra (a), Tauc plots (b), PL spectra (c), EIS patterns (d), and photocurrent responses (e) of C3N4, C2N3, and C3N5

Figure 5. Photocatalytic H2O2 production yields of C3N4, C2N3, and C3N5 (a), reuse experiment of C2N3 (b), EPR spectra (c) and photocatalytic H2O2 production yield (d) of C2N3-Ar

Figure 6. Comparison of H2O2 production yields by C2N3 in air and Ar (a), the O2 adsorption model of C2N3 without nitrogen vacancies (b) and C2N3 with nitrogen vacancies (c)

Figure 7. Effects of different scavengers on photocatalytic H2O2 production by C2N3 (a), EPR spectra of DMPO-•O2− (b) and TEMP-1O2 (c) over C2N3, schematic diagram of the reaction pathway for photocatalytic H2O2 production by C2N3 (d)

References 52

[1]	He, F. T.; Lu, Y. M.; Wu, Y. Z.; Wang, S. L.; Zhang, Y.; Dong, P.; Wang, Y. Q.; Zhao, C. C.; Wang, S. J.; Zhang, J. Q.; Wang, S. B. Adv. Mater. 2023, 36, 2307490. doi: 10.1002/adma.v36.9
[2]	Yan, S. R.; Liu, W. H.; Duan, F.; Chen, M. Q.; Dong, W. F.; Lu, S. L.; Du, M. L. Acta Chim. Sinica 2025, 83, 685 (in Chinese). doi: 10.6023/A25030077
	(闫生荣, 刘文浩, 段芳, 陈明清, 东为富, 陆双龙, 杜明亮, 化学学报, 2025, 83, 685.) doi: 10.6023/A25030077
[3]	Tong, H. J.; Odutola, J.; Song, J. S.; Peng, L.; Tkachenko, N.; Antonietti, M.; Pelicano, C. M. Adv. Mater. 2024, 36, 2412753. doi: 10.1002/adma.v36.49
[4]	Tian, T.; Shen, Q.; Yuan, Y.; Wang, J.; Yang, X. N.; Jiang, D. C.; Zhu, C. H.; Xu, G. S.; Yuan, Y. P. Appl. Catal., B 2025, 378, 125567. doi: 10.1016/j.apcatb.2025.125567
[5]	Ma, J.; Peng, C.; Peng, X. X.; Liang, S. C.; Zhou, Z. X.; Wu, K. Q.; Chen, R.; Liu, S. Q.; Shen, Y. F.; Ma, H. B.; Zhang, Y. J. J. Am. Chem. Soc. 2024, 146, 21147. doi: 10.1021/jacs.4c07170
[6]	Chai, H.; Nan, J.; Jin, W. X.; Wu, F. M.; Liu, B. H.; Guo, Y. Chem. Eng. J. 2024, 489, 151293. doi: 10.1016/j.cej.2024.151293
[7]	Ma, J.; Peng, X. X.; Zhou, Z. X.; Yang, H.; Wu, K. Q.; Fang, Z. Z.; Han, D.; Fang, Y. F.; Liu, S. Q.; Shen, Y. F.; Zhang, Y. J. Angew. Chem., Int. Ed. 2022, 61, 202210856.
[8]	Wang, Y. K.; Xu, Y. T.; Zhang, X. R.; Qian, R.; Chen, X.; Chen, Q.; Wu, X. F.; Fang, Y. X. Small 2025, 21, 2501656. doi: 10.1002/smll.v21.21
[9]	Chen, Q. C.; Ning, C.; Fang, J. W.; Ping, B. Y.; Li, G. Y.; Kong, L. Q.; Chen, J. Y.; Sun, Z. M.; Wang, J. L.; Ruan, Q. S.; Niu, X. H.; Tao, L. Chem. Eng. J. 2024, 487, 150581. doi: 10.1016/j.cej.2024.150581
[10]	Choi, J. W.; Byeon, A.; Kim, S.; Hwang, C. K.; Zhang, W. J.; Lee, J.; Yun, W. C.; Paek, S. Y.; Kim, J. H.; Jeong, G.; Lee, S. Y.; Moon, J.; Han, S. S.; Lee, J. W.; Kim, J. M. Adv. Mater. 2025, 37, 2415712. doi: 10.1002/adma.v37.9
[11]	Yan, H. J.; Peng, Y.; Huang, Y. Y.; Shen, M. H.; Wei, X. Q.; Zou, W. X.; Tong, Q.; Zhou, N. B.; Xu, J. Q.; Zhang, Y. X.; Ye, Y. X.; Ouyang, G. F. Adv. Mater. 2024, 36, 2311535. doi: 10.1002/adma.v36.18
[12]	Yu, X. H.; Hu, Y. P.; Shao, C. C.; Huang, W.; Li, Y. G. Mater. Today 2023, 71, 152. doi: 10.1016/j.mattod.2023.10.005
[13]	Liu, Y.; Li, M.; Liu, T.; Wu, Z.; Zhang, L. Y. J. Mater. Sci. Technol. 2025, 233, 201. doi: 10.1016/j.jmst.2025.03.005
[14]	Shan, T. S.; Wang, Y.; Luo, D.; Huang, Z. C.; Zhang, F. S.; Wu, H.; Huang, L. L.; Li, J. D.; Chen, L. H.; Xiao, H. Appl. Catal., B 2024, 349, 123872. doi: 10.1016/j.apcatb.2024.123872
[15]	Seo, D.; Somjit, V.; Wi, D. H.; Galli, G.; Choi, K. S. J. Am. Chem. Soc. 2025, 147, 3261. doi: 10.1021/jacs.4c13290
[16]	Meng, K.; Zhang, J. J.; Cheng, B.; Ren, X. G.; Xia, Z. S.; Xu, F. Y.; Zhang, L. Y.; Yu, J. G. Adv. Mater. 2024, 36, 2406460. doi: 10.1002/adma.v36.32
[17]	Li, Y. H.; Gu, M. L.; Zhang, X. M.; Fan, J. J.; Lv, K. L.; Carabineiro, S. A. C.; Dong, F. Mater. Today 2020, 41, 270. doi: 10.1016/j.mattod.2020.09.004
[18]	Yuan, S. J.; Dai, L. H.; Xie, M. F.; Liu, J. Y.; Peng, H. J. Chem. Eng. Sci. 2024, 296, 120245. doi: 10.1016/j.ces.2024.120245
[19]	Wang, W. K.; Zhang, H. M.; Zhang, S. B.; Liu, Y. Y.; Wang, G. Z.; Sun, C. H.; Zhao, H. J. Angew. Chem., Int. Ed. 2019, 58, 16644. doi: 10.1002/anie.v58.46
[20]	Zhou, X.; Yang, S. Y.; Wang, X. J.; Wu, Z.; Huo, Y. T.; Zhang, J. J. J. Mater. Sci. Technol. 2025, 234, 60. doi: 10.1016/j.jmst.2025.02.027
[21]	Zhou, S.; Wen, D.; Zhong, W.; Zhang, J. J.; Su, Y. R.; Meng, A. Y. J. Mater. Sci. Technol. 2024, 199, 53. doi: 10.1016/j.jmst.2024.02.048
[22]	Zhang, Q. Q.; Wang, B.; Miao, H.; Fan, J.; Sun, T.; Liu, E. Z. Chem. Eng. J. 2024, 482, 148844. doi: 10.1016/j.cej.2024.148844
[23]	Du, R. F.; Xiao, K.; Li, B. Y.; Han, X.; Zhang, C. Q.; Wang, X.; Zuo, Y.; Guardia, P.; Li, J. S.; Chen, J. B.; Arbiol, J.; Cabot, A. Chem. Eng. J. 2022, 441, 135999. doi: 10.1016/j.cej.2022.135999
[24]	Li, S. N.; Dong, G. H.; Hailili, R.; Yang, L. P.; Li, Y. X.; Wang, F.; Zeng, Y. B.; Wang, C. Y. Appl. Catal., B 2016, 190, 26. doi: 10.1016/j.apcatb.2016.03.004
[25]	Ma, J.; Peng, X. X.; Zhou, Z. X.; Shen, Y. F.; Zhang, Y. J. Chin. Chem. Lett. 2023, 34, 108784. doi: 10.1016/j.cclet.2023.108784
[26]	Zhao, C.; Shi, C. J.; Li, Q.; Wang, X. Y.; Zeng, G.; Ye, S.; Jiang, B. J.; Liu, J. Mater. Today Energy 2021, 24, 100926.
[27]	Peng, C.; Han, L. X.; Huang, J. M.; Wang, S. Y.; Zhang, X. H.; Chen, H. Chin. J. Catal. 2022, 43, 410. doi: 10.1016/S1872-2067(21)63813-5
[28]	Tang, D. M.; Shao, C. T.; Jiang, S. J.; Sun, C. Z.; Song, S. Q. ACS Nano 2021, 15, 7208. doi: 10.1021/acsnano.1c00477
[29]	Tang, R. D.; Gong, D. X.; Zhou, Y. Y.; Deng, Y. C.; Feng, C. Y.; Xiong, S.; Huang, Y.; Peng, G. W.; Li, L. Appl. Catal., B 2022, 303, 120929. doi: 10.1016/j.apcatb.2021.120929
[30]	Xu, Y.; Wang, G. H.; Li, W.; Yuan, Z. H.; Si, C. L. Chem. Eng. J. 2025, 503, 158655. doi: 10.1016/j.cej.2024.158655
[31]	Li, J. S.; Li, Y. X.; Wei, S. C.; Wu, S. Y.; Peng, Z. Y.; Zhang, F. S.; Huang, L. L.; Chen, L. H.; Li, J. D.; Xiao, H. Appl. Catal., B 2025, 366, 125073. doi: 10.1016/j.apcatb.2025.125073
[32]	Zheng, C. J.; Guo, Y. B.; Zhang, C. J.; Cao, X. J.; Wan, J. F. Appl. Catal., B 2025, 365, 124879. doi: 10.1016/j.apcatb.2024.124879
[33]	Chu, C. C.; Miao, W.; Li, Q. J.; Wang, D. D.; Liu, Y.; Mao, S. Chem. Eng. J. 2022, 428, 132531. doi: 10.1016/j.cej.2021.132531
[34]	Xiong, T.; Cen, W. L.; Zhang, Y. X.; Dong, F. ACS Catal. 2016, 6, 2462. doi: 10.1021/acscatal.5b02922
[35]	Zhang, W. B.; Zhang, Z. J.; Kwon, S.; Zhang, F. C.; Stephen, B.; Kim, K. K.; Jung, R.; Kwon, S.; Chung, K. B.; Yang, W. Appl. Catal., B 2017, 206, 271. doi: 10.1016/j.apcatb.2017.01.034
[36]	Huang, G. Z.; Li, K. W.; Luo, Y. N.; Zhang, Q.; Pan, Y. L.; Gao, H. L. Acta Chim. Sinica 2024, 82, 314 (in Chinese). doi: 10.6023/A23110484
	(黄广峥, 李坤玮, 罗艳楠, 张强, 潘远龙, 高洪林, 化学学报, 2024, 82, 314.) doi: 10.6023/A23110484
[37]	Qin, X.; Zhang, L.; Xu, M. Y.; Li, R. F.; Jia, T. K.; Zhang, C. Q.; Wang, W. J.; Che, C. Y.; Jiang, B.; Xu, S. Y.; Wang, J.; Wang, W. Z. Appl. Catal., B 2025, 362, 124723. doi: 10.1016/j.apcatb.2024.124723
[38]	Cai, Y. W.; Fang, M.; Xu, Y.; Wakeel, M.; Hu, B. W.; Wang, X. K. Chem. Eng. J. 2025, 518, 164670. doi: 10.1016/j.cej.2025.164670
[39]	Pawar, O. Y.; Li, H.; Patil, O. A.; Xu, J. K.; Dongale, T. D.; Lu, B. Y.; Lim, S. Chem. Eng. J. 2025, 519, 165069. doi: 10.1016/j.cej.2025.165069
[40]	Babu, B.; Shim, J.; Kadam, A. N.; Yoo, K. Catal. Commun. 2019, 124, 123. doi: 10.1016/j.catcom.2019.01.009
[41]	Liu, H. H.; Chen, D. L.; Wang, Z. Q.; Jing, H. J.; Zhang, R. Appl. Catal., B 2017, 203, 300. doi: 10.1016/j.apcatb.2016.10.014
[42]	Asghar, Z.; Jrar, J. A.; Alauddin; Butt, F. K.; Wang, X. Z.; Tahir, M.; Zheng, K. W.; Zhang, Y. C.; Hou, J. H. Renew. Energy 2026, 257, 124741. doi: 10.1016/j.renene.2025.124741
[43]	Liu, L. L.; Chen, F.; Wu, J. H.; Ke, M. K.; Cui, C.; Chen, J. J.; Yu, H. Q. Appl. Catal., B 2022, 302, 120845. doi: 10.1016/j.apcatb.2021.120845
[44]	Luo, J.; Liu, Y. N.; Fan, C. Z.; Tang, L.; Yang, S. J.; Liu, M. L.; Wang, M. E.; Feng, C. Y.; Ouyang, X. L.; Wang, L. L.; Xu, L.; Wang, J. J.; Yan, M. ACS Catal. 2021, 11, 11440. doi: 10.1021/acscatal.1c03103
[45]	Ma, L. X.; Gao, Y. P.; Wei, B. Q.; Huang, L.; Zhang, N.; Weng, Q.; Zhang, L.; Liu, S. Z.; Jiang, R. B. ACS Catal. 2024, 14, 2775. doi: 10.1021/acscatal.3c05360
[46]	Zhang, X.; Ma, P. J.; Wang, C.; Gan, L. Y.; Chen, X. J.; Zhang, P.; Wang, Y.; Li, H.; Wang, L. H.; Zhou, X. Y.; Zheng, K. Energy Environ. Sci. 2022, 15, 830. doi: 10.1039/D1EE02369A
[47]	Zhu, Y. L.; Liu, X. T.; Liu, H.; He, G. L.; Xiao, J. M.; Xie, H. J.; Sun, Y. Y.; Han, L. SusMat 2022, 2, 617. doi: 10.1002/sus2.v2.5
[48]	Li, J. M.; Xu, N.; Zhang, Y. F.; Dong, H. J.; Li, C. M. Chin. Chem. Lett. 2025, 36, 110470. doi: 10.1016/j.cclet.2024.110470
[49]	Wang, D. H.; Elmansour, H.; Li, S. L.; Zhang, H. Y.; Fu, Y. H.; Chen, F. Chem. Eng. J. 2025, 515, 163232. doi: 10.1016/j.cej.2025.163232
[50]	Chen, Z.; Yao, D. C.; Chu, C. C.; Mao, S. Chem. Eng. J. 2023, 451, 138489. doi: 10.1016/j.cej.2022.138489
[51]	Yang, J. D.; Zeng, X. K.; Tebytekerwa, M.; Wang, Z. Y.; Bie, C. B.; Sun, X.; Marriam, I.; Zhang, X. W. Adv. Energy Mater. 2024, 14, 2400740. doi: 10.1002/aenm.v14.23
[52]	Jiang, Z. C.; Long, Q.; Cheng, B.; He, R. A.; Wang, L. X. J. Mater. Sci. Technol. 2023, 162, 1. doi: 10.1016/j.jmst.2023.03.045

氮化碳的氮空位与可见光催化产H₂O₂研究

Study on the Nitrogen Vacancy in Carbon Nitride Photocatalysts for Visible-Light-Driven H₂O₂ Production

RichHTML

PDF

Supporting Info.

Knowledge

Abstract

Cite this article

share this article

Fig. & Tab. 7

References 52

Related Articles 14

Recommended Articles

Metrics

Comments

[1]	Huiying Chen, Ningyu Huang, Peiqin Liao. A Novel Silver-Carbon Bond-Engineered Metal-Organic Framework toward Efficient Artificial Photosynthesis of Hydrogen Peroxide^★ [J]. Acta Chimica Sinica, 2026, 84(5): 626-630.
[2]	Chencheng Wang, Banlai Ouyang, Pinyong Zhong, Yingrong Zhang, Jinbiao Liu. Photocatalyzed Desulfurative Cyclization of 2-Aminobenzyl Alcohols and Isothiocyanates for the Synthesis of 2-Amino-1,3-Benzoxazines [J]. Acta Chimica Sinica, 2026, 84(1): 1-7.
[3]	Qionghui Peng, Jia Peng, Yingli Cai, Zuli Wang, Rongnan Yi, Chao Shen, Weimin He. Ph₂O-Mediated CeO₂-Photocatalyzed Semi-Heterogeneous Fluoroalkylation of 2-Isocyanobiaryls [J]. Acta Chimica Sinica, 2025, 83(9): 1013-1017.
[4]	Yue Zeng, Xiao Tang, Yuzhi Zhou, Yanhong Li, Chuan Jing, Faling Ling, Hongmei Yang, Xianju Zhou. Study on Factors Affecting Performance of C-Rich Carbon Nitride-based All-Solid-State Photo-Supercapacitor [J]. Acta Chimica Sinica, 2025, 83(5): 488-497.
[5]	Guangzheng Huang, Kunwei Li, Yannan Luo, Qiang Zhang, Yuanlong Pan, Honglin Gao. Hydrothermal Treatment for Constructing K Doping and Surface Defects in g-C₃N₄ Nanosheets Promote Photocatalytic Hydrogen Production [J]. Acta Chimica Sinica, 2024, 82(3): 314-322.
[6]	Zhongshu Xie, Zhongxin Xue, Ziwen Xu, Qian Li, Hongyu Wang, Wei-Shi Li. Conjugated Crosslinking Modification of Graphitic Carbon Nitrides and Its Effect on Visible Light-Driven Photocatalytic Hydrogen Production [J]. Acta Chimica Sinica, 2022, 80(9): 1231-1237.
[7]	Yaru Wei, Jing Ma, Tingting Yuan, Jiawei Jiang, Yinli Duan, Juanqin Xue. Preparation and Adsorption Properties of Lithium Chloride Intercalation Carbon Nitride [J]. Acta Chimica Sinica, 2022, 80(4): 494-502.
[8]	Min Yang, Baibai Ye, Jianqiang Chen, Jie Wu. Visible-light Photocatalytic Alkylsulfonylation of Aroylhydrazides with Alkylsulfonyl Radicals [J]. Acta Chimica Sinica, 2022, 80(1): 11-15.
[9]	Lirong He, Xiao Tang, Ling Zhang, Yanhong Li, Guotao Xiang, Xianju Zhou, Faling Ling, Lu Yao, Hao Jiang. Study on Photoelectrochemical Properties of Colorful Carbon Nitrides Synthesized in Liquid-Phase [J]. Acta Chimica Sinica, 2021, 79(4): 506-512.
[10]	Dong Kui, Liu Qiang, Wu Li-Zhu. Cross-Coupling Hydrogen Evolution Reactions [J]. Acta Chimica Sinica, 2020, 78(4): 299-310.
[11]	Chen, Yilin, Chang, Liang, Zuo, Zhiwei. Visible Light Photoredox-Induced Smiles Rearrangement [J]. Acta Chimica Sinica, 2019, 77(9): 794-802.
[12]	Dai, Jianling, Lei, Wenlong, Liu, Qiang. Visible-Light-Driven Difluoroalkylation of Aromatics Catalyzed by Copper [J]. Acta Chimica Sinica, 2019, 77(9): 911-915.
[13]	Liu Ruxue, He Xiaoyan, Niu Litong, Lv Bolin, Yu Fei, Zhang Zhe, Yang Zhiwang. Hierarchical In₂S₃/CdIn₂S₄ Heterostructured Nanohybrids as Photocatalyst for Coupling of Benzyl Amines under Visible Light [J]. Acta Chim. Sinica, 2019, 77(7): 653-660.
[14]	Ma Yali, Liu Ruxue, Meng Shuangyan, Niu Litong, Yang Zhiwang, Lei Ziqiang. Preparation and Photocatalytic Activity of Fe-ZrO₂ Composites from UiO-66 Precursor under Visible Light Irritation [J]. Acta Chimica Sinica, 2019, 77(2): 153-159.

氮化碳的氮空位与可见光催化产H2O2研究