| INORGANIC MATERIALS AND CERAMIC MATRIX COMPOSITES |
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| Optimizing the Photocatalytic Hydrogen Evolution Performance of Graphitic Carbon Nitride by Crystallinity Regulation |
| ZHAO Zhengliang1, SONG Zhenzhen2,3, SHU Zhu4,5,*, ZHOU Jun4,5
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1 College of Chemistry and Materials, Taiyuan Normal University, Jinzhong 030619, Shanxi, China 2 Institute of Geographical Science, Taiyuan Normal University, Jinzhong 030619, Shanxi, China 3 Shanxi Key Laboratory of Surface Processes and Resource Ecological Security in Fenhe River Basin, Taiyuan Normal University, Taiyuan 030619, China 4 MOE Engineering Research Center of Nano-Geomaterials, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430074, China 5 Hubei Three Gorges Laboratory, Yichang 443007, Hubei, China |
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Abstract Graphitic carbon nitride (g-C3N4) is a green and safe non-metallic photocatalyst. However, its photocatalytic activity is limited by the low efficiency of photo-generated carrier separation and transfer, while enhancing crystallinity can significantly improve the photocatalytic activity of carbon nitride. Therefore, in this study, a one-step calcination method was employed, using melamine as the precursor and regulating the molar ratios of NH4Cl and NaOH, to successfully synthesize sodium-doped crystalline carbon nitride (NaCCNx, where x refers to the molar ratio of NH4Cl to NaOH), achieving controllable modulation of both in-plane and interlayer crystallinity. Systematic material characterizations revealed that the crystallinity of NaCCNx was significantly enhanced, with NaCCN2.5 exhibiting the optimal in-plane and interlayer crystallinity, along with a substantial improvement in visible light absorption and charge carrier separation and transport efficiency. Under visible-light irradiation, NaCCN2.5 exhibited a superior photocatalytic hydrogen production rate of 1 848 μmol·g-1·h-1, which is 11.6-fold as high as that of bulk g-C3N4. This breakthrough not only confirms the crucial role of crystallinity regulation in enhancing photocatalytic performance, but also provides new ideas and experimental basis for designing efficient non-metallic photocatalysts.
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Published:
Online: 2026-02-13
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Corresponding Authors:
shuzhu@cug.edu.cn
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1 Wang X, Maeda K, Thomas A, et al. Nature Materials, 2009, 8(1), 76. 2 Zhu J, Ling M, Ma R, et al. Materials Reports, 2024, 38(11), 23010115 (in Chinese). 朱杰, 凌敏, 马润东, 等. 材料导报, 2024, 38(11), 23010115. 3 Liu L, Ou H, Zhang Y, et al. ACS Catalysis, 2016, 6(6), 3921. 4 Yang Y, Wang S, Jiao Y, et al. Advanced Functional Materials, 2018, 28(47), 1805698. 5 Schlomber H, Kroger J, Savasic G, et al. Chemistry of Materials, 2019, 31(18), 7478. 6 Chen L, Chen C, Yang Z, et al. Advanced Functional Materials, 2021, 31(46), 2105731. 7 Xu Y, Fan M, Yang W, et al. Advanced Materials, 2021, 33(39), e2101455. 8 Zhang G, Li G, Heil T, et al. Angewandte Chemie International Edition, 2019, 58(11), 3433. 9 Wang W, Shu Z, Zhou J, et al. Journal of Materials Chemistry A, 2020, 8(14), 6785. 10 Song Z, Gao H, Li J, et al. Journal of Water Process Engineering, 2025, 71, 107196. 11 Liu J, Zhao H, Li H, et al. Materials Reports, 2024, 38(21), 23070238 (in Chinese). 刘京津, 赵华, 李会鹏, 等. 材料导报, 2024, 38(21), 23070238. 12 Ma Y, Liu F, Liu Y, et al. Chemical Engineering Journal, 2021, 414, 128802. 13 Zhang G, Li G, Lan Z A, et al. Angewandte Chemie International Edition, 2017, 56(43), 13445. 14 Lin L, Ren W, Wang C, et al. Applied Catalysis B, 2018, 231, 234. 15 Wang Y, Zhao S, Zhang Y, et al. Applied Surface Science, 2018, 440, 258. 16 Zhu H, Zhao J, Duan L, et al. ACS Applied Materials & Interfaces, 2024, 16(5), 6008. 17 Zhang G, Liu L, Li G, et al. Angewandte Chemie International Edition, 2018, 57(30), 9372. 18 Zeng Z, Yu H, Quan X, et al. Applied Catalysis B, 2018, 227, 153. 19 Guo F, Hu B, Yang C, et al. Advanced Materials, 2021, 33(42), e2101466. 20 Zhong T, Tang S, Huang W B, et al. Applied Catalysis B, 2024, 343, 123476. 21 Liu Y, Wang G, Li Y, et al. Catalysis Science & Technology, 2022, 12(4), 1368. 22 Zhang G, Xu Y, Zhang P, et al. Advanced Functional Materials, 2024, 2315116. 23 Chueh L, Lin T, Leee H, et al. Small, 2024, 20, 2304813. 24 Zhang K, Liu C X, Liu Q, et al. Catalysts, 2023, 13, 717. 25 Zhang G, Xu Y, Zhu J, et al. Applied Catalysis B, 2023, 338, 123049. 26 Yu Q, Liu C, Jin T, et al. Materials Reports, 2024, 38(11), 22090279 (in Chinese). 于巧玲, 刘成宝, 金涛, 等. 材料导报, 2024, 38(11), 22090279. 27 Ji J, Wen J, Shen Y, et al. Journal of the American Chemical Society, 2017, 139(34), 11698. 28 Wang J, Li P, Wang Y, et al. Advanced Science, 2023, 10(5), 2205542. 29 Pelicano C M, Li J X, Cabrero-Antonino M, et al. Journal of Materials Chemistry A, 2023, 12(1), 475. 30 Li J, Barrio J, Fang Y X, et al. Energy & Fuels, 2023, 37(23), 18145. 31 Gao Y, Li Y X, Shanguan L, et al. Journal of Colloid and Interface Science, 2023, 644, 116. |
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