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通过人工光合作用在缺陷石墨相氮化碳上生产过氧化氢

HO Production via Artificial Photosynthesis Over Defective Graphitic Carbon Nitride.

作者信息

Zhang Yiwen, Wu Dingle, Zeng Xiaofei, Qiu Bocheng, Zhu Qiaohong, Zhang Jinlong

机构信息

Key Laboratory of Organosilicon Chemistry and Material Technology, Ministry of Education, Zhejiang Key Laboratory of Organosilicon Material Technology, College of Material, Chemistry and Chemical Engineering, Hangzhou Normal University, Hangzhou, Zhejiang, 311121, China.

Jiangsu Key Laboratory of Pesticide Sciences, Department of Chemistry, College of Sciences, Nanjing Agricultural University, Nanjing, 210095, China.

出版信息

Adv Sci (Weinh). 2025 Sep;12(33):e07913. doi: 10.1002/advs.202507913. Epub 2025 Aug 12.

Abstract

Metal-free graphitic carbon nitride has been considered as a promising candidate for hydrogen peroxide (HO) photosynthesis, with the advantage of low-cost, high stability, and environmentally friendly capacity. However, such a solar-to-chemical conversion still suffers from limited light utilization, confined surface adsorption, and restricted reduction/oxidation reaction pathway. At this juncture, this bottleneck has been overcome through diverse modifications over carbon nitride, such as defect engineering graphitic carbon nitride with modulated physical and chemical properties, which performs satisfactory visible-light absorption, sufficient active sites, and promotes charge transfer kinetics for artificial solar-to-chemical conversion. In this review, the recent advances for HO photosynthesis over defective graphitic carbon nitride are described, including the existing principles for HO formation, the factors affecting photosynthesis, the fabrication strategies toward novel materials, and the detailed pathways for HO formation. The functions of defects, the properties of materials, and the reaction mechanisms, and the selectivity, as well as in situ characterizations for catalyst synthesis and pathway exploration, have been summarized clearly. Finally, the advantages and shortcomings, together with the challenges and prospects, are highlighted for the development of defect engineering over carbon nitride for HO photosynthesis.

摘要

无金属的石墨相氮化碳被认为是用于过氧化氢(H₂O₂)光合成的一种有前景的候选材料,具有低成本、高稳定性和环境友好的优势。然而,这种太阳能到化学能的转换仍然存在光利用有限、表面吸附受限以及还原/氧化反应途径受限的问题。在这个时候,通过对氮化碳进行多种修饰克服了这一瓶颈,例如对具有调制物理和化学性质的石墨相氮化碳进行缺陷工程,其具有令人满意的可见光吸收、足够的活性位点,并促进人工太阳能到化学能转换的电荷转移动力学。在这篇综述中,描述了在有缺陷的石墨相氮化碳上进行H₂O₂光合成的最新进展,包括H₂O₂形成的现有原理、影响光合成的因素、新型材料的制备策略以及H₂O₂形成的详细途径。缺陷的功能、材料的性质、反应机制、选择性以及催化剂合成和途径探索的原位表征都已被清晰总结。最后,强调了在用于H₂O₂光合成的氮化碳缺陷工程发展方面的优点和缺点,以及挑战与前景。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3764/12412509/ff73e7a8f393/ADVS-12-e07913-g001.jpg

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