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用于光催化析氢的改进的金属-配体电荷转移机制。

An Improved Metal-to-Ligand Charge Transfer Mechanism for Photocatalytic Hydrogen Evolution.

机构信息

College of Chemistry and Chemical Engineering, Jiangsu Key Laboratory of Environmental Engineering and Monitoring, Yangzhou University, 180 Si-Wang-Ting Road, Yangzhou, 225002, China.

Centre for Clean Energy Technology, Faculty of Science, University of Technology Sydney, Broadway, Sydney, NSW 2007, Australia.

出版信息

ChemSusChem. 2019 Sep 20;12(18):4221-4228. doi: 10.1002/cssc.201901609. Epub 2019 Aug 21.

DOI:10.1002/cssc.201901609
PMID:31364799
Abstract

It is of great significance to fabricate a full-spectrum-active photocatalysts for more efficient utilization of solar energy. An improved metal-to-ligand charge transfer (MLCT) mechanism is proposed for a photocatalyst based on graphitic carbon nitride (g-C N ). UV/Vis spectroscopy indicates that the as-prepared photocatalyst absorbs light at λ<1100 nm. The rather stable photocatalyst is found to be 26.1 times more active in photocatalytic hydrogen evolution (868.9 μmol h  g ) than bulk g-C N (B-CN) under visible light. The material exhibits high activity under near-infrared (NIR) irradiation (49.1 μmol h  g ). The mechanism of photocatalytic activity and stability are investigated by both experiment and theory. This proposed mechanism may have great potential for engineering renewable photocatalysts in the future.

摘要

制备全光谱活性光催化剂对于更有效地利用太阳能具有重要意义。本文提出了一种基于石墨相氮化碳(g-C3N4)的光催化剂的改进的金属-配体电荷转移(MLCT)机制。紫外-可见光谱表明,所制备的光催化剂在 λ<1100nm 处吸收光。实验发现,所制备的光催化剂在可见光下的光催化析氢活性(868.9 μmol h-1 g-1)比体相 g-C3N4(B-CN)高 26.1 倍。该材料在近红外(NIR)照射下表现出很高的活性(49.1 μmol h-1 g-1)。通过实验和理论研究了光催化活性和稳定性的机理。该提出的机制在未来可能具有很大的潜力来设计可再生光催化剂。

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