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金属有机骨架复合材料上光催化产氢与苄胺选择性氧化的耦合

Photocatalytic Hydrogen Production Coupled with Selective Benzylamine Oxidation over MOF Composites.

作者信息

Liu Hang, Xu Caiyun, Li Dandan, Jiang Hai-Long

机构信息

Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Soft Matter Chemistry, Collaborative Innovation Center of Suzhou Nano Science and Technology, Department of Chemistry, University of Science and Technology of China, Hefei, Anhui, 230026, P.R. China.

出版信息

Angew Chem Int Ed Engl. 2018 May 4;57(19):5379-5383. doi: 10.1002/anie.201800320. Epub 2018 Mar 30.

Abstract

Photocatalytic water splitting requires separation of the mixed H and O products and is often hampered by the sluggish O -producing half reaction. An approach is now reported to address these issues by coupling the H -producing half reaction with value-added benzylamine oxidation reaction using metal-organic framework (MOF) composites. Upon MOF photoexcitation, the electrons rapidly reduce the protons to generate H and the holes promote considerable benzylamine oxidation to N-benzylbenzaldimine with high selectivity. Further experimental characterizations and theoretical calculation reveal that the highly conjugated s-triazine strut in the MOF structure is crucial to the efficient charge separation and excellent photocatalytic activity.

摘要

光催化水分解需要分离混合的氢和氧产物,并且常常受到缓慢的析氧半反应的阻碍。现在报道了一种方法,通过使用金属有机框架(MOF)复合材料将析氢半反应与增值苄胺氧化反应耦合来解决这些问题。在MOF光激发后,电子迅速还原质子以产生氢气,空穴促进大量苄胺以高选择性氧化为N-苄基苯甲亚胺。进一步的实验表征和理论计算表明,MOF结构中高度共轭的s-三嗪支柱对于有效的电荷分离和优异的光催化活性至关重要。

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