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一种四吡啶铜(II)配合物将一氧化碳光催化转化为二氧化碳

Photocatalytic Conversion of CO to CO by a Copper(II) Quaterpyridine Complex.

作者信息

Guo Zhenguo, Yu Fei, Yang Ying, Leung Chi-Fai, Ng Siu-Mui, Ko Chi-Chiu, Cometto Claudio, Lau Tai-Chu, Robert Marc

机构信息

Institute of Molecular Functional Materials and Department of Chemistry, City University of Hong Kong, Tat Chee Avenue, Kowloon Tong, Hong Kong, P. R. China.

Department of Science and Environmental Studies, The Education University of Hong Kong, 10 Lo Ping Road, Tai Po, Hong Kong, P. R. China.

出版信息

ChemSusChem. 2017 Oct 23;10(20):4009-4013. doi: 10.1002/cssc.201701354. Epub 2017 Sep 13.

Abstract

The invention of efficient systems for the photocatalytic reduction of CO comprising earth-abundant metal catalysts is a promising approach for the production of solar fuels. One bottleneck is to design highly selective and robust molecular complexes that are able to transform the CO gas. The Cu quaterpyridine complex [Cu(qpy)] (1) is found to be a highly efficient and selective catalyst for visible-light driven CO reduction in CH CN using [Ru(bpy) ] (bpy: bipyridine) as photosensitizer and BIH/TEOA (1,3-dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]imidazole/triethanolamine) as sacrificial reductant. The photocatalytic reaction is greatly enhanced by the presence of H O (1-4 % v/v), and a turnover number of >12 400 for CO production can be achieved with 97 % selectivity, which is among the highest of molecular 3d CO reduction catalysts. Results from Hg poisoning and dynamic light scattering experiments suggest that this photocatalyst is homogenous. To the best of our knowledge, 1 is the first example of molecular Cu-based catalyst for the photoreduction of CO .

摘要

包含储量丰富的金属催化剂的高效光催化还原CO系统的发明,是一种生产太阳能燃料的有前景的方法。一个瓶颈是设计能够转化CO气体的高选择性且稳健的分子配合物。发现铜四吡啶配合物Cu(qpy)是一种高效且选择性的催化剂,用于在CH CN中以Ru(bpy) 作为光敏剂以及BIH/TEOA(1,3 - 二甲基 - 2 - 苯基 - 2,3 - 二氢 - 1H - 苯并[d]咪唑/三乙醇胺)作为牺牲还原剂进行可见光驱动的CO还原。H O(1 - 4 % v/v)的存在极大地增强了光催化反应,并且对于CO生成可以实现>12 400的周转数以及97 %的选择性,这在分子3d CO还原催化剂中是最高的之一。汞中毒和动态光散射实验的结果表明这种光催化剂是均相的。据我们所知,1是用于光还原CO的分子基铜催化剂的首个实例。

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