Men Yu-Long, You Ya, Pan Yun-Xiang, Gao Hongcai, Xia Yang, Cheng Dang-Guo, Song Jie, Cui Da-Xiang, Wu Nan, Li Yutao, Xin Sen, Goodenough John B
Institute of Nano Biomedicine and Engineering, Department of Instrument Science and Engineering, School of Electronic Information and Electrical Engineering , Shanghai Jiao Tong University , Shanghai 200240 , P. R. China.
Department of Mechanical Engineering , The University of Texas at Austin , Austin , Texas 78712 , United States.
J Am Chem Soc. 2018 Oct 10;140(40):13071-13077. doi: 10.1021/jacs.8b08552. Epub 2018 Oct 1.
A selective CO evolution from photoreduction of CO in water was achieved on a noble-metal-free, carbide-based composite catalyst, as demonstrated by a CO selectivity of 98.3% among all carbon-containing products and a CO evolution rate of 29.2 μmol h, showing superiority to noble-metal-based catalyst. A rapid separation of the photogenerated electron-hole pairs and improved CO adsorption on the surface of the carbide component are responsible for the excellent performance of the catalyst. The high CO selectivity is accompanied by a predominant H evolution, which is believed to provide a proton-deficient environment around the catalyst to favor the formation of hydrogen-deficient carbon products. The present work provides general insights into the design of a catalyst with a high product selectivity and also the carbon evolution chemistry during a photocatalytic reaction.
在一种无贵金属的碳化物基复合催化剂上实现了水中CO光还原的选择性CO析出,在所有含碳产物中CO选择性为98.3%,CO析出速率为29.2 μmol/h,显示出优于贵金属基催化剂的性能。光生电子-空穴对的快速分离以及碳化物组分表面CO吸附的改善是该催化剂优异性能的原因。高CO选择性伴随着主要的H析出,这被认为在催化剂周围提供了一个质子缺乏的环境,有利于形成缺氢碳产物。本工作为设计具有高产物选择性的催化剂以及光催化反应过程中的碳析出化学提供了一般性的见解。