文献类型：期刊文献

英文题名：Covalently Grafting Cobalt Porphyrin onto Carbon Nanotubes for Efficient CO2 Electroreduction

作者：Zhu, Minghui[1];Chen, Jiacheng[1];Huang, Libei[2];Ye, Ruquan[2];Xu, Jing[1];Han, Yi-Fan[1,3]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]City Univ Hong Kong, Dept Chem, Hong Kong 999077, Peoples R China;[3]Zhengzhou Univ, Sch Chem Engn & Energy, Res Ctr Heterogeneous Catalysis & Engn Sci, Zhengzhou 450001, Henan, Peoples R China

年份：2019

卷号：58

期号：20

起止页码：6595

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20190806519042);WOS:【SCI-EXPANDED(收录号:WOS:000471977400019)】；

基金：We gratefully acknowledge the National Key R&D Program of China (2018YFB0605803), the National Natural Science Foundation of China (21576084), and the Fundamental Research Funds for the Central Universities (222201718002). M.Z. thanks the Start-up Grant of the East China University of Science and Technology (SG1503A003). L.H. and R.Y. thank the Start-up Grant of the City University of Hong Kong (Project No. 7200600) and the CityU New Research Initiatives/Infrastructure Support from Central (APRC 9610426). We appreciate the generous help of the staff of the BL14W1 beamline at the Shanghai Synchrotron Radiation Facility (SSRF) in XAS experiments.

语种：英文

外文关键词：carbon nanotubes; CO2 reduction; electroreduction; grafting; porphyrin

摘要：Molecular complexes with inexpensive transition-metal centers have drawn extensive attention, as they show a high selectivity in the electrochemical conversion of CO2 to CO. In this work, we propose a new strategy to covalently graft cobalt porphyrin onto the surface of a carbon nanotube by a substitution reaction at the metal center. Material characterization and electrochemical studies reveal that the porphyrin molecules are well dispersed at a high loading of 10wt.%. As a result, the turnover frequency for CO formation is improved by a factor of three compared to traditional physically-mixed catalysts with the same cobalt content. This leads to an outstanding overall current density of 25.1mAcm(-2) and a Faradaic efficiency of 98.3% at 490mV overpotential with excellent long-term stability. This work provides an effective pathway for the improvement of the performance of electrocatalysts that could inspire rational design of molecular catalysts in the future.