文献类型：期刊文献

英文题名：Local structure tuning in Fe-N-C catalysts through support effect for boosting CO2 electroreduction

作者：Tuo, Jinqin[1];Lin, Yunxiang[3];Zhu, Yihua[1];Jiang, Hongliang[2];Li, Yuhang[1];Cheng, Ling[1];Pang, Ruichao[1];Shen, Jianhua[1];Song, Li[3];Li, Chunzhong[1,2]

机构：[1]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn, Key Lab Ultrafine Mat,Minist Educ, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]Univ Sci & Technol China, CAS Ctr Excellence Nanosci, Natl Synchrotron Radiat Lab, Hefei 230029, Anhui, Peoples R China

年份：2020

卷号：272

外文期刊名：APPLIED CATALYSIS B-ENVIRONMENTAL

收录：;EI(收录号：20201708508173);WOS:【SCI-EXPANDED(收录号:WOS:000533148700034)】；

基金：This work was supported by the National Natural Science Foundation of China (21676093, 21838003, 21776092, 21808061, 91834301), the Shanghai Scientific and Technological Innovation Project (18JC1410500), the Social Development Program of Shanghai (17DZ1200900), the Innovation Program of Shanghai Municipal Education Commission, and the Fundamental Research Funds for the Central Universities (222201718002).

语种：英文

外文关键词：Support effect; Carbon nanotube; Single atom; Fe-N coordination; CO2 electroreduction

摘要：Metal-N-C materials have attracted considerable attention for electrocatalytic CO2 reduction. Local electronic and geometric structure of active sites in the metal-N-C catalysts significantly determine catalytic reactivity. In this work, atomically dispersed Fe species with different coordination environment are anchored into carbon supports through introducing aminated carbon nanotubes, as effectively revealed by the Cs-corrected transmission electron microscope and X-ray absorption near edge structure spectra. Electrochemical tests show that the catalyst with the aminated carbon nanotubes has a low overpotential (0.39 V) and high selectivity of CO up to 95.47 % at -0.6 V vs. RHE. The density functional theory calculation results indicate that the additional axial Fe-N coordination compared with the planar Fe-N coordination can reduce the free energy required for the desorption of CO from the adsorption site and inhibit the occurrence of hydrogen evolution reaction, thus leading to improve the selectivity of CO.