文献类型：期刊文献

英文题名：Metal-organic framework derived single-atom catalysts for electrochemical CO2 reduction

作者：Xie, Mengna[1,2];Wang, Jiawei[1,2];Du, Xian-Long[1,3,4];Gao, Na[1,4];Liu, Tao[5];Li, Zhi[5];Xiao, GuoPing[1,3,4];Li, Tao[2];Wang, Jian-Qiang[1,3,4]

机构：[1]Chinese Acad Sci, Shanghai Inst Appl Phys, Key Lab Interfacial Phys & Technol, Shanghai 201800, Peoples R China;[2]East China Univ Sci & Technol, State Key Lab Chem Engn, Minist Educ, Engn Res Ctr Large Scale Reactor Engn & Technol, Shanghai 200237, Peoples R China;[3]Univ Chinese Acad Sci, Beijing 100049, Peoples R China;[4]Chinese Acad Sci, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China;[5]Shandong Energy Grp Co Ltd, Jinan 250014, Peoples R China

年份：2022

卷号：12

期号：50

起止页码：32518

外文期刊名：RSC ADVANCES

收录：;EI(收录号：20225013226751);WOS:【SCI-EXPANDED(收录号:WOS:000885099000001)】；

基金：This work was partly supported by the Transformational Technologies for Clean Energy and Demonstration Strategic Priority Research Program of the Chinese Academy of Sciences (XDA2100000), the Youth Innovation Promotion Association of the Chinese Academy of Sciences (2018298), the Young Potential Program of Shanghai Institute of Applied Physics, Chinese Academy of Sciences (E055300101), the Major Scientific and Technological Innovation Project of Shandong Province (2020CXGC010402).

语种：英文

外文关键词：Carbon - Carbon dioxide - Catalyst activity - Catalyst selectivity - Copper compounds - Doping (additives) - Electrolytic reduction - High resolution transmission electron microscopy - Iron compounds - Manganese compounds - Metal ions - Nickel compounds - Nitrogen - Organometallics - Pyrolysis - Scanning electron microscopy - Transition metals - X ray photoelectron spectroscopy

摘要：With maximum atomic utilization, transition metal single atom catalysts (SACs) show great potential in electrochemical reduction of CO2 to CO. Herein, by a facile pyrolysis of zeolitic imidazolate frameworks (ZIFs) assembled with tiny amounts of metal ions, a series of metal-nitrogen-carbon (M-N-C) based SACs (M = Fe, Ni, Mn, Co and Cu), with metal single atoms decorated on a nitrogen-doped carbon support, have been precisely constructed. X-ray photoelectron spectroscopy (XPS) for M-N-C showed that the N 1s spectrum was deconvoluted into five peaks for pyridinic (similar to 398.3 eV), M-N coordination (similar to 399.6 eV), pyrrolic (similar to 400.4 eV), quaternary (similar to 401.2 eV) and oxidized (similar to 402.9 eV) N species, demonstrating the existence of M-N bonding. High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) indicates homogeneous distribution of metal species throughout the N-doped carbon matrix. Among the catalysts examined, the Fe-N-C catalyst exhibits the best catalytic performance in electrocatalytic CO2 reduction reaction (CO2RR) with nearly 100% faradaic efficiency for CO (FECO) at -0.9 V vs. the reversible hydrogen electrode (RHE). Ni-N-C is the second most active catalyst towards CO2RR performance, then followed by Mn-N-C, Co-N-C and Cu-N-C. Considering the optimum activity of Fe-N-C catalyst for the CO2RR, we then further investigate the effect of pyrolysis temperature on CO2RR of the Fe-N-C catalyst. We find the Fe-N-C catalyst pyrolyzed at 1000 degrees C exhibits the best catalytic activity in CO2RR with excellent CO selectivity.