文献类型：期刊文献

英文题名：Size-dependent selectivity of iron-based electrocatalysts for electrochemical CO2 reduction

作者：Xie, Mengna[1];Gao, Na[2,4];Xiao, GuoPing[2,3,4];Ge, Min[2,3,4];Du, Xian-Long[2,3,4];Mei, BingBao[2,3,5];Wang, Jian-Qiang[1,2,4];Li, Tao[1]

机构：[1]East China Univ Sci & Technol, Engn Res Ctr Large Scale Reactor Engn & Technol, State Key Lab Chem Engn, Minist Educ, Shanghai 200237, Peoples R China;[2]Chinese Acad Sci, Shanghai Inst Appl Phys, Key Lab Interfacial Phys & Technol, Shanghai 201800, 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]Chinese Acad Sci, Zhangjiang Natl Lab, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China

年份：2022

卷号：6

期号：3

起止页码：736

外文期刊名：SUSTAINABLE ENERGY & FUELS

收录：;EI(收录号：20220711637480);WOS:【SCI-EXPANDED(收录号:WOS:000738034500001)】；

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), and the Young Potential Program of Shanghai Institute of Applied Physics, Chinese Academy of Sciences (E055300101).

语种：英文

外文关键词：Atoms - Carbon dioxide - Doping (additives) - Iron - Particle size - Reduction - X ray absorption spectroscopy

摘要：Applying non-precious metal catalysts to electrocatalytic CO2 reduction (CO2R) to CO efficiently, rather than gold-based nanomaterials, is of practical significance. Here, we adopt zeolitic imidazolate frameworks (ZIFs) to assist the synthesis of Fe metal catalysts with various sizes, ranging from single atoms to over 100 nm. As a result, the CO2 reduction performance of Fe metal catalysts with different particle sizes is different. Dominantly, Fe single-atomic sites exhibit optimum activity in producing CO, presenting a current density of 46.5 mA cm(-2), with nearly 100% faradaic efficiency (FE) for CO (at -0.9 V vs. RHE), while the result for 7.6 nm Fe nanoparticles is slightly lower (ca. 92%). With further increasing the Fe particle size, the CO2RR performance weakens and allows the H-2 evolution reaction (HER), which demonstrates the size-dependent selectivity of iron-based electrocatalysts for electrochemical CO2 reduction. Operando X-ray absorption spectroscopy revealed the active sites to be discrete Fe2+ ions, coordinated to the pyrrolic nitrogen (N) atoms of the N-doped carbon support.