Boosting faradaic efficiency of CO_(2)electroreduction to CO for Fe-NC single-site catalysts by stabilizing Fe^(3+)sites via F-doping
作者机构：Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Lab for NanotechnologySchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China
出 版 物：《Nano Research》 (纳米研究（英文版）)
年 卷 期：2022年第15卷第9期
页 面：7896-7902页
核心收录：
学科分类：07[理学] 070304[理学-物理化学(含∶化学物理)] 0703[理学-化学]
基 金：the National Key Research and Development Program of China(Nos.2021YFA1500900,2017YFA0206500,and 2018YFA0209103) the National Natural Science Foundation of China(Nos.21832003,21972061,and 52071174) the Natural Science Foundation of Jiangsu Province,Major Project(No.BK20212005) Nanjing University Innovation Program for PhD candidate(No.CXYJ21-38).
主 题：carbon dioxide electroreduction iron-nitrogen-carbon single-site catalysts fluorine-doping active site regulation
摘 要：The atomically dispersed Fe^(3+)sites of Fe-N-C single-site catalysts(SSCs)are demonstrated as the active sites for CO_(2)electroreduction(CO_(2)RR)to CO but suffer from the reduction to Fe^(2+)at~−0.5 V,accompanied by the drop of CO faradaic efficiency(FECO)and deterioration of partial current(JCO).Herein,we report the construction of F-doped Fe-N-C SSCs and the electron-withdrawing character of fluorine could stabilize Fe3+sites,which promotes the FECO from the volcano-like highest value(88.2%@−0.40 V)to the high plateau(88.5%@−0.40-−0.60 V),with a much-increased JCO(from 3.24 to 11.23 mA·cm^(−2)).The enhancement is ascribed to the thermodynamically facilitated CO_(2)RR and suppressed competing hydrogen evolution reaction,as well as the kinetically increased electroactive surface area and improved charge transfer,due to the stabilized Fe^(3+)sites and enriched defects by fluorine doping.This finding provides an efficient strategy to enhance the CO_(2)RR performance of Fe-N-C SSCs by stabilizing Fe^(3+).
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