Identification of the optimal doping position of hetero-atoms in chalcogen-doped Fe-N-C catalysts for oxygen reduction reaction  

作　　者：Weihao Liu Huanhuan He Qingtao Liu Xin Wan Jianglan Shui 

机构地区：[1]School of Materials Science and Engineering,Beihang University,Beijing,100191,China [2]School of Space and Environment,Beihang University,Beijing,102206,China [3]Tianmushan Laboratory,Hangzhou,310023,China

出　　处：《Particuology》2024年第6期99-108,共10页颗粒学报（英文版）

基　　金：supported by the National Key Research and Development Program of China(grant No.2021YFB4000601);Natural Science Foundation of Beijing Municipality(grant No.Z200012);National Natural Science Foundation of China(grant No.21975010,U21A20328);the China Postdoctoral Science Foundation(grant No.2022M720013).

摘　　要：The excellent oxygen reduction reaction(ORR)activity of Fe–N–C catalysts in acidic media makes them potential for low-cost proton exchange membrane fuel cells.In recent years,it has been shown that heteroatoms(B,O,S,P,Cl,F,etc.)can be used as electron-withdrawing groups to modulate the planar structure and electron distribution of the Fe–Nx active sites to achieve simultaneous improvement of catalytic activity and stability.However,the optimal location of the heteroatoms remains unclear.Here,taking chalcogen heteroatoms(S and Se)as an example,we control the doping positions and investigate their effect on the ORR performance of the Fe–N–C catalysts.The first coordination shell of the iron single atom is identified as the optimal doping position.The optimized catalysts Fe–N_(3)Se_(1)/NC and Fe–N_(3)Se_(1)/NC demonstrate improved activity and stability in both half cells and fuel cells.This work provides insights into the enhancement mechanism of heteroatom doping in single-atom catalysts.

关 键 词：Oxygen reduction reaction Fe-N-C catalysts Hetero-atom doping Doping position Enhancement mechanism 

分 类 号：O64[理学—物理化学]