How the microenvironment dominated by the distance effect to regulate the FeN_(4)site ORR activity and selectivity?  

作　　者：Peng Li Qingfeng Guo Jianrui Zhang Ruilin Chen Shujiang Ding Yaqiong Su 

机构地区：[1]School of Chemistry,Engineering Research Center of Energy Storage Materials and Devices of Ministry of Education,National Innovation Platform(Center)for Industry-Education Integration of Energy Storage Technology,Xi’an Jiaotong University,Xi’an 710049,China [2]Huanghe Science and Technology College,Zhengzhou 450063,China [3]General Research Institute of Engineering of Gotion High-Tech,Hefei 230041,China

出　　处：《Nano Research》2024年第6期5735-5741,共7页纳米研究（英文版）

摘　　要：The distance effect of the doped heteroatoms away from the catalytic centers has rarely been reported.In this work,we conducted density functional theory calculations to thoroughly investigate the influence of heteroatom(N,P,B,and S atoms)doping distance on the oxygen reduction reaction(ORR)activity of graphene-based FeN_(4)sites.We uncovered a Sabatier-like relationship between heteroatom doping distance and ORR activity of FeN_(4)sites.The nearest doping does not significantly improve and even block the ORR activity of FeN_(4)sites.Optimal ORR activity is achieved when the heteroatoms are 4-5Å(N,P,and S atoms)or 6-7Å(B atoms)away from the Fe atoms.Analysis of electronic structure indicates that distance effect can modulate the local chemical environment of Fe atoms,thereby account for the changes in ORR activity along with the doping distance and doping atoms.This study provides insights into the influence of heteroatom doping on the chemical environment of reaction active centers,and provides the theoretical guidance for controlling the doping distance of heteroatoms to achieve optimal catalytic activity and selectivity.

关 键 词：distance effect MICROENVIRONMENT heteroatom doping FeN_(4) Sabatier-like relationship structure-activity relationship 

分 类 号：O64[理学—物理化学]