Surface engineering,which modulates the electronic structure and adsorption/desorption properties of electrocatalysts,is one of the key strategies for improving the catalytic performance.Herein,we demonstrate a facile...Surface engineering,which modulates the electronic structure and adsorption/desorption properties of electrocatalysts,is one of the key strategies for improving the catalytic performance.Herein,we demonstrate a facile solid-phase reaction for surface engineering of MnO_(2)to boost the oxygen reduction kinetics.Via reaction with surface hydroxy groups,La single atoms with loading amount up to 2.7 wt%are anchored onto a-MnO_(2)nanorods.After surface engineering,the oxygen reduction reaction(ORR)kinetics is significantly improved with the half-wave potential from 0.70 to 0.84 V,the number of transferred electrons from 2.5 to 3.9 and the limiting current density from 4.8 to 6.0 mA·cm^(-2).In addition,the catalyst delivers superior discharge performance in both alkaline and neutral metal–air batteries.Density functional theory(DFT)calculations reveal that atomic La modulates the surface electronic configuration of MnO_(2),reduces its d-band center and thus lowers the OOH*and O*reaction energy barrier.This work provides a new route for rational design of highly active electrocatalyst and holds great potential for application in various catalytic reactions.展开更多
基金financially supported by the Scientific Research Fund of Hunan Provincial Education Department(No.21B0289)Changsha Municipal Science and Technology Projects(No.2022cskj006)。
文摘Surface engineering,which modulates the electronic structure and adsorption/desorption properties of electrocatalysts,is one of the key strategies for improving the catalytic performance.Herein,we demonstrate a facile solid-phase reaction for surface engineering of MnO_(2)to boost the oxygen reduction kinetics.Via reaction with surface hydroxy groups,La single atoms with loading amount up to 2.7 wt%are anchored onto a-MnO_(2)nanorods.After surface engineering,the oxygen reduction reaction(ORR)kinetics is significantly improved with the half-wave potential from 0.70 to 0.84 V,the number of transferred electrons from 2.5 to 3.9 and the limiting current density from 4.8 to 6.0 mA·cm^(-2).In addition,the catalyst delivers superior discharge performance in both alkaline and neutral metal–air batteries.Density functional theory(DFT)calculations reveal that atomic La modulates the surface electronic configuration of MnO_(2),reduces its d-band center and thus lowers the OOH*and O*reaction energy barrier.This work provides a new route for rational design of highly active electrocatalyst and holds great potential for application in various catalytic reactions.
