Density functional theory study of active sites and reaction mechanism of ORR on Pt surfaces under anhydrous conditions

作     者：Guangdong Liu Huiqiu Deng Jeffrey Greeley Zhenhua Zeng 刘广东;邓辉球;Greeley Jeffrey;曾振华

作者机构：School of Physics and ElectronicsHunan UniversityChangsha 410082HunanChina Davidson School of Chemical EngineeringPurdue UniversityWest LafayetteIN 47907USA 

基　　金：supported through the U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical, Biological, and Geosciences Division under DE-SC0010379 the support from an ECS Toyota Young Investigator Fellowship 

出 版 物：《Chinese Journal of Catalysis》 (催化学报（英文）)

年 卷 期：2022年第43卷第12期

页      码：3126-3133页

摘      要：Identifying active sites and catalytic mechanism of the oxygen reduction reaction under anhydrous conditions are crucial for the development of next generation proton exchange membrane fuel cells(PEMFCs)operated at a temperature>100℃.Here,by employing density functional theory calculations,we studied ORR on flat and stepped Pt(111)surfaces with both(110)and(100)type of *** found that,in contrast to ORR under hydrous conditions,(111)terrace sites are not active for ORR under anhydrous conditions,because of weakened binding of ORR intermediates induced by O*accumulation on the *** the other hand,step edges,which are generally not active for ORR under hydrous conditions,are predicted to be the active sites for ORR under anhydrous *** them,(110)type step edge with a unique configuration of accumulated O stabilizes O_(2)adsorption and facilitates O_(2)dissociation,which lead an overpotential<0.4 *** improve ORR catalysts in high-temperature PEMFCs,it is desirable to maximize(110)step edge sites that present between two(111)facets of nanoparticles.

主 题 词：Oxygen reduction Active site Anhydrous condition High-temperature PEMFCs Density functional theory 

学科分类：0808[工学-自动化类] 081705[081705] 08[工学] 0817[工学-轻工类] 

核心收录：

D　O　I：10.1016/S1872-2067(22)64125-1

馆 藏 号：203115481...