文献类型：期刊文献

英文题名：Strategies to Improve the Oxygen Reduction Reaction Activity on Pt-Bi Bimetallic Catalysts: A Density Functional Theory Study

作者：Zhang, Yan-Ping[1,2,3];Su, Zi-Xiang[1,2,3];Wei, He-He[1,2,3];Wang, Zhi-Qiang[1,2,3];Gong, Xue-Qing[1,2,3]

机构：[1]East China Univ Sci & Technol, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Ctr Computat Chem, Joint Int Res Lab Precis Chem & Mol Engn, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Res Inst Ind Catalysis, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China

年份：2023

卷号：14

期号：7

起止页码：1990

外文期刊名：JOURNAL OF PHYSICAL CHEMISTRY LETTERS

收录：;EI(收录号：20230913639986);WOS:【SCI-EXPANDED(收录号:WOS:000936016200001)】；

基金：ACKNOWLEDGMENTS This work was supported by the National Key R&D Program of China (2021YFA1500700 and 2018YFA0208602) , the National Nature Science Foundation of China (22203030, 22102057, 21825301, and 92045303) , the Shanghai Sailing Program (21YF1409400) , and the China Postdoctoral Science Foundation (2020M671020) .

语种：英文

外文关键词：Association reactions - Binary alloys - Density functional theory - Electrolytic reduction - Oxygen - Platinum - Platinum alloys - Proton exchange membrane fuel cells (PEMFC) - Tensile strain

摘要：Decreasing the level of use of Pt in proton exchange membrane fuel cells is of great research interest both academically and industrially. In this work, we systematically studied the oxygen reduction reaction (ORR) following the four-electron association mechanism at various Pt-Bi surfaces with density functional theory calculations. The results showed that the introduction of Bi changes the potential-determining step of ORR. Moreover, the hydroxy adsorption free energy (GOH*) can be used as a descriptor of ORR activity, and 0.74 eV is the ideal GOH* for it to reach its maximum. Notably, we also found that the tensile strain introduced by Bi and electron transfer between Pt and Bi synergize to modulate the d -band of Pt to contract, shift downward, and break the 5d96s1 valence electron configuration of Pt, and accordingly, PtBi(100), with the lowest d-band center, gives the best ORR activity, which is even slightly higher than that of Pt(111).