文献类型：期刊文献

英文题名：Improving the electrochemical oxidation of formic acid by tuning the electronic properties of Pd-based bimetallic nanoparticles

作者：Hu, Shuozhen[1];Che, Fanglin[2];Khorasani, Bita[2];Jeon, Mina[3];Yoon, Chang Won[3];McEwen, Jean-Sabin[2,4,5,6,7];Scudiero, Louis[6];Ha, Su[2]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]Washington State Univ, Gene & Linda Voiland Sch Chem Engn & Bioengn, Pullman, WA 99164 USA;[3]Korea Inst Sci & Technol, Fuel Cell Res Ctr, Seoul 02792, South Korea;[4]Pacific Northwest Natl Lab, Inst Integrated Catalysis, Richland, WA 99352 USA;[5]Washington State Univ, Dept Phys & Astron, Pullman, WA 99164 USA;[6]Washington State Univ, Dept Chem, Pullman, WA 99164 USA;[7]Washington State Univ, Dept Biol Syst Engn, Pullman, WA 99164 USA

年份：2019

卷号：254

起止页码：685

外文期刊名：APPLIED CATALYSIS B-ENVIRONMENTAL

收录：;EI(收录号：20192206977080);WOS:【SCI-EXPANDED(收录号:WOS:000472697500069)】；

基金：The experimental work was funded by the National Science Foundation under Agreement CBET-1033601, DMR-9503304 and CHE-1048600. F.C. and J.-S.M. were primarily funded by the U.S. Department of Energy, Office of Basic Energy Science, Division of Chemical Sciences, Biosciences and Geosciences (DE-SC0014560) for the corresponding DFT-based calculations. We would like also to thank the Murdock Charitable Trust for its financial support in upgrading our existing XPS instrument. The Pacific Northwest National Laboratory is operated by Battelle for the U.S. DOE.

语种：英文

外文关键词：Pd-based bimetallic nanoparticles; d-band center; Formic acid electrochemical oxidation; Volcano plot; DFT-based calculations

摘要：Pd-based bimetallic nanoparticles have superior electrochemical activity and stability for formic acid oxidation (FAO) than pure Pd. Previous DFT-based calculations show that the catalytic properties of the Pd surface could be altered by modifying its electronic properties. However, only a few experimental studies investigate how the electronic properties of Pd are modified by introducing various metals and how the resulting electronic perturbation affects its electrochemical activity and stability for FAO. Here, we demonstrate a correlation between electrochemistry and electronic properties for Pd-M bimetallic nanoparticles (M = Ru, Pt, Cu, Au, and Ag). The volcano shape relationship obtained between activity and d-band center values suggests that the electronic effects play a major role in modifying the surface electrochemical properties of Pd-M bimetallic nanoparticles for FAO. Among all the bimetallic catalysts investigated in this study, Pd-Pt/C and Pd-Cu/C with d-band center values of 2.58 eV and 2.85 eV, respectively, demonstrate the highest activities and Pd-Cu/C exhibits the highest stability for FAO.