title: Improved ethanol electrooxidation performance by shortening Pd-Ni active site distance in Pd-Ni-P nanocatalysts.
abstract: Incorporating oxophilic metals into noble metal-based catalysts represents an emerging strategy to improve the catalytic performance of electrocatalysts in fuel cells. However, effects of the distance between the noble metal and oxophilic metal active sites on the catalytic performance have rarely been investigated. Herein, we report on ultrasmall (∼5 nm) Pd-Ni-P ternary nanoparticles for ethanol electrooxidation. The activity is improved up to 4.95 A per mgPd, which is 6.88 times higher than commercial Pd/C (0.72 A per mgPd), by shortening the distance between Pd and Ni active sites, achieved through shape transformation from Pd/Ni-P heterodimers into Pd-Ni-P nanoparticles and tuning the Ni/Pd atomic ratio to 1:1. Density functional theory calculations reveal that the improved activity and stability stems from the promoted production of free OH radicals (on Ni active sites) which facilitate the oxidative removal of carbonaceous poison and combination with CH3CO radicals on adjacent Pd active sites.
authors.affiliation: State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China.
authors.forename: Lin
authors.initials: L
authors.lastname: Chen
authors.affiliation: School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan 430081, China.
authors.forename: Lilin
authors.initials: L
authors.lastname: Lu
authors.affiliation: State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China.
authors.forename: Hengli
authors.initials: H
authors.lastname: Zhu
authors.affiliation: State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China.|Department of Chemistry, Tsinghua University, Beijing 100086, China.
authors.forename: Yueguang
authors.initials: Y
authors.lastname: Chen
authors.affiliation: Department of Materials Science &Engineering, University of California Los Angeles, California 90095, USA.
authors.forename: Yu
authors.initials: Y
authors.lastname: Huang
authors.affiliation: Department of Chemistry, Tsinghua University, Beijing 100086, China.
authors.forename: Yadong
authors.initials: Y
authors.lastname: Li
authors.affiliation: State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China.
authors.forename: Leyu
authors.initials: L
authors.lastname: Wang