Improved ethanol electrooxidation performance by shortening Pd–Ni active site distance in Pd–Ni–P nanocatalysts

Lin Chen, Lilin Lu, Hengli Zhu, Yueguang Chen, Yu Huang, Yadong Li and Leyu Wang ()
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Lin Chen: State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology
Lilin Lu: School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology
Hengli Zhu: State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology
Yueguang Chen: State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology
Yu Huang: University of California
Yadong Li: Tsinghua University
Leyu Wang: State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology

Nature Communications, 2017, vol. 8, issue 1, 1-9

Abstract: 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.

Date: 2017
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DOI: 10.1038/ncomms14136

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