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

[Display omitted] •Pd-M bimetallic NPs over carbon support were synthesized and characterized.•XPS valence band spectra confirm a charge transfer between Pd and M metals.•A volcano shaped relationship exists between FAO activity and d-band center of NPs.•Pd-Cu/C shows the best FAO activity and stabi...

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Bibliographic Details
Published in:Applied catalysis. B, Environmental Environmental, 2019-10, Vol.254 (C), p.685-692
Main Authors: Hu, Shuozhen, Che, Fanglin, Khorasani, Bita, Jeon, Mina, Yoon, Chang Won, McEwen, Jean-Sabin, Scudiero, Louis, Ha, Su
Format: Article
Language:English
Subjects:
Bimetals
Catalysis
Catalysts
Copper
d-band center
DFT-based calculations
Electrochemical analysis
Electrochemical oxidation
Electrochemistry
Formic acid
Formic acid electrochemical oxidation
Gold
Metals
Nanoparticles
Oxidation
Palladium
Pd-based bimetallic nanoparticles
Perturbation
Platinum
Properties (attributes)
Silver
Stability
Volcano plot
Volcanoes
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Summary:[Display omitted] •Pd-M bimetallic NPs over carbon support were synthesized and characterized.•XPS valence band spectra confirm a charge transfer between Pd and M metals.•A volcano shaped relationship exists between FAO activity and d-band center of NPs.•Pd-Cu/C shows the best FAO activity and stability with 64 wt.% Pd metal reduction. 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.
ISSN:0926-3373
1873-3883
DOI:10.1016/j.apcatb.2019.03.072