Bimetallic Au-Pd alloy catalysts for N 2O decomposition: Effects of surface structures on catalytic activity
Journal
Journal of Physical Chemistry C
Journal Volume
116
Journal Issue
10
Pages
6222-6232
Date Issued
2012
Author(s)
Abstract
Highly dispersed and well-homogenized Au-Pd alloy nanoparticles with average particle sizes of ∼2 nm and tunable Au/Pd ratios were prepared by an adsorption-reduction method on the amine-functionalized SBA-15 support. The chemisorptions of H 2 and CO as well as the IR spectra of CO adsorption show that with increase of the Au/Pd ratios the surface Pd atoms are separated by gold atoms gradually until totally isolated at Au/Pd ≥ 0.95, which indicates the formation of Pd single atoms at higher Au/Pd ratios. The chemisorption of O 2 shows that both the adsorption heat and the saturation uptake decrease with an increase of Au/Pd ratio, suggesting alloying Pd with gold will facilitate the desorption of oxygen adatoms as O 2, which is generally the rate-determining step for N 2O decomposition reaction. Theoretical investigations using periodic DFT methods confirm the tunable O 2 desorption ability by alloying Pd with Au and indicate that contiguously located Pd sites are indispensable for N 2O decomposition because they function as the active sites for the elementary step of N 2O decomposition into N 2 and oxygen adatom, which becomes the rate-determining step over the Au-Pd alloy catalysts. © 2012 American Chemical Society.
SDGs
Type
journal article