Catalytic role of pre-adsorbed CO in platinum-based catalysts : the reduction of SO 2 by CO on Pt l Au m (CO) n


Autoria(s): Gao, Guo-Ping; Wei, Shi-Hao; Gu, Xiao; Duan, Xiang-Mei
Data(s)

2013

Resumo

Using density functional theory, we have investigated the catalytic properties of bimetallic complex catalysts PtlAum(CO)n (l + m = 2, n = 1–3) in the reduction of SO2 by CO. Due to the strong coupling between the C-2p and metal 5d orbitals, pre-adsorption of CO molecules on the PtlAum is found to be very effective in not only reducing the activation energy, but also preventing poisoning by sulfur. As result of the coupling, the metal 5d band is broadened and down-shifted, and charge is transferred from the CO molecules to the PtlAum. As SO2 is adsorbed on the catalyst, partial charge moves to the anti-σ bonding orbitals between S and O in SO2, weakening the S–O bond strength. This effect is enhanced by pre-adsorbing up to three CO molecules, therefore the S–O bonds become vulnerable. Our results revealed the mechanism of the excellent catalytic properties of the bimetallic complex catalysts.

Formato

application/pdf

Identificador

http://eprints.qut.edu.au/74074/

Publicador

Royal Society of Chemistry

Relação

http://eprints.qut.edu.au/74074/1/74074.pdf

DOI:10.1039/C3CP44712J

Gao, Guo-Ping, Wei, Shi-Hao, Gu, Xiao, & Duan, Xiang-Mei (2013) Catalytic role of pre-adsorbed CO in platinum-based catalysts : the reduction of SO 2 by CO on Pt l Au m (CO) n. Physical Chemistry Chemical Physics, 15(31), pp. 12846-12851.

Direitos

Copyright 2013 Royal Society of Chemistry

Fonte

Science & Engineering Faculty

Palavras-Chave #030601 Catalysis and Mechanisms of Reactions #030799 Theoretical and Computational Chemistry not elsewhere classified
Tipo

Journal Article