Acetic acid adsorption and decomposition on Pd(110)

被引:72
作者
Bowker, M [1 ]
Morgan, C [1 ]
Couves, J [1 ]
机构
[1] Univ Reading, Dept Chem, Ctr Surface Sci & Catalysis, Reading RG6 6AD, Berks, England
关键词
molecule-solid reactions; adsorption kinetics; catalysis; chemisorption; surface chemical reaction; palladium; carboxylic acid; sticking;
D O I
10.1016/j.susc.2003.12.040
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The reaction of acetic acid with Pd(1 10) has been investigated using temperature-programmed desorption (TPD) and a molecular beam reactor. The sticking of acetic acid is very efficient and results in hydrogen evolution and acetate formation at room temperature. The acetate decomposes between 320 and 440 K to produce CO2 and hydrogen coincidently and leaves C adsorbed on the surface. The presence of carbon results in a changed desorption profile after readsorbing acid on the surface, manifesting an autocatalytic decomposition profile, with a half-height width of as low as 9 K and a slowed decomposition rate (higher peak temperature). Surprisingly, at higher temperatures where the acetate is unstable (>450 K), the sticking of acetic acid continues at a steady-state rate and is not poisoned by the buildup of C on the crystal. This is due to the fact that most of the C deposited is lost from the surface to the bulk in a facile manner above about 450 K, leaving a reactive surface which is apparently continually available for decomposition. The reactive surface appears to be Pd(1 1 0) with 0.5 monolayers of C adsorbed in the c(2 x 2) structure, which acts as a template for increased stability and ordering of the acetate adlayer. (C) 2004 Published by Elsevier B.V.
引用
收藏
页码:145 / 156
页数:12
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