期刊
CATALYSIS TODAY
卷 205, 期 -, 页码 76-85出版社
ELSEVIER
DOI: 10.1016/j.cattod.2012.08.022
关键词
Palladium; Selective oxidation; Operando; XAS; Mesoporous supports
资金
- EPSRC [EP/G007594/2] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [EP/G007594/2] Funding Source: researchfish
The selective aerobic oxidation of crotyl alcohol to crotonaldehyde was investigated by time-resolved synchronous DRIFTS/MS/XAS over silica and alumina supported Pd nanoparticles. Alcohol and oxygen reactant feeds were cycled through the catalyst bed while dynamic measurements of the palladium oxidation state, molecular adsorbates and evolved product distribution were made simultaneously on a sub-second timescale. Highly dispersed palladium nanoparticles remained in a partially oxidised state <100 degrees C, independent of the redox environment, and were selective for crotonaldehyde formation. Higher temperatures facilitated rapid catalyst reduction on exposure to crotyl alcohol, with palladium metal driving crotonaldehyde decarbonylation to propene and CO, while slower (surface diffusion-limited) reoxidation on exposure to oxygen re-opened selective oxidation pathways. Surface palladium oxide is identified as the desired active species. (C) 2012 Elsevier B.V. All rights reserved.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据