在表面化学中,观众控制选择性:Pd上的阿克罗莱因部分化
Karl-Heinz Dostert1, Casey P O'Brien1, Francisco Ivars-Barceló1
1Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany.
Journal of the American Chemical Society
|October 21, 2015
概括
在经过修改的Palladium ((111) 表面上,可以选择性地将烯酸转化为烯酸. 一个独特的oxopropyl观众层使近乎完美的CO键选择性,形成不和醇.
科学领域:
- 不同质的催化
- 表面科学
- 有机合成
背景情况:
- 对于生产有价值的化学物质而言,阿克罗莱因化是至关重要的.
- 对于CC键化而言,实现高选择性仍然具有挑战性.
- 基于 (Pd) 的催化剂被广泛研究为化反应.
研究的目的:
- 在模型Pd表面上研究选择性化机制.
- 确定允许选择性C键化的条件和表面物种.
- 了解表面修饰在指导反应路径中的作用.
主要方法:
- 使用单晶Pd(111) 和支持Pd纳米颗粒的机制研究.
- 进行多分子束脉冲实验.
- 在现场的红外反射吸收光谱 (IRRAS).
主要成果:
- 在Pd{\displaystyle Pd{\displaystyle Pd{\text{\text{\text{\text}}}上实现了近100%的CO化为不和酒精的选择性.
- 用氧观众层修饰表面对于选择性至关重要.
- 氧观众和氧反应中间体的鉴定
- 同时监测中间演变和产品形成.
结论:
- 在特定的表面条件下,可对Pd{\displaystyle Pd{\text{11}}}进行选择性化.
- 通过表面介导的观众物种可以有效控制催化选择性.
- 这些发现为设计选择性化催化剂提供了基本的见解.
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