A quantum chemical study of hydrogen adsorption on carbon-supported palladium clusters.
A quantum chemical study of hydrogen adsorption on carbon-supported palladium clusters.
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DOI：
10.1039/c9cp04606b
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发表时间：
2019-10
期刊：
影响因子：
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通讯作者：
Lisa Warczinski;C. Hättig
中科院分区：
文献类型：
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作者：
Lisa Warczinski;C. Hättig
更好地了解催化加氢反应的关键步骤是详细了解氢在催化剂上的吸附过程。本文重点研究氢在碳载钯簇上的吸附，钯簇是当今工业应用中最常见的催化剂之一。应用密度泛函理论研究了Pd 6和Pd 21团簇，揭示了碳载体材料对催化剂性能的影响以及对氢吸附的机理和能量学的影响。在一般情况下，逐步氢吸附过程中观察到的分子吸附，然后解离化学吸附组成。碳载体材料不明显影响反应机理，但对能垒和优先吸附位点有很大影响。我们对Pd6和Pd21系统的比较表明，小簇，如Pd6，能够模拟钯纳米颗粒的一些但不是所有重要性质，因此，研究较大的簇尺寸也是必要的。
A key step for achieving better insight into catalytic hydrogenation reactions is to understand in detail the process of hydrogen adsorption on the catalyst. The present article focuses on hydrogen adsorption on carbon-supported palladium clusters, which are nowadays one of the most common catalysts in industrial applications. Density functional theory is applied to study Pd6 and Pd21 clusters to reveal the influence of the carbon support material on the properties of the catalyst as well as on the mechanisms and energetics of the hydrogen adsorption. In general, a stepwise hydrogen adsorption process is observed consisting of molecular adsorption followed by dissociative chemisorption. The carbon support material does not noticeably affect the reaction mechanisms, but has a large influence on energy barriers and preferential adsorption sites. Our comparison of Pd6 and Pd21 systems reveals that small clusters, such as Pd6, are able to model some but not all important properties of palladium nanoparticles and, therefore, it is essential to also study larger cluster sizes.