A quantum chemical study of hydrogen adsorption on carbon-supported palladium clusters

文献情報

出版日 2019-09-10

DOI 10.1039/C9CP04606B

インパクトファクター 3.676

著者

Lisa Warczinski, Christof Hättig

原文を見る

要旨

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.

掲載誌

Physical Chemistry Chemical Physics

CiteScore: 5.5

自己引用率: 10.3%

年間論文数: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.