Theoretical characterization of zeolite encapsulated platinum clusters in the presence of water molecules

文献情報

出版日 2021-10-07

DOI 10.1039/D1CP03766H

インパクトファクター 3.676

著者

原文を見る

要旨

Zeolite encapsulated metal clusters have shown high catalytic activity and superior stability due to confinement effects, the synergy between acidic and metal active sites, and strong metal–zeolite interactions. In the present work, density functional theory calculations were employed to study the stability of encapsulated Ptn (n = 1–6) clusters in the zeolitic frameworks including Silicalite-1 and H-MFI. It has been found that the metal-zeolite interaction becomes stronger with the increasing Ptn cluster size for both zeolitic frameworks. The encapsulated Ptn clusters in the vicinity of the Brønsted acid site (BAS) of H-MFI form more stable PtnHx (x = 1, 2) clusters. The presence of water molecules around the encapsulated Pt6 cluster further enhances its stability, while the oxidation states of the encapsulated Ptn cluster are largely affected by the BAS site and the surrounding water molecules. As the water concentration increases, water dissociation becomes more facile on the Pt6@Silicalite-1 cluster while an opposite trend is found over the Pt6H2@H-MFI cluster. The proton of the BAS site can be transferred to the encapsulated Pt6 cluster via a hydronium cluster H+(H2O)n, leading to the formation of the Pt6H2@H-MFI cluster.

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.