Modeling the active sites of Co-promoted MoS2 particles by DFT

文献信息

发布日期 2016-12-08
DOI 10.1039/C6CP06881B
影响因子 3.676
作者

Manuel Šarić, Jan Rossmeisl, Poul Georg Moses


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摘要

The atomic-scale structure of the Co-promoted MoS2 catalyst (CoMoS), used for hydrodesulfurization and as a potential replacement for platinum in the acidic hydrogen evolution reaction has been analyzed by modeling its sites using density functional theory and applying thermochemical corrections to account for different reaction conditions. The equilibrium structures of the edges, basal plane and corners have been found and used to obtain a picture of an ideal CoMoS nanoparticle under hydrodesulfurization and hydrogen evolution reaction conditions. Under hydrodesulfurization conditions small energy differences between structures having an additional or missing sulfur atom relative to the equilibrium structures have been observed for the edges and corners explaining their activity towards hydrodesulfurization at the atomic scale. The lack of these small energy differences at the basal plane explains why it is inert towards hydrodesulfurization. The adsorption free energy of hydrogen was calculated and used as a descriptor for qualifying each site in the context of hydrogen evolution, finding that the corner site should perform better than the edges.

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来源期刊

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
自引率: 10.3%
年发文量: 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.

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