Insights into how the aqueous environment influences the kinetics and mechanisms of heterogeneously-catalyzed COH* and CH3OH* dehydrogenation reactions on Pt(111)

文献情報

出版日 2019-04-18

DOI 10.1039/C9CP00824A

インパクトファクター 3.676

著者

Cameron J. Bodenschatz, Tianjun Xie, Xiaohong Zhang, Rachel B. Getman

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要旨

Water influences catalytic reactions in multiple ways, including energetic and mechanistic effects. While simulations have provided significant insight into the roles that H2O molecules play in aqueous-phase heterogeneous catalysis, questions still remain as to the extent to which H2O structures influence catalytic mechanisms. Specifically, influences of the configurational variability in the water structures at the catalyst interface are yet to be understood. Configurational variability is challenging to capture, as it requires multiscale approaches. Herein, we apply a multiscale sampling approach to calculate reaction thermodynamics and kinetics for COH* dehydrogenation to CO* and CH3OH* dehydrogenation to CH2OH* on Pt(111) catalysts under liquid H2O. We explore various pathways for these dehydrogenation reactions that could influence the overall mechanism of methanol decomposition by including participation of H2O structures both energetically and mechanistically. We find that the liquid H2O environment significantly influences the mechanism of COH* dehydrogenation to CO* but leaves the mechanism of CH3OH* dehydrogenation to CH2OH* largely unaltered.

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.

Insights into how the aqueous environment influences the kinetics and mechanisms of heterogeneously-catalyzed COH* and CH3OH* dehydrogenation reactions on Pt(111)

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