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Issue 19, 2019
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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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Abstract

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.

Graphical abstract: 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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Article information


Submitted
10 Feb 2019
Accepted
16 Apr 2019
First published
18 Apr 2019

Phys. Chem. Chem. Phys., 2019,21, 9895-9904
Article type
Paper
Author version available

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

C. J. Bodenschatz, T. Xie, X. Zhang and R. B. Getman, Phys. Chem. Chem. Phys., 2019, 21, 9895
DOI: 10.1039/C9CP00824A

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