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• W2617087070 abstract "Gaining insights into the working principles of photocatalysts on an atomic scale is a challenging task. The obviously high complexity of the reaction mechanism involving photoexcited electrons and holes is one reason. Another complicating aspect is that the electromagnetic field, driving photocatalysis, is not homogeneous on a nanoscale level for particle-based catalysts as it is influenced by the particle’s shape and size. We present a simple model, inspired by the CO2 reduction on titania anatase, which addresses the impact of these heterogeneities on the photocatalytic kinetics by combining kinetic Monte Carlo with electromagnetic wave simulations. We find that average activity and especially efficiency might differ significantly between different particles. Moreover, we find sizable variation of the catalytic activity on a single facet of a nanocrystal. Besides this quantitative heterogeneity, the coverage situation in general changes laterally on this facet, and we observe a concomitant change of the rate-determining steps. This heterogeneity on all levels of photocatalytic activity is masked in experimental studies, where only the spatially averaged activity can be addressed. Microkinetic models based on experimental findings might therefore not represent the true microscopic behavior, and mechanistic conclusion drawn from these needs to be handled with care." @default.
• W2617087070 created "2017-06-05" @default.
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• W2617087070 date "2020-01-08" @default.
• W2617087070 modified "2023-09-27" @default.
• W2617087070 title "Field Heterogeneities and Their Impact on Photocatalysis: Combining Optical and Kinetic Monte Carlo Simulations on the Nanoscale" @default.
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• W2617087070 doi "https://doi.org/10.1021/acs.jpcc.9b11469" @default.
• W2617087070 hasPublicationYear "2020" @default.
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