Solid-to-liquid Phase Transitions of Sub-nanometer Clusters Enhance Chemical Transformation

Overview

Journal Nat Commun

Specialty Biology

Date 2019 Nov 29

PMID 31776346

Citations 4

Authors

Juan-Juan Sun

Jun Cheng

Affiliations

Soon will be listed here.

Abstract

Understanding the nature of active sites is crucial in heterogeneous catalysis, and dynamic changes of catalyst structures during reaction turnover have brought into focus the dynamic nature of active sites. However, much less is known on how the structural dynamics couples with elementary reactions. Here we report an anomalous decrease in reaction free energies and barriers on dynamical sub-nanometer Au clusters. We calculate temperature dependence of free energies using ab initio molecular dynamics, and find significant entropic effects due to solid-to-liquid phase transitions of the Au clusters induced by adsorption of different states along the reaction coordinate. This finding demonstrates that catalyst dynamics can play an important role in catalyst activity.

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