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Predicting Catalyst Performance From Pt/CeO2 Redispersion Kinetics
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DOI：10.1002/anie.4743891.png)
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Abstract
En 中文
Quantitative description of the structural dynamics of nanoparticles by kinetic data is challenging but would represent a significant knowledge leap, as this would enable the forecast of their properties, e.g., in catalysis. A striking example in catalysis is the redispersion of Pt nanoparticles into single atoms in Pt/CeO2-based catalysts. In this work, we combined environmental transmission electron microscopy (ETEM) measurements with catalytic data to monitor the individual decay of Pt nanoparticles on defined CeO2 nanocubes. Supported by density functional theory modeling, this provides unprecedented insight into their dynamic behavior, including kinetics. We observed that the rate of noble metal redispersion is strongly dependent on the local structural environment: the presence of other nearby nanoparticles and heterogeneities on the CeO2 surface reduced the redispersion rate. Independent of the initial particle size and local environment, the particle volume decreases linearly in time, indicating a constant flux of Pt atoms from the nanoparticles. These findings at the atomic scale were correlated to the observed changes in the integral catalytic performance, allowing a first prediction of the catalyst activity based on the redispersion process and demonstrating how atomic-scale kinetic insights can be correlated to macroscopic effects.
Keywords:
catalyst deactivation
ceria cubes
DFT
ETEM
noble metal redispersion
platinum
structural kinetics
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