Journal
ACS CATALYSIS
Volume 10, Issue 11, Pages 6149-6158Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c01005
Keywords
active sites; Boltzmann statistics; heterogeneous catalysis; nanoparticles; structure-activity relations
Categories
Funding
- European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programme (Project SHAPE) [677423]
- National Science Foundation [1634880]
- Foundation Blanceflor Boncompagni Ludovisi, nee Bildt
- Div Of Civil, Mechanical, & Manufact Inn
- Directorate For Engineering [1634880] Funding Source: National Science Foundation
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Although nanoparticle catalysts obtain different sizes and shapes under reaction conditions, computational modeling in heterogeneous catalysis is usually based on well-defined crystallographic planes. Herein, we combine density functional theory (DFT) calculations with Boltzmann statistics to describe ensembles of nanoparticles obtaining different morphologies under reaction conditions (temperature and gas-phase chemical potential) and their respective distribution of active sites. We apply our methodology on Rh catalytic nanoparticles, and we address the contribution of metastable nanostructures on the overall CO dissociation catalytic activity. Importantly, we demonstrate how catalytic trends can change when accounting for an ensemble of nanoparticles compared to a single, thermodynamically stable nanoparticle. Thus, our work enlightens the impact of statistical representation of catalyst morphology on modeling structure-sensitive reactions.
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