Global Optimization of Adsorbate Covered Supported Cluster Catalysts: The Case of Pt7H10CH3 on α-Al2O3

Zhai, Huanchen; Sautet, Philippe; Alexandrova, Anastassia N.

doi:10.1002/cctc.201901830

Title: Global Optimization of Adsorbate Covered Supported Cluster Catalysts: The Case of Pt₇H₁₀CH₃ on α-Al₂O₃

Journal Article · 24 October 2019 · ChemCatChem

DOI: https://doi.org/10.1002/cctc.201901830 · OSTI ID:1594249

Zhai, Huanchen ^[1]; Sautet, Philippe ^[2];

^[3]

Univ. of California, Los Angeles, CA (United States); University of California, Los Angeles
Univ. of California, Los Angeles, CA (United States)
Univ. of California, Los Angeles, CA (United States); California NanoSystems Inst., Los Angeles, CA (United States)

Determining structures of supported sub-nanometer catalytic clusters is important for finding binding sites, active sites, and reaction mechanisms. In realistic conditions, the cluster may be covered with adsorbed reactants and intermediates, which strongly affect the structure of the cluster compared to the low coverage regime. The global optimization of supported adsorbate-covered clusters is not possible with existing methods. In this paper, we present a customized Basin Hopping (BH) approach, with a core (metal cluster) – shell (adsorbates) separation scheme, and perform first applications to the search of low-energy isomers of Pt₇/α-Al₂O₃ at high hydrogen coverage (10H). The presence of adsorbates significantly alters the low-energy isomers compared to bare Pt₇/α-Al₂O₃. Molecular dynamics simulations additionally show the different time-scales associated with the mobility of H and Pt atoms. The revised BH method with core-shell separation presents key advantages for the structural exploration of adsorbate-covered supported catalysts, relevant to realistic catalytic conditions.

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Research Organization:: Univ. of California, Los Angeles, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: SC0019152; AC02-05CH11231; AC02-06CH11357

OSTI ID:: 1594249

Journal Information:: ChemCatChem, Journal Name: ChemCatChem Journal Issue: 3 Vol. 12; ISSN 1867-3880

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Global Optimization of Adsorbate Covered Supported Cluster Catalysts: The Case of Pt₇H₁₀CH₃ on α-Al₂O₃