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Title: Global Optimization of Adsorbate Covered Supported Cluster Catalysts: The Case of Pt 7H 10CH 3 on α-Al 2O 3

Abstract

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 Pt 7/α-Al 2O 3 at high hydrogen coverage (10H). The presence of adsorbates significantly alters the low-energy isomers compared to bare Pt 7/α-Al 2O 3. 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.

Authors:
 [1];  [1]; ORCiD logo [2]
  1. Univ. of California, Los Angeles, CA (United States)
  2. Univ. of California, Los Angeles, CA (United States); California NanoSystems Inst., Los Angeles, CA (United States)
Publication Date:
Research Org.:
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 Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
OSTI Identifier:
1594249
Grant/Contract Number:  
SC0019152; AC02-05CH11231; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
ChemCatChem
Additional Journal Information:
Journal Name: ChemCatChem; Journal ID: ISSN 1867-3880
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English

Citation Formats

Zhai, Huanchen, Sautet, Philippe, and Alexandrova, Anastassia N. Global Optimization of Adsorbate Covered Supported Cluster Catalysts: The Case of Pt7H10CH3 on α-Al2O3. United States: N. p., 2019. Web. doi:10.1002/cctc.201901830.
Zhai, Huanchen, Sautet, Philippe, & Alexandrova, Anastassia N. Global Optimization of Adsorbate Covered Supported Cluster Catalysts: The Case of Pt7H10CH3 on α-Al2O3. United States. doi:10.1002/cctc.201901830.
Zhai, Huanchen, Sautet, Philippe, and Alexandrova, Anastassia N. Thu . "Global Optimization of Adsorbate Covered Supported Cluster Catalysts: The Case of Pt7H10CH3 on α-Al2O3". United States. doi:10.1002/cctc.201901830.
@article{osti_1594249,
title = {Global Optimization of Adsorbate Covered Supported Cluster Catalysts: The Case of Pt7H10CH3 on α-Al2O3},
author = {Zhai, Huanchen and Sautet, Philippe and Alexandrova, Anastassia N.},
abstractNote = {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.},
doi = {10.1002/cctc.201901830},
journal = {ChemCatChem},
number = ,
volume = ,
place = {United States},
year = {2019},
month = {10}
}

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