Premium
Global Optimization of Adsorbate Covered Supported Cluster Catalysts: The Case of Pt 7 H 10 CH 3 on α‐Al 2 O 3
Author(s) -
Zhai Huanchen,
Sautet Philippe,
Alexandrova Anastassia N.
Publication year - 2020
Publication title -
chemcatchem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.497
H-Index - 106
eISSN - 1867-3899
pISSN - 1867-3880
DOI - 10.1002/cctc.201901830
Subject(s) - cluster (spacecraft) , catalysis , binding energy , molecular dynamics , chemical physics , adsorption , chemistry , transition metal , hydrogen , metal , materials science , nanotechnology , computational chemistry , atomic physics , physics , computer science , biochemistry , programming language , organic chemistry
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. 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 2 O 3 at high hydrogen coverage (10H). The presence of adsorbates significantly alters the low‐energy isomers compared to bare Pt 7 /α‐Al 2 O 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.