Dynamic formation of single-atom catalytic active sites on ceria-supported gold nanoparticles

Yang Gang Wang; Donghai Mei; Vassiliki Alexandra Glezakou; Jun Li; Roger Rousseau

doi:10.1038/ncomms7511

Dynamic formation of single-atom catalytic active sites on ceria-supported gold nanoparticles

Yang Gang Wang, Donghai Mei, Vassiliki Alexandra Glezakou, Jun Li, Roger Rousseau

Research output: Contribution to journal › Article › peer-review

407 Scopus citations

Abstract

Catalysis by gold supported on reducible oxides has been extensively studied, yet issues such as the nature of the catalytic site and the role of the reducible support remain fiercely debated topics. Here we present ab initio molecular dynamics simulations of an unprecedented dynamic single-atom catalytic mechanism for the oxidation of carbon monoxide by ceria-supported gold clusters. The reported dynamic single-atom catalytic mechanism results from the ability of the gold cation to strongly couple with the redox properties of the ceria in a synergistic manner, thereby lowering the energy of redox reactions. The gold cation can break away from the gold nanoparticle to catalyse carbon monoxide oxidation, adjacent to the metal/oxide interface and subsequently reintegrate back into the nanoparticle after the reaction is completed. Our study highlights the importance of the dynamic creation of active sites under reaction conditions and their essential role in catalysis..

Original language	English
Article number	6511
Journal	Nature Communications
Volume	6
DOIs	https://doi.org/10.1038/ncomms7511
State	Published - Mar 4 2015
Externally published	Yes

Funding

This work was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences and performed at Pacific Northwest National Laboratory (PNNL). PNNL is a multi-programme national laboratory operated by Battelle for the US Department of Energy. J.L. and Y.-G.W. were also financially supported by NKBRSF (2011CB932400) and NSFC (91026003, 21101098) of China. Computational resources were provided at W.R. Wiley Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility located at PNNL and sponsored by the US Department of Energy, Office of Science, Office of Biological and Environmental Research and at the National Energy Research Scientific Computing Center (NERSC) located at Lawrence Berkeley National Laboratory.

Funders	Funder number
NKBRSF	2011CB932400
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Biological and Environmental Research
Lawrence Berkeley National Laboratory
Pacific Northwest National Laboratory
Chemical Sciences, Geosciences, and Biosciences Division
National Natural Science Foundation of China	91026003, 21101098

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abstract = "Catalysis by gold supported on reducible oxides has been extensively studied, yet issues such as the nature of the catalytic site and the role of the reducible support remain fiercely debated topics. Here we present ab initio molecular dynamics simulations of an unprecedented dynamic single-atom catalytic mechanism for the oxidation of carbon monoxide by ceria-supported gold clusters. The reported dynamic single-atom catalytic mechanism results from the ability of the gold cation to strongly couple with the redox properties of the ceria in a synergistic manner, thereby lowering the energy of redox reactions. The gold cation can break away from the gold nanoparticle to catalyse carbon monoxide oxidation, adjacent to the metal/oxide interface and subsequently reintegrate back into the nanoparticle after the reaction is completed. Our study highlights the importance of the dynamic creation of active sites under reaction conditions and their essential role in catalysis..",

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AU - Wang, Yang Gang

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AU - Rousseau, Roger

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AB - Catalysis by gold supported on reducible oxides has been extensively studied, yet issues such as the nature of the catalytic site and the role of the reducible support remain fiercely debated topics. Here we present ab initio molecular dynamics simulations of an unprecedented dynamic single-atom catalytic mechanism for the oxidation of carbon monoxide by ceria-supported gold clusters. The reported dynamic single-atom catalytic mechanism results from the ability of the gold cation to strongly couple with the redox properties of the ceria in a synergistic manner, thereby lowering the energy of redox reactions. The gold cation can break away from the gold nanoparticle to catalyse carbon monoxide oxidation, adjacent to the metal/oxide interface and subsequently reintegrate back into the nanoparticle after the reaction is completed. Our study highlights the importance of the dynamic creation of active sites under reaction conditions and their essential role in catalysis..

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Dynamic formation of single-atom catalytic active sites on ceria-supported gold nanoparticles

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