Structure sensitivity of ceria-supported Au catalysts for CO oxidation

Ya Qiong Su; Yan-Yang Qin; Tiantian Wu; De-Yin Wu

doi:10.1016/j.jcat.2022.02.008

Structure sensitivity of ceria-supported Au catalysts for CO oxidation

Ya Qiong Su (Corresponding author), Yan-Yang Qin, Tiantian Wu, De-Yin Wu

Inorganic Materials & Catalysis

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

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Abstract

Single-atom catalysis is at the center of the attention of the heterogeneous catalysis community. It remains a challenge to determine the thermodynamic stability of single atoms on an oxide support and compare their activity to that of small clusters and nanoparticles. We conducted density functional theory calculations to compare the stability of Au(CO) complexes on the CeO₂(1 1 1) terrace and step-edge of CeO₂(1 1 1) against CeO₂( 11 1)-supported nanoparticles. The different single atom Au and Au cluster models were compared for CO oxidation at low temperature. Trapped as dopants substituting for Ce in the surface or in a ceria O vacancy, Au cannot catalyze CO oxidation. Single Au atoms at step-edges represent candidate active sites for low-temperature CO oxidation. The CO oxidation at the interface between Au nanoparticles and CeO₂ can directly take place through a Mars-van Krevelen mechanism and account for a promising reactivity when the dislodgment of Au(CO) complex is hindered. The possibility of CO-induced dislodgement of a single Au atom depends critically on the topology of the Au-CeO₂ interface.

Original language	English
Pages (from-to)	353-363
Number of pages	11
Journal	Journal of Catalysis
Volume	407
DOIs	https://doi.org/10.1016/j.jcat.2022.02.008
Publication status	Published - Mar 2022

Bibliographical note

Funding Information:
This work is financially supported by the National Natural Science Foundation of China (No. 22103059). Y. Su acknowledges the ?Young Talent Support Plan? of Xi'an Jiaotong University and the Open Funds of State Key Laboratory of Physical Chemistry of Solid Surfaces (Xiamen University No. 202018). Supercomputing facilities were provided by The Netherlands Organization for Scientific Research (NWO) and Hefei Advanced Computing Center.

Keywords

CeO
CO oxidation
Density functional theory
Single-atom catalysis
Topology

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title = "Structure sensitivity of ceria-supported Au catalysts for CO oxidation",

abstract = "Single-atom catalysis is at the center of the attention of the heterogeneous catalysis community. It remains a challenge to determine the thermodynamic stability of single atoms on an oxide support and compare their activity to that of small clusters and nanoparticles. We conducted density functional theory calculations to compare the stability of Au(CO) complexes on the CeO2(1 1 1) terrace and step-edge of CeO2(1 1 1) against CeO2( 11 1)-supported nanoparticles. The different single atom Au and Au cluster models were compared for CO oxidation at low temperature. Trapped as dopants substituting for Ce in the surface or in a ceria O vacancy, Au cannot catalyze CO oxidation. Single Au atoms at step-edges represent candidate active sites for low-temperature CO oxidation. The CO oxidation at the interface between Au nanoparticles and CeO2 can directly take place through a Mars-van Krevelen mechanism and account for a promising reactivity when the dislodgment of Au(CO) complex is hindered. The possibility of CO-induced dislodgement of a single Au atom depends critically on the topology of the Au-CeO2 interface.",

keywords = "CeO, CO oxidation, Density functional theory, Single-atom catalysis, Topology",

author = "Su, {Ya Qiong} and Yan-Yang Qin and Tiantian Wu and De-Yin Wu",

note = "Funding Information: This work is financially supported by the National Natural Science Foundation of China (No. 22103059). Y. Su acknowledges the ?Young Talent Support Plan? of Xi'an Jiaotong University and the Open Funds of State Key Laboratory of Physical Chemistry of Solid Surfaces (Xiamen University No. 202018). Supercomputing facilities were provided by The Netherlands Organization for Scientific Research (NWO) and Hefei Advanced Computing Center. ",

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AU - Su, Ya Qiong

AU - Qin, Yan-Yang

AU - Wu, Tiantian

AU - Wu, De-Yin

N1 - Funding Information: This work is financially supported by the National Natural Science Foundation of China (No. 22103059). Y. Su acknowledges the ?Young Talent Support Plan? of Xi'an Jiaotong University and the Open Funds of State Key Laboratory of Physical Chemistry of Solid Surfaces (Xiamen University No. 202018). Supercomputing facilities were provided by The Netherlands Organization for Scientific Research (NWO) and Hefei Advanced Computing Center.

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N2 - Single-atom catalysis is at the center of the attention of the heterogeneous catalysis community. It remains a challenge to determine the thermodynamic stability of single atoms on an oxide support and compare their activity to that of small clusters and nanoparticles. We conducted density functional theory calculations to compare the stability of Au(CO) complexes on the CeO2(1 1 1) terrace and step-edge of CeO2(1 1 1) against CeO2( 11 1)-supported nanoparticles. The different single atom Au and Au cluster models were compared for CO oxidation at low temperature. Trapped as dopants substituting for Ce in the surface or in a ceria O vacancy, Au cannot catalyze CO oxidation. Single Au atoms at step-edges represent candidate active sites for low-temperature CO oxidation. The CO oxidation at the interface between Au nanoparticles and CeO2 can directly take place through a Mars-van Krevelen mechanism and account for a promising reactivity when the dislodgment of Au(CO) complex is hindered. The possibility of CO-induced dislodgement of a single Au atom depends critically on the topology of the Au-CeO2 interface.

AB - Single-atom catalysis is at the center of the attention of the heterogeneous catalysis community. It remains a challenge to determine the thermodynamic stability of single atoms on an oxide support and compare their activity to that of small clusters and nanoparticles. We conducted density functional theory calculations to compare the stability of Au(CO) complexes on the CeO2(1 1 1) terrace and step-edge of CeO2(1 1 1) against CeO2( 11 1)-supported nanoparticles. The different single atom Au and Au cluster models were compared for CO oxidation at low temperature. Trapped as dopants substituting for Ce in the surface or in a ceria O vacancy, Au cannot catalyze CO oxidation. Single Au atoms at step-edges represent candidate active sites for low-temperature CO oxidation. The CO oxidation at the interface between Au nanoparticles and CeO2 can directly take place through a Mars-van Krevelen mechanism and account for a promising reactivity when the dislodgment of Au(CO) complex is hindered. The possibility of CO-induced dislodgement of a single Au atom depends critically on the topology of the Au-CeO2 interface.

KW - CeO

KW - CO oxidation

KW - Density functional theory

KW - Single-atom catalysis

KW - Topology

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ER -

Structure sensitivity of ceria-supported Au catalysts for CO oxidation

Abstract

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Keywords

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