Is oxygen diffusion faster in bulk ceo2 or on a (111)-ceo2 surface? a theoretical study

Aditya Wibawa Sakti; Chien Pin Chou; Yoshifumi Nishimura; Hiromi Nakai

doi:10.1246/cl.200895

Is oxygen diffusion faster in bulk ceo2 or on a (111)-ceo2 surface? a theoretical study

Aditya Wibawa Sakti, Chien Pin Chou, Yoshifumi Nishimura, Hiromi Nakai^*

^*Corresponding author for this work

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

3 Citations (Scopus)

Abstract

Ceria (CeO2) is a promising metal-oxide support that is used in three-way catalysis (TWC). The activity of ceria-supported TWC depends on the location and concentration of oxygen vacancies. Oxygen diffusion can occur once the oxygen vacancy is created, and it leads to enhanced catalytic activity. In this study, the density-functional tight-binding method was used to estimate the free-energy barriers of oxygen diffusion in bulk CeO2 and on a (111)-CeO2 surface. The reconstructed freeenergy surfaces from metadynamics sampling show that the diffusion in the bulk CeO2 is faster than that on the (111)-CeO2 surface, with activation barriers of 7.4 and 31.6 kcal/mol, respectively.

Original language	English
Pages (from-to)	568-571
Number of pages	4
Journal	Chemistry Letters
Volume	50
Issue number	4
DOIs	https://doi.org/10.1246/cl.200895
Publication status	Published - 2021 Apr

Keywords

Metadynamics
Oxygen diffusion
Three-way catalyst

ASJC Scopus subject areas

Chemistry(all)

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10.1246/cl.200895

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title = "Is oxygen diffusion faster in bulk ceo2 or on a (111)-ceo2 surface? a theoretical study",

abstract = "Ceria (CeO2) is a promising metal-oxide support that is used in three-way catalysis (TWC). The activity of ceria-supported TWC depends on the location and concentration of oxygen vacancies. Oxygen diffusion can occur once the oxygen vacancy is created, and it leads to enhanced catalytic activity. In this study, the density-functional tight-binding method was used to estimate the free-energy barriers of oxygen diffusion in bulk CeO2 and on a (111)-CeO2 surface. The reconstructed freeenergy surfaces from metadynamics sampling show that the diffusion in the bulk CeO2 is faster than that on the (111)-CeO2 surface, with activation barriers of 7.4 and 31.6 kcal/mol, respectively.",

keywords = "Metadynamics, Oxygen diffusion, Three-way catalyst",

author = "Sakti, {Aditya Wibawa} and Chou, {Chien Pin} and Yoshifumi Nishimura and Hiromi Nakai",

note = "Funding Information: Parts of the presented calculations were performed at the Research Center for Computational Science (RCCS), Okazaki Research Facilities, Institute of Natural Sciences (NINS). This work was partly supported by a Grant-in-Aid for Scientific Research KAKENHI (Grant number: JP18H05264) from the Japan Society for the Promotion of Science (JSPS). This work was also supported by the Element Strategy Initiative (Grant number: JPMXP0112101003) from the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan. Publisher Copyright: {\textcopyright} 2021 Chemical Society of Japan. All rights reserved.",

year = "2021",

month = apr,

doi = "10.1246/cl.200895",

language = "English",

volume = "50",

pages = "568--571",

journal = "Chemistry Letters",

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T1 - Is oxygen diffusion faster in bulk ceo2 or on a (111)-ceo2 surface? a theoretical study

AU - Sakti, Aditya Wibawa

AU - Chou, Chien Pin

AU - Nishimura, Yoshifumi

AU - Nakai, Hiromi

N1 - Funding Information: Parts of the presented calculations were performed at the Research Center for Computational Science (RCCS), Okazaki Research Facilities, Institute of Natural Sciences (NINS). This work was partly supported by a Grant-in-Aid for Scientific Research KAKENHI (Grant number: JP18H05264) from the Japan Society for the Promotion of Science (JSPS). This work was also supported by the Element Strategy Initiative (Grant number: JPMXP0112101003) from the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan. Publisher Copyright: © 2021 Chemical Society of Japan. All rights reserved.

PY - 2021/4

Y1 - 2021/4

N2 - Ceria (CeO2) is a promising metal-oxide support that is used in three-way catalysis (TWC). The activity of ceria-supported TWC depends on the location and concentration of oxygen vacancies. Oxygen diffusion can occur once the oxygen vacancy is created, and it leads to enhanced catalytic activity. In this study, the density-functional tight-binding method was used to estimate the free-energy barriers of oxygen diffusion in bulk CeO2 and on a (111)-CeO2 surface. The reconstructed freeenergy surfaces from metadynamics sampling show that the diffusion in the bulk CeO2 is faster than that on the (111)-CeO2 surface, with activation barriers of 7.4 and 31.6 kcal/mol, respectively.

AB - Ceria (CeO2) is a promising metal-oxide support that is used in three-way catalysis (TWC). The activity of ceria-supported TWC depends on the location and concentration of oxygen vacancies. Oxygen diffusion can occur once the oxygen vacancy is created, and it leads to enhanced catalytic activity. In this study, the density-functional tight-binding method was used to estimate the free-energy barriers of oxygen diffusion in bulk CeO2 and on a (111)-CeO2 surface. The reconstructed freeenergy surfaces from metadynamics sampling show that the diffusion in the bulk CeO2 is faster than that on the (111)-CeO2 surface, with activation barriers of 7.4 and 31.6 kcal/mol, respectively.

KW - Metadynamics

KW - Oxygen diffusion

KW - Three-way catalyst

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JO - Chemistry Letters

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Is oxygen diffusion faster in bulk ceo2 or on a (111)-ceo2 surface? a theoretical study

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