Mechanisms of enhanced sulfur tolerance on samarium (Sm)-doped cerium oxide (CeO2) from first principles

Dong Hee Lim; Hee Su Kim; Sung Pil Yoon; Jonghee Han; Chang Won Yoon; Sun Hee Choi; Suk Woo Nam; Hyung Chul Ham

doi:10.1039/c4cp00777h

Mechanisms of enhanced sulfur tolerance on samarium (Sm)-doped cerium oxide (CeO₂) from first principles

Dong Hee Lim, Hee Su Kim, Sung Pil Yoon, Jonghee Han, Chang Won Yoon, Sun Hee Choi, Suk Woo Nam, Hyung Chul Ham

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

18 Citations (Scopus)

Abstract

The role of samarium (Sm) 4f states and Sm-perturbed O 2p states in determining the sulfur tolerance of Sm-doped CeO₂ was elucidated by using the density functional theory (DFT) + U calculation. We find that the sulfur tolerance of Sm-doped CeO₂ is closely related to the modification of O 2p states by the strong interaction between Sm 4f and O 2p states. In particular, the availability of unoccupied O 2p states near the Fermi level is responsible for enhancing the sulfur tolerance of Sm-doped CeO ₂ compared to the pure CeO₂ by increasing the activity of the surface lattice oxygen toward sulfur adsorption, by weakening the interaction between Sm-O, and by increasing the migration tendency of the subsurface oxygen ion toward the surface. This journal is

Original language	English
Pages (from-to)	10727-10733
Number of pages	7
Journal	Physical Chemistry Chemical Physics
Volume	16
Issue number	22
DOIs	https://doi.org/10.1039/c4cp00777h
Publication status	Published - 2014 Jun 14

ASJC Scopus subject areas

General Physics and Astronomy
Physical and Theoretical Chemistry

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title = "Mechanisms of enhanced sulfur tolerance on samarium (Sm)-doped cerium oxide (CeO2) from first principles",

abstract = "The role of samarium (Sm) 4f states and Sm-perturbed O 2p states in determining the sulfur tolerance of Sm-doped CeO2 was elucidated by using the density functional theory (DFT) + U calculation. We find that the sulfur tolerance of Sm-doped CeO2 is closely related to the modification of O 2p states by the strong interaction between Sm 4f and O 2p states. In particular, the availability of unoccupied O 2p states near the Fermi level is responsible for enhancing the sulfur tolerance of Sm-doped CeO 2 compared to the pure CeO2 by increasing the activity of the surface lattice oxygen toward sulfur adsorption, by weakening the interaction between Sm-O, and by increasing the migration tendency of the subsurface oxygen ion toward the surface. This journal is",

author = "Lim, {Dong Hee} and Kim, {Hee Su} and Yoon, {Sung Pil} and Jonghee Han and Yoon, {Chang Won} and Choi, {Sun Hee} and Nam, {Suk Woo} and Ham, {Hyung Chul}",

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AU - Lim, Dong Hee

AU - Kim, Hee Su

AU - Yoon, Sung Pil

AU - Han, Jonghee

AU - Yoon, Chang Won

AU - Choi, Sun Hee

AU - Nam, Suk Woo

AU - Ham, Hyung Chul

PY - 2014/6/14

Y1 - 2014/6/14

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Mechanisms of enhanced sulfur tolerance on samarium (Sm)-doped cerium oxide (CeO₂) from first principles

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