Oxygen-Vacancy Dynamics and Entanglement with Polaron Hopping at the Reduced CeO2 (111) Surface

Autores
Zhang, Dawei; Han, Zhong Kang; Murgida, Gustavo Ezequiel; Ganduglia Pirovano, M. Verónica; Gao, Yi
Año de publicación
2019
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The migration of oxygen vacancies (VO) in ceria-based systems is crucial to their functionality in applications. Yet, although the VO's structure and the distribution of the Ce3+ polarons at the CeO2(111) surface has received extensive attention, the dynamic behaviors of VO's and polarons are not fully understood. By combining density functional theory calculations and ab initio molecular dynamics simulations, we show that the movements of VO's and polarons exhibit very distinct entanglement characteristics within a temperature range of 300-900 K, and that the positions of the Ce3+ polarons play a key role in the VO migration. Long-distance vacancy migration occurs at moderate temperatures when the "suitable" Ce3+ distribution remains long enough to promote oxygen migration. This study provides microscopic insight into the interplay between the electronic and ionic charge transport in ceria that will be beneficial for the rational design of conductive ceria-based materials.
Fil: Zhang, Dawei. Chinese Academy of Sciences. Shanghai Institute of Applied Physics ; China
Fil: Han, Zhong Kang. Chinese Academy of Sciences. Shanghai Institute of Applied Physics ; China. Chinese Academy of Sciences; República de China
Fil: Murgida, Gustavo Ezequiel. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Ganduglia Pirovano, M. Verónica. Consejo Superior de Investigaciones Científicas. Instituto de Catálisis y Petroleoquímica; España
Fil: Gao, Yi. Chinese Academy of Sciences. Shanghai Institute of Applied Physics ; China. Chinese Academy of Sciences; República de China
Materia
POLARONS
VACANCIES
OXIDES
MOLECULAR DYNAMICS
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/109120
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/109120
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Oxygen-Vacancy Dynamics and Entanglement with Polaron Hopping at the Reduced CeO2 (111) SurfaceZhang, DaweiHan, Zhong KangMurgida, Gustavo EzequielGanduglia Pirovano, M. VerónicaGao, YiPOLARONSVACANCIESOXIDESMOLECULAR DYNAMICShttps://purl.org/becyt/ford/1.3https://purl.org/becyt/ford/1The migration of oxygen vacancies (VO) in ceria-based systems is crucial to their functionality in applications. Yet, although the VO's structure and the distribution of the Ce3+ polarons at the CeO2(111) surface has received extensive attention, the dynamic behaviors of VO's and polarons are not fully understood. By combining density functional theory calculations and ab initio molecular dynamics simulations, we show that the movements of VO's and polarons exhibit very distinct entanglement characteristics within a temperature range of 300-900 K, and that the positions of the Ce3+ polarons play a key role in the VO migration. Long-distance vacancy migration occurs at moderate temperatures when the "suitable" Ce3+ distribution remains long enough to promote oxygen migration. This study provides microscopic insight into the interplay between the electronic and ionic charge transport in ceria that will be beneficial for the rational design of conductive ceria-based materials.Fil: Zhang, Dawei. Chinese Academy of Sciences. Shanghai Institute of Applied Physics ; ChinaFil: Han, Zhong Kang. Chinese Academy of Sciences. Shanghai Institute of Applied Physics ; China. Chinese Academy of Sciences; República de ChinaFil: Murgida, Gustavo Ezequiel. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Ganduglia Pirovano, M. Verónica. Consejo Superior de Investigaciones Científicas. Instituto de Catálisis y Petroleoquímica; EspañaFil: Gao, Yi. Chinese Academy of Sciences. Shanghai Institute of Applied Physics ; China. Chinese Academy of Sciences; República de ChinaAmerican Physical Society2019-03info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/109120Zhang, Dawei; Han, Zhong Kang; Murgida, Gustavo Ezequiel; Ganduglia Pirovano, M. Verónica; Gao, Yi; Oxygen-Vacancy Dynamics and Entanglement with Polaron Hopping at the Reduced CeO2 (111) Surface; American Physical Society; Physical Review Letters; 122; 9; 3-2019; 1-60031-9007CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://journals.aps.org/prl/abstract/10.1103/PhysRevLett.122.096101info:eu-repo/semantics/altIdentifier/doi/10.1103/PhysRevLett.122.096101info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-10T13:17:05Zoai:ri.conicet.gov.ar:11336/109120instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-09-10 13:17:05.236CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Oxygen-Vacancy Dynamics and Entanglement with Polaron Hopping at the Reduced CeO2 (111) Surface
title Oxygen-Vacancy Dynamics and Entanglement with Polaron Hopping at the Reduced CeO2 (111) Surface
spellingShingle Oxygen-Vacancy Dynamics and Entanglement with Polaron Hopping at the Reduced CeO2 (111) Surface
Zhang, Dawei
POLARONS
VACANCIES
OXIDES
MOLECULAR DYNAMICS
title_short Oxygen-Vacancy Dynamics and Entanglement with Polaron Hopping at the Reduced CeO2 (111) Surface
title_full Oxygen-Vacancy Dynamics and Entanglement with Polaron Hopping at the Reduced CeO2 (111) Surface
title_fullStr Oxygen-Vacancy Dynamics and Entanglement with Polaron Hopping at the Reduced CeO2 (111) Surface
title_full_unstemmed Oxygen-Vacancy Dynamics and Entanglement with Polaron Hopping at the Reduced CeO2 (111) Surface
title_sort Oxygen-Vacancy Dynamics and Entanglement with Polaron Hopping at the Reduced CeO2 (111) Surface
dc.creator.none.fl_str_mv Zhang, Dawei
Han, Zhong Kang
Murgida, Gustavo Ezequiel
Ganduglia Pirovano, M. Verónica
Gao, Yi
author Zhang, Dawei
author_facet Zhang, Dawei
Han, Zhong Kang
Murgida, Gustavo Ezequiel
Ganduglia Pirovano, M. Verónica
Gao, Yi
author_role author
author2 Han, Zhong Kang
Murgida, Gustavo Ezequiel
Ganduglia Pirovano, M. Verónica
Gao, Yi
author2_role author
author
author
author
dc.subject.none.fl_str_mv POLARONS
VACANCIES
OXIDES
MOLECULAR DYNAMICS
topic POLARONS
VACANCIES
OXIDES
MOLECULAR DYNAMICS
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.3
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv The migration of oxygen vacancies (VO) in ceria-based systems is crucial to their functionality in applications. Yet, although the VO's structure and the distribution of the Ce3+ polarons at the CeO2(111) surface has received extensive attention, the dynamic behaviors of VO's and polarons are not fully understood. By combining density functional theory calculations and ab initio molecular dynamics simulations, we show that the movements of VO's and polarons exhibit very distinct entanglement characteristics within a temperature range of 300-900 K, and that the positions of the Ce3+ polarons play a key role in the VO migration. Long-distance vacancy migration occurs at moderate temperatures when the "suitable" Ce3+ distribution remains long enough to promote oxygen migration. This study provides microscopic insight into the interplay between the electronic and ionic charge transport in ceria that will be beneficial for the rational design of conductive ceria-based materials.
Fil: Zhang, Dawei. Chinese Academy of Sciences. Shanghai Institute of Applied Physics ; China
Fil: Han, Zhong Kang. Chinese Academy of Sciences. Shanghai Institute of Applied Physics ; China. Chinese Academy of Sciences; República de China
Fil: Murgida, Gustavo Ezequiel. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Ganduglia Pirovano, M. Verónica. Consejo Superior de Investigaciones Científicas. Instituto de Catálisis y Petroleoquímica; España
Fil: Gao, Yi. Chinese Academy of Sciences. Shanghai Institute of Applied Physics ; China. Chinese Academy of Sciences; República de China
description The migration of oxygen vacancies (VO) in ceria-based systems is crucial to their functionality in applications. Yet, although the VO's structure and the distribution of the Ce3+ polarons at the CeO2(111) surface has received extensive attention, the dynamic behaviors of VO's and polarons are not fully understood. By combining density functional theory calculations and ab initio molecular dynamics simulations, we show that the movements of VO's and polarons exhibit very distinct entanglement characteristics within a temperature range of 300-900 K, and that the positions of the Ce3+ polarons play a key role in the VO migration. Long-distance vacancy migration occurs at moderate temperatures when the "suitable" Ce3+ distribution remains long enough to promote oxygen migration. This study provides microscopic insight into the interplay between the electronic and ionic charge transport in ceria that will be beneficial for the rational design of conductive ceria-based materials.
publishDate 2019
dc.date.none.fl_str_mv 2019-03
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/109120
Zhang, Dawei; Han, Zhong Kang; Murgida, Gustavo Ezequiel; Ganduglia Pirovano, M. Verónica; Gao, Yi; Oxygen-Vacancy Dynamics and Entanglement with Polaron Hopping at the Reduced CeO2 (111) Surface; American Physical Society; Physical Review Letters; 122; 9; 3-2019; 1-6
0031-9007
CONICET Digital
CONICET
url http://hdl.handle.net/11336/109120
identifier_str_mv Zhang, Dawei; Han, Zhong Kang; Murgida, Gustavo Ezequiel; Ganduglia Pirovano, M. Verónica; Gao, Yi; Oxygen-Vacancy Dynamics and Entanglement with Polaron Hopping at the Reduced CeO2 (111) Surface; American Physical Society; Physical Review Letters; 122; 9; 3-2019; 1-6
0031-9007
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/https://journals.aps.org/prl/abstract/10.1103/PhysRevLett.122.096101
info:eu-repo/semantics/altIdentifier/doi/10.1103/PhysRevLett.122.096101
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv American Physical Society
publisher.none.fl_str_mv American Physical Society
dc.source.none.fl_str_mv reponame:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
_version_ 1842980933524783104
score 12.993085

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