Connecting the surface structure, morphology and photocatalytic activity of Ag2O: An in depth and unified theoretical investigation
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Publication Date: | 2020 |
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Format: | Article |
Language: | eng |
Source: | Repositório Institucional da UFRN |
Download full: | https://repositorio.ufrn.br/handle/123456789/38003 |
Summary: | The surface morphology of the materials is known to have significant influence on the overall photocatalytic performance. Therefore, identifying the corresponding electronic structures associated with the surface redox centers is essential for the rational design of Ag2O-based photocatalysts. In this study, comprehensive and sys- tematic theoretical calculations revealed the connection between electronic structure and morphology responsible for the photo-induced mechanism. First-principles calculations showed that the activity of Ag+ cations on the exposed surfaces is dependent of their local coordination and electronic configuration. Electrons were found to migrate to the energetically favorable (1 1 1) surface, while holes are concentrated in the more unstable (1 0 0) and (1 1 0) surfaces. The complete set of available morphologies was obtained, enabling us to rationalize the photocatalytic activity in terms of composition, geometry, and electronic structure of the exposed surfaces. Moreover, the localization and characterization of excited electronic states of both bulk material and exposed surfaces allow us to discuss the fundamental reactions involved in the photocatalytic mechanism underlying the morphological evolution and would promote significantly the development and application of singlet-triplet mechanism. The detailed insights provided by our work could benefit the design and preparation of new efficient photocatalysts based on Ag2O |
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Ribeiro, Renan Augusto PontesOliveira, Marisa Carvalho deDelmonte, Maurício Roberto BomioLazaro, Sérgio Ricardo deAndrés, JuanSilva, Elson Longo da2021-09-24T12:31:15Z2021-09-24T12:31:15Z2020-04-15RIBEIRO, R.A.P.; OLIVEIRA, M.C.; BOMIO, M.R.D.; LAZARO, S.R. de; ANDRÉS, J.; LONGO, E.. Connecting the surface structure, morphology and photocatalytic activity of Ag2O: an in depth and unified theoretical investigation. Applied Surface Science, [S.L.], v. 509, p. 145321, abr. 2020. Disponível em: https://www.sciencedirect.com/science/article/abs/pii/S0169433220300775?via%3Dihub#!. Acesso em: 20 abr. 2021. http://dx.doi.org/10.1016/j.apsusc.2020.145321.0169-4332https://repositorio.ufrn.br/handle/123456789/3800310.1016/j.apsusc.2020.145321ElsevierAttribution 3.0 Brazilinfo:eu-repo/semantics/openAccessPhotocatalysisAg2OSurface structureDensity functional theoryMorphologyFundamental and excited electronic statesConnecting the surface structure, morphology and photocatalytic activity of Ag2O: An in depth and unified theoretical investigationinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/articleThe surface morphology of the materials is known to have significant influence on the overall photocatalytic performance. Therefore, identifying the corresponding electronic structures associated with the surface redox centers is essential for the rational design of Ag2O-based photocatalysts. In this study, comprehensive and sys- tematic theoretical calculations revealed the connection between electronic structure and morphology responsible for the photo-induced mechanism. First-principles calculations showed that the activity of Ag+ cations on the exposed surfaces is dependent of their local coordination and electronic configuration. Electrons were found to migrate to the energetically favorable (1 1 1) surface, while holes are concentrated in the more unstable (1 0 0) and (1 1 0) surfaces. The complete set of available morphologies was obtained, enabling us to rationalize the photocatalytic activity in terms of composition, geometry, and electronic structure of the exposed surfaces. Moreover, the localization and characterization of excited electronic states of both bulk material and exposed surfaces allow us to discuss the fundamental reactions involved in the photocatalytic mechanism underlying the morphological evolution and would promote significantly the development and application of singlet-triplet mechanism. The detailed insights provided by our work could benefit the design and preparation of new efficient photocatalysts based on Ag2Oengreponame:Repositório Institucional da UFRNinstname:Universidade Federal do Rio Grande do Norte (UFRN)instacron:UFRNORIGINALConnectingSurfaceStructure_BOMIO_2020.pdfConnectingSurfaceStructure_BOMIO_2020.pdfapplication/pdf4301551https://repositorio.ufrn.br/bitstream/123456789/38003/4/ConnectingSurfaceStructure_BOMIO_2020.pdf3125fc2583f67b68e046e9562e173a7fMD54CC-LICENSElicense_rdflicense_rdfapplication/rdf+xml; charset=utf-8914https://repositorio.ufrn.br/bitstream/123456789/38003/2/license_rdf4d2950bda3d176f570a9f8b328dfbbefMD52LICENSElicense.txtlicense.txttext/plain; charset=utf-81484https://repositorio.ufrn.br/bitstream/123456789/38003/3/license.txte9597aa2854d128fd968be5edc8a28d9MD53123456789/380032022-12-15 18:28:54.983oai:https://repositorio.ufrn.br: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Repositório de PublicaçõesPUBhttp://repositorio.ufrn.br/oai/opendoar:2022-12-15T21:28:54Repositório Institucional da UFRN - Universidade Federal do Rio Grande do Norte (UFRN)false |
dc.title.pt_BR.fl_str_mv |
Connecting the surface structure, morphology and photocatalytic activity of Ag2O: An in depth and unified theoretical investigation |
title |
Connecting the surface structure, morphology and photocatalytic activity of Ag2O: An in depth and unified theoretical investigation |
spellingShingle |
Connecting the surface structure, morphology and photocatalytic activity of Ag2O: An in depth and unified theoretical investigation Ribeiro, Renan Augusto Pontes Photocatalysis Ag2O Surface structure Density functional theory Morphology Fundamental and excited electronic states |
title_short |
Connecting the surface structure, morphology and photocatalytic activity of Ag2O: An in depth and unified theoretical investigation |
title_full |
Connecting the surface structure, morphology and photocatalytic activity of Ag2O: An in depth and unified theoretical investigation |
title_fullStr |
Connecting the surface structure, morphology and photocatalytic activity of Ag2O: An in depth and unified theoretical investigation |
title_full_unstemmed |
Connecting the surface structure, morphology and photocatalytic activity of Ag2O: An in depth and unified theoretical investigation |
title_sort |
Connecting the surface structure, morphology and photocatalytic activity of Ag2O: An in depth and unified theoretical investigation |
author |
Ribeiro, Renan Augusto Pontes |
author_facet |
Ribeiro, Renan Augusto Pontes Oliveira, Marisa Carvalho de Delmonte, Maurício Roberto Bomio Lazaro, Sérgio Ricardo de Andrés, Juan Silva, Elson Longo da |
author_role |
author |
author2 |
Oliveira, Marisa Carvalho de Delmonte, Maurício Roberto Bomio Lazaro, Sérgio Ricardo de Andrés, Juan Silva, Elson Longo da |
author2_role |
author author author author author |
dc.contributor.author.fl_str_mv |
Ribeiro, Renan Augusto Pontes Oliveira, Marisa Carvalho de Delmonte, Maurício Roberto Bomio Lazaro, Sérgio Ricardo de Andrés, Juan Silva, Elson Longo da |
dc.subject.por.fl_str_mv |
Photocatalysis Ag2O Surface structure Density functional theory Morphology Fundamental and excited electronic states |
topic |
Photocatalysis Ag2O Surface structure Density functional theory Morphology Fundamental and excited electronic states |
description |
The surface morphology of the materials is known to have significant influence on the overall photocatalytic performance. Therefore, identifying the corresponding electronic structures associated with the surface redox centers is essential for the rational design of Ag2O-based photocatalysts. In this study, comprehensive and sys- tematic theoretical calculations revealed the connection between electronic structure and morphology responsible for the photo-induced mechanism. First-principles calculations showed that the activity of Ag+ cations on the exposed surfaces is dependent of their local coordination and electronic configuration. Electrons were found to migrate to the energetically favorable (1 1 1) surface, while holes are concentrated in the more unstable (1 0 0) and (1 1 0) surfaces. The complete set of available morphologies was obtained, enabling us to rationalize the photocatalytic activity in terms of composition, geometry, and electronic structure of the exposed surfaces. Moreover, the localization and characterization of excited electronic states of both bulk material and exposed surfaces allow us to discuss the fundamental reactions involved in the photocatalytic mechanism underlying the morphological evolution and would promote significantly the development and application of singlet-triplet mechanism. The detailed insights provided by our work could benefit the design and preparation of new efficient photocatalysts based on Ag2O |
publishDate |
2020 |
dc.date.issued.fl_str_mv |
2020-04-15 |
dc.date.accessioned.fl_str_mv |
2021-09-24T12:31:15Z |
dc.date.available.fl_str_mv |
2021-09-24T12:31:15Z |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/article |
format |
article |
status_str |
publishedVersion |
dc.identifier.citation.fl_str_mv |
RIBEIRO, R.A.P.; OLIVEIRA, M.C.; BOMIO, M.R.D.; LAZARO, S.R. de; ANDRÉS, J.; LONGO, E.. Connecting the surface structure, morphology and photocatalytic activity of Ag2O: an in depth and unified theoretical investigation. Applied Surface Science, [S.L.], v. 509, p. 145321, abr. 2020. Disponível em: https://www.sciencedirect.com/science/article/abs/pii/S0169433220300775?via%3Dihub#!. Acesso em: 20 abr. 2021. http://dx.doi.org/10.1016/j.apsusc.2020.145321. |
dc.identifier.uri.fl_str_mv |
https://repositorio.ufrn.br/handle/123456789/38003 |
dc.identifier.issn.none.fl_str_mv |
0169-4332 |
dc.identifier.doi.none.fl_str_mv |
10.1016/j.apsusc.2020.145321 |
identifier_str_mv |
RIBEIRO, R.A.P.; OLIVEIRA, M.C.; BOMIO, M.R.D.; LAZARO, S.R. de; ANDRÉS, J.; LONGO, E.. Connecting the surface structure, morphology and photocatalytic activity of Ag2O: an in depth and unified theoretical investigation. Applied Surface Science, [S.L.], v. 509, p. 145321, abr. 2020. Disponível em: https://www.sciencedirect.com/science/article/abs/pii/S0169433220300775?via%3Dihub#!. Acesso em: 20 abr. 2021. http://dx.doi.org/10.1016/j.apsusc.2020.145321. 0169-4332 10.1016/j.apsusc.2020.145321 |
url |
https://repositorio.ufrn.br/handle/123456789/38003 |
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eng |
language |
eng |
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Attribution 3.0 Brazil info:eu-repo/semantics/openAccess |
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Attribution 3.0 Brazil |
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openAccess |
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Elsevier |
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Elsevier |
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