Local Environments in Iron-Bearing Clay Minerals by DFT Approaches: The Case of Structural Fe in Kaolinite

Autores
Richard, Diego; Rendtorff Birrer, Nicolás Maximiliano
Año de publicación
2021
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Technological properties of kaolins depend on the internal structure of the particles that constitute them. For this reason, unraveling the structural features from the micro to the nanoscale is a permanent matter of interest, even in the case of raw samples. From the experimental point of view, because naturally-occurring kaolins contain iron, Mössbauer spectroscopy is a very convenient technique to reach the nanoscopic scale avoiding experimental difficulties related to the sample's lack of structural order at the crystallographic scale. In this work, first-principles calculations based on the Density Functional Theory (DFT) were used to model such iron environments in kaolinite, and to assess the performance of the Gauge-Included Projector Augmented Waves (GIPAW) method to describe the changes to the host structure and the electronic modifications produced by the iron atoms. To this purpose, structural relaxation, Grimme's D2 dispersion, and Hubbard corrections (DFT+U approach) were considered. A detailed analysis was done for the obtained predictions for the Fe local structure, oxidation state, and Mössbauer quadrupole splitting, including comparisons with available experimental data. The results contribute to better understand the naturally-occurring kaolins, and support the DFT+U approach for the description of the layer structure and the electronic properties of iron-containing clay minerals.
Fil: Richard, Diego. Provincia de Buenos Aires. Gobernación. Comisión de Investigaciones Científicas. Centro de Tecnología de Recursos Minerales y Cerámica. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Centro de Tecnología de Recursos Minerales y Cerámica; Argentina. Universidad Nacional de La Plata. Facultad de Ciencias Exactas; Argentina
Fil: Rendtorff Birrer, Nicolás Maximiliano. Provincia de Buenos Aires. Gobernación. Comisión de Investigaciones Científicas. Centro de Tecnología de Recursos Minerales y Cerámica. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Centro de Tecnología de Recursos Minerales y Cerámica; Argentina. Universidad Nacional de La Plata. Facultad de Ciencias Exactas; Argentina
Materia
CLAY
DFT
ELECTRON TRANSFER
IRON-DOPED MATERIALS
KAOLINITE
MÖSSBAUER
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/180769
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/180769
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Local Environments in Iron-Bearing Clay Minerals by DFT Approaches: The Case of Structural Fe in KaoliniteRichard, DiegoRendtorff Birrer, Nicolás MaximilianoCLAYDFTELECTRON TRANSFERIRON-DOPED MATERIALSKAOLINITEMÖSSBAUERhttps://purl.org/becyt/ford/2.5https://purl.org/becyt/ford/2https://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1https://purl.org/becyt/ford/1.5https://purl.org/becyt/ford/1Technological properties of kaolins depend on the internal structure of the particles that constitute them. For this reason, unraveling the structural features from the micro to the nanoscale is a permanent matter of interest, even in the case of raw samples. From the experimental point of view, because naturally-occurring kaolins contain iron, Mössbauer spectroscopy is a very convenient technique to reach the nanoscopic scale avoiding experimental difficulties related to the sample's lack of structural order at the crystallographic scale. In this work, first-principles calculations based on the Density Functional Theory (DFT) were used to model such iron environments in kaolinite, and to assess the performance of the Gauge-Included Projector Augmented Waves (GIPAW) method to describe the changes to the host structure and the electronic modifications produced by the iron atoms. To this purpose, structural relaxation, Grimme's D2 dispersion, and Hubbard corrections (DFT+U approach) were considered. A detailed analysis was done for the obtained predictions for the Fe local structure, oxidation state, and Mössbauer quadrupole splitting, including comparisons with available experimental data. The results contribute to better understand the naturally-occurring kaolins, and support the DFT+U approach for the description of the layer structure and the electronic properties of iron-containing clay minerals.Fil: Richard, Diego. Provincia de Buenos Aires. Gobernación. Comisión de Investigaciones Científicas. Centro de Tecnología de Recursos Minerales y Cerámica. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Centro de Tecnología de Recursos Minerales y Cerámica; Argentina. Universidad Nacional de La Plata. Facultad de Ciencias Exactas; ArgentinaFil: Rendtorff Birrer, Nicolás Maximiliano. Provincia de Buenos Aires. Gobernación. Comisión de Investigaciones Científicas. Centro de Tecnología de Recursos Minerales y Cerámica. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Centro de Tecnología de Recursos Minerales y Cerámica; Argentina. Universidad Nacional de La Plata. Facultad de Ciencias Exactas; ArgentinaElsevier Science2021-11info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/180769Richard, Diego; Rendtorff Birrer, Nicolás Maximiliano; Local Environments in Iron-Bearing Clay Minerals by DFT Approaches: The Case of Structural Fe in Kaolinite; Elsevier Science; Applied Clay Science; 213; 106251; 11-2021; 1-80169-1317CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1016/j.clay.2021.106251info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0169131721002751info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-nd/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T10:33:56Zoai:ri.conicet.gov.ar:11336/180769instacron: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:34982025-09-29 10:33:56.708CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Local Environments in Iron-Bearing Clay Minerals by DFT Approaches: The Case of Structural Fe in Kaolinite
title Local Environments in Iron-Bearing Clay Minerals by DFT Approaches: The Case of Structural Fe in Kaolinite
spellingShingle Local Environments in Iron-Bearing Clay Minerals by DFT Approaches: The Case of Structural Fe in Kaolinite
Richard, Diego
CLAY
DFT
ELECTRON TRANSFER
IRON-DOPED MATERIALS
KAOLINITE
MÖSSBAUER
title_short Local Environments in Iron-Bearing Clay Minerals by DFT Approaches: The Case of Structural Fe in Kaolinite
title_full Local Environments in Iron-Bearing Clay Minerals by DFT Approaches: The Case of Structural Fe in Kaolinite
title_fullStr Local Environments in Iron-Bearing Clay Minerals by DFT Approaches: The Case of Structural Fe in Kaolinite
title_full_unstemmed Local Environments in Iron-Bearing Clay Minerals by DFT Approaches: The Case of Structural Fe in Kaolinite
title_sort Local Environments in Iron-Bearing Clay Minerals by DFT Approaches: The Case of Structural Fe in Kaolinite
dc.creator.none.fl_str_mv Richard, Diego
Rendtorff Birrer, Nicolás Maximiliano
author Richard, Diego
author_facet Richard, Diego
Rendtorff Birrer, Nicolás Maximiliano
author_role author
author2 Rendtorff Birrer, Nicolás Maximiliano
author2_role author
dc.subject.none.fl_str_mv CLAY
DFT
ELECTRON TRANSFER
IRON-DOPED MATERIALS
KAOLINITE
MÖSSBAUER
topic CLAY
DFT
ELECTRON TRANSFER
IRON-DOPED MATERIALS
KAOLINITE
MÖSSBAUER
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.5
https://purl.org/becyt/ford/2
https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
https://purl.org/becyt/ford/1.5
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Technological properties of kaolins depend on the internal structure of the particles that constitute them. For this reason, unraveling the structural features from the micro to the nanoscale is a permanent matter of interest, even in the case of raw samples. From the experimental point of view, because naturally-occurring kaolins contain iron, Mössbauer spectroscopy is a very convenient technique to reach the nanoscopic scale avoiding experimental difficulties related to the sample's lack of structural order at the crystallographic scale. In this work, first-principles calculations based on the Density Functional Theory (DFT) were used to model such iron environments in kaolinite, and to assess the performance of the Gauge-Included Projector Augmented Waves (GIPAW) method to describe the changes to the host structure and the electronic modifications produced by the iron atoms. To this purpose, structural relaxation, Grimme's D2 dispersion, and Hubbard corrections (DFT+U approach) were considered. A detailed analysis was done for the obtained predictions for the Fe local structure, oxidation state, and Mössbauer quadrupole splitting, including comparisons with available experimental data. The results contribute to better understand the naturally-occurring kaolins, and support the DFT+U approach for the description of the layer structure and the electronic properties of iron-containing clay minerals.
Fil: Richard, Diego. Provincia de Buenos Aires. Gobernación. Comisión de Investigaciones Científicas. Centro de Tecnología de Recursos Minerales y Cerámica. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Centro de Tecnología de Recursos Minerales y Cerámica; Argentina. Universidad Nacional de La Plata. Facultad de Ciencias Exactas; Argentina
Fil: Rendtorff Birrer, Nicolás Maximiliano. Provincia de Buenos Aires. Gobernación. Comisión de Investigaciones Científicas. Centro de Tecnología de Recursos Minerales y Cerámica. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Centro de Tecnología de Recursos Minerales y Cerámica; Argentina. Universidad Nacional de La Plata. Facultad de Ciencias Exactas; Argentina
description Technological properties of kaolins depend on the internal structure of the particles that constitute them. For this reason, unraveling the structural features from the micro to the nanoscale is a permanent matter of interest, even in the case of raw samples. From the experimental point of view, because naturally-occurring kaolins contain iron, Mössbauer spectroscopy is a very convenient technique to reach the nanoscopic scale avoiding experimental difficulties related to the sample's lack of structural order at the crystallographic scale. In this work, first-principles calculations based on the Density Functional Theory (DFT) were used to model such iron environments in kaolinite, and to assess the performance of the Gauge-Included Projector Augmented Waves (GIPAW) method to describe the changes to the host structure and the electronic modifications produced by the iron atoms. To this purpose, structural relaxation, Grimme's D2 dispersion, and Hubbard corrections (DFT+U approach) were considered. A detailed analysis was done for the obtained predictions for the Fe local structure, oxidation state, and Mössbauer quadrupole splitting, including comparisons with available experimental data. The results contribute to better understand the naturally-occurring kaolins, and support the DFT+U approach for the description of the layer structure and the electronic properties of iron-containing clay minerals.
publishDate 2021
dc.date.none.fl_str_mv 2021-11
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/11336/180769
Richard, Diego; Rendtorff Birrer, Nicolás Maximiliano; Local Environments in Iron-Bearing Clay Minerals by DFT Approaches: The Case of Structural Fe in Kaolinite; Elsevier Science; Applied Clay Science; 213; 106251; 11-2021; 1-8
0169-1317
CONICET Digital
CONICET
url http://hdl.handle.net/11336/180769
identifier_str_mv Richard, Diego; Rendtorff Birrer, Nicolás Maximiliano; Local Environments in Iron-Bearing Clay Minerals by DFT Approaches: The Case of Structural Fe in Kaolinite; Elsevier Science; Applied Clay Science; 213; 106251; 11-2021; 1-8
0169-1317
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1016/j.clay.2021.106251
info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0169131721002751
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv Elsevier Science
publisher.none.fl_str_mv Elsevier Science
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_ 1844614355115573248
score 13.070432

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