Evidence of hydrogen content and monovalent Ni oxidation state in non-superconducting bulk anchored infinite-layer nickelates

Autores
Gainza, Javier; Lopez, Carlos Alberto; Serrano Sánchez, Federico; Rodrigues, João Elias F. S.; Rosa, Angelika D.; Sobrados, María Isabel; Nemes, Norbert M.; Biskup, Neven; Fernández Díaz, María Teresa; Martínez, José Luis; Alonso, José Antonio
Año de publicación
2023
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Since superconductivity was first reported in nickelate thin films, many studies have been published about this family of materials, and different hypotheses have been proposed for explaining the mechanisms and structural dependence. Here, we report the synthesis of anchored infinite-layer LaNi0.9Al0.1O2.1 and its hole-doped derivatives by topotactic reduction from La1−xSrxNi0.9Al0.1O3 rhombohedral perovskites. LaNiO2 derivatives constitute a new family of high-temperature superconductors, with the same structure as high-Tc cuprates but based on nickel, only showing superconductivity in thin films for now. We describe a strategy to stabilize LaNiO2 derivatives in bulk: the presence of Al at the octahedral sites helps to stabilize/anchor the infinite-layer structure. The reasons for the bulk being non-superconductors are hotly debated in the literature. An important question is whether there is some hydrogen incorporated into the structure during the reduction process from LaNiO3 to LaNiO2, predicted theoretically but not reported experimentally. Our neutron powder diffraction data show that, indeed, hydrogen occupies the centers of the Ni–O squares, and spectroscopic evidence from EELS and XAS suggests that Ni is reduced to the Ni+ oxidation state, consistent with the crystallochemical data.
Fil: Gainza, Javier. Instituto de Ciencia de Materiales de Madrid; España
Fil: Lopez, Carlos Alberto. Universidad Nacional de San Luis. Facultad de Química, Bioquímica y Farmacia; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis. Instituto de Investigaciones en Tecnología Química. Universidad Nacional de San Luis. Facultad de Química, Bioquímica y Farmacia. Instituto de Investigaciones en Tecnología Química; Argentina
Fil: Serrano Sánchez, Federico. Instituto de Ciencia de Materiales de Madrid; España
Fil: Rodrigues, João Elias F. S.. European Synchrotron Radiation Facility; Francia
Fil: Rosa, Angelika D.. European Synchrotron Radiation Facility; Francia
Fil: Sobrados, María Isabel. Instituto de Ciencia de Materiales de Madrid; España
Fil: Nemes, Norbert M.. Instituto de Ciencia de Materiales de Madrid; España. Universidad Complutense de Madrid; España
Fil: Biskup, Neven. Universidad Complutense de Madrid; España
Fil: Fernández Díaz, María Teresa. Institut Laue Langevin; Francia
Fil: Martínez, José Luis. Instituto de Ciencia de Materiales de Madrid; España
Fil: Alonso, José Antonio. Instituto de Ciencia de Materiales de Madrid; España
Materia
Hydrogen
Oxidation
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:11336/231970
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/231970
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Evidence of hydrogen content and monovalent Ni oxidation state in non-superconducting bulk anchored infinite-layer nickelatesGainza, JavierLopez, Carlos AlbertoSerrano Sánchez, FedericoRodrigues, João Elias F. S.Rosa, Angelika D.Sobrados, María IsabelNemes, Norbert M.Biskup, NevenFernández Díaz, María TeresaMartínez, José LuisAlonso, José AntonioHydrogenOxidationhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Since superconductivity was first reported in nickelate thin films, many studies have been published about this family of materials, and different hypotheses have been proposed for explaining the mechanisms and structural dependence. Here, we report the synthesis of anchored infinite-layer LaNi0.9Al0.1O2.1 and its hole-doped derivatives by topotactic reduction from La1−xSrxNi0.9Al0.1O3 rhombohedral perovskites. LaNiO2 derivatives constitute a new family of high-temperature superconductors, with the same structure as high-Tc cuprates but based on nickel, only showing superconductivity in thin films for now. We describe a strategy to stabilize LaNiO2 derivatives in bulk: the presence of Al at the octahedral sites helps to stabilize/anchor the infinite-layer structure. The reasons for the bulk being non-superconductors are hotly debated in the literature. An important question is whether there is some hydrogen incorporated into the structure during the reduction process from LaNiO3 to LaNiO2, predicted theoretically but not reported experimentally. Our neutron powder diffraction data show that, indeed, hydrogen occupies the centers of the Ni–O squares, and spectroscopic evidence from EELS and XAS suggests that Ni is reduced to the Ni+ oxidation state, consistent with the crystallochemical data.Fil: Gainza, Javier. Instituto de Ciencia de Materiales de Madrid; EspañaFil: Lopez, Carlos Alberto. Universidad Nacional de San Luis. Facultad de Química, Bioquímica y Farmacia; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis. Instituto de Investigaciones en Tecnología Química. Universidad Nacional de San Luis. Facultad de Química, Bioquímica y Farmacia. Instituto de Investigaciones en Tecnología Química; ArgentinaFil: Serrano Sánchez, Federico. Instituto de Ciencia de Materiales de Madrid; EspañaFil: Rodrigues, João Elias F. S.. European Synchrotron Radiation Facility; FranciaFil: Rosa, Angelika D.. European Synchrotron Radiation Facility; FranciaFil: Sobrados, María Isabel. Instituto de Ciencia de Materiales de Madrid; EspañaFil: Nemes, Norbert M.. Instituto de Ciencia de Materiales de Madrid; España. Universidad Complutense de Madrid; EspañaFil: Biskup, Neven. Universidad Complutense de Madrid; EspañaFil: Fernández Díaz, María Teresa. Institut Laue Langevin; FranciaFil: Martínez, José Luis. Instituto de Ciencia de Materiales de Madrid; EspañaFil: Alonso, José Antonio. Instituto de Ciencia de Materiales de Madrid; EspañaCell Press2023-12info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/231970Gainza, Javier; Lopez, Carlos Alberto; Serrano Sánchez, Federico; Rodrigues, João Elias F. S.; Rosa, Angelika D.; et al.; Evidence of hydrogen content and monovalent Ni oxidation state in non-superconducting bulk anchored infinite-layer nickelates; Cell Press; Cell Reports Physical Science; 4; 12; 12-2023; 1-162666-3864CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1016/j.xcrp.2023.101724info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S2666386423005696info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-nd/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-22T11:25:28Zoai:ri.conicet.gov.ar:11336/231970instacron: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:34982025-10-22 11:25:29.275CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Evidence of hydrogen content and monovalent Ni oxidation state in non-superconducting bulk anchored infinite-layer nickelates
title Evidence of hydrogen content and monovalent Ni oxidation state in non-superconducting bulk anchored infinite-layer nickelates
spellingShingle Evidence of hydrogen content and monovalent Ni oxidation state in non-superconducting bulk anchored infinite-layer nickelates
Gainza, Javier
Hydrogen
Oxidation
title_short Evidence of hydrogen content and monovalent Ni oxidation state in non-superconducting bulk anchored infinite-layer nickelates
title_full Evidence of hydrogen content and monovalent Ni oxidation state in non-superconducting bulk anchored infinite-layer nickelates
title_fullStr Evidence of hydrogen content and monovalent Ni oxidation state in non-superconducting bulk anchored infinite-layer nickelates
title_full_unstemmed Evidence of hydrogen content and monovalent Ni oxidation state in non-superconducting bulk anchored infinite-layer nickelates
title_sort Evidence of hydrogen content and monovalent Ni oxidation state in non-superconducting bulk anchored infinite-layer nickelates
dc.creator.none.fl_str_mv Gainza, Javier
Lopez, Carlos Alberto
Serrano Sánchez, Federico
Rodrigues, João Elias F. S.
Rosa, Angelika D.
Sobrados, María Isabel
Nemes, Norbert M.
Biskup, Neven
Fernández Díaz, María Teresa
Martínez, José Luis
Alonso, José Antonio
author Gainza, Javier
author_facet Gainza, Javier
Lopez, Carlos Alberto
Serrano Sánchez, Federico
Rodrigues, João Elias F. S.
Rosa, Angelika D.
Sobrados, María Isabel
Nemes, Norbert M.
Biskup, Neven
Fernández Díaz, María Teresa
Martínez, José Luis
Alonso, José Antonio
author_role author
author2 Lopez, Carlos Alberto
Serrano Sánchez, Federico
Rodrigues, João Elias F. S.
Rosa, Angelika D.
Sobrados, María Isabel
Nemes, Norbert M.
Biskup, Neven
Fernández Díaz, María Teresa
Martínez, José Luis
Alonso, José Antonio
author2_role author
author
author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv Hydrogen
Oxidation
topic Hydrogen
Oxidation
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Since superconductivity was first reported in nickelate thin films, many studies have been published about this family of materials, and different hypotheses have been proposed for explaining the mechanisms and structural dependence. Here, we report the synthesis of anchored infinite-layer LaNi0.9Al0.1O2.1 and its hole-doped derivatives by topotactic reduction from La1−xSrxNi0.9Al0.1O3 rhombohedral perovskites. LaNiO2 derivatives constitute a new family of high-temperature superconductors, with the same structure as high-Tc cuprates but based on nickel, only showing superconductivity in thin films for now. We describe a strategy to stabilize LaNiO2 derivatives in bulk: the presence of Al at the octahedral sites helps to stabilize/anchor the infinite-layer structure. The reasons for the bulk being non-superconductors are hotly debated in the literature. An important question is whether there is some hydrogen incorporated into the structure during the reduction process from LaNiO3 to LaNiO2, predicted theoretically but not reported experimentally. Our neutron powder diffraction data show that, indeed, hydrogen occupies the centers of the Ni–O squares, and spectroscopic evidence from EELS and XAS suggests that Ni is reduced to the Ni+ oxidation state, consistent with the crystallochemical data.
Fil: Gainza, Javier. Instituto de Ciencia de Materiales de Madrid; España
Fil: Lopez, Carlos Alberto. Universidad Nacional de San Luis. Facultad de Química, Bioquímica y Farmacia; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis. Instituto de Investigaciones en Tecnología Química. Universidad Nacional de San Luis. Facultad de Química, Bioquímica y Farmacia. Instituto de Investigaciones en Tecnología Química; Argentina
Fil: Serrano Sánchez, Federico. Instituto de Ciencia de Materiales de Madrid; España
Fil: Rodrigues, João Elias F. S.. European Synchrotron Radiation Facility; Francia
Fil: Rosa, Angelika D.. European Synchrotron Radiation Facility; Francia
Fil: Sobrados, María Isabel. Instituto de Ciencia de Materiales de Madrid; España
Fil: Nemes, Norbert M.. Instituto de Ciencia de Materiales de Madrid; España. Universidad Complutense de Madrid; España
Fil: Biskup, Neven. Universidad Complutense de Madrid; España
Fil: Fernández Díaz, María Teresa. Institut Laue Langevin; Francia
Fil: Martínez, José Luis. Instituto de Ciencia de Materiales de Madrid; España
Fil: Alonso, José Antonio. Instituto de Ciencia de Materiales de Madrid; España
description Since superconductivity was first reported in nickelate thin films, many studies have been published about this family of materials, and different hypotheses have been proposed for explaining the mechanisms and structural dependence. Here, we report the synthesis of anchored infinite-layer LaNi0.9Al0.1O2.1 and its hole-doped derivatives by topotactic reduction from La1−xSrxNi0.9Al0.1O3 rhombohedral perovskites. LaNiO2 derivatives constitute a new family of high-temperature superconductors, with the same structure as high-Tc cuprates but based on nickel, only showing superconductivity in thin films for now. We describe a strategy to stabilize LaNiO2 derivatives in bulk: the presence of Al at the octahedral sites helps to stabilize/anchor the infinite-layer structure. The reasons for the bulk being non-superconductors are hotly debated in the literature. An important question is whether there is some hydrogen incorporated into the structure during the reduction process from LaNiO3 to LaNiO2, predicted theoretically but not reported experimentally. Our neutron powder diffraction data show that, indeed, hydrogen occupies the centers of the Ni–O squares, and spectroscopic evidence from EELS and XAS suggests that Ni is reduced to the Ni+ oxidation state, consistent with the crystallochemical data.
publishDate 2023
dc.date.none.fl_str_mv 2023-12
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/11336/231970
Gainza, Javier; Lopez, Carlos Alberto; Serrano Sánchez, Federico; Rodrigues, João Elias F. S.; Rosa, Angelika D.; et al.; Evidence of hydrogen content and monovalent Ni oxidation state in non-superconducting bulk anchored infinite-layer nickelates; Cell Press; Cell Reports Physical Science; 4; 12; 12-2023; 1-16
2666-3864
CONICET Digital
CONICET
url http://hdl.handle.net/11336/231970
identifier_str_mv Gainza, Javier; Lopez, Carlos Alberto; Serrano Sánchez, Federico; Rodrigues, João Elias F. S.; Rosa, Angelika D.; et al.; Evidence of hydrogen content and monovalent Ni oxidation state in non-superconducting bulk anchored infinite-layer nickelates; Cell Press; Cell Reports Physical Science; 4; 12; 12-2023; 1-16
2666-3864
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.xcrp.2023.101724
info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S2666386423005696
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 Cell Press
publisher.none.fl_str_mv Cell Press
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
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score 12.982451

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