Structural evolution, optical gap and thermoelectric properties of CH3NH3SnBr3 hybrid perovskite, prepared by mechanochemistry

Autores
Lopez, Carlos Alberto; Abia, Carmen; Gainza, Javier; Kayser, Paula; Nemes, Norbert; Dura, Oscar J.; Martinez, Jose L.; Fernandez Diaz, Maria Teresa; Alvarez Galvan, M. Consuelo; Alonso, José Antonio
Año de publicación
2021
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Direct bandgap semiconductors of the hybrid-perovskite family CH3NH3PbX3 (X = I, Br, Cl) exhibit outstanding light absorption properties and are the materials of choice for solar energy applications. As an alternative to poisonous Pb, tin-containing perovskites would show a lower effective mass thus exhibiting a higher charge carrier mobility. An auspicious candidate is CH3NH3SnBr3, with an estimated band gap of 1.902 eV, anticipating applications in photovoltaic devices for the visible to ultra-violet wavelength region. We describe that this perovskite can be prepared by ball milling in a straightforward way, yielding specimens with a superior crystallinity. A structural investigation from synchrotron X-ray powder diffraction (SXRD) data was essential to revisit the successive phase transitions this compound experiences down to 120 K, guided by specific heat capacity and DSC measurements. From the cubic structure identified at RT and 270 K, there is a gradual evolution of the patterns, analysed as a phase admixture between the cubic and the low-symmetry phase present at 160 K. This corresponds to an orthorhombic Pmc21 superstructure; this acentric space group enables polarization along the c-axis where there is a twofold screw axis, evidenced in the distribution of Sn-Br distances. Furthermore, there are two conspicuous changes in the orthorhombic framework, yet keeping the Pmc21 space group, which agree with the main calorimetric events (observed at 224 and 147 K). We interpret these changes as an interplay between the tilting of the SnBr6 octahedra of the inorganic framework and the breaking and reconstruction of H-bond interactions with the organic CH3NH+3 unit. The stereochemical effect of the lone electron pair of the Sn2+ ion is clear in the SnBr6 octahedral distortion. Diffuse reflectance UV/Vis spectroscopy yields an optical gap of ∼2.1 eV, in agreement with ab- initio calculations. A Seebeck coefficient of ∼2000 μV K-1 is determined near RT, which is one order of magnitude higher than those reported for other halide perovskites.
Fil: Lopez, Carlos Alberto. 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. Instituto de Ciencia de Materiales de Madrid; España
Fil: Abia, Carmen. Institut Laue Langevin; Francia. Instituto de Ciencia de Materiales de Madrid; España
Fil: Gainza, Javier. Instituto de Ciencia de Materiales de Madrid; España
Fil: Kayser, Paula. Instituto de Ciencia de Materiales de Madrid; España
Fil: Nemes, Norbert. Instituto de Ciencia de Materiales de Madrid; España
Fil: Dura, Oscar J.. Universidad de Castilla-La Mancha; España
Fil: Martinez, Jose L.. Instituto de Ciencia de Materiales de Madrid; España
Fil: Fernandez Diaz, Maria Teresa. Institut Laue Langevin; Francia
Fil: Alvarez Galvan, M. Consuelo. Consejo Superior de Investigaciones Científicas; España
Fil: Alonso, José Antonio. Instituto de Ciencia de Materiales de Madrid; España
Materia
CH3NH3SnBr3
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/171878
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/171878
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Structural evolution, optical gap and thermoelectric properties of CH3NH3SnBr3 hybrid perovskite, prepared by mechanochemistryLopez, Carlos AlbertoAbia, CarmenGainza, JavierKayser, PaulaNemes, NorbertDura, Oscar J.Martinez, Jose L.Fernandez Diaz, Maria TeresaAlvarez Galvan, M. ConsueloAlonso, José AntonioCH3NH3SnBr3https://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Direct bandgap semiconductors of the hybrid-perovskite family CH3NH3PbX3 (X = I, Br, Cl) exhibit outstanding light absorption properties and are the materials of choice for solar energy applications. As an alternative to poisonous Pb, tin-containing perovskites would show a lower effective mass thus exhibiting a higher charge carrier mobility. An auspicious candidate is CH3NH3SnBr3, with an estimated band gap of 1.902 eV, anticipating applications in photovoltaic devices for the visible to ultra-violet wavelength region. We describe that this perovskite can be prepared by ball milling in a straightforward way, yielding specimens with a superior crystallinity. A structural investigation from synchrotron X-ray powder diffraction (SXRD) data was essential to revisit the successive phase transitions this compound experiences down to 120 K, guided by specific heat capacity and DSC measurements. From the cubic structure identified at RT and 270 K, there is a gradual evolution of the patterns, analysed as a phase admixture between the cubic and the low-symmetry phase present at 160 K. This corresponds to an orthorhombic Pmc21 superstructure; this acentric space group enables polarization along the c-axis where there is a twofold screw axis, evidenced in the distribution of Sn-Br distances. Furthermore, there are two conspicuous changes in the orthorhombic framework, yet keeping the Pmc21 space group, which agree with the main calorimetric events (observed at 224 and 147 K). We interpret these changes as an interplay between the tilting of the SnBr6 octahedra of the inorganic framework and the breaking and reconstruction of H-bond interactions with the organic CH3NH+3 unit. The stereochemical effect of the lone electron pair of the Sn2+ ion is clear in the SnBr6 octahedral distortion. Diffuse reflectance UV/Vis spectroscopy yields an optical gap of ∼2.1 eV, in agreement with ab- initio calculations. A Seebeck coefficient of ∼2000 μV K-1 is determined near RT, which is one order of magnitude higher than those reported for other halide perovskites.Fil: Lopez, Carlos Alberto. 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. Instituto de Ciencia de Materiales de Madrid; EspañaFil: Abia, Carmen. Institut Laue Langevin; Francia. Instituto de Ciencia de Materiales de Madrid; EspañaFil: Gainza, Javier. Instituto de Ciencia de Materiales de Madrid; EspañaFil: Kayser, Paula. Instituto de Ciencia de Materiales de Madrid; EspañaFil: Nemes, Norbert. Instituto de Ciencia de Materiales de Madrid; EspañaFil: Dura, Oscar J.. Universidad de Castilla-La Mancha; EspañaFil: Martinez, Jose L.. Instituto de Ciencia de Materiales de Madrid; EspañaFil: Fernandez Diaz, Maria Teresa. Institut Laue Langevin; FranciaFil: Alvarez Galvan, M. Consuelo. Consejo Superior de Investigaciones Científicas; EspañaFil: Alonso, José Antonio. Instituto de Ciencia de Materiales de Madrid; EspañaRoyal Society of Chemistry2021-04info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/171878Lopez, Carlos Alberto; Abia, Carmen; Gainza, Javier; Kayser, Paula; Nemes, Norbert; et al.; Structural evolution, optical gap and thermoelectric properties of CH3NH3SnBr3 hybrid perovskite, prepared by mechanochemistry; Royal Society of Chemistry; Materials Advances; 2; 11; 4-2021; 3620-36282633-5409CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://pubs.rsc.org/en/Content/ArticleLanding/2021/MA/D1MA00196Einfo:eu-repo/semantics/altIdentifier/doi/10.1039/D1MA00196Einfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-22T11:03:44Zoai:ri.conicet.gov.ar:11336/171878instacron: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 11:03:45.091CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Structural evolution, optical gap and thermoelectric properties of CH3NH3SnBr3 hybrid perovskite, prepared by mechanochemistry
title Structural evolution, optical gap and thermoelectric properties of CH3NH3SnBr3 hybrid perovskite, prepared by mechanochemistry
spellingShingle Structural evolution, optical gap and thermoelectric properties of CH3NH3SnBr3 hybrid perovskite, prepared by mechanochemistry
Lopez, Carlos Alberto
CH3NH3SnBr3
title_short Structural evolution, optical gap and thermoelectric properties of CH3NH3SnBr3 hybrid perovskite, prepared by mechanochemistry
title_full Structural evolution, optical gap and thermoelectric properties of CH3NH3SnBr3 hybrid perovskite, prepared by mechanochemistry
title_fullStr Structural evolution, optical gap and thermoelectric properties of CH3NH3SnBr3 hybrid perovskite, prepared by mechanochemistry
title_full_unstemmed Structural evolution, optical gap and thermoelectric properties of CH3NH3SnBr3 hybrid perovskite, prepared by mechanochemistry
title_sort Structural evolution, optical gap and thermoelectric properties of CH3NH3SnBr3 hybrid perovskite, prepared by mechanochemistry
dc.creator.none.fl_str_mv Lopez, Carlos Alberto
Abia, Carmen
Gainza, Javier
Kayser, Paula
Nemes, Norbert
Dura, Oscar J.
Martinez, Jose L.
Fernandez Diaz, Maria Teresa
Alvarez Galvan, M. Consuelo
Alonso, José Antonio
author Lopez, Carlos Alberto
author_facet Lopez, Carlos Alberto
Abia, Carmen
Gainza, Javier
Kayser, Paula
Nemes, Norbert
Dura, Oscar J.
Martinez, Jose L.
Fernandez Diaz, Maria Teresa
Alvarez Galvan, M. Consuelo
Alonso, José Antonio
author_role author
author2 Abia, Carmen
Gainza, Javier
Kayser, Paula
Nemes, Norbert
Dura, Oscar J.
Martinez, Jose L.
Fernandez Diaz, Maria Teresa
Alvarez Galvan, M. Consuelo
Alonso, José Antonio
author2_role author
author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv CH3NH3SnBr3
topic CH3NH3SnBr3
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Direct bandgap semiconductors of the hybrid-perovskite family CH3NH3PbX3 (X = I, Br, Cl) exhibit outstanding light absorption properties and are the materials of choice for solar energy applications. As an alternative to poisonous Pb, tin-containing perovskites would show a lower effective mass thus exhibiting a higher charge carrier mobility. An auspicious candidate is CH3NH3SnBr3, with an estimated band gap of 1.902 eV, anticipating applications in photovoltaic devices for the visible to ultra-violet wavelength region. We describe that this perovskite can be prepared by ball milling in a straightforward way, yielding specimens with a superior crystallinity. A structural investigation from synchrotron X-ray powder diffraction (SXRD) data was essential to revisit the successive phase transitions this compound experiences down to 120 K, guided by specific heat capacity and DSC measurements. From the cubic structure identified at RT and 270 K, there is a gradual evolution of the patterns, analysed as a phase admixture between the cubic and the low-symmetry phase present at 160 K. This corresponds to an orthorhombic Pmc21 superstructure; this acentric space group enables polarization along the c-axis where there is a twofold screw axis, evidenced in the distribution of Sn-Br distances. Furthermore, there are two conspicuous changes in the orthorhombic framework, yet keeping the Pmc21 space group, which agree with the main calorimetric events (observed at 224 and 147 K). We interpret these changes as an interplay between the tilting of the SnBr6 octahedra of the inorganic framework and the breaking and reconstruction of H-bond interactions with the organic CH3NH+3 unit. The stereochemical effect of the lone electron pair of the Sn2+ ion is clear in the SnBr6 octahedral distortion. Diffuse reflectance UV/Vis spectroscopy yields an optical gap of ∼2.1 eV, in agreement with ab- initio calculations. A Seebeck coefficient of ∼2000 μV K-1 is determined near RT, which is one order of magnitude higher than those reported for other halide perovskites.
Fil: Lopez, Carlos Alberto. 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. Instituto de Ciencia de Materiales de Madrid; España
Fil: Abia, Carmen. Institut Laue Langevin; Francia. Instituto de Ciencia de Materiales de Madrid; España
Fil: Gainza, Javier. Instituto de Ciencia de Materiales de Madrid; España
Fil: Kayser, Paula. Instituto de Ciencia de Materiales de Madrid; España
Fil: Nemes, Norbert. Instituto de Ciencia de Materiales de Madrid; España
Fil: Dura, Oscar J.. Universidad de Castilla-La Mancha; España
Fil: Martinez, Jose L.. Instituto de Ciencia de Materiales de Madrid; España
Fil: Fernandez Diaz, Maria Teresa. Institut Laue Langevin; Francia
Fil: Alvarez Galvan, M. Consuelo. Consejo Superior de Investigaciones Científicas; España
Fil: Alonso, José Antonio. Instituto de Ciencia de Materiales de Madrid; España
description Direct bandgap semiconductors of the hybrid-perovskite family CH3NH3PbX3 (X = I, Br, Cl) exhibit outstanding light absorption properties and are the materials of choice for solar energy applications. As an alternative to poisonous Pb, tin-containing perovskites would show a lower effective mass thus exhibiting a higher charge carrier mobility. An auspicious candidate is CH3NH3SnBr3, with an estimated band gap of 1.902 eV, anticipating applications in photovoltaic devices for the visible to ultra-violet wavelength region. We describe that this perovskite can be prepared by ball milling in a straightforward way, yielding specimens with a superior crystallinity. A structural investigation from synchrotron X-ray powder diffraction (SXRD) data was essential to revisit the successive phase transitions this compound experiences down to 120 K, guided by specific heat capacity and DSC measurements. From the cubic structure identified at RT and 270 K, there is a gradual evolution of the patterns, analysed as a phase admixture between the cubic and the low-symmetry phase present at 160 K. This corresponds to an orthorhombic Pmc21 superstructure; this acentric space group enables polarization along the c-axis where there is a twofold screw axis, evidenced in the distribution of Sn-Br distances. Furthermore, there are two conspicuous changes in the orthorhombic framework, yet keeping the Pmc21 space group, which agree with the main calorimetric events (observed at 224 and 147 K). We interpret these changes as an interplay between the tilting of the SnBr6 octahedra of the inorganic framework and the breaking and reconstruction of H-bond interactions with the organic CH3NH+3 unit. The stereochemical effect of the lone electron pair of the Sn2+ ion is clear in the SnBr6 octahedral distortion. Diffuse reflectance UV/Vis spectroscopy yields an optical gap of ∼2.1 eV, in agreement with ab- initio calculations. A Seebeck coefficient of ∼2000 μV K-1 is determined near RT, which is one order of magnitude higher than those reported for other halide perovskites.
publishDate 2021
dc.date.none.fl_str_mv 2021-04
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/11336/171878
Lopez, Carlos Alberto; Abia, Carmen; Gainza, Javier; Kayser, Paula; Nemes, Norbert; et al.; Structural evolution, optical gap and thermoelectric properties of CH3NH3SnBr3 hybrid perovskite, prepared by mechanochemistry; Royal Society of Chemistry; Materials Advances; 2; 11; 4-2021; 3620-3628
2633-5409
CONICET Digital
CONICET
url http://hdl.handle.net/11336/171878
identifier_str_mv Lopez, Carlos Alberto; Abia, Carmen; Gainza, Javier; Kayser, Paula; Nemes, Norbert; et al.; Structural evolution, optical gap and thermoelectric properties of CH3NH3SnBr3 hybrid perovskite, prepared by mechanochemistry; Royal Society of Chemistry; Materials Advances; 2; 11; 4-2021; 3620-3628
2633-5409
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/http://pubs.rsc.org/en/Content/ArticleLanding/2021/MA/D1MA00196E
info:eu-repo/semantics/altIdentifier/doi/10.1039/D1MA00196E
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv Royal Society of Chemistry
publisher.none.fl_str_mv Royal Society of Chemistry
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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