Mesoscopic behaviour of multi-layered graphene: The meaning of supercapacitance revisited

Autores
Gutierrez, Fabiana Andrea; Bedatty Fernandes, Flavio Cesar; Rivas, Gustavo Adolfo; Bueno, Paulo Roberto
Año de publicación
2017
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The electronic density of states and its contribution to the capacitance of graphene compounds (oxidized and reduced) were investigated using an electrochemical impedance-derived capacitance spectroscopic approach. It is clearly demonstrated that graphene oxide, which is known to exhibit semiconductor electronic characteristics, has little influence on the magnitude of the measured capacitance. Moreover, when graphene oxide is electrochemically reduced to graphene, the capacitance increases dramatically by about three orders of magnitude (from microfaradays to millifaradays). This increased capacitive effect has been interpreted as being directly associated with the electrochemical non-faradaic (super- or ultracapacitive) characteristics of the interface (i.e. associated with its electroactive area, for instance). The results obtained and interpretation made in this work demonstrate that the magnitude of the measured capacitance is a consequence of an electrochemical capacitive phenomenon (mesoscopic in essence; thus, the associated capacitance is equivalently termed mesoscopic capacitance) that energetically contains, in series, both electrostatic (geometrical) and quantum effects, thus being essentially different from those exclusively related to the amount of existing interfacial sites for ions (i.e. beyond those associated with pure double-layer capacitive effects). Conceptually, it is proposed that the mesoscopic capacitance of reduced graphene can be explained mainly through quantum chemical effects, ultimately following first-principles quantum mechanics supported on density functional theory, wherein the density of states is central.
Fil: Gutierrez, Fabiana Andrea. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina. Universidade Estadual Paulista Julio de Mesquita Filho; Brasil
Fil: Bedatty Fernandes, Flavio Cesar. Universidade Estadual Paulista Julio de Mesquita Filho; Brasil
Fil: Rivas, Gustavo Adolfo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina
Fil: Bueno, Paulo Roberto. Universidade Estadual Paulista Julio de Mesquita Filho; Brasil
Materia
Mesoscopic Capacitance
Electrostatic Effects
Quantum Effects
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:11336/62331
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/62331
network_acronym_str CONICETDig
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network_name_str CONICET Digital (CONICET)
spelling Mesoscopic behaviour of multi-layered graphene: The meaning of supercapacitance revisitedGutierrez, Fabiana AndreaBedatty Fernandes, Flavio CesarRivas, Gustavo AdolfoBueno, Paulo RobertoMesoscopic CapacitanceElectrostatic EffectsQuantum Effectshttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1The electronic density of states and its contribution to the capacitance of graphene compounds (oxidized and reduced) were investigated using an electrochemical impedance-derived capacitance spectroscopic approach. It is clearly demonstrated that graphene oxide, which is known to exhibit semiconductor electronic characteristics, has little influence on the magnitude of the measured capacitance. Moreover, when graphene oxide is electrochemically reduced to graphene, the capacitance increases dramatically by about three orders of magnitude (from microfaradays to millifaradays). This increased capacitive effect has been interpreted as being directly associated with the electrochemical non-faradaic (super- or ultracapacitive) characteristics of the interface (i.e. associated with its electroactive area, for instance). The results obtained and interpretation made in this work demonstrate that the magnitude of the measured capacitance is a consequence of an electrochemical capacitive phenomenon (mesoscopic in essence; thus, the associated capacitance is equivalently termed mesoscopic capacitance) that energetically contains, in series, both electrostatic (geometrical) and quantum effects, thus being essentially different from those exclusively related to the amount of existing interfacial sites for ions (i.e. beyond those associated with pure double-layer capacitive effects). Conceptually, it is proposed that the mesoscopic capacitance of reduced graphene can be explained mainly through quantum chemical effects, ultimately following first-principles quantum mechanics supported on density functional theory, wherein the density of states is central.Fil: Gutierrez, Fabiana Andrea. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina. Universidade Estadual Paulista Julio de Mesquita Filho; BrasilFil: Bedatty Fernandes, Flavio Cesar. Universidade Estadual Paulista Julio de Mesquita Filho; BrasilFil: Rivas, Gustavo Adolfo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; ArgentinaFil: Bueno, Paulo Roberto. Universidade Estadual Paulista Julio de Mesquita Filho; BrasilRoyal Society of Chemistry2017-01-06info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/62331Gutierrez, Fabiana Andrea; Bedatty Fernandes, Flavio Cesar; Rivas, Gustavo Adolfo; Bueno, Paulo Roberto; Mesoscopic behaviour of multi-layered graphene: The meaning of supercapacitance revisited; Royal Society of Chemistry; Physical Chemistry Chemical Physics; 19; 9; 6-1-2017; 6792-68061463-90761463-9084CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://pubs.rsc.org/en/Content/ArticleLanding/2017/CP/C6CP07775Ginfo:eu-repo/semantics/altIdentifier/doi/10.1039/C6CP07775Ginfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T10:26:23Zoai:ri.conicet.gov.ar:11336/62331instacron: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 10:26:24.143CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Mesoscopic behaviour of multi-layered graphene: The meaning of supercapacitance revisited
title Mesoscopic behaviour of multi-layered graphene: The meaning of supercapacitance revisited
spellingShingle Mesoscopic behaviour of multi-layered graphene: The meaning of supercapacitance revisited
Gutierrez, Fabiana Andrea
Mesoscopic Capacitance
Electrostatic Effects
Quantum Effects
title_short Mesoscopic behaviour of multi-layered graphene: The meaning of supercapacitance revisited
title_full Mesoscopic behaviour of multi-layered graphene: The meaning of supercapacitance revisited
title_fullStr Mesoscopic behaviour of multi-layered graphene: The meaning of supercapacitance revisited
title_full_unstemmed Mesoscopic behaviour of multi-layered graphene: The meaning of supercapacitance revisited
title_sort Mesoscopic behaviour of multi-layered graphene: The meaning of supercapacitance revisited
dc.creator.none.fl_str_mv Gutierrez, Fabiana Andrea
Bedatty Fernandes, Flavio Cesar
Rivas, Gustavo Adolfo
Bueno, Paulo Roberto
author Gutierrez, Fabiana Andrea
author_facet Gutierrez, Fabiana Andrea
Bedatty Fernandes, Flavio Cesar
Rivas, Gustavo Adolfo
Bueno, Paulo Roberto
author_role author
author2 Bedatty Fernandes, Flavio Cesar
Rivas, Gustavo Adolfo
Bueno, Paulo Roberto
author2_role author
author
author
dc.subject.none.fl_str_mv Mesoscopic Capacitance
Electrostatic Effects
Quantum Effects
topic Mesoscopic Capacitance
Electrostatic Effects
Quantum Effects
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv The electronic density of states and its contribution to the capacitance of graphene compounds (oxidized and reduced) were investigated using an electrochemical impedance-derived capacitance spectroscopic approach. It is clearly demonstrated that graphene oxide, which is known to exhibit semiconductor electronic characteristics, has little influence on the magnitude of the measured capacitance. Moreover, when graphene oxide is electrochemically reduced to graphene, the capacitance increases dramatically by about three orders of magnitude (from microfaradays to millifaradays). This increased capacitive effect has been interpreted as being directly associated with the electrochemical non-faradaic (super- or ultracapacitive) characteristics of the interface (i.e. associated with its electroactive area, for instance). The results obtained and interpretation made in this work demonstrate that the magnitude of the measured capacitance is a consequence of an electrochemical capacitive phenomenon (mesoscopic in essence; thus, the associated capacitance is equivalently termed mesoscopic capacitance) that energetically contains, in series, both electrostatic (geometrical) and quantum effects, thus being essentially different from those exclusively related to the amount of existing interfacial sites for ions (i.e. beyond those associated with pure double-layer capacitive effects). Conceptually, it is proposed that the mesoscopic capacitance of reduced graphene can be explained mainly through quantum chemical effects, ultimately following first-principles quantum mechanics supported on density functional theory, wherein the density of states is central.
Fil: Gutierrez, Fabiana Andrea. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina. Universidade Estadual Paulista Julio de Mesquita Filho; Brasil
Fil: Bedatty Fernandes, Flavio Cesar. Universidade Estadual Paulista Julio de Mesquita Filho; Brasil
Fil: Rivas, Gustavo Adolfo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina
Fil: Bueno, Paulo Roberto. Universidade Estadual Paulista Julio de Mesquita Filho; Brasil
description The electronic density of states and its contribution to the capacitance of graphene compounds (oxidized and reduced) were investigated using an electrochemical impedance-derived capacitance spectroscopic approach. It is clearly demonstrated that graphene oxide, which is known to exhibit semiconductor electronic characteristics, has little influence on the magnitude of the measured capacitance. Moreover, when graphene oxide is electrochemically reduced to graphene, the capacitance increases dramatically by about three orders of magnitude (from microfaradays to millifaradays). This increased capacitive effect has been interpreted as being directly associated with the electrochemical non-faradaic (super- or ultracapacitive) characteristics of the interface (i.e. associated with its electroactive area, for instance). The results obtained and interpretation made in this work demonstrate that the magnitude of the measured capacitance is a consequence of an electrochemical capacitive phenomenon (mesoscopic in essence; thus, the associated capacitance is equivalently termed mesoscopic capacitance) that energetically contains, in series, both electrostatic (geometrical) and quantum effects, thus being essentially different from those exclusively related to the amount of existing interfacial sites for ions (i.e. beyond those associated with pure double-layer capacitive effects). Conceptually, it is proposed that the mesoscopic capacitance of reduced graphene can be explained mainly through quantum chemical effects, ultimately following first-principles quantum mechanics supported on density functional theory, wherein the density of states is central.
publishDate 2017
dc.date.none.fl_str_mv 2017-01-06
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/11336/62331
Gutierrez, Fabiana Andrea; Bedatty Fernandes, Flavio Cesar; Rivas, Gustavo Adolfo; Bueno, Paulo Roberto; Mesoscopic behaviour of multi-layered graphene: The meaning of supercapacitance revisited; Royal Society of Chemistry; Physical Chemistry Chemical Physics; 19; 9; 6-1-2017; 6792-6806
1463-9076
1463-9084
CONICET Digital
CONICET
url http://hdl.handle.net/11336/62331
identifier_str_mv Gutierrez, Fabiana Andrea; Bedatty Fernandes, Flavio Cesar; Rivas, Gustavo Adolfo; Bueno, Paulo Roberto; Mesoscopic behaviour of multi-layered graphene: The meaning of supercapacitance revisited; Royal Society of Chemistry; Physical Chemistry Chemical Physics; 19; 9; 6-1-2017; 6792-6806
1463-9076
1463-9084
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://pubs.rsc.org/en/Content/ArticleLanding/2017/CP/C6CP07775G
info:eu-repo/semantics/altIdentifier/doi/10.1039/C6CP07775G
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
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 13.070432

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