Direct Observation of Spatially Heterogeneous Single-Layer Graphene Oxide Reduction Kinetics

Autores
McDonald, Matthew P.; Eltom, Ahmed; Vietmeyer, Felix; Thapa, Janak; Morozov, Yurii V.; Sokolov, Denis A.; Hodak, Jose Hector; Vinodgopal, Kizhanipuram; Kamat, Prashant V.; Kuno, Masaru
Año de publicación
2013
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Graphene oxide (GO) is an important precursor in the production of chemically derived graphene. During reduction, GO’s electrical conductivity and band gap change gradually. Doping and chemical functionalization are also possible, illustrating GO’s immense potential in creating functional devices through control of its local hybridization. Here we show that laser-induced photolysis controllably reduces individual single-layer GO sheets. The reaction can be followed in real time through sizable decreases in GO’s photoluminescence efficiency along with spectral blueshifts. As-produced reduced graphene oxide (rGO) sheets undergo additional photolysis, characterized by dramatic emission enhancements and spectral redshifts. Both GO’s reduction and subsequent conversion to photobrightened rGO are captured through movies of their photoluminescence kinetics. Rate maps illustrate sizable spatial and temporal heterogeneities in sp2 domain growth and reveal how reduction “flows” across GO and rGO sheets. The observed heterogeneous reduction kinetics provides mechanistic insight into GO’s conversion to chemically derived graphene and highlights opportunities for overcoming its dynamic, chemical disorder.
Fil: McDonald, Matthew P. . University Of Notre Dame-indiana; Estados Unidos
Fil: Eltom, Ahmed . University Of Waterloo; Canadá
Fil: Vietmeyer, Felix . University Of Notre Dame-indiana; Estados Unidos
Fil: Thapa, Janak . Illinois Wesleyan University; Estados Unidos
Fil: Morozov, Yurii V. . Taras Shevchenko National University of Kiev; Ucrania
Fil: Sokolov, Denis A. . University Of Notre Dame-indiana; Estados Unidos
Fil: Hodak, Jose Hector. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina. Universidad de Buenos Aires; Argentina
Fil: Vinodgopal, Kizhanipuram . North Carolina Central University; Estados Unidos
Fil: Kamat, Prashant V. . University Of Notre Dame-indiana; Estados Unidos
Fil: Kuno, Masaru . University Of Notre Dame-indiana; Estados Unidos
Materia
Graphene Oxide
Reduced Graphene Oxide
Photolysis
Reduction
Photobrightening
Fluorescence Intermittency
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:11336/8113
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/8113
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Direct Observation of Spatially Heterogeneous Single-Layer Graphene Oxide Reduction KineticsMcDonald, Matthew P. Eltom, Ahmed Vietmeyer, Felix Thapa, Janak Morozov, Yurii V. Sokolov, Denis A. Hodak, Jose HectorVinodgopal, Kizhanipuram Kamat, Prashant V. Kuno, Masaru Graphene OxideReduced Graphene OxidePhotolysisReductionPhotobrighteningFluorescence Intermittencyhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Graphene oxide (GO) is an important precursor in the production of chemically derived graphene. During reduction, GO’s electrical conductivity and band gap change gradually. Doping and chemical functionalization are also possible, illustrating GO’s immense potential in creating functional devices through control of its local hybridization. Here we show that laser-induced photolysis controllably reduces individual single-layer GO sheets. The reaction can be followed in real time through sizable decreases in GO’s photoluminescence efficiency along with spectral blueshifts. As-produced reduced graphene oxide (rGO) sheets undergo additional photolysis, characterized by dramatic emission enhancements and spectral redshifts. Both GO’s reduction and subsequent conversion to photobrightened rGO are captured through movies of their photoluminescence kinetics. Rate maps illustrate sizable spatial and temporal heterogeneities in sp2 domain growth and reveal how reduction “flows” across GO and rGO sheets. The observed heterogeneous reduction kinetics provides mechanistic insight into GO’s conversion to chemically derived graphene and highlights opportunities for overcoming its dynamic, chemical disorder.Fil: McDonald, Matthew P. . University Of Notre Dame-indiana; Estados UnidosFil: Eltom, Ahmed . University Of Waterloo; CanadáFil: Vietmeyer, Felix . University Of Notre Dame-indiana; Estados UnidosFil: Thapa, Janak . Illinois Wesleyan University; Estados UnidosFil: Morozov, Yurii V. . Taras Shevchenko National University of Kiev; UcraniaFil: Sokolov, Denis A. . University Of Notre Dame-indiana; Estados UnidosFil: Hodak, Jose Hector. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina. Universidad de Buenos Aires; ArgentinaFil: Vinodgopal, Kizhanipuram . North Carolina Central University; Estados UnidosFil: Kamat, Prashant V. . University Of Notre Dame-indiana; Estados UnidosFil: Kuno, Masaru . University Of Notre Dame-indiana; Estados UnidosAmerican Chemical Society2013-11info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/8113McDonald, Matthew P. ; Eltom, Ahmed ; Vietmeyer, Felix ; Thapa, Janak ; Morozov, Yurii V. ; et al.; Direct Observation of Spatially Heterogeneous Single-Layer Graphene Oxide Reduction Kinetics; American Chemical Society; Nano Letters; 13; 12; 11-2013; 5777-57841530-6984enginfo:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/abs/10.1021/nl402057jinfo:eu-repo/semantics/altIdentifier/doi/10.1021/nl402057jinfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-10T13:07:35Zoai:ri.conicet.gov.ar:11336/8113instacron: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:34982025-09-10 13:07:35.491CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Direct Observation of Spatially Heterogeneous Single-Layer Graphene Oxide Reduction Kinetics
title Direct Observation of Spatially Heterogeneous Single-Layer Graphene Oxide Reduction Kinetics
spellingShingle Direct Observation of Spatially Heterogeneous Single-Layer Graphene Oxide Reduction Kinetics
McDonald, Matthew P.
Graphene Oxide
Reduced Graphene Oxide
Photolysis
Reduction
Photobrightening
Fluorescence Intermittency
title_short Direct Observation of Spatially Heterogeneous Single-Layer Graphene Oxide Reduction Kinetics
title_full Direct Observation of Spatially Heterogeneous Single-Layer Graphene Oxide Reduction Kinetics
title_fullStr Direct Observation of Spatially Heterogeneous Single-Layer Graphene Oxide Reduction Kinetics
title_full_unstemmed Direct Observation of Spatially Heterogeneous Single-Layer Graphene Oxide Reduction Kinetics
title_sort Direct Observation of Spatially Heterogeneous Single-Layer Graphene Oxide Reduction Kinetics
dc.creator.none.fl_str_mv McDonald, Matthew P.
Eltom, Ahmed
Vietmeyer, Felix
Thapa, Janak
Morozov, Yurii V.
Sokolov, Denis A.
Hodak, Jose Hector
Vinodgopal, Kizhanipuram
Kamat, Prashant V.
Kuno, Masaru
author McDonald, Matthew P.
author_facet McDonald, Matthew P.
Eltom, Ahmed
Vietmeyer, Felix
Thapa, Janak
Morozov, Yurii V.
Sokolov, Denis A.
Hodak, Jose Hector
Vinodgopal, Kizhanipuram
Kamat, Prashant V.
Kuno, Masaru
author_role author
author2 Eltom, Ahmed
Vietmeyer, Felix
Thapa, Janak
Morozov, Yurii V.
Sokolov, Denis A.
Hodak, Jose Hector
Vinodgopal, Kizhanipuram
Kamat, Prashant V.
Kuno, Masaru
author2_role author
author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv Graphene Oxide
Reduced Graphene Oxide
Photolysis
Reduction
Photobrightening
Fluorescence Intermittency
topic Graphene Oxide
Reduced Graphene Oxide
Photolysis
Reduction
Photobrightening
Fluorescence Intermittency
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Graphene oxide (GO) is an important precursor in the production of chemically derived graphene. During reduction, GO’s electrical conductivity and band gap change gradually. Doping and chemical functionalization are also possible, illustrating GO’s immense potential in creating functional devices through control of its local hybridization. Here we show that laser-induced photolysis controllably reduces individual single-layer GO sheets. The reaction can be followed in real time through sizable decreases in GO’s photoluminescence efficiency along with spectral blueshifts. As-produced reduced graphene oxide (rGO) sheets undergo additional photolysis, characterized by dramatic emission enhancements and spectral redshifts. Both GO’s reduction and subsequent conversion to photobrightened rGO are captured through movies of their photoluminescence kinetics. Rate maps illustrate sizable spatial and temporal heterogeneities in sp2 domain growth and reveal how reduction “flows” across GO and rGO sheets. The observed heterogeneous reduction kinetics provides mechanistic insight into GO’s conversion to chemically derived graphene and highlights opportunities for overcoming its dynamic, chemical disorder.
Fil: McDonald, Matthew P. . University Of Notre Dame-indiana; Estados Unidos
Fil: Eltom, Ahmed . University Of Waterloo; Canadá
Fil: Vietmeyer, Felix . University Of Notre Dame-indiana; Estados Unidos
Fil: Thapa, Janak . Illinois Wesleyan University; Estados Unidos
Fil: Morozov, Yurii V. . Taras Shevchenko National University of Kiev; Ucrania
Fil: Sokolov, Denis A. . University Of Notre Dame-indiana; Estados Unidos
Fil: Hodak, Jose Hector. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina. Universidad de Buenos Aires; Argentina
Fil: Vinodgopal, Kizhanipuram . North Carolina Central University; Estados Unidos
Fil: Kamat, Prashant V. . University Of Notre Dame-indiana; Estados Unidos
Fil: Kuno, Masaru . University Of Notre Dame-indiana; Estados Unidos
description Graphene oxide (GO) is an important precursor in the production of chemically derived graphene. During reduction, GO’s electrical conductivity and band gap change gradually. Doping and chemical functionalization are also possible, illustrating GO’s immense potential in creating functional devices through control of its local hybridization. Here we show that laser-induced photolysis controllably reduces individual single-layer GO sheets. The reaction can be followed in real time through sizable decreases in GO’s photoluminescence efficiency along with spectral blueshifts. As-produced reduced graphene oxide (rGO) sheets undergo additional photolysis, characterized by dramatic emission enhancements and spectral redshifts. Both GO’s reduction and subsequent conversion to photobrightened rGO are captured through movies of their photoluminescence kinetics. Rate maps illustrate sizable spatial and temporal heterogeneities in sp2 domain growth and reveal how reduction “flows” across GO and rGO sheets. The observed heterogeneous reduction kinetics provides mechanistic insight into GO’s conversion to chemically derived graphene and highlights opportunities for overcoming its dynamic, chemical disorder.
publishDate 2013
dc.date.none.fl_str_mv 2013-11
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/11336/8113
McDonald, Matthew P. ; Eltom, Ahmed ; Vietmeyer, Felix ; Thapa, Janak ; Morozov, Yurii V. ; et al.; Direct Observation of Spatially Heterogeneous Single-Layer Graphene Oxide Reduction Kinetics; American Chemical Society; Nano Letters; 13; 12; 11-2013; 5777-5784
1530-6984
url http://hdl.handle.net/11336/8113
identifier_str_mv McDonald, Matthew P. ; Eltom, Ahmed ; Vietmeyer, Felix ; Thapa, Janak ; Morozov, Yurii V. ; et al.; Direct Observation of Spatially Heterogeneous Single-Layer Graphene Oxide Reduction Kinetics; American Chemical Society; Nano Letters; 13; 12; 11-2013; 5777-5784
1530-6984
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/abs/10.1021/nl402057j
info:eu-repo/semantics/altIdentifier/doi/10.1021/nl402057j
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
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
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 12.993085

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