Proton conduction mechanisms in GPTMS/TEOS-derived organic/silica hybrid films prepared by sol-gel process
Autor(a) principal: | |
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Data de Publicação: | 2020 |
Outros Autores: | , , , |
Tipo de documento: | Artigo |
Idioma: | eng |
Título da fonte: | Repositório Institucional da UNESP |
Texto Completo: | http://dx.doi.org/10.1016/j.synthmet.2020.116448 http://hdl.handle.net/11449/201845 |
Resumo: | In this work, we employed impedance spectroscopy measurements to investigate the electrical properties of hybrid films obtained with the sol-gel process using 3-glycidoxypropyltrimethoxysilane (GPTMS) and tetraethylorthosilicate (TEOS) at different GPTMS/TEOS molar ratios and temperatures of thermal treatment. For the GPTMS/TEOS-derived samples with 1:1 composition, the DC conductivity (σdc) and charge carrier mobility (μdc) increased linearly with heat treatment temperature from 25 to 80 °C, while σdc increased from 3.2 to 22.4 nS/cm with a 7-fold increase in the GPTMS concentration. These results could be rationalized with the Miller-Abraham model using a charge carrier activation energy of 0.54 ± 0.03 eV. Using FTIR spectroscopy we demonstrated that the structural arrangement of the hybrid matrix involves epoxy ring opening, thus favoring proton conduction, which occurs as in the Grotthuss mechanism via hopping between nearest oxygen atoms of polymerized glycidoxypropyl groups. It is significant that electrical properties of organic/silica matrices can be predicted and tuned for tailored applications using the modeling presented here. |
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Proton conduction mechanisms in GPTMS/TEOS-derived organic/silica hybrid films prepared by sol-gel processConduction mechanismsEpoxy polymerizationImpedance spectroscopyOrganic/silica hybridsProton conductivitySol-gelIn this work, we employed impedance spectroscopy measurements to investigate the electrical properties of hybrid films obtained with the sol-gel process using 3-glycidoxypropyltrimethoxysilane (GPTMS) and tetraethylorthosilicate (TEOS) at different GPTMS/TEOS molar ratios and temperatures of thermal treatment. For the GPTMS/TEOS-derived samples with 1:1 composition, the DC conductivity (σdc) and charge carrier mobility (μdc) increased linearly with heat treatment temperature from 25 to 80 °C, while σdc increased from 3.2 to 22.4 nS/cm with a 7-fold increase in the GPTMS concentration. These results could be rationalized with the Miller-Abraham model using a charge carrier activation energy of 0.54 ± 0.03 eV. Using FTIR spectroscopy we demonstrated that the structural arrangement of the hybrid matrix involves epoxy ring opening, thus favoring proton conduction, which occurs as in the Grotthuss mechanism via hopping between nearest oxygen atoms of polymerized glycidoxypropyl groups. It is significant that electrical properties of organic/silica matrices can be predicted and tuned for tailored applications using the modeling presented here.Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES)Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)Department of Physics Sao Paulo State University (UNESP) Institute of Geosciences and Exact SciencesSao Carlos Institute of Physics University of Sao Paulo (USP), CP 369Department of Physics Sao Paulo State University (UNESP) Institute of Geosciences and Exact SciencesFAPESP: 2011/18149-5FAPESP: 2013/14262-7CNPq: 427220/2018-1CNPq: 444810/2014-5Universidade Estadual Paulista (Unesp)Universidade de São Paulo (USP)Monteiro, Daniela A. [UNESP]Gozzi, Giovani [UNESP]Chinaglia, Dante Luis [UNESP]Oliveira, Osvaldo N.de Vicente, Fabio S. [UNESP]2020-12-12T02:43:22Z2020-12-12T02:43:22Z2020-09-01info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/articlehttp://dx.doi.org/10.1016/j.synthmet.2020.116448Synthetic Metals, v. 267.0379-6779http://hdl.handle.net/11449/20184510.1016/j.synthmet.2020.1164482-s2.0-8508606896284082163499573780000-0001-7696-3004Scopusreponame:Repositório Institucional da UNESPinstname:Universidade Estadual Paulista (UNESP)instacron:UNESPengSynthetic Metalsinfo:eu-repo/semantics/openAccess2021-10-23T00:57:31Zoai:repositorio.unesp.br:11449/201845Repositório InstitucionalPUBhttp://repositorio.unesp.br/oai/requestopendoar:29462024-08-05T23:03:53.078162Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP)false |
dc.title.none.fl_str_mv |
Proton conduction mechanisms in GPTMS/TEOS-derived organic/silica hybrid films prepared by sol-gel process |
title |
Proton conduction mechanisms in GPTMS/TEOS-derived organic/silica hybrid films prepared by sol-gel process |
spellingShingle |
Proton conduction mechanisms in GPTMS/TEOS-derived organic/silica hybrid films prepared by sol-gel process Monteiro, Daniela A. [UNESP] Conduction mechanisms Epoxy polymerization Impedance spectroscopy Organic/silica hybrids Proton conductivity Sol-gel |
title_short |
Proton conduction mechanisms in GPTMS/TEOS-derived organic/silica hybrid films prepared by sol-gel process |
title_full |
Proton conduction mechanisms in GPTMS/TEOS-derived organic/silica hybrid films prepared by sol-gel process |
title_fullStr |
Proton conduction mechanisms in GPTMS/TEOS-derived organic/silica hybrid films prepared by sol-gel process |
title_full_unstemmed |
Proton conduction mechanisms in GPTMS/TEOS-derived organic/silica hybrid films prepared by sol-gel process |
title_sort |
Proton conduction mechanisms in GPTMS/TEOS-derived organic/silica hybrid films prepared by sol-gel process |
author |
Monteiro, Daniela A. [UNESP] |
author_facet |
Monteiro, Daniela A. [UNESP] Gozzi, Giovani [UNESP] Chinaglia, Dante Luis [UNESP] Oliveira, Osvaldo N. de Vicente, Fabio S. [UNESP] |
author_role |
author |
author2 |
Gozzi, Giovani [UNESP] Chinaglia, Dante Luis [UNESP] Oliveira, Osvaldo N. de Vicente, Fabio S. [UNESP] |
author2_role |
author author author author |
dc.contributor.none.fl_str_mv |
Universidade Estadual Paulista (Unesp) Universidade de São Paulo (USP) |
dc.contributor.author.fl_str_mv |
Monteiro, Daniela A. [UNESP] Gozzi, Giovani [UNESP] Chinaglia, Dante Luis [UNESP] Oliveira, Osvaldo N. de Vicente, Fabio S. [UNESP] |
dc.subject.por.fl_str_mv |
Conduction mechanisms Epoxy polymerization Impedance spectroscopy Organic/silica hybrids Proton conductivity Sol-gel |
topic |
Conduction mechanisms Epoxy polymerization Impedance spectroscopy Organic/silica hybrids Proton conductivity Sol-gel |
description |
In this work, we employed impedance spectroscopy measurements to investigate the electrical properties of hybrid films obtained with the sol-gel process using 3-glycidoxypropyltrimethoxysilane (GPTMS) and tetraethylorthosilicate (TEOS) at different GPTMS/TEOS molar ratios and temperatures of thermal treatment. For the GPTMS/TEOS-derived samples with 1:1 composition, the DC conductivity (σdc) and charge carrier mobility (μdc) increased linearly with heat treatment temperature from 25 to 80 °C, while σdc increased from 3.2 to 22.4 nS/cm with a 7-fold increase in the GPTMS concentration. These results could be rationalized with the Miller-Abraham model using a charge carrier activation energy of 0.54 ± 0.03 eV. Using FTIR spectroscopy we demonstrated that the structural arrangement of the hybrid matrix involves epoxy ring opening, thus favoring proton conduction, which occurs as in the Grotthuss mechanism via hopping between nearest oxygen atoms of polymerized glycidoxypropyl groups. It is significant that electrical properties of organic/silica matrices can be predicted and tuned for tailored applications using the modeling presented here. |
publishDate |
2020 |
dc.date.none.fl_str_mv |
2020-12-12T02:43:22Z 2020-12-12T02:43:22Z 2020-09-01 |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/article |
format |
article |
status_str |
publishedVersion |
dc.identifier.uri.fl_str_mv |
http://dx.doi.org/10.1016/j.synthmet.2020.116448 Synthetic Metals, v. 267. 0379-6779 http://hdl.handle.net/11449/201845 10.1016/j.synthmet.2020.116448 2-s2.0-85086068962 8408216349957378 0000-0001-7696-3004 |
url |
http://dx.doi.org/10.1016/j.synthmet.2020.116448 http://hdl.handle.net/11449/201845 |
identifier_str_mv |
Synthetic Metals, v. 267. 0379-6779 10.1016/j.synthmet.2020.116448 2-s2.0-85086068962 8408216349957378 0000-0001-7696-3004 |
dc.language.iso.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
Synthetic Metals |
dc.rights.driver.fl_str_mv |
info:eu-repo/semantics/openAccess |
eu_rights_str_mv |
openAccess |
dc.source.none.fl_str_mv |
Scopus reponame:Repositório Institucional da UNESP instname:Universidade Estadual Paulista (UNESP) instacron:UNESP |
instname_str |
Universidade Estadual Paulista (UNESP) |
instacron_str |
UNESP |
institution |
UNESP |
reponame_str |
Repositório Institucional da UNESP |
collection |
Repositório Institucional da UNESP |
repository.name.fl_str_mv |
Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP) |
repository.mail.fl_str_mv |
|
_version_ |
1808129486016741376 |