Understanding the Microstructure Connectivity in Photopolymerizable Aluminum-Phosphate-Silicate Sol-Gel Hybrid Materials for Additive Manufacturing

Detalhes bibliográficos
Autor(a) principal: Tayama, Gabriel Toshiaki [UNESP]
Data de Publicação: 2023
Outros Autores: Santagneli, Silvia Helena [UNESP], de Oliveira Junior, Marcos, Messaddeq, Younes [UNESP]
Tipo de documento: Artigo
Idioma: eng
Título da fonte: Repositório Institucional da UNESP
Texto Completo: http://dx.doi.org/10.1021/acs.jpcc.2c08027
http://hdl.handle.net/11449/249627
Resumo: In this paper, we report the synthesis and structural characterization of transparent and photopolymerizable aluminum-phosphate-silicate hybrid materials obtained via the sol-gel route, with different aluminum/phosphate (Al/P) ratios. We explored the system Si(1-x)-(Al/P) (x) with x varying from 0.3 to 1, and atomic ratios of Al/P are 1:3, 1:1, and 3:1. All compositions contain high inorganic mass content (up to 40 wt %). Furthermore, they are compatible with vat-photopolymerization platforms. The structural evolution of the hybrid materials with the silicon concentration was investigated by SEM, phase-contrast AFM, and solid-state NMR techniques, using single- and double-resonance experiments. The structure follows the build-up principle using aluminum-phosphate species and alkoxysilane chains as fundamental building blocks. These aluminum-phosphate species were identified as monomeric and dimeric chain structures by comparing different parameters obtained from NMR data to compound models. Monomeric and dimeric aluminum-phosphate chain structures were predominant in 3:1 and 1:3 Al/P ratio samples, respectively, promoting and hindering the heterocondensation with the alkoxysilane precursor, respectively. The photopolymerization mechanism leads to the percolation of the inorganic networks through a parallel polymethylmethacrylate network, resulting in a material with structural heterogeneities in the range of 5 nm, evidenced by phase-contrast AFM.
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spelling Understanding the Microstructure Connectivity in Photopolymerizable Aluminum-Phosphate-Silicate Sol-Gel Hybrid Materials for Additive ManufacturingIn this paper, we report the synthesis and structural characterization of transparent and photopolymerizable aluminum-phosphate-silicate hybrid materials obtained via the sol-gel route, with different aluminum/phosphate (Al/P) ratios. We explored the system Si(1-x)-(Al/P) (x) with x varying from 0.3 to 1, and atomic ratios of Al/P are 1:3, 1:1, and 3:1. All compositions contain high inorganic mass content (up to 40 wt %). Furthermore, they are compatible with vat-photopolymerization platforms. The structural evolution of the hybrid materials with the silicon concentration was investigated by SEM, phase-contrast AFM, and solid-state NMR techniques, using single- and double-resonance experiments. The structure follows the build-up principle using aluminum-phosphate species and alkoxysilane chains as fundamental building blocks. These aluminum-phosphate species were identified as monomeric and dimeric chain structures by comparing different parameters obtained from NMR data to compound models. Monomeric and dimeric aluminum-phosphate chain structures were predominant in 3:1 and 1:3 Al/P ratio samples, respectively, promoting and hindering the heterocondensation with the alkoxysilane precursor, respectively. The photopolymerization mechanism leads to the percolation of the inorganic networks through a parallel polymethylmethacrylate network, resulting in a material with structural heterogeneities in the range of 5 nm, evidenced by phase-contrast AFM.Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)Natural Sciences and Engineering Research Council of CanadaThe Research CouncilChemistry Institute São Paulo State University─UNESP, Rua Francisco Degni 55, AraraquaraCentre de Optique Photonique et Laser─COPL─Universite Laval, 2375 rue de la TerraseSão Carlos Institute of Physics University of São Paulo, São CarlosChemistry Institute São Paulo State University─UNESP, Rua Francisco Degni 55, AraraquaraUniversidade Estadual Paulista (UNESP)Photonique et Laser─COPL─Universite LavalUniversidade de São Paulo (USP)Tayama, Gabriel Toshiaki [UNESP]Santagneli, Silvia Helena [UNESP]de Oliveira Junior, MarcosMessaddeq, Younes [UNESP]2023-07-29T16:04:51Z2023-07-29T16:04:51Z2023-02-09info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/article2416-2429http://dx.doi.org/10.1021/acs.jpcc.2c08027Journal of Physical Chemistry C, v. 127, n. 5, p. 2416-2429, 2023.1932-74551932-7447http://hdl.handle.net/11449/24962710.1021/acs.jpcc.2c080272-s2.0-85147262232Scopusreponame:Repositório Institucional da UNESPinstname:Universidade Estadual Paulista (UNESP)instacron:UNESPengJournal of Physical Chemistry Cinfo:eu-repo/semantics/openAccess2023-07-29T16:04:51Zoai:repositorio.unesp.br:11449/249627Repositório InstitucionalPUBhttp://repositorio.unesp.br/oai/requestopendoar:29462024-08-05T17:24:49.300995Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP)false
dc.title.none.fl_str_mv Understanding the Microstructure Connectivity in Photopolymerizable Aluminum-Phosphate-Silicate Sol-Gel Hybrid Materials for Additive Manufacturing
title Understanding the Microstructure Connectivity in Photopolymerizable Aluminum-Phosphate-Silicate Sol-Gel Hybrid Materials for Additive Manufacturing
spellingShingle Understanding the Microstructure Connectivity in Photopolymerizable Aluminum-Phosphate-Silicate Sol-Gel Hybrid Materials for Additive Manufacturing
Tayama, Gabriel Toshiaki [UNESP]
title_short Understanding the Microstructure Connectivity in Photopolymerizable Aluminum-Phosphate-Silicate Sol-Gel Hybrid Materials for Additive Manufacturing
title_full Understanding the Microstructure Connectivity in Photopolymerizable Aluminum-Phosphate-Silicate Sol-Gel Hybrid Materials for Additive Manufacturing
title_fullStr Understanding the Microstructure Connectivity in Photopolymerizable Aluminum-Phosphate-Silicate Sol-Gel Hybrid Materials for Additive Manufacturing
title_full_unstemmed Understanding the Microstructure Connectivity in Photopolymerizable Aluminum-Phosphate-Silicate Sol-Gel Hybrid Materials for Additive Manufacturing
title_sort Understanding the Microstructure Connectivity in Photopolymerizable Aluminum-Phosphate-Silicate Sol-Gel Hybrid Materials for Additive Manufacturing
author Tayama, Gabriel Toshiaki [UNESP]
author_facet Tayama, Gabriel Toshiaki [UNESP]
Santagneli, Silvia Helena [UNESP]
de Oliveira Junior, Marcos
Messaddeq, Younes [UNESP]
author_role author
author2 Santagneli, Silvia Helena [UNESP]
de Oliveira Junior, Marcos
Messaddeq, Younes [UNESP]
author2_role author
author
author
dc.contributor.none.fl_str_mv Universidade Estadual Paulista (UNESP)
Photonique et Laser─COPL─Universite Laval
Universidade de São Paulo (USP)
dc.contributor.author.fl_str_mv Tayama, Gabriel Toshiaki [UNESP]
Santagneli, Silvia Helena [UNESP]
de Oliveira Junior, Marcos
Messaddeq, Younes [UNESP]
description In this paper, we report the synthesis and structural characterization of transparent and photopolymerizable aluminum-phosphate-silicate hybrid materials obtained via the sol-gel route, with different aluminum/phosphate (Al/P) ratios. We explored the system Si(1-x)-(Al/P) (x) with x varying from 0.3 to 1, and atomic ratios of Al/P are 1:3, 1:1, and 3:1. All compositions contain high inorganic mass content (up to 40 wt %). Furthermore, they are compatible with vat-photopolymerization platforms. The structural evolution of the hybrid materials with the silicon concentration was investigated by SEM, phase-contrast AFM, and solid-state NMR techniques, using single- and double-resonance experiments. The structure follows the build-up principle using aluminum-phosphate species and alkoxysilane chains as fundamental building blocks. These aluminum-phosphate species were identified as monomeric and dimeric chain structures by comparing different parameters obtained from NMR data to compound models. Monomeric and dimeric aluminum-phosphate chain structures were predominant in 3:1 and 1:3 Al/P ratio samples, respectively, promoting and hindering the heterocondensation with the alkoxysilane precursor, respectively. The photopolymerization mechanism leads to the percolation of the inorganic networks through a parallel polymethylmethacrylate network, resulting in a material with structural heterogeneities in the range of 5 nm, evidenced by phase-contrast AFM.
publishDate 2023
dc.date.none.fl_str_mv 2023-07-29T16:04:51Z
2023-07-29T16:04:51Z
2023-02-09
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/10.1021/acs.jpcc.2c08027
Journal of Physical Chemistry C, v. 127, n. 5, p. 2416-2429, 2023.
1932-7455
1932-7447
http://hdl.handle.net/11449/249627
10.1021/acs.jpcc.2c08027
2-s2.0-85147262232
url http://dx.doi.org/10.1021/acs.jpcc.2c08027
http://hdl.handle.net/11449/249627
identifier_str_mv Journal of Physical Chemistry C, v. 127, n. 5, p. 2416-2429, 2023.
1932-7455
1932-7447
10.1021/acs.jpcc.2c08027
2-s2.0-85147262232
dc.language.iso.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv Journal of Physical Chemistry C
dc.rights.driver.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv 2416-2429
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
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