Understanding the Microstructure Connectivity in Photopolymerizable Aluminum-Phosphate-Silicate Sol-Gel Hybrid Materials for Additive Manufacturing
Autor(a) principal: | |
---|---|
Data de Publicação: | 2023 |
Outros Autores: | , , |
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. |
id |
UNSP_d179ba9fac86eac38e547fb10ea2e642 |
---|---|
oai_identifier_str |
oai:repositorio.unesp.br:11449/249627 |
network_acronym_str |
UNSP |
network_name_str |
Repositório Institucional da UNESP |
repository_id_str |
2946 |
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 |
|
_version_ |
1808128807019741184 |