Acidic V-MCM-41 catalysts for the liquid-phase ketalization of glycerol with acetone
Autor(a) principal: | |
---|---|
Data de Publicação: | 2019 |
Outros Autores: | , , |
Tipo de documento: | Artigo |
Idioma: | eng |
Título da fonte: | Repositório Institucional da UNESP |
Texto Completo: | http://dx.doi.org/10.1016/j.micromeso.2018.07.006 http://hdl.handle.net/11449/186872 |
Resumo: | SiMCM-41 and V-MCM-41 were hydrothermally synthesized with different quantities of vanadium, characterized by small angle X-ray scattering, nitrogen physisorption, and the insertion of vanadium was assessed by temperature-programed desorption of ammonia, pyridine chemisorption followed by infrared spectroscopy and H2 temperature-programed reduction. Vanadium-based materials are notable oxidation catalysts, however acid sites can be developed, making them potential bifunctional catalysts combining redox and Lewis acid sites. Herein, mesoporous vanadosilicates were used as acidic catalysts in the Ketalization of glycerol with acetone for solketal formation. The catalytic activity was dependent on the amount of acid sites, based on three types of vanadium oxide species: (i) isolated or (ii) oligomeric vanadium species inserted in the silica framework, i.e. -Si-O-(V-O-V)n, where n = 1 and n > 1, respectively, and (iii) surface vanadium oxides highly dispersed or interacting with surface hydroxyl groups. By performing recycling experiments it was possible to conclude that the surface vanadium oxides species, despite of being more active, are leached by water molecules formed in the course of the reaction, decreasing the activity. On the other hand, framework vanadium are more stable Lewis acid sites for liquid-phase Ketalization reaction. |
id |
UNSP_5ccbd7396c4840bc403d40daa934ff33 |
---|---|
oai_identifier_str |
oai:repositorio.unesp.br:11449/186872 |
network_acronym_str |
UNSP |
network_name_str |
Repositório Institucional da UNESP |
repository_id_str |
2946 |
spelling |
Acidic V-MCM-41 catalysts for the liquid-phase ketalization of glycerol with acetoneGlycerol condensationMCM-41SolketalVanadosilicatesSiMCM-41 and V-MCM-41 were hydrothermally synthesized with different quantities of vanadium, characterized by small angle X-ray scattering, nitrogen physisorption, and the insertion of vanadium was assessed by temperature-programed desorption of ammonia, pyridine chemisorption followed by infrared spectroscopy and H2 temperature-programed reduction. Vanadium-based materials are notable oxidation catalysts, however acid sites can be developed, making them potential bifunctional catalysts combining redox and Lewis acid sites. Herein, mesoporous vanadosilicates were used as acidic catalysts in the Ketalization of glycerol with acetone for solketal formation. The catalytic activity was dependent on the amount of acid sites, based on three types of vanadium oxide species: (i) isolated or (ii) oligomeric vanadium species inserted in the silica framework, i.e. -Si-O-(V-O-V)n, where n = 1 and n > 1, respectively, and (iii) surface vanadium oxides highly dispersed or interacting with surface hydroxyl groups. By performing recycling experiments it was possible to conclude that the surface vanadium oxides species, despite of being more active, are leached by water molecules formed in the course of the reaction, decreasing the activity. On the other hand, framework vanadium are more stable Lewis acid sites for liquid-phase Ketalization reaction.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)Instituto de Química Universidade Estadual Paulista - Unesp, Rua Prof. Francisco Degni 55GICIC (Grupo de Investigaciones en Ciencia y Ingenieria Cataliticas) INCAPE-UNL-CONICET, Colectora Ruta Nac. 168Instituto de Química Universidade Estadual Paulista - Unesp, Rua Prof. Francisco Degni 55FAPESP: #2013/10204-2FAPESP: #2016/10597-2CNPq: #304698/2014-8Universidade Estadual Paulista (Unesp)GICIC (Grupo de Investigaciones en Ciencia y Ingenieria Cataliticas) INCAPE-UNL-CONICETAbreu, Thiago H. [UNESP]Meyer, Camilo I.Padró, CristinaMartins, Leandro [UNESP]2019-10-06T15:18:20Z2019-10-06T15:18:20Z2019-01-01info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/article219-225http://dx.doi.org/10.1016/j.micromeso.2018.07.006Microporous and Mesoporous Materials, v. 273, p. 219-225.1387-1811http://hdl.handle.net/11449/18687210.1016/j.micromeso.2018.07.0062-s2.0-85049635499Scopusreponame:Repositório Institucional da UNESPinstname:Universidade Estadual Paulista (UNESP)instacron:UNESPengMicroporous and Mesoporous Materialsinfo:eu-repo/semantics/openAccess2021-10-23T20:19:25Zoai:repositorio.unesp.br:11449/186872Repositório InstitucionalPUBhttp://repositorio.unesp.br/oai/requestopendoar:29462024-08-05T23:26:47.354927Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP)false |
dc.title.none.fl_str_mv |
Acidic V-MCM-41 catalysts for the liquid-phase ketalization of glycerol with acetone |
title |
Acidic V-MCM-41 catalysts for the liquid-phase ketalization of glycerol with acetone |
spellingShingle |
Acidic V-MCM-41 catalysts for the liquid-phase ketalization of glycerol with acetone Abreu, Thiago H. [UNESP] Glycerol condensation MCM-41 Solketal Vanadosilicates |
title_short |
Acidic V-MCM-41 catalysts for the liquid-phase ketalization of glycerol with acetone |
title_full |
Acidic V-MCM-41 catalysts for the liquid-phase ketalization of glycerol with acetone |
title_fullStr |
Acidic V-MCM-41 catalysts for the liquid-phase ketalization of glycerol with acetone |
title_full_unstemmed |
Acidic V-MCM-41 catalysts for the liquid-phase ketalization of glycerol with acetone |
title_sort |
Acidic V-MCM-41 catalysts for the liquid-phase ketalization of glycerol with acetone |
author |
Abreu, Thiago H. [UNESP] |
author_facet |
Abreu, Thiago H. [UNESP] Meyer, Camilo I. Padró, Cristina Martins, Leandro [UNESP] |
author_role |
author |
author2 |
Meyer, Camilo I. Padró, Cristina Martins, Leandro [UNESP] |
author2_role |
author author author |
dc.contributor.none.fl_str_mv |
Universidade Estadual Paulista (Unesp) GICIC (Grupo de Investigaciones en Ciencia y Ingenieria Cataliticas) INCAPE-UNL-CONICET |
dc.contributor.author.fl_str_mv |
Abreu, Thiago H. [UNESP] Meyer, Camilo I. Padró, Cristina Martins, Leandro [UNESP] |
dc.subject.por.fl_str_mv |
Glycerol condensation MCM-41 Solketal Vanadosilicates |
topic |
Glycerol condensation MCM-41 Solketal Vanadosilicates |
description |
SiMCM-41 and V-MCM-41 were hydrothermally synthesized with different quantities of vanadium, characterized by small angle X-ray scattering, nitrogen physisorption, and the insertion of vanadium was assessed by temperature-programed desorption of ammonia, pyridine chemisorption followed by infrared spectroscopy and H2 temperature-programed reduction. Vanadium-based materials are notable oxidation catalysts, however acid sites can be developed, making them potential bifunctional catalysts combining redox and Lewis acid sites. Herein, mesoporous vanadosilicates were used as acidic catalysts in the Ketalization of glycerol with acetone for solketal formation. The catalytic activity was dependent on the amount of acid sites, based on three types of vanadium oxide species: (i) isolated or (ii) oligomeric vanadium species inserted in the silica framework, i.e. -Si-O-(V-O-V)n, where n = 1 and n > 1, respectively, and (iii) surface vanadium oxides highly dispersed or interacting with surface hydroxyl groups. By performing recycling experiments it was possible to conclude that the surface vanadium oxides species, despite of being more active, are leached by water molecules formed in the course of the reaction, decreasing the activity. On the other hand, framework vanadium are more stable Lewis acid sites for liquid-phase Ketalization reaction. |
publishDate |
2019 |
dc.date.none.fl_str_mv |
2019-10-06T15:18:20Z 2019-10-06T15:18:20Z 2019-01-01 |
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.micromeso.2018.07.006 Microporous and Mesoporous Materials, v. 273, p. 219-225. 1387-1811 http://hdl.handle.net/11449/186872 10.1016/j.micromeso.2018.07.006 2-s2.0-85049635499 |
url |
http://dx.doi.org/10.1016/j.micromeso.2018.07.006 http://hdl.handle.net/11449/186872 |
identifier_str_mv |
Microporous and Mesoporous Materials, v. 273, p. 219-225. 1387-1811 10.1016/j.micromeso.2018.07.006 2-s2.0-85049635499 |
dc.language.iso.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
Microporous and Mesoporous Materials |
dc.rights.driver.fl_str_mv |
info:eu-repo/semantics/openAccess |
eu_rights_str_mv |
openAccess |
dc.format.none.fl_str_mv |
219-225 |
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_ |
1808129521884332032 |