Progress of the Catalytic Deactivation of H-ZSM-5 Zeolite in Glycerol Dehydration

Detalhes bibliográficos
Autor(a) principal: Catuzo, Gabriel L. [UNESP]
Data de Publicação: 2021
Outros Autores: Possato, Luiz G. [UNESP], Sad, María Eugenia, Padró, Cristina, Martins, Leandro [UNESP]
Tipo de documento: Artigo
Idioma: eng
Título da fonte: Repositório Institucional da UNESP
Texto Completo: http://dx.doi.org/10.1002/cctc.202100576
http://hdl.handle.net/11449/222256
Resumo: Glycerol conversion into value-added chemicals has received much attention due to the prospect of increasing the biodiesel industry‘s profitability. The dehydration of glycerol is one of the most explored reactions in the valorization of glycerol, and the zeolite H-ZSM-5 is one of the furthermost used structures. In this study, several characterization techniques were used to investigate the detailed aging of coke in spent H-ZSM-5 zeolites after their use in the gas-phase glycerol dehydration to produce acrolein. The carbonaceous deposits formed almost totally in the first minutes of the reaction. They rapidly got trapped inside the pores, hampering the accessibility to active sites and the zeolite‘s full catalytic action. Two types of coke were formed during the reaction: polyglycols, on the external surface, and aromatics, inside the pores, representing the majority (∼98 wt.%) of the carbonaceous compounds. Besides, aromatic compounds age over time, becoming bulkier and more deficient in hydrogen. We also found a correlation between the amount of coke, its size, accessibility to the acid active sites, and changes in crystallographic parameters of the zeolite with the presence of coke.
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spelling Progress of the Catalytic Deactivation of H-ZSM-5 Zeolite in Glycerol DehydrationAcid catalysisCokeDeactivationDehydrationGlycerolZSM-5 zeoliteGlycerol conversion into value-added chemicals has received much attention due to the prospect of increasing the biodiesel industry‘s profitability. The dehydration of glycerol is one of the most explored reactions in the valorization of glycerol, and the zeolite H-ZSM-5 is one of the furthermost used structures. In this study, several characterization techniques were used to investigate the detailed aging of coke in spent H-ZSM-5 zeolites after their use in the gas-phase glycerol dehydration to produce acrolein. The carbonaceous deposits formed almost totally in the first minutes of the reaction. They rapidly got trapped inside the pores, hampering the accessibility to active sites and the zeolite‘s full catalytic action. Two types of coke were formed during the reaction: polyglycols, on the external surface, and aromatics, inside the pores, representing the majority (∼98 wt.%) of the carbonaceous compounds. Besides, aromatic compounds age over time, becoming bulkier and more deficient in hydrogen. We also found a correlation between the amount of coke, its size, accessibility to the acid active sites, and changes in crystallographic parameters of the zeolite with the presence of coke.Instituto de Química UNESP – Universidade Estadual Paulista, Prof. Francisco Degni 55Facultad de Ingeniería Química UNL – Universidad Nacional del Litoral, Santiago del Estero 2829Instituto de Química UNESP – Universidade Estadual Paulista, Prof. Francisco Degni 55Universidade Estadual Paulista (UNESP)UNL – Universidad Nacional del LitoralCatuzo, Gabriel L. [UNESP]Possato, Luiz G. [UNESP]Sad, María EugeniaPadró, CristinaMartins, Leandro [UNESP]2022-04-28T19:43:36Z2022-04-28T19:43:36Z2021-01-01info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/articlehttp://dx.doi.org/10.1002/cctc.202100576ChemCatChem.1867-38991867-3880http://hdl.handle.net/11449/22225610.1002/cctc.2021005762-s2.0-85113290106Scopusreponame:Repositório Institucional da UNESPinstname:Universidade Estadual Paulista (UNESP)instacron:UNESPengChemCatCheminfo:eu-repo/semantics/openAccess2022-04-28T19:43:36Zoai:repositorio.unesp.br:11449/222256Repositório InstitucionalPUBhttp://repositorio.unesp.br/oai/requestopendoar:29462024-08-05T17:47:46.847639Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP)false
dc.title.none.fl_str_mv Progress of the Catalytic Deactivation of H-ZSM-5 Zeolite in Glycerol Dehydration
title Progress of the Catalytic Deactivation of H-ZSM-5 Zeolite in Glycerol Dehydration
spellingShingle Progress of the Catalytic Deactivation of H-ZSM-5 Zeolite in Glycerol Dehydration
Catuzo, Gabriel L. [UNESP]
Acid catalysis
Coke
Deactivation
Dehydration
Glycerol
ZSM-5 zeolite
title_short Progress of the Catalytic Deactivation of H-ZSM-5 Zeolite in Glycerol Dehydration
title_full Progress of the Catalytic Deactivation of H-ZSM-5 Zeolite in Glycerol Dehydration
title_fullStr Progress of the Catalytic Deactivation of H-ZSM-5 Zeolite in Glycerol Dehydration
title_full_unstemmed Progress of the Catalytic Deactivation of H-ZSM-5 Zeolite in Glycerol Dehydration
title_sort Progress of the Catalytic Deactivation of H-ZSM-5 Zeolite in Glycerol Dehydration
author Catuzo, Gabriel L. [UNESP]
author_facet Catuzo, Gabriel L. [UNESP]
Possato, Luiz G. [UNESP]
Sad, María Eugenia
Padró, Cristina
Martins, Leandro [UNESP]
author_role author
author2 Possato, Luiz G. [UNESP]
Sad, María Eugenia
Padró, Cristina
Martins, Leandro [UNESP]
author2_role author
author
author
author
dc.contributor.none.fl_str_mv Universidade Estadual Paulista (UNESP)
UNL – Universidad Nacional del Litoral
dc.contributor.author.fl_str_mv Catuzo, Gabriel L. [UNESP]
Possato, Luiz G. [UNESP]
Sad, María Eugenia
Padró, Cristina
Martins, Leandro [UNESP]
dc.subject.por.fl_str_mv Acid catalysis
Coke
Deactivation
Dehydration
Glycerol
ZSM-5 zeolite
topic Acid catalysis
Coke
Deactivation
Dehydration
Glycerol
ZSM-5 zeolite
description Glycerol conversion into value-added chemicals has received much attention due to the prospect of increasing the biodiesel industry‘s profitability. The dehydration of glycerol is one of the most explored reactions in the valorization of glycerol, and the zeolite H-ZSM-5 is one of the furthermost used structures. In this study, several characterization techniques were used to investigate the detailed aging of coke in spent H-ZSM-5 zeolites after their use in the gas-phase glycerol dehydration to produce acrolein. The carbonaceous deposits formed almost totally in the first minutes of the reaction. They rapidly got trapped inside the pores, hampering the accessibility to active sites and the zeolite‘s full catalytic action. Two types of coke were formed during the reaction: polyglycols, on the external surface, and aromatics, inside the pores, representing the majority (∼98 wt.%) of the carbonaceous compounds. Besides, aromatic compounds age over time, becoming bulkier and more deficient in hydrogen. We also found a correlation between the amount of coke, its size, accessibility to the acid active sites, and changes in crystallographic parameters of the zeolite with the presence of coke.
publishDate 2021
dc.date.none.fl_str_mv 2021-01-01
2022-04-28T19:43:36Z
2022-04-28T19:43:36Z
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/10.1002/cctc.202100576
ChemCatChem.
1867-3899
1867-3880
http://hdl.handle.net/11449/222256
10.1002/cctc.202100576
2-s2.0-85113290106
url http://dx.doi.org/10.1002/cctc.202100576
http://hdl.handle.net/11449/222256
identifier_str_mv ChemCatChem.
1867-3899
1867-3880
10.1002/cctc.202100576
2-s2.0-85113290106
dc.language.iso.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv ChemCatChem
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
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