Adsorption and dynamics of linear and mono-branched hexane isomers in MIL-140 metal-organic frameworks
Autor(a) principal: | |
---|---|
Data de Publicação: | 2019 |
Outros Autores: | , , , , , |
Tipo de documento: | Artigo |
Idioma: | eng |
Título da fonte: | Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
Texto Completo: | http://hdl.handle.net/10198/19892 |
Resumo: | Recent breakthrough experiments revealed the iso-reticular Zr-MOFs, MIL-140B and MIL-140C, as promising sorbents for the separation of C6 isomers. Interestingly while the ultra-small pore MIL-140B exhibited hexane isomer sorption hierarchy according to the normal boiling point order (n-C6 > 3MP (3-methyl pentane)), an uncommon shift in the elution order was observed in the larger pore MIL-140C. It was only speculated that the flexibility of the MOFs might be the origin of this intriguing behavior. Herein, flexible force field hybrid osmotic Monte Carlo combined with molecular dynamics simulations were carried out to unravel the microscopic mechanism of the adsorption and dynamics of both C6 isomers in MIL140B and MIL140C. Thermodynamically preferred adsorption of n-C6 over 3MP was predicted for MIL-140B and to a slightly less extent for MIL-140C. Interestingly while the mobility of n-C6 was found to remain higher than that of 3MP in the whole range of loading for MIL-140B, 3MP becomes more mobile than n-C6 at saturation in MIL-140C. This suggests that this kinetics order is most probably the origin of the inversion of the elution order observed experimentally for MIL-140C. The translational and rotational dynamics of the two guests in MIL-140B and MIL-140C was further understood in-depth. |
id |
RCAP_5fd23258f41cfae369842c2830af8c3d |
---|---|
oai_identifier_str |
oai:bibliotecadigital.ipb.pt:10198/19892 |
network_acronym_str |
RCAP |
network_name_str |
Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
repository_id_str |
7160 |
spelling |
Adsorption and dynamics of linear and mono-branched hexane isomers in MIL-140 metal-organic frameworksForce-fieldSeparationSimulationsDiffusionMixturesRecent breakthrough experiments revealed the iso-reticular Zr-MOFs, MIL-140B and MIL-140C, as promising sorbents for the separation of C6 isomers. Interestingly while the ultra-small pore MIL-140B exhibited hexane isomer sorption hierarchy according to the normal boiling point order (n-C6 > 3MP (3-methyl pentane)), an uncommon shift in the elution order was observed in the larger pore MIL-140C. It was only speculated that the flexibility of the MOFs might be the origin of this intriguing behavior. Herein, flexible force field hybrid osmotic Monte Carlo combined with molecular dynamics simulations were carried out to unravel the microscopic mechanism of the adsorption and dynamics of both C6 isomers in MIL140B and MIL140C. Thermodynamically preferred adsorption of n-C6 over 3MP was predicted for MIL-140B and to a slightly less extent for MIL-140C. Interestingly while the mobility of n-C6 was found to remain higher than that of 3MP in the whole range of loading for MIL-140B, 3MP becomes more mobile than n-C6 at saturation in MIL-140C. This suggests that this kinetics order is most probably the origin of the inversion of the elution order observed experimentally for MIL-140C. The translational and rotational dynamics of the two guests in MIL-140B and MIL-140C was further understood in-depth.The Royal Society of ChemistryBiblioteca Digital do IPBZhao, HengliSilva, José A.C.Henrique, AdrianoNouar, FaridSerre, ChristianMaurin, GuillaumeGhoufi, Aziz2019-12-06T10:23:38Z20232023-01-01T00:00:00Zinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10198/19892engZhao, Hengli; Silva, José A.C.; Henrique, Adriano; Nouar, Farid; Serre, Christian; Maurin, Guillaume; Ghoufi, Aziz (2023). Adsorption and dynamics of linear and mono-branched hexane isomers in MIL-140 metal-organic frameworks. Physical Chemistry Chemical Physics. eISSN 1463-9084. 25:17, p. 12057-120641463-907610.1039/d2cp05371c1463-9084info:eu-repo/semantics/openAccessreponame:Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)instname:Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãoinstacron:RCAAP2023-11-21T10:45:24Zoai:bibliotecadigital.ipb.pt:10198/19892Portal AgregadorONGhttps://www.rcaap.pt/oai/openaireopendoar:71602024-03-19T23:10:33.642098Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãofalse |
dc.title.none.fl_str_mv |
Adsorption and dynamics of linear and mono-branched hexane isomers in MIL-140 metal-organic frameworks |
title |
Adsorption and dynamics of linear and mono-branched hexane isomers in MIL-140 metal-organic frameworks |
spellingShingle |
Adsorption and dynamics of linear and mono-branched hexane isomers in MIL-140 metal-organic frameworks Zhao, Hengli Force-field Separation Simulations Diffusion Mixtures |
title_short |
Adsorption and dynamics of linear and mono-branched hexane isomers in MIL-140 metal-organic frameworks |
title_full |
Adsorption and dynamics of linear and mono-branched hexane isomers in MIL-140 metal-organic frameworks |
title_fullStr |
Adsorption and dynamics of linear and mono-branched hexane isomers in MIL-140 metal-organic frameworks |
title_full_unstemmed |
Adsorption and dynamics of linear and mono-branched hexane isomers in MIL-140 metal-organic frameworks |
title_sort |
Adsorption and dynamics of linear and mono-branched hexane isomers in MIL-140 metal-organic frameworks |
author |
Zhao, Hengli |
author_facet |
Zhao, Hengli Silva, José A.C. Henrique, Adriano Nouar, Farid Serre, Christian Maurin, Guillaume Ghoufi, Aziz |
author_role |
author |
author2 |
Silva, José A.C. Henrique, Adriano Nouar, Farid Serre, Christian Maurin, Guillaume Ghoufi, Aziz |
author2_role |
author author author author author author |
dc.contributor.none.fl_str_mv |
Biblioteca Digital do IPB |
dc.contributor.author.fl_str_mv |
Zhao, Hengli Silva, José A.C. Henrique, Adriano Nouar, Farid Serre, Christian Maurin, Guillaume Ghoufi, Aziz |
dc.subject.por.fl_str_mv |
Force-field Separation Simulations Diffusion Mixtures |
topic |
Force-field Separation Simulations Diffusion Mixtures |
description |
Recent breakthrough experiments revealed the iso-reticular Zr-MOFs, MIL-140B and MIL-140C, as promising sorbents for the separation of C6 isomers. Interestingly while the ultra-small pore MIL-140B exhibited hexane isomer sorption hierarchy according to the normal boiling point order (n-C6 > 3MP (3-methyl pentane)), an uncommon shift in the elution order was observed in the larger pore MIL-140C. It was only speculated that the flexibility of the MOFs might be the origin of this intriguing behavior. Herein, flexible force field hybrid osmotic Monte Carlo combined with molecular dynamics simulations were carried out to unravel the microscopic mechanism of the adsorption and dynamics of both C6 isomers in MIL140B and MIL140C. Thermodynamically preferred adsorption of n-C6 over 3MP was predicted for MIL-140B and to a slightly less extent for MIL-140C. Interestingly while the mobility of n-C6 was found to remain higher than that of 3MP in the whole range of loading for MIL-140B, 3MP becomes more mobile than n-C6 at saturation in MIL-140C. This suggests that this kinetics order is most probably the origin of the inversion of the elution order observed experimentally for MIL-140C. The translational and rotational dynamics of the two guests in MIL-140B and MIL-140C was further understood in-depth. |
publishDate |
2019 |
dc.date.none.fl_str_mv |
2019-12-06T10:23:38Z 2023 2023-01-01T00:00:00Z |
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://hdl.handle.net/10198/19892 |
url |
http://hdl.handle.net/10198/19892 |
dc.language.iso.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
Zhao, Hengli; Silva, José A.C.; Henrique, Adriano; Nouar, Farid; Serre, Christian; Maurin, Guillaume; Ghoufi, Aziz (2023). Adsorption and dynamics of linear and mono-branched hexane isomers in MIL-140 metal-organic frameworks. Physical Chemistry Chemical Physics. eISSN 1463-9084. 25:17, p. 12057-12064 1463-9076 10.1039/d2cp05371c 1463-9084 |
dc.rights.driver.fl_str_mv |
info:eu-repo/semantics/openAccess |
eu_rights_str_mv |
openAccess |
dc.format.none.fl_str_mv |
application/pdf |
dc.publisher.none.fl_str_mv |
The Royal Society of Chemistry |
publisher.none.fl_str_mv |
The Royal Society of Chemistry |
dc.source.none.fl_str_mv |
reponame:Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) instname:Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação instacron:RCAAP |
instname_str |
Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação |
instacron_str |
RCAAP |
institution |
RCAAP |
reponame_str |
Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
collection |
Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
repository.name.fl_str_mv |
Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação |
repository.mail.fl_str_mv |
|
_version_ |
1799135371592728576 |