Interchain-expanded extra-large-pore zeolites

Stable aluminosilicate zeolites with extra-large pores that are open through rings of more than 12 tetrahedra could be used to process molecules larger than those currently manageable in zeolite materials. However, until very recently1,2,3, they proved elusive. In analogy to the interlayer expansion...

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Autores: Gao, Zihao Rei, Yu, Huajian, Chen, Fei-Jian, Mayoral, Álvaro, Niu, Zijian, Niu, Ziwen, Li, Xintong, Deng, Hua, Márquez-Álvarez, Carlos, He, Hong, Xu, Shutao, Zhou, Yida, Xu, Jun, Xu, Hao, Fan, Wei, Balestra, Salvador R. G., Ma, Chao, Hao, Jiazheng, Li, Jian, Wu, Peng, Yu, Jihong, Camblor, Miguel A.
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2024
País:España
Institución:Universidad de Zaragoza
Repositorio:Zaguán. Repositorio Digital de la Universidad de Zaragoza
OAI Identifier:oai:zaguan.unizar.es:134585
Acceso en línea:http://zaguan.unizar.es/record/134585
Access Level:acceso abierto
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spelling Interchain-expanded extra-large-pore zeolitesGao, Zihao ReiYu, HuajianChen, Fei-JianMayoral, ÁlvaroNiu, ZijianNiu, ZiwenLi, XintongDeng, HuaMárquez-Álvarez, CarlosHe, HongXu, ShutaoZhou, YidaXu, JunXu, HaoFan, WeiBalestra, Salvador R. G.Ma, ChaoHao, JiazhengLi, JianWu, PengYu, JihongCamblor, Miguel A.Stable aluminosilicate zeolites with extra-large pores that are open through rings of more than 12 tetrahedra could be used to process molecules larger than those currently manageable in zeolite materials. However, until very recently1,2,3, they proved elusive. In analogy to the interlayer expansion of layered zeolite precursors4,5, we report a strategy that yields thermally and hydrothermally stable silicates by expansion of a one-dimensional silicate chain with an intercalated silylating agent that separates and connects the chains. As a result, zeolites with extra-large pores delimited by 20, 16 and 16 Si tetrahedra along the three crystallographic directions are obtained. The as-made interchain-expanded zeolite contains dangling Si–CH3 groups that, by calcination, connect to each other, resulting in a true, fully connected (except possible defects) three-dimensional zeolite framework with a very low density. Additionally, it features triple four-ring units not seen before in any type of zeolite. The silicate expansion–condensation approach we report may be amenable to further extra-large-pore zeolite formation. Ti can be introduced in this zeolite, leading to a catalyst that is active in liquid-phase alkene oxidations involving bulky molecules, which shows promise in the industrially relevant clean production of propylene oxide using cumene hydroperoxide as an oxidant2024info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionapplication/pdfhttp://zaguan.unizar.es/record/134585reponame:Zaguán. Repositorio Digital de la Universidad de Zaragozainstname:Universidad de ZaragozaInglésinfo:eu-repo/grantAgreement/ES/AEI/FJC2018-035697-Iinfo:eu-repo/grantAgreement/ES/DGA/E13-20Rinfo:eu-repo/grantAgreement/EC/H2020/823717This project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No H2020 823717-ESTEEM3info:eu-repo/grantAgreement/ES/MCIU/PID2019- 105479RB-I00info:eu-repo/grantAgreement/ES/MCIN/AEIinfo:eu-repo/grantAgreement/ES/MICINN/RYC-2018-024561-Iinfo:eu-repo/grantAgreement/ES/MICINN/TED2021-131223B-I00info:eu-repo/semantics/openAccessoai:zaguan.unizar.es:1345852026-05-29T13:59:51Z
dc.title.none.fl_str_mv Interchain-expanded extra-large-pore zeolites
title Interchain-expanded extra-large-pore zeolites
spellingShingle Interchain-expanded extra-large-pore zeolites
Gao, Zihao Rei
title_short Interchain-expanded extra-large-pore zeolites
title_full Interchain-expanded extra-large-pore zeolites
title_fullStr Interchain-expanded extra-large-pore zeolites
title_full_unstemmed Interchain-expanded extra-large-pore zeolites
title_sort Interchain-expanded extra-large-pore zeolites
dc.creator.none.fl_str_mv Gao, Zihao Rei
Yu, Huajian
Chen, Fei-Jian
Mayoral, Álvaro
Niu, Zijian
Niu, Ziwen
Li, Xintong
Deng, Hua
Márquez-Álvarez, Carlos
He, Hong
Xu, Shutao
Zhou, Yida
Xu, Jun
Xu, Hao
Fan, Wei
Balestra, Salvador R. G.
Ma, Chao
Hao, Jiazheng
Li, Jian
Wu, Peng
Yu, Jihong
Camblor, Miguel A.
author Gao, Zihao Rei
author_facet Gao, Zihao Rei
Yu, Huajian
Chen, Fei-Jian
Mayoral, Álvaro
Niu, Zijian
Niu, Ziwen
Li, Xintong
Deng, Hua
Márquez-Álvarez, Carlos
He, Hong
Xu, Shutao
Zhou, Yida
Xu, Jun
Xu, Hao
Fan, Wei
Balestra, Salvador R. G.
Ma, Chao
Hao, Jiazheng
Li, Jian
Wu, Peng
Yu, Jihong
Camblor, Miguel A.
author_role author
author2 Yu, Huajian
Chen, Fei-Jian
Mayoral, Álvaro
Niu, Zijian
Niu, Ziwen
Li, Xintong
Deng, Hua
Márquez-Álvarez, Carlos
He, Hong
Xu, Shutao
Zhou, Yida
Xu, Jun
Xu, Hao
Fan, Wei
Balestra, Salvador R. G.
Ma, Chao
Hao, Jiazheng
Li, Jian
Wu, Peng
Yu, Jihong
Camblor, Miguel A.
author2_role author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
description Stable aluminosilicate zeolites with extra-large pores that are open through rings of more than 12 tetrahedra could be used to process molecules larger than those currently manageable in zeolite materials. However, until very recently1,2,3, they proved elusive. In analogy to the interlayer expansion of layered zeolite precursors4,5, we report a strategy that yields thermally and hydrothermally stable silicates by expansion of a one-dimensional silicate chain with an intercalated silylating agent that separates and connects the chains. As a result, zeolites with extra-large pores delimited by 20, 16 and 16 Si tetrahedra along the three crystallographic directions are obtained. The as-made interchain-expanded zeolite contains dangling Si–CH3 groups that, by calcination, connect to each other, resulting in a true, fully connected (except possible defects) three-dimensional zeolite framework with a very low density. Additionally, it features triple four-ring units not seen before in any type of zeolite. The silicate expansion–condensation approach we report may be amenable to further extra-large-pore zeolite formation. Ti can be introduced in this zeolite, leading to a catalyst that is active in liquid-phase alkene oxidations involving bulky molecules, which shows promise in the industrially relevant clean production of propylene oxide using cumene hydroperoxide as an oxidant
publishDate 2024
dc.date.none.fl_str_mv 2024
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://zaguan.unizar.es/record/134585
url http://zaguan.unizar.es/record/134585
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv info:eu-repo/grantAgreement/ES/AEI/FJC2018-035697-I
info:eu-repo/grantAgreement/ES/DGA/E13-20R
info:eu-repo/grantAgreement/EC/H2020/823717
This project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No H2020 823717-ESTEEM3
info:eu-repo/grantAgreement/ES/MCIU/PID2019- 105479RB-I00
info:eu-repo/grantAgreement/ES/MCIN/AEI
info:eu-repo/grantAgreement/ES/MICINN/RYC-2018-024561-I
info:eu-repo/grantAgreement/ES/MICINN/TED2021-131223B-I00
dc.rights.none.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
publisher.none.fl_str_mv
dc.source.none.fl_str_mv reponame:Zaguán. Repositorio Digital de la Universidad de Zaragoza
instname:Universidad de Zaragoza
instname_str Universidad de Zaragoza
reponame_str Zaguán. Repositorio Digital de la Universidad de Zaragoza
collection Zaguán. Repositorio Digital de la Universidad de Zaragoza
repository.name.fl_str_mv
repository.mail.fl_str_mv
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