Ordered macro-microporous metal-organic framework single crystals

Handle URI:
http://hdl.handle.net/10754/626978
Title:
Ordered macro-microporous metal-organic framework single crystals
Authors:
Shen, Kui ( 0000-0002-4132-4533 ) ; Zhang, Lei; Chen, Xiaodong; Liu, Lingmei; Zhang, Daliang ( 0000-0003-3494-7000 ) ; Han, Yu ( 0000-0003-1462-1118 ) ; Chen, Junying ( 0000-0003-3881-7238 ) ; Long, Jilan; Luque, Rafael ( 0000-0003-4190-1916 ) ; Li, Yingwei ( 0000-0003-1527-551X ) ; Chen, Banglin ( 0000-0001-8707-8115 )
Abstract:
We constructed highly oriented and ordered macropores within metal-organic framework (MOF) single crystals, opening up the area of three-dimensional-ordered macro-microporous materials (that is, materials containing both macro- and micropores) in single-crystalline form. Our methodology relies on the strong shaping effects of a polystyrene nanosphere monolith template and a double-solvent-induced heterogeneous nucleation approach. This process synergistically enabled the in situ growth of MOFs within ordered voids, rendering a single crystal with oriented and ordered macro-microporous structure. The improved mass diffusion properties of such hierarchical frameworks, together with their robust single-crystalline nature, endow them with superior catalytic activity and recyclability for bulky-molecule reactions, as compared with conventional, polycrystalline hollow, and disordered macroporous ZIF-8.
KAUST Department:
Advanced Membranes and Porous Materials Research Center; Physical Sciences and Engineering (PSE) Division; Chemical Science Program; Imaging and Characterization Core Lab
Citation:
Shen K, Zhang L, Chen X, Liu L, Zhang D, et al. (2018) Ordered macro-microporous metal-organic framework single crystals. Science 359: 206–210. Available: http://dx.doi.org/10.1126/science.aao3403.
Publisher:
American Association for the Advancement of Science (AAAS)
Journal:
Science
Issue Date:
16-Jan-2018
DOI:
10.1126/science.aao3403
Type:
Article
ISSN:
0036-8075; 1095-9203
Sponsors:
We thank the National Natural Science Foundation of China (grants 21606087, 21436005, 51621001, 21576095, and 21606088), the Fundamental Research Funds for the Central Universities (grants 2017PY004 and 2017MS069), the Guangdong Natural Science Foundation (grants 2014A030310445, 2016A050502004, and 2017A030312005), and the Welch Foundation (grant AX-1730) for financial support. K.S. thanks D. Tong for help with the schematic design and Y. Zhao for GFP preparation. K.S., Y.L., and B.C. conceived the idea and designed the experiments. K.S. synthesized the materials and carried out most of the structural characterization. Y.H., L.L., and D.Z. performed the HRTEM images and analyzed the results. K.S., L.Z., X.C., J.C., and J.L. performed the catalytic tests and some structural characterization. K.S., Y.L., B.C., and R.L. cowrote the paper. All authors discussed and commented on the manuscript. All data are reported in the main text and supplementary materials. K.S. and Y.L. are inventors on a patent/patent application (201710819873.9) held/submitted by South China University of Technology that covers the method for preparing ordered macroporous MOF single crystals.
Additional Links:
http://science.sciencemag.org/content/359/6372/206
Appears in Collections:
Articles; Advanced Membranes and Porous Materials Research Center; Advanced Nanofabrication, Imaging and Characterization Core Lab; Physical Sciences and Engineering (PSE) Division; Chemical Science Program

Full metadata record

DC FieldValue Language
dc.contributor.authorShen, Kuien
dc.contributor.authorZhang, Leien
dc.contributor.authorChen, Xiaodongen
dc.contributor.authorLiu, Lingmeien
dc.contributor.authorZhang, Daliangen
dc.contributor.authorHan, Yuen
dc.contributor.authorChen, Junyingen
dc.contributor.authorLong, Jilanen
dc.contributor.authorLuque, Rafaelen
dc.contributor.authorLi, Yingweien
dc.contributor.authorChen, Banglinen
dc.date.accessioned2018-02-01T07:25:00Z-
dc.date.available2018-02-01T07:25:00Z-
dc.date.issued2018-01-16en
dc.identifier.citationShen K, Zhang L, Chen X, Liu L, Zhang D, et al. (2018) Ordered macro-microporous metal-organic framework single crystals. Science 359: 206–210. Available: http://dx.doi.org/10.1126/science.aao3403.en
dc.identifier.issn0036-8075en
dc.identifier.issn1095-9203en
dc.identifier.doi10.1126/science.aao3403en
dc.identifier.urihttp://hdl.handle.net/10754/626978-
dc.description.abstractWe constructed highly oriented and ordered macropores within metal-organic framework (MOF) single crystals, opening up the area of three-dimensional-ordered macro-microporous materials (that is, materials containing both macro- and micropores) in single-crystalline form. Our methodology relies on the strong shaping effects of a polystyrene nanosphere monolith template and a double-solvent-induced heterogeneous nucleation approach. This process synergistically enabled the in situ growth of MOFs within ordered voids, rendering a single crystal with oriented and ordered macro-microporous structure. The improved mass diffusion properties of such hierarchical frameworks, together with their robust single-crystalline nature, endow them with superior catalytic activity and recyclability for bulky-molecule reactions, as compared with conventional, polycrystalline hollow, and disordered macroporous ZIF-8.en
dc.description.sponsorshipWe thank the National Natural Science Foundation of China (grants 21606087, 21436005, 51621001, 21576095, and 21606088), the Fundamental Research Funds for the Central Universities (grants 2017PY004 and 2017MS069), the Guangdong Natural Science Foundation (grants 2014A030310445, 2016A050502004, and 2017A030312005), and the Welch Foundation (grant AX-1730) for financial support. K.S. thanks D. Tong for help with the schematic design and Y. Zhao for GFP preparation. K.S., Y.L., and B.C. conceived the idea and designed the experiments. K.S. synthesized the materials and carried out most of the structural characterization. Y.H., L.L., and D.Z. performed the HRTEM images and analyzed the results. K.S., L.Z., X.C., J.C., and J.L. performed the catalytic tests and some structural characterization. K.S., Y.L., B.C., and R.L. cowrote the paper. All authors discussed and commented on the manuscript. All data are reported in the main text and supplementary materials. K.S. and Y.L. are inventors on a patent/patent application (201710819873.9) held/submitted by South China University of Technology that covers the method for preparing ordered macroporous MOF single crystals.en
dc.publisherAmerican Association for the Advancement of Science (AAAS)en
dc.relation.urlhttp://science.sciencemag.org/content/359/6372/206en
dc.titleOrdered macro-microporous metal-organic framework single crystalsen
dc.typeArticleen
dc.contributor.departmentAdvanced Membranes and Porous Materials Research Centeren
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.contributor.departmentChemical Science Programen
dc.contributor.departmentImaging and Characterization Core Laben
dc.identifier.journalScienceen
dc.contributor.institutionSchool of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640, , Chinaen
dc.contributor.institutionDepartamento de Química Orgánica, Universidad de Córdoba, Edificio Marie Curie, Carretera Nacional IV-A, Km 396, E14014, Córdoba, , Spainen
dc.contributor.institutionDepartment of Chemistry, University of Texas at San Antonio, One UTSA Circle, San Antonio, TX, 78249, , United Statesen
kaust.authorLiu, Lingmeien
kaust.authorZhang, Daliangen
kaust.authorHan, Yuen
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