Ordered macro-microporous metal-organic framework single crystals

Kui Shen; Lei Zhang; Xiaodong Chen; Lingmei Liu; Daliang Zhang; Yu Han; Junying Chen; Jilan Long; Rafael Luque; Yingwei Li; Banglin Chen

doi:10.1126/science.aao3403

Ordered macro-microporous metal-organic framework single crystals

Kui Shen, Lei Zhang, Xiaodong Chen, Lingmei Liu, Daliang Zhang, Yu Han, Junying Chen, Jilan Long, Rafael Luque, Yingwei Li^*, Banglin Chen

^*Corresponding author for this work

Physical Sciences and Engineering

Research output: Contribution to journal › Article › peer-review

871 Scopus citations

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.

Original language	English (US)
Pages (from-to)	206-210
Number of pages	5
Journal	SCIENCE
Volume	359
Issue number	6372
DOIs	https://doi.org/10.1126/science.aao3403
State	Published - Jan 12 2018

Bibliographical note

Funding Information:
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.

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title = "Ordered macro-microporous metal-organic framework single crystals",

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.",

author = "Kui Shen and Lei Zhang and Xiaodong Chen and Lingmei Liu and Daliang Zhang and Yu Han and Junying Chen and Jilan Long and Rafael Luque and Yingwei Li and Banglin Chen",

note = "Funding Information: 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.",

year = "2018",

month = jan,

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doi = "10.1126/science.aao3403",

language = "English (US)",

volume = "359",

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journal = "SCIENCE",

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TY - JOUR

T1 - Ordered macro-microporous metal-organic framework single crystals

AU - Shen, Kui

AU - Zhang, Lei

AU - Chen, Xiaodong

AU - Liu, Lingmei

AU - Zhang, Daliang

AU - Han, Yu

AU - Chen, Junying

AU - Long, Jilan

AU - Luque, Rafael

AU - Li, Yingwei

AU - Chen, Banglin

N1 - Funding Information: 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.

PY - 2018/1/12

Y1 - 2018/1/12

N2 - 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.

AB - 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.

UR - http://www.scopus.com/inward/record.url?scp=85040460886&partnerID=8YFLogxK

U2 - 10.1126/science.aao3403

DO - 10.1126/science.aao3403

M3 - Article

C2 - 29326271

AN - SCOPUS:85040460886

SN - 0036-8075

VL - 359

SP - 206

EP - 210

JO - SCIENCE

JF - SCIENCE

IS - 6372

ER -

Ordered macro-microporous metal-organic framework single crystals

Abstract

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