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Title: Construction of hierarchically porous metal–organic frameworks through linker labilization

Abstract

One major goal of metal–organic framework (MOF) research is the expansion of pore size and volume. Although many approaches have been attempted to increase the pore size of MOF materials, it is still a challenge to construct MOFs with precisely customized pore apertures for specific applications. W present a new method, namely linker labilization, to increase the MOF porosity and pore size, giving rise to hierarchical-pore architectures. Microporous MOFs with robust metal nodes and pro-labile linkers were initially synthesized. The mesopores were subsequently created as crystal defects through the splitting of a pro-labile-linker and the removal of the linker fragments by acid treatment. We also demonstrate that linker labilization method can create controllable hierarchical porous structures in stable MOFs, which facilitates the diffusion and adsorption process of guest molecules to improve the performances of MOFs in adsorption and catalysis.

Authors:
 [1];  [1];  [2];  [1]; ORCiD logo [3];  [1];  [1];  [1];  [4];  [5]; ORCiD logo [6]
  1. Texas A & M Univ., College Station, TX (United States). Dept. of Chemistry
  2. Texas A & M Univ., College Station, TX (United States). Dept. of Chemistry; King Saud Univ., Riyadh (Saudi Arabia). Chemistry Dept.
  3. Texas A & M Univ., College Station, TX (United States). Dept. of Materials Science and Engineering
  4. King Saud Univ., Riyadh (Saudi Arabia). Chemistry Dept.
  5. Texas A & M Univ., College Station, TX (United States). Dept. of Materials Science and Engineering, Artie McFerrin Dept. of Chemical Engineering
  6. Texas A & M Univ., College Station, TX (United States). Dept. of Chemistry, Dept. of Materials Science and Engineering; King Saud Univ., Riyadh (Saudi Arabia). Chemistry Dept.
Publication Date:
Research Org.:
Univ. of California, Berkeley, CA (United States); Texas A & M Univ., College Station, TX (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1389292
Grant/Contract Number:  
SC0001015; FE0026472
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; metal-organic frameworks; solid-state chemistry

Citation Formats

Yuan, Shuai, Zou, Lanfang, Qin, Jun-Sheng, Li, Jialuo, Huang, Lan, Feng, Liang, Wang, Xuan, Bosch, Mathieu, Alsalme, Ali, Cagin, Tahir, and Zhou, Hong-Cai. Construction of hierarchically porous metal–organic frameworks through linker labilization. United States: N. p., 2017. Web. doi:10.1038/ncomms15356.
Yuan, Shuai, Zou, Lanfang, Qin, Jun-Sheng, Li, Jialuo, Huang, Lan, Feng, Liang, Wang, Xuan, Bosch, Mathieu, Alsalme, Ali, Cagin, Tahir, & Zhou, Hong-Cai. Construction of hierarchically porous metal–organic frameworks through linker labilization. United States. doi:10.1038/ncomms15356.
Yuan, Shuai, Zou, Lanfang, Qin, Jun-Sheng, Li, Jialuo, Huang, Lan, Feng, Liang, Wang, Xuan, Bosch, Mathieu, Alsalme, Ali, Cagin, Tahir, and Zhou, Hong-Cai. Thu . "Construction of hierarchically porous metal–organic frameworks through linker labilization". United States. doi:10.1038/ncomms15356. https://www.osti.gov/servlets/purl/1389292.
@article{osti_1389292,
title = {Construction of hierarchically porous metal–organic frameworks through linker labilization},
author = {Yuan, Shuai and Zou, Lanfang and Qin, Jun-Sheng and Li, Jialuo and Huang, Lan and Feng, Liang and Wang, Xuan and Bosch, Mathieu and Alsalme, Ali and Cagin, Tahir and Zhou, Hong-Cai},
abstractNote = {One major goal of metal–organic framework (MOF) research is the expansion of pore size and volume. Although many approaches have been attempted to increase the pore size of MOF materials, it is still a challenge to construct MOFs with precisely customized pore apertures for specific applications. W present a new method, namely linker labilization, to increase the MOF porosity and pore size, giving rise to hierarchical-pore architectures. Microporous MOFs with robust metal nodes and pro-labile linkers were initially synthesized. The mesopores were subsequently created as crystal defects through the splitting of a pro-labile-linker and the removal of the linker fragments by acid treatment. We also demonstrate that linker labilization method can create controllable hierarchical porous structures in stable MOFs, which facilitates the diffusion and adsorption process of guest molecules to improve the performances of MOFs in adsorption and catalysis.},
doi = {10.1038/ncomms15356},
journal = {Nature Communications},
number = ,
volume = 8,
place = {United States},
year = {2017},
month = {5}
}

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Cited by: 62 works
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Figures / Tables:

Figure 1 Figure 1: Schematic representations. (a) Linker installation; (b) linker labilization; (c) hierarchically porous MOF developed by linker labilization.

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    Works referencing / citing this record:

    Copper Benzene Tricarboxylate Metal–Organic Framework with Wide Permanent Mesopores Stabilized by Keggin Polyoxometallate Ions
    journal, June 2012

    • Wee, Lik H.; Wiktor, Christian; Turner, Stuart
    • Journal of the American Chemical Society, Vol. 134, Issue 26
    • DOI: 10.1021/ja302089w

    Thermodynamically Guided Synthesis of Mixed-Linker Zr-MOFs with Enhanced Tunability
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    • Yuan, Shuai; Qin, Jun-Sheng; Zou, Lanfang
    • Journal of the American Chemical Society, Vol. 138, Issue 20
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    CH4 storage and CO2 capture in highly porous zirconium oxide based metal–organic frameworks
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    • Yang, Qingyuan; Guillerm, Vincent; Ragon, Florence
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    • DOI: 10.1002/anie.201505461

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    • DOI: 10.1021/jacs.5b03904

    Linker Installation: Engineering Pore Environment with Precisely Placed Functionalities in Zirconium MOFs
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    • Yuan, Shuai; Chen, Ying-Pin; Qin, Jun-Sheng
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    Heterogeneity within Order in Crystals of a Porous Metal–Organic Framework
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    Establishing Porosity Gradients within Metal–Organic Frameworks Using Partial Postsynthetic Ligand Exchange
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    • Chemical Society Reviews, Vol. 38, Issue 5, p. 1450-1459
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    Immobilization of MP-11 into a Mesoporous Metal–Organic Framework, MP-11@mesoMOF: A New Platform for Enzymatic Catalysis
    journal, July 2011

    • Lykourinou, Vasiliki; Chen, Yao; Wang, Xi-Sen
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    • DOI: 10.1021/ja2038003

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    • Gomez-Gualdron, Diego A.; Gutov, Oleksii V.; Krungleviciute, Vaiva
    • Chemistry of Materials, Vol. 26, Issue 19
    • DOI: 10.1021/cm502304e

    Metal-Organic Framework Nanospheres with Well-Ordered Mesopores Synthesized in an Ionic Liquid/CO2/Surfactant System
    journal, December 2010

    • Zhao, Yueju; Zhang, Jianling; Han, Buxing
    • Angewandte Chemie International Edition, Vol. 50, Issue 3
    • DOI: 10.1002/anie.201005314

    Sequential Linker Installation: Precise Placement of Functional Groups in Multivariate Metal–Organic Frameworks
    journal, March 2015

    • Yuan, Shuai; Lu, Weigang; Chen, Ying-Pin
    • Journal of the American Chemical Society, Vol. 137, Issue 9
    • DOI: 10.1021/ja512762r

    Solvent-Assisted Linker Exchange: An Alternative to the De Novo Synthesis of Unattainable Metal-Organic Frameworks
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      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.