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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); Energy Frontier Research Centers (EFRC) (United States). Center for Gas Separations Relevant to Clean Energy Technologies (CGS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
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. https://doi.org/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. https://doi.org/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 = {Thu May 25 00:00:00 EDT 2017},
month = {Thu May 25 00:00:00 EDT 2017}
}

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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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Modulated Synthesis of Zr-Based Metal-Organic Frameworks: From Nano to Single Crystals
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Synthesis, structural properties, and catalytic behavior of Cu-BTC and mixed-linker Cu-BTC-PyDC in the oxidation of benzene derivatives
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journal, November 2015


Metal–Organic Framework (MOF) Defects under Control: Insights into the Missing Linker Sites and Their Implication in the Reactivity of Zirconium-Based Frameworks
journal, August 2015

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journal, September 2011

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journal, August 2012

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An Interweaving MOF with High Hydrogen Uptake
journal, March 2006

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  • Journal of the American Chemical Society, Vol. 128, Issue 12
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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

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Heterogeneity within Order in Crystals of a Porous Metal–Organic Framework
journal, August 2011

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Cooperative Template-Directed Assembly of Mesoporous Metal–Organic Frameworks
journal, December 2011

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Postsynthetic Ligand and Cation Exchange in Robust Metal–Organic Frameworks
journal, October 2012

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Introduction of Functionalized Mesopores to Metal–Organic Frameworks via Metal–Ligand–Fragment Coassembly
journal, December 2012

  • Park, Jinhee; Wang, Zhiyong U.; Sun, Lin-Bing
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Template-Free Synthesis of Hierarchical Porous Metal–Organic Frameworks
journal, June 2013

  • Yue, Yanfeng; Qiao, Zhen-An; Fulvio, Pasquale F.
  • Journal of the American Chemical Society, Vol. 135, Issue 26
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Perfluoroalkane Functionalization of NU-1000 via Solvent-Assisted Ligand Incorporation: Synthesis and CO2 Adsorption Studies
journal, October 2013

  • Deria, Pravas; Mondloch, Joseph E.; Tylianakis, Emmanuel
  • Journal of the American Chemical Society, Vol. 135, Issue 45, p. 16801-16804
  • DOI: 10.1021/ja408959g

Structural Complexity in Metal–Organic Frameworks: Simultaneous Modification of Open Metal Sites and Hierarchical Porosity by Systematic Doping with Defective Linkers
journal, June 2014

  • Fang, Zhenlan; Dürholt, Johannes P.; Kauer, Max
  • Journal of the American Chemical Society, Vol. 136, Issue 27
  • DOI: 10.1021/ja503218j

Topology-Guided Design and Syntheses of Highly Stable Mesoporous Porphyrinic Zirconium Metal–Organic Frameworks with High Surface Area
journal, December 2014

  • Liu, Tian-Fu; Feng, Dawei; Chen, Ying-Pin
  • Journal of the American Chemical Society, Vol. 137, Issue 1
  • DOI: 10.1021/ja5111317

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

High Efficiency Adsorption and Removal of Selenate and Selenite from Water Using Metal–Organic Frameworks
journal, June 2015

  • Howarth, Ashlee J.; Katz, Michael J.; Wang, Timothy C.
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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.