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Title: Engineering Structural Dynamics of Zirconium Metal–Organic Frameworks Based on Natural C4 Linkers

Abstract

Engineering the structural flexibility of MOF materials for separation-related applications remains a great challenge. In this paper, we present a strategy of mixing rigid and soft linkers in a MOF structure to achieve tunable structural flexibility, as exemplified in a series of stable isostructural Zr-MOFs built with natural C4 linkers (fumaric acid, succinic acid and malic acid). As shown by the differences in linker bond stretching and bending freedom, these MOFs display distinct responsive dynamics to external stimuli, namely changes in temperature or guest molecule type. Comprehensive in-situ characterizations reveal a clear correlation between linker character and MOF dynamic behavior, which leads to the discovery of a multivariate flexible MOF. It shows an optimal combination of both good working capacity and significantly enhanced selectivity for CO2/N2 separation. In principle, it provides a new avenue for potentially improving the ability of microporous MOFs to separate other gaseous and liquid mixtures.

Authors:
ORCiD logo [1];  [2];  [3]; ORCiD logo [4];  [5];  [4];  [3];  [2];  [6]; ORCiD logo [7]; ORCiD logo [8]; ORCiD logo [9]; ORCiD logo [4];  [3]; ORCiD logo [10]
  1. PSL Université, Institut des Matériaux Poreux de Paris, (France); Univ. of Science and Technology of China, Hefei (China)
  2. PSL Université, Institut des Matériaux Poreux de Paris, (France)
  3. Université Montpellier, Place Eugène Bataillon (France)
  4. Univ. of Texas at Dallas, Richardson, TX (United States)
  5. Université Catholique de Louvain, Louvain-la-Neuve (Belgium)
  6. Université de Versailles Saint-Quentin-en-Yvelines, Université Paris-Saclay (France)
  7. Synchrotron SOLEIL, L’Orme des Merisiers, Saint-Aubin, Gif-Sur-Yvette (France)
  8. Université de Versailles Saint-Quentin-en-Yvelines, Université Paris-Saclay (France); CEMHTI (France)
  9. Université Catholique de Louvain (Belgium)
  10. PSL Université, Institut des Matériaux Poreux de Paris (France)
Publication Date:
Research Org.:
Univ. of Texas at Dallas, Richardson, TX (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1604798
Grant/Contract Number:  
SC0019902; FG02-08ER46491
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 141; Journal Issue: 43; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Wang, Sujing, Xhaferaj, Nertil, Wahiduzzaman, Mohammad, Oyekan, Kolade, Li, Xiao, Wei, Kevin, Zheng, Bin, Tissot, Antoine, Marrot, Jérôme, Shepard, William, Martineau-Corcos, Charlotte, Filinchuk, Yaroslav, Tan, Kui, Maurin, Guillaume, and Serre, Christian. Engineering Structural Dynamics of Zirconium Metal–Organic Frameworks Based on Natural C4 Linkers. United States: N. p., 2019. Web. doi:10.1021/jacs.9b07816.
Wang, Sujing, Xhaferaj, Nertil, Wahiduzzaman, Mohammad, Oyekan, Kolade, Li, Xiao, Wei, Kevin, Zheng, Bin, Tissot, Antoine, Marrot, Jérôme, Shepard, William, Martineau-Corcos, Charlotte, Filinchuk, Yaroslav, Tan, Kui, Maurin, Guillaume, & Serre, Christian. Engineering Structural Dynamics of Zirconium Metal–Organic Frameworks Based on Natural C4 Linkers. United States. doi:10.1021/jacs.9b07816.
Wang, Sujing, Xhaferaj, Nertil, Wahiduzzaman, Mohammad, Oyekan, Kolade, Li, Xiao, Wei, Kevin, Zheng, Bin, Tissot, Antoine, Marrot, Jérôme, Shepard, William, Martineau-Corcos, Charlotte, Filinchuk, Yaroslav, Tan, Kui, Maurin, Guillaume, and Serre, Christian. Mon . "Engineering Structural Dynamics of Zirconium Metal–Organic Frameworks Based on Natural C4 Linkers". United States. doi:10.1021/jacs.9b07816.
@article{osti_1604798,
title = {Engineering Structural Dynamics of Zirconium Metal–Organic Frameworks Based on Natural C4 Linkers},
author = {Wang, Sujing and Xhaferaj, Nertil and Wahiduzzaman, Mohammad and Oyekan, Kolade and Li, Xiao and Wei, Kevin and Zheng, Bin and Tissot, Antoine and Marrot, Jérôme and Shepard, William and Martineau-Corcos, Charlotte and Filinchuk, Yaroslav and Tan, Kui and Maurin, Guillaume and Serre, Christian},
abstractNote = {Engineering the structural flexibility of MOF materials for separation-related applications remains a great challenge. In this paper, we present a strategy of mixing rigid and soft linkers in a MOF structure to achieve tunable structural flexibility, as exemplified in a series of stable isostructural Zr-MOFs built with natural C4 linkers (fumaric acid, succinic acid and malic acid). As shown by the differences in linker bond stretching and bending freedom, these MOFs display distinct responsive dynamics to external stimuli, namely changes in temperature or guest molecule type. Comprehensive in-situ characterizations reveal a clear correlation between linker character and MOF dynamic behavior, which leads to the discovery of a multivariate flexible MOF. It shows an optimal combination of both good working capacity and significantly enhanced selectivity for CO2/N2 separation. In principle, it provides a new avenue for potentially improving the ability of microporous MOFs to separate other gaseous and liquid mixtures.},
doi = {10.1021/jacs.9b07816},
journal = {Journal of the American Chemical Society},
number = 43,
volume = 141,
place = {United States},
year = {2019},
month = {10}
}

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