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Title: Self-adjusting binding pockets enhance H 2 and CH 4 adsorption in a uranium-based metal–organic framework

Abstract

A new, air-stable, permanently porous uranium(IV) metal–organic framework U(bdc)2 (1, bdc2- = 1,4-benzenedicarboxylate) was synthesized and its H2 and CH4 adsorption properties were investigated. Low temperature adsorption isotherms confirm strong adsorption of both gases in the framework at low pressures. In situ gas-dosed neutron diffraction experiments with different D2 loadings revealed a rare example of cooperative framework contraction (ΔV = -7.8%), triggered by D2 adsorption at low pressures. This deformation creates two optimized binding pockets for hydrogen (Qst = -8.6 kJ mol-1) per pore, in agreement with H2 adsorption data. Analogous experiments with CD4 (Qst = -24.8 kJ mol-1) and N,N-dimethylformamide as guests revealed that the binding pockets in 1 adjust by selective framework contractions that are unique for each adsorbent, augmenting individual host–guest interactions. Our results suggest that the strategic combination of binding pockets and structural flexibility in metal–organic frameworks holds great potential for the development of new adsorbents with an enhanced substrate affinity.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3];  [4]; ORCiD logo [5]; ORCiD logo [1]
+ Show Author Affiliations
  1. Department of Chemistry, University of California, Berkeley, USA, Materials Sciences Division
  2. Chemistry and Nanoscience Department, National Renewable Energy Laboratory, Golden, USA, Center for Neutron Research
  3. Department of Chemistry, University of California, Berkeley, USA, Chemical Sciences Division
  4. Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, USA
  5. Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, USA, Department of Chemical Engineering
Publication Date:
Research Org.:
National Renewable Energy Laboratory (NREL), Golden, CO (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1632240
Alternate Identifier(s):
OSTI ID: 1660190; OSTI ID: 1667372
Report Number(s):
NREL/JA-5900-76743
Journal ID: ISSN 2041-6520; CSHCBM
Grant/Contract Number:  
AC02-05CH11231; AC02-06CH11357; AC36-08GO28308
Resource Type:
Published Article
Journal Name:
Chemical Science
Additional Journal Information:
Journal Name: Chemical Science Journal Volume: 11 Journal Issue: 26; Journal ID: ISSN 2041-6520
Publisher:
Royal Society of Chemistry
Country of Publication:
United Kingdom
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CH4 adsorption; H2 adsorption; metal-organic framework; self-adjusting binding pockets; uranium

Citation Formats

Halter, Dominik P., Klein, Ryan A., Boreen, Michael A., Trump, Benjamin A., Brown, Craig M., and Long, Jeffrey R. Self-adjusting binding pockets enhance H 2 and CH 4 adsorption in a uranium-based metal–organic framework. United Kingdom: N. p., 2020. Web. doi:10.1039/D0SC02394A.
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Halter, Dominik P., Klein, Ryan A., Boreen, Michael A., Trump, Benjamin A., Brown, Craig M., & Long, Jeffrey R. Self-adjusting binding pockets enhance H 2 and CH 4 adsorption in a uranium-based metal–organic framework. United Kingdom. https://doi.org/10.1039/D0SC02394A
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Halter, Dominik P., Klein, Ryan A., Boreen, Michael A., Trump, Benjamin A., Brown, Craig M., and Long, Jeffrey R. Wed . "Self-adjusting binding pockets enhance H 2 and CH 4 adsorption in a uranium-based metal–organic framework". United Kingdom. https://doi.org/10.1039/D0SC02394A.
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@article{osti_1632240,
title = {Self-adjusting binding pockets enhance H 2 and CH 4 adsorption in a uranium-based metal–organic framework},
author = {Halter, Dominik P. and Klein, Ryan A. and Boreen, Michael A. and Trump, Benjamin A. and Brown, Craig M. and Long, Jeffrey R.},
abstractNote = {A new, air-stable, permanently porous uranium(IV) metal–organic framework U(bdc)2 (1, bdc2- = 1,4-benzenedicarboxylate) was synthesized and its H2 and CH4 adsorption properties were investigated. Low temperature adsorption isotherms confirm strong adsorption of both gases in the framework at low pressures. In situ gas-dosed neutron diffraction experiments with different D2 loadings revealed a rare example of cooperative framework contraction (ΔV = -7.8%), triggered by D2 adsorption at low pressures. This deformation creates two optimized binding pockets for hydrogen (Qst = -8.6 kJ mol-1) per pore, in agreement with H2 adsorption data. Analogous experiments with CD4 (Qst = -24.8 kJ mol-1) and N,N-dimethylformamide as guests revealed that the binding pockets in 1 adjust by selective framework contractions that are unique for each adsorbent, augmenting individual host–guest interactions. Our results suggest that the strategic combination of binding pockets and structural flexibility in metal–organic frameworks holds great potential for the development of new adsorbents with an enhanced substrate affinity.},
doi = {10.1039/D0SC02394A},
journal = {Chemical Science},
number = 26,
volume = 11,
place = {United Kingdom},
year = {Wed Jul 08 00:00:00 EDT 2020},
month = {Wed Jul 08 00:00:00 EDT 2020}
}
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https://doi.org/10.1039/D0SC02394A
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