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Self-adjusting binding pockets enhance H2 and CH4 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 (?V = -7.8%), triggered by D2 adsorption at low pressures. This deformation creates two optimized binding pockets for hydrogen (Q st = -8.6 kJ mol-1) per pore, in agreement with H2 adsorption data. Analogous experiments with CD4 (Q st = -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.

SUBMITTER: Halter DP 

PROVIDER: S-EPMC7473405 | biostudies-literature | 2020 Jul

REPOSITORIES: biostudies-literature

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Self-adjusting binding pockets enhance H<sub>2</sub> and CH<sub>4</sub> adsorption in a uranium-based metal-organic framework.

Halter Dominik P DP   Klein Ryan A RA   Boreen Michael A MA   Trump Benjamin A BA   Brown Craig M CM   Long Jeffrey R JR  

Chemical science 20200527 26


A new, air-stable, permanently porous uranium(iv) metal-organic framework U(bdc)<sub>2</sub> (<b>1</b>, bdc<sup>2-</sup> = 1,4-benzenedicarboxylate) was synthesized and its H<sub>2</sub> and CH<sub>4</sub> adsorption properties were investigated. Low temperature adsorption isotherms confirm strong adsorption of both gases in the framework at low pressures. <i>In situ</i> gas-dosed neutron diffraction experiments with different D<sub>2</sub> loadings revealed a rare example of cooperative framewo  ...[more]

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