Enhanced Sulfur Dioxide Adsorption in UiO-66 Through Crystal Engineering and Chalcogen Bonding

Walton, Ian; Chen, Carmen; Rimsza, Jessica M.; Nenoff, Tina M.; Walton, Krista S.

doi:10.1021/acs.cgd.0c00846

Enhanced Sulfur Dioxide Adsorption in UiO-66 Through Crystal Engineering and Chalcogen Bonding

Journal Article · Wed Jul 15 00:00:00 EDT 2020 · Crystal Growth and Design

DOI:https://doi.org/10.1021/acs.cgd.0c00846· OSTI ID:1670718

Walton, Ian ^[1]; Chen, Carmen ^[1]; ^[2]; ^[2]; ^[1]

Georgia Inst. of Technology, Atlanta, GA (United States)
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Adsorption of corrosive SO₂ gas occurs in metal–organic frameworks (MOFs) including UiO-66. Improvements in SO₂ capacity is obtained through the incorporation of residual modulators in the UiO-66 framework by introducing new binding sites in the material, through residual modulators. Four residual modulators were investigated (acetic acid, trifluoroacetic acid, 3-DMAP acid, cyanoacetic acid), and the UiO-66 framework modulated with cyanoacetic acid exhibited nearly twice the SO₂ uptake for the 18:1 modulator/linker synthesis ratio compared with other modulated UiO-66 structures. Density functional theory investigations confirmed that targeted host–guest interactions were maintained after the modulator was incorporated into the framework. The strongest binding energy was between SO₂ and cyanoacetic acid, consistent with dynamic SO₂ adsorption data, and identified contributions from both the SO₂ reacting with the residual modulator and the coordinating linkers. The successful increase in dynamic SO₂ capacity illustrates how often-overlooked non-covalent interactions can be used in targeted adsorption applications. Further investigation into weak electrostatic interactions for adsorption properties is also needed to advance the potential selectivity and capacity in the adsorption sphere.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC04-94AL85000; NA0003525

OSTI ID:: 1670718

Report Number(s):: SAND--2019-15328J; 682064

Journal Information:: Crystal Growth and Design, Journal Name: Crystal Growth and Design Journal Issue: 9 Vol. 20; ISSN 1528-7483

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Enhanced Sulfur Dioxide Adsorption in UiO-66 Through Crystal Engineering and Chalcogen Bonding

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