4.8 Article

Adsorption of Sulfur Dioxide in Cu(II)-Carboxylate Framework Materials: The Role of Ligand Functionalization and Open Metal Sites

Journal

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 144, Issue 29, Pages 13196-13204

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/jacs.2c03280

Keywords

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Funding

  1. EPSRC [EP/I011870, EP/P001386]
  2. Royal Society
  3. University of Manchester
  4. European Research Council (ERC) under the European Union [742401]

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We report high adsorption of SO2 in a series of Cu(II)-carboxylate-based metal-organic framework materials. The functionalization of ligands and the presence of open metal sites contribute to the reversible adsorption of SO2. Specifically, MFM-101 and MFM-190(F) exhibit fully reversible SO2 adsorption with the highest capacities among all reported porous solids under ambient conditions.
The development of efficient sorbent materials for sulfur dioxide (SO2) is of key industrial interest. However, due to the corrosive nature of SO2, conventional porous materials often exhibit poor reversibility and limited uptake toward SO2 sorption. Here, we report high adsorption of SO2 in a series of Cu(II)-carboxylate-based metal-organic framework materials. We de-scribe the impact of ligand functionalization and open metal sites on the uptake and reversibility of SO2 adsorption. Specifically, MFM-101 and MFM-190(F) show fully reversible SO2 adsorption with remarkable capacities of 18.7 and 18.3 mmol g(-1), respectively, at 298 K and 1 bar; the former represents the highest reversible uptake of SO2 under ambient conditions among all porous solids reported to date. In situ neutron powder diffraction and synchrotron infrared microspectroscopy enable the direct visualization of binding domains of adsorbed SO2 molecules as well as host-guest binding dynamics. We have found that the combination of open Cu(II) sites and ligand functionalization, together with the size and geometry of metal-ligand cages, plays an integral role in the enhancement of SO2 binding.

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