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Adsorption of sulfur dioxide in Cu(II)-carboxylate framework materials: the role of ligand functionalization and open metal sites

DOI: 10.1021/jacs.2c03280 DOI Help

Authors: Weiyao Li (University of Manchester) , Jiangnan Li (University of Manchester) , Thien D. Duong (University of Manchester) , Sergey A. Sapchenko (University of Manchester) , Xue Han (University of Manchester) , Jack D. Humby (University of Manchester) , George F. S. Whitehead (University of Manchester) , Inigo J. Vitórica-Yrezábal (University of Manchester) , Ivan Da Silva (ISIS Facility) , Pascal Manuel (ISIS Facility) , Mark D. Frogley (Diamond Light Source) , Gianfelice Cinque (Diamond Light Source) , Martin Schroeder (University of Manchester) , Sihai Yang (University of Manchester)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Journal Of The American Chemical Society , VOL 12

State: Published (Approved)
Published: July 2022
Diamond Proposal Number(s): 28479 , 23480

Open Access Open Access

Abstract: 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 describe 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.

Journal Keywords: Adsorption; Materials; Mathematical methods; Metal organic frameworks; Stabilit

Diamond Keywords: Gas Separation

Subject Areas: Materials, Chemistry, Environment

Instruments: B22-Multimode InfraRed imaging And Microspectroscopy , I19-Small Molecule Single Crystal Diffraction

Other Facilities: TOSCA, WISH at ISIS

Added On: 20/07/2022 10:11


Discipline Tags:

Desertification & Pollution Earth Sciences & Environment Chemistry Materials Science Metal-Organic Frameworks Metallurgy Organometallic Chemistry

Technical Tags:

Diffraction Spectroscopy Single Crystal X-ray Diffraction (SXRD) Infrared Spectroscopy Synchtron-based Fourier Transform Infrared Spectroscopy (SR-FTIR)