Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 36, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202207259
Keywords
Capture; Conversion; Crystallography; Metal-Organic Frameworks; Sulfur Dioxide
Categories
Funding
- EPSRC [EP/I011870]
- Royal Society
- University of Manchester
- European Research Council (ERC) under the European Union [742401]
- European Research Council (ERC) [742401] Funding Source: European Research Council (ERC)
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Reversible high-capacity adsorption of SO2 has been achieved in Zr-based metal-organic framework (MOF) materials. By introducing amine, atomically-dispersed Cu-II, or heteroatomic sulphur sites into the pores, the capture of SO2 at low concentrations is enhanced, and the captured SO2 can be converted to a valuable pharmaceutical intermediate.
We report reversible high capacity adsorption of SO2 in robust Zr-based metal-organic framework (MOF) materials. Zr-bptc (H(4)bptc=biphenyl-3,3 ',5,5 '-tetracarboxylic acid) shows a high SO2 uptake of 6.2 mmol g(-1) at 0.1 bar and 298 K, reflecting excellent capture capability and removal of SO2 at low concentration (2500 ppm). Dynamic breakthrough experiments confirm that the introduction of amine, atomically-dispersed Cu-II or heteroatomic sulphur sites into the pores enhance the capture of SO2 at low concentrations. The captured SO2 can be converted quantitatively to a pharmaceutical intermediate, aryl N-aminosulfonamide, thus converting waste to chemical values. In situ X-ray diffraction, infrared micro-spectroscopy and inelastic neutron scattering enable the visualisation of the binding domains of adsorbed SO2 molecules and host-guest binding dynamics in these materials at the atomic level. Refinement of the pore environment plays a critical role in designing efficient sorbent materials.
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