Reversible coordinative binding and separation of sulfur dioxide in a robust metal–organic framework with open copper sites

Gemma L. Smith, Jennifer E. Eyley, Xue Han, Xinran Zhang, Jiangnan Li, Nicholas M. Jacques, Harry G.W. Godfrey, Stephen P. Argent, Laura J. McCormick McPherson, Simon J. Teat, Yongqiang Cheng, Mark D. Frogley, Gianfelice Cinque, Sarah J. Day, Chiu C. Tang, Timothy L. Easun, Svemir Rudić, Anibal J. Ramirez-Cuesta, Sihai Yang, Martin Schröder

Research output: Contribution to journalArticlepeer-review

196 Scopus citations

Abstract

Emissions of SO2 from flue gas and marine transport have detrimental impacts on the environment and human health, but SO2 is also an important industrial feedstock if it can be recovered, stored and transported efficiently. Here we report the exceptional adsorption and separation of SO2 in a porous material, [Cu2(L)] (H4L = 4′,4‴-(pyridine-3,5-diyl)bis([1,1′-biphenyl]-3,5-dicarboxylic acid)), MFM-170. MFM-170 exhibits fully reversible SO2 uptake of 17.5 mmol g−1 at 298 K and 1.0 bar, and the SO2 binding domains for trapped molecules within MFM-170 have been determined. We report the reversible coordination of SO2 to open Cu(ii) sites, which contributes to excellent adsorption thermodynamics and selectivities for SO2 binding and facile regeneration of MFM-170 after desorption. MFM-170 is stable to water, acid and base and shows great promise for the dynamic separation of SO2 from simulated flue gas mixtures, as confirmed by breakthrough experiments.

Original languageEnglish
Pages (from-to)1358-1365
Number of pages8
JournalNature Materials
Volume18
Issue number12
DOIs
StatePublished - Dec 1 2019

Funding

We thank EPSRC (EP/I011870), ERC (AdG 742041), the Royal Society and University of Manchester for funding. We are especially grateful to Diamond Light Source, Advanced Light Source, Oak Ridge National Laboratory and STFC/ISIS Neutron Facility for access to the beamlines B22/I11, 11.3.1, VISION and TOSCA, respectively. We thank M. Kibble for help at TOSCA beamline. The computing resources were made available through the VirtuES and the ICE-MAN projects, funded by the Laboratory Directed Research and Development programme at ORNL. This research used resources of the Advanced Light Source, which is a US Department of Energy Office of Science User Facility under contract no. DE-AC02-05CH11231. J.L. and X.Z. thank the China Scholarship Council (CSC) for funding.

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