Reversible coordinative binding and separation of sulfur dioxide in a robust metal–organic framework with open copper sites
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. In this paper, 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.
- Authors:
-
- Univ. of Manchester, Manchester (United Kingdom)
- Univ. of Nottingham, Nottingham (United Kingdom)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Diamond Light Source, Didcot (United Kingdom)
- Cardiff Univ., Cardiff (United Kingdom)
- STFC Rutherford Appleton Lab., Chilton (United Kingdom)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
- OSTI Identifier:
- 1580420
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Materials
- Additional Journal Information:
- Journal Volume: 18; Journal Issue: 12; Journal ID: ISSN 1476-1122
- Publisher:
- Springer Nature - Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Smith, Gemma L., Eyley, Jennifer E., Han, Xue, Zhang, Xinran, Li, Jiangnan, Jacques, Nicholas M., Godfrey, Harry G. W., Argent, Stephen P., McCormick McPherson, Laura J., Teat, Simon J., Cheng, Yongqiang, Frogley, Mark D., Cinque, Gianfelice, Day, Sarah J., Tang, Chiu C., Easun, Timothy L., Rudić, Svemir, Ramirez-Cuesta, Anibal J., Yang, Sihai, and Schröder, Martin. Reversible coordinative binding and separation of sulfur dioxide in a robust metal–organic framework with open copper sites. United States: N. p., 2019.
Web. doi:10.1038/s41563-019-0495-0.
Smith, Gemma L., Eyley, Jennifer E., Han, Xue, Zhang, Xinran, Li, Jiangnan, Jacques, Nicholas M., Godfrey, Harry G. W., Argent, Stephen P., McCormick McPherson, Laura J., Teat, Simon J., Cheng, Yongqiang, Frogley, Mark D., Cinque, Gianfelice, Day, Sarah J., Tang, Chiu C., Easun, Timothy L., Rudić, Svemir, Ramirez-Cuesta, Anibal J., Yang, Sihai, & Schröder, Martin. Reversible coordinative binding and separation of sulfur dioxide in a robust metal–organic framework with open copper sites. United States. https://doi.org/10.1038/s41563-019-0495-0
Smith, Gemma L., Eyley, Jennifer E., Han, Xue, Zhang, Xinran, Li, Jiangnan, Jacques, Nicholas M., Godfrey, Harry G. W., Argent, Stephen P., McCormick McPherson, Laura J., Teat, Simon J., Cheng, Yongqiang, Frogley, Mark D., Cinque, Gianfelice, Day, Sarah J., Tang, Chiu C., Easun, Timothy L., Rudić, Svemir, Ramirez-Cuesta, Anibal J., Yang, Sihai, and Schröder, Martin. Mon .
"Reversible coordinative binding and separation of sulfur dioxide in a robust metal–organic framework with open copper sites". United States. https://doi.org/10.1038/s41563-019-0495-0. https://www.osti.gov/servlets/purl/1580420.
@article{osti_1580420,
title = {Reversible coordinative binding and separation of sulfur dioxide in a robust metal–organic framework with open copper sites},
author = {Smith, Gemma L. and Eyley, Jennifer E. and Han, Xue and Zhang, Xinran and Li, Jiangnan and Jacques, Nicholas M. and Godfrey, Harry G. W. and Argent, Stephen P. and McCormick McPherson, Laura J. and Teat, Simon J. and Cheng, Yongqiang and Frogley, Mark D. and Cinque, Gianfelice and Day, Sarah J. and Tang, Chiu C. and Easun, Timothy L. and Rudić, Svemir and Ramirez-Cuesta, Anibal J. and Yang, Sihai and Schröder, Martin},
abstractNote = {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. In this paper, 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.},
doi = {10.1038/s41563-019-0495-0},
journal = {Nature Materials},
number = 12,
volume = 18,
place = {United States},
year = {2019},
month = {10}
}
Web of Science
Figures / Tables:

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Figures / Tables found in this record: