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

doi:10.1038/s41563-019-0495-0

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 journal › Article › peer-review

175 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 language	English
Pages (from-to)	1358-1365
Number of pages	8
Journal	Nature Materials
Volume	18
Issue number	12
DOIs	https://doi.org/10.1038/s41563-019-0495-0
State	Published - Dec 1 2019

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Publisher Copyright:
© 2019, The Author(s), under exclusive licence to Springer Nature Limited.

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Smith, G. L., Eyley, J. E., Han, X., Zhang, X., Li, J., Jacques, N. M., Godfrey, H. G. W., Argent, S. P., McCormick McPherson, L. J., Teat, S. J., Cheng, Y., Frogley, M. D., Cinque, G., Day, S. J., Tang, C. C., Easun, T. L., Rudić, S., Ramirez-Cuesta, A. J., Yang, S., & Schröder, M. (2019). Reversible coordinative binding and separation of sulfur dioxide in a robust metal–organic framework with open copper sites. Nature Materials, 18(12), 1358-1365. https://doi.org/10.1038/s41563-019-0495-0

@article{62173edf1c24405d9346781f39cbcf37,

title = "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. 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.",

author = "Smith, {Gemma L.} and Eyley, {Jennifer E.} and Xue Han and Xinran Zhang and Jiangnan Li and Jacques, {Nicholas M.} and Godfrey, {Harry G.W.} and Argent, {Stephen P.} and {McCormick McPherson}, {Laura J.} and Teat, {Simon J.} and Yongqiang Cheng and Frogley, {Mark D.} and Gianfelice Cinque and Day, {Sarah J.} and Tang, {Chiu C.} and Easun, {Timothy L.} and Svemir Rudi{\'c} and Ramirez-Cuesta, {Anibal J.} and Sihai Yang and Martin Schr{\"o}der",

note = "Publisher Copyright: {\textcopyright} 2019, The Author(s), under exclusive licence to Springer Nature Limited.",

year = "2019",

month = dec,

day = "1",

doi = "10.1038/s41563-019-0495-0",

language = "English",

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Smith, GL, Eyley, JE, Han, X, Zhang, X, Li, J, Jacques, NM, Godfrey, HGW, Argent, SP, McCormick McPherson, LJ, Teat, SJ, Cheng, Y, Frogley, MD, Cinque, G, Day, SJ, Tang, CC, Easun, TL, Rudić, S, Ramirez-Cuesta, AJ, Yang, S & Schröder, M 2019, 'Reversible coordinative binding and separation of sulfur dioxide in a robust metal–organic framework with open copper sites', Nature Materials, vol. 18, no. 12, pp. 1358-1365. https://doi.org/10.1038/s41563-019-0495-0

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T1 - Reversible coordinative binding and separation of sulfur dioxide in a robust metal–organic framework with open copper sites

AU - Smith, Gemma L.

AU - Eyley, Jennifer E.

AU - Han, Xue

AU - Zhang, Xinran

AU - Li, Jiangnan

AU - Jacques, Nicholas M.

AU - Godfrey, Harry G.W.

AU - Argent, Stephen P.

AU - McCormick McPherson, Laura J.

AU - Teat, Simon J.

AU - Cheng, Yongqiang

AU - Frogley, Mark D.

AU - Cinque, Gianfelice

AU - Day, Sarah J.

AU - Tang, Chiu C.

AU - Easun, Timothy L.

AU - Rudić, Svemir

AU - Ramirez-Cuesta, Anibal J.

AU - Yang, Sihai

AU - Schröder, Martin

PY - 2019/12/1

Y1 - 2019/12/1

N2 - 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.

AB - 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.

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U2 - 10.1038/s41563-019-0495-0

DO - 10.1038/s41563-019-0495-0

M3 - Article

C2 - 31611671

AN - SCOPUS:85075443968

SN - 1476-1122

VL - 18

SP - 1358

EP - 1365

JO - Nature Materials

JF - Nature Materials

IS - 12

ER -

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

Abstract

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