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Title: Post-synthetic modulation of the charge distribution in a metal–organic framework for optimal binding of carbon dioxide and sulfur dioxide

Abstract

Modulation of pore environment is an effective strategy to optimize guest binding in porous materials. We report the post-synthetic modification of the charge distribution in a charged metal–organic framework, MFM-305-CH3, [Al(OH)(L)]Cl, [(H2L)Cl ¼ 3,5-dicarboxy-1-methylpyridinium chloride] and its effect on guest binding. MFM-305-CH3 shows a distribution of cationic (methylpyridinium) and anionic (chloride) centers and can be modified to release free pyridyl N-centres by thermal demethylation of the 1- methylpyridinium moiety to give the neutral isostructural MFM-305. This leads simultaneously to enhanced adsorption capacities and selectivities (two parameters that often change in opposite directions) for CO2 and SO2 in MFM-305. The host–guest binding has been comprehensively investigated by in situ synchrotron X-ray and neutron powder diffraction, inelastic neutron scattering, synchrotron infrared and 2 H NMR spectroscopy and theoretical modelling to reveal the binding domains of CO2 and SO2 in these materials. CO2 and SO2 binding in MFM-305-CH3 is shown to occur via hydrogen bonding to the methyl and aromatic-CH groups, with a long range interaction to chloride for CO2. In MFM-305 the hydroxyl, pyridyl and aromatic C–H groups bind CO2 and SO2 more effectively via hydrogen bonds and dipole interactions. Post-synthetic modification via dealkylation of the as-synthesised metal–organic framework is a powerfulmore » route to the synthesis of materials incorporating active polar groups that cannot be prepared directly.« less

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [3];  [4];  [4]; ORCiD logo [4];  [5];  [5];  [4];  [4];  [4];  [4];  [2];  [6];  [6];  [5];  [6];  [6]; ORCiD logo [3]; ORCiD logo [4] more »; ORCiD logo [4] « less
+ Show Author Affiliations
  1. Univ. of Manchester (United Kingdom). School of Chemistry Manchester; Sun Yat-Sen Univ., Guangzhou (China). School of Chemistry. Lehn Inst. of Functional Materials
  2. STFC Rutherford Appleton Lab., Chilton (United Kingdom). ISIS Neutron Facility
  3. Russian Academy of Sciences (RAS), Novosibirsk (Russian Federation). Boreskov Inst. of Catalysis; Novosibirsk State Univ. (Russian Federation)
  4. Univ. of Manchester (United Kingdom). School of Chemistry Manchester
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences and Engineering Division. Neutron Sciences Directorate
  6. Harwell Science Campus, Oxfordshire (United Kingdom). Diamond Light Source
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1624963
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Chemical Science
Additional Journal Information:
Journal Volume: 10; Journal Issue: 5; Journal ID: ISSN 2041-6520
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry

Citation Formats

Li, Lei, da Silva, Ivan, Kolokolov, Daniil I., Han, Xue, Li, Jiangnan, Smith, Gemma, Cheng, Yongqiang, Daemen, Luke L., Morris, Christopher G., Godfrey, Harry G. W., Jacques, Nicholas M., Zhang, Xinran, Manuel, Pascal, Frogley, Mark D., Murray, Claire A., Ramirez-Cuesta, Anibal J., Cinque, Gianfelice, Tang, Chiu C., Stepanov, Alexander G., Yang, Sihai, and Schroder, Martin. Post-synthetic modulation of the charge distribution in a metal–organic framework for optimal binding of carbon dioxide and sulfur dioxide. United States: N. p., 2019. Web. doi:10.1039/c8sc01959b.
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Li, Lei, da Silva, Ivan, Kolokolov, Daniil I., Han, Xue, Li, Jiangnan, Smith, Gemma, Cheng, Yongqiang, Daemen, Luke L., Morris, Christopher G., Godfrey, Harry G. W., Jacques, Nicholas M., Zhang, Xinran, Manuel, Pascal, Frogley, Mark D., Murray, Claire A., Ramirez-Cuesta, Anibal J., Cinque, Gianfelice, Tang, Chiu C., Stepanov, Alexander G., Yang, Sihai, & Schroder, Martin. Post-synthetic modulation of the charge distribution in a metal–organic framework for optimal binding of carbon dioxide and sulfur dioxide. United States. https://doi.org/10.1039/c8sc01959b
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Li, Lei, da Silva, Ivan, Kolokolov, Daniil I., Han, Xue, Li, Jiangnan, Smith, Gemma, Cheng, Yongqiang, Daemen, Luke L., Morris, Christopher G., Godfrey, Harry G. W., Jacques, Nicholas M., Zhang, Xinran, Manuel, Pascal, Frogley, Mark D., Murray, Claire A., Ramirez-Cuesta, Anibal J., Cinque, Gianfelice, Tang, Chiu C., Stepanov, Alexander G., Yang, Sihai, and Schroder, Martin. Tue . "Post-synthetic modulation of the charge distribution in a metal–organic framework for optimal binding of carbon dioxide and sulfur dioxide". United States. https://doi.org/10.1039/c8sc01959b. https://www.osti.gov/servlets/purl/1624963.
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@article{osti_1624963,
title = {Post-synthetic modulation of the charge distribution in a metal–organic framework for optimal binding of carbon dioxide and sulfur dioxide},
author = {Li, Lei and da Silva, Ivan and Kolokolov, Daniil I. and Han, Xue and Li, Jiangnan and Smith, Gemma and Cheng, Yongqiang and Daemen, Luke L. and Morris, Christopher G. and Godfrey, Harry G. W. and Jacques, Nicholas M. and Zhang, Xinran and Manuel, Pascal and Frogley, Mark D. and Murray, Claire A. and Ramirez-Cuesta, Anibal J. and Cinque, Gianfelice and Tang, Chiu C. and Stepanov, Alexander G. and Yang, Sihai and Schroder, Martin},
abstractNote = {Modulation of pore environment is an effective strategy to optimize guest binding in porous materials. We report the post-synthetic modification of the charge distribution in a charged metal–organic framework, MFM-305-CH3, [Al(OH)(L)]Cl, [(H2L)Cl ¼ 3,5-dicarboxy-1-methylpyridinium chloride] and its effect on guest binding. MFM-305-CH3 shows a distribution of cationic (methylpyridinium) and anionic (chloride) centers and can be modified to release free pyridyl N-centres by thermal demethylation of the 1- methylpyridinium moiety to give the neutral isostructural MFM-305. This leads simultaneously to enhanced adsorption capacities and selectivities (two parameters that often change in opposite directions) for CO2 and SO2 in MFM-305. The host–guest binding has been comprehensively investigated by in situ synchrotron X-ray and neutron powder diffraction, inelastic neutron scattering, synchrotron infrared and 2 H NMR spectroscopy and theoretical modelling to reveal the binding domains of CO2 and SO2 in these materials. CO2 and SO2 binding in MFM-305-CH3 is shown to occur via hydrogen bonding to the methyl and aromatic-CH groups, with a long range interaction to chloride for CO2. In MFM-305 the hydroxyl, pyridyl and aromatic C–H groups bind CO2 and SO2 more effectively via hydrogen bonds and dipole interactions. Post-synthetic modification via dealkylation of the as-synthesised metal–organic framework is a powerful route to the synthesis of materials incorporating active polar groups that cannot be prepared directly.},
doi = {10.1039/c8sc01959b},
journal = {Chemical Science},
number = 5,
volume = 10,
place = {United States},
year = {Tue Jan 01 00:00:00 EST 2019},
month = {Tue Jan 01 00:00:00 EST 2019}
}
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