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Post-synthetic modulation of the charge distribution in a metal-organic framework for optimal binding of carbon dioxide and sulfur dioxide. / Li, Lei; Da Silva, Ivan; Kolokolov, Daniil I. и др.

в: Chemical Science, Том 10, № 5, 07.02.2019, стр. 1472-1482.

Результаты исследований: Научные публикации в периодических изданияхстатьяРецензирование

Harvard

Li, L, Da Silva, I, Kolokolov, DI, Han, X, Li, J, Smith, G, Cheng, Y, Daemen, LL, Morris, CG, Godfrey, HGW, Jacques, NM, Zhang, X, Manuel, P, Frogley, MD, Murray, CA, Ramirez-Cuesta, AJ, Cinque, G, Tang, CC, Stepanov, AG, Yang, S & Schroder, M 2019, 'Post-synthetic modulation of the charge distribution in a metal-organic framework for optimal binding of carbon dioxide and sulfur dioxide', Chemical Science, Том. 10, № 5, стр. 1472-1482. https://doi.org/10.1039/c8sc01959b

APA

Li, L., Da Silva, I., Kolokolov, D. I., Han, X., Li, J., Smith, G., Cheng, Y., Daemen, L. L., Morris, C. G., Godfrey, H. G. W., Jacques, N. M., Zhang, X., Manuel, P., Frogley, M. D., Murray, C. A., Ramirez-Cuesta, A. J., Cinque, G., Tang, C. C., Stepanov, A. G., ... Schroder, M. (2019). Post-synthetic modulation of the charge distribution in a metal-organic framework for optimal binding of carbon dioxide and sulfur dioxide. Chemical Science, 10(5), 1472-1482. https://doi.org/10.1039/c8sc01959b

Vancouver

Li L, Da Silva I, Kolokolov DI, Han X, Li J, Smith G и др. Post-synthetic modulation of the charge distribution in a metal-organic framework for optimal binding of carbon dioxide and sulfur dioxide. Chemical Science. 2019 февр. 7;10(5):1472-1482. doi: 10.1039/c8sc01959b

Author

BibTeX

@article{390e7fcd09a14ab4b380813ceada8ffc,
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 = 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 2H 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.",
keywords = "COORDINATION POLYMER, IONIC LIQUIDS, CO2 BINDING, FLUE-GAS, ADSORPTION, DESULFURIZATION, SELECTIVITY, ABSORPTION, CHEMISTRY, SERIES",
author = "Lei Li and {Da Silva}, Ivan and Kolokolov, {Daniil I.} and Xue Han and Jiangnan Li and Gemma Smith and Yongqiang Cheng and Daemen, {Luke L.} and Morris, {Christopher G.} and Godfrey, {Harry G.W.} and Jacques, {Nicholas M.} and Xinran Zhang and Pascal Manuel and Frogley, {Mark D.} and Murray, {Claire A.} and Ramirez-Cuesta, {Anibal J.} and Gianfelice Cinque and Tang, {Chiu C.} and Stepanov, {Alexander G.} and Sihai Yang and Martin Schroder",
note = "Publisher Copyright: {\textcopyright} The Royal Society of Chemistry.",
year = "2019",
month = feb,
day = "7",
doi = "10.1039/c8sc01959b",
language = "English",
volume = "10",
pages = "1472--1482",
journal = "Chemical Science",
issn = "2041-6520",
publisher = "Royal Society of Chemistry",
number = "5",

}

RIS

TY - JOUR

T1 - Post-synthetic modulation of the charge distribution in a metal-organic framework for optimal binding of carbon dioxide and sulfur dioxide

AU - Li, Lei

AU - Da Silva, Ivan

AU - Kolokolov, Daniil I.

AU - Han, Xue

AU - Li, Jiangnan

AU - Smith, Gemma

AU - Cheng, Yongqiang

AU - Daemen, Luke L.

AU - Morris, Christopher G.

AU - Godfrey, Harry G.W.

AU - Jacques, Nicholas M.

AU - Zhang, Xinran

AU - Manuel, Pascal

AU - Frogley, Mark D.

AU - Murray, Claire A.

AU - Ramirez-Cuesta, Anibal J.

AU - Cinque, Gianfelice

AU - Tang, Chiu C.

AU - Stepanov, Alexander G.

AU - Yang, Sihai

AU - Schroder, Martin

N1 - Publisher Copyright: © The Royal Society of Chemistry.

PY - 2019/2/7

Y1 - 2019/2/7

N2 - 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 = 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 2H 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.

AB - 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 = 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 2H 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.

KW - COORDINATION POLYMER

KW - IONIC LIQUIDS

KW - CO2 BINDING

KW - FLUE-GAS

KW - ADSORPTION

KW - DESULFURIZATION

KW - SELECTIVITY

KW - ABSORPTION

KW - CHEMISTRY

KW - SERIES

UR - http://www.scopus.com/inward/record.url?scp=85060862795&partnerID=8YFLogxK

U2 - 10.1039/c8sc01959b

DO - 10.1039/c8sc01959b

M3 - Article

C2 - 30842819

AN - SCOPUS:85060862795

VL - 10

SP - 1472

EP - 1482

JO - Chemical Science

JF - Chemical Science

SN - 2041-6520

IS - 5

ER -

ID: 18487529