Analysis of high and selective uptake of CO2 in an oxamide-containing {Cu2(OOCR)4}-based metal-organic framework

The porous framework [Cu2(H2O)2L].4H2O.2DMA ((H¬4¬L = oxalylbis(azanediyl)diisophthalic acid; DMA = N,N-dimethylacetamide), denoted NOTT-125, is formed by connection of {Cu2(RCOO)4} paddlewheels with the isophthalate linkers in L4-. A single crystal structure determination reveals that NOTT-125 cry...

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Main Authors: Alsmail, Nada H., Suyetin, Mikhail, Yan, Yong, Cabot, Rafel, Krap, Christina P., Lü, Jian, Easun, Timothy L., Biskoutskaia, Elena, Lewis, William, Blake, Alexander J., Schröder, Martin
Format: Article
Published: Wiley-VCH Verlag 2014
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Online Access:https://eprints.nottingham.ac.uk/29702/
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author Alsmail, Nada H.
Suyetin, Mikhail
Yan, Yong
Cabot, Rafel
Krap, Christina P.
Lü, Jian
Easun, Timothy L.
Biskoutskaia, Elena
Lewis, William
Blake, Alexander J.
Schröder, Martin
author_facet Alsmail, Nada H.
Suyetin, Mikhail
Yan, Yong
Cabot, Rafel
Krap, Christina P.
Lü, Jian
Easun, Timothy L.
Biskoutskaia, Elena
Lewis, William
Blake, Alexander J.
Schröder, Martin
author_sort Alsmail, Nada H.
building Nottingham Research Data Repository
collection Online Access
description The porous framework [Cu2(H2O)2L].4H2O.2DMA ((H¬4¬L = oxalylbis(azanediyl)diisophthalic acid; DMA = N,N-dimethylacetamide), denoted NOTT-125, is formed by connection of {Cu2(RCOO)4} paddlewheels with the isophthalate linkers in L4-. A single crystal structure determination reveals that NOTT-125 crystallises in monoclinic cell with a = 27.9161(6) Å, b = 18.6627(4) Å and c = 32.3643(8) Å, space group P2 (1)/c. The structure of this material shows fof topology, which can be viewed as the packing of two types of cages (Cage A and Cage B) in 3-dimensional space. Cage A is constructed by twelve {Cu2(OOCR)4} paddlewheels and six linkers to form an ellipsoid-shaped cavity approximately 24.0 Å along its long axis and 9.6 Å across the central diameter. Cage B consists of six {Cu2(OOCR)4} units and twelve linkers with a spherical diameter of 12.7 Å taking into account the van der Waals radii of the atoms. NOTT-125 incorporates oxamide functionality within the pore walls, and this, combined with high porosity in the desolvated NOTT-125a, is responsible for excellent CO2 uptake (40.1 wt% at 273 K and 1 bar) and selectivity for CO2 over CH4 or N2. Grand canonical Monte Carlo (GCMC) simulations show excellent agreement with the experimental gas isotherm data, and a computational study into the specific interactions and binding energies of both CO2 and CH4 with the linkers in NOTT-125 reveals a set of strong interactions between CO2 and the oxamide motif, which are not possible with a single amide.
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spelling nottingham-297022020-05-04T16:48:19Z https://eprints.nottingham.ac.uk/29702/ Analysis of high and selective uptake of CO2 in an oxamide-containing {Cu2(OOCR)4}-based metal-organic framework Alsmail, Nada H. Suyetin, Mikhail Yan, Yong Cabot, Rafel Krap, Christina P. Lü, Jian Easun, Timothy L. Biskoutskaia, Elena Lewis, William Blake, Alexander J. Schröder, Martin The porous framework [Cu2(H2O)2L].4H2O.2DMA ((H¬4¬L = oxalylbis(azanediyl)diisophthalic acid; DMA = N,N-dimethylacetamide), denoted NOTT-125, is formed by connection of {Cu2(RCOO)4} paddlewheels with the isophthalate linkers in L4-. A single crystal structure determination reveals that NOTT-125 crystallises in monoclinic cell with a = 27.9161(6) Å, b = 18.6627(4) Å and c = 32.3643(8) Å, space group P2 (1)/c. The structure of this material shows fof topology, which can be viewed as the packing of two types of cages (Cage A and Cage B) in 3-dimensional space. Cage A is constructed by twelve {Cu2(OOCR)4} paddlewheels and six linkers to form an ellipsoid-shaped cavity approximately 24.0 Å along its long axis and 9.6 Å across the central diameter. Cage B consists of six {Cu2(OOCR)4} units and twelve linkers with a spherical diameter of 12.7 Å taking into account the van der Waals radii of the atoms. NOTT-125 incorporates oxamide functionality within the pore walls, and this, combined with high porosity in the desolvated NOTT-125a, is responsible for excellent CO2 uptake (40.1 wt% at 273 K and 1 bar) and selectivity for CO2 over CH4 or N2. Grand canonical Monte Carlo (GCMC) simulations show excellent agreement with the experimental gas isotherm data, and a computational study into the specific interactions and binding energies of both CO2 and CH4 with the linkers in NOTT-125 reveals a set of strong interactions between CO2 and the oxamide motif, which are not possible with a single amide. Wiley-VCH Verlag 2014-05-07 Article PeerReviewed Alsmail, Nada H., Suyetin, Mikhail, Yan, Yong, Cabot, Rafel, Krap, Christina P., Lü, Jian, Easun, Timothy L., Biskoutskaia, Elena, Lewis, William, Blake, Alexander J. and Schröder, Martin (2014) Analysis of high and selective uptake of CO2 in an oxamide-containing {Cu2(OOCR)4}-based metal-organic framework. Chemistry - a European Journal, 20 (24). pp. 7317-7324. ISSN 0947-6539 Metal-organic framework CO2 methane copper isophthalate carboxylic acid amide http://onlinelibrary.wiley.com/doi/10.1002/chem.201304005/abstract doi:10.1002/chem.201304005 doi:10.1002/chem.201304005
spellingShingle Metal-organic framework
CO2
methane
copper
isophthalate
carboxylic acid
amide
Alsmail, Nada H.
Suyetin, Mikhail
Yan, Yong
Cabot, Rafel
Krap, Christina P.
Lü, Jian
Easun, Timothy L.
Biskoutskaia, Elena
Lewis, William
Blake, Alexander J.
Schröder, Martin
Analysis of high and selective uptake of CO2 in an oxamide-containing {Cu2(OOCR)4}-based metal-organic framework
title Analysis of high and selective uptake of CO2 in an oxamide-containing {Cu2(OOCR)4}-based metal-organic framework
title_full Analysis of high and selective uptake of CO2 in an oxamide-containing {Cu2(OOCR)4}-based metal-organic framework
title_fullStr Analysis of high and selective uptake of CO2 in an oxamide-containing {Cu2(OOCR)4}-based metal-organic framework
title_full_unstemmed Analysis of high and selective uptake of CO2 in an oxamide-containing {Cu2(OOCR)4}-based metal-organic framework
title_short Analysis of high and selective uptake of CO2 in an oxamide-containing {Cu2(OOCR)4}-based metal-organic framework
title_sort analysis of high and selective uptake of co2 in an oxamide-containing {cu2(oocr)4}-based metal-organic framework
topic Metal-organic framework
CO2
methane
copper
isophthalate
carboxylic acid
amide
url https://eprints.nottingham.ac.uk/29702/
https://eprints.nottingham.ac.uk/29702/
https://eprints.nottingham.ac.uk/29702/