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Analysis of High and Selective Uptake of CO2in 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.; Bichoutskaia, Elena; Lewis, William; Blake, Alexander J.; Schröder, Martin

Authors

Nada H. Alsmail

Mikhail Suyetin

Yong Yan

Rafel Cabot

Christina P. Krap

Jian Lü

Timothy L. Easun

ELENA BESLEY Elena.Besley@nottingham.ac.uk
Professor of Theoretical Computational Chemistry

William Lewis

Alexander J. Blake

Martin Schröder M.Schroder@man.ac.uk



Abstract

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.

Citation

Alsmail, N. H., Suyetin, M., Yan, Y., Cabot, R., Krap, C. P., Lü, J., …Schröder, M. (2014). Analysis of High and Selective Uptake of CO2in an Oxamide-Containing {Cu2(OOCR)4}-Based Metal-Organic Framework. Chemistry - A European Journal, 20(24), 7317-7324. https://doi.org/10.1002/chem.201304005

Journal Article Type Article
Acceptance Date Jan 12, 2014
Online Publication Date May 7, 2014
Publication Date Jun 10, 2014
Deposit Date Aug 27, 2015
Publicly Available Date Aug 27, 2015
Journal Chemistry - A European Journal
Print ISSN 0947-6539
Electronic ISSN 0947-6539
Publisher Wiley
Peer Reviewed Not Peer Reviewed
Volume 20
Issue 24
Pages 7317-7324
DOI https://doi.org/10.1002/chem.201304005
Keywords Metal-organic framework, CO2, methane, copper, isophthalate, carboxylic acid, amide
Public URL http://eprints.nottingham.ac.uk/id/eprint/29702
Publisher URL http://onlinelibrary.wiley.com/doi/10.1002/chem.201304005/abstract
Related Public URLs http://www.interscience.wiley.com
Copyright Statement Copyright information regarding this work can be found at the following address: http://eprints.nottingh.../end_user_agreement.pdf
Additional Information This is the pre-peer reviewed version of the following article:Analysis of high and selective uptake of CO2 in an oxamide-containing {Cu2(OOCR)4}-based metal-organic framework / Alsmail, N.H., Suyetin, M., Yan, Y., Cabot, R., Krap, C.P., Lü, J., Easun, T.L., Bichoutskaia, E., Lewis, W., Blake, A. J. and Schröder, M. Chemistry : a European Journal (2014), 20: 7317–7324 which has been published in final form at http://onlinelibrary.wi...chem.201304005/abstract

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Copyright Statement
Copyright information regarding this work can be found at the following address: http://eprints.nottingham.ac.uk/end_user_agreement.pdf





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