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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 Bichoutskaia

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.

Journal Article Type Article
Publication Date Jun 10, 2014
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Peer Reviewed Not Peer Reviewed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
APA6 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
DOI https://doi.org/10.1002/chem.201304005
Keywords Metal-organic framework, CO2, methane, copper, isophthalate, carboxylic acid, amide
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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