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https://hdl.handle.net/2440/78252
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Type: | Journal article |
Title: | Post-synthetic structural processing in a metal-organic framework material as a mechanism for exceptional CO₂/N₂ selectivity |
Other Titles: | Post-synthetic structural processing in a metal-organic framework material as a mechanism for exceptional CO(2)/N(2) selectivity |
Author: | Bloch, W. Babarao, R. Hill, M. Doonan, C. Sumby, C. |
Citation: | Journal of the American Chemical Society, 2013; 135(28):10441-10448 |
Publisher: | Amer Chemical Soc |
Issue Date: | 2013 |
ISSN: | 0002-7863 1520-5126 |
Statement of Responsibility: | Witold M. Bloch, Ravichandar Babarao, Matthew R. Hill, Christian J. Doonan, Christopher J. Sumby |
Abstract: | Here we report the synthesis and ceramic-like processing of a new metal-organic framework (MOF) material, [Cu(bcppm)H2O], that shows exceptionally selective separation for CO2 over N2 (ideal adsorbed solution theory, S(ads) = 590). [Cu(bcppm)H2O]·xS was synthesized in 82% yield by reaction of Cu(NO3)2·2.5H2O with the link bis(4-(4-carboxyphenyl)-1H-pyrazolyl)methane (H2bcppm) and shown to have a two-dimensional 4(4)-connected structure with an eclipsed arrangement of the layers. Activation of [Cu(bcppm)H2O] generates a pore-constricted version of the material through concomitant trellis-type pore narrowing (b-axis expansion and c-axis contraction) and a 2D-to-3D transformation (a-axis contraction) to give the adsorbing form, [Cu(bcppm)H2O]-ac. The pore contraction process and 2D-to-3D transformation were probed by single-crystal and powder X-ray diffraction experiments. The 3D network and shorter hydrogen-bonding contacts do not allow [Cu(bcppm)H2O]-ac to expand under gas loading across the pressure ranges examined or following re-solvation. This exceptional separation performance is associated with a moderate adsorption enthalpy and therefore an expected low energy cost for regeneration. |
Keywords: | Metal‐organic Framework gas separation carbon capture dynamic behavior post‐synthesis processing |
Rights: | © 2013 American Chemical Society |
DOI: | 10.1021/ja4032049 |
Grant ID: | http://purl.org/au-research/grants/arc/FT0991910 http://purl.org/au-research/grants/arc/FT100100400 |
Published version: | http://dx.doi.org/10.1021/ja4032049 |
Appears in Collections: | Aurora harvest Chemistry publications Environment Institute publications |
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