Chris Hawes c.s.hawes@keele.ac.uk
Porous Polyrotaxane Coordination Networks Containing Two Distinct Conformers of a Discontinuously Flexible Ligand
Hawes, Chris S.; Knowles, Gregory P.; Chaffee, Alan L.; White, Keith F.; Abrahams, Brendan F.; Batten, Stuart R.; Turner, David R.
Authors
Gregory P. Knowles
Alan L. Chaffee
Keith F. White
Brendan F. Abrahams
Stuart R. Batten
David R. Turner
Abstract
A new divergent homopiperazine-derived ligand N,N'-bis(4-carboxyphenyl)-1,4-diazacycloheptane H2L has been prepared, containing a semirigid saturated heterocyclic core which is capable of providing multiple distinct bridging geometries. Reaction of H2L with zinc acetate in DMSO gives a two-dimensional parallel interpenetrated polyrotaxane structure 1 in which the loops and rods are formed by the bent cis-(eq,ax) twist boat and trans-(ax,ax) twist chair conformers, respectively. By matching the distances between the solvated metal sites in the structure of 1, a related material 2 can be prepared incorporating the pillaring ligand trans-1,2-bis(4-pyridyl)ethylene bpe. Compound 2 displays a similar polyrotaxane interpenetration mode, permitted by the presence of both cis and trans ligand conformers, but displays a three-dimensional 2.69 topology related to the dia diamondoid network. The guest exchange and gas adsorption properties of both materials were investigated; while compound 1 displays poor stability to guest exchange and negligible gas uptake, the higher connectivity microporous compound 2 shows facile guest exchange and a surprisingly high CO2 capacity of 12 wt % at 1 bar and 273 K, and a zero-loading enthalpy of adsorption of -32 kJ mol-1 . High-pressure adsorption isotherms also show moderate physisorption of H2 and CH4 within the material.
Acceptance Date | Sep 26, 2016 |
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Publication Date | Sep 26, 2016 |
Journal | Inorganic Chemistry |
Print ISSN | 0020-1669 |
Publisher | American Chemical Society |
Pages | 10467 -10474 |
DOI | https://doi.org/10.1021/acs.inorgchem.6b01713 |
Publisher URL | http://doi.org/10.1021/acs.inorgchem.6b01713 |
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