期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 140, 期 44, 页码 15031-15037出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b09522
关键词
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资金
- National Science Centre, Poland [UMO-2014/14/E/ST5/00652]
- Spanish MINECO [CTQ2017-84692-R]
- EU Feder
- Wroclaw Centre of Biotechnology, The Leading National Research Centre (KNOW)
Selective separation of gases/vapors with similar physicochemical properties involves energetically costly distillation processes. Alternative separation processes based on shape-selective molecular sieving, taking place on porous frameworks (or membranes), are less energy demanding but require an optimal balance between selectivity and diffusion kinetics (permeability). Herein, we report a rational strategy to select an optimal soft noncovalent microporous material (NPM) suitable for the low-energy separation of C-6-hydrocarbons with kinetic diameters in the range of 4.3-6.3 angstrom. This strategy is based on a Cambridge Structural Database search of diamondoid NPMs with a low packing factor, leading to the selection of an oxidotetrazinc cluster based diamondoid NPM network named DiaMM-1 containing tetrahedral voids of 336 angstrom(3) (tetrahedron insphere diameter of 5.8 angstrom accessible through 8.2 angstrom triangular windows) suitable for this separation. Based on this result the fluorinated analogue DiaMM-2 was designed and synthesized. DiaMM-1 and DiaMM-2 exhibit permanent porosity and high thermal stability. The optimal combination of molecular crystal softness, pore size, and decoration of pore surface of DiaMM-1,-2 leads to high adsorbate diffusivity and low adsorption energy, allowing fast separation of hexane isomers and benzene/cyclohexane mixtures at low temperature.
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