Controlled thermal oxidative crosslinking of polymers of intrinsic microporosity towards tunable molecular sieve membranes

Qilei Song, Shuai Cao, Robyn H. Pritchard, Behnam Ghalei, Shaheen A. Al-Muhtaseb, Eugene M. Terentjev, Anthony K. Cheetham and Easan Sivaniah ()
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Qilei Song: Cavendish Laboratory, University of Cambridge
Shuai Cao: University of Cambridge
Robyn H. Pritchard: Cavendish Laboratory, University of Cambridge
Behnam Ghalei: Institute for Integrated Cell-Material Sciences (iCeMS), Kyoto University
Shaheen A. Al-Muhtaseb: Qatar University
Eugene M. Terentjev: Cavendish Laboratory, University of Cambridge
Anthony K. Cheetham: University of Cambridge
Easan Sivaniah: Cavendish Laboratory, University of Cambridge

Nature Communications, 2014, vol. 5, issue 1, 1-12

Abstract: Abstract Organic open frameworks with well-defined micropore (pore dimensions below 2 nm) structure are attractive next-generation materials for gas sorption, storage, catalysis and molecular level separations. Polymers of intrinsic microporosity (PIMs) represent a paradigm shift in conceptualizing molecular sieves from conventional ordered frameworks to disordered frameworks with heterogeneous distributions of microporosity. PIMs contain interconnected regions of micropores with high gas permeability but with a level of heterogeneity that compromises their molecular selectivity. Here we report controllable thermal oxidative crosslinking of PIMs by heat treatment in the presence of trace amounts of oxygen. The resulting covalently crosslinked networks are thermally and chemically stable, mechanically flexible and have remarkable selectivity at permeability that is three orders of magnitude higher than commercial polymeric membranes. This study demonstrates that controlled thermochemical reactions can delicately tune the topological structure of channels and pores within microporous polymers and their molecular sieving properties.

Date: 2014
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DOI: 10.1038/ncomms5813

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