Abstract
A self-assembling, biporous covalent organic framework has been constructed from a single monomer and applied to gas separations. Coordination of transition metals in the monomer leads to highly ordered arrangements of metals in the 2D-materials.
Highlights
We report a unique synthesis of a nanoporous two-dimensional covalent organic framework (COF) from a single self-assembling monomer
We demonstrate the synthetic flexibility of the material by coordination of various transition metals into the framework and its application as a membrane for degasification and gas separation
Density functional theory (DFT) and molecular mechanics (MM) calculations were used to inform the computational construction of material models, allowing for the interpretation of pXRD data to elucidate the crystallographic structure of the novel materials, including the revelation that disordered monomer vacancies are likely present in the material
Summary
In the past decade there has been increasing interest in covalent two-dimensional organic frameworks (2D-COFs) due to their synthetic flexibility and highly ordered porous structures.[1,2,3] These polymers have enormous potential in the areas of separations,[4,5,6,7] gas storage,[8] energy storage,[9,10,11] and catalysis.[12,13,14] Schiff-base chemistry, i.e. the formation of imine bonds by reaction of an aldehyde or ketone with a primary amine, is one of the primary methods of COF formation.[2,15] These reactions are centered on the judicious selection of two or more building blocks that, under appropriate reaction conditions, can reversibly form strong covalent linkages to produce highly ordered materials. The novel 2D-COF (DPCOF) contains two chemically distinct nanopores, one that can coordinate transition metals and a second more unreactive pore that is approximately the size of small gas molecules.
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