Publication date: 11th July 2022
Synthetic two-dimensional polymers (2DPs) are an emerging class of structurally-defined crystalline materials that comprise covalent networks with topologically planar repeat units. Yet, synthesizing 2DP single crystals via irreversible reactions remains challenging. Herein, utilizing the surfactant-monolayer-assisted interfacial synthesis (SMAIS) method, few-layer, large-area, skeleton-charged 2DP (C2DP) single crystals were successfully synthesized through irreversible Katritzky reaction, under pH control. The resultant periodically ordered 2DPs comprise aromatic pyridinium cations and counter BF4- anions. The representative C2DP-Por crystals display a tunable thickness of 2-30 nm and a lateral size up to 120 μm2. Using imaging and diffraction methods, a highly uniform square-patterned structure with the in-plane lattice of a = b = 30.5 Å was resolved with near-atomic precision. Significantly, the C2DP-Por crystals with cationic polymer skeleton and columnar-like pore arrays offer a high chloride ion selectivity with a coefficient up to 0.9, thus ensuring the integration as the anion-selective membrane for the osmotic energy generation. Our studies reveal a route to synthesize 2DP single crystals using a kinetically controlled irreversible reaction and will propel the development of membrane-based energy-conversion technologies.
This work was financially supported by the EU Graphene Flagship (GrapheneCore3, no. 881603), an ERC starting grant (FC2DMOF, grant no. 852909), an ERC Consolidator Grant (T2DCP), a DFG project (2D polyanilines, no. 426572620), Coordination Networks: Building Blocks for Functional Systems (SPP 1928, COORNET), H2020-MSCA-ITN (ULTIMATE, no. 813036), H2020-FETOPEN (PROGENY, 899205), CRC 1415 (Chemistry of Synthetic Two-Dimensional Materials, no. 417590517), SPP 2244 (2DMP), as well as the German Science Council and Center of Advancing Electronics Dresden.
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