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Chemically Gradient Hydrogen‐Bonded Organic Framework Crystal Film

Hydrogen-bonded organic frameworks (HOFs) are ordered supramolecular solid structures, however, nothing much explored as centimeter-scale self-standing films. The fabrication of such crystals comprising self-supported films is challenging due to the limited flexibility and interaction of the crystals, and therefore studies on 2D macrostructures of HOFs are limited to external supports. Herein, we introduce a novel chemical gradient strategy to fabricate a crystal-deposited HOF film on an in-situ-formed COP-film (Tam-Bdca-CGHOF). The fabricated film showed versatility in chemical bonding along its thickness from covalent to hydrogen-bonded network. The kinetic-controlled Tam-Bdca-CGHOF showed enhanced proton conductivity (0.83 µS cm-1) compared to its rapid kinetic analogue, Tam-Bdca-COP (0.21 µS cm-1), which signifies the advantage of bonding-engineering in the same system.

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