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Surface open polar sites within the voids of porous molecular crystals define the localized physicochemical environment for critical functions such as gas separation and molecular recognition. This study presents a new charge‐assisted hydrogen bonding (H‐bonding) motif, by exploiting inorganic ammonium (NH4+) cations as H‐bond donors, to regulate the assembly of C2‐symmetric carboxylic tectons for...
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