Two flexible porous coordination materials, [Mn(pybimc) 2 ]·2H 2 O·G (G = toluene, 1 tol ; THF, 1 thf ), where pybimc = 2-(2′-pyridyl)-benzimidazole-5-carboxylate, featuring identical one-dimensional chain structure have been characterized. Guest exchange studies have exhibited that 1 tol cannot be converted to 1 thf through direct replacement of guest toluene molecules by THF molecules, but, of particular interest, 1 thf is actually converted to 1 tol and 1 aromatic (where aromatic = o-, m-, p-xylene) upon the exchange of THF to toluene and other aromatic molecules, respectively. This signifies a single-crystal to single-crystal transformation accompanied irreversible crystal expansion. In-depth analyses reveal that the nature of the weak yet sufficiently strong framework−guest C−H···π interactions, rather than the guest size, observed in this system plays a key role in guiding the adsorption of liquid-phase aromatics in the soft crystalline materials.
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