AbstractUnlike most crystallizable polymers, some polyalkylbenzimidazoles do not crystallize when pure but do crystallize with ionized solvent molecules to produce solid stoichiometrical, solvated crystals. The polymer–solvent interaction is strongly exothermic, and a crosslinked polymer swells in the solvent over hundredfold. This leads to a negative χ1 value for the system. The cocrystallization with stoichiometric amounts of ionized solvent cannot be examined on the assumption that it is a polyelectrolyte gel since ion mobility is precluded. It also cannot be treated according to the corresponding states theory since the latter does not allow for negative χ1. A theoritical derivation, originating from Flory's semiflexible chain treatment, apparently predicts and explains the behavior of the polyalkylbenzimidazole–solvent s
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