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By dehydrating actinide salts with an ionic liquid containing a common anion and subsequent reaction with N-heterocyclic ligands, we challenge the concept that actinides prefer O- over N-donors; rather the acidic hydrogen atoms of protic solvents hinder the formation of more elusive f-element N-donor coordination complexes.

The ionic liquid (IL) 1-ethyl-3-methylimidazolium acetate was utilized as a liquid-state crystallization agent to form ionic co-crystals using amphoteric azoles selected as model compounds for active pharmaceutical ingredients. Weakly acidic azoles crystallize the IL relatively quickly, while stronger acidic azoles undergo slower ion exchange with the IL to form salts.