Ionothermal reactions of uranyl salts in several ionic liquids containing cyclic cations produced single crystals of five new uranyl compounds. (C4H7N2)[(UO2)(AsO4)] (1), (C8H15N2)2[(UO2)4(SeO3)5] (2), (C6H11N2)2[(UO2)3(C2H5PO4)4] (3), and (C5H5N)2[(UO2)2(SeO4)3] (4) are each comprised of two-dimensional structural units. (C4H7N2)[(UO2)5(PO4)3(HPO4)(H2O)2]·3H2O (5) is composed of a three-dimensional network. While the uranyl structural units in all five compounds are directly related to ones found in either uranyl minerals or compounds produced in aqueous media, each contain cyclic ionic liquid constituents as charge-balancing agents. These results suggest that the cation selectivity of these structural units is low, even under various solvation conditions and templating effects from cyclic cations donated from ionic liquid media.
