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Six novel uranyl nitrate compounds K3[(UO2)(NO3)Cl3](NO3) (1, 2), α-Cs2[(UO2)(NO3)Cl3] (3), [(UO2)(NO3)2(H2O)2][(CH3NH3)2(NO3)2] (4), Cs2[(UO2)(NO3)4] (5), and [(UO2)2(OH)2(NO3)2(H2O)3](H2O) (6) have been prepared from aqueous solutions. Their structures were analyzed using single-crystal X-ray diffraction technique. Structural studies have shown that the crystals of 1 and 2 are isotypic but differ in the distortion at the counter ion’s sites. The crystal of 3 is a low-temperature polymorph modification of the recently studied compound. The crystal structure of 4 is composed of uranyl-dinitrate-dihydrate and methylamine-nitrate electroneutral complexes linked through the system of H-bonds. The crystal structure of 5 is based on the finite [(UO2)(NO3)4]2− clusters that are arranged in pseudo-chained complexes extended along [100] and are arranged according to a hexagonal packing or rods. The crystal of 6 is also a novel polymorph modification of previously studied compound, the structure of which is based on the very rare topological type of the finite clusters. Nowadays, uranyl nitrate finite clusters of nine various topological types are known. We give herein a short review of their topological features and relationships. Crystallization of uranyl nitrates usually occurs when all other competitive anions in the system have already formed crystalline phases, or the reaction of reagents have slowed down or even stopped. Thus it is suggested that crystallization of uranyl nitrates can be used as a key indicator of the reaction progress, which points to the necessity of the initial concentrations of reagents correction, or to the replacement of reagents and adjustment of the thermodynamic (P,T) parameters of the synthesis.

Uranyl Nitrates: By-Products of the Synthetic Experiments or Key Indicators of the Reaction Progress?