Amine‐templated zinc sulfates of the formulae, [Zn(SO 4 )(H 2 O) 2 (C 10 N 2 H 8 )] ( I ) and [C 3 N 2 H 12 ][Zn(SO 4 )] ( II ) both with linear structures have been prepared under hydro/solvothermal conditions. Of these, I has the chain structure formed by ZnO 4 N 2 octahedra and SO 4 tetrahedra, while II comprises ladders formed by corner‐sharing four‐membered rings. Amine‐templated thorium sulfates of the formula [HN(CH 2 ) 6 NH] 2 [Th 2 (SO 4 ) 6 (H 2 O) 2 ]·2H 2 O, ( III ) and [H 2 N(CH 2 ) 4 NH 2 ][Th 3 (SO 4 ) 7 (H 2 O) 4 ]·5H 2 O ( IV ) are also obtained under hydrothermal conditions. III has a sheet structure consisting of cages whereas IV has a two‐dimensional structure derived from the connectivity of ladders.
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