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The synthesis, infra-red, Raman and NMR spectra and crystal structure of 2, 4, 4-trimethyl-4, 5-dihydro-3H-benzo [b] [1,4] diazepin-1-ium tetrachlorocadmate, [C 12 H 17 N 2 ] 2 CdCl 4 and benzene-1,2-diaminium decachlorotricadmate(II) [C 6 H 10 N 2 ] 2 Cd 3 Cl 10 are reported.The [C 12 H 17 N 2 ] 2 CdCl 4 compound crystallizes in the triclinic system ( space group) with Z = 2 and the following unit cell dimensions: a = 9.6653(8) Å, b = 9.9081(9) Å, c = 15.3737(2) Å, α = 79.486(1)°, β = 88.610(8)° and γ = 77.550(7)°. The structure was solved by using 4439 independent reflections down to R value of 0.029. In crystal structure, the tetrachlorocadmiate anion is connected to two organic cations through N-H...Cl hydrogen bonds and van der Waals interaction as to build cation-anion-cation cohesion. The [C 6 H 10 N 2 ] 2 Cd 3 Cl 10 crystallizes in the triclinic system ( space group). The unit cell dimensions are a = 6.826 (5)Å, b = 9.861 (7)Å, c = 10.344 (3)Å, α = 103.50 (1)°, β = 96.34 (4)° and γ = 109.45 (3)°, Z = 2. The final R value is 0.053 (Rw = 0.128). Its crystal structure consists of organic cations and polymeric chains of [Cd 3 Cl 10 ] 4anions running along the [011] direction, in the [C 6 H 10 N 2 ] 2 Cd 3 Cl 10 compounds hydrogen bond interactions between the inorganic chains and the organic cations, contribute to the crystal packing.

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