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4-Aminopyridinium tetrabromocadmate(II) monohydrate (1) crystallizes in the orthorhombic space group Pbcm with a = 6.876(2), b = 14.089(2), and c = 18.845(2) Å , Z = 4, T = 296 K. In the crystal structure, a [CdBr 4 ] 2−  anion, a 4-aminopyridinium cation, and a water molecule are alternately connected into chains by hydrogen bonds N-H···Br and O-H···Br. 2,3,5,6- Tetramethylpyrazinium tetrabromocadmate(II) (2) crystallizes in the orthorhombic space group P2 1 2 1 2 1  with a = 14.640(12), b = 15.615(7), c = 6.686(5) Å , Z = 4, T = 296 K. In the crystal structure, a [CdBr 4 ] 2−  anion and a 2,3,5,6-tetramethylpyrazinium cation are interconnected by bifurcated hydrogen bonds N-H· · ·2Br and form infinite chains.  81 Br NQR spectra with three lines with an intensity ratio of 1 : 1 : 2 (77 K ≤ T ≤ ca. 325 K) and four lines with an intensity ratio of 1 : 1 : 1 : 1 (77 K ≤ T ≤ ca. 330 K) were observed for crystalline 1 and 2, respectively, which are consistent with the crystal structure data. DSC measurements showed the existence of thermal anomalies at high temperatures in both 1 and 2.

Crystal Structure, NQR and DSC Studies of Tetrabromocadmates(II): [4-H 2 NC 5 H 4 NH] 2 CdBr 4 · H 2 O and [2,3,5,6-(CH 3 ) 4 C 4 N 2 H 2 ]CdBr 4