The influence of the pH on the synthesis of Zn(II) complexes derived from 1H-benzimidazol-2ylmethanamine (HL) has been investigated with X-ray crystallography, FAB mass spectrometry, NMR, infrared and Raman spectroscopy. The crystal structures of (1H-benzimidazol-2ylmethanamine)tetrachlorozincate( 2 -) dihydrogen [H 3 LZnCl 4 ] (2), (1H-benzimidazol-2ylmethanamine-κN 3 )trichlorozincate(1-) hydrogen hydrate [H 2 LZnCl 3 ]•H 2 O (3), (1Hbenzimidazol-2-ylmethanamine-κ 2 N 2 ,N 3 )dichlorozinc(II)

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... [HLZnCl 2 ] (4) and Bis[1Hbenzimidazol-2-ylmethanamine-k 2 N 2 ,N 3 ]chlorozinc(II) chloride hydrate [(HL) 2 ZnCl]Cl•H 2 O (5) are reported. Compounds 2-4 exhibit a distorted tetrahedral environment around the metal center. Complex 5 has distorted trigonal bipyramidal geometry. The crystalline structures of 2-5 show the presence of strong intermolecular hydrogen bond interactions that produces graph sets with pseudo-macrocyclic network. The NMR studies show the dynamic behavior of compounds 3-5 due to break-formation phenomena of N→Zn bonds.