Four Mn(NCS)2 based compounds of the types [Mn(SCN)2(L1)]·EtOH (1), [Mn(SCN)2(L2)]·½EtOH (2), [Mn(SCN)2(L3)] (3), and [Mn(SCN)2(L4)2]n·3nMeCN (4) [L1 = benzilbis((pyridin‐2‐yl)methylidenehydrazone), L2 = benzilbis((acetylpyridin‐2‐yl)methylidenehydrazone, L3 = benzilbis((phenylpyridin‐2‐yl)methylidenehydrazone, and L4 = benzilbis((pyridin‐3‐yl)methylidenehydrazone)] were synthesized and characterized by single‐crystal X‐ray diffraction studies, elemental analysis, and IR spectroscopy. The first three complexes of general formula Mn(SCN)2(L1–3) consist of discrete units, whereas the fourth one consists of one‐dimensional coordination polymer. The central metal atoms in 1–4 exhibit a distorted octahedral arrangement.
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