O-atom-transfer oxidation of [molybdenum(IV) oxo{3,6-(acylamino)2- 1,2-benzenedithiolato}2]2- promoted by intramolecular NH...S hydrogen bonds |
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Authors: | Baba Koji Okamura Taka-aki Suzuki Chie Yamamoto Hitoshi Yamamoto Tetsuo Ohama Mitsuo Ueyama Norikazu |
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Institution: | Chemical Analysis Research Center, National Institute for Agro-Environmental Sciences, Tsukuba, Ibaraki 305-8604, Japan. |
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Abstract: | Novel molybdenum dithiolene compounds having neighboring amide groups as models for molybdoenzymes, (NEt(4))(2)Mo(IV)O{1,2-S(2)-3,6-(RCONH)(2)C(6)H(2)}(2)] (R = CH(3), CF(3), t-Bu, Ph(3)C), were designed and synthesized. The contributions of the NH...S hydrogen bond to the electrochemical properties of the metal ion and the reactivity of the O-atom-transfer reaction were investigated by a comparison with Mo(IV)O(1,2-S(2)C(6)H(4))(2)](2)(-). The MoOS(4) core of Mo(IV)O{1,2-S(2)-3,6-(CH(3)CONH)(2)C(6)H(2)}(2)](2)(-) shows no significant geometrical difference from that of Mo(IV)O(1,2-S(2)C(6)H(4))(2)](2)(-) in the crystal. The hydrogen bonds positively shifted the Mo(IV/V) redox potential and accelerated the reduction of Me(3)NO. |
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