Abstract
A new synthetic method using [MoIV(S‐tBu)4], 1,2‐benzenedithiol containing bulky hydrophobic acylamino substituents, 3,6‐[(4‐tBuC6H4)3CCONH]2C6H2‐1,2‐(SH)2 (LH2), a tertiary amine [R3N = Et3N or 2,6‐lutidine (Lu)], and an equimolar amount of water afforded (R3NH)2[MoIVO(L)2] [(R3NH)2[1]]. Each compound formed a strong NH+···O=Mo hydrogen bond between the tertiary ammonium cation and the terminal oxo ligand in toluene, which unexpectedly promoted the one‐electron oxidation of MoIV by lutidinium ion or 0.5 equiv. Me3NO to produce [MoVO(L)2]–. In contrast, in polar solvents, typical oxygen atom transfer (OAT) from Me3NO to [1]2– was observed. A possible mechanism is presented and the role of the hydrogen bond in molybdenum enzymes is discussed.
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