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Most molybdenum-containing enzymes catalze reactions which are formally oxygen atom transfer processes. The coordination enviorment of the Mo Sites are dominated by terminal oxo group. A number of the enzymatic reactions appear to involve conversions between dioxo-Mo(Ⅵ) and mono oxo-Mo(Ⅳ) forms. Synthetic model systems were sought which approximate the structural, spectroscopic, and reactivity properties of the enzymatic Mo Sites.