The controlled generation of hydrogen sulfide (HS) under biologically relevant conditions is of paramount importance due to therapeutic interests. Via exploring the reactivity of a structurally characterized phenolate-bridged dinuclear zinc(II)-aqua complex {Zn(OH)}(ClO) () as a hydrolase model, we illustrate in this report that complex readily hydrolyses CS in the presence of EtN to afford HS. In contrast, penta-coordinated [Zn] sites in dinuclear {(Zn)(μ-X)}(ClO) complexes (, X = OAc; , X = dimethylpyrazolyl) do not mediate CS hydrolysis in the presence of externally added water and EtN presumably due to the unavailability of a coordination site for water at the [Zn] centers. Moreover, [Zn]-OH sites present in the isolated tetranuclear zinc(II) complex {(Zn)(μ-OH)}(ClO) () react with CS, thereby suggesting that the [Zn]-OH site serves as the active nucleophile. Furthermore, mass spectrometric analyses on the reaction mixture consisting of /EtN and CS suggest the involvement of zinc(II)-thiocarbonate () and COS species, thereby providing mechanistic insights into CS hydrolysis mediated by the dinuclear [Zn] hydrolase model complex .
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