| Abstract: | In this work, a pincer‐type complex [Cp*Ir‐(SNPh)(SNHPh)(C2B10H9)] ( 2 ) was synthesized and its reactivity studied in detail. Interestingly, molecular hydrogen can induce the transformation between the metalloradical [Cp*Ir‐(SNPh)2(C2B10H9)] ( 5 .) and 2 . A mixed‐valence complex, [(Cp*Ir)2‐(SNPh)2(C2B10H8)] ( 7 .+), was also synthesized by one‐electron oxidation. Studies show that 7 .+ is fully delocalized, possessing a four‐centered‐one‐electron (S‐Ir‐Ir‐S) bonding interaction. DFT calculations were also in good agreement with the experimental results. |
