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Creators/Authors contains: "Gardner, Evan J."

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  1. ; ; ; ; ; ; ; ( , Journal of the American Chemical Society)
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  2. ; ; ; ; ; ; ( , Angewandte Chemie)
    Abstract

    Low‐temperature reaction of the tris(pyrazolyl)borate copper(II) hydroxide [iPr2TpCu]2(μ‐OH)2with triphenylsilane under a dinitrogen atmosphere gives the bridging dinitrogen complex [iPr2TpCu]2(μ‐1,2‐N2) (3). X‐ray crystallography reveals an only slightly activated N2ligand (N‐N: 1.111(6) Å) that bridges between two monovalentiPr2TpCu fragments. While DFT studies of mono‐ and dinuclear copper dinitrogen complexes suggest weak π‐backbonding between the d10CuIcenters and the N2ligand, they reveal a degree of cooperativity in the dinuclear Cu‐N2‐Cu interaction. Addition of MeCN, CNAr2,6‐Me, or O2to3releases N2with formation ofiPr2TpCu(L) (L=NCMe, CNAr2,6‐Me2) or [iPr2TpCu]2(μ‐η2:η2‐O2) (1). Addition of triphenylsilane to [iPr2TpCu]2(μ‐OH)2in pentane allows isolation of a key intermediate [iPr2TpCu]2(μ‐H) (5). Although5thermally decays under N2to give3, it reduces unsaturated substrates, such as CO and HC≡CPh to HC(O)H and H2C=CHPh, respectively.

     
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