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The coordinatively unsaturated gold(iii) chelate complex [(C^N-CH)Au(C 6 F 5 )] + ( 1  + ) reacts with main group hydrides H-BPin and H-SiEt 3 in dichloromethane solution at -70 °C to form the corresponding σ-complexes, which were spectroscopically characterized (C^N-CH = 2-(C 6 H 3 Bu  t  )-6-(C 6 H 4 Bu  t  )pyridine anion; Pin = OCMe 2 CMe 2 O). In the presence of an external base such as diethyl ether, heterolytic cleavage of the silane H-Si bond leads to the gold hydrides [{(C^N-CH)AuC 6 F 5 } 2 (μ-H)] + ( 2  + ) and (C^N-CH)AuH(C 6 F 5 ) ( 5 ), together with spectroscopically detected [Et 3 Si-OEt 2 ] + . The activation of dihydrogen also involves heterolytic H-H bond cleavage but requires a higher temperature (-20 °C). H 2 activation proceeds in two mechanistically distinct steps: the first leading to 2 plus [H(OEt 2 ) 2 ] + , the second to protonation of one of the C^N pyridine ligands and reductive elimination of C 6 F 5 H. By comparison, formation of gold hydrides by cleavage of suitably activated C-H bonds is very much more facile; e.g. the reaction of 1·OEt 2  with Hantzsch ester is essentially instantaneous and quantitative at -30 °C. This is the first experimental observation of species involved in the initial steps of gold catalyzed hydroboration, hydrosilylation and hydrogenation and the first demonstration of the ability of organic C-H bonds to act as hydride donors towards gold.

Heterolytic bond activation at gold: evidence for gold(iii) H–B, H–Si complexes, H–H and H–C cleavage