Electrochemical oxidation of methanol on platinum and platin

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29 Formation and Decomposition of RPt(IV) in the Shilov System . . . . . . . . . . . . . 1 Conversion of RPt(II) to RPt(IV) . . . . . . . . . . . . . . . . . . . . . . . . . . 2 Formation of R–X from RPt(IV) . . . . . . . . . . . . . . . . . . . . . . . . . . . 35 3 Does C–H Activation in the Shilov System Involve Pt(IV) Intermediates? .

55 References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . A. E. A. E. Bercaw 1 Introduction Today, there are well-established examples of facile C–H bond activation by just about every transition metal in the periodic table, but the historical pride of precedence goes to platinum. The conversion of alkanes to alcohols by chloroplatinate salts, under what appeared at the time to be remarkably mild conditions, was first reported by Alexander Shilov and his coworkers around 1970.

C–C reductive elimination was also observed upon thermolysis of (i-Prnacnac) PtMe3 (1a) and (anim)PtMe3 (3) [83, 92]. 1(2) Â 10–5 s–1 measured for 1a and 3, respectively. Although the (i-Prnacnac)PtMe3 and (anim)PtMe3 complexes appear quite similar in their structures, the change in the electronics of the ligand backbone with the incorporation of an arene ring in the anim ligand results in almost an order of magnitude difference in their rate constants for reductive elimination. It had previously been difficult to make such direct comparisons concerning the key C–C bond-forming step as prior measurements of rate constants of reductive elimination from Pt(IV) involved contributions from the preliminary ligand dissociation step.

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