Abstract
The mechanism of conversion of terminal alkynes RCCH to coordinated carbyne OsCCH2R by Os(H)2ClXL2 (L = PiPr3) has been studied for X = OTf and BArF4 (ArF = 3,5-di(CF3)2(C6H3). Ready loss of these X makes possible detection of η2-RCCH (4-electron donor) and CH(CH2R) intermediates, and D-labeling (RCCD) gives OsDClX(CCH2R)L2. The energy of various intermediates, including the only experimentally unobserved one, η2-vinyl, was evaluated with DFT(PBE) calculations.
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