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• W1989728470 endingPage "16599" @default.
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• W1989728470 abstract "Anodic oxidation of the important half-sandwich compound CoCp(CO)2, 1, has been studied under gentle electrolyte conditions, e.g., chlorinated hydrocarbons with weakly coordinating anion (WCA) supporting electrolyte anions. The 17-electron cation 1+ produced at E1/2(1) = 0.37 V vs FeCp20/+ undergoes a surprising reaction with neutral 1 to form the dimer radical cation [Co2Cp2(CO)4]+, 2+, which has a metal−metal bond unsupported by bridging ligands. The dimer radical is oxidized at a slightly more positive potential (E1/2 = 0.47 V) to the corresponding dication 22+. Observation of the oxidation of 2+ is without precedent in confirming a radical−substrate (R−S) dimerization process by direct voltammetric detection of the R−S intermediate, Keq = 3 × 104 M-1 for [2+]/[1][1+]. The R−S mechanism and the reaction products have been characterized by voltammetry, electrolysis, fiber-optic IR spectroscopy, and ESR measurements. DFT calculations indicate that removal of an electron from 1 results in rehybridization in 1+, thereby opening the metal center for interaction with the neutral compound 1, which has a relatively basic metal center. The LUMO of the dimer dication 22+ is metal−metal antibonding, and its half-occupancy in 2+ results in lengthening of the Co−Co bond from 2.64 Å to 3.14 Å. Inclusion of solvent in the (COSMO) calculations shows that solvation effects are necessary to account for the fact that E1/2(2) > E1/2(1). These results show the importance of medium effects in probing the fundamental redox chemistry of half-sandwich metal complexes." @default.
• W1989728470 created "2016-06-24" @default.
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• W1989728470 date "2006-12-01" @default.
• W1989728470 modified "2023-09-26" @default.
• W1989728470 title "Electrochemical Oxidation of CoCp(CO)₂: Radical−Substrate Reaction of a 17 e^-/18 e^- Pair and Production of a Unique Dimer Radical" @default.
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• W1989728470 doi "https://doi.org/10.1021/ja0653775" @default.
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