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Journal Article
Research Support, Non-U.S. Gov't
CO-Reduction Chemistry: Reaction of a CO-Derived Formylhydridoborate with Carbon Monoxide, with Carbon Dioxide, and with Dihydrogen.
Journal of the American Chemical Society 2017 May 11
Treatment of the bulky metallocene hydride Cp*2 Zr(H)OMes (Cp* = pentamethylcyclopentadienyl, Mes = mesityl) with Piers' borane [HB(C6 F5 )2 ] and carbon monoxide (CO) gave the formylhydridoborate complex [Zr]-O═CH-BH(C6 F5 )2 ([Zr] = Cp*2 Zr-OMes). From the dynamic NMR behavior, its endergonic equilibration with the [Zr]-O-CH2 -B(C6 F5 )2 isomer was deduced, which showed typical reactions of an oxygen/boron frustrated Lewis pair. It was trapped with CO to give an O-[Zr] bonded borata-β-lactone. Trapping with carbon dioxide (CO2 ) gave the respective O-[Zr] bonded cyclic boratacarbonate product. These reaction pathways were analyzed by density functional theory calculation. The formylhydridoborate complex was further reduced by dihydrogen via two steps; it reacted rapidly with H2 to give Cp*2 Zr(OH)OMes and H3 C-B(C6 F5 )2 , which then slowly reacted further with H2 to eventually give [Zr]-O(H)-B(H)(C6 F5 )2 and methane (CH4 ). Most complexes were characterized by X-ray diffraction.
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