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Iridium-, Ruthenium-, and Nickel-Catalyzed C–C Couplings of Methanol, Formaldehyde, and Ethanol with π-Unsaturated Pronucleophiles via Hydrogen Transfer

Cole C. Meyer, Michael J. Krische

2022The Journal of Organic Chemistry32 citationsDOIOpen Access PDF

Abstract

In this Perspective, the use of methanol and ethanol as C1 and C2 feedstocks in metal-catalyzed C-C couplings to π-unsaturated pronucleophiles via hydrogen auto-transfer is surveyed. In these processes, alcohol oxidation to form an aldehyde electrophile is balanced by reduction of an π-unsaturated hydrocarbon to form a transient organometallic nucleophile. Mechanistically related reductive couplings of paraformaldehyde mediated by alcohol reductants or formic acid also are described. These processes encompass the first catalytic enantioselective C-C couplings of methanol and ethanol and, more broadly, illustrate how the native reducing ability of alcohols enable the departure from premetalated reagents in carbonyl addition.

Topics & Concepts

FormaldehydeRutheniumCatalysisMethanolIridiumNickelEthanolChemistryTransfer hydrogenationHydrogenOrganic chemistryAsymmetric Hydrogenation and CatalysisCarbon dioxide utilization in catalysisCatalysis for Biomass Conversion
Iridium-, Ruthenium-, and Nickel-Catalyzed C–C Couplings of Methanol, Formaldehyde, and Ethanol with π-Unsaturated Pronucleophiles via Hydrogen Transfer | Litcius