Ruthenium-catalyzed reduction of carbon dioxide to formaldehyde

Sébastien Bontemps (1) , Laure Vendier (1) , Sylviane Sabo-Etienne (1)

1 LCC - Laboratoire de chimie de coordination

Functionalization of CO2 is a challenging goal and precedents exist for the generation of HCOOH, CO, CH3OH, and CH4 in mild conditions. In this series, CH2O, a very reactive molecule, remains an elementary C1 building block to be observed. Herein we report the direct observation of free formaldehyde from the borane reduction of CO2 catalyzed by a polyhydride ruthenium complex. Guided by mechanistic studies, we disclose the selective trapping of formaldehyde by in situ condensation with a primary amine into the corresponding imine in very mild conditions. Subsequent hydrolysis into amine and a formalin solution demonstrates for the first time that CO2 can be used as a C1 feedstock to produce formaldehyde.

Mots clés: Redox reactions; Aldehydes; Precursors; Catalysts; Catalytic reactions

Domaines: Chimie de coordination; Catalyse

Sébastien Bontemps, Laure Vendier, Sylviane Sabo-Etienne. Ruthenium-catalyzed reduction of carbon dioxide to formaldehyde. Journal of the American Chemical Society, 2014, 136 (11), pp.4419-4425. ⟨10.1021/ja500708w⟩. ⟨hal-00990999⟩