title: Reducing CO₂ to methanol using frustrated Lewis pairs: on the mechanism of phosphine-borane-mediated hydroboration of CO₂.
abstract: The full mechanism of the hydroboration of CO2 by the highly active ambiphilic organocatalyst 1-Bcat-2-PPh2-C6H4 (Bcat = catecholboryl) was determined using computational and experimental methods. The intramolecular Lewis pair was shown to be involved in every step of the stepwise reduction. In contrast to traditional frustrated Lewis pair systems, the lack of steric hindrance around the Lewis basic fragment allows activation of the reducing agent while moderate Lewis acidity/basicity at the active centers promotes catalysis by releasing the reduction products. Simultaneous activation of both the reducing agent and carbon dioxide is the key to efficient catalysis in every reduction step.
authors.affiliation: Département de Chimie, Centre de de Catalyse et Chimie Verte (C3V), Université Laval , 1045 Avenue de la Médecine, Québec, QC, Canada G1V 0A6.
authors.forename: Marc-André
authors.initials: MA
authors.lastname: Courtemanche
authors.forename: Marc-André
authors.initials: MA
authors.lastname: Légaré
authors.forename: Laurent
authors.initials: L
authors.lastname: Maron
authors.forename: Frédéric-Georges
authors.initials: FG
authors.lastname: Fontaine