Iron catalyzed CO2 hydrogenation to formate enhanced by Lewis acid co-catalysts.

摘要: A family of iron(II) carbonyl hydride complexes supported by either a bifunctional PNP ligand containing secondary amine, or with tertiary amine that prevents metal–ligand cooperativity, were found to promote the catalytic hydrogenation CO2 formate in presence Bronsted base. In both cases remarkable enhancement activity was observed upon addition Lewis acid (LA) co-catalysts. For system, turnover numbers approximately 9000 for production achieved, while catalysts ligand, nearly 60 000 turnovers observed; highest reported an earth abundant catalyst date. The LA co-catalysts raise number more than order magnitude each case. mechanistic investigations implicated disrupting intramolecular hydrogen bond between N–H moiety and oxygen resting state. This destabilization iron-bound accelerates product extrusion, rate-limiting step catalysis. systems ligands it demonstrated originates from cation assisted substitution dihydrogen during slow