Catalytic Metal-Free Deoxygenation of Nitrous Oxide with Disilanes

Abstract

Because of its high kinetic stability, conditions to reduce the greenhouse gas N2O are limited; therefore, a better understanding of N2O chemistry and N–O bond cleavage is required. In this work, N2O was deoxygenated under metal-free conditions. Using disilanes as reducing agents and a catalytic amount of fluoride anions or alkoxides allowed a mild reduction at ambient pressure and temperature. DFT calculations unveiled the mechanism, which shows a nucleophilic addition of a silyl anion to the central N atom of N2O and release of N2 from a pseudo-Brook rearrangement.