The conversion of dinitrogen to more useful and reactive molecules has been the focus of intense research by chemists. In contrast to reductive N2 fixation, direct oxidation of N2 by O2 to nitric oxide under mild conditions via a thermochemical process is extremely challenging. Herein, we report the first example of N2 and O2 activation and coupling under thermochemical conditions through the remarkable ability of Y2BO+ to react with one N2 and two O2 molecules.

Plausible mechanisms for reactions of the ionized O-3 with N-2 are studied by DFT and electron correlation methods. Calculations show that formation of the primary products O-2(+) + N2O and N2O+ + O-2 arises from an intermediate [O-2...ON2](+) in the ground state and its charge-transfer excited state, respectively. New routes to NO2 + NO+ through an intermediate [ON2...O-2](+) and to [ON...NO](+) + O-2 via the reactions of O-3(+) with N2O are proposed.