Plasma-promoted reactions of the heterobimetallic anions CuNb− with dinitrogen and subsequent reactions with carbon dioxide: formation of C–N bonds

Abstract

The activation and functionalization of dinitrogen with carbon dioxide into useful chemicals containing C–N bonds are significant research projects but highly challenging. Herein, we report that N₂ molecules are dissociated by heterobimetallic CuNb⁻ anions assisted by surface plasma radiation, leading to the formation of CuNbN₂⁻ anions; the CuNbN₂⁻ anions can further react with CO₂ to generate products NCO⁻ with one C–N bond and NbO₂NCN⁻ with two C–N bonds under thermal collision conditions. For the activation of dinitrogen, the plasma atmosphere is conducive to the dissociation of the NN bond, which renders the coupling reactions of N₂ and CO₂ molecules easier to proceed. This is the first report of coupling of N₂ and CO₂ to generate C–N bonds by making good use of the plasma effect to assist in the activation of N₂ molecules. This new strategy with the assistance of plasma provides a practicable route to construct C–N bonds by directly using N₂ and CO₂ at room temperature.