Conversion of carbon dioxide to a novel molecule NCNBO− mediated by NbBN2− anions at room temperature

Abstract

The activation of carbon dioxide (CO₂) mediated by NbBN₂⁻ cluster anions under the conditions of thermal collision has been investigated by time-of-flight mass spectrometry combined with density functional theory calculations. Two CO double bonds in the CO₂ molecule are completely broken and two C–N bonds are further generated to form the novel molecule NCNBO⁻. To the best of our knowledge, this new molecule is synthesized and reported for the first time. In addition, one oxygen atom transfer channel produces another product, NbBN₂O⁻. Both of the Nb and B atoms in NbBN₂⁻ donate electrons to reduce CO₂, and the carbon atom originating from CO₂ serves as an electron reservoir. The reaction of NbB⁻ with N₂ was also investigated theoretically, and the formation of NbBN₂⁻ from this reaction is thermodynamically and kinetically quite favorable, indicating that NCNBO⁻ might be produced from the coupling of N₂ and CO₂ mediated by NbB⁻ anions.