Room-Temperature Dinitrogen and Carbon Dioxide Activation
to Form Nitrogen–Carbon Bonds by Quaternary Cluster Anions:
Gold-Assisted Enhancement of Reactivity
posted on 2022-01-10, 13:34authored byYong-Qi Ding, Ying Li, Fei Ying, Ming Wang, Jia-Bi Ma
Coupling
conversion of CO2 and N2 molecules
under mild conditions to form useful N–C bond-containing products
has attracted significant attention. However, the activation and direct
coupling of such very inert molecules are quite challenging. Herein,
we determined that this coupling reaction can be realized by AuNbBO– quaternary anions at room temperature. The well-defined
AuNbBO– anions can cleave the NN bond in
N2 and two CO bonds in CO2 to form a
novel product NCNBO–. To the best of our knowledge,
the NCNBO– anion has been experimentally synthesized
for the first time by coupling N2 and CO2. Comparative
studies with Nb2BO–/N2 and
NbBO–/N2 systems further indicate that
the presence of a Au atom in AuNbBO– is indispensable
for this N2 and CO2 coupling reaction, because
the Au atom can decrease the active orbital energies of AuNbBO– anions to facilitate the π-back-donating interaction
between AuNbBO– and N2.