Room-Temperature Dinitrogen and Carbon Dioxide Activation to Form Nitrogen-Carbon Bonds by Quaternary Cluster Anions: Gold-Assisted Enhancement of Reactivity

Yong-Qi Ding; Ying Li; Fei Ying; Ming Wang; Jia-Bi Ma

doi:10.1021/acs.jpclett.1c03774

Room-Temperature Dinitrogen and Carbon Dioxide Activation to Form Nitrogen-Carbon Bonds by Quaternary Cluster Anions: Gold-Assisted Enhancement of Reactivity

J Phys Chem Lett. 2022 Jan 20;13(2):492-497. doi: 10.1021/acs.jpclett.1c03774. Epub 2022 Jan 10.

Authors

Yong-Qi Ding¹, Ying Li¹, Fei Ying¹, Ming Wang¹, Jia-Bi Ma¹

Affiliation

¹ Key Laboratory of Cluster Science of Ministry of Education, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, Key Laboratory of Cluster Science of Ministry of Education, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 102488, China.

PMID: 35001630
DOI: 10.1021/acs.jpclett.1c03774

Abstract

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 N≡N bond in N₂ and two C═O 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.