Issue 32, 2022

Mutual functionalization of dinitrogen and methane mediated by heteronuclear metal cluster anions CoTaC2

Abstract

The direct coupling of dinitrogen (N2) and methane (CH4) to construct the N–C bond is a fascinating but challenging approach for the energy-saving synthesis of N-containing organic compounds. Herein we identified a likely reaction pathway for N–C coupling from N2 and CH4 mediated by heteronuclear metal cluster anions CoTaC2, which starts with the dissociative adsorption of N2 on CoTaC2 to generate a Taδ+–Ntδ (terminal-nitrogen) Lewis acid–base pair (LABP), followed by the further activation of CH4 by CoTaC2N2 to construct the N–C bond. The N[triple bond, length as m-dash]N cleavage by CoTaC2 affording two N atoms with strong charge buffering ability plays a key part, which facilitates the H3C–H cleavage via the LABP mechanism and the N–C formation via a CH3 migration mechanism. A novel Nt triggering strategy to couple N2 and CH4 molecules using metal clusters was accordingly proposed, which provides a new idea for the direct synthesis of N-containing compounds.

Graphical abstract: Mutual functionalization of dinitrogen and methane mediated by heteronuclear metal cluster anions CoTaC2−

Supplementary files

Article information

Article type
Edge Article
Submitted
29 Apr 2022
Accepted
13 Jul 2022
First published
14 Jul 2022
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2022,13, 9366-9372

Mutual functionalization of dinitrogen and methane mediated by heteronuclear metal cluster anions CoTaC2

L. Mou, Y. Li, G. Wei, Z. Li, Q. Liu, H. Chen and S. He, Chem. Sci., 2022, 13, 9366 DOI: 10.1039/D2SC02416K

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