Efficient Room-Temperature Activation of Methane by TaN+ under C−N Coupling.

The thermal reaction of diatomic tantalum nitride cation [TaN]+ with methane has been explored using FT-ICR mass spectrometry complemented by high-level quantum chemical calculation; based on this combined experimental/computational approach, mechanistic aspects of this novel, highly efficient C−N coupling process have been uncovered. In distinct contrast to [TaN]+, its lighter congeners [VN]+ and [NbN]+ are inert towards methane under ambient conditions, and the origins of the remarkably variable efficiencies of the three metal nitrides are uncovered by CCSD(T) calculations. [ABSTRACT FROM AUTHOR]