Efficient Room‐Temperature Activation of Methane by TaN+ under C−N Coupling. Issue 38 (11th August 2016)

• Record Type: Journal Article
• Authors: Zhou, Shaodong; Li, Jilai; Schlangen, Maria; Schwarz, Helmut
• Is Part Of: Angewandte Chemie international edition. Volume 55:Issue 38(2016)
• Page Start: 11678
• Page End: 11681
• Publication Date: 2016-08-11
• Subjects: C−N coupling -- gas-phase reactions -- methane activation -- quantum chemical calculations -- tantalum nitride; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.201606259
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: 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 : MeTa‐lated : Thermal activation of methane by [TaN] + under C−N coupling and formation of H2 was detected by mass spectrometry and confirmed by quantum chemical calculations. The lighter congeners [VN] + and [NbN] + are inert towards methane under the same conditions. (In the picture the signal labeled with "×" arises from reactions with background contaminants.)