Complete cleavage of the N≡N triple bond by Ta₂N⁺ via degenerate ligand exchange at ambient temperature: A perfect catalytic cycle.

ABSTRACT: An unprecedented, spontaneous, and complete cleavage of the triple bond of N₂ in the thermal reaction of ¹⁵N₂ with Ta₂ ¹⁴N⁺ was observed experimentally by Fourier transform ion cyclotron resonance mass spectrometry; mechanistic aspects of the degenerate ligand exchange were addressed by high-level quantum chemical calculations. The "hidden" dis- and reassembly of N₂, mediated by Ta₂N⁺, constitutes a full catalytic cycle. A frontier orbital analysis reveals that the scission of the N₂ triple bond is essentially governed by the donation of d-electrons from the 2 metal centers into antibonding π*-orbitals of N₂ and by the concurrent migration of electrons from bonding π- an

SUBMITTER: Geng C 

PROVIDER: S-EPMC6815182 | biostudies-literature | 2019 Oct

REPOSITORIES: biostudies-literature