Insights into facile methane activation by a spin forbidden reaction with Ta ions in the gas phase.

The activation of methane (CH) by transition-metal cations in the gas phase provides a model for understanding the impact of electronic spin on reactivity, with implications in single atom catalysis. In this work, we present a mixed quantum-classical trajectory surface hopping study on the nominally spin-forbidden reaction Ta + CH → TaCH + H. To facilitate the dynamics calculations, full twelve-dimensional PESs for three low-lying spin (quintet, triplet, and singlet) states are constructed using a machine learning method from density functional theory data.