Marcel Meta

Insights into Facile Methane Activation by a Spin Forbidden Reaction with Ta+ Ions in the Gas Phase The activation of methane (CH4) 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+ + CH4 → TaCH2+ + H2.

Dynamics of carbene formation in the reaction of methane with the tantalum cation in the gas phase† The controlled activation of methane has drawn significant attention throughout various disciplines over the last few decades. In gas-phase experiments, the use of model systems with reduced complexity compared to condensed-phase catalytic systems allows us to investigate the intrinsic reactivity of elementary reactions down to the atomic level.

Ta+ and Nb+ + CO2: intersystem crossing in ion–molecule reactions† The reactions of Ta+ and Nb+ with CO2 proceed only by a highly efficient oxygen atom transfer reaction to the respective oxide at room temperature in the gas phase. Although the product spin states are not determined, thermochemistry dictates that they must be different from ground state quintet Ta+ and Nb+, implying that intersystem crossing (ISC) has occurred.