Time-of-flight mass spectrometry and density functional theory were used to study the reactions of vanadium–silicon heteronuclear oxide cluster cations with methane. In their Full Paper on page 11463 ff., S.-G. He et al. demonstrate that the stoichiometric oxide clusters [V2O5(SiO2)1–4]+ and [(V2O5)2SiO2]+, which contain terminal-oxygen-centered radicals (Ot.) responsible for high CH activation, are able to activate methane under near-room-temperature conditions.