Cu-ion exchanged CHA zeolites that contain detectable quantities of ZCuOH activate molecular O2 to form CuxOy species active for partial methane oxidation (PMO), nitrogen oxide decomposition, and carbon monoxide oxidation. Temporally-resolved resonance Raman spectroscopy (λex = 532 nm) evinces the genesis of reactive CuxOy species that form at ZCuOH sites via the activation of O2. The population of these Raman-active species correlate strongly with increases in the yield of methanol from stoichiometric PMO, whereas, rates of the bulk oxidation of Cu(I) to Cu(II) proceed significantly faster as observed with X-ray absorption spectroscopy. These kinetic comparisons suggest that kinetically-relevant structural rearrangements (and O-O bond rupture) determine formation rates of the CuxOy complex responsible for methanol formation and that rates of Cu(I) oxidation do not correspond to the formation of the reactive intermediate.