Disclosed is an electrochemical method for continuous regeneration of a PtIV oxidant to furnish overall electrochemical methane oxidation. Cl-adsorbed Pt electrodes catalyze facile oxidation of PtII to PtIV without concomitant methanol oxidation. Exploiting this electrochemistry, the PtII/IV ratio in solution is maintained via in situ monitoring of the solution potential coupled with dynamic modulation of the electric current. Remarkably, this method leads to sustained methane oxidation catalysis with ˜70% selectivity for methanol.