Electrochemical Reoxidation Enables Continuous Methane-to-MethanolCatalysis with Aqueous Pt Salts

摘要

The direct conversion of methane to methanol would enable better utilization of abundant natural gas resources. In the presence of stoichiometric Pt^IV oxidants, Pt^II ions are capable of catalyzing this reaction in aqueous solutions at modest temperatures. Practical implementation of this chemistry requires a viable strategy for replacing or regenerating the expensive Pt^IV oxidant. Herein, we establish an electrochemical strategy for continuous regeneration of the Pt^IV oxidant to furnish overall electrochemical methane oxidation. We show that Cl-adsorbed Pt electrodes catalyze facile oxidation of Pt^II to Pt^IV at low overpotential without concomitant methanol oxidation. Exploiting this facile electrochemistry, we maintain the Pt^II/IV ratio during Pt^II-catalyzed methane oxidation via in situ monitoring of the solution potential coupled with dynamic modulation of the electric current. This approach leads to sustained methane oxidation catalysis with 70% selectivity for methanol.