Renewable Energy-driven Oxidation of Methane to Value-added Products

Abstract

Methane, as the primary component of natural gas, is an abundant but chemically inert molecule that represents both a challenge and an opportunity in modern catalysis. Recent advances in renewable electricity generation, notably from solar, wind, and hydroelectric sources, have accelerated the transition of electricity to chemicals. This progress provides a compelling rationale for developing electricity-driven catalytic processes that can be operated under ambient conditions, aiming to convert methane using electrons rather than high-temperature thermal energy. Such novel electrochemical approaches enable precise modulation of reaction potentials, interfacial energetics, and reactive intermediate formation, thereby offering a controllable and sustainable pathway for methane oxidation.

However, the most critical challenge in methane oxidation reaction lies in the activation of methane molecule. Its high C–H bond dissociation energy, highly symmetric and nonpolar molecular structure, restrain the efficient activation and selectively conversion of methane under mild conditions, and often leading to overoxidation into CO2 or undesired by-products. Overcoming this kinetic and thermodynamic barrier is therefore a central issue for realizing the direct conversion of methane into value-added chemicals. Designing an efficient strategy to achieve selectively methane conversion under ambient conditions remains one of the most demanding goals in catalysis, and often regarded as the “Holy Grail” of catalytic chemistry.

This thesis focuses on the development of renewable electricity–driven electrocatalytic systems for the selective oxidation of methane under ambient conditions.