High-Yield Methane to Methanol Conversion at Mild Conditions by Tailoring Methane Activation and Methanol Extraction

The direct conversion of methane to methanol at mild conditions is a pathway to utilize methane and form a value-added fuel like methanol over distributed scales, unlike conventional industrial methane reforming processes that require high temperature and pressure. However, over-oxidation of methanol limits the maximum methanol yield, energy efficiency, and scalability of the process. For the first time, we show how molecular excitations and reaction timescales can be tailored in thermal non-equilibrium to break this limit. We show how reaction pathways can be engineered to form preferential intermediates that restrict the generation of unwanted byproducts. We combine these excitations with synergistic transport timescales that control accumulation and extraction of methanol to extend high methanol selectivity (> 30%) to high methane conversion (> 50%). We use these methods to demonstrate the highest methanol yield (> 20%) reported via single-step methane conversion at near-atmospheric conditions. We generalize these advances using process descriptors to demonstrate a pathway to scalable and energy-efficient methanol synthesis in mild conditions using electrical energy.