(329h) Concerted Methane Fixation at Ambient Temperature and Pressure Mediated By an Enzymatic and Fe-ZSM-5 Catalytic Couple

Anthropogenic methane emissions to the atmosphere pose a technological challenge for conversion into commodity chemicals due to their diffuse and dilute nature. However, the low temperature and concentration of these emission streams make them challenging to address by current routes of methane oxidation, which rely on high temperatures or pressures to drive methane oxidation rapidly and efficiently. Herein, we introduce a novel tandem catalytic system of alcohol oxidase with an iron-modified ZSM-5 that operates as a synthetic methanotrophic system capable of partially oxidizing methane at ambient temperatures and pressures, producing chemically useful intermediates for material synthesis. We show that the methane-to-formaldehyde selectivity can exceed 90% at room temperature. The generated formaldehyde intermediate can be rapidly incorporated into a growing urea polymer, with a material growth rate exceeding 5.0 mg g_cat^-1 hr^-1, commensurate and even exceeding rates for many cultured methanotrophic bacteria systems. Strategies to enhance the stability of this tandem catalysis and technical analysis for future application scenarios will be discussed.