Publication date: 10th April 2024
Methane (CH4) is a potent greenhouse gas. One potential solution to limit the emission of CH4 is to convert or upgrade it to value-added products. Oxidation of C-H bond in methane under mild conditions constitutes longstanding challenges which are of fundamental and technological importance, from biological and industrial to environmental. Earth’s atmosphere relies on free radicals to remove climate-damaging methane and other organic pollutants from the air. In recent decades, intensive efforts have been focused on leveraging free radicals for methane oxidation. Free radicals are one of key mediators underpinning many active sites in thermal catalysis and these enhancement effects induced by the light and electric fields. However, it remains unclear how free radicals as active species mediate the C-H bond activation in methane and dictate the products distribution.
In this talk, we will discuss our recent advances in photocatalytic oxidation of methane to methanol which combined rational design of photocatalysts, photocatalytic studies, as well as in-situ free radical detection. Our results unravel interactions between these free radicals and the solid co-catalysts, ions, and gases molecules in water, as well as their impact on methane removal and its selective oxidation. Our studies highlight the neglected while important interplay between photogenerated radicals and co-catalysts, ion impurities, and gas molecules in promoting methane removal and controlling the products distribution. Furthermore, we report an inherent trade-off in the photochemical methane to methanol conversion. A new design principle featuring isolating different reaction steps is developed to circumvent this trade-off.
Such molecular-level insights into photocatalysts and their interactions with free radicals are expected to promote the methane removal and its selective functionalization and offer informative design principles for chemical bonds activations that are driven by light, thermal catalysis, and electric fields.
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