The abundance of methane and its low cost makes it an attractive raw material for chemical precursors and energy-dense fuels. Conventional synthesis of methanol from synthesis gas involve a multistep process, which requires high energy input and high cost. The electrochemical oxidation of methane offers an interesting option for a single-step approach to the direct conversion of methane to methanol at low temperatures and cost. To date, a variety of the catalysts, including various supported metals and metal oxides (V2O5, Fe2O3, CoO, Mn2O3, MoO3, CrO), have been tested in electrochemical cells and shown promise for this approach [2]. However, further systematic studies are essential to understand the mechanism of methane oxidation and thereby guide the rational design of catalysts. In this regard supported single-atom catalysts are particularly interesting. These catalysts are ideal model catalysts to identify active sites and contribute to understanding the reaction process at a molecular level. However, in spite of great interest, it remains challenging to achieve atomically dispersed metals in high loadings for efficient catalysis. In this presentation, we will describe the preparation of MOF-derived, supported Fe and Cu single-atom catalysts. Metal containing MOFs were synthesized and subsequently pyrolyzed, yielding carbon-supported dispersed single-site catalyst. These catalysts were characterized for electrochemical oxidation of methane to methanol. Structural and chemical analyses of these catalysts using a combination of various microscopic and spectroscopic techniques were used to establish structure/property relationship. The insights gained from this work provide a valuable basis for developing a scientifically-guided approach towards the design of supported single-atom catalysts for the electrochemical oxidation of methane to

Design of single-site transition metal catalysts for electrochemical oxidation of methane to methanol

2019 Fall National Meeting

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