Electrocatalysis of hydrocarbons to selectively produce alcohols has the potential to transform the manufacturing of chemicals and consumer goods in a sustainable way by replacing existing fossil-fuel-based processes by energy-saving successor technologies that utilize renewable energy. Selective hydrocarbon oxidations to alcohols have the ultimate goal of gas-to-liquid conversion of methane to methanol without energy-intensive steam reforming. Better catalysts, reaction control, and understanding of electrocatalytic processes are needed to achieve high selectivity for single non-overoxidized products at high activity. We developed earth-abundant mixed-metal (hydr)oxide nanocatalysts that were synthesized by pulsed laser in liquids synthesis, a technique that offers several advantages over conventional nanomaterials preparation methods: Laser-made nanocatalysts are intrinsically more active; mixed-metal and metastable nanomaterials, especially oxides, are easily accessible; resulting nanomaterials have uniform and independently controlled properties; no surfactants are necessary, which can block catalytically active surface sites; and the laser synthesis is rapid enough to create arrays of nanomaterials in sufficient quantities to study them in bulk. We employed our laser-made catalysts on high-surface-area carbon supports to selectively electrooxidize toluene to benzyl alcohol. We show how choice of catalyst composition and electrolyte engineering lead to selectivity for the alcohol.

Laser-made mixed-metal (hydr)oxide nanocatalysts for selective electrooxidation of hydrocarbons to alcohols

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