Science · 2016 · 648 citations · 21 references
Natural SciencesChemical EngineeringChemistryCatalysisReaction EngineeringSurface ChemistryCatalyst DesignCatalyst SynthesisCatalytic MaterialsCatalytic Reaction EngineeringSupported CatalystsSurface CatalysisAtom-efficient SynthesisCatalyst Surface EngineeringDirect SynthesisHydrogenationMetal Oxide CatalystsPalladium CatalystsSupported Metal CatalystsSupported Metal Oxide Catalysts
The direct synthesis of hydrogen peroxide (H2O2) from H2 and O2 represents a potentially atom-efficient alternative to the current industrial indirect process. We show that the addition of tin to palladium catalysts coupled with an appropriate heat treatment cycle switches off the sequential hydrogenation and decomposition reactions, enabling selectivities of >95% toward H2O2. This effect arises from a tin oxide surface layer that encapsulates small Pd-rich particles while leaving larger Pd-Sn alloy particles exposed. We show that this effect is a general feature for oxide-supported Pd catalysts containing an appropriate second metal oxide component, and we set out the design principles for producing high-selectivity Pd-based catalysts for direct H2O2 production that do not contain gold.
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