Enhanced Electrocatalytic Activity of Ethanol Oxidation Reaction on Palladium-Silver Nanoparticles via Removable Surface Ligands.

Abstract

This work developed a facile colloidal route to synthesize BH4--capped PdxAgy nanoparticles (NPs) in water using the reducing ionic liquids of [Cnmim]BH4, and the resulting NPs were prone to form the nanocomposites with [amim]+-modified reduced graphene (RG). The removal of the metal-free inorganic ions of BH4- can create the profoundly exposed interfaces on the PdxAgy NPs during the electrooxidation, and favor the ethanol oxidation reaction (EOR) in lowering energy barrier. The counterions of [Cnmim]+ can gather ethanol, OH- ions, and the reaction intermediates on catalysts, and synergistically interact with RG to facilitate the charge transfer in nanocomposites. The interface-modified RG nanosheets can effectively segregate the PdxAgy NPs from aggregation during the EOR. Along with the small size of 4.7 nm, the high alloying degree of 60.2%, the large electrochemical active surface area of 64.1 m2 g-1, and the great peak current density of 1501 mA cm-2 mg-1, Pd1Ag2@[C2mim]BH4-amimRG nanocomposite exhibits the low oxidation potentials, strong poison resistance, and stable catalytic activity for EOR in alkaline media, and hence can be employed as a promising anodic catalyst in ethanol fuel cells.