Publication date: 28th August 2024
Metal|Metal oxide (M|MOx) interfaces are becoming key components in electrocatalysis due to their ability to enhance catalytic performance. The case of reducible oxides is particularly notable due to their ability to generate M+ sites accompanied by the loss of lattice oxygen.[1] These interfaces have been already extensively studied in the field of thermal catalysis, where reducible oxides are shown to dynamically transform under reducible conditions while enhancing the interactions at the M|MOx interface. [2] However, the transformations of these systems under electrochemical reduction conditions are far from being understood due to the added complexity of experiments.
Cu|TiOx is a system of interest for different photo-electro and electro- catalytic transformations, which span from dye-sensitized solar cells to water splitting, and, more recently, CO2 electroreduction. [3, 4] Yet, the fundamental relationships between the reduction driven transformations, and the overall catalytic behavior of the system are underexplored.
Herein, we synthesize well-defined and tunable Cu@TiOx core@shell nanostructures and used them as a platform for understanding the fundamental interactions between Cu and TiOx under CO2 electroreduction conditions. We tailored the extent of the Cu|TiOx interface as well as the composition thanks to the use of colloidal atomic layer deposition (cALD) as previously developed in our group.[5] The oxide shell shows a strong interaction with copper and inhibits its reduction as previously reported for non-reducible oxides.[6] Nonetheless, even the TiOx shell readily encapsulates the nanocrystals it does not insulate the surface and it dynamically transforms under electrochemical reduction conditions. Varying the extent of the interface and composition yield fundamental insights of the dynamics at the interface under operating conditions. Currently, studies are being conducted to understand the implications in catalysis.
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