The utilization of “plasmonic” nanomaterials in electrochemical systems for energy conversion and catalysis has shown great promise. Fundamental studies into these systems are challenging, however, due to their inherently heterogeneous nature. Variations in particle size, shape, coupling, etc. can complicate the interpretation of experimental results, particularly when one is interested in effects due to plasmon excitation. While optical detection schemes have been employed to study electrochemical reactions occurring at individual plasmonic nanostructures, the assumptions necessary for data interpretation often severely limit the utility of this approach. Herein, the use of a combined electrochemical and optical approach to the study of these systems is described. Scanning electrochemical cell microscopy is employed to directly measure the rate of electrochemical reactions at individual plasmonic nanostructures, while optical spectroscopy is used to probe the geometry of these nanostructures in situ. This complementary approach allows for the correlation of reliable electrochemical kinetic data with structural information and for the effects of plasmon excitation on electrochemical reaction rates to be examined in a direct, quantitative manner. Initial studies applying this methodology to model electrocatalytic systems will be presented.

Probing electrocatalytic reactions at individual plasmonic nanostructures: A combined direct electrochemical and optical approach

256th National Meeting (2018)

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