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Optical Fluorescence Microscopy for Spatially Characterizing Electron Transfer across a Solid-Liquid Interface on Heterogeneous Electrodes

Published online by Cambridge University Press:  28 April 2016

Eric Choudhary*
Affiliation:
Center for Nanoscale Science and Technology, National Institute of Standards and Technology 100 Bureau Dr, Gaithersburg, MD 20899, U.S.A.
Jeyavel Velmurugan
Affiliation:
Maryland NanoCenter, University of Maryland, College Park, MD 20742, U.S.A.
James M. Marr
Affiliation:
Maryland NanoCenter, University of Maryland, College Park, MD 20742, U.S.A.
James A. Liddle
Affiliation:
Center for Nanoscale Science and Technology, National Institute of Standards and Technology 100 Bureau Dr, Gaithersburg, MD 20899, U.S.A.
Veronika Szalai
Affiliation:
Center for Nanoscale Science and Technology, National Institute of Standards and Technology 100 Bureau Dr, Gaithersburg, MD 20899, U.S.A.
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Abstract

Heterogeneous catalytic materials and electrodes are used for (electro)chemical transformations, including those important for energy storage and utilization. 1, 2 Due to the heterogeneous nature of these materials, activity measurements with sufficient spatial resolution are needed to obtain structure/activity correlations across the different surface features (exposed facets, step edges, lattice defects, grain boundaries, etc.). These measurements will help lead to an understanding of the underlying reaction mechanisms and enable engineering of more active materials. Because (electro)catalytic surfaces restructure with changing environments, 1 it is important to perform measurements in operando. Sub-diffraction fluorescence microscopy is well suited for these requirements because it can operate in solution with resolution down to a few nm. We have applied sub-diffraction fluorescence microscopy to a thin cell containing an electrocatalyst and a solution containing the redox sensitive dye p-aminophenyl fluorescein to characterize reaction at the solid-liquid interface. Our chosen dye switches between a nonfluorescent reduced state and a one-electron oxidized bright state, a process that occurs at the electrode surface. This scheme is used to investigate the activity differences on the surface of polycrystalline Pt, in particular to differentiate reactivity at grain faces and grain boundaries. Ultimately, this method will be extended to study other dye systems and electrode materials.

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Articles
Copyright
Copyright © Materials Research Society 2016 

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Optical Fluorescence Microscopy for Spatially Characterizing Electron Transfer across a Solid-Liquid Interface on Heterogeneous Electrodes
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