Imaging Water-Splitting Electrocatalysts with pH-Sensing Confocal Fluorescence Microscopy

Abstract

Hydrogen generation by water electrolysis is promising for energy storage, and imaging the reaction dynamics near a H_2-evolving electrode can provide valuable insights. We utilized laser-scanning confocal fluorescence microscopy to map the product/reactant concentration at a H_2-evolving electrode at micron-scale resolution which identifies areas with fast reaction kinetics. Small concentrations of a pH indicator dye added to the aqueous electrolyte enables ratiometric fluorescence sensing for quantitative pH detection over the range pH 5.3-7.5 and minimally perturbs the local environment. To overcome diffusion limitations, a miniature flow cell was utilized in the microscope to achieve micron-scale resolution in steady state while applying galvanostatic current. We demonstrated the technique using F:SnO_2-coated glass with varied metal catalyst patterns and compositions resulting in clear images of increased pH near areas of high water-reducing activity. Simulations of the pH profiles near the electrolyte-patterned catalyst interface were also performed using the COMSOL finite-element software package to solve the convection/diffusion equations, and the calculation results agreed well with the experimentally-observed fluorescence profiles. Flow cell fluoresecence microscopy shows promise in imaging comparative catalyst activity as well as three-dimensional product/reactant profiles in complex electrode architectures.

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