Abstract
A three-dimensional finite element method (FEM) model simulating the electrochemical behaviour of Pt coplanar thin-film electrodes used for liquid cell transmission electron microscopy measurements was developed. The model included reaction kinetics and it was applied for the oxygen evolution reaction (OER). Kinetic parameters of OER in the liquid cell were experimentally acquired and applied to the FEM model. Comparison between the experimental and simulated polarization curves demonstrated the reliability of the FEM predictions. The simulations were used to produce maps of the potential and current density distributions of the working and counter electrodes as well as for calculating the distribution of the current density in the liquid electrolyte. Two distinctive electrode geometries were evaluated with the FEM model. It was predicted that non-symmetrical electrode designs can cause unexpected electrochemical behaviour with respect to the electrolyte current density between working and counter electrodes accompanied by the presence of hot spots. The findings suggest that FEM simulations could be key to designing well-performing electrochemical microcells for liquid phase electron microscopy experiments.
Highlights
To cite this article: Morgan Binggeli et al 2021 J
Oxygen evolution reaction (OER) kinetic parameters measurement in the liquid cell.—To perform a reliable finite element analysis, the anodic and cathodic exchange current densities (i0,a and i0,b) as well as the COMSOL anodic and cathodic Tafel coefficients (Aa and Ac) values need to be determined from experimental OER measurements in the liquid cell
Comparison of experimental polarization curve with simulation results.—To perform the simulation of the OER kinetic in the liquid cell, a stationary solution of the model was implemented by applying a current between 20 and 56 nA with 3 nA increment between each simulation
Summary
To cite this article: Morgan Binggeli et al 2021 J. The use of this holder provides a stable reference potential which is accommodated by a bulk Ag/AgCl electrode. Under the primary current distribution model, the effect of the overpotential is neglected This is a central effect for electrocatalytic reactions and, the governing equation of the overpotential at the electrode-electrolyte interface is defined to follow a secondary current distribution, which is a kinetic-based model that considers charge migration and neglects mass transport. We specify the experimental kinetic equation describing the relation between the current density i and the activation overpotential η at the electrode-electrolyte interface. Input geometry.—To design the 3D geometry for the simulation, we focused on the non-passivated region of the top chip, i.e. for D1
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