Quantitative analysis of electrocatalytic reactions using transient voltammetry

forthcoming

This proposal aims to develop a rigorous quantitative framework for analyzing electrocatalytic reactions, addressing a critical gap between experimental studies and theoretical models in the field of electrocatalysis. The project will combine Fourier-transformed ac voltammetry (FTACV) measurements on single-crystal electrodes (SCEs) with Bayesian inference techniques to validate and test kinetic models describing electrocatalytic reactions. The objectives are to: (1) Validate kinetic models for simple electron transfer reactions on well-defined surfaces, (2) Quantify the effects of reaction environment modifications on validated kinetic models, and (3) Extract with high-confidence reaction parameters for important electrocatalytic reactions like hydrogen evolution/oxidation and CO2 reduction The innovative methodology integrates the high kinetic sensitivity FTACV, the well-defined nature of SCEs, and the statistical power of Bayesian inference. This combination will enable rigorous model validation, parameter estimation with confidence intervals, and quantitative comparison between competing models. By establishing clear validity boundaries for kinetic models and relating physical processes to model parameters, this work will strengthen the foundation for accurate model-experiment comparisons in electrocatalysis. The outcomes will be significant for developing more active, durable, and selective catalysts, as well as advancing theoretical modeling of electrocatalytic reactions. The project will contribute to the development of electrochemical technologies crucial for reducing the environmental impact of energy and chemical production.