Abstract
Understanding the influence of potential on electrochemical surface reaction kinetics remains a challenge in identifying catalytic materials for numerous important reactions including water splitting (OER), hydrogen evolution (HER), and CO2 reduction, among others. Limitations in computational methods, complicated by the unique environment of the electrode–electrolyte interface, have compelled many studies to focus on the thermodynamics of reaction schemes and to generalize inferences about the kinetics of charge transfer. In instances where activation barrier estimates are available, they are typically assumed to follow the empirical Butler–Volmer (BV) model. In this Perspective, we illustrate that the relative magnitudes and potential-dependences of elementary barriers can have a marked effect on the properties of a catalyst deemed “optimal” for a given reaction. We use a simple pseudosteady-state analysis of two sequential surface-mediated charge transfers to assess the degree of rate control of each s...
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