Microkinetic Model to Rationalize the Lifetime of Electrocatalysis: Trade-off between Activity and Stability.

Electrocatalysts which can operate for several years are required to produce hydrogen and commodity chemicals in an environmentally friendly manner. However, designing materials with long operational lifetimes is challenging, due to the lack of a conceptual framework to predict catalytic lifetimes quantitatively. Here, we report a microkinetic equation which quantifies the lifetime of an electrocatalyst undergoing dissolution. This equation was obtained by taking advantage of the fact that catalysis is much faster than deactivation, which allows the ordinary differential equations to be solved via the quasi steady-state approximation. All chemical reactions were modeled as irreversible, first-order elementary reactions. Under this assumption, the catalytic rate correlates linearly with the deactivation rate, leading to a trade-off relationship between activity and stability. Our model was supported by the correlation between theoretical and experimental lifetimes ( = 0.86) of a manganese oxide electrocatalyst during the oxygen evolution reaction.