Optimizing entropy-stabilized synthesis kinetics to modulate the oxygen evolution mechanism

Abstract

Adapting the catalytic reaction pathway and optimizing catalyst activity is a significant challenge in the field of catalysis. Herein, we derived the fundamental form of the diffusion flux-driving force equation using ion diffusion as a research framework, and defined the linear and exponential control coefficients that influence synthesis kinetics. By manipulating these control coefficients, we synthesized high-entropy perovskite La(Co_0.2Cr_0.2Fe_0.2Mn_0.2Ni_0.2)O₃ samples with different degrees of kinetic control. Phase testing results showed that adjusting the control coefficients resulted in varying degrees of kinetic control. Experimental evidence and theoretical simulations demonstrated that samples with a higher proportion of kinetic control exhibited faster catalytic pathways, following the lattice oxygen oxidation mechanism (LOM), and showed the highest catalytic activity. As the proportion of kinetic control decreased, the oxygen evolution reaction (OER) catalytic pathway underwent corresponding transitions. These findings contribute to a new research paradigm aimed at bridging the gap between synthesis design and catalytic performance.