LAUSR

Spin engineering has garnered significant attention due to its ability to modulate the interaction between active sites and reaction intermediates, thereby enhancing catalytic kinetics. In this study, we present a strategy to tune the coordination environment of Co via topological transformation, effectively modulating its spin state. The resulting CoSexOy-200 exhibited enhanced catalytic kinetics toward ethanol oxidation reaction, achieving a current density of 10 mA cm−2 at a low potential of 1.34 V. The improved catalytic performance is attributed to a topochemical transition-induced spin reconstruction, optimizing the adsorption of reaction intermediates. Building on these findings, the catalyst was further applied to a zinc–ethanol–air battery, leading to a decrease in charging voltage and a narrowed charge–discharge voltage window, which is less than 650 mV. This study establishes a controllable spin-state modulation strategy via topochemical transformation, paving the way for the rational design of advanced electrocatalyst for water electrolysis and next-generation zinc–ethanol–air batteries.