Abstract
Unlike single‐step reactions, multi‐step reactions can be greatly facilitated only if all the intermediate reactions can be catalyzed simultaneously and progressively. Herein, the theoretical analysis and experiments to illustrate the superiority of the cascade oxygen evolution reaction (OER) are conducted. As different OER intermediate reactions demand FexNi1‐xOOH with altered Fe/Ni ratios, gradient Fe‐doped NiOOH can be an ideal electrocatalyst for the efficient cascade OER in line. Fine controlling of the nucleation sequence of iron and nickel sulfides leads to a FeS2@NiS2 core–shell structure. The activated outward diffusion of Fe dopants results in the gradient Fe/Ni ratios in the FexNi1‐xOOH shell, where a cascade OER can happen. Electrochemical tests suggest that the FeS2@NiS2 only needs an overpotential of 237 mV to reach the current density of 10 mA cm−2, with fast reaction kinetics and good stability.
In ideal conditions, the continuous intermediate reactions in oxygen evolution reaction (OER) require active sites with high, moderate, and low Fe/Ni ratios, as well as gradient spatial distribution of them. Here, activating FeS2@NiS2 core–shell structure results in a shell of FexNi1‐xOOH with gradient Fe/Ni ratios, thus realizing cascade OER with superior performance.