Monodentate adsorption of oxygen intermediates results in a theoretical overpotential limit of ≈0.35 V for oxygen evolution reaction (OER), which causes the sluggish kinetics of the OER process. In this work, nonprecious chromium dopant is introduced into the self‐supported CoFe layered double hydroxides (LDHs) on nickel foam (Cr‐CoFe LDHs/NF) via a facile one‐step hydrothermal method, which exhibits a preeminent electrocatalytic activity toward the OER with an ultralow overpotential of 238 mV to obtain 10 mA cm−2 and a high stability after cyclic voltammetry for 5000 cycles in alkaline solution (1 m KOH). Density functional theory (DFT) calculations unveil that Cr dopants as new active sites could improve the electron‐donation ability of the resultant Cr‐CoFe LDHs due to the smaller electronegativity of Cr in comparison with Fe and Co. Therefore, the scaling relation of adsorption energy among four oxygen intermediates is broken and consequently the OER performance is further promoted. This work provides a strategy to develop efficient metal layered double hydroxide OER catalysts.

Vanadium-doped Ni2P nanosheet arrays grown on carbon cloth as a highly efficient electrode for the hydrogen evolution reaction.