Intrinsic Electrocatalytic Activity for Oxygen Evolution of Crystalline 3d‐Transition Metal Layered Double Hydroxides

Layered double hydroxides (LDHs) are among the most active and studied catalysts for oxygen evolution reaction (OER) in alkaline electrolytes. However, previous studies have generally either focused on a small number of LDHs, applied synthetic routes with limited structural control, or used non-intrinsic activity metrics, thus hampering construction consistent structure–activity-relations. Herein, by employing new individually developed synthesis strategies atomic we obtained broad series crystalline α-MA(II)MB(III) LDH β-MA(OH)2 electrocatalysts (MA=Ni, Co, MB=Co, Fe, Mn). We further derived their intrinsic through electrochemical surface area normalization, yielding trend NiFe > CoFe Fe-free Co-containing Fe-Co-free Ni-based catalysts. Our theoretical reactivity analysis revealed that these trends originate from dual-metal-site nature centers, which lead to composition-dependent synergies diverse scaling relationships may be design improved performance.