Regulating the Synergistic Effect in Bimetallic Two‐Dimensional Polymer Oxygen Evolution Reaction Catalysts by Adjusting the Coupling Strength Between Metal Centers

Abstract Bimetallic electrocatalysts with its superior performance has a broad application prospect in oxygen evolution reaction (OER), but the fundamental understanding of the mechanism of synergistic effect is still limited since there lacks a practical way to decouple the influence factors on the intrinsic activity of active sites from others. Herein, a series of bimetallic Co−Ni two‐dimensional polymer (2DP) model OER catalysts with well‐defined architecture, monolayer characteristic, were designed and synthesized to explore the influence of the coupling strength between metal centers on OER performance. The coupling strength was regulated by adjusting the spacing between metal centers or the conjugation degree of bridge skeleton. Among the examined 2DPs, CoTAPP‐Ni‐MF‐2DP, which has the strongest coupling strength between metal centers exhibited the best OER performance. These model systems can help to explore the precise structure‐performance relationships, which is important for the rational catalyst design at the atomic/molecular levels.