Hierarchically Structured Two‐Dimensional Bimetallic CoNi‐Hexaaminobenzene Coordination Polymers Derived from Co(OH)2 for Enhanced Oxygen Evolution Catalysis

Abstract Conjugated coordination polymers (CPs) with designable and predictable structures have drawn tremendous attention in recent years. However, the poor electrical conductivity and low structural stability seriously restrict their practical applications in electronic devices. Herein, the rational design and synthesis of a hierarchically structured 2D bimetallic CoNi‐hexaaminobenzene CPs derived from Co(OH) 2 are reported as an efficient oxygen evolution reaction (OER) self‐supported electrode. The as‐obtained electrode possesses high electrochemical surface area and intrinsic activity, exhibiting high electrochemical catalytic activity, favorable reaction kinetics performance, and strong durability compared with those of the powder catalysts. As a result, the electrode delivers low overpotential of 219 mV @ 10 mA cm −2 and Tafel slope of 42 mV dec −1 as well as 91.3% retention of current density after 24 h of reaction time. The results of density functional theory computations reveal that the synergistic effect of Co and Ni plays an important role in OER. This work not only presents a strategy to fabricate advanced self‐supported electrodes with abundant and dense active sites, but also promotes the development of conjugated CPs for electrocatalysis.