In this study, we synthesized novel three-dimensional (3D) cross-flowered Co-Ni metal–organic framework (Co-Ni-MOF) precursors using the chemical precipitation method. Subsequently, we obtained Co-Ni-Fe layered double hydroxides (Co-Ni-Fe-LDHs) through an ion exchange strategy, which preserved their original morphology while consisting of ultrathin layered hydroxide nanosheets. The interlayer spacing of the LDH lamellar structure was finely tuned by varying the ratios of Co to Ni. The results demonstrated that Co-Ni-Fe LDHs, characterized by a unique three-dimensional cross-shaped structure and an optimal composition ratio of Co2+:Ni2+ = 2:1, exhibited increased interlayer spacing. This structural characteristic contributed to their excellent electrochemical performance, positioning them as optimal electrode materials for catalytic oxygen evolution reactions (OER). Our observations revealed that Co-Ni-Fe-LDHs exhibited remarkable OER activity, characterized by a low Tafel slope of 41.82 mV dec−1, a low overpotential of 322 mV at a current density of 10 mA cm−2, and outstanding stability over a 48-hour period. In-situ Raman spectroscopy results indicated that the active site of the composite was γ-CoOOH. Additionally, the room temperature stirring and standing strategy employed in this study is easier to scale up and yields a higher quantity of reaction products compared to traditional high-temperature and high-pressure conditions. This investigation provides novel insights into the design and fabrication of Co-Ni-Fe-LDHs catalyst with 3D cross-flower structures, demonstrating enhanced electrocatalytic activity and commendable stability. These findings suggest promising applications in the field of electrolyzed water.
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