Enhancing the Performance of 2D Ni‐Fe Layered Double Hydroxides by Cabbage‐Inspired Carbon Conjunction for Oxygen Evolution Reactions

Abstract Layered double hydroxide (LDH) nanosheets as one type of two‐dimensional materials have garnered increasing attention in the field of oxygen evolution reaction (OER) in recent decades. To address the challenges associated with poor conductivity and limited electron and charge transfer capability in LDH materials, we have developed a straightforward one‐pot synthesis method to successfully fabricate a composite material with a microstructure resembling cabbage, which encompasses NiFe‐LDH and nanocarbon (referred as NiFe‐LDH@C). Atomic force microscopy (AFM) and high‐resolution transmission electron microscopy (HRTEM) revealed that the monolayer NiFe‐LDH with a height of ~0.5–0.8 nm is uniformly distributed and closely bonded to the carbon support, leading to a significant enhancement in conductivity and facilitating faster electron and charge transfer. Moreover, the NiFe‐LDH@C exhibits a substantial number of surface defect sites, which enhances the interaction with oxygen species. This dual enhancement in charge transfer and oxygen species‐mediated transfer greatly improves the catalytic OER performance, which is further corroborated by theoretical calculations. Notably, the Ni 10 Fe 6 ‐LDH@C with the highest concentration of surface oxygen vacancies demonstrated superior water oxidation performance, surpassing commercially available RuO 2 catalysts; an OER overpotential of 231 mV@10 mA cm −2 with a Tafel slope of 71 mV dec −1 was achieved.