CoC_x‑induced interfacial octahedral Co²⁺ sites of NiCo-LDH electrode with improved faradic reactivity toward...

Battery-like electrode materials are characterized by large theoretical capacitance but suffer from poor surface reactivity and insufficient electroactive sites thus limiting their practical charge storage capacity. To overcome this challenge, an effective strategy for vacancy modulation on battery-like electrode materials is necessary. Herein, we report for the first time an elaborately designed three-dimensional (3D) hierarchical heterostructure consisting of CoC_x@NiCo-LDH on conductive nickel foam as a freestanding supercapacitor electrode. Benefiting from the weakening of the coordination of CoO bonds, the CoC_x structure induces in-situ reconstruction of the NiCo-LDH lattice, resulting in the formation of abundant oxygen vacancies (interfacial octahedral Co²⁺ sites) that lower the OH^- adsorption energy as determined by the density functional theory (DFT) calculation. The resulting CoC_x@NiCo-LDH/NF electrode exhibits an ultrahigh rate capability (2330 mF cm^-2 at 0.3 mA cm^-2, with capacitance retention of 51.5 % at 30 mA cm^-2) and remarkable cycling performance (capacitance retention of 81.6 % after 10,000 cycles). Additionally, the assembled asymmetric devices deliver an extremely high energy density of 246 μWh cm^-2 at the power density of 798 μW cm^-2, with 87.8 % capacitance retention after 10,000 cycles at 8 mA cm^-2. Overall, this study presents a simple yet effective strategy to construct high-performance battery-like electrodes for potential applications in energy storage, transportation, and communication.