Solution Processing of Spinel Nickel Cobaltite: Exfoliation Mechanism, Dispersion Stability, and Applications

The exfoliation of nonlayered materials to mono- or few-layers is of growing interest to realize their full potential for various applications. Nickel cobaltite (NiCo₂O₄), which has a spinel crystal structure, is one such nonlayered material with unique properties and has been utilized in a wide range of applications. Herein, NiCo₂O₄ is synthesized from NiCo₂- Layered double hydroxides using a topochemical conversion technique. Subsequently, bulk NiCo₂O₄ is exfoliated into mono- or few-layer nickel cobaltene nanosheets using liquid-phase exfoliation in various low-boiling point solvents. An analytical centrifuge technique is also utilized to understand the solute-solvent interactions by determining their dispersion stability using parameters such as the instability index and sedimentation velocity. Among the studied solvents, water/isopropyl alcohol cosolvent is found to have better dispersion stability. In addition, density functional theory calculations are carried out to understand the exfoliation mechanism. It is found that the surface termination arising from the Co-O bond needs the least energy for exfoliation. Furthermore, the obtained nickel cobaltene nanosheets are utilized as an active material for supercapacitors without any conductive additives or binders. A solid-state symmetric supercapacitor delivers a specific capacitance of 10.2 mF cm^-2 with robust stability, retaining ∼98% capacitance after 4000 cycles.