Optimizing nickel-aluminium layered double hydroxides for supercapacitors: The role of 3D structural assembly

Nickel-aluminium layered double hydroxides (NiAl-LDHs) have emerged as promising electrode materials for supercapacitors (SCs) due to their inherently high specific surface area and theoretical specific capacitance, which are primarily attributed to the rapid pseudocapacitive response at the surface. However, NiAl-LDHs typically form agglomerated nanosheets, leading to a significant reduction in specific surface area, which is crucial for enhancing the number of active sites and improving the capacitive properties of the materials. To overcome this limitation, 2D nanostructures were assembled into 3D architectures by synthesizing NiAl-LDHs with distinct morphologies in a one-step hydrothermal process using an alkaline agent (NH₄F). This approach resulted in the formation of 3D NiAl-LDH/HN₄F structures, which exhibit a larger contact area and a greater number of redox-active sites. Consequently, the 3D NiAl-LDH/HN₄F electrodes demonstrated a significantly higher specific surface area, leading to remarkable improvements in specific capacitance (1219 ± 30F g^-1) and energy density (61 ± 1 Wh kg^-1) compared to their 2D counterparts. This structural enhancement increases both the surface area and active site density while providing a new framework for designing high-performance LDH-based electrodes.