Atomic Scale Optimization Strategy of Al-Based Layered Double Hydroxide for Alkali Stability and Supercapacitors

The pseudocapacitor material is easily decomposed when immersed in alkaline solution for a long time. Hence, it is necessary to find a strategy to improve the alkali stability of pseudocapacitor materials. In addition, the relationship between alkali stability and electrochemical performance is still unclear. In this work, a series of Al-based LDH (Layered double hydroxide) and derived Ni/Co-based sulfides are prepared, and corresponding alkali stability and electrochemical performance are analyzed. The alkali stability of CoAl LDH is so poor and can be improved effectively by doping of Ni. Ni₁Co₂S₄ and Ni₂Co₁Al LDH exhibit an outstanding alkali stability, and Ni₂Co₁S₄ exhibits an extremely poor alkali stability. The variable valence state of Co element and the solubility of Al in alkali solution are the fundamental reasons for the poor alkali stability of CoAl LDH and Ni₂Co₁S₄. Ni₂Co₁S₄ showed an outstanding electrochemical performance in a three-electrode system, which is better than that of Ni₁Co₂S₄, indicating that there is no direct correlation between alkali stability and electrochemical properties. Sulfidation improved the electrical conductivity and electrochemical activity of electrode materials, whereas alkali etching suppressed the occurrence of the electrochemical reaction. Overall, this work provides a clear perspective to understand the relationship between alkali stability and electrochemical properties.