Dual-Functional Acetate Intercalation in NiMn-LDH Cathode: Interlayer Pillaring and Electronic Delocalization Toward...

Aqueous zinc-ion batteries (AZIBs) are regarded as attractive candidates for safe and sustainable energy storage, but their further development remains constrained by sluggish ion/electron transport and limited structural stability of cathode materials. To overcome these limitations, we designed an acetate-intercalated NiMn layered double hydroxide cathode (Ac-NiMn-LDH) using a template-guided assembly route. This approach effectively mitigates the restacking of NiMn-LDH nanosheets, endowing the material with a robust structure and enlarged active surface area. Serving as functional pillars, the intercalated acetate anions expand the interlayer gallery and weaken Zn²⁺-host interactions, thereby reducing ion-migration resistance and reinforcing the layered structure. Furthermore, the strong electronic coupling between the acetate groups and the host layers triggers localized charge redistribution, promoting d-electron delocalization at Mn/Ni sites and enhancing charge transport. Benefiting from this coupled structural and electronic regulation, the Ac-NiMn-LDH cathode achieves a capacity of 274.6 mAh g^-1 at 0.1 A g^-1 and retains stable cycling at 1 A g^-1, corresponding to a low capacity decay of 0.002% per cycle over 2200 cycles. Moreover, flexible AZIBs assembled with this cathode operate steadily under bending deformation. This work offers a synergistic strategy for modulating both the physical architecture and electronic states of layered cathodes for advanced AZIBs.