Glycocalyx-inspired hierarchical heterogeneous interface based on thermo-kinetic synergy for highly stable aqueous zinc batteries

Abstract

Aqueous zinc-ion batteries (AZIBs) possess considerable application potential in large-scale energy storage; however, waterinduced parasitic reactions (such as hydrogen evolution corrosion) and continuous proliferation of zinc dendrites at the zinc anode interface have limited their commercialization. Inspired by the "regulation-transport-capture" interfacial homeostasis mechanism of the cellular glycocalyx, engineer a biomimetic hierarchical heterogeneous interface a hierarchical heterogeneous interface (Sb-MXene(PMETAC)) strategy. This composite system improves the stability of the zinc anode via the combined synergistic control of thermodynamic and kinetic processes. The poly([2-(methacryloyloxy)ethyl]trimethylammonium chloride) (PMETAC) functions as a thermodynamic regulation unit. Driven by its high-density quaternary ammonium groups and strong dipole interactions, this polymer layer competitively converts highly active solvated water into bound water, effectively suppressing side reactions and promoting the desolvation of Zn 2+ .At the same time, the highly conductive two-dimensional MXene framework efficiently regulates ion flux and limits bulky anions; additionally, the underlying in-situ Sb layer serves as a zincophilic nucleation template, reducing the nucleation energy barrier and directing the horizontal epitaxial growth of zinc. Owing to this synergistic effect, the modified symmetric battery sustains exceptional cycling stability and an ultra-long cycle life exceeding 5000 h at 2 mA cm -2 (50 times compared to bare zinc). Coupled with an AlVO-NMP cathode, the full battery exhibits a high capacity retention rate of 71.7% after 5000 cycles at a high rate of 5 A g -1 . This work provides a biomimetic interface design concept for dual thermodynamic-kinetic synergistic regulation of interfaces in high-performance aqueous metal batteries.