Amphiphilic Interfacial Environment Reconfiguration Unlocks Long-Life Zinc-Ion Batteries With Lean Electrolytes and...

Water-induced parasitic reactions and dendrite growth severely limit the performance of aqueous zinc-ion batteries (AZIBs), particularly under practical conditions with ultra-low negative/positive (N/P) ratios and electrolyte/capacity (E/C) ratios. Herein, a trace amount of amphiphilic carbinol (hydroxyl) terminated polydimethylsiloxane (CTP) is employed to reconfigure the interfacial charge environment at the Zn anode. The hydrophobic Si─O backbone of the CTP molecule adsorbs directionally onto the Zn surface through electrostatic forces, which facilitates compact coverage on the anode and effectively blocks the interfacial H₂O contact to suppress parasitic reactions. Furthermore, theoretical calculations reveal that CTP exhibits high permanent and asymmetric dipole moments, serving as a highly efficient interfacial charge regulator. Upon capturing Zn²⁺ by the hydrophilic hydroxyl groups, the CTP molecules effectively mediate interfacial charge distribution and electron transfer kinetics, thus promoting uniform Zn deposition. Consequently, the Zn//NH₄V₄O₁₀ battery exhibits exceptional cycling stability over 800 cycles at 0.5 A g^-1 with a limited N/P ratio of 1.3 and E/C ratio of 15.84 µL mAh^-1. This work highlights the significance of constructing dipole-mediated amphiphilic interfacial environments for advancing practical AZIBs under harsh working conditions.