Self‐Activated Liquid‐Metal Hosts Stabilize Anode‐Free Aluminum Batteries

ABSTRACT

Anode‐free aluminum batteries offer a promising route toward high energy density and low‐cost energy storage, but their development is limited by uncontrolled Al nucleation/growth and cumulative irreversible Al loss during cycling. Here, we report a Ga–In–Sn liquid‐metal‐modified carbon cloth, LM@CC, as a self‐activated interfacial host for anode‐free graphite aluminum batteries in molten‐salt electrolytes at 100°C. Upon exposure to the molten salt after cell assembly, LM@CC spontaneously reconstructs and undergoes in situ pre‐aluminization, forming an intrinsically aluminophilic and electrochemically activated interface before cycling. This adaptive liquid‐metal interface lowers the Al nucleation overpotential, accelerates interfacial charge transfer, and guides spatially uniform Al deposition/stripping. Consistent with these interfacial advantages, LM@CC‐based symmetric cells sustain stable Al plating/stripping for approximately 1000 h at 1 mA cm ⁻² and 5 mAh cm ⁻² . As a result, the graphite||LM@CC anode‐free full cell operates for over 20 000 cycles at 2 A g ⁻¹ and 80 000 cycles at 10 A g ⁻¹ with average Coulombic efficiencies of 99.60% and 97.79%, respectively. These findings highlight interfacial reconstruction as a route to stable, high‐rate anode‐free aluminum batteries.