Uniform Ion Flow Effect of Dynamic Electrostatic Shielding Layer for Facilitating Homogeneous Nucleation and Deposition on Aluminum Anode

Abstract Rechargeable aluminum batteries (RABs) present considerable potential for large‐scale energy storage, particularly within power stations. Nonetheless, their operational lifespan and commercialization are hindered by issues like Al anode dendrite formation and electrolyte corrosion. To address the aforementioned issues, a stabilizer has been proposed to enhance the electrolyte/anode interface. Experimental and computational simulation results indicate that the surface tension of the SDBS alkyl chain facilitates its preferential adsorption onto the electrode surface, thereby establishing a protective layer that mitigates the corrosion of the chloroaluminate ionic liquid (ILs). Additionally, the suitable electronegativity of the phenyl‐SO 3 group generates an electrostatic shielding effect that not only dynamically regulates ion flow but also equilibrates the nucleation and deposition velocity, ultimately promoting the stable planar Al deposition. Consequently, the SDBS‐modified Al//Al symmetric battery demonstrates stable cycling for 500 and 1000 h under high current density (5 mA cm −2 ) and large area capacity (5 mAh cm −2 ), respectively. The Al//flake graphite full battery achieves reversible capacity of 90.01 mAh g −1 after 1000 cycles at 0.5 A g −1 , significantly improving capacity retention. This study also further explores the effect of additive functional groups and ions on Al anodes, offering insights for the rational design of RABs electrolytes.