Abstract
Abstract
Aluminum (Al) foil anodes are promising candidates for sustainable lithium-ion batteries owing to their high theoretical capacity (993 mAh g⁻¹) and intrinsically coating-free, foil-based architecture. However, their practical application is limited by severe mechanical degradation and insufficient cycling stability. Within the GREENCell-concept, two fully scalable stabilization strategies based exclusively on commercially available Al alloy foils and fluorine-free polyisobutylene-bound LiMn₂O₄ cathodes were investigated: nickel (Ni) plating of Al alloy foil 8011 as an additional current-collecting layer and the use of high silicon-content Al alloy foil 4343 with 7.5wt% Si. Full-cell and half-cell cycling, electrochemical impedance spectroscopy, and post-mortem morphological analysis reveal clear correlations between electrochemical performance and structural evolution. Ni-plating improves current distribution and mechanical integrity, thereby reducing initial capacity loss, lowering ohmic resistance, and suppressing crack propagation, resulting in a 15% higher capacity retention after 100 cycles compared with untreated Al alloy foil 8011. In contrast, Ni-plated high Si-content Al alloy foil 4343 shows larger initial irreversible losses but pronounced intermediate-cycle activation and enhanced diffusion-controlled kinetics, achieving 67% capacity retention after 100 cycles and a 24% improvement relative to the untreated low Si-content Al reference. These results establish practical design principles for scalable, cost-efficient Al-based anodes in next-generation LiBs.