Smita Talande, Ievgen Obraztsov, Vishal Shrivastav, Mahima Khandelwal, Mansi, Michal Otyepka, Radek Zbořil, Aristides Bakandritsos
Aluminum-ion capacitors (AICs) attract significant research interest as multivalent energy-storage devices that aim to increase energy density beyond that of conventional monovalent-ion supercapacitors. Owing to the trivalent charge of Al3+ and the abundance, low cost, and relative chemical stability of aluminum, AICs hold strong potential for sustainable and scalable energy storage. This review provides a comprehensive overview of their fundamental charge-storage mechanisms, recent advances in electrode materials, electrolyte engineering, and device architectures. Particular emphasis is placed on overcoming the intrinsic challenges associated with Al3+-based charge carriers, such as intricate solvation chemistry, sluggish desolvation kinetics, and limited ion transport within host frameworks, through structural design, defect engineering, and interfacial optimization. Progress in aqueous, ionic-liquid, deep-eutectic, and quasi-solid-state electrolytes is critically assessed alongside the key role of 2D materials, such as graphene and MXenes. Finally, insights from operando characterization and computational modeling are discussed to guide future directions toward high-rate, long-life, and flexible Al3+-based supercapacitors. By integrating these perspectives, this review provides a conceptual framework and roadmap for advancing AICs toward next-generation energy storage.