Cathode Design for Aqueous Rechargeable Multivalent Ion Batteries: Challenges and Opportunities

With the rapid growth in energy consumption, renewable energy is a promising solution. However, renewable energy (e.g., wind, solar, and tidal) is discontinuous and irregular by nature, which poses new challenges to the new generation of large‐scale energy storage devices. Rechargeable batteries using aqueous electrolyte and multivalent ion charge are considered more suitable candidates compared to lithium‐ion and lead‐acid batteries, owing to their low cost, ease of manufacture, good safety, and environmentally benign characteristics. However, some substantial challenges hinder the development of aqueous rechargeable multivalent ion batteries (AMVIBs), including the narrow stable electrochemical window of water (≈1.23 V), sluggish ion diffusion kinetics, and stability issues of electrode materials. To address these challenges, a range of encouraging strategies has been developed in recent years, in the aspects of electrolyte optimization, material structure engineering and theoretical investigations. To inspire new research directions, this review focuses on the latest advances in cathode materials for aqueous batteries based on the multivalent ions (Zn2+, Mg2+, Ca2+, Al3+), their common challenges, and promising strategies for improvement. In addition, further suggestions for development directions and a comparison of the different AMVIBs are covered.