AlCl4-Deficient Eutectic Electrolytes Enable Reversible Iodine Redox-Amphoteric Conversion for Aluminum Battery Cathodes

Research output: Contribution to journalResearch articleContributedpeer-review

Contributors

Abstract

Aluminum (Al) batteries are promising for sustainable and large-scale energy storage due to the inherent safety, low cost, and attractive metrics of the Al anode. However, the development of high-voltage and high-capacity cathodes remains a key challenge. Herein, we achieve the reversible iodine redox-amphoteric conversion (i.e., I/I0/I+) in Al batteries, wherein AlCl4-deficient eutectic electrolytes are identified critical for stabilizing the conversion process. In contrast to ionic liquid electrolytes prone to parasitic Cl2 evolution, eutectic systems facilitate the I/I0/I+ conversion process with high reversibility and significantly suppressed Cl2 generation. Spectroscopic and theoretical investigations reveal AlCl4 as the dominant species limiting anodic stability of the electrolyte, and its reduced presence in eutectic electrolytes directly enhances iodine conversion reversibility. The optimized electrolyte allows the I2 electrode to deliver a specific capacity of 358 mAh g−1 and an energy density of 490 Wh kg−1 (based on I2 mass), along with excellent cycling stability (83.8% retention over 1000 cycles). High-loading I2 electrodes (8.52 mg cm−2) achieve a high areal capacity of 2.25 mAh cm−2 and demonstrate practical feasibility in a single-layer pouch cell. This work establishes a new design framework for high-energy-density Al batteries and opens avenues for advancing conversion chemistries in multivalent systems.

Details

Original languageEnglish
Article numbere202516059
JournalAngewandte Chemie - International Edition
Volume64
Issue number48
Publication statusE-pub ahead of print - 5 Oct 2025
Peer-reviewedYes

External IDs

ORCID /0000-0002-0211-0778/work/196677268

Keywords

ASJC Scopus subject areas

Keywords

  • Aluminum batteries, Eutectic electrolytes, Iodine cathodes, Iodine conversion, Redox amphoteric