Locally Concentrated Ionic Liquid Electrolytes for Wide‐Temperature‐Range Aluminum‐Sulfur Batteries

• Published in: Angewandte Chemie International Edition 2024-03, Vol.63 (10), p.e202318204-n/a
• Main Authors: Xu, Cheng, Diemant, Thomas, Mariani, Alessandro, Di Pietro, Maria Enrica, Mele, Andrea, Liu, Xu, Passerini, Stefano
• Format: Article
• Language: English
• Subjects: Aluminum; Aluminum sulfur batteries; Electrolytes; Electrolytic cells; Energy storage; Fluidity; Ion currents; Ion transport; ionic liquid electrolytes; Ionic liquids; Kinetics; locally concentrated electrolytes; non-solvating co-solvent; Specific capacity; Sulfur; Temperature; Viscosity; wide temperature range
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.202318204

Aluminum−sulfur (Al−S) batteries are promising energy storage devices due to their high theoretical capacity, low cost, and high safety. However, the high viscosity and inferior ion transport of conventionally used ionic liquid electrolytes (ILEs) limit the kinetics of Al−S batteries, especially at sub‐zero temperatures. Herein, locally concentrated ionic liquid electrolytes (LCILE) formed via diluting the ILEs with non‐solvating 1,2‐difluorobenzene (dFBn) co‐solvent are proposed for wide‐temperature‐range Al−S batteries. The addition of dFBn effectively promotes the fluidity and ionic conductivity without affecting the AlCl4−/Al2Cl7− equilibrium, which preserves the reversible stripping/plating of aluminum and further promotes the overall kinetics of Al−S batteries. As a result, Al−S cells employing the LCILE exhibit higher specific capacity, better cyclability, and lower polarization with respect to the neat ILE in a wide temperature range from −20 to 40 °C. For instance, Al−S batteries employing the LCILE sustain a remarkable capacity of 507 mAh g−1 after 300 cycles at 20 °C, while only 229 mAh g−1 is delivered with the dFBn‐free electrolyte under the same condition. This work demonstrates the favorable use of LCILEs for wide‐temperature Al−S batteries. A locally concentrated ionic liquid electrolyte formed via diluting ionic liquid electrolytes with non‐solvating 1,2‐difluorobenzene (dFBn) co‐solvent is proposed for wide‐temperature‐range Al−S batteries. It presents better fluidity and ionic conductivity without affecting the AlCl4−/Al2Cl7− equilibrium, as well as a faster kinetics, enabling a long‐life‐span Al−S batteries under −20–40 °C.