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Cation-driven phase transition and anion-enhanced kinetics for high energy efficiency zinc-interhalide complex
Wei Zhong1,2,3, Hao Cheng4,5,6, Shichao Zhang1
1State Key Laboratory of Chemical Engineering, Institute of Pharmaceutical Engineering, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027, China.
Nature Communications
|May 17, 2025
Summary
This study enhances aqueous zinc-halogen batteries by using tetramethylammonium cations to control zinc deposition and suppress polyhalide shuttle, improving energy storage and lifespan.
Area of Science:
- Electrochemistry
- Materials Science
- Energy Storage
Background:
- Aqueous Zn-halogen batteries offer safety and cost benefits but are limited by polyhalide shuttle and irregular zinc deposition.
- These issues reduce battery efficiency and operational lifespan, hindering widespread adoption.
Purpose of the Study:
- To develop strategies for suppressing the polyhalide shuttle effect and promoting uniform zinc electrodeposition in aqueous Zn-halogen batteries.
- To enhance the energy efficiency and long-term stability of these battery systems.
Main Methods:
- Investigated the role of tetramethylammonium halide (TMAX) electrolytes in modifying zinc deposition and polyhalide behavior.
- Employed a cation-driven positive electrode phase transition and anion kinetic enhancement strategy.
- Analyzed zinc (101) deposition, interhalide complex formation, and electrochemical conversion kinetics.
Main Results:
- Tetramethylammonium (TMA+) cations directed uniform zinc (101) deposition via electrostatic shielding, extending cycling life.
- TMA+ captured triiodide (I3-) ions, forming stable solid-phase interhalide complexes and improving coulombic efficiency.
- Modified electrolytes demonstrated high energy efficiency (95.2% at 0.2 A g-1) and remarkable stability (0.1% capacity decay per 1000 cycles, 0.1‰ decay per cycle over 10,000 cycles at 1 A g-1).
Conclusions:
- A cation-driven phase transition and anion kinetic enhancement effectively suppress polyhalide shuttle and chaotic zinc deposition.
- The developed strategies significantly improve the energy efficiency and long-term cyclability of aqueous Zn-halogen batteries.
- This research offers valuable insights for designing advanced, stable, and efficient sustainable energy storage solutions.
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