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Suppressing Shuttle Effect through Solvent Coordination and Nitrate Synergy Enables Stable Lithium-Sulfur Batteries
Beichen Xiong1, M Sai Bhargava Reddy1, Sayan Das1
1Davidson School of Chemical Engineering, Purdue University, West Lafayette, Indiana47907, United States.
ACS Applied Materials & Interfaces
|April 28, 2026
Summary
Researchers developed a novel electrolyte for lithium-sulfur (Li-S) batteries using a binary solvent system. This balanced approach mitigates polysulfide shuttling, significantly improving capacity retention and Coulombic efficiency for advanced energy storage.
Area of Science:
- Electrochemistry
- Materials Science
- Energy Storage
Background:
- Polysulfide (PS) shuttling between electrodes causes rapid capacity fade in lithium-sulfur (Li-S) batteries, hindering commercialization.
- Existing electrolyte strategies face a trade-off between suppressing the shuttle effect and maintaining high battery capacity.
- Strongly coordinating electrolytes boost sulfur utilization but worsen polysulfide migration, often requiring LiNO3 additives for anode stability.
Purpose of the Study:
- To design a balanced electrolyte that suppresses polysulfide shuttling while maintaining high capacity in Li-S batteries.
- To investigate the correlation between solvent coordination strength, polysulfide solubility, LiNO3 concentration, and the shuttle effect.
- To optimize electrolyte composition for enhanced Li-S battery performance and longevity.
Main Methods:
- Utilized a binary solvent system combining tetrahydrofuran (THF) and cyclopentyl methyl ether (CPME) with varying ratios.
- Investigated the influence of solvent polarity (dielectric constant) on polysulfide dissolution and redox kinetics.
- Employed LiNO3 as an additive at a concentration of 0.7 M in the optimized THF:CPME electrolyte.
Main Results:
- Achieved 92% capacity retention over 100 cycles with the 4:1 THF:CPME electrolyte containing 0.7 M LiNO3, a ~20% improvement over conventional electrolytes.
- Demonstrated high Coulombic efficiency ranging from 99-100% with the novel electrolyte system.
- Confirmed the formation of a LiNO3-derived protective interphase and regulated polysulfide dissolution on electrode surfaces.
Conclusions:
- The balanced binary solvent electrolyte effectively suppresses the shuttle effect in Li-S batteries.
- Optimized solvent polarity and LiNO3 concentration enable sufficient polysulfide dissolution for robust kinetics without accelerating capacity decay.
- This strategy offers a promising pathway for developing high-performance and durable Li-S batteries.
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