High-entropy electrolytes (HEEs) represent a paradigm shift in battery chemistry by leveraging multi-component systems to achieve unprecedented stability. Recent studies have shown that HEEs composed of five or more salts (e.g., LiPF6, LiTFSI, LiFSI) exhibit ionic conductivities exceeding 5 mS/cm at -20°C, outperforming conventional electrolytes by >50%. The entropy-driven mixing suppresses crystallization and enhances thermal stability up to 300°C, making HEEs ideal for extreme environments.
The electrochemical stability window of HEEs has been extended to >5 V vs. Li/Li+, enabling compatibility with high-voltage cathodes like NMC811 (>4.3 V). This is achieved through synergistic interactions among multiple anions, which form stable solid-electrolyte interphases (SEIs) on both anode and cathode surfaces. Experimental data shows SEI thicknesses of <10 nm with minimal impedance growth (<5%) after 1,000 cycles at C/2 rates.
HEEs also mitigate gas evolution during cycling, a common issue in lithium-ion batteries (LIBs). By incorporating fluorinated solvents and additives like vinylene carbonate (VC), gas generation is reduced by >80% compared to traditional electrolytes. This improvement is critical for pouch cell designs where gas accumulation can lead to swelling and safety hazards.
Despite their advantages, HEEs face challenges related to cost and scalability due to the complexity of multi-salt formulations. Current research focuses on optimizing salt ratios using machine learning algorithms to minimize costs while maintaining performance metrics.
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