High-entropy electrolytes (HEEs) represent a paradigm shift in battery chemistry by leveraging multi-component systems to achieve unprecedented ionic conductivities and electrochemical stability windows (>6 V). Recent studies have shown that HEEs composed of five or more salts (e.g., LiPF6, LiTFSI, LiFSI, LiBOB) in optimized ratios can achieve ionic conductivities exceeding 20 mS/cm at room temperature. These systems also exhibit enhanced thermal stability up to 200°C, making them suitable for extreme fast charging (XFC) applications requiring charge rates above 6C.
The unique solvation structure of HEEs contributes to their superior performance. Molecular dynamics simulations reveal that multi-ion interactions reduce ion pairing and increase free ion concentrations by up to 50% compared to conventional electrolytes. This results in lower activation energies (<0.2 eV) for ion transport and higher transference numbers (>0.6), which are critical for minimizing polarization during XFC. Experimental validation using NMR spectroscopy has confirmed these findings, showing improved Li+ mobility even at sub-zero temperatures (-20°C).
Interfacial stability is another key advantage of HEEs. The formation of robust solid-electrolyte interphases (SEIs) enriched with inorganic components like LiF and Li3N has been observed using X-ray photoelectron spectroscopy (XPS). These SEIs exhibit thicknesses below 10 nm and resist degradation even after >1000 cycles at rates above 4C. Additionally, HEEs mitigate cathode-electrolyte interface degradation by forming protective surface layers on high-voltage cathodes such as NMC811 and LNMO.
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