High-voltage cathodes (>4.5 V), such as Ni-rich NCM811 and LiCoO2 derivatives, require electrolytes with exceptional oxidative stability. Conventional carbonate-based electrolytes decompose above ~4.3 V, leading to rapid capacity fade (<50% retention after 100 cycles). Advanced fluorinated solvents like FEC and dimethyl carbonate derivatives have extended stability windows beyond ~5 V vs. Li/Li+, enabling stable cycling at high voltages with capacity retention >90% after 500 cycles at C/3 rates,Additive engineering plays a critical role in stabilizing high-voltage interfaces.LiPF6 salt decomposition products form HF which accelerates cathode degradation.Recent innovations include HF scavengers like tris(trimethylsilyl)phosphate(TMSPa)and lithium bis(oxalato borate)(LiBOB)
which reduce HF concentrations below detectable levels(<1 ppm)and improve capacity retention by up tp30%.These additives also enhance SEI formation on graphite anodes ensuring balanced performance across full cells."
The development of localized high-concentration electrolytes(LHCEs)has further pushed the boundaries of high-voltage operation.LHCEs utilize diluents like hydrofluoroethers(HFE)solvents reduce viscosity while maintaining solvation structures that stabilize reactive species.For example,a LHCE comprising1M LiFSI in DME:HFE(1:2 v/v)demonstrated capacity retention>95%after300 cycles at C/2 rates even when paired with ultra-high voltage cathodes(>4.V).
Computational modeling is accelerating the discovery of novel electrolyte formulations.Machine learning algorithms trained on experimental datasets containing thousands unique combinations identified key descriptors(e.g.,solvation energy,dipole moment)predicting oxidative stability.Recent findings revealed that asymmetric fluorinated carbonates exhibit superior stability windows(~V vs.Li/Li+)due their unique molecular configurations.
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