Sodium bis(oxalato)borate (NaBOB) has emerged as a transformative electrolyte additive for high-voltage lithium-ion batteries, enabling stable operation at voltages exceeding 4.5 V. Recent studies have demonstrated that NaBOB forms a robust cathode-electrolyte interphase (CEI) on high-nickel cathodes, significantly reducing transition metal dissolution and electrolyte decomposition. In experiments with LiNi0.8Co0.1Mn0.1O2 (NCM811) cathodes, cells with 2 wt% NaBOB exhibited a capacity retention of 92.3% after 500 cycles at 4.6 V, compared to 68.7% for baseline electrolytes. The CEI layer formed by NaBOB was found to be rich in boron-oxygen compounds, as confirmed by X-ray photoelectron spectroscopy (XPS), with a thickness of ~5 nm, providing both ionic conductivity and electronic insulation.
The role of NaBOB in suppressing gas evolution during high-voltage cycling has been extensively investigated using in situ differential electrochemical mass spectrometry (DEMS). At 4.8 V, cells with NaBOB additives showed a 78% reduction in CO2 evolution and a 65% reduction in O2 release compared to control cells. This is attributed to the preferential oxidation of oxalate anions over carbonate solvents, forming a stable passivation layer. Furthermore, thermal stability tests revealed that NaBOB-containing electrolytes exhibited a delayed onset temperature for exothermic reactions by ~15°C, with peak heat flow reduced from 120 mW/mg to 85 mW/mg during accelerated rate calorimetry (ARC) testing.
NaBOB's impact on ionic conductivity and charge transfer kinetics has been quantified through electrochemical impedance spectroscopy (EIS). At room temperature, electrolytes with 1 wt% NaBOB demonstrated an ionic conductivity of 10.2 mS/cm, only slightly lower than the baseline's 11.5 mS/cm, while the charge transfer resistance decreased by 42% from 18 Ω to 10.5 Ω at the cathode interface. This improvement is linked to the formation of boron-rich species that facilitate lithium-ion transport across the CEI layer.
The economic and environmental implications of NaBOB adoption have been evaluated through life cycle assessment (LCA). Incorporating NaBOB into commercial battery production could reduce electrolyte costs by up to 12% due to extended cycle life and reduced need for additives like vinylene carbonate (VC). Additionally, the use of NaBOB could decrease the carbon footprint of battery manufacturing by ~8%, primarily through reduced material consumption and waste generation over the battery's lifetime.
Future research directions focus on optimizing NaBOB concentration for specific cathode chemistries and exploring its compatibility with solid-state electrolytes. Preliminary results show promising synergy between NaBOB and sulfide-based solid electrolytes, with interfacial resistance reduced by ~30% at room temperature when using optimized formulations.
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