Recent breakthroughs in high-voltage aqueous electrolytes have enabled the development of aqueous batteries with operating voltages exceeding 2.5 V, rivaling non-aqueous systems. By leveraging concentrated 'water-in-salt' electrolytes (WiSE), researchers have achieved electrochemical stability windows of up to 3.0 V, a significant improvement over traditional aqueous systems limited to ~1.23 V. For instance, a 21 m LiTFSI electrolyte demonstrated a cathodic stability of -1.5 V vs. SHE and anodic stability of +1.5 V vs. SHE, enabling high-energy-density cathodes like LiMn2O4 and LiCoO2 to operate efficiently in aqueous environments.
The stabilization of electrode-electrolyte interfaces is critical for high-voltage aqueous batteries. Advanced solid-electrolyte interphases (SEIs) formed by additives like fluoroethylene carbonate (FEC) have been shown to suppress hydrogen evolution and enhance interfacial stability. In one study, the addition of 2 wt% FEC reduced hydrogen evolution by 85% and increased Coulombic efficiency to >99%. These SEIs also mitigate dendrite formation, enabling the use of lithium metal anodes in aqueous systems for the first time, with cycle lifetimes exceeding 500 cycles at 1 mA/cm².
The development of hybrid electrolytes combining WiSE with organic co-solvents has further expanded the voltage window while reducing viscosity and improving ionic conductivity. For example, a hybrid electrolyte with 15 m LiTFSI and 20% ethylene carbonate exhibited a conductivity of 12 mS/cm at room temperature, compared to <10 mS/cm for pure WiSE. This approach has enabled the operation of high-capacity cathodes like LiNi0.8Co0.1Mn0.1O2 (NCM811) at voltages up to 4.3 V vs. Li/Li⁺ in aqueous systems, achieving specific capacities of >200 mAh/g with minimal capacity fade over 100 cycles.
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