Lithium nitrate (LiNO3) has emerged as a critical additive for stabilizing the solid-electrolyte interphase (SEI) in lithium metal batteries (LMBs). Recent studies reveal that LiNO3 decomposes at the anode surface to form a robust, inorganic-rich SEI layer, significantly enhancing Coulombic efficiency (CE). For instance, a 2023 study demonstrated that adding 0.5 wt% LiNO3 to a conventional carbonate electrolyte increased the CE from 85.2% to 98.7% over 100 cycles at 1 mA/cm². This improvement is attributed to the formation of Li3N and Li2O compounds, which exhibit high ionic conductivity and mechanical stability. Moreover, LiNO3 suppresses dendritic growth by homogenizing lithium-ion flux, as evidenced by in situ atomic force microscopy (AFM) imaging showing a 75% reduction in dendrite height after 50 cycles.
The role of LiNO3 in mitigating electrolyte decomposition has been quantified through advanced spectroscopic techniques. Fourier-transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS) analyses reveal that LiNO3 reduces the formation of organic byproducts such as ROCO2Li and ROLi by up to 60%. This reduction is critical for minimizing impedance growth at the electrode-electrolyte interface. A 2022 study reported that cells with LiNO3 exhibited an interfacial resistance of only 12 Ω·cm² after 200 cycles, compared to 45 Ω·cm² in control cells. Additionally, nuclear magnetic resonance (NMR) studies confirm that LiNO3 enhances lithium-ion transference number from 0.34 to 0.52, improving rate capability and cycle life.
The impact of LiNO3 on high-voltage stability has been systematically investigated for next-generation LMBs with nickel-rich cathodes (e.g., NMC811). A recent breakthrough showed that adding 1 wt% LiNO3 to a dual-salt electrolyte (LiPF6-LiTFSI) extended the cycle life of NMC811||Li cells from 150 to 400 cycles at a cutoff voltage of 4.5 V. This improvement is attributed to the formation of a protective cathode-electrolyte interphase (CEI) enriched with NOx species, which inhibits transition metal dissolution and gas evolution. Gas chromatography-mass spectrometry (GC-MS) data confirmed a 90% reduction in CO2 evolution during cycling, highlighting the role of LiNO3 in enhancing electrochemical stability.
The scalability of LiNO3-based electrolytes has been validated through pilot-scale testing under realistic conditions. A large-format pouch cell (10 Ah) incorporating LiNO3 achieved an energy density of 350 Wh/kg with a capacity retention of 92% after 500 cycles at C/2 rate. Thermal runaway tests revealed that cells with LiNO3 exhibited a peak temperature increase of only 120°C under nail penetration, compared to >200°C for conventional cells, demonstrating improved safety. Furthermore, cost analysis indicates that adding LiNO3 increases electrolyte cost by less than $0.05/Wh, making it economically viable for commercialization.
Future research directions focus on optimizing LiNO3 concentration and exploring synergistic effects with other additives like fluoroethylene carbonate (FEC) and vinylene carbonate (VC). Preliminary results show that combining 0.5 wt% LiNO3 with FEC further enhances CE to >99% and reduces capacity fade to <0.05%/cycle over extended cycling (>1000 cycles). Advanced computational modeling predicts that tailored multi-additive formulations could push LMB energy densities beyond 500 Wh/kg while maintaining safety and longevity.
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