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Bifunctional trifluoromethoxy-isocyanate additive promotes LiF/Li2O-enriched hybrid SEI for durable lithium metal batteries
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DOI：10.1016/j.jechem.2026.07.024.png)
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Abstract
En 中文
Lithium metal batteries (LMBs) are promising candidates for high energy density storage. However, practical implementation is impeded by intrinsic interfacial instability, leading to pronounced volume fluctuations and uncontrolled dendritic growth, particularly under lean-lithium conditions. Herein, 4-(trifluoromethoxy)phenyl isocyanate (TFMPI) is employed as a bifunctional electrolyte additive to regulate early interfacial reactions and construct a robust organic–inorganic hybrid solid electrolyte interphase (SEI). Through the combined effects of the –OCF3 and –NCO groups, TFMPI directs the formation of a gradient hybrid SEI featuring a rigid-flexible architecture that promotes more uniform Li+ transport, suppresses dendritic Li growth, and buffers interfacial stress during repeated plating/stripping, thereby improving the rate capability and cycling stability of LMBs. The electrolyte modified with TFMPI enables Li||LiFePO4 cells to retain ∼80% of their initial capacity after 1180 cycles at 1C. Even under the stringent condition of using a 50 μm thin Li, the cells still maintain 80.1% of their initial capacity after 450 cycles. This work highlights a functional-group-guided additive strategy to build durable interphases for practical LMBs.
Keywords:
Li metal batteries
Electrolyte additive
Hybrid interphase
TFMPI
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