4.5-V-Class Safe Lithium-Ion Batteries with Silicon-Majority-Graphite Anodes Enabled by Self-Limiting Interphase
Longji Xu1, Xue Han2, Jaekyung Sung3
1Center for Advancing Materials Performance from the Nanoscale (CAMP-Nano), State Key Laboratory for Mechanical Behavior of Materials, Xi'an Jiaotong University, Xi'an, Shaanxi, 710049, China.
Advanced Materials (Deerfield Beach, Fla.)
|November 17, 2025
Summary
A new hybrid-sulfonamide electrolyte (HSE) enables stable operation of high-voltage lithium-ion batteries with silicon-majority graphite anodes. This electrolyte forms a self-limiting interphase on silicon, enhancing cycling stability and safety.
Area of Science:
- Materials Science
- Electrochemistry
- Energy Storage
Background:
- High-energy lithium-ion batteries (LIBs) utilizing 4.5 V-class LiNi0.8Mn0.1Co0.1O2 (NMC811) cathodes and silicon-majority graphite (SmG) anodes offer energy densities exceeding 400 Wh kg-1.
- Key challenges for these advanced LIBs include poor cycling stability, safety concerns, and limited low-temperature performance, primarily due to difficulties in forming stable interphases.
- The aggressive electrochemical environment at high voltages and with silicon anodes necessitates novel electrolyte solutions.
Purpose of the Study:
- To develop a hybrid-sulfonamide electrolyte (HSE) capable of withstanding the harsh conditions of high-voltage NMC811 cathodes and silicon anodes.
- To engineer a self-limiting inorganic interphase on silicon anodes to improve battery performance and longevity.
- To demonstrate the practical application of this electrolyte in high-energy LIBs.
Main Methods:
- A novel hybrid-sulfonamide electrolyte (HSE) was synthesized and tested.
- The electrolyte's interaction with silicon anodes was investigated, focusing on the formation of a self-limiting interphase.
- Electrochemical performance was evaluated using NMC811||SmG coin cells and 1.4 Ah pouch cells, including cycling stability, temperature range, and thermal stability tests.
Main Results:
- The HSE successfully survived the aggressive chemistry of high-voltage NMC811 and programmed a self-limiting inorganic interphase on Si anodes.
- NMC811||SmG coin cells using HSE retained 80% capacity after 500 cycles at 4.5 V and operated effectively between -40 °C and 60 °C.
- 1.4 Ah pouch cells demonstrated 80.0% capacity retention after 1150 cycles and exhibited excellent thermal stability up to 300 °C.
Conclusions:
- The developed hybrid-sulfonamide electrolyte provides a viable solution for enhancing the stability and safety of high-energy LIBs.
- The self-limiting interphase formation on silicon anodes is a critical strategy for achieving long-cycle life in advanced battery systems.
- This work paves the way for practical electrolyte design targeting improved performance in next-generation lithium-ion batteries.
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