跳到主要內容區塊

Intrinsically Ductile Argyrodite Solid Electrolytes to Improve the Performance of All-Solid-State Lithium Batteries
本質延展性高的銀鍺石固態電解質提升全固態鋰電池性能


Berhanu Degagsa Dandena,  Liang-Ting Wu,  Tsung-I Yeh,  Chia-Yu Chang,  Jyh-Chiang Jiang*,  Dah-Shyang Tsai,  Martin Ihrig,  Gashahun Gobena Serbessa,  Sheng-Chiang Yang,  Keseven Lakshmanan,  Hwo-Shuenn Sheu,  Chia-Hsin Wang,  She-Huang Wu*,  Wei-Nien Su*,  Bing Joe Hwang*
https://doi.org/10.1016/j.cej.2025.162450
SEED Member: Jyh-Chiang Jiang, She-Huang Wu, Wei-Nien Su, Bing Joe Hwang

 

Schematic illustration.

 

Major Contributions

1. Development of a Ductile Ga-Doped Li-Argyrodite Solid Electrolyte:
A novel Li6.1P0.95Ga0.05S5Cl solid electrolyte was synthesized by doping with liquid metal gallium, resulting in outstanding mechanical properties. This electrolyte exhibits enhanced ductility, higher density, and reduced formation of voids and cracks compared to undoped counterparts, as confirmed by stress–strain analysis, loading–unloading curves, and density measurements.

2. Superior Interfacial Stability and Dendrite Suppression:
The Ga-doped electrolyte demonstrates exceptional interfacial compatibility with lithium metal anodes. The formation of a Li-Ga alloy at the interface promotes uniform lithium deposition, achieving a critical current density of 14.75 mA cm−2 without dendrite penetration or mechanical fractures. Long-term cycling tests reveal remarkable stability, with no significant increase in overpotential or interfacial resistance after extended operation.

3. Enhanced Electrochemical and Thermal Performance in Full Cells:
When applied in full cells with high-nickel cathodes (NCM811), the Ga-doped electrolyte delivers superior capacity retention, higher Coulombic efficiency, and minimal heat evolution during cycling. This indicates improved compatibility with both lithium metal anodes and oxygen-releasing cathode materials, supporting the potential for commercialization of sulfide-based all-solid-state lithium batteries.



主要貢獻

1. 開發具延展性的Ga摻雜鋰銀鍺石固態電解質
成功合成以液態金屬鎵摻雜的Li6.1P0.95Ga0.05S5Cl固態電解質,展現出優異的機械性能。該電解質相較於未摻雜者,具有更高的延展性、更高的密度,且明顯減少了孔隙與裂縫的產生,這些特性已透過應力—應變分析、壓縮—卸載曲線及密度測量得到驗證。

2. 優異的界面穩定性與鋰枝晶抑制能力:
Ga摻雜電解質展現出與鋰金屬負極極佳的界面相容性。在界面上形成的Li-Ga合金有助於鋰均勻沉積,實現14.75 mA cm−2的臨界電流密度,無枝晶穿透或機械斷裂。長循環測試顯示,該材料在長時間運作後並未出現過電位或界面阻抗顯著增加,展現極高穩定性。

3. 全電池中優異的電化學與熱穩定表現:
應用於高鎳正極(NCM811)的全電池中,Ga摻雜電解質展現出更佳的容量保持率、更高的庫倫效率,且在循環過程中產生的熱量極低,顯示與鋰金屬及釋氧正極材料均具良好相容性,為硫化物基全固態鋰電池的商業化提供有力支撐。