Schematic demonstration of (a) the Lewis acid–base formation between LPSC and Lewis acid additive. (b) Schematic illustration of LPSC-H2O reaction suppression using Lewis acid additives (c) to (h).

Major Contributions

1.Enhanced Moisture Stability of Li₆PS₅Cl through Lewis Acid Treatment
We developed a novel method to improve the moisture robustness of Li₆PS₅Cl (LPSC) by treating it with Lewis acid additives at the nanoscale. This treatment forms a Lewis acid-base interaction between the additives and sulfur atoms in LPSC, effectively shielding it from moisture-induced degradation. This approach successfully suppresses the generation of toxic H₂S gas and maintains the structural integrity of LPSC under humid conditions.

2.Preservation of Ionic Conductivity Post-Treatment
Our method ensures that ionic conductivity remains largely intact after treatment with specific Lewis acid additives, such as triphenyl carbenium tetrafluoroborate (tpctfb), tritylium hexafluorophosphate (tthfp), and aluminum acetylacetonate (acaca). These additives minimally impact lithium-ion mobility, making the treated LPSC suitable for practical applications without compromising electrochemical performance.

3.Validation in All-Solid-State Batteries
We demonstrated the practical applicability of Lewis acid-treated LPSC in ASSBs. Even after exposure to humid air, cells utilizing treated LPSC retained significant capacity and structural stability compared to untreated samples, which suffered severe degradation. This highlights the potential of our approach to enable durable and high-performance ASSBs under real-world conditions.


主要貢獻

1.透過路易斯酸處理提升Li₆PS₅Cl的耐濕穩定性
我們開發了一種創新方法，利用在奈米尺度上添加路易斯酸添加劑來處理Li₆PS₅Cl（LPSC），顯著提升其耐濕穩定性。這種處理方法通過在路易斯酸添加劑與LPSC中的硫原子之間形成路易斯酸-鹼相互作用，有效地防止了濕氣引起的降解。此方法成功抑制了有毒H₂S氣體的生成，並在潮濕環境下保持LPSC的結構完整性。

2.處理後保持離子導電性不受影響
我們的方法確保經過特定路易斯酸添加劑（如三苯甲鎓四氟硼酸鹽(tpctfb)、三苯甲鎓六氟磷酸鹽(tthfp)和鋁乙酰丙酮(acaca)）處理後，LPSC的離子導電性幾乎不受影響。這些添加劑對鋰離子遷移性的影響極小，使得經處理的LPSC在不犧牲電化學性能的情況下適合實際應用。

3.在全固態電池中的應用驗證
我們進一步驗證了經路易斯酸處理的LPSC在全固態電池中的實際應用價值。即使在暴露於潮濕空氣後，使用經處理LPSC的電池仍然能夠保持顯著的容量和結構穩定性，而未處理樣品則因結構劣化而性能大幅下降。這表明我們的方法能夠有效增強全固態電池在實際環境中的耐久性和性能表現。