Major Contributions

1.Development of a Novel BTCMP-Based Additive for LHCEs
We introduced Bis(2,2,2-trifluoroethyl) (methoxycarbonylmethyl)phosphonate (BTCMP), a fluorinated phosphonate-based additive for localized high-concentration electrolytes (LHCEs). This innovative additive effectively modifies the solvation structure of the electrolyte, dispersing ion aggregates into smaller fragments, which enhances lithium-ion transport and stabilizes the cathode electrolyte interphase (CEI). Our additive also suppresses solvent decomposition, as confirmed by Density Functional Theory (DFT) analysis, leading to improved interfacial stability and battery performance.

2.Enhanced Battery Performance and Safety
By incorporating BTCMP into LHCEs, we achieved significant improvements in cycling stability and safety. For instance, in Li||LNMO cells, our BTCMP-based electrolyte retained 82% of its initial capacity after 200 cycles at 0.5 C, compared to only 47.2% retention for the pristine LHCE after 150 cycles. Additionally, the BTCMP-based electrolyte demonstrated flame-retardant properties, making it safer than conventional commercial electrolytes.

3.Formation of a Stable SEI and CEI
Our research revealed that BTCMP promotes the formation of fluorine-rich solid electrolyte interphase (SEI) and CEI layers, primarily composed of lithium fluoride (LiF). These layers enhance lithium-ion transport and prevent dendritic growth on the lithium metal anode. The resulting stable interphases improve both the safety and longevity of lithium metal batteries while reducing transition metal dissolution from the cathode.


主要貢獻

1.開發基於BTCMP的新型添加劑以提升LHCE性能
我們引入了一種新型含氟磷酸酯基添加劑——Bis(2,2,2-trifluoroethyl) (methoxycarbonylmethyl)phosphonate (BTCMP)，用於局部高濃度電解液（Localized High-Concentration Electrolytes, LHCE）。這種創新的添加劑有效地改變了電解液的溶劑化結構，將離子聚集體分散為更小的碎片，從而提升鋰離子遷移能力並穩定陰極電解質界面（Cathode Electrolyte Interphase, CEI）。此外，BTCMP還抑制了溶劑分解，這一點通過密度泛函理論（DFT）分析得到證實，從而顯著改善了界面穩定性和電池性能。

2.提升電池的循環穩定性與安全性
我們的BTCMP基LHCE在循環穩定性和安全性方面表現出色。例如，在Li||LNMO電池中，BTCMP基電解液在0.5 C條件下經過200次循環後仍能保持82%的初始容量，而未添加BTCMP的LHCE僅能在150次循環後保持47.2%的容量。此外，BTCMP基電解液展現了阻燃特性，相比傳統商用電解液更為安全。

3.形成穩定且富含氟的SEI與CEI層
我們的研究表明，BTCMP促進了富含鋰氟化物（LiF）的固態電解質界面（Solid Electrolyte Interphase, SEI）和CEI層的形成。這些層提高了鋰離子傳輸性能並防止鋰金屬負極上的枝晶生長。穩定的界面結構不僅提升了鋰金屬電池的安全性與壽命，還減少了來自陰極材料的過渡金屬溶解。