鋰離子電池電極上生成鈍性膜(solid liquid interface, SEI)的組成和形態對於電池的性能有顯著影響。微量雜質如水的存在是六氟磷酸鋰(LiPF6)裂解的主要原因。所分解產物進一步與水反應生成酸。這些非離子傳導性的產物沉積在SEI上，加上酸與SEI成分發生化學反應都將導致SEI特性的惡化。本論文旨在開發新型電解液添加劑和電化學處理程序，以減少水/酸等雜質對於電池系統效能的損害。主要係針對石墨負極，追求電解液添加劑的協同效用，以達高效和有效生成SEI膜，能對較寬的工作溫度範圍達到性能提升的目的。內文對於電解質添加劑和電化學處理方法對石墨電極的效果，SEI表面組成和電解液穩定性都做了深入的研究。
考慮的氮矽(N- Si)鍵的路易斯鹼特性，提出1-三甲基甲矽烷咪唑（1-TMSI）作為一種新型的電解液除水添加劑，來抑制的六氟磷酸鋰的分解。通過實驗和密度泛函理論（DFT）計算，吾人針對1-TMSI對MCMB電極和電解質之間的除水能力，以及所產生的界面化學功效進行研究。核磁共振分析(NMR)顯示，通過0.2體積％1-TMSI的添加，可有效地抑制由水所造成的六氟磷酸鋰分解。以XPS表面分析表徵MCMB電極，發現1-TMSI的存在可降低六氟磷酸鋰分解所生成離子絕緣性產物的沉積。這些證據都指向使用1-TMSI添加劑的電池較未添加的電池，可藉由促進生成有較佳離子傳導性的鈍性膜（SEI），達到更好的性能表現。
關於電解液添加劑的協同作用，乃針對常見的電解質成分的性質 -碳酸乙烯酯（EC）和氟代碳酸乙烯酯（FEC），探討添加 4-氯甲基-1,3,2- dioxathiolane -2-氧化物（CMDO）來改善前述成分的作法。MCMB電極因碳酸丙烯酯（PC）為主的電解液界面所產生的電極鈍化層，亦發現添加CMDO可以有效降低不可逆電容量的損失和形成較薄的鈍化膜。事實上，三種添加劑的組合起了關鍵作用，提高MCMB電極在較低溫或室溫環境下的可逆電容量。電化學測定分析顯示，通過使用三種添加劑的混合物，所形成的鈍性膜能讓鋰離子更容易地嵌入嵌出。
通過對電解液施加定電位的電化學處理程序，可避免有機電解液中的水雜質所致的負面影響。電化學處理後，刻意摻水的電解質中所測量的水量顯著下降。此外，處理後的Li/ MCMB電池的電化學測試中亦顯示，可對產生Li/ MCMB電池的特性產生積極的作用，並藉以改善Li/MCMB電池的性能，顯示此電化學處理程序可避免有機電解液中水雜質，具有發展潛力。

The composition and morphology of solid electrolyte interphase (SEI) plays a significant role on the performance of lithium ion batteries. The presence of trace impurities such as water causes decomposition of LiPF6. The decomposed product further reacts with water and leading to form acid. The deposition of ionic insulating products on SEI and the reaction of acid with SEI components cause SEI deterioration. In this work, electrolyte additive and electrochemical process have been developed to reduce water/acid impurities and minimize their effect to overall degradation of cell system. In addition, synergetic effect of electrolyte additives is achieved for efficient and effective SEI former to enhance performance of graphite electrode for wide temperature range. The effect of electrolyte additives and electrochemical process on the performance of graphite electrode, surface composition and electrolyte stability have been investigated in detail.

Considering the Lewis-base feature of N-Si bond, 1-(Trimethylsilyl)imidazole (1-TMSI) is proposed as a novel water scavenging electrolyte additive to suppress LiPF6 decomposition. The scavenging ability of 1-TMSI and beneficiary interfacial chemistry between the MCMB electrode and electrolyte are studied through a combination of experiments and density functional theory (DFT) calculations. NMR analysis indicated that LiPF6 decomposition by water was effectively suppressed in the presence of 0.2 vol % 1-TMSI. XPS surface analysis of MCMB electrode showed that the presence of 1-TMSI reduced deposition of ionic insulating products caused by LiPF6 decomposition. The results showed that the cells with 1-TMSI additive have better performance than the cell without 1-TMSI by facilitating the formation of solid-electrolyte interphase (SEI) layer with better ionic conductivity.
Synergetic effect of electrolyte additives was explored. 4-(Chloromethyl)-1,3,2-dioxathiolane-2-oxide (CMDO) was prepared to improve the properties of commonly used electrolyte constituents - ethylene carbonate (EC), and fluoroethylene carbonate (FEC). The formation of efficient passivation layer in Propylene Carbonate (PC)-based electrolyte for MCMB electrode was investigated. The addition of CMDO resulted in a much less irreversible capacity and induces thin SEI formation. In fact, the combination of the three additives played a key role to enhance reversible capacity of MCMB electrode at lower or ambient temperature. The electrochemical measurement analysis showed that the SEI formed by using a mixture of the three additives gave better intercalation-deintercalation of lithium ions.
The electrochemical treatment process was performed by applying voltage to avoid water impurity from organic electrolyte. After electrochemical treatment, the electrolyte with intentionally added water showed the measured water amount was significantly decreased. In addition, the electrochemical performance test of Li/MCMB cells showed that the electrochemical treatment has a positive effect on the electrolyte to improve the performance of Li/MCMB cells. The electrochemical treatment method is promising in avoiding water impurity from organic electrolyte.

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