鑑於將鋰電池應用於儲能系統和電動車的需求逐年攀升，發展具高能量密度的高效能鋰電池如全固態鋰金屬電池及無陽極鋰金屬電池，對於進一步提升鋰電池的能量密度及安全性至關重要。然而學界對於固態聚合物電解質與鋰金屬陽極之間的界面反應仍缺乏瞭解，同時也缺少材料設計的方針。現今高分子電解質仍需面對如導離度低及於陽極上不可逆的分解等問題，同時無陽極鋰金屬電池也需克服嚴重的活性鋰損失。為了解決上述難題，設計具有適當導離度且能形成有效鈍化電極表面之固態電解質介面層的新型聚合物電解質極其重要。
此研究使用了密度泛函理論與第一原理分子動力學研究固態聚合物電解質與陽極表面的界面反應。主要專注於各種聚合物 (PEO、PCL、PEC、PTMC、PTeMC、POHM) 及鋰鹽 (LiTFSI、LiBF4、LiBOB、LiDFOB) 於鋰金屬陽極上的分解反應以建立完整的分解反應網絡，計算結果可用於釐清和解釋實驗中觀察到的現象及預測該電解質之分解產物，經由監測各種電解質所產生的降解產物，並可分析其在固態電解質介面層的作用，可用於進一步評估此電解質的電化學性能。另外無陽極鋰金屬電池中常以銅金屬作為集電器材料，因此，研究銅金屬於電解質分解中扮演的角色及鋰金屬於銅集電器上之電沉積作用，也為本研究之重點。根據計算結果發現，當銅作為集電器時，可誘導出聚合物與鋰金屬之間獨特的協同作用力，可加速聚合物上羰基的分解。最後，本研究也針對一現有的自修復聚合物電解質進行分子間作用力與鋰離子傳導路徑之計算，同時也模擬該電解質於鋰-銅陽極表面的分解現象，此一結果對於設計新型電解質提供了重要的見解。具體來說，本研究提出了數種新型的自修復單離子傳導聚合物，可望其具有適當的導離度、能於陽極表面形成穩定的鈍化層，同時可引導鋰離子於陽極表面均勻的沉積，如此一來預期可提高鋰電池之循環性能。整體來說，本研究旨在透過理論計算與分子模擬，增進讀者對於聚合物電解質與陽極之間界面反應的理解，同時也期望為未來的實驗研究者於聚合物設計提供指導，促進高效能聚合物電解質之研發。

Given the increasing demand for lithium batteries in energy storage systems and electric vehicles, there is a need to develop high-performance lithium batteries, such as all-solid-state lithium metal batteries (ASSLMBs) and anode-free lithium metal batteries (AFLMBs). These advancements are crucial for improving the energy density and safety of lithium batteries. However, there is still a lack of knowledge regarding the interfacial reactions of solid-state polymer electrolytes (SPEs) on the Li-metal anode surface, and a comprehensive guideline for materials design is yet to be established. Currently, SPEs face challenges including low ionic conductivity and irreversible electrolyte degradation on the reactive Li-metal anode. AFLMBs, on the other hand, suffer from significant active Li loss. To address these issues, it is crucial to design polymers with suitable ionic conductivity and the ability to form an effective passivation layer, known as the solid electrolyte interphase (SEI) layer.
This work has employed density functional theory (DFT) calculations and ab initio molecular dynamics (AIMD) simulations to investigate the interfacial reactions between SPEs, composed of polymers (PEO, PCL, PEC, PTMC, PTeMC, and POHM) and Li salts (LiTFSI, LiBF4, LiBOB, and LiDFOB), with a Li-metal anode. The focus is on understanding the decomposition mechanisms of different polymers and Li salts, and establishing a reaction network. The computational results have demonstrated their utility in clarifying experimental observations and predicting the degradation products. The resulting degradation products of each system were monitored to analyze their role in the SEI layer, and further evaluate the electrochemical performance of SPEs. On the other hand, the role of Cu as an anodic current collector in AFLMBs and the Li-plating process on the Cu surface is investigated in this study. It is observed that the presence of Cu on the Li/Cu surface influenced the reactivity of carbonyl-containing polymers due to unique cooperative interactions between the polymer and Li induced by the Cu substrate. Additionally, the study delved into the driving force behind the self-healing property, the Li diffusion pathway, and the interfacial degradation of self-healing polymer electrolytes. These investigations provided useful computational insights for the design of novel polymer materials. Specifically, this study has proposed several self-healing single-ion conducting polymer electrolytes, which hold promise for the application of Li-metal batteries. These electrolytes are expected to exhibit suitable ionic conductivity, promote the formation of a stable SEI layer on the Li surface, and facilitate uniform Li plating during the plating process, which helps to enhance the battery's cycling stability. Overall, the computational results play a crucial role in enhancing the understanding of the SPE-anode interfacial reactions. They provide guidance for future experimental investigations and facilitate the design of more efficient SPE materials.

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