由於過量鋰材料擁有高比電容量~270 mAhg-1及高工作電壓特性，近十年受到廣泛的研究。然而，因其導電性不佳、於長圈數測試下電壓衰退及界面的不穩定性，導致尚無法導入實際應用。
本研究分為兩個策略進行，一為增加粉體之導電性，藉由低濃度乙烯與氬氣之混合氣於過量鋰粉體作化學氣相沉積，使得由乙烯所裂解的碳沉積於過量鋰粉體上，以提升粉體之導電性。二為增加粉體之穩定性，藉由低濃度氫氣和二氧化碳與氬氣之混合氣於過量鋰粉體表面作化學氣相沉積，於反應後，形成一穩定有機碳層(人工固態電解質界面)包覆過量鋰粉體，以提升粉體之界面穩定性和充放電穩定性。除了分別針對上述兩種製程作討論之外，本研究亦嘗試將兩種製程作不同順序結合，再比較單一製程改質之樣品與未改質前粉體之結構及電化學性能差異。
經雙重改質後，於粒子表面形成3 奈米穩定碳層及碳酸鋰沉積，且造成表面約5奈米深度的主體結構，由原本的層狀轉為類尖晶石狀。此雙重改質程序製備之樣品，於高速率充放電3C之電流下，仍有~80 mAhg-1之電容量；於穩定性方面，於110圈之充放電測試，亦具有85.7%之電容量維持率，較未改質前之樣品高出5.4%。
本研究針對過量鋰正極氧化物建立一化學氣相沉積改質程序，在不影響結構的情況下，成功於還原性之碳源氣氛下，進行碳沉積和生成人工固態電解質界面，以提升電化學效能。本研究發現先以碳沉積，再於表面形成穩定碳層之雙重改質樣品(C1S4)，於影響結構最少情況下，得到最佳的穩定性，且提升導電性和降低阻抗。

關鍵字：過量鋰、正極材料、表面改質、化學氣相沉積、碳改質、固態
電解質界面、界面穩定性、導電性。

Lithium-rich cathode materials are drawing high attention recently as next generation cathode materials for Li-ion battery due to its high operating voltage and high capacity ~270 mAhg-1. However, its poor electronic conductivity, rapid voltage fading during cycles and interphase instability still hinder its practical applications.
This study consists of two parts: first, to deposit carbon on Li rich powders by chemical vapor deposition (CVD) with dilute ethylene and argon for enhancing electronic conductivity of powder. Second, to form a carbonaceous layer (Artificial SEI layer) covering Li-rich particles by CVD with a mixture of gases of dilute hydrogen, carbon dioxide and argon with the aim of enriching high stability and interface stability.
The effects of the combination and applied sequence of two aforementioned approaches on the properties and electrochemical performance of cathode powders are also studied and compared against the individually treated and pristine materials.
In the results and discussion part, the modified powders are examined by bulk/surface structure and surface composition separately. Finally, it is summarized by enhanced electrochemical properties without impairing bulk structure.
The most potential modified sample, C1S4, was coated by CVD carbon deposition first, followed by the coverage of 3 nm carbonaceous layer and Li2CO3 growth on the Li-rich powder surface. It is also to note that a spinel-like structure was also formed in the depth of 5 nm. Overall, the C1S4 modified sample delivered a discharging capacity as high as 80 mAhg-1 at 3C and high retention of 85.7% after 110 cycling test, which surpassed the pristine powder, 5.4% higher.
This research sheds light on carbon coating and carbonaceous layer covering as an artificial SEI layer onto Li-rich cathode material with novel combination of reducing gases via CVD. The improved material performance and the process features make this proposed surface modification method suitable for production in near future.

Keywords: Lithium-rich, cathode material, surface modification, carbon coating, solid electrolyte interphase, interphase stability, electronic conductivity.

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