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研究生： 張瑜芳
Zhang, Yu-Fang
論文名稱： 表面披覆二氧化鈦無鈷富鋰層狀正極材料之電化學性質
Electrochemical properties of TiO2-coated Cobalt free Lithium rich Layered Oxide Cathodes
指導教授： 劉全璞
Liu, Chuan-Pu
學位類別： 碩士
Master
系所名稱： 工學院 - 材料科學及工程學系
Department of Materials Science and Engineering
論文出版年： 2025
畢業學年度： 113
語文別： 中文
論文頁數： 114
中文關鍵詞： 無鈷 、富鋰 、TiO2披覆 、水熱法 、層狀正極材料
外文關鍵詞： cobalt-free, Layer structure, Cathode material, TiO2 coating
相關次數： 點閱：11  下載：0 
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    • 近年來，隨著電動車的發展及綠能政策的走向帶動了智慧電網與儲能裝置的需求，具有高能量密度的鋰離子電池成為了現在大眾所關注的要點。而在鋰離子電池系統中，正極材料除了要在電容量及工作電壓上扮演著重要角色，也大幅影響了成本，而現在為因應政策還得需思考環境友善的問題，在如此多方考量下，要開發出高能量密度的正極材料，是研究正極材料中十分重要的一環。而無鈷富鋰層狀正極材料(LMNO)具有低成本、環境友善等特性，且能量密度可高達1000Wh/kg，遠超越目前所有商用正極材料。然而，其卻因材料內部易引發不可逆的相轉變而使可用電容與平均電壓隨充放電循環迅速衰減，而較差的導電性也使無鈷富鋰正極材料無法應用於高速充放電循環中問題。
    而為了解決上述問題，以發揮無鈷富鋰層狀正極材料的優點，本研究使用使用水熱法；一種簡單的濕式化學披覆的方式披覆TiO2-Bronze，藉由控制披覆濃度及後退火溫度的方式了解披覆TiO2-Bronze相的正極材料之電化學反應，而在後續對披覆過後的材料進行分析，可以發現TiO2-Bronze的披覆可以提高正極材料之電容量及在不同退火溫度下對過渡金屬析出的解決能力。

    In recent decades, the growing demand for high energy density has intensified research interest in lithium-ion batteries (LIBs). Specifically cobalt-free lithium- and manganese-rich layered oxides (LMNOs) have high theoretical energy density (exceeding 1000 Wh/kg), low cost, and environmental benignity. However, LMNO, suffer from structural instability. This structural degradation results in severe voltage and capacity fading.In this study, LMNO cathode were synthesized via a carbonate co-precipitation method. For the first time, the electrochemical performance of LMNO coated with a TiO₂-bronze phase was systematically investigated. The results demonstrate that TiO₂-coated LMNO exhibits a significantly enhanced initial discharge capacity of 342.5 mAh/g, along with excellent capacity retention. After 100 cycles, the discharge capacity remains above 200 mAh/g, indicating the effectiveness of the TiO₂-bronze coating in mitigating capacity degradation and improving cycling stability.

    摘要 i Extended Abstract ii 致謝 xvii 目錄 xix 表目錄 xxiii 圖目錄 xxiv 第一章 緒論 1 1.1 前言 1 1.2 研究動機與目的 1 第二章 理論基礎與文獻回顧 2 2.1 鋰離子電池介紹 2 2.1.1 鋰離子電池工作原理 2 2.1.2 鋰離子電池材料組成 3 2.1.2.1 正極 (Cathode) 4 2.1.2.2 負極 (Anode) 5 2.1.2.3 電解質 (Electrolyte) 6 2.1.2.4 隔離膜 (Separator) 8 2.2 正極材料介紹 9 2.2.1 層狀正極材料 (Layered-typed cathode) 9 2.2.2 尖晶石正極材料 (Spinel-typed cathode) 11 2.2.3 橄欖石正極材料 (Olivine-typed cathode) 13 2.3 富鋰正極材料(Li-Rich Cathodes) 14 2.3.1 富鋰正極材料之結構 14 2.3.2 富鋰正極材料之電化學特性 15 2.3.3 富鋰正極材料當前困境 17 2.4 提升電化學特性之方法 18 2.4.1 化學成分改質 18 2.4.1.1 離子摻雜 (Ion doping/Substitution) 18 2.4.1.2 殼層組合 (Core-Shell Composition) 19 2.4.2 表面披覆 (Surface coating) 20 2.5 二氧化鈦介紹 21 2.5.1 板鈦礦 (Brooklite) 22 2.5.2 銳鈦礦 (Anatase) 23 2.5.3 金紅石 (Rutile) 24 2.5.4 TiO2-B (Bronze) 25 第三章 實驗步驟與分析方法 26 3.1 富鋰正極粉末材料合成與披覆方法 26 3.1.1 共沉法(Co-precipitation)備置富鋰正極粉末材料 26 3.1.2 水熱法(Hydrothermal method)進行二氧化鈦(TiO2-B)之表面披覆 27 3.2 電極製備與鈕扣型半電池組裝 28 3.2.1 電極製備 28 3.2.2 鈕扣型半電池組裝 28 3.3 材料分析儀器 29 3.3.1 高解析掃描式電子顯微鏡 (High Resolution Scanning Electron Microscope, SEM) 29 3.3.2 高解析穿透式電子顯微鏡 (Ultrahigh Resolution Transmission Electron Microscope, TEM) 31 3.3.3 X光光電子能譜儀 (X-Ray Photoelectron Spectrometer, XPS) 32 3.3.4 X光繞射儀 (X-ray Diffractometer, XRD) 33 3.3.5高解析感應耦合電漿質譜分析儀 (Inductively coupled plasma-mass spectrometer) 34 3.4 電化學分析儀器 35 3.4.1 電池充放電循環測試 (Electrochemical cycling tests) 35 3.4.2 電化學阻抗分析 (Electrochemical Impedance Spectroscopy, EIS) 35 第四章 結果與討論 37 4.1 富鋰正極Li1.2NixMn0.8-xO2粉材 37 4.1.1 材料分析 37 4.1.1.1 富鋰正極Li1.2NixMn0.8-xO2粉材化學成分分析 37 4.1.1.2 Li1.2NixMn0.8-xO2 晶相結構分析 38 4.1.1.3 Li1.2NixMn0.8-xO2 表面形貌與微觀結構分析 40 4.1.1.4 Li1.2NixMn0.8-xO2 表面元素價態鑑定 42 4.1.2 電化學性能分析 44 4.2 不同濃度TiO2包覆Li1.2NixMn0.8-xO2之影響 46 4.2.1 材料分析 46 4.2.1.1 Li1.2NixMn0.8-xO2@TiO2晶相結構分析 46 4.2.1.2 Li1.2NixMn0.8-xO2 表面形貌與微觀結構分析 47 4.2.2 電化學性能分析 49 4.3 不同後退火溫度對TiO2包覆Li1.2NixMn0.8-xO2之影響 51 4.3.1 材料分析 51 4.3.1.1 Li1.2NixMn0.8-xO2 晶相結構分析 51 4.3.1.2 Li1.2NixMn0.8-xO2 表面形貌與微觀結構分析 52 4.3.2 電化學性能分 54 4.4 Li1.2NixMn0.8-xO2與最佳化TiO2包覆參數之比較 56 4.4.1 材料分析 56 4.4.1.1 化學成分分析 56 4.4.1.2 微觀結構分析 57 4.4.1.3 表面元素價態鑑定 59 4.4.2 電化學性能分析 63 4.4.2.1 首圈充放電性能與循環測試 63 4.4.2.2 微分容量 dQ/dV 測試 66 4.4.2.3 倍率性能測試 68 4.4.2.4 電化學阻抗頻譜 69 第五章 結論 73 第六章 參考文獻 74

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