高熵氧化物應用於鋰離子電池負極並探討最佳負極/正極配方

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姓名

吳奕廷(Yi-Tin Wu) 查詢紙本館藏

畢業系所

材料科學與工程研究所

論文名稱

高熵氧化物應用於鋰離子電池負極並探討最佳負極/正極配方
(High Entropy Oxides for lithium-ion battery Anode and study the best ratio of Anode/Cathode)

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至系統瀏覽論文 (2027-9-1以後開放)

摘要(中)

近年來因著科技發展快速，鋰離子電池的普及率也隨之上升。本研究利用溶膠凝膠自動燃燒法合成具有單相岩鹽結構之高熵氧化物(High Entropy Oxides, HEOs)，作為鋰離子電池之負極材料，並比較了不同酸鹼值之高熵氧化物的材料特徵及半電池電化學性能。此外，為了解決高熵材料在大電流底下的循環穩定度，本研究在製作高熵氧化物負極電極時，加入了具有鍊狀之導電奈米碳管(Carbon Nanotubes, CNTs)，藉此強化電子在負極電極內的傳輸效能，達到改善循環穩定度的目的。但高熵氧化物一直存在著初期不可逆電容的問題，為了解決此問題，在與商用富含鎳之鋰鎳錳鈷氧化物正極(LiNi0.8Mn0.1Co0.1O2)組裝成全電池前，透過使用了負極預鋰化的方式，去除了高熵材料的不可逆電容(包含SEI層的初步生成)，避免高熵氧化物負極消耗過多正極的鋰離子，造成全電池電容嚴重衰退之情形發生。此外，為了探討全電池最佳負極/正極電容比例(Anode/Cathode ratio)，本研究也利用了COMSOL模擬分析軟體進行高熵氧化物負極和鋰鎳錳鈷氧化物正極半電池平衡電位測試，由分析結果來看，當A/C比取1.1時，出於工作電壓的考量，當整個電池充滿電達到高電壓的狀態時，負極的電池電量狀態(State Of Charge, SOC)會超出鋰離子可以容納的範圍；但當A/C比取1.5時，負極的SOC部分則落在鋰離子可以容納的範圍內，由此可見A/C比取1.5是比較適當的比例參數。

摘要(英)

In recent years, the rapid development of technology has led to an increase in the popularity of lithium-ion batteries. This study synthesizes high entropy oxides (HEOs) with a single-phase rock-salt structure using the sol-gel auto combustion method as an anode material for lithium-ion batteries. In this study, we compares the material characteristics and electrochemical performance of half cells with HEOs at different pH values. To address the issue of cycling stability of high entropy materials at high current conditions, conductive carbon nanotubes (CNTs) were added during the preparation of the HEOs anode to provide additional pathways for lithium-ion transport, thereby improving cycling stability.However, HEOs have a persistent problem of initial irreversible capacity. To mitigate this, pre-lithiation of the anode was performed before assembling the full cell with a commercial nickel-rich lithium nickel manganese cobalt oxide cathode (LiNi0.8Mn0.1Co0.1O2). This pre-lithiation process allows for the formation of the solid electrolyte interface (SEI) layer on the surface of the anode, preventing excessive consumption of lithium ions from the cathode and avoiding severe capacity degradation of the full cell. Additionally, to determine the optimal anode/cathode (A/C) ratio for the full cell, COMSOL simulation software was used to analyze the equilibrium potential of half cells with HEOs anodes and lithium nickel manganese cobalt oxide cathodes. The analysis results indicate that when the A/C ratio is set to 1.1, the state of charge (SOC) of the anode exceeds the allowable range when the battery is fully charged to a high voltage. However, when the A/C ratio is increased to 1.5, the SOC of the anode remains within the normal range. Therefore, an A/C ratio of 1.5 is considered the more appropriate parameter.

關鍵字(中)

★ 鋰離子電池
★ 高熵氧化物
★ 溶膠凝膠自動燃燒法
★ 循環穩定度
★ 負極/正極容量比例

關鍵字(英)

論文目次

目錄
中文摘要 I
Abstract II
誌謝 III
目錄 IV
圖目錄 VII
表目錄 IX
第一章緒論 1
1-1 前言及ESG指標 1
1-2 研究動機 2
1-3 電池種類介紹 3
第二章基礎理論及文獻回顧 6
2-1 鋰離子電池介紹 6
2-1-1　鋰離子電池之運作原理 6
2-1-2　影響鋰離子電池運作性能的因素 8
2-1-3 負極/正極容量比(A/C比)介紹 8
2-2　全電池負極去除不可逆電容及預鋰化處理比較 9
2-3 高熵材料介紹及鋰離子電池領域應用 11
2-3-1　高熵材料的定義及其特性 11
2-3-2　高熵材料在鋰離子電池領域之應用 12
2-4 常見高熵氧化物製備方法及其優缺點比較 15
第三章實驗步驟 21
3-1 實驗之化學藥品 21
3-2　高熵氧化物粉末製備 23
3-3　鋰離子電池電極製備 24
3-4　鋰離子半電池封裝流程 24
3-4-1　鈕扣型半電池封裝 24
3-4-2　袋裝型（軟包裝）半電池封裝 25
3-5　鋰離子全電池封裝流程 26
3-5-1　負極預鋰化處理 26
3-5-2　全電池封裝 27
3-6 實驗分析儀器 27
3-6-1　材料特徵分析 27
3-7 鋰離子電池電化學量測系統 30
3-7-1　循環伏安法 30
3-7-2　電化學阻抗圖譜 30
3-7-3　充放電率測試 31
3-7-4　恆電流長時間循環穩定性測試 31
第四章結果與討論 32
4-1 高熵氧化物粉末材料特徵分析與討論 32
4-1-1　高熵氧化物粉末之X射線繞射儀分析 32
4-1-2　高熵氧化物粉末之粒徑分析 34
4-1-3　高熵氧化物粉末之感應耦合電漿分析 35
4-1-4　高熵氧化物粉末之掃描式電子顯微鏡分析 36
4-1-5　高熵氧化物粉末之X射線光電子能譜分析 38
4-2　高熵氧化物負極半電池電性測試分析與討論 40
4-2-1　循環伏安圖分析 40
4-2-2　電化學阻抗圖譜 41
4-2-3　充放電速率測試 42
4-2-4　恆電流長時間循環穩定性測試 43
4-3 全電池電性測試分析與討論 44
4-3-1　電化學阻抗圖譜 45
4-3-2　充放電率測試 45
4-3-3　恆電流長時間循環穩定性測試 47
4-4　全電池最佳負極/正極配方比討論 47
第五章結論與未來工作 51
5-1 結論 51
5-2 未來工作 52

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指導教授

洪緯璿(Wei-Hsuan Hung)

審核日期

2024-7-29

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