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| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 劉如熹 | zh_TW |
| dc.contributor.advisor | Ru-Shi Liu | en |
| dc.contributor.author | 劉祐碩 | zh_TW |
| dc.contributor.author | Yu-Shuo Liu | en |
| dc.date.accessioned | 2025-07-09T16:14:18Z | - |
| dc.date.available | 2025-07-10 | - |
| dc.date.copyright | 2025-07-09 | - |
| dc.date.issued | 2025 | - |
| dc.date.submitted | 2025-06-26 | - |
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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/97649 | - |
| dc.description.abstract | 隨科技之進步，電動車與數位產品之普及，鋰離子二次電池之需求急速上升。為提升鋰離子二次電池之能量密度與安全性，鹵化物固態電解質為不可或缺之選項。其相對液態電解質可大幅提升安全性，且其匹配高電壓陰極可顯著增加鋰離子二次電池之能量密度。
本研究重點於鹵化物型固態電解質鋰銦氯(Li3InCl6)中摻雜高價數鉭(Ta)離子，以增加結構中之鋰空位(lithium vacancy)，以提升離子導電度(ionic conductivity)。故本研究使用針對鉭離子進行Li3−2xIn1−xTaxCl6系列之合成，於其中Li2.8In0.9Ta0.1Cl6作為電解質具最佳離子導電度於室溫達1.27 mS/cm，此說明鉭摻雜可增加鋰空位，並降低活化能(activation energy)。其中最優化之條件為前驅物經球磨法後並於200°C條件下真空燒結4 h，產物之固態電解質活化能僅0.293 eV，並證實其熱穩定性達410°C。本研究亦藉中子繞射與X光吸收光譜鑑定Li3−2xIn1−xTaxCl6系列，使用結構之精修證明鉭摻雜不僅可增加鋰空位，且可提升Li2之位置佔有率，提升鋰離子遷移能力，並說明過多之鉭摻雜將使結構扭曲破壞，使Li3之四面體為鋰離子之遷移瓶頸，而降低離子導電度。並藉理論計算證明鉭摻雜有助於降低二維遷移之活化能，提升離子導電度。 同時為解決陰極與固態電解質之電位不匹配，本研究使用鈮酸鋰(LiNbO3)塗層保護鎳錳酸鋰(LiNi0.5Mn1.5O4; LNMO)。本研究亦說明鈮酸鋰塗層可保護鎳錳酸鋰陰極，避免鎳錳酸鋰陰極與固態電解質發生反應。並揭示無鈮酸鋰塗層將使Li2.8In0.9Ta0.1Cl6之In3+與Ta5+還原且鎳錳酸鋰之Mn3+氧化。 最後本研究組裝Li2.8In0.9Ta0.1Cl6之鈷酸鋰(LiCoO2; LCO)全固態電池，其首次放電電容量可達135.6 mAh/g，於第50次循環之放電電容量達121.8 mAh/g，其保持率(retention rate)於50次循環後達90%。其中Li2.8In0.9Ta0.1Cl6之LNMO全固態電池首次放電電容量可達111.6 mAh/g。 | zh_TW |
| dc.description.abstract | As technology progresses, electric vehicles (EVs) and other products spread throughout our lives, and the demand for lithium secondary batteries increases. Halide solid-state electrolytes (HSSEs) are the best candidates for pursuing safety and energy density. Compared to liquid electrolytes (LE), HSSEs are not flammable and show high energy density. Moreover, their compatibility with high-voltage cathodes is extraordinary.
This research focuses on doping high-valent Ta in HSSEs Li3InCl6 to increase the vacancy in the structure, increasing in ionic conductivity. A series of electrolyte Li3−2xIn1−xTaxCl6 was synthesized. The highest ionic conductivity was Li2.8In0.9Ta0.1Cl6, with an ionic conductivity of 1.27 mS/cm and an activation energy of 0.293 eV. The optimized process was precursors sintered at 200°C for 4 h in a vacuum. The refinements of neutron powder diffraction reveal that the dopant Ta could increase the lithium vacancy in position Li2. On the other hand, redundant dopants result in structure distortion, and the ionic conductivity decreases. Also, the theoretical calculation proves the decrease of activation energy in the 2D conduction pathway. To solve the incompatibility between the electrolyte and cathode, we use LiNbO3 (LNO) to protect the LiNi0.5Mn1.5O4 (LNMO) cathode. This research demonstrates the effect of LNO, which could avoid the reaction between the halide solid electrolyte and the cathode. The absence of LNO could lead to the oxidation of Mn3+, and the reduction of In3+ and Ta5+. In the last part of this research, the discharge capacity of the full cell using Li2.8In0.9Ta0.1Cl6 and LiCoO2 (LCO) cathode was 135.6 mAh/g and 121.8 mAh/g at the 1st and 50th cycle, respectively. The discharge capacity of the full cell using the LNMO cathode shows 111.6 mAh/g at the 1st cycle。 | en |
| dc.description.provenance | Submitted by admin ntu (admin@lib.ntu.edu.tw) on 2025-07-09T16:14:18Z No. of bitstreams: 0 | en |
| dc.description.provenance | Made available in DSpace on 2025-07-09T16:14:18Z (GMT). No. of bitstreams: 0 | en |
| dc.description.tableofcontents | 口試委員審定書 i
誌謝 ii 摘要 iii Abstract iv 目次 v 圖次 viii 表次 xiv 第一章 緒論 1 1.1 電池之原理與發展 1 1.2 鋰離子二次電池 4 1.3 鋰離子電池之構造與原理 8 1.3.1 鋰離子電池之構造 8 1.3.2 常見之鋰離子電池參數 10 1.3.3 鋰離子電池之原理 10 1.4 鋰離子二次電池之陽極材料 12 1.4.1 碳陽極材料 12 1.4.2 矽陽極材料 13 1.4.3 鋰金屬與鋰合金 14 1.5 鋰離子二次電池之陰極材料 17 1.5.1 磷酸鐵鋰 18 1.5.2 鈷酸鋰 18 1.5.3 鎳鈷錳三元材料 20 1.5.4 鎳錳酸鋰 21 1.6 液態電解質 24 1.7 固態電解質 25 1.7.1 氧化物固態電解質 25 1.7.2 硫化物固態電解質 27 1.7.3 氮化物固態電解質 30 1.7.4 鹵化物固態電解質 31 1.7.5 鋰銦氯固態電解質 38 1.8 固態電解質摻雜 41 1.8.1 陰離子摻雜 41 1.8.2 陽離子摻雜 42 1.9 固態電解質之鋰離子遷移機制 44 1.10 研究動機與目的 45 第二章 實驗步驟與分析儀器 46 2.1 化學藥品列表 46 2.2 實驗步驟 47 2.2.1 鉭摻雜鹵化物固態電解質之合成 47 2.2.2 鈮酸鋰包覆於鎳錳酸鋰陰極之合成 48 2.2.3 全固態鋰離子電池之組裝 49 2.3 分析儀器 50 2.3.1 X光繞射儀 50 2.3.2 中子粉末繞射 55 2.3.3 掃描式電子顯微鏡 57 2.3.4 穿透式電子顯微鏡 59 2.3.5 X光吸收光譜儀 60 2.3.6 X光光電子能譜儀 63 2.3.7 電化學阻抗交流儀 64 2.3.8 線性伏安儀 68 2.3.9 對稱電池測試儀 69 2.3.10 充電放電測試儀 70 第三章 結果與討論 71 3.1 Li3−2xIn1−xTaxCl6之合成鑑定 71 3.1.1 Li3−2xIn1−xTaxCl6之X光繞射圖譜鑑定 71 3.1.2 Li3−2xIn1−xTaxCl6之掃描式電子顯微鏡鑑定 75 3.1.3 Li3−2xIn1−xTaxCl6之電化學阻抗鑑定 76 3.1.4 Li3−2xIn1−xTaxCl6之活化能鑑定 79 3.1.5 Li3−2xIn1−xTaxCl6之中子繞射鑑定 82 3.1.6 Li3−2xIn1−xTaxCl6之X光吸收光譜鑑定 89 3.1.7 Li3−2xIn1−xTaxCl6之理論計算 95 3.1.8 Li3−2xIn1−xTaxCl6之線性伏安法與對電極電位量測 97 3.1.9 Li3−2xIn1−xTaxCl6之對稱循環測試 99 3.2 鈮酸鋰塗層包覆於鎳錳酸鋰陰極之鑑定 100 3.2.1 X光繞射圖譜鑑定 100 3.2.2 穿透式電子顯微鏡鑑定 101 3.2.3 X光光電子能譜鑑定 101 3.3 全固態電池鑑定 107 3.3.1 應用於鈷酸鋰陰極充電放電循環測試 107 第四章 結論 111 參考文獻 112 | - |
| dc.language.iso | zh_TW | - |
| dc.subject | 鹵化物型固態電解質 | zh_TW |
| dc.subject | 鋰離子全固態電池 | zh_TW |
| dc.subject | 鉭摻雜 | zh_TW |
| dc.subject | all-solid-state lithium battery | en |
| dc.subject | tantalum doping | en |
| dc.subject | halide solid-state electrolyte | en |
| dc.title | 鉭摻雜之鹵化物型固態電解質應用於鋰離子電池 | zh_TW |
| dc.title | Tantalum-Doped Halide Solid-State Electrolyte for Lithium-Ion Batteries | en |
| dc.type | Thesis | - |
| dc.date.schoolyear | 113-2 | - |
| dc.description.degree | 碩士 | - |
| dc.contributor.oralexamcommittee | 王建隆;陳錦明;洪太峰;廖譽凱 | zh_TW |
| dc.contributor.oralexamcommittee | Chien-Lung Wang;Jin-Ming Chen;Tai-Feng Hung;Yu-Kai Liao | en |
| dc.subject.keyword | 鉭摻雜,鹵化物型固態電解質,鋰離子全固態電池, | zh_TW |
| dc.subject.keyword | tantalum doping,halide solid-state electrolyte,all-solid-state lithium battery, | en |
| dc.relation.page | 127 | - |
| dc.identifier.doi | 10.6342/NTU202501329 | - |
| dc.rights.note | 同意授權(全球公開) | - |
| dc.date.accepted | 2025-06-30 | - |
| dc.contributor.author-college | 理學院 | - |
| dc.contributor.author-dept | 化學系 | - |
| dc.date.embargo-lift | 2025-07-10 | - |
| 顯示於系所單位： | 化學系 | |
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