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姓名	劉明松(Ming-Song Liu)  查詢紙本館藏	畢業系所	材料科學與工程研究所
論文名稱	鋰離子固態電池界面改進方法研究 (Research on the interface improvement in lithium-ion solid-state battery)
相關論文	★ 鋅空氣電池之電解質開發 ★ 添加石墨烯助導劑對活性碳超高電容電極性質的影響 ★ 耐高壓離子液體電解質 ★ 熱裂解法製備RuO2-Ta2O5/Ti電極 應用於離子液體電解液 ★ 碳系超級電容器用耐高壓電解液研發 ★ 離子液體與碸類溶劑混合型電解液應用於鋰離子電池矽負極材料 ★ 三元素摻雜LLTO混LLZO應用鋰離子電池 ★ 以濕蝕刻法於可撓性聚亞醯胺基板製作微通孔之研究 ★ 以二氧化釩奈米粒子調變矽化鎂熱電材料之性能 ★ 可充電式鋁電池的 4-ethylpyridine–AlCl3電解液、規則中孔碳正極材料以及自放電特性研究 ★ 釹摻雜鑭鍶鈷鐵奈米纖維應用於質子傳輸型陶瓷電化學電池空氣電極 ★ 於丁二腈電解質添加碳酸乙烯酯對鋰離子電池性能之影響 ★ 多孔鎳集電層應用於三維微型固態超級電容器 ★ 二氧化錳/銀修飾奈米碳纖維應用於超級電容器 ★ 氧化鎳-鑭鍶鈷鐵奈米纖維陰極電極應用於質子傳導型固態氧化物電化學電池 ★ 應用丁二腈基離子導體修飾PVDF-HFP 複合聚合物電解質與鋰電極界面之高穩定鋰離子電池
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摘要(中)	隨著科技與人口的提升，對能源的需求量日益漸增，然而因石化燃料的浩劫與對環境的影響，導致人們轉往使用綠色能源，而許多綠能卻又被地形、氣候等繁多限制所侷限，導致其效用不佳且無法攜帶，然而鋰電池雖不可發電，卻可將能源儲存在可攜帶裝置內，並且轉換效率高，而受到重視，例如常見的手機、手錶、電腦等，在新興科技中的電動車、無人機等也是極為重要的零組件，並隨著科技的進步，人們對於鋰離子電池的能量密度與功率密度的需求漸增，其附帶的使得鋰電池的安全性受到極大的重視，故學者們紛紛提出各種方法提升其性能，並期望可同時改善安全性上的問題，其中以固態電解質取代傳統液態電解質被認為是最有效的方法之一，然而固態電解質目前面臨兩大問題，即為界面電阻過高與離子導率不佳，然而學者們目前提出的解決方式皆會面臨新的挑戰，其中以加入界面層及共燒結為目前介面改善的主要研究方向之一。本研究著重在界面上的改善，故以幾項實驗來提出解決方案，其中有以助燒結劑的方式來改善固態電解質燒結溫度與正極不匹配的問題，使共燒結成為可能的選項之一，亦有評估/開發新的電解質材料，並想以單一成分的方式製備出全電池，以防止電極與電解質因共燒結元素互相擴散，而形成高阻抗層，最後還有製備開發優良的丁二腈基介面修飾劑，以此抑制電解質與鋰金屬的不良副反應，以上的研究皆有不錯的效果，為未來鋰電池固態電解質實際運用上提供個一些不錯的建議與經驗。
摘要(英)	With the advancement of technology and population growth, the demand for energy is increasing steadily. However, the catastrophic effects of fossil fuels on the environment have led people to shift towards the use of green energy. Yet, many renewable energy sources are limited by various factors such as terrain and climate, resulting in their limited effectiveness and lack of portability. On the other hand, although lithium batteries cannot generate electricity, they can store energy in portable devices and have high conversion efficiency. They have gained significant attention in common devices like mobile phones, watches, and computers, as well as in emerging technologies such as electric vehicles and drones, where they serve as vital components. With technological advancements, the demand for higher energy density and power density in lithium batteries has increased, placing a great emphasis on their safety. As a result, researchers have proposed various methods to improve their performance while addressing safety issues. One of the most effective approaches is considered to be replacing traditional liquid electrolytes with solid-state electrolytes. However, solid-state electrolytes currently face two major challenges: high interfacial resistance and poor ion conductivity. The solutions proposed by researchers to overcome these challenges also encounter new obstacles. Among them, the addition of interface layers and co-sintering is currently the main research direction for interface improvement. This study focuses on interface enhancement and proposes solutions through several experiments. These experiments include the use of sintering aids to address the mismatch between the sintering temperature of the solid-state electrolyte and the positive electrode, making co-sintering a viable option. The evaluation and development of new electrolyte materials are also being explored with the aim of preparing a full cell using a single component to prevent electrode-electrolyte interdiffusion and the formation of high-impedance layers. Finally, efforts are being made to prepare and develop excellent acrylonitrile-based interface modifiers to suppress adverse reactions between the electrolyte and lithium metal. The studies above have shown promising results, providing valuable suggestions and experiences for the practical application of solid-state electrolytes in future lithium batteries.
關鍵字(中)	★ 鋰離子二次電池 ★ 固態電解質 ★ 界面修飾	關鍵字(英)	★ Lithium-ion secondary battery ★ Solid-state electrolytes ★ Interface modification
論文目次	摘要 vi Summary vii Table of Contents x List of Figures xiii List of Tables xvii I. Preface and literature review 1 1. Introduction 1 2. Lithium-ion battery operating principle and development direction 3 2.1 How the battery works 3 2.2 History of battery development 4 3. Introduction to common solid-state electrolytes 7 3.1 Crystalline electrolyte 8 (a) Sulfide electrolyte 9 (b) Oxide electrolyte 10 (1) NASICON structure 10 (2) Garnet structure 10 (3) Peroskite structure 11 3.2 Glassy electrolyte 12 3.3 Glass-ceramic electrolyte 13 3.4 Composite electrolytes 13 4. Experimental equipment 15 4.1 Magnetic stirrer 15 4.2 Oven 15 4.3 Furnace tube 15 4.4 X-ray diffraction 16 4.5 Raman 17 4.6 Potentiostat and charge-discharge motor 17 4.7 Rotation and revolution mixer 18 4.8 Glove box 18 4.9 Scraper machine 19 4.10 Hydraulic press 19 4.11 Fume hood 20 4.12 Electrospinning 20 4.13 Scanning electron microscopy 20 4.14 X-ray photoelectron spectroscopy 21 4.15 Transmission electron microscopy 21 II. Research I: Reducing the sintering temperature of Li7La3Zr2O12 with sintering aids 23 1. Introduction to LLZO solid-state electrolytes 23 2. Recent research on LLZO solid-state electrolytes 24 2.1 LLZO electrochemical stability 25 2.2 Sintering temperature reduction 25 2.3 Electrode interface 26 2.4 Stability in air 27 3. Research on the use of sintering aids in lithium-ion solid-state electrolytes 28 4. Research motivation and purpose 30 5. Experimental drugs and procedures 31 5.1 Experimental drugs 31 5.2 Experimental procedure 31 a. Sintering aid preparation and full battery preparation 31 b. Compound electrolyte analysis 32 6. Results and discussion 34 6.1 Characterization of LLZO pristine solid-state electrolytes 34 6.2 Characterization of LLZO composite solid-state electrolytes 37 6.3 Full battery performance analysis 51 III. Research II: Li3V2(PO4)3 solid-state electrolytes development 56 1. Introduction of Li3V2(PO4)3 56 2. Recent research on LVP 59 3. Research motivation and purpose 61 4. Experimental drugs and procedures 62 4.1 Experimental drugs 62 4.2 Experimental procedure 62 a. Synthesis of monoclinic-LVP 62 b. Synthesis of rhombohedral-LVP 62 c. Synthesis of Zr-doped rhombohedral-LVP 62 d. Electrochemical measurement sample preparation 63 e. Sample analysis 63 5. Results and discussion 64 5.1 Analysis of LVP matrix powder 64 5.2 Analysis of LVP electrolyte 69 5.3 Analysis of Zr-doped rhombohedral-LVP electrolyte 72 IV. Research III: Effect of PVDF-HFP-based composite electrolyte and succinonitrole-based interface modifier 78 1. Introduction of PVDF and PVDF-HFP 78 1.1 PVDF-HFP based solid composite electrolyte 79 1.2 Interface modifier 81 a. Introduction of interface modifier-liquid electrolyte 83 b. Introduction of interface modifier-succinonitrile-based electrolyte 84 2. Research motivation and purpose 85 3. Experimental drugs and procedures 86 3.1 Experimental drugs 86 3.2 Experimental procedure 86 a. PVDF-HFP based composite polymer electrolyte 86 b. Interface modifier configuration 87 c. Electrochemical measurement cell assembly 87 d. Electrochemical analysis 88 4. Results and discussion 89 4.1 LLTO nanowire analysis 89 4.2 Analysis of PVDF-HFP composite solid-state electrolytes 91 4.3 Interface modified composite polymer electrolyte 94 4.4 Effects of modifiers on lithium deposition and PVDF-HFP composite electrolyte 100 4.5 Full battery electrical properties of PVDF-HFP-based composite polymer electrolyte 105 V. Three research conclusions and future prospects 112 VI. References 114
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指導教授	李勝偉(Sheng-Wei Lee)	審核日期	2023-7-28
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