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研究生： 李承翰
Lee, Cheng-Han
論文名稱： 以高分子強化微米級矽基負極之機械性質與導電性於鋰離子電池之應用
Polymeric Approach for High Performance Micrometer-sized Silicon Anode in Li-ion Batteries with Enhanced Mechanical Properties and Conductivity
指導教授： 杜正恭
Duh, Jenq-Gong
林姿瑩
Lin, Tzu-Ying
口試委員: 洪崧富
Hung, Sung-Fu
林玠廷
Lin, Chieh-Ting
學位類別： 碩士
Master
系所名稱： 工學院 - 材料科學工程學系
Materials Science and Engineering
論文出版年： 2023
畢業學年度： 111
語文別： 英文
論文頁數： 94
中文關鍵詞： 矽基負極 、廢料矽 、永續材料
外文關鍵詞： silicon anode, Kerf-loss waste, sustainable materials
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    • 黏結劑為傳統電池溼式製程中黏合電極重要的一員，因為矽與水有相當好之親合力，水溶性黏結劑─聚丙烯酸(PAA)─能與矽表面產生更好的交互作用。本研究使用具高度彈性的聚合物─poly-pseudorotaxane(p-PR)─應用於調整PAA之機械性質。經修飾的黏結劑複合材料，以多種成分詳細地研究其作用與效應，p-PR與PAA間鍵結可經真空中脫水反應強化結構混定性。10% p-PR的成分可達到最佳循環效率，在250 mA g-1之充放電速率下展現出2770 mAh g-1之初始電容量，且於100圈後還維持80%的效率，其原因為電極整體產生之龜裂最少。於阻抗分析中，10%樣品於循環後展現最穩定之SEI與較低之阻抗值。經p-PR修飾之矽碳混和電極能產生710 mAh g-1之初始電容量，且以250 mA g-1之速率充放下經300圈能達到70%之循環效率。

    Binder is essential in conventional wet processes of battery manufacturing for electrode adhesion. Since silicon shows great affinity with water, water-soluble binders, e.g., polyacrylic acid (PAA), is preferable to silicon surface forming stronger interaction. In this study, a highly elastic polymer, poly-pseudorotaxane (p-PR), is applied to adjust the mechanical properties of stiff PAA binder. The modified binder composites with several compositions are thoroughly investigated to analyze the interactions and effects. The bonding between p-PR and PAA by dehydration reaction in a vacuum ensures structural stability. The integrity of the electrode with 10% p-RR demonstrates the best retention due to less crack formation. The initial capacity of 10% p-PR sample acquires 2770 mAh g-1, retaining 80% after 100 cycles at a rate of 250 mA g-1. In impedance analysis, 10% p-PR also reveals the most stable solid‐electrolyte interphase (SEI) after cycling together with a decreased resistance. In addition, the p-PR modified graphite/Si composite electrode delivers an initial capacity of 710 mAh g-1 at a rate of 250 mA g-1 and a substantial cyclability of 70% retention after 300 cycles.

    Content Abstract...........................................................ii Content............................................................iv Figure Lists.......................................................vii Table List.........................................................x Chapter 1 Introduction.............................................1 1.1 Background.....................................................1 1.2 Motivations and Objectives in This Study.......................2 Chapter 2 Literature Review........................................5 2.1 Introduction of Lithium Ion Battery............................5 2.2 Development of Silicon Anode...................................20 2.2.1 Overview of Silicon-based Anode..............................20 2.2.2 Critical Issues of Silicon Materials.........................22 2.2.3 Innovations of Silicon Anode Design..........................25 2.3 Introduction of Binder and Polymer in Silicon Anode............33 2.3.1 Binder Development in Si Anode...............................33 2.3.2 Advanced Binder Design and Polymeric Technique...............38 Chapter 3 Experimental Procedure...................................47 3.1 Materials Prepearation.........................................47 3.1.1 Synthesis of Poly-pseudorotaxane.............................47 3.1.2 Silicon Powder Preparation from Waste Sludge.................47 3.1.3 Electrode and Coin Cell Battery Preparation..................48 3.2 Characterization and Analysis..................................49 3.2.1 Size Analysis................................................49 3.2.2 Chemical Analysis............................................50 3.2.3 SEM and EPMA Observation.....................................50 3.3 Electrochemical Analysis.......................................51 3.3.1 Cycling and Charging-rate Test...............................51 3.3.2 Cyclic Voltammetry...........................................51 3.3.3 Electrochemical Impedance Spectroscopy.......................51 3.4 Mechanical Test of Electrode...................................52 3.4.1 Tape Peeling Test............................................52 3.4.2 Nano-indentation.............................................52 Chapter 4 The Investigation of p-PR on Conventional Binder (PAA)...54 4.1 The Size Distribution of Milled Si Waste.......................54 4.2 FTIR Analysis..................................................56 4.3 Electrochemical Analysis of Si-based Electrodes................58 4.4 Investigations of Si-based Electrodes..........................69 4.4.1 Tape Peeling Test............................................69 4.4.2 Nano-indentation.............................................70 4.4.3 Morphologies.................................................72 4.5 Performance of Si/graphite-mixed Electrode.....................74 Chapter 5 Conclusion...............................................76 Appendix...........................................................79 A.1 The Enhanced Performance with Conductive Polymer as Binder.....79 A.2 The Mechanical Stabilization Effect of p-PR on PEDOT: PSS Electrodes.........................................................80 References.........................................................83

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