以回收太陽能板之矽基材料結合石墨製備Si/SiOx/C複合負極應用於鋰離子電池之研究

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陳禹心(Yu-Sin Chen) 查詢紙本館藏

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化學工程與材料工程學系

論文名稱

以回收太陽能板之矽基材料結合石墨製備Si/SiOx/C複合負極應用於鋰離子電池之研究
(Fabrication of Si/SiOx/C Composite Negative Electrode for Lithium-Ion Battery by Utilizing Silicon-Based Materials from Recycled Solar Panels)

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至系統瀏覽論文 (2028-6-30以後開放)

摘要(中)

隨著科技進步和人口增長，環境和能源問題越來越受到關注。太陽能作為可再生能源之一，由於其普遍性、永久性和低污染性，成為許多國家推動綠色能源的主力。然而，太陽能板的使用壽命有限，不當處理可能對環境造成危害。因此回收及重複利用太陽能板已然成為重要的議題。太陽能板一般含有太陽能電池、鋁框架與乙烯/醋酸乙烯酯(EVA)共聚物等組件，其電池多由矽(Si)所構成。由於矽具有無毒、含量豐富、極高的理論電容量(4200 mAh/g)與低電壓平台(0.2-0.3 V)，使矽成為鋰離子電池應用中極具潛力之負極材料。然而，矽在充放電過程中會產生劇烈的體積膨脹/收縮變化，使得電容量快速衰退。為解決上述問題，本研究通過經濟有效的球磨和鍛燒處理，將太陽能板粉末再製成負極材料。藉由調整鍛燒溫度以觀察EVA殘留量，優化球磨和鍛燒的順序，製備出Si/SiOx負極材料並結合碳紙集電體應用於鋰電池中，最後定義出鍛燒500 oC後以300 rpm轉速球磨為最佳參數(500-BM(300))，於充放電100圈後擁有1170 mAh/g之電容量(200 mA/g電流密度下)。此外，因考量商用負極材料需求，將此參數應用於銅箔基材中，並透過矽基材料結合石墨進行複合製備Si/SiOx/C複合材料。結果顯示以Si/C複合比例1:0.6，並結合交聯黏著劑於充放電100圈後可擁有電容量488 mAh/g。為進一步使性能提升，於混漿時添加不同比例之乙醇作為溶劑，協助矽顆粒於漿料中的分散性，使顆粒不易團聚。結果顯示經由水：乙醇比例4：2擁有最佳之電化學性能表現，於100圈循環後擁有748 mAh/g之電容量。以上結果表明本研究可透過低成本且有效的球磨與鍛燒製程，將回收太陽能板之矽基材料結合石墨再製成Si/SiOx/C複合材料，透過交聯黏著劑與乙醇輔助方式協助性能的提升，於銅箔集電體提供高效能的充放電表現。

摘要(英)

With technology and population growth, environmental and energy concerns are increasing. Among various renewable energy sources, solar energy has emerged as a leading green energy solution due to its ubiquity, sustainability, and low environmental impact. However, solar panels have a limited lifespan, and improper disposal can pose environmental hazards. Therefore, the recycling and reuse of solar panels have become crucial. Solar panels typically consist of solar cells, aluminum frames, and ethylene-vinyl acetate (EVA) components, with the solar cells predominantly composed of silicon (Si). Silicon, with its non-toxic nature, abundance, high theoretical capacity (4200 mAh/g), and low voltage platform (0.2-0.3 V), shows promise as a negative electrode material for lithium-ion batteries. However, silicon undergoes significant volume expansion/contraction during charging and discharging, leading to rapid capacity degradation. To address this issue, this study employed an economical and efficient ball milling and calcination process to convert recycled solar panel powder into negative electrode material. By adjusting the calcinating temperature to observe the residual EVA content and optimizing the sequence of ball milling and calcination, Si/SiOx material was prepared and combined with carbon paper current collector for application in lithium batteries. The optimal parameters were defined as calcinating at 500°C followed by ball milling at 300 rpm, resulting in a capacity of 1170 mAh/g after 100 cycles. Considering the demand for commercial negative electrode materials, in this study, silicon was combined with graphite to prepare Si/SiOx/C composite material. The results showed that a Si/C composite ratio of 1:0.6, combined with a crosslinking binder, resulted in a capacity of 488 mAh/g. To further enhance the performance, different ratios of ethanol were added as a solvent during slurry mixing to assist in the dispersion of Si particles and prevent aggregation. The results indicated that a water:ethanol ratio of 4:2 exhibited the best electrochemical performance, with a capacity of 748 mAh/g after 100 cycles. These results demonstrate that this study successfully utilizing recycled solar panels and transformed them into Si/SiOx/C composite material using a low-cost and efficient ball milling and annealing process. The performance was further improved through the use of a crosslinking binder and ethanol-assisted dispersion, providing high-performance charge-discharge behavior on copper foil current collectors.

關鍵字(中)

★ 回收太陽能板
★ 矽/碳複合材料
★ 鋰離子電池負極
★ 交聯黏著劑

關鍵字(英)

★ Recycled solar panels
★ silicon/carbon composites
★ negative electrodes of lithium-ion batteries
★ cross-linked binder

論文目次

摘要 i
Abstract ii
誌謝 iii
目錄 v
圖目錄 ix
表目錄 xiii
第一章緒論 1
1-1 能源環境現況 1
1-2 太陽能模組與產業介紹 3
1-3 研究動機 6
第二章文獻回顧 7
2-1 鋰離子電池之發展與應用 7
2-2 鋰離子電池之運作原理 9
2-3 鋰離子電池之組成材料 11
2-3-1 負極材料(Negative Electrode Materials) 12
2-3-2 正極材料(Positive Electrode Materials) 18
2-3-3 電解質(Electrolyte) 20
2-3-4 隔離膜(Separator) 21
2-3-5 導電劑(Conductive Agent) 21
2-3-6 黏著劑(Binder) 22
2-3-7 集電體(Current Collector) 23
2-4 矽基負極材料(Silicon-based Negative Electrode Materials) 24
2-5 矽/碳複合材料(Si/C Composite Materials) 30
2-6 碳纖維集電體(Carbon Fiber Current Collector) 34
2-7 新型交聯黏著劑(Novel Cross-linking Binder) 36
第三章實驗方法 39
3-1 實驗架構 39
3-2 矽負極材料與鈕扣型電池製備 41
3-2-1 實驗藥品與實驗儀器 41
3-2-2　Si/SiOx負極活性物質之製備 43
3-2-3　Si/SiOx/C負極活性物質之製備 44
3-2-4　Si/SiOx碳紙集電體極片之製備 45
3-2-5　Si/SiOx/C銅箔集電體極片之製備 46
3-2-6　交聯Si/SiOx/C銅箔集電體極片之製備 46
3-2-7　乙醇輔助Si/SiOx/C銅箔集電體極片之製備 47
3-2-8　CR2032鈕扣型鋰離子電池之組裝 47
3-3 材料分析與電化學性能測試 49
3-3-1 超高解析場發射掃描式電子顯微鏡 (Field Emission Scanning Electron Microscope, FE-SEM) 49
3-3-2 X光繞射儀 (X-ray Diffraction, XRD) 49
3-3-3 X射線光電子能譜儀 (X-ray Photoelectron Spectroscopy, XPS) 50
3-3-4 高解析穿透式電子顯微鏡(High Resolution Transmission Electron Microscope, HR-TEM) 51
3-3-5 動態光散射儀(Dynamic Light Scattering, DLS) 51
3-3-6 熱重分析儀(Thermogravimetric Analysis, TGA) 51
3-3-7 感應耦合電漿質譜分析儀(Inductively Coupled Plasma Mass Spectrometry, ICP-MS) 52
3-3-8 Zeta電位量測儀(Zeta Potential) 52
3-3-9 傅立葉轉換紅外光譜(Fourier-transform Infrared Spectroscopy, FTIR) 54
3-3-10 交流阻抗分析(Electrochemical Impedance Spectroscopy, EIS) 54
3-3-11 循環充放電與倍率性能測試(Charge and Discharge Test) 56
第四章結果與討論 57
4-1 Si/SiOx應用於碳纖維紙集電體之材料與電性分析 57
4-1-1 ICP-MS定量分析 57
4-1-2 TGA分析 57
4-1-3 X光繞射分析 60
4-1-4 FE-SEM分析 62
4-1-5 DLS分析 64
4-1-6 XPS分析 67
4-1-7 循環充放電分析 71
4-1-8 不同電流密度快速充放電分析 74
4-2 Si/SiOx應用於銅箔基材之電性分析 75
4-3 Si/SiOx/C應用於銅箔基材之材料與電性分析 83
4-3-1 X光繞射分析 83
4-3-2 FE-SEM分析 85
4-3-3 HR-TEM分析 88
4-3-4 循環充放電分析 91
4-3-5 不同電流密度快速充放電分析 93
4-3-6 交流阻抗分析 94
4-4 交聯Si/SiOx/C應用於銅箔基材之材料與電性分析 96
4-4-1 FTIR分析 96
4-4-2 FE-SEM分析 98
4-4-3 循環充放電分析 101
4-4-4 不同電流密度快速充放電分析 104
4-4-5 交流阻抗分析 106
4-5 乙醇輔助Si/SiOx/C應用於銅箔基材之分析 108
4-5-1 Zeta電位分析 108
4-5-2 循環充放電分析 110
4-5-3 不同電流密度快速充放電分析 112
第五章結論與未來展望 113
5-1 結論 113
5-1-1 Si/SiOx應用於碳纖維紙集電體 113
5-1-2 Si/SiOx應用於銅箔集電體 115
5-1-3 Si/SiOx/C應用於銅箔集電體 116
5-2 未來展望 118
參考文獻 119

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指導教授

劉奕宏(Yi-Hung Liu)

審核日期

2023-8-11

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