利用生質碳源製備成多孔洞結構之碳材 於高效能鋰(鈉)離子電池負極材料之應用 及複合式有機無機固(膠)態高分子電解質之結構鑑定與電化學性質研究

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呂秉峻(Bing-Jyun Lu) 查詢紙本館藏

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論文名稱

利用生質碳源製備成多孔洞結構之碳材於高效能鋰(鈉)離子電池負極材料之應用及複合式有機無機固(膠)態高分子電解質之結構鑑定與電化學性質研究

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至系統瀏覽論文 (2026-6-30以後開放)

摘要(中)

本論文分為兩部分，第一部分主要是利用生質碳源以模板法製備多孔洞碳材PCC並應用於電池之負極材料。生質碳源因來自生物質藉由適當的製備方式，可保留其天然之微量元素達到自摻雜的效果，本研究之PCC碳材經一系列材料鑑定發現還具有氮、硫、矽和磷元素，對於材料在電性上的表現有一定程度的幫助，且有著高比表面積和多樣孔洞的特殊結構也使得材料有著更大的電容量。此材料在鋰離子電池系統以電流密度100 mA g-1進行充放電循環測試，經過393圈後能得到699.4 mA h g-1優異的電容量表現，另外在鈉離子系統中以電流密度1000 mA g-1進行充放電循環測試，在493圈後能穩定得到150.9 mA h g-1的電容量顯示此材料具有良好的循環穩定性。
第二部分為複合式有機無機高分子電解質之合成，根據使用需求製備成固態和膠態兩種形式，並應用於鋰離子電池之電解質。本實驗利用兩種不同特性之高分子材料M-2070和ED2003分別與4,4’-Methylene diphenyl diisocyanate(MDI)交聯形成線性前驅物，接著依據不同重量百分比並改變其氧鋰比合成出混摻型有機無機固態高分子電解質其在30℃下離子導電度達到1.19×〖10〗^(-4) S cm-1，在膠態系統中更是高達2.19×〖10〗^(-3) S cm-1，且在硬幣型電池的充放電循環測試中經過18圈有著高達154.7 mA h g-1的電容量表現優於市售隔離膜。

摘要(英)

Recently, biomass derived carbons have gained enormous attention mainly due to their abundance, environmental friendliness and the factors associated with the utilization in energy conversion and storage systems. Heteroatom doping is an effective strategy to optimize the electrochemical performance of biomass-derived carbon electrode materials. Furthermore, fast redox reactions originating from surface functional groups can contribute to extra pseudo-capacitance. Biomass-based carbons with heteroatom doping can be realized by choosing heteroatom-enriched precursors or chemical dopants and processed by appropriate synthesis method. In this study, ordered mesoporous silica (KIT-6) is used as template with pine cone powder to prepare pine cone derived carbon (PCC). The PCC delivers a high reversible capacity of 699.4 mA h g-1 after 393 cycles at a current density of 100 mA g-1 when use as anode for lithium-ion battery. When investigated in sodium-ion battery, the PCC anode has exhibited a high reversible discharge capacity of 151 mA h g-1 after 493 cycles even at current density of 1000 mA g-1. Besides, the mixed storage mechanism is further studied by kinetic calculation.
In the second part, the synthesis of a new hybrid organic-inorganic polymer electrolyte based on 4,4’-methylene diphenyl diisocyanate, ED2003, M-2070 and organosilane ICPTES is discussed. The solid polymer electrolyte (SPE) has delivered the maximum ionic conductivity value of 1.19 × 10-4 S cm-1 at 30 ℃. A maximum ionic conductivity value of 2.19 × 10-3 S cm-1 is achieved for the plasticized polymer electrolytes (PPE) immersed in liquid electrolyte. The lithium battery prepared with the plasticized polymer electrolyte and LiFePO4 cathode has exhibited a high reversible discharge capacity of 154.7 mA h g-1 after 18 cycles at a current rate of 0.3 C. The new hybrid polymer electrolyte holds promise for application in next generation lithium-ion batteries.

關鍵字(中)

★ 鋰離子電池
★ 鈉離子電池
★ 生質碳材
★ 高分子電解質
★ 固態高分子電解質
★ 膠態高分子電解質

關鍵字(英)

論文目次

第一章緒論 1
1-1 前言 1
1-2 鋰離子電池 2
1-3 金屬離子電池 6
1-4 生物質碳材 8
1-5 高分子電解質 9
1-6 研究目的 10
第二章文獻回顧 11
2-1 負極材料 11
2-1-1 碳材 11
2-1-2 非碳材 13
2-2 生質碳材 14
2-3-1 以生物質材料作為碳源合成碳材 15
2-3-2 以不同方式增加生質碳材之電化學性質 17
2-3 高分子電解質 21
2-4-1 固態高分子電解質 23
2-4-2 膠態高分子電解質 30
2-4-3 鋰離子鹽類 36
2-4-4 有機矽高分子 41
第三章實驗藥品與儀器原理 42
3-1 實驗藥品 42
3-2 實驗鑑定儀器 45
3-3 材料鑑定儀器之原理 46
3-3-1 X射線粉末繞射(XRD) 46
3-3-2 氮氣等溫吸脫附曲線、表面積與孔洞性質鑑定(BET) 47
3-3-3 熱重分析儀(TGA) 51
3-3-4 示差掃描量熱儀(DSC) 52
3-3-5 傅立葉紅外線吸收光譜儀(FTIR) 53
第四章實驗方法 54
4-1 負極材料製備 54
4-1-1 六角柱狀p6mm中孔洞矽材KIT-6合成 54
4-1-2 以生質碳源利用KIT-6為模板合成碳材(PCC) 55
4-1-3 提升氮摻雜量之生質碳材(N-PCC)合成 56
4-2 高分子電解質製備 57
4-2-1 固態高分子電解質製備 57
4-2-2 膠態高分子電解質製備 60
4-3 電化學測試之材料製備 61
4-3-1 負極極片製作 61
4-3-2 正極極片製作 62
4-3-3 硬幣型2032型電池組裝 62
4-4 電池性能測試方法 64
4-4-1 定(變)電流充放電循環壽命測試 64
4-4-2 循環伏安法(CV) 64
第五章結果與討論-利用松果製備生質碳材應用於負極材料 65
5-1 材料鑑定 65
5-1-1 小角度X光繞射分析(SAXRD) 65
5-1-2 大角度粉末X光繞射分析(PXRD) 67
5-1-3 氮氣吸脫附結果分析(BET) 68
5-1-4 拉曼光譜分析(Raman) 71
5-1-5 熱重分析(TGA) 72
5-1-6 元素分析(EA) 73
5-1-7 X光電子能譜(XPS)分析 74
5-1-8 掃描式電子顯微鏡(SEM)結果分析 76
5-1-9 穿透式電子顯微鏡(TEM)結果分析 79
5-2 生質碳材(PCC)之電化學測試 84
5-2-1 循環伏安法(CV)分析 84
5-2-2 電化學交流阻抗頻譜分析(EIS) 86
5-2-3 電性暨電池性能分析 88
5-3 生質碳材(PCC)之動力學探討 105
5-3-1 離子擴散係數計算 105
5-3-2 贋電容貢獻度計算 107
5-4 相關文獻比較 110
第六章結果與討論-固(膠)態高分子電解質MMEDMI-X-Y 111
6-1 高分子電解質MMEDMI-X-Y之材料鑑定 111
6-1-1 熱重分析(TGA) 112
6-1-2 示差掃描量熱分析(DSC) 114
6-1-3 紅外線吸收光譜(IR)分析 117
6-1-4 SEM表面分析 121
6-1-5 固態核磁共振光譜(SSNMR)分析 124
6-2 高分子電解質MMEDMI-X-Y之電化學測試 127
6-2-1 固態高分子電解質之離子導電度測試 128
6-2-2 固態高分子電解質之線性掃描伏安法(LSV) 132
6-2-3 膠態高分子電解質之膨潤度測試 134
6-2-4 膠態高分子電解質之離子導電度測試 138
6-2-5 電池性能測試 140
第七章結論 143
參考文獻 145

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指導教授

高憲明(Hsien-Ming Kao)

審核日期

2021-7-29

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