臺灣博碩士論文加值系統

　　本研究中共有兩個主要的研究主題，第一主題是合成以理論計算所設計之層狀LiAl1-xCoxNi1/3Mn1/3O2正極材料。由計算所得之LiAl1/3Ni1/3Mn1/3O2充放電平台，可以看出LiAl1/3Ni1/3Mn1/3O2是一種相當具有潛力的鋰離子電池正極材料。但是在實際實驗中卻無法以溶膠凝膠法合成出純相的LiAl1/3Ni1/3Mn1/3O2，為了抑制合成過程中不純物質的產生，LiAl1/3Ni1/3Mn1/3O2中的部分Al被以Co來取代，當層狀LiAl1-xCoxNi1/3Mn1/3O2正極材料中的Co含量，介於1/6≤x≤1/3時，可以在氧氣氣氛、900oC的煆燒溫度下合成出單一純相的LiAl1-xCoxNi1/3Mn1/3O2正極材料，在實驗中發現Co含量的增加可以提升LiAl1-xCoxNi1/3Mn1/3O2正極材料的放電電容量與導電度，同時藉由Co的摻雜而提升的導電度與結晶純度，對LiAl1-xCoxNi1/3Mn1/3O2正極材料的電化學表現影響十分深遠。
　　第二個研究主題，則是發展可以對鋰離子充電之無線充電模組。本研究所發展的無線充電技術，克服了以往技術的瓶頸，並可以藉由控制輸入電能與距離的方式，成功的對植入型鋰離子電池進行充電，在經過20次充放電後，仍可保有相當不錯的循環特性，雖然本研究所發展的無線充電模組的轉換效率約只有2~5%（發射天線輸入電能對電池輸出電能之間比值），但其轉換效率仍可藉由發射天線與接收天線的改良，而有所改善。
　　其次，本研究亦對LiNi0.45Mn0.45Co0.1O2/Li、LiMn2O4/Li、 Li4Ti5O12/Li、 MCMB/Li、 LiFePO4/Li 與 LiMn2O4/Li4Ti5O12等半電池與全電池在無線充電過程中，所呈現之循環特性與材料結構之變化進行探討。在研究中發現尖晶石結構之LiMn2O4與橄欖石結構之LiFePO4在無線充電過程中的電容量保持率，優於層狀結構之LiNi0.45Mn0.45Co0.1O2，尖晶石結構與橄欖石結構的正極材料，在經過無線充電測試後，其結構並無明顯變化，然而層狀結構之LiNi0.45Mn0.45Co0.1O2卻產生了相當嚴重的陽離子錯位排列。
　　另外，本研究亦對鋰離子負極材料，在無線充電過程中的循環特性與材料結構之變化進行探討，於實驗中發現尖晶石結構的Li4Ti5O12在無線過程中的電容量維持率高於層狀結構的MCMB(Meso-Carbon Micro-bead)，在經過無線充電測試後Li4Ti5O12的材料結構並無明顯的變化，但是層狀結構之MCMB則碎裂成小顆的碳粒，由此可知尖晶石結構的Li4Ti5O12，具有較佳的結晶結構穩定度，其結果與正極材料所得之結果相同。此外全尖晶石材料所組成之全電池，在無線充電過程中亦保有相當優異的電容量維持率。

　There are two main objectives of this study. The first objective is to synthesize the layered LiAl1-xCoxNi1/3Mn1/3O2 (0≦x≦1/3) cathode material designed by a computational approach. The calculated voltage curve of LiNi1/3Al1/3Mn1/3O2 compound is presented, indicating it is of great potential for a cathode material of lithium ion batteries. Unfortunately, it was found that the LiNi1/3Al1/3Mn1/3O2 compound without impurity phase could not be synthesized via a sol-gel process. To obtain a layered compound without impurity phase, partial of Al is replaced by Co in LiNi1/3Al1/3Mn1/3O2 compound in this study. Layered LiAl1/3-xCoxNi1/3Mn1/3O2 (0≦x≦1/3) compounds were synthesized via sol-gel reaction at 900oC under an oxygen stream. Single phase of the LiAl1/3-xCoxNi1/3Mn1/3O2 in 1/6≦x≦1/3 region could be prepared successfully. The discharge capacity and conductivity increased with an increase in the Co-substitution content. The enhancement of the conductivity and phase purity by the introduction of Co content shows profound influence on the performance of the LiAl1/3-xCoxNi1/3Mn1/3O2 compounds.
　The second object is to develop a wireless charging process for the lithium ion battery. In this work, we developed the wireless microwave charging module to overcome the disadvantages of previous methods. The wireless microwave charging module can charge the implanted lithium ion battery in a suitable distance by tuning the power input and the implanted lithium ion battery shows excellent cycleability after 20 cycles. Although the conversion of the wireless microwave charging is only 2~5%, it can be improved by using other designs of antenna (microwave generation part) and rectify antenna (receive and conversion part).
　The cycling performance of the LiNi0.45Mn0.45Co0.1O2/Li, LiMn2O4/Li, Li4Ti5O12/Li, MCMB/Li, LiFePO4/Li and LiMn2O4/Li4Ti5O12 cells and the structural stability of these electrode materials in the wireless powering process have been investigated in this work. It was found that the capacity retention of the spinel LiMn2O4 and olivine LiFePO4 cathode materials are better than that of the layered LiNi0.45Mn0.45Co0.1O2 in the wireless powering process. The structure of the spinel and olivine materials remains unchanged but the undesired cation mixing was observed in the layered LiNi0.45Mn0.45Co0.1O2.
　The cycling performance and the structural stability of these various anode materials in the wireless powering process have also been investigated in this work. It was found that the capacity retention of the spinel Li4Ti5O12 is better than that of the layered MCMB (Meso-carbon Micro-bead) in the wireless powering process. The structure of the Li4Ti5O12 materials remains unchanged but the particles of the MCMB were disintegrated significantly after the cycling, indicating that the structural stability of the spinel anode is much better than that of the layered one in the wireless powering process. It is worthy to note that the same observation has been reported for the cathode materials in the wireless powering process. Consequently, the full cell of LiMn2O4/Li4Ti5O12 was demonstrated to be excellent capacity retention in the wireless powering process.

目 錄
第一章 緒論……………………………………………………………1
1-1 無線能量傳輸之發展………………………………………2
1-2 鋰離子電池之發展…………………………………………5
1-2-1 鋰離子電池正極材料發展之文獻回顧…………………7
1-2-1-1 LiCoO2層狀結構之正極材料…………………………8
1-2-1-2 LiNiO2層狀結構之正極材料…………………………12
1-2-1-3 LixNi1-yCoyO2層狀結構之正極材料……………… 15
1-2-1-4 LixNi1-y-zCoyMnzO2層狀結構之正極材料…………17
1-2-1-5 LiNixCo1-2xMnxO2層狀結構之正極材料……………24
1-2-1-6 Li[Li1/3-2x/3NixMn2/3-x/3]O2層狀結構之正極材料………25
1-2-2 尖晶石結構之正極材料……………………………………… 29
1-2-2-1 LiMn2-x-yMxNyO4尖晶石結構之正極材料…………… 31
1-2-3 球狀及柱狀之鋰離子電池正極材料………………………… 33
1-2-4 LiFePO4橄欖石結構正極材料…………………………………36
1-2-4-1 固態燒結法……………………………………………39
1-2-4-2 溶膠凝膠法…………………………………………… 42
1-2-4-3共沉澱法…………………………………………………47
1-2-4-4微乳化法…………………………………………………49
1-2-4-5 水熱法…………………………………………………51
1-2-5 鋰離子電池高電壓正極材料…………………………………53
1-3 負極材料………………………………………………………… 56
1-3-1 碳材負極材料……………………………………………56
1-3-2 非碳材負極材料…………………………………………58
1-3-2-1 鋰合金………………………………………………58
1-3-2-2金屬氧化物………………………………………… 59
1-3-2-3 矽合金與矽複合物…………………………………62
1-3-3 Li4Ti5O12負極材料…………………………………… 65
1-4電解質………………………………………………………………66
1-4-1 液態電解質………………………………………………66
1-4-2 高分子電解質……………………………………………67
1-4-2-1 固態高分子電解質……………………………………67
1-4-2-2 膠態高分子電解質……………………………………68
1-5 隔離膜…………………………………………………………… 69
1-6研究動機……………………………………………………………71
第二章 實驗原理與方法………………………………………………72
2-1 實驗藥品………………………………………………………… 72
2-2 儀器設備………………………………………………………… 73
2-3 正極材料製備…………………………………………………… 74
2-4 材料鑑定………………………………………………………… 76
2-4-1 X光繞射原理…………………………………………… 76
3-4-2X光繞射分析條件………………………………………… 77
2-4-3 SEM表面形態分析……………………………………… 77
2-5 電化學性質量測………………………………………………… 78
2-5-1 陰極極片之製作………………………………………… 78
2-5-2 鈕扣型電池組裝………………………………………… 79
2-5-3 充放電測試…………………………………………………… 82
2-5-3-1 傳統充放電測試……………………………………… 82
2-5-3-2 無線充放電測試……………………………………… 82
第三章 正極材料合成……………………………………………… 87
3-1 Co含量對LiAl1/3-xCoxNi1/3Mn1/3O2電化學特性之影響…… 88
3-1-1 理論計算………………………………………………… 88
3-1-2 LiAl1/3Ni1/3Mn1/3O2合成與電化學特性……………………92
3-2 結論………………………………………………………………105
第四章 無線充電對鋰離子電池材料之影響……………………… 106
4-1 無線充電效率及充電電路對電池充放電效率之影響…………107
4-2無線充電對鋰離子電池正極材料之影響……………………… 116
4-2-1層狀與尖晶石正極材料…………………………………… 116
4-2-2 橄欖石正極材料………………………………………… 128
4-3無線充電對Li4Ti5O12與MCMB負極材料之影響……………… 136
4-4 結論………………………………………………………………149
第五章 總結…………………………………………………………152
第六章 未來研究方向………………………………………… 155

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