以CoO及SnO2/ MoS2複合物修飾管狀有序中孔洞碳材CMK-9於高能鋰離子電池負極材料之應用

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林政維(Cheng-Wei Lin) 查詢紙本館藏

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化學學系

論文名稱

以CoO及SnO2/ MoS2複合物修飾管狀有序中孔洞碳材CMK-9於高能鋰離子電池負極材料之應用
(CoO nanoparticles and SnO2/ MoS2 composite confined in tube-like mesoporous carbon as efficient nanocomposite anodes for lithium-ion batteries)

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摘要(中)

本論文主要探討將高理論電容的過渡金屬氧化物 (Transition-metal oxides)及過渡金屬硫化物 (Transition-metal dichalcogenides )修飾於有序中孔洞管狀碳材CMK-9上，應用於鋰離子電池負極的複合材料。利用高分子界面活性劑P123作為模板，和矽源TEOS(Tetraethyl orthosilicate)在酸性下進行合成，得到對稱性為Ia3 ¯d構型為cubic的中孔洞矽材KIT-6，利用糠醇做為碳源將矽材碳化後，可得到有序中孔洞管狀碳材CMK-9。
第一部份為CoO@CMK-9的合成，CoO具有高的理論電容(716 mAh g?1)，價格便宜等優點，但有體積膨脹率大的問題，利用中孔洞碳材CMK-9能限制住充放電時的體積變化，使電容量有所提升，以100 mA/g電流密度進行測試，測試200圈後，電容量仍高達828 mAh/g。
第二部分為利用水熱法一步合成SnO2/MoS2@CMK-9，MoS2為層狀結構，加入SnO2能有效分隔MoS2避免堆疊，CMK-9有增加導電度及限制SnO2體積膨脹的功能，以100mA/g的電流密度，循環測試50圈以後，電容量達782mAh/g。

摘要(英)

Transition metal oxides and Transition-metal dichalcogenides as anode materials in lithium ion batteries have attracted tremendous attention because of their high theoretical capacities compared with commercial graphite. However, the large volume expansion during the charge-discharge process leads to low electrical conductivities.
In first part, we design a tubular nanocomposite of CoO@CMK-9 to overcome this problem. A three-dimensional (3-D) hollow-type ordered mesoporous carbon (CMK-9) could not only provide enough space during the Li+ insertion-extraction process, but also increase the electrical conductivity. CoO is regarded as one of the most promising anode material for lithium ion batteries (LIBs), due to its high theoretical capacity (715 mAh/g), natural abundance, and low cost. CoO@CMK-9 delivers a reversible capacity of 828 mAh/g after 200 cycles at a current density of 100 mAh/g with an outstanding rate performance. The CoO@CMK-9 nanocomposite is expected to have high specific capacity and good cycling performance.
In second part, we design a novel structured SnO2/MoS2@CMK-9, MoS2 is a graphene-like layered structure, Mo is sandwiched between two S layers. The atoms in the layers are bound strongly by covalent bonds, while the adjacent layers interact by weak van der Waals forces. MoS2 nanosheets can be easily restacked together during charge–discharge processes. To solve this problem, we add SnO2 nanoparticles which can avoid to restack of MoS2 nanosheets. SnO2/MoS2@CMK-9 demonstrate an excellent Li-storage performance as an anode of LIBs, deliver a high reversible charge capacity of 782 mAh/g after 50 cycles at a current density of 100 mAh/g.

關鍵字(中)

★ 鋰離子電池
★ 中孔洞碳材
★ 氧化鈷
★ 二氧化錫
★ 二硫化鉬

關鍵字(英)

論文目次

中文摘要 i
謝誌 iv
目錄 v
圖目錄 x
表目錄 xv
第一章緒論 1
1-1前言 1
1-2 二次電池 2
1-3鋰離子電池介紹 4
1-4研究目的 7
第二章文獻回顧 9
2-1 有序中孔洞碳材 9
2-1-1奈米模鑄法 ( Nanocasting )合成機制 12
2-1-2奈米模鑄法合成有序中孔洞碳材之發展 14
2-2 負極材料 21
2-2-1碳材 21
2-2-2 非碳材 25
2-2-3 碳材-非碳材複合材料 26
2-2-3-1 氧化鈷(CoO)修飾碳材的負極材料 28
2-2-3-2 二硫化鉬(MoS2)修飾碳材的負極材料 35
第三章實驗方法 40
3-1 藥品 40
3-2奈米模鑄法合成三維孔道結構 (Ia3d)中孔洞碳材 42
3-2-1三維立方Ia3d中孔洞矽材模板KIT-6合成 42
3-2-2三維立方Ia3d中孔洞管狀碳材CMK-9合成 42
3-3含浸法合成CoO@CMK-9負極複合材料 43
3-4水熱法合成SnO2/MoS2@CMK-9負極材料 43
3-5材料電化學測試 45
3-5-1負極極片製作 45
3-5-2硬幣型電池組裝 45
3-5-3電池性能測試方法 47
3-5-3-1定(變)電流充放電循環測試 47
3-5-3-2電化學阻抗分析 (EIS) 47
3-5-3-3循環伏安法 (CV) 47
3-6實驗鑑定儀器 48
3-7鑑定儀器之原理 49
3-7-1同步輻射光束線 49
3-7-2 X射線粉末繞射 (Powder X-Ray Diffractometer, XRD) 52
3-7-3氮氣等溫吸脫附曲線、表面積與孔洞特性鑑定 53
3-7-4熱重分析儀 (Thermogravimetric Analyzer, TGA) 57
3-7-5 穿透式電子顯微鏡 (Transmission Electron Microscope, TEM) 59
3-7-6掃描式電子顯微鏡 (Scanning Electron Microscope, SEM) 60
第四章結果與討論 62
4-1含浸法合成CoO@CMK-9負極複合材料 62
4-1-1 小角度X光繞射圖譜分析(SAXRD) 62
4-1-2大角度X光繞射圖譜分析 64
4-1-3氮氣吸脫附結果分析 66
4-1-4 熱重分析(TGA) 70
4-1-5 SEM結果分析 72
4-1-6 TEM結果分析 74
4-1-7 XPS結果分析 79
4-1-8 拉曼光譜分析 80
4-1-9 CoO@CMK-9電性分析 81
4-1-10循環伏安法分析 85
4-1-11 交流阻抗分析 87
4-1-12充放電後的SEM結果分析 90
4-2水熱法合成SnO2/MoS2@CMK-9負極複合材料 92
4-2-1 X光繞射圖譜分析(XRD) 92
4-2-2氮氣吸脫附結果分析 95
4-2-3 熱重分析(TGA) 98
4-2-4 SEM結果分析 100
4-2-5 TEM結果分析 103
4-2-6 XPS結果分析 106
4-2-7拉曼光譜分析 107
4-2-8 SnO2/MoS2@CMK-9電性分析 108
4-2-10循環伏安法分析 112
4-2-11交流阻抗分析 114
第五章結論 118
參考文獻 120

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指導教授

高憲明

審核日期

2018-7-24

推文