以乙二醇為基底之深共熔溶劑應用於鈉離子電池電解液之研究

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周品均(Pin-chun Chou) 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

以乙二醇為基底之深共熔溶劑應用於鈉離子電池電解液之研究
(Deep eutectic solvents based on ethylene glycol as electrolytes for sodium-ion batteries)

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摘要(中)

本文主要是研究以乙二醇為基底之新型深共熔(Deep eutectic solvent, DES)電解液之電化學特性，並將其應用於鈉離子電池中。本研究首次提出以便宜且低黏度的乙二醇(Ethylene glycol, EG)作為氫鍵予體，搭配鈉鹽及 [C2mim][BF4]、醋酸膽鹼(ChOAc)，製備出高導電度、製程簡單且價格低廉之新型深共熔電解液。此新型深共熔電解液之電位視窗最大可達4.2 V；在26 ℃之下的離子導電度範圍落在2.3 mS/cm至11.3 mS/cm區間；在25 ℃之下的黏度範圍則落在16 cp至77 cp區間。
與傳統鈉離子電池所使用之有機電解液1 M NaClO4溶於EC-DEC(1:1 v/v) 相比，新型深共熔電解液具有較佳的熱穩定性(~100 ℃熱分解)及更寬廣的應用溫度範圍。且由燃燒測試可知ChOAc及[C2mim][BF4] 均為效果良好之阻燃劑。此外，進一步將此三元電解液系統之應用於鈉離子電池中，以Na0.44MnO2為正極材料、以NaTi2(PO4)3為負極材料，測試不同電解液之電池性能表現及循環穩定性，由實驗結果可知在100 mA/g的電流密度下經過100圈充放電循環後，新型深共熔電解液系統之電容維持率最高可達100 %，幾乎沒有任何電容量衰退; 與之相比，傳統有機電解液系統1 M NaClO4溶於EC-DEC(1:1 v/v) 之電容維持率為94 %，低於其它DES電解液系統。
基於以上實驗結果，可知新型深共熔溶劑可做為一新穎之鈉離子電池電解液，且比起傳統有機電解液系統(1 M NaClO4溶於EC-DEC(1:1 v/v)) 可提高其安全性能，是一項具有發展潛力之電解液選項。

摘要(英)

In this research, we study the electrochemical properties of new Deep eutectic solvent (DES) from the view of their possible application as non-aqueous electrolytes in sodium-ion batteries. The new DES electrolytes are formulated by mixing ethylene glycol, sodium salts and additives (Choline acetate, ChOAc and 1-Ethyl-3-methylimidazolium tetrafluoroborate, [C2mim][BF4]) at room temperature. The potential window of different electrolytes is studied by linear sweep voltammetry (LSV) and cyclic voltammetry (CV) measurements. The new DES electrolytes containing ChOAc and [C2mim][BF4] are found to be electrochemically stable up to 4.1 V and 4.2 V (potential window). The ionic conductivity and viscosity of the new DES electrolytes are found exhibit ranging from 2.3 mS/cm to 11.3 mS/cm at 26 ℃and 16 cp to 77 cp at 25 ℃, respectively.
Compared to conventional organic electrolyte (1 M NaClO4 in EC-DEC (1:1 v/v)), the new DES electrolytes show better thermal stability (~100 ℃) and non-flammability. In addition, different electrolytes used in Na-ion battery system (with Na0.44MnO2 and NaTi2(PO4)3 as a positive and negative electrode, respectively) are tested at room temperature. It was found that the new DES electrolytes show better capacity retention than traditional organic electrolyte (1 M NaClO4 in EC-DEC (1:1 v/v)) after 100 charge-discharge cycles.
Based on its excellent electrochemical properties and cycling performances, the ethylene glycol based new DES can be considered as promising electrolytes for high-safety applications in sodium-ion battery.

關鍵字(中)

★ 電解液
★ 深共熔溶劑
★ 鈉離子電池

關鍵字(英)

論文目次

摘要 i
Abstract iii
致謝 iv
目錄 v
圖目錄 ix
表目錄 xiv
第一章緒論 1
1-1 前言 1
1-2 研究動機 4
第二章文獻回顧 6
2-1 鈉離子電池概述 6
2-1-1 鈉離子電池之發展 6
2-1-2 鈉離子電池之工作原理 10
2-2 鈉離子電池之正極材料 12
2-3 鈉離子電池之負極材料 18
2-4 鈉離子電池之電解液 20
2-4-1 水溶液系統 21
2-4-2有機電解液 24
2-4-3離子液體 30
2-4-4 共熔混合物 34
第三章實驗方法與步驟 41
3-1 實驗流程 41
3-2 實驗藥品及設備 42
3-2-1 實驗藥品 42
3-2-2 實驗設備 45
3-3 正極的製備 47
3-4 負極的製備 47
3-5 電解液的製備 49
3-5-1 醋酸膽鹼(Choline Acetate, ChOAc)的合成 49
3-5-2 電解液的製備 51
3-6 電解液特性分析 54
3-6-1 電位窗(Potential window)量測 54
3-6-2 離子導電度(Ionic conductivity)量測 58
3-6-3 黏度(Viscosity)量測 60
3-6-4熱重分析(Thermogravimetric analyzer, TGA) 61
3-6-5差式掃描熱量分析(Differential Scanning Calorimetry, DSC) 61
3-6-6 凝固觀測溫度(Observed temperature of solidification) 63
3-6-7 燃燒測試(Flammability test) 64
3-7 電池組裝與充放電測試 65
3-7-1 電池組裝 65
3-7-2 循環充放電測試 66
第四章實驗結果與討論 67
4-1電解液特性分析 67
4-1-1電位視窗(Potential window) 67
4-1-2離子導電度(Ionic conductivity) 77
4-1-3黏度(Viscosity) 82
4-1-4熱重分析( TGA) 85
4-1-5差式掃描熱量分析(DSC) 88
4-1-6凝固觀測溫度(Observed temperature of solidification) 91
4-1-7燃燒測試(Flammability) 93
4-2電解液應用於鈉離子電池之循環充放電測試 98
4-2-1充放電特性測試 98
4-2-2循環壽命測試 105
第五章結論與未來工作 112
5-1 結論 112
5-2 未來工作 115
參考文獻 116
附錄 129

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指導教授

李岱洲(Tai-Chou Lee)

審核日期

2015-7-30

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