利用網印方法製備全固態石墨烯複合電極於高能量密度之微型電容的研究

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姓名

遲睿功(Jui-Kung Chih) 查詢紙本館藏

畢業系所

機械工程學系

論文名稱

利用網印方法製備全固態石墨烯複合電極於高能量密度之微型電容的研究
(The investigation of high energy density of the all screen printable solid-state microsupercapacitors integrated by graphene based hybrid electrodes)

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摘要(中)

微型超級電容器(micro-supercapacitors，MSCs)由於其體積小、重量輕、極高的充電放電速率和功率密度以及高彎折性，被視為一種微型儲能元件的選擇，以滿足可穿戴電子和高密度整合晶片上日益增長的需求。然而，現今MSCs的所面臨的關鍵挑戰是低能量密度的限制及其複雜、高成本且耗時的製作過程。
本研究展示一種全網版印刷式的微電容製作方法，通過電化學剝離石墨烯和長單壁碳納米管之複合電極，製造全固態（包括電解質）的軟性微電容。其中該方法顯示了一種簡單、快速且可大面積量產的途徑，以用於製造和組裝具有成本效益和高產量的微電容器。
實驗結果顯示本實驗之微電容裝置具有高的單位面積電容7.7 mF/cm2與單位體積電容77.3 F / cm3，並且在15000次循環後仍保持> 99％的優異循環穩定性，這歸因於石墨烯與奈米碳管之複合電極所提供的高擴散路徑和促進離子傳輸能力。在能量和功率密度分別為10.7 mWh / cm3和3.17 W / cm3。此外，當彎曲程度達到0.5mm的曲率半徑時，電容幾乎無劣化，顯示優異的機械柔韌性和工作穩定性。
此外，整體元件的總電荷儲存量可以透過活性材料的垂直疊層的方式來作擴充，而輸出電壓和電流則可以通過串聯和並聯多個MSC元件的設計來提升，以滿足各種應用上的所需。最重要的是，這項工作提供了一種具擴展性且經濟效益的方法來生產高能量密度的固態可撓式微電容，為未來的可穿戴設備開展新的方向。

摘要(英)

Microsupercapacitors (MSCs) is an alternative power source that promises to fulfill the increasing demand for wearable and on-chip electronics due to the small, lightweight, extremely high charge/discharge rate and power density, as well as high flexibility. However, the critical challenge of nowadays MSCs is the limitation of low energy density and their complicated process with the high cost and time-consuming. Here, we reported an all-screen-printable method for fabricating all solid (including electrolyte) and flexible MSCs by rational designed composite electrodes of electrochemical exfoliated graphene (ECG) and long single-walled carbon nanotubes (CNTs), where the method shows features of a facile and scalable route to fabricate and assemble MSCs with cost-effectiveness and high throughput.
As a result, the resulting MSCs device exhibits an areal capacitance of 7.7 mF/cm2 and volumetric capacitance of 77.3 F/cm3, and excellent cyclic stability of >99 % after 15000 cycles, which was due to the creation of high diffusion path and the promotion of ion transport capability. The cell exhibits energy and power densities of 10.7 mWh/cm3 and 3.17 W/cm3, respectively. Moreover, there was negligible degradation on capacitance when suffering the bending deformation with radius reduce to 0.5 mm, indicating excellent mechanical flexibility and operation stability. In addition, the output voltage and current can be rationally designed by multiple connections of MSCs devices in series and parallel to fulfill the demanded applications. This work provides a scalable and cost-effective method to produce solid-state MSCs with high energy density, which paves the way for potential wearable devices.

關鍵字(中)

★ 微型超級電容器
★ 石墨烯
★ 網印

關鍵字(英)

★ microsupercapacitors
★ graphene
★ screen printing

論文目次

摘要 i
Abstract ii
總目錄 iv
圖目錄 vii
表目錄 xi
公式目錄 xii
第一章緒論 1
1-1 前言 1
1-2 電容器介紹 2
第二章研究背景與文獻回顧 4
2-1 微型超級電容器介紹 4
2-2 微型超級電容器之儲能機制 5
2-2-1 電雙層電容器 5
2-2-2 擬電容器 8
2-2-3 混合電容器 9
2-3 微型超級電容器之材料 10
2-3-1 碳材料(Carbon based material) 10
2-3-2 金屬氧化物(Metal oxide) 10
2-3-3 導電高分子(Conducting polymer) 10
2-4 電解液介紹 12
2-5 微電容器製造方式介紹 14
2-5-1 微影 (Photolithography) 14
2-5-2 遮罩輔助圖案化 (mask patterning) 17
2-5-3 雷射掃描與雷射蝕刻 (laser scribing/etching) 19
2-5-4 噴墨印刷 (ink-jet printing) 20
2-6 研究動機 22
第三章實驗方法與分析原理 24
3-1 實驗用品與儀器 24
3-1-1 實驗用品 24
3-1-2 實驗儀器 24
3-2 實驗架構 26
3-3 實驗流程 28
3-3-1 電化學剝離石墨烯製備 28
3-3-2 石墨烯導電漿料配置 28
3-3-3 電解液製備 29
3-3-4 指叉結構設計 29
3-3-5 微電容印刷 31
3-3-6 三極式試片製作 32
3-4 材料分析 33
3-4-1 光學顯微鏡 (Optical Microscopes, OM) 33
3-4-2 掃描式電子顯微鏡 (Scanning Electron Microscope, SEM) 33
3-4-3 穿透式電子顯微鏡 (Transmission Electron Microscope，TEM) 33
3-4-4 探針式輪廓儀 (profiler) 34
3-4-5 黏度計 (Viscometer) 34
3-4-6 四點探針量測儀 (Four Point Probe) 34
3-4-7 X光光電子能譜儀 (X-ray Photoelectron Spectroscopy，XPS) 35
3-4-8 比表面積與孔隙分佈分析儀 (Specific Surface Area & Pore Size Distribution Analyzer by Gas Adsorption Method，ASPS) 35
3-4-9 拉曼光譜分析 (Raman Spectroscopy) 35
3-5 電化學分析 37
3-5-1 循環伏安法分析 (Cyclic Voltammetry，CV) 37
3-5-2 計時電位法分析 (Chronopotentiometry，CP) 37
3-5-3 交流阻抗分析 (Electrochemical Impedance Spectroscopy，EIS) 38
第四章結果與討論 43
4-1 石墨烯漿料之優化 (The optimized study of graphene ink) 43
4-1-1 不同漿料濃度對微電容器特性分析 43
4-1-2添加奈米碳管對ECG電極之影響 49
4-2 調整指叉結構組態 (The optimized study of pattern geometry) 66
4-2-1 指叉寬度對MSCs影響之探討 66
4-2-2 指叉間距對微電容元件之影響 75
4-2-3 微電容元件的穩定性與耐久度測試 80
4-3 輔助電極對微電容器之優化 (Modified the MSCs with additional current collector) 83
4-3-1 形貌與材料分析 83
4-3-2 循環伏安法分析 85
4-3-3 計時電位法分析 88
4-3-4 交流阻抗分析 89
4-4 電解液濃度對微電容的影響 (The influence of electrolyte concentration) 90
4-4-1 循環伏安法分析 91
4-4-2 交流阻抗分析 97
4-4-3 計時電位法分析 98
4-5微電容的整合與應用 (Vertical and in-plane integration of MSCs device) 100
4-5-1垂直疊層對電容效能的影響 100
4-5-2微電容之平面整合 103
4-5-3應用測試 105
4-6各微型電容器之比較 (Compare with previous works) 106
第五章結論 114
第六章未來工作 115
6-1 電解液塗佈方式的優化 115
6-2 電極材料導電性的提升 117
6-2-1 循環伏安法分析 117
6-2-2 交流阻抗分析 119
6-3電極材料離子傳輸效能的提升 120
參考文獻 121

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指導教授

蘇清源(Ching-Yuan Su)

審核日期

2019-6-4

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