多孔金集電層應用於微型固態超級電容器

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姓名

蕭立仁(Li-Ren Hsiao) 查詢紙本館藏

畢業系所

材料科學與工程研究所

論文名稱

多孔金集電層應用於微型固態超級電容器
(All-solid-state micro-supercapacitors with nanoporous-gold current collector)

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摘要(中)

隨著科技發展，攜帶式與穿戴式之電子設備大量生產，舉凡行動裝置與穿戴式活動感應器等設備皆對人類生活習慣帶來巨大影響。然而，能源的消耗隨之增加，電化學儲能裝置的需求也日益增加。其中，可撓性固態微型超級電容器不僅擁有傳統超電容優異的功率密度與儲電能力，更可輕薄化裝置用於有限的空間。
在此研究中，我們使用聚亞醯胺(Polyimide，PI)作為可撓基材，將蒸鍍製程之金銀膜層結構進行合金化與去合金化製程，得到多孔金(Nanoporous-gold，NPG)結構，作為電流收集層。再以濺鍍製程將氧化鉬作為活性物質，進而製備出指叉式微型超電容。製備完成之元件在0.01 mA/cm2 電流密度下，可達到之最高體積比電容值為88.24 F/cm3。經過10000圈穩定度測試之重複充放電後，比電容值維持率為83.54 %，代表試片具有一定的穩定度可多次充放電使用。同時也進行可撓性質之相關測試。在不同彎曲曲率下，進行循環伏安的測試。由測試結果可知，因元件之循環伏安曲線在不同曲率的彎曲下，並未發現有明顯的變化，故元件擁有好的可撓性質。
活性材料的高導電性對於金屬氧化物的擬電容實現高的比電容以及功率和能量密度至關重要。基於金銀膜層電極具備一定之性能，本研究將多孔金電極鍍一層銀薄膜，希望藉此提升效能，結果表示多孔金電極鍍銀能使比電容由78.89提升至88.24 F/cm3。
經過改良後之元件展現一定水準之電化學性能，表示多孔金鍍銀之設計有助於提升效能。結果顯示，本研究所設計之表面與製程在微型固態儲能系統具有巨大的潛力。

摘要(英)

With the development of technology, many portable and wearable electronic devices have been produced and have a great impact on human living habits. However, the consumption of energy has increased, the requirement for electrochemical energy storage devices has also increased. Flexible solid-state micro-supercapacitors (MSCs) not only have the excellent power density and storage capacity, but also can be used in a limited space.
In this work, we use Polyimide as flexible substrates. First, the alloying and de-alloying process of the gold-silver film of the vapor-deposited process is carried out to obtain a nanoporous-gold (NPG) structure as a current collector. Second, a molybdenum oxide is used as an active material in a sputtering process to prepare a finger-type MSC. The MSC device shows the highest volumetric capacitance of 88.24 F/cm3, and the capacitance remains about 83.54 % after a large cycling number of 10000 times. Bending tests are also introduced in this work. Under different bending conditions, the results show that the cyclic voltammetry curves of the device don’t change obviously. This represents that our MSC device has good flexibility.
This work indicates that high conductivity of active materials is important for high specific capacitance and power density of metal oxides. Based on the gold-silver film electrodes have great performance, we coat the porous gold electrode with a silver film by sputtering. The results show that the volumetric capacitance increases from 78.89 to 88.24 F/cm3.
The improved MSC device demonstrates great electrochemical performance. Therefore, the surface and process designed by this work have great potential in micro-solid energy storage systems.

關鍵字(中)

★ 超級電容器
★ 可撓超電容
★ 擬電容
★ 多孔金
★ 電化學
★ 儲能元件

關鍵字(英)

★ Supercapacitor
★ Flexible supercapacitor
★ Pseudocapacitor
★ Nanoporous-gold
★ Electrochemistry
★ Energy storage device

論文目次

摘要 I
Abstract II
目錄 III
圖目錄 VII
表目錄 XI
第一章緒論 1
1.1前言 1
1.2基本原理與文獻回顧 2
1.2.1超級電容器簡介 2
1.2.2超級電容器之電極基板材料 9
1.2.2.1金屬基板 120
1.2.2.2碳材料 120
1.2.2.3石墨烯(Graphene) 121
1.2.2.4碳紙纖維(Carbon fiber paper) 121
1.2.2.5傳統紙基板(Paper) 11
1.2.2.6海綿基板(Spong) 12
1.2.2.7纖維基板(Cabon fiber) 12
1.2.3超級電容器之電極活性材料 12
1.2.4超級電容器之電解質 15
1.2.5超級電容器之電化學原理與技術 19
1.3微型超級電容器 24
1.3.1可撓型超級電容器 26
1.4多孔金屬應用於超級電容器之電極 27
1.4.1多孔金屬之定義 27
1.4.2多孔金屬的製備方式 28
1.4.3多孔金屬應用於超級電容器之優勢 29
1.5研究動機與目的 29
第二章實驗程序與方法 31
2.1實驗藥品 31
2.2製程與分析儀器 2.2.1雷射光罩製作系統(Laser Direct Write Image System) 32
2.2.2光罩對準曝光機(Mask Aligner) 32
2.2.3旋轉塗佈機(Spin Coater) 32
2.2.4高真空電子束暨熱阻式蒸鍍系統(E-gun & Thermal Evaporation System) 33
2.2.5射頻與直流磁控濺鍍機(RF&DC Magnetron Sputtering) 33
2.2.6紫外光臭氧清洗機(UV-Ozone Stripper) 34
2.2.7恆電位儀(Potentiostat) 34
2.2.8快速熱退火系統 (Rapid Thermal Annealing ,RTA) 35
2.2.9掃描式電子顯微鏡(Scanning Electron Microscopy, SEM) 35
2.2.10掃描穿透式電子顯微鏡(Scanning Transmission Electron Microscopy, STEM) 36
2.2.11雙束型聚焦離子束顯微鏡(Dual Beam Focus Ion Beam, DB-FIB) 36
2.3實驗流程 37
2.4實驗製程 37
2.4.1指叉圖形結構與組態之設計 37
2.4.2黃光微影製程(第一道) 39
2.4.3製備金/銀集電極 39
2.4.4集電極(金/銀)掀離製程 39
2.4.5合金化製程 40
2.4.6去合金化製程 40
2.4.7黃光微影製程(第二道) 40
2.4.8製備活性物質 40
2.4.9掀離製程 41
2.4.10製備固態電解質 41
第三章結果與討論(材料分析) 42
3.1片電阻(Sheet Resistance) 42
3.2掃描電子顯微鏡分析(SEM) 43
3.3不同電流收集層材料之MoOx指叉式微型可撓固態超級電容器特性分析 45
3.3.1循環伏安與恆電流充放電分析 46
3.3.2電化學交流阻抗分析 52
3.3.3頻率響應分析 53
3.3.4循環穩定性分析 57
3.3.5可撓指叉式微型固態超級電容器之抗撓曲分析 58
第四章結論 61
第五章參考文獻 62

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指導教授

李勝偉(Sheng-Wei Lee)

審核日期

2019-10-17

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