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博碩士論文 etd-0911109-150644 詳細資訊
Title page for etd-0911109-150644
論文名稱
Title
DMFC性能衰退原因探討及16-cell DMFC電池組研發
Studies of the Performance Decay of a DMFC and the Development of a 16-cell DMFC Stack
系所名稱
Department
畢業學年期
Year, semester
語文別
Language
學位類別
Degree
頁數
Number of pages
78
研究生
Author
指導教授
Advisor
召集委員
Convenor
口試委員
Advisory Committee
口試日期
Date of Exam
2009-09-04
繳交日期
Date of Submission
2009-09-11
關鍵字
Keywords
碳纖維束單極板、直接甲醇燃料電池、自然進氣
air-breathing, carbon fiber Monopolar plate, DMFC
統計
Statistics
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中文摘要
本論文主要在發展與製作不須變壓的16-cell可攜式直接甲醇燃料電池(簡稱DMFC)電池組,此電池組可直接提供手機操作或充電。製作電池組之前首先探討DMFC性能衰退原因及避免電池組因未適當保存引起的性能衰退,此外亦探討膜極組(MEA)的處理方式對DMFC性能的影響,最後找出DMFC最佳的保存與處理方式。
為避免甲醇crossover導致陰極毒化,DMFC操作時應使用適當濃度甲醇,實驗結束前電池須適當的放電。此外電池組不使用時,MEA須維持適當溼潤,藉著這些措施可使性能不致快速衰退。此外,在陰極觸媒使用Pt/Ru取代Pt,亦為避免陰極毒化的有效措施。
16-cell電池組使用本實驗室所發展出的新型非均質碳纖維束單極板,與兩片各含8組電極的MEA,在電池外部將16個cell串聯而成。此輕巧型16-cell DMFC電池組總體積約99cc (長9cm×寬5.5cm×厚2.0 cm),重量約55g(不含3M甲醇溶液20cc),總電極面積約50 cm2 (16cell × 3.15cm2 per cell)。應用本燃料電池實驗室所發展的碳纖維束單極板與MEA製作,16-cell電池在常溫自然吸氣下,電壓在4V時,輸出總功率可達1.65W,功率密度33 mW/cm2,重量功率密度22.4mW/g,體積功率密度可達16.9mW/g。此電池可直接提供一般手機使用或充電。
Abstract
In this paper, a 16-cell direct methanol fuel cell (called DMFC) stack was developed to power or charge a mobile phone without any voltage transformer. The various types of the performance decay of DMFCs are studied before a 16-cell DMFC stack is made. The decays due to improper storage are found and avoided. The influences of the MEA treatments on the performance are also studied. Eventually, we try to find the best storage and treatment methods to keep stacks in a good condition all the way.
In order to solve the problem of methanol crossover lead to the cathode poisoned, it is necessary to operate under the proper methanol concentration and to discharge before finishing the whole experiment. It is also necessary to maintain MEAs in proper wetness so that the performance will not decline during storage. Additionally, the catalyst in the cathode will use Pt/Ru to replace Pt.
This 16-cell DMFC stack is composed of two 8-banded MEAs and 16 carbon fiber bunches. Each MEA is made with 8 sets of electrodes on a piece of membrane. The stack with 16 cells will be connected in series outside of the reaction chamber. The weight and volume of this 16-cell DMFC stack are 55 g (not including 20 c.c. methanol solution) and 99 cm3. The total electrode is 50 cm2 (16-cell×3.15 cm2 per cell). The power at voltage 4V is 1680mW when it is operating at room temperature and air breathing. The maximum power density can reach 33 mW/cm2. The specific power density is 22 mW/g and the volumetric power density is 16.9 mW/cm3. This stack can power or charge a mobile phone directly.
目次 Table of Contents
目錄
目錄 I
圖目錄 IV
表目錄 VII
中文摘要 VIII
英文摘要 IX

第一章 緒論 1
1.1前言 1
1.2燃料電池 2
1.3 文獻回顧 3
1.4研究目的 7
第二章 直接甲醇燃料電池理論分析 8
2.1甲醇於DMFC中之理論消耗量 10
2.2燃料電池質傳現象 10
2.3 燃料電池極化現象 11
第三章DMFC電池組設計與元件製作 14
3.1 DMFC電池組設計 14
3.1.1Banded Type MEA 14
3.1.2單/雙極板 15
3.1.2.1單/雙極板功能 15
3.1.2.2傳統硬質表面單/雙極板 15
3.1.2.3新型非均質碳纖維單/雙極板 16
3.1.2.4碳纖維單/雙極板與傳統單/雙極板的優劣比較 17
3.2 DMFC電池組製作 18
3.2.1碳纖維束製造流程 19
3.2.2 MEA製作 22
3.2.2.1 質子交換膜處理 22
3.2.2.2電極預備 22
3.2.2.3 MEA熱壓 23
3.2.3 16-cell電池組 23
第四章 實驗方法 25
4.1 實驗材料與設備 25
4.2 實驗步驟 26
第五章 實驗結果與分析 28
5.1單電池含水量對性能影響 28
5.2 DMFC性能衰退與對策 28
5.2.1 保存方式對DMFC性能之影響 29
5.2.2 MEA重新熱壓與煮稀硫酸對恢復性能的影響 30
5.2.3稀硫酸濃度對性能之影響 30
5.2.4 MEA浸泡醇類對性能恢復的影響 31
5.3 MEA處理方式對DMFC性能提昇的影響 32
5.3.1 MEA浸泡不同甲醇濃度對性能之影響 33
5.3.2 MEA浸泡不同醇類對性能之影響 34
5.4不同甲醇溶液濃度對性能之影響 34
5.5避免DMFC性能衰退之措施 35
5.6暫態性能測試 35
5.7 16-cell電池組性能與應用 36
5.8 16-cell與其它DMFC之比較 36
第六章 結論 37
參考文獻 38









圖目錄
圖1.1 直接甲醇燃料電池工作原理示意圖 40
圖3.1MEA與傳統硬質表面單極板結合 41
圖3.2MEA與新型碳纖維束單極板結合 41
圖3.3 16-cell DMFC電池組零件組示意圖 42
圖3.4 16-cell DMFC電路串聯購造示意圖 42
圖3.5 18K碳纖維 43
圖3.6圓形紙筒上碳纖維束均勻展開纏繞於方形捲筒上 43
圖3.7 方形捲筒的3束薄層纖維束同時逆向並排反繞於另一端的圓柱形捲筒 44
圖3.8上膠機 44
圖3.9步級馬達驅動二可捲動的柱狀圓筒 45
圖3.10沾膠後不鏽鋼線橫向加膠於薄纖維束上 45
圖3.11加膠後碳纖維片 45
圖3.12 20mm的碳纖維薄片,中央黏貼長45mm×1.5mm寬的固態熱熔膠 46
圖3.13為碳纖維堆疊步驟 46
圖3.14堆疊好的碳纖維放至熱壓機準備熱壓 47
圖3.15纖維束熱壓完成分割前照片 47
圖3.16纖維束分割及修整後照片 47
圖3.17 16-cell膜極組熱壓前電極與烤盤紙 48
圖3.18電極熱壓模具 48
圖3.19三點式熱壓機 49
圖3.20 熱壓完16-cell MEA 49
圖3.21 16-cell零組件 50
圖3.22 16-cell組裝後 50
圖4.1單電池零組件 51
圖4.2單電池組裝後 51
圖4.3電子負載器 52
圖4.4三用電表(KEITHLEY 2000) 52
圖5.1 MEA煮稀硫酸與沒煮稀硫酸之單電池性能曲線比較 53
圖5.2保存時間對DMFC性能之影響(放置於大氣中) 53
圖5.3 質子交換膜在水中膨脹、收縮量與時間關係 54
圖5.4保存時間對DMFC性能之影響(每次實驗完保存於DI water中) 54
圖5.5 MEA處理方式對性能恢復之影響 55
圖5.6 MEA煮不同稀硫酸濃度對性能恢復之影響 55
圖5.7 MEA不同處理方式對性能恢復之影響,初始最大功率密度(a) MEA1 6mW/cm2(b) MEA2 10mW/cm2 56
圖5.8 MEA未經任何處理電池性能與時間關係 57
圖5.9 MEA不同處理方式對性能之影響 57
圖5.10 MEA放置在防潮箱、煮水與浸泡甲醇溶液對性能之影響 58
圖5.11 MEA浸泡不同濃度甲醇對DMFC性能之影響 58
圖5.12 MEA浸泡在純甲醇電極剝離的情形 59
圖5.13 MEA浸泡不同醇類對性能之影響 59
圖5.14浸泡異丙醇水溶液 60
圖5.15甲醇濃度對DMFC性能之影響 60
圖5.16陰極使用Pt/Ru,浸泡去離子水與甲醇溶液對性能之影響 61
圖5.17陰極使用Pt/Ru與Pt性能比較 61
圖5.18不同初始甲醇濃度,負載1Ω下,輸出電壓隨著時間之變化 62
圖5.19初始甲醇濃度3M於30min時補充純甲醇電壓隨時間之變化 62
圖5.20 16-cell DMFC stack輸出電壓與功率隨電流之變化 63
圖5.21 16-cell DMFC平均電壓與功率密度隨電流密度之變化 63
圖5.22 16-cell DMFC應用於3C手機上 64
表目錄
表5-1小於 2Watt之DMFC系統的比較 65
表5-2本研究室發展的DMFC電池組之比較 66
參考文獻 References
1."Optimization of properties and operating parameters of a passive DMFC mini-stack at ambient temperature," V. Baglio, A. Stassi, F.V. Matera, A. Di Blasi, V. Antonucci, A.S. Arico, Electrochemistry Communications 10 (2008) 1606–1609.
2."Performance evaluation of passive direct methanol fuel cell with
methanol vapour supplied througha flow channel,"Ikwhang Chang, Seungbum Ha, Jinho Kim,JaeYong Lee, Suk Won Cha, Journal of Power Sources 184(2008)9-15.
3."Performance improvement in direct methanol fuel cells using a highly porous corrosion-resisting stainless steel flow field,"Toshio Shudo , Kensuke Suzuki.
4."MEA with double-layered catalyst cathode to mitigate methanol crossover in DMFC ,"Tongtao Wang, Caishun Lin, Feng Ye, Yong Fang, Jingjing Li, Xindong Wang, Electrochemistry Communications 10(2008) 1261–1263.
5."Influence of cathode oxygen transport on the discharging time of passive DMFC,"Qin-Zhi Lai, Ge-Ping Yin, Jian Zhang, Zhen-Bo Wang, Ke-Di Cai, Peng Liu, Journal of Power Sources 175 (2008) 458–463.
6."A Novel Design of a Cylindrical Portable Direct Methanol Fuel Cell," Lee, Ming-San., Chen, Long-Jeng., Hung, Min-Fa, Lo, Ming-Yuan, Sue, Shan-Jay, LO, Chin-Hung, and Wang, Yung-Pin 2003, J. of Fuel Cell Science and Technology, Vol. 5, No 3, 031004-1~8, Aug. 2008.
7."A novel anode for preventing liquid sealing effect in DMFC,"M.B. Ji, Z.D. Wei, S.G. Chenb, X.Q. Qi, L. Li, Q. Zhan, C. Liao, R. Tang, i n t e r n a t i o n a l j o u rna l o f hydrogen energy 34 (2009) 2765 – 2770.
8."低成本自然吸氣式可攜式直接甲醇燃料電池組開發與製作研究,"洪嘉隆,碩士論文,國立中山大學機械與機電工程學系國中華民國九十六年七月。
9."A novel MEA architecture for improving the performance of a DMFC,"Chunguang Suo, Xiaowei Liu, XiaoChuan Tang, Yufeng Zhang, Bo Zhang, Peng Zhang, Electrochemistry Communications 10 (2008) 1606–1609.
10."The improved methanol tolerance using Pt/C in cathode of direct methanol fuel cell,"Yong-Hun Cho, Hyun-Seo Park, Yoon-Hwan Cho, In-Su Park, Yung-Eun Sung, Electrochimica Acta 53 (2008) 5909–5912.
11."Development of a heterogeneous composite bipolar plate of a Proton Exchange Membrane Fuel Cell, " Ming-San Lee, Long-Jeng chen,Zheng-Ru He,Shih-Hong Yang,The Journal of Fuel Cell Science and Technology,2005.
12."Development of a 2W Direct Methanol Fuel Cell Power Source, "Xie, C.G., Bostaph, J., and Pavio, J., 2004, J. Power Sources, Vol. 136, pp. 55–65.
13."Toshiba’s Direct Methanol Fuel Cell Officially Certified as World’s Smallest by Guinness World Records," Toshiba Corporation, 2005, http://www.toshiba.co.jp/about/press/2005_02/pr2801.htm,2005/2/28.
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