全球暖化問題引發人們對環保議題的關注，推動發展再生能源和尋找替代能源。在這個背景下，燃料電池因其優點成為未來最具潛力的動力來源。隨著科技進步，行動裝置趨向輕薄短小、易於穿戴和收納，因此可撓性電池成為當前的熱門研究課題。雙極板作為燃料電池的核心部件之一，是燃料電池運作的基礎結構體，不僅佔整個燃料電池成本的23%，還構成了大部分的重量。
為了降低成本和重量，本研究針對雙極板進行深入探討，選擇熱塑性聚氨酯為基體，與28 wt%牡蠣殼粉混練，製作出複合材料雙極板。並進行三種不同含水量石墨稀的噴塗，最後與3D列印所製造的TPU端版組成可撓曲質子交換膜燃料電池，對其進行全面分析。
研究結果顯示，在粒狀原物料分析方面，添加28 wt%的OS導致複合材料的流動指數上升約52.26%，而添加OS提高了複合材料的熱穩定性，並且未發現新的化學變化；不同OS添加比例下的TPU/OS複合雙極板分析方面，XRD和拉曼分析證實OS為填充劑，SEM觀察顯示添加OS後產生顆粒聚集，拉伸後的孔洞增加；EDS分析確認鈣元素微小團聚；表面粗糙度明顯增加；不論是否添加OS，TPU/OS複合雙極板皆具親水性；添加OS後的雙極板在腐蝕環境中有較佳的耐腐蝕性；不同含水量石墨稀表面改質TPU/OS複合雙極板分析方面，XRD和Raman分析顯示，石墨稀無論有無添加OS都成功覆蓋表面，SEM觀察顯示TPU/OS雙極板較厚，EDS顯示主要元素為碳、氮和氧，腐蝕電位和電流結果顯示TPU/OS雙極板耐腐蝕性優於純TPU雙極板，附著力與導電性分析結果顯示TPU/OS雙極板附著力高且平均導電性優於純TPU雙極板；在最佳參數下在不同撓曲半徑下進行單電池測試，電池在彎曲狀態下的最大功率提高了2倍，但效率差和雜訊主要是由極耳接觸不良引起。

Global warming has led to increased attention towards environmental issues, driving the development of renewable energy and the search for alternative sources. Fuel cells have emerged as the most promising future power source due to their numerous advantages. As technology progresses, there is a growing demand for lightweight, compact, and flexible devices, making flexible batteries a hot research topic. Among the key components of fuel cells, the bipolar plate plays a crucial role as the fundamental structural element, constituting 23% of the total fuel cell cost and a significant portion of its weight.
To reduce costs and weight, this study focuses on the bipolar plate, selecting Thermo Polyurethane (TPU) as the matrix material and incorporating 28 wt% of Oyster Shell (OS) powder to produce a composite bipolar plate. Additionally, three different water content graphite slurries were applied via spray coating to the TPU/OS composite, ultimately forming a flexible proton exchange membrane fuel cell with a 3D-printed TPU endplate for comprehensive analysis.
The research findings demonstrate that, in the analysis of granular raw materials, the addition of 28 wt% of OS resulted in an approximately 52.26% increase in the flow index of the composite material. Moreover, the inclusion of OS enhanced the thermal stability of the composite material, with no evidence of new chemical changes. Regarding the analysis of TPU/OS composite bilayer electrodes with varying OS proportions, X-ray diffraction (XRD) and Raman spectroscopy confirmed the role of OS as a filler. Scanning electron microscopy (SEM) observations indicated the emergence of particle aggregation and increased pore formation upon stretching after OS addition. Energy-dispersive X-ray spectroscopy (EDS) verified the presence of localized calcium elements. The surface roughness was notably augmented, and regardless of OS addition, the TPU/OS composite bilayer electrodes exhibited hydrophilicity. The OS-incorporated bilayer electrodes displayed improved corrosion resistance in corrosive environments. In the context of surface-modified TPU/OS composite bilayer electrodes with varying water content of graphene oxide, XRD and Raman analyses revealed successful coverage of the surface by graphene oxide, irrespective of OS addition. SEM observations indicated increased thickness of the TPU/OS bilayer electrodes. EDS analyses highlighted carbon, nitrogen, and oxygen as the primary elemental components. Corrosion potential and current results indicated superior corrosion resistance of TPU/OS bilayer electrodes over pure TPU counterparts. Adhesion and conductivity analyses revealed elevated adhesion and superior average conductivity of TPU/OS bilayer electrodes compared to pure TPU counterparts. Single-cell fuel cell testing under optimal parameters at various bending radii demonstrated a twofold increase in maximum power output under bending conditions. However, observed efficiency disparities and noise were primarily attributed to poor contact at the electrode tab.

摘要................................................................i
Abstract...........................................................ii
誌謝...............................................................iv
目錄................................................................v
表目錄...........................................................viii
圖目錄..............................................................x
符號說明.........................................................xiii
第一章、緒論........................................................1
1.1前言............................................................1
1.2研究動機與目的...................................................4
1.3研究方法........................................................7
1.4論文架構........................................................9
第二章、文獻回顧與基礎理論..........................................10
2.1 燃料電池......................................................10
2.1.1燃料電池種類..................................................11
2.1.2燃料電池運作原理..............................................14
2.1.3燃料電池發展趨勢..............................................16
2.2可撓曲燃料電池..................................................18
2.2.1可撓曲質子交換膜..............................................19
2.2.2可撓曲催化劑層................................................22
2.2.3可撓曲氣體擴散層..............................................24
2.2.4可撓曲雙極板..................................................27
2.2.5可撓曲電池組裝................................................29
2.2.6可撓曲電池系統................................................31
2.2.7可撓曲燃料電池的性能和耐久性...................................33
2.2.8可撓曲燃料電池的發展趨勢.......................................36
2.3雙極板.........................................................37
2.3.1雙極板種類...................................................38
2.3.2可撓曲雙極板發展與相關文獻.....................................41
2.3.3雙極板高分子基材(TPU)介紹.....................................44
2.3.4雙極板添加材(OS)介紹..........................................46
2.4添加碳酸鈣後的機械性質相關文獻...................................47
第三章、實驗方法與設備.............................................48
3.1實驗流程與步驟.................................................49
3.1.1以雙螺桿混煉不同TPU/OS複合材料................................50
3.1.2以射出成形製備不同OS添加比例(0與28wt%)之TPU/OS複合雙極板.......53
3.1.3以不同含水量(20~30 wt%)石墨稀表面改質TPU/OS之複合雙極板........56
3.1.4以光固化3D列印製作可彎曲TPU端版...............................60
3.1.5可撓曲PEMFC之設計與不同曲率半徑之燃料電池實驗..................64
3.2 分析設備介紹.................................................66
3.2.1熔融指數試驗機(Melt Flow Indexer, MI)........................67
3.2.2熱重分析儀(Thermogravimetric Analyzer, TGA).................69
3.2.3差示掃描量熱法(Differential scanning calorimetry, DSC).......71
3.2.4傅立葉轉換紅外光譜(Fourier Transform Infrared Spectroscopy, FTIR).......73
3.2.5萬能試驗機(Universal Testing Machine).......................75
3.2.6蕭氏硬度計(Shore)...........................................79
3.2.7X-ray繞射分析儀(X-ray Diffractometer, XRD)..................81
3.2.8拉曼光譜學（Raman spectroscopy）............................83
3.2.9掃描式電子顯微鏡(Scanning Electron Microscope, SEM)..........85
3.2.10量散射光譜分析儀（Energy Dispersive Spectroscopy, EDS）.....86
3.2.11表面粗度計.................................................87
3.2.12水滴接觸角(Water Contact Angle, WCA).......................89
3.2.13微拉伸試驗機(Tensile Testing Machine)......................91
3.2.14四點探針量測儀(Four Point Probe, FPP)......................93
3.2.15恆電位儀(Potentiostat).....................................95
第四章、實驗結果與討論............................................96
4.1不同OS添加比例(0與28 wt%)之TPU/OS複合粒狀原物料分析.............96
4.1.1不同OS添加比例之TPU/OS複合粒狀原物料之MI分析..................97
4.1.2不同OS添加比例之TPU/OS複合粒狀原物料之TGA分析.................98
4.1.3不同OS添加比例之TPU/OS複合粒狀原物料之DSC分析................100
4.1.4不同OS添加比例之TPU/OS複合粒狀原物料之FTIR分析...............102
4.2不同OS添加比例(0與28 wt%)之TPU/OS複合雙極板分析................104
4.2.1不同OS添加比例之TPU/OS複合雙極板之拉伸試驗...................104
4.2.2不同OS添加比例之TPU/OS複合雙極板之楊氏模量...................106
4.2.3不同OS添加比例之TPU/OS複合雙極板之彈性回復率試驗..............108
4.2.4不同OS添加比例之TPU/OS複合雙極板之硬度試驗...................109
4.2.5不同OS添加比例之TPU/OS複合雙極板之XRD分析...................110
4.2.6不同OS添加比例之TPU/OS複合雙極板之Raman分析...................111
4.2.7不同OS添加比例之TPU/OS複合雙極板之SEM分析...................112
4.2.8不同OS添加比例之TPU/OS複合雙極板之EDS分析...................113
4.2.9不同OS添加比例之TPU/OS複合雙極板之表面粗糙分析...................115
4.2.10不同OS添加比例之TPU/OS複合雙極板之WCA分析...................116
4.2.11不同OS添加比例之TPU/OS複合雙極板之腐蝕試驗...................117
4.3不同含水量(20~30 wt%)石墨稀表面改質TPU/OS複合雙極板分析..............119
4.3.1不同含水量石墨稀表面改質TPU/OS複合雙極板之XRD分析...................119
4.3.2不同含水量石墨稀表面改質TPU/OS複合雙極板之Raman分析...................121
4.3.3不同含水量石墨稀表面改質TPU/OS複合雙極板之SEM分析...................123
4.3.4不同含水量石墨稀表面改質TPU/OS複合雙極板之EDS分析...................125
4.3.5不同含水量石墨稀表面改質TPU/OS複合雙極板之表面粗糙分析分析............127
4.3.6不同含水量石墨稀表面改質TPU/OS複合雙極板之WCA分析...................128
4.3.7含水量25 wt%石墨稀表面改質TPU/OS複合雙極板之腐蝕試驗...................129
4.3.8不同含水量石墨稀表面改質TPU/OS複合雙極板之附著力分析...................131
4.3.9不同含水量石墨稀表面改質TPU/OS複合雙極板之導電率分析...................133
4.4最佳參數含水量25 wt%石墨稀表面改質TPU/OS 28 wt%雙極板之不同撓曲 半徑(0與15.6 cm)之PEMFC單電池測試.....................................................135
第五章、結論與未來展望...................................................137
5.1結論.............................................................137
5.2未來展望.........................................................139
參考文獻..............................................................140
Extended Abstract......................................................147

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