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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
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dc.contributor.advisor | 趙基揚(Chi-Yang Chao) | |
dc.contributor.author | Chih-Ting Wang | en |
dc.contributor.author | 王誌亭 | zh_TW |
dc.date.accessioned | 2021-05-20T19:58:32Z | - |
dc.date.available | 2014-08-22 | |
dc.date.available | 2021-05-20T19:58:32Z | - |
dc.date.copyright | 2011-08-22 | |
dc.date.issued | 2011 | |
dc.date.submitted | 2011-08-18 | |
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G., Proton-Exchange Membranes by Radiation Grafting of Styrene onto Fep Films .4. Evaluation of the States of Water. J Appl Polym Sci 1995, 57 (7), 855-862. 64. Kusumocahyo, S. P.; Sano, K.; Sudoh, M.; Kensaka, M., Water permselectivity in the pervaporation of acetic acid-water mixture using crosslinked poly(vinyl alcohol) membranes. Sep Purif Technol 2000, 18 (2), 141-150. | |
dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/8570 | - |
dc.description.abstract | 本論文主要目的是製備磺酸化sulfonated poly ( styrene – block - (ethylene – ran - butylene) – block - styrene) (sSEBS)交聯質子傳導膜,研究交聯後質子交換膜的性質和微結構,以期應用於氫氧燃料電池或是甲醇燃料電池。
本論文分二部分:第一部份是以不同醇官能基數目的一級醇作為交聯劑,第二部分為合成具磺酸根的一級醇作為交聯劑。交聯的形成是利用在高溫熱處理時sSEBS的磺酸根會和交聯劑的醇基進行脫水形成磺酸酯鍵結。此二部分合成的交聯膜將對微結構、熱穏定性、機械強度、耐化學性和質子傳導性質等依交聯劑添加量的不同作系統性的研究。 在第一部分我們以glycerol, D-mannitol 和poly vinyl alcohol ( PVA )此三種具不同數目醇基的交聯劑作比較。前二者可分類為小分子的交聯劑,PVA則是以高分子型態進行掍摻交聯。在加入以上交聯劑後的sSEBS交聯膜顯現出熱穏定性、機械強度的提升;耐化學性則是依具化學結構和交聯劑的添加量而改變。微結構的觀察裡,glycerol和mannitol 交聯的質子交換膜和初始sSEBS膜具有相同的微結構,並不會受到交聯劑添加量多寡的影響。但PVA交聯膜則是在PVA添加到一定量以上時開始有微結構的變形。離子交換容率和質子傳導度則是由於交聯時犧牲磺酸根,故隨著交聯劑的添加而減少,PVA交聯膜在此方面的影響尤其顯著。甲醇滲透率則是隨著glycerol和PVA的添加而能有效下降,但mannitol則是顯出上升的趨勢。變溫變濕試驗顯示交聯後的sSEBS薄膜有著質子傳導度的提升,特別是在低濕狀態中,可能原因為交聯後的結構具有保水性和交聯劑的醇基也提供了部份保水性。質子傳導度則是出現較複雜的趨勢,此可能和交聯劑分子大小、交聯後的結構與交聯劑添加量有關。 第二部份我們合成具磺酸根的苯環交聯劑,離子交換容率和質子傳導度並沒有隨著交聯劑的摻入量增加而降低,代表交聯劑上的磺酸根的確可補償sSEBS因為交聯所失去的磺酸根。另外此交聯膜在阻擋甲醇滲透和耐化學性方面皆比未交聯的sSEBS膜好。 | zh_TW |
dc.description.abstract | The major purposes of this thesis are to prepare crosslinked sulfonated poly(styrene-block-(ethylene-ran-butylene)-block-styrene) (sSEBS) membranes as the proton conducting membranes for proton exchange membrane fuel cells (PEMFCs) and direct methanol fuel cells (DMFCs) as well as to investigate the properties and the microstructure of the crosslinked membranes. Two parts of studies are presented using non-sulfonated (Part I) or sulfonated (Part II) multi-functional alcohols as crosslinkers. Crosslinking occurs within the sulfonated polystyrene (sPS) domains through the formation of sulfonate esters between the hydroxyl groups of the crosslinkers and the sulfonic acids of sPS via thermal curing. In each part, the dependence of transport properties, thermal stability, mechanical strength, chemical stability and morphology of the membrane on the chemical structure and the loading amount of the crosslinkers are systematically studied.
In the first part, the crosslinkers with different number of hydroxyl groups, including glycerol, D-mannitol and poly(vinyl alcohol) ( PVA ). The first two alcohols are classified as low molecular weight crosslinkers and PVA is classified as polymeric crosslinker.The introduction of these crosslinkers is demonstrated to improve the thermal stability, mechanical strengths and chemical stability and the enhancements are found to relate to the chemical structure and the loading amount of the crosslinkers. The microstructure of the crosslinked membranes are similar to that of the prisitine sSEBS membrane when glycerol and mannitol are used regardless the loading amount while the addition of PVA with high loading amount alters the microstructure. Ion exchange capacity and proton conductivity decrease with increasing loading of crosslinkers due to the loss of sulfonic acids to form crosslinking and the use of PVA leads to the most significant decrease comparing with pristine sSEBS. The use of glycerol and PVA provide the crosslinked membranes suppressed methanol crossover and improved selectivity. The crosslinked membranes also show much improved proton conductivity at elevated temperature and low relative humidity, probably owing to the better water retention within the membrane attributed to the presence of crosslinks and the hydroxyl groups of the crosslinkers. All the transport properties show complicated trends against the chemical structure and the loading amount of the crosslinkers. In the second part, a novel bifunctinoal alcohol containing two sulfonic acids is designed and synthesized as the crosslinker. Interestingly, IEC and proton conductivity of the corresponding crosslinked membrane are almost constants regardless the loading amount of the crosslinkers, indicating the use of this novel crosslinker could compensate the loss of sulfonic acids originating from the crosslinking. The resulted membranes also exhibit lower methanol permeability and enhanced selectivity. In addition, these membranes also show improved chemical resistance comparing with pristine sSEBS. | en |
dc.description.provenance | Made available in DSpace on 2021-05-20T19:58:32Z (GMT). No. of bitstreams: 1 ntu-100-R97527049-1.pdf: 5986816 bytes, checksum: 80973017aa1f6b06a950c92e5dfc40ee (MD5) Previous issue date: 2011 | en |
dc.description.tableofcontents | 誌謝......................................................................II
中文摘要.................................................................III Abstract...................................................................V 目錄.....................................................................VII 圖索引.....................................................................X 表索引...................................................................XIV 第一章 緒論...............................................................1 1.1 研究背景.......................................................1 1.2 實驗目的與策略.................................................2 第二章 文獻回顧...........................................................3 2.1 燃料電池介紹...................................................3 2.2 質子交換膜.....................................................6 2.2.1 團鍊共聚高分子電解質質子交換膜(Block polyelectrolyte).....9 2.2.2 Block copolymer,sulfonated SEBS之介紹....................13 2.3 高分子交聯之介紹..............................................16 2.3.1 Interpenetration network membrane (IPN membrane).........18 2.3.2 Ionically crosslinked acid base blends and acid base ionomer membrane..........................................19 2.3.3 Covalently Crosslinked Membrane...........................20 第三章 實驗步驟與原理....................................................24 3.1 實驗使用之藥品................................................24 3.2 所需藥品之製備................................................25 3.2.1 磺酸化 poly(styrene—b—(ethylene–ran–butylene)—b— styrene)(sulfonated SEBS,sSEBS)之製備................25 3.2.2 Polystyrene sulfonic acid(PSSA)之磺酸酯反應.............26 3.2.3 2,2'-(biphenyl-4,4'-diylbis(oxy))diethanol(BPDO)之製備..26 3.2.4 Sodium 4,4'-bis(2-hydroxyethoxy)biphenyl 3,3'-disulfonate.26 3.2.5 4,4'-bis(2-hydroxyethoxy)biphenyl-3,3'-disulfonic acid....27 3.3 交聯薄膜之製備................................................27 3.3.1 sSEBS溶液之調配...........................................27 3.3.2 調配交聯劑高分子溶液與成膜................................28 3.3.3 熱處理形成交聯薄膜興脫膜..................................28 3.4 質子傳導膜之性質分析..........................................28 3.4.1 傅立葉紅外線光譜儀(FTIR)................................28 3.4.2 穿透式電子顯微鏡(TEM)...................................28 3.4.3 核磁共振磁譜儀(Nuclear magnetic resonance,NMR).........29 3.4.4 小角度X光繞射(Small Angle X-ray Scattering, SAXS).......29 3.4.5 熱示差掃描卡量計(Differential Scanning Calorimetry,DSC)29 3.4.6 熱重分析儀(Thermal Gravimetric Analyze, TGA)............29 3.4.7 拉伸強度試驗(Tensile test)..............................30 3.4.8 質子傳導度量測(Proton conductivity).....................30 3.4.9 吸水率(Water uptake)....................................31 3.4.10 離子交換容率(Ion Exchange Capacity,IEC)...............31 3.4.11 甲醇滲透率之測定(Methanol permeability)................32 3.4.12 氧化穏定性 (Fenton Test)...............................32 第四章 結果與討論........................................................33 4.1 SEBS之磺酸化..................................................33 4.2 Polystyrene sulfonic acid(PSSA) 的sulfonate ester 的形成和交 聯條件之選定..................................................35 4.3 sSEBS質子交換膜之製備與性質...................................39 4.3.1 Crosslinked sSEBS 於TEM下的結構...........................40 4.3.2 Crosslinked sSEBS的Small-angle X-ray圖譜探討..............45 4.4 TGA分析.......................................................48 4.5 交聯膜的質子交換膜性質探討....................................56 4.5.1 離子交換容率(IEC).......................................56 4.5.2 質子傳導度(proton conductivity,PTC)的比較..............57 4.5.3 吸水率(water uptake,WU)的比較..........................58 4.5.4 甲醇滲透率(methanol permeability)的比較.................58 4.5.5 交聯膜的選擇性(selectivity).............................59 4.6 以DSC觀察質子交換膜水分子性質.................................61 4.6.1 變溫變濕環境質子傳導度....................................63 4.7 質子交換膜強度性質的探討......................................66 4.7.1 膜拉伸強度................................................66 4.7.2 化學耐性的測試 (Fenton Test)............................67 4.8 具磺酸基團的苯環交聯劑設計和合成..............................68 4.9 BPDO和sBPDO交聯質子交換膜的性質探討...........................72 4.9.1 BPDO和sBPDO之SAXS之微結構.................................72 4.9.2 BPDO和sBPDO之TGA..........................................75 4.9.3 sBPDO之質子交換膜性質.....................................76 第五章 結論..............................................................80 第六章 未來展望..........................................................81 參考文獻..................................................................82 | |
dc.language.iso | zh-TW | |
dc.title | 磺酸化苯乙烯-乙烯/丁烯-苯乙烯嵌段共聚合物之交聯質子交換膜 | zh_TW |
dc.title | Crosslinked Sulfonated Polystyrene-block-poly(ethylene-ran-butylene)-block-polystyrene as Proton Exchange Membrane | en |
dc.type | Thesis | |
dc.date.schoolyear | 99-2 | |
dc.description.degree | 碩士 | |
dc.contributor.oralexamcommittee | 林金福(King-Fu Lin),邱文英(Wen-Yen Chiu),諸柏仁(Peter Po-Jen Chu) | |
dc.subject.keyword | 燃料電池,質子交換膜,交聯,團鍊共聚高分子,sSEBS, | zh_TW |
dc.subject.keyword | fuel cell,proton exchange membrane,crosslink,block copolymer,sSEBS, | en |
dc.relation.page | 86 | |
dc.rights.note | 同意授權(全球公開) | |
dc.date.accepted | 2011-08-18 | |
dc.contributor.author-college | 工學院 | zh_TW |
dc.contributor.author-dept | 材料科學與工程學研究所 | zh_TW |
顯示於系所單位: | 材料科學與工程學系 |
文件中的檔案:
檔案 | 大小 | 格式 | |
---|---|---|---|
ntu-100-1.pdf | 5.85 MB | Adobe PDF | 檢視/開啟 |
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