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姓名	陳晧軒(Hao-Hsuan Chen)  查詢紙本館藏	畢業系所	能源工程研究所
論文名稱	以滴塗製程控制Nafion自組織成膜並提升質子傳導與燃料電池功率密度 (Control of self-organization of dropcasted Nafion film for improving proton conduction in PEMFC to raise output power density)
相關論文	★ 定開孔率下流道設計與疏水流場對質子交換膜燃料電池之性能影響 ★ 熱風循環烘箱熱傳特性研究 ★ 以陽極處理製備奈米結構之氧化鐵光觸媒薄膜應用在光電化學產氫 ★ 規則多孔碳應用在燃料電池陰極觸媒擔體之研究 ★ 鉑錫/多孔碳觸媒應用於燃料電池陰極反應之研究 ★ 腐蝕特性對金屬多孔材質子交換膜燃料電池性能影響之研究 ★ 碎形理論應用在質子交換膜燃料電池中氣體擴散層熱傳導係數之研究 ★ 中溫固態氧化物燃料電池複合系統分析 ★ 中文質子傳輸型固態氧化物燃料電池陽極之研究 ★ 鋯摻雜鋇鈰釔氧化物微結構與電化學特性之研究 ★ 發展應用脈衝雷射沉積製備奈米顆粒堆疊多孔觸媒層與滴塗聚苯並咪唑介面層製作高溫型質子交換膜燃料電池 ★ 直接甲醇燃料電池氣體擴散層之研究 ★ 不同流道設計之透明質子交換膜燃料電池陰極水生成現象探討 ★ 鋰離子電池陰極材料LiCoO2粉體尺寸與形貌對電池性能的影響 ★ 多孔性碳材應用於質子交換膜燃料電池觸媒層之研究 ★ 多孔材應用於質子交換膜燃料電池散熱之研究
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摘要(中)	本研究使用脈衝雷射沉積法(Pulsed Laser Deposition, PLD)製備Pt 奈米顆粒並應用於燃料電池陰陽極端之觸媒層，並結合滴塗Nafion薄膜(Dropcasted Nafion film)將質子交換膜直接滴塗於觸媒層上，優化觸媒層與質子交換膜的介面，增加質子傳輸之通道，提升觸媒利用率。 因滴塗Nafion薄膜製程其Nafion直接進入觸媒層，重新調整其各項參數從滴塗溶液之組成比例、成膜之乾化溫度、組成MEA之熱壓參數，陰陽極觸媒量及膜厚最薄之極限，將之組成燃料電池量測性能及電化學阻抗並透過電化學診斷，去探討及優化滴塗Nafion薄膜整套製程。 透過控制乾化過程之溫度，使乾化溫度85°C之滴塗Nafion薄膜相較商用膜其歐姆阻抗下降35%，雖然因使用滴塗製程使Nafion深入觸媒層孔隙會減少氣體傳輸通道，當擔載量為100 μg/cm2其性能相較商用膜低15%，但當擔載量提升至200 μg/cm2時其優點發揮出來，能利用到整體之觸媒電流密度相對擔載量100 μg/cm2時提升近40%之性能，相較商用膜擔載量提升至200 μg/cm2時只提升7%之電流密度。提升擔載量時便提升觸媒層厚度，同時使用商用膜時其質子傳輸受限於質子擴散距離，因增加之觸媒無法有良好質子傳輸，整體觸媒利用率下降，電流密度趨近飽和，而滴塗Nafion薄膜則滲透整層觸媒層使觸媒皆有良好質子傳輸能力於兩大氣壓下性能達到1994.9 mA/cm2。
摘要(英)	In recent days, efficient green power generation has gained significant attention to control the rise in global warming. Hydrogen energy is considered as the source of energy storage and generation. The proton exchange membrane fuel cell (PEMFC) with higher efficiency is developed with increase in amount of noble metal catalyst, i.e., increasing the thickness of catalyst layer. But, the presence of higher amount of nano porous catalyst layer may not provide efficient transfer of generated protons from anode to cathode due lower contact of membrane with the catalyst. This may decrease the overall performance of PEMFC. This thesis is focused on developing high efficiency PEMFC with efficient proton transfer from anode to cathode with good contact of nafion and porous catalyst in the anode. In this study, Pt nanoparticles are coated on the carbon paper by pulsed laser deposition technique are used as the anode and cathode. Further, nafion is coated on the catalyst by drop casted on the catalyst layer. The drop casted nafion acts as the proton exchange membrane and also offers good contact to the catalyst for fast proton transfer. Processing parameters of the in-situ membrane development (nafion solution composition ratio, drop-casting, drying temperature of film) process, membrane electrode assembly and thickness of the nafion on the performance of PEMFC is well investigated with electrochemical analysis and diagnostics techniques. The amount of the catalyst layer and thickness are also considered in this study. The experimental results of in-situ membrane development shows that, annealing of nafion film at 85 ᵒC reduces the ohmic resistance by 35 % compared to the PEMFC assembled with commercial MEA as the drop casting of nafion reduces the gas transfer path. The performance of PEMFC with 100 µg/cm2 catalyst loading is 15 % lower than the commercial PEMFC. But, PEMFC with 200 µg/cm2 catalyst and in-situ membrane exhibits 40 % higher in performance compared to the commercial PEMFC. This higher performance is achieved with the good intact between the catalyst and nafion (proton exchange) membrane. In commercial MEA, the proton transfer is limited due to the higher thickness of catalyst and lower contact between the catalyst and the membrane. An increase in 7.3% of performance of commercial PEMFC is observed with rise of catalyst loading from 100 µg/cm2 to 200 µg/cm2. Whereas, the PEMFC with in-situ MEA exhibits 39.37% with rise of catalyst loading from 100 µg/cm2 to 200 µg/cm2. The efficient proton transfer between catalyst and nafion membrane could help in increasing the efficiency of PEMFC. The in-situ MEA (catalyst loading: 200 µg/cm2) PEMFC exhibits current density of 1454.2 mA/cm2. Further, the same cell exhibits current density of 1994.9 mA/cm2 with 2 atmospheric pressure at anode and cathode. An in-situ proton exchange (nafion) membrane development by simple process for high efficiency PEMFC is demonstrated in this thesis. Also, in-situ membrane development could reduce the cost of PEMFC with reduced cost of membrane. This work helps in designing MEA for high efficiency PEMFC for green power generation.
關鍵字(中)	★ 脈衝雷射沉積 ★ 滴塗質子交換膜 ★ 質子交換膜燃料電池	關鍵字(英)	★ pulsed laser deposition ★ proton exchange membrane fuel cell ★ drop casting ★ nafion
論文目次	摘要 i Abstract iv 致謝 vi 目錄 vii 表目錄 xi 圖目錄 xii 第一章 緒論 1 1-1 前言 1 1-2 燃料電池介紹 2 1-2-1 質子交換膜燃料電池運作原理 4 1-2-2 質子交換膜燃料電池基本構造 5 1-2-3 膜電極組基本構造及製備方式 7 1-3 觸媒層製程發展 9 1-3-1 製備觸媒層之方式 9 1-3-2 燃料電池觸媒層各製程之現況 19 1-3-3 PEMFC主要發展之瓶頸 21 1-4 本團隊已完成之工作 23 1-5 研究動機與目的 24 第二章 文獻回顧 25 2-1 質子交換膜燃料電池 25 2-2 質子交換膜之研究 26 2-3 金屬多孔材之研究與應用 26 2-4 電化學交流阻抗分析 28 2-5 PEMFC觸媒研究發展 29 2-5-1 Pt觸媒表面形貌及顆粒大小研究探討 29 2-6 應用脈衝雷射沉積於燃料電池 30 2-6-1 脈衝雷射沉積鉑於氣體擴散層 30 2-7 直接滴塗質子交換膜之燃料電池 32 第三章 實驗方法與設備 33 3-1 實驗流程 33 3-2 實驗所需之材料 34 3-3 脈衝雷射沉積系統(Pulsed Laser Deposition, PLD) 35 3-3-1 脈衝雷射系統架設 35 3-3-2 奈米合金觸媒樣品製備參數 37 3-4 滴塗 Nafion薄膜製備方式(Dropcasted Nafion film) 38 3-4-1 Dropcasted Nafion film之溶液製備 38 3-4-2 接觸角測試(Contect angle) 39 3-4-3 2-D CNC printer Dropcasted Nafion film 39 3-5 膜電極組製備與方式 41 3-5-1 商用膜之膜電極組製備及組裝 41 3-5-2 Dropcasted Nafion film之膜電極組製備及組裝 42 3-6 觸媒與Dropcasted Nafion film檢測方式 43 3-6-1 掃描式電子顯微鏡 43 3-6-1 穿透式電子顯微鏡 45 3-6-2 循環伏安法 (Cyclic Voltammetry, CV) 46 3-7 導電式原子力顯微鏡 51 3-8 離子切割研磨機含冷凍控溫及空氣阻斷系統(Ion Milling with Cooling control unit and Air Protection System) 52 3-9 燃料電池測試 53 3-9-1 測試系統介紹 53 3-9-2 單電池測試系統之操作程序 54 3-9-3 電子阻抗頻譜測試 57 第四章 實驗結果與討論 60 4-1 Dropcasted Nafion film之溶液組成分析 60 4-1-1 接觸角量測 60 4-1-2 Dropcasted Nafion film表面完整性分析 61 4-1-3 Dropcasted Nafion film之表面分布分析 63 4-1-4 Dropcasted Nafion film之膜厚分析 64 4-2 不同乾化溫度對薄膜之影響 64 4-2-1 不同乾化溫度薄膜之燃料電池性能比較 64 4-2-2 不同乾化溫度薄膜之燃料電池EIS分析 66 4-2-3 不同乾化溫度膜之C-AFM 68 4-3 熱壓參數對Dropcasted Nafion film膜之影響 69 4-3-1 Dropcasted Nafion film不同熱壓參數之性能比較 69 4-3-2 Dropcasted Nafion film不同熱壓參數之EIS分析 71 4-4 不同擔載量及不同操作壓力之燃料電池 72 4-4-1 相同操作壓力商用膜與滴塗質子交換膜之性能比較 72 4-4-2 相同操作壓力商用膜與滴塗質子交換膜之EIS分析 73 4-4-3 商用膜與滴塗Nafion薄膜之PEMFC性能比較 75 4-4-4 不同陽極端擔載量之燃料電池性能比較 79 4-5 Dropcasted Nafion film之結構分析及不同膜厚性能比較 80 4-5-1 商用膜與Dropcasted Nafion film MEA之結構分析 80 4-5-2 Dropcasted Nafion film不同膜厚之燃料電池性能比較 82 4-5-3 Dropcasted Nafion film不同膜厚之EIS分析 83 第五章 結論 84 第六章 未來展望 85 參考文獻 86
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指導教授	曾重仁(Chung-jen Tseng)	審核日期	2021-8-19
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