博碩士論文 107328013 詳細資訊




以作者查詢圖書館館藏 以作者查詢臺灣博碩士 以作者查詢全國書目 勘誤回報 、線上人數:48 、訪客IP:18.226.164.199
姓名 郎家君(Chia-Chun Lang)  查詢紙本館藏   畢業系所 能源工程研究所
論文名稱 以全雷射製程技術製備高質量比功率密度和高耐久性之鉑殼合金觸媒層應用於低溫燃料電池陰極端
(Fabrication of Pt-skin nanoporous alloy thin film as high mass-specific power density and high durability catalyst for polymer-electrolyte-membrane fuel cells by laser-based techniques)
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檔案 [Endnote RIS 格式]    [Bibtex 格式]    [相關文章]   [文章引用]   [完整記錄]   [館藏目錄]   至系統瀏覽論文 (2028-9-1以後開放)
摘要(中) 本研究使用脈衝雷射沉積法(Pulsed Laser Deposition, PLD)製備Pt/Co (25/75 at %, PtCo3)奈米顆粒並應用於燃料電池陰極端之觸媒層。PtCo3於總擔量100 μg/cm2時,其質量比功率密度(Mass Specific Power Density, MSPD)在0.6 V下僅有3.5 kW/gPt,是因為大約減量了50%的白金擔載量。
而後結合了連續雷射退火(Continuous Wave Laser Processing, CWLP) 以有效提升Pt使用率及耐久性。本研究經過CWLP於2.4 W 0.35 mm/s條件下,可以有效增加奈米顆粒觸媒層的Pt反應表面積進而提升電池之性能,其MSPD於0.6 V下可以達到8.79 kW/gPt,比起沒有結合CWLP之電池整整提升了2.5倍之多;合金觸媒可以在降低Pt擔載量的同時,仍然保有優良的觸媒活性,推論是因為由PLD建立的觸媒微結構比起傳統的塗佈製程更能夠建立有效的三相點,再加上CWLP可以使觸媒表面重新排列形成Pt殼層,提高觸媒利用率進而得到高MSPD。
有結合CWLP之觸媒在經過5000圈加速老化循環測試後仍保有50%以上的化學活性表面積,此結果顯示使用CWLP進行熱處理可以於奈米觸媒製造出具有Pt殼層的PtCo3合金觸媒,同時也會有燒結作用,增強顆粒間之鍵結,以提升觸媒耐久性,具良好的化學穩定性。
結合PLD及CWLP製程所製備之PtCo3奈米顆粒觸媒層,可有效降低燃料電池中Pt擔載量並保有優良的觸媒活性,提高觸媒使用率。進而提升燃料電池性及耐久性並降低燃料電池成本,使燃料電池更加普及進而永續環境。
摘要(英) The catalyst layers for polymer-electrolyte-membrane fuel cells (PEMFC) are fabricated by deposition of platinum directly onto the gas diffusion layer using pulsed laser deposition (PLD). This technique reduces the number of steps required to synthesize the catalyst layer and the required Pt loading for PEMFC. In this study, PLD is used to reduce the Pt loading and the cost of the cell. A thin film of PtCo3 nanoparticles was deposited on gas diffusion layer by PLD process and further subjecting the film to scanning continuous-wave laser processing (CWLP). In CWLP, the Pt skin forms over the surface of PtCo3 nanoparticles via Pt segregation with enhanced firm contact between nanoparticles. Thereby increasing electrochemical surface area with concomitant sintering effecting. The Pt skin formation could retain the stability and performance of catalyst with decrease in Pt loading. Application of such catalyst to the cathode of a PEMFC exhibits a 2.5-fold increase in mass-specific power density (MSPD) with respect to that without laser processing, raising the cathode MSPD to 8.79 kW gPt−1 with 1 atm oxygen and 12.02 kW gPt−1 with 1.5 atm oxygen. Further increase in Pt-mass-specific power density might be achieved by reducing the Pt content in the starting Pt alloy and changing the ambient gas pressure in pulsed laser deposition to optimize the initial particle size.
關鍵字(中) ★ 脈衝雷射沉積法
★ 連續雷射處理
★ 質子交換膜燃料電池
★ 合金觸媒
關鍵字(英) ★ Pulsed laser deposition
★ scanning continuous-wave laser processing
★ PEM fuel cell
★ cathode
★ alloy catalysts
論文目次 摘要 i
Abstract ii
致謝 iii
目錄 v
表目錄 ix
圖目錄 x
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基本構造 4
1-2-2 質子交換膜燃料電池運作原理 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 26
2-1 質子交換膜燃料電池 26
2-2 金屬多孔材之研究與應用 27
2-3 電化學交流阻抗分析 28
2-4 PEMFC合金觸媒研究發展 30
2-4-1 Pt觸媒表面形貌及顆粒大小研究探討 30
2-4-2 PtxMy觸媒研究探討 31
2-4-3 Core-Shell結構研究探討 34
2-5 應用脈衝雷射沉積於燃料電池 36
第三章 實驗方法與設備 39
3-1 實驗流程 39
3-2 實驗所需之材料 40
3-3 脈衝雷射沉積系統 41
3-3-1 脈衝雷射系統架設 41
3-3-2 奈米合金觸媒樣品製備參數 43
3-4 連續雷射退火 44
3-4-1 連續雷射退火系統架設 44
3-4-2 雷射升溫曲線檢測 45
3-4-3 鉑殼奈米合金觸媒樣品製備參數 46
3-5 膜電極組製備方式 46
3-5-1 膜電極組之組裝 46
3-5-2 熱壓方式 47
3-6 觸媒檢測方式 48
3-6-1 掃描式電子顯微鏡 48
3-6-2 能量色散X射線譜 49
3-6-3 穿透式電子顯微鏡 49
3-6-4 X光光電子能譜儀(XPS) 50
3-6-5 循環伏安法 52
3-6-6 加速老化測試 55
3-7 燃料電池測試 56
3-7-1 測試系統介紹 56
3-7-2 單電池測試系統之操作程序 57
3-7-3 J-V曲線量測 58
3-7-4 電子阻抗頻譜測試 59
第四章 實驗結果與討論 62
4-1 應用PLD技術製備PtCo3奈米觸媒於PEMFC陰極端 62
4-1-1 不同奈米觸媒於相同擔載量之電化學性能比較 62
4-1-2 不同奈米觸媒於相同擔載量之燃料電池性能比較 63
4-1-3 不同奈米觸媒於相同擔載量之EIS分析 64
4-1-4 不同奈米觸媒於相同擔載量之加速老化測試比較 65
4-1-5 不同奈米觸媒表面形貌與結構元素分析 66
4-2 應用CWLP於PtCo3奈米觸媒於PEMFC陰極端 69
4-2-1 CWLP雷射光斑診斷與樣品上之加熱曲線 69
4-2-2 CWLP之不同雷射能量與掃速對PtCo3奈米觸媒相同擔載量之電化學性能比較 74
4-2-3 相同擔載量之PtCo3奈米觸媒電池之性能比較 77
4-2-4 PtCo3奈米觸媒電池之EIS分析 80
4-2-5 PtCo3奈米觸媒之加速老化測試 83
4-2-6 CWLP對PtCo3奈米觸媒表面形貌結構之差異 86
4-3 應用雷射技術製備不同擔載量之不同觸媒比較 95
4-3-1 不同觸媒於不同擔載量下之PEMFC性能比較 96
4-3-2 不同觸媒燃料電池背壓測試 97
第五章 結論 98
第六章 未來展望 99
參考文獻 100
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指導教授 曾重仁 審核日期 2020-8-19
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