應用雷射材料製程技術於製備Pt3Co奈米結構陰極觸媒層以提升質子交換膜燃料電池性能

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敖昱弘(Yu-Hung Ao) 查詢紙本館藏

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論文名稱

應用雷射材料製程技術於製備Pt3Co奈米結構陰極觸媒層以提升質子交換膜燃料電池性能
(Production of Pt3Co nanoporous cathode catalyst by laser based material application methods for high performance PEMFC)

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摘要(中)

近年來人類對能源需求日益攀升，在使用化石燃料同時亦產生汙染物而破壞環境。為求潔淨能源以永續環境，燃料電池的發展刻不容緩。燃料電池使用貴重金屬鉑(Platimun, Pt)做為觸媒層，然而傳統塗佈製程因具有孤島效應導致Pt於觸媒層使用量高，因成本較高使燃料電池未能普及。本研究藉由脈衝雷射沉積法(Pulsed Laser Deposition, PLD) 製備 Pt3Co合金奈米顆粒觸媒層應用於燃料電池觸媒層。相較傳統製程於陰極端Pt使用量需400 μg/cm2，PLD能製作更均勻分散的奈米顆粒觸媒層，僅使用Pt3Co 100 μg/cm2，Pt含量90.8 μg/cm2，應用於陰極端並結合化學去合金(Dealloy)製程及連續雷射處理(Continous Wave Laser Processing, CWLP)以有效提升Pt使用率及耐久性。本研究經2小時最佳化Dealloy製程，增加奈米顆粒觸媒層的Pt有效裸露表面積以提升電池性能，電池性能於0.6 V下電流密度約為998.65 mA/cm2。
而後使用CWLP進行雷射處理將奈米顆粒觸媒間進行燒結，且於單一奈米顆粒觸媒製造出具有Pt殼層的Pt3Co合金觸媒以提升觸媒耐久性。藉由CWLP進行雷射退火使觸媒產生致密Pt殼層提升觸媒耐久性。在CWLP 0.3 W下，於0.6 V電流密度為1164 mA/cm2，與PLD製備之Pt樣品及400 μg/cm2之商用觸媒電池性能幾乎一致，於陰極端的MSPD上升至6.96 kW/g。且在經過5000圈加速老化循環測試後仍保有56%的化學活性表面積，此結果顯示CWLP使奈米顆粒觸媒之間燒結並使單一顆粒產生緻密Pt殼層而能有效提升觸媒耐久性，具良好的化學穩定性。
結合PLD、Dealloy及CWLP製程製備之Pt3Co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)

In recent years, human demand for energy has risen steadily, and the use of fossil fuels has also produced pollutants and destroyed the environment. In order to get clean energy to protect environment. Developing fuel cell is of great urgency. In this study, the catalyst layers for polymer-electrolyte-membrane (PEM) fuel cells are fabricated by deposition of Pt3Co directly onto the gas diffusion layer (GDL) using pulsed laser deposition (PLD) to decrease the amount of Pt loading in PEMFC. Comparing with traditional production, using PLD can get more uniform catalyst layer to improve Mass Specific Power Density (MSPD).
The Current density at 0.6 V is 998.65 mA/cm2 in cathode side, using Pt3Co 100 μg/cm2 (Pt: 90.8 μg/cm2) with 2 hrs of dealloying process, the properties of electrochemistry and I-V performance are measured. We produce Pt-Shell/Pt3Co core Structure to promote Pt reactive surface area.The maximum current density at 0.6 V is 998 mA/cm2 were obtained for the sample with 2 hr dealloying time. This technique reduces the number of steps required to synthesize the catalyst layers and the amount of required Pt loading.
After dealloying, we use Continuous Wave Laser Processing (CWLP) to get compact Pt-shell to improve durability of Pt3Co catalyst. In 0.3 W CWLP, the current density at 0.6 V is 1164 mA/cm2. Besides, we also do Accelerate Degradation Test(ADT) to test durability. After 5000 cycles ADT, the Pt3Co catalyst still retain 56% MSECSA. The result reveals the CWLP production can improve the durability of catalyst and MSPD in cathode side up to 6.96 kW/g.
Using PLD and CWLP production can get compact Pt-Shell with Pt3Co-Core to improve PEMFC MSPD and durability.

關鍵字(中)

★ 脈衝雷射沉積法
★ 質子交換膜燃料電池
★ 陰極
★ 合金觸媒

關鍵字(英)

★ Pulsed laser deposition
★ PEM fuel cell
★ Cathode
★ Alloy catalysts

論文目次

摘要 I
Abstract III
目錄 III
圖目錄 IV
表目錄 VII
第一章緒論 1
1-1 前言 1
1-2 PEMFC發展 2
1-2-1 PEMFC基本構造與原理 2
1-2-2 MEA構造 5
1-3 觸媒層製程發展現況 6
1-3-1 觸媒層製程方式 6
1-3-2各製程方法之現況 16
1-3-3 PEMFC主要發展瓶頸 18
1-4 PEMFC合金觸媒研究發展 20
1-4-1 Pt觸媒表面形貌及顆粒大小研究探討 20
1-4-2 PtxMy觸媒研究探討 21
1-4-3 Core-Shell結構研究探討 24
1-5本團隊已完成之工作 25
1-6研究目的 26
第二章實驗方法與實驗設備 27
2-1實驗架構與流程 27
2-2脈衝雷射沉積系統 28
2-2-1雷射系統光路 28
2-2-2雷射系統元件 29
2-2-3 PLD觸媒樣品製作 30
2-3 Dealloy製程 31
2-4使用連續波雷射退火系統強化觸媒化學耐久性 31
2-4-1 雷射系統元件樣品座 32
2-5 MEA製作方式 32
2-5-1觸媒漿料調配與塗佈 33
2-5-2 MEA熱壓方式 33
2-6 觸媒檢測方式 34
2-6-1 物理微結構之觀測 34
2-6-2 電化學性能測定 39
2-7燃料電池系統分析 44
2-7-1 I-V曲線量測 47
2-7-2電子阻抗頻譜測試 48
第三章實驗結果與討論 51
3-1 應用PLD製備Pt3Co奈米顆粒觸媒於PEMFC陰極端 51
3-1-1 Pt與Pt3Co觸媒於相同總擔載量之燃料電池性能比較 51
3-1-2 電池陰極端使用不同觸媒材料之EIS分析 52
3-1-3 Pt與Pt3Co觸媒電化學性能比較 53
3-1-4 Pt與Pt3Co觸媒表面形貌結構及觸媒顆粒影響 53
3-2 Dealloy製程應用於Pt3Co奈米顆粒觸媒層於PEMFC陰極端…...55
3-2-1不同Dealloy製程時間對相同Pt3Co奈米觸媒擔載量之燃料電池性能比較 55
3-2-2不同Dealloy製程時間對相同Pt3Co奈米觸媒擔載量之EIS分析 56
3-2-3 不同Dealloy製程時間對相同Pt3Co奈米觸媒擔載量之電化學性能比較 58
3-2-4 不同Dealloy製程時間對相同Pt3Co奈米觸媒擔載量之表面形貌結構及觸媒顆粒影響 60
3-3 結合CWLP強化最佳Dealloy製程時間之Pt3Co奈米顆粒觸媒耐久性……………………………………………...…………………………..61
3-3-1 不同CWLP能量對相同Dealloy製程時間之燃料電池性能比較………………………………………………………………………..…...61
3-3-2 不同CWLP能量對相同Dealloy製程時間之Pt3Co奈米觸媒擔載量之燃料電池EIS分析 62
3-3-3 不同CWLP能量對相同Dealloy製程時間之Pt3Co奈米顆粒觸媒之電化學性能比較 64
3-3-4 不同CWLP能量對相同Dealloy製程時間之Pt3Co奈米顆粒觸媒之表面形貌結構及觸媒顆粒影響 65
3-3-5 CWLP製程對Pt3Co奈米顆粒觸媒層影響 66
3-3-6 不同CWLP能量之Pt3Co奈米觸媒耐久性測試 68
3-3-7不同製程對Pt3Co奈米顆粒觸媒層之影響 70
第四章結論 72
第五章未來展望 73
第六章參考文獻 74

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指導教授

曾重仁(Chung-Jen Tseng)

審核日期

2018-8-20

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