使用Ni1-xCox-BCZY陽極提升以甲烷為燃料之質子傳導型固態氧化物燃料電池耐碳性

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林家銘(Chia-Ming Lin) 查詢紙本館藏

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機械工程學系

論文名稱

使用Ni1-xCox-BCZY陽極提升以甲烷為燃料之質子傳導型固態氧化物燃料電池耐碳性
(Carbon tolerant Ni1-xCox-BCZY anode for methane-fed proton conducting solid oxide fuel cell)

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至系統瀏覽論文 (2026-9-1以後開放)

摘要(中)

本研究使用合金觸媒Ni1-xCox (x = 0.1, 0.2, 0.3)取代傳統鎳金屬觸媒作為固態氧化物燃料電池陽極之觸媒材料，達到改善陽極材料在長時間操作時，因使用碳氫燃料所造成陽極之積碳問題。透過固態反應法(Solid State Reaction, SSR)製備Ni1-xCox-BCZY作為質子傳導型固態氧化物燃料電池(P-SOFC)之合金陽極，並使用刮刀法及旋塗法製作陽極支撐型電池，並分別通以氫氣和甲烷進行電池性能及穩定性測試。目標以少許鈷元素(Cobalt, Co)與鎳元素(Nickel, Ni)進行置換，使Ni1-xCox電池達到比傳統以Ni金屬為主之電池更加優異的穩定性。
實驗結果顯示，四種參雜比例中，Ni0.9Co0.1電池具有較佳之電池性能，在800 ºC下以氫氣為燃料時，最大功率密度質為390 mW/cm2，其歐姆阻抗與極化阻抗為1.714 Ω·cm2及0.017Ω·cm2，而以傳統鎳金屬為觸媒之電池性能為361 mW/cm2，其歐姆阻抗與極化阻抗為1.734Ω·cm2及0.021Ω·cm2；以甲烷為燃料時，Ni0.9Co0.1電池之最大功率密度質為169.1 mW/cm2，其歐姆阻抗與極化阻抗為1.932 Ω·cm2及0.417 Ω·cm2，而Ni電池之性能為162.2 mW/cm2，其歐姆阻抗與極化阻抗為1.954 Ω·cm2及0.431Ω·cm2，而在甲烷下之穩定性測試中Ni0.9Co0.1電池之壽命為19.5小時，比Ni電池5.5小時之電池壽命多3倍以上。

摘要(英)

The rise in global warming and the Paris agreement on the control of temperature rise has increased the significance of green and carbon-neutral research for energy generation. Proton conducting solid oxide fuel cells (P-SOFC) are used for the conversion of hydrocarbon into electrical energy with carbon capture. Carbon form hydrocarbon fuels partially deposit on the Ni-BCZY anode of P-SOFC and further degrades the functioning of P-SOFC. In this thesis, Ni-BCZY anode is doped with Co for carbon deposition resistance and similar cell performance in P-SOFC operation. Ni1-xCox-BCZY (x = 0.1, 0.2, 0.3) anode material is prepared by easily scalable solid-state reaction process. The tape-casting process is used for developing an anode layer in P-SOFC cell integration. Further, electrochemical experiments were performed with CH4 as fuel for integrated P-SOFC to analyze the carbon resistance property of Ni1-xCox-BCZY anode. Also, the performance of integrated P-SOFC with H2 as fuel is also analyzed.
The experimental results show that P-SOFC with Ni0.9Co0.1-BCZY anode exhibits a maximum power density of 390 mW/cm2 with pure H2 at 800 ᵒC, ohmic and polarization resistance is 1.714 Ω·cm2 and 0.017 Ω·cm2. Higher performance of 29 mW/cm2 compared to traditional Ni-BCZY anode P-SOFC is observed for Ni0.9Co0.1-BCZY anode. Ohmic and polarization resistance of Ni-BCZY anode is 1.734 Ω·cm2 and 0.021 Ω·cm2. The lower ohmic and polarization resistance of Ni0.9Co0.1-BCZY anode compared to traditional Ni anode indicate that the catalytic activity of Ni anode can be improved with cobalt doping. The higher performance of Ni0.9Co0.1-BCZY anode could be due to efficient conversion of gas to power and easy electron transfer.
The Ni0.9Co0.1-BCZY anode P-SOFC with CH4 fuel exhibits a maximum power density of 169.1 mW/cm2 at 800 ᵒC. P-SOFC with Ni-BCZY anode generates a maximum power density of 162.2 mW/cm2 at 800 ᵒC. The ohmic and polarization resistance of Ni0.9Co0.1-BCZY anode P-SOFC is 1.932 Ω·cm2 and 0.417 Ω·cm2. Whereas for Ni-BCZY anode P-SOFC, ohmic and polarization resistance is 1.954 Ω·cm2 and 0.431 Ω·cm2. The lower resistance and higher performance of Ni0.9Co0.1-BCZY anode compared to Ni-BCZY attributes to the low carbon deposition and immediate conversion of CH4 to power. P-SOFC with Ni0.9Co0.1-BCZY anode exhibits nearly 3.5 times longer life time compared to Ni-BCZY anode with CH4 as fuel.
A NiCo-BCZY anode for lower carbon deposition and higher performance of P-SOFC with pure H2 and CH4 is developed in this work. This work helps for generating both clean and carbon capture energy generation.

關鍵字(中)

★ 質子傳導固態氧化物燃料電池
★ 甲烷
★ 穩定性
★ 鎳鈷合金陽極

關鍵字(英)

★ proton conducting solid oxide fuel cell
★ methane
★ stability
★ nickel cobalt anode

論文目次

中文摘要 I
Abstract II
目錄 IV
圖目錄 VI
表目錄 IX
一、緒論 1
1-1 前言 1
1-2 燃料電池(Fuel cell, FC) 2
1-3 固態氧化物燃料電池(SOFC) 3
1-2-1 P-SOFC及O-SOFC 4
1-2-1 P-SOFC原理 5
1-3 P-SOFC材料之特性 6
1-3-1 P-SOFC電解質 7
1-3-2 P-SOFC陽極材料 11
1-3-3 P-SOFC陰極材料 14
1-4 研究目的 15
二、文獻回顧 16
2-1 碳沉積對SOFC之影響 16
2-2 改變合金比例對於陽極材料性質的影響 19
三、實驗方法 22
3-1 實驗製程設備 22
3-1-1 實驗藥品 22
3-1-2 製程設備 23
3-2 實驗流程 24
3-2-1 陽極與電解質粉末製備流程 24
3-2-2 陽極基板製備流程 25
3-2-3 單電池製備流程 25
3-3 材料分析儀器 26
3-3-1 X光繞射儀(X-Ray Diffraction, XRD) 26
3-3-2 掃描式電子顯微鏡(Scanning Electron Microscope, SEM) 27
3-3-3 燃料電池測試系統 28
3-3-4 恆電位儀 30
四、結果與討論 32
4-1 鎳鈷合金陽極材料分析 32
4-2 鎳鈷電池性能分析 37
4-2-1 氫氣下之鎳鈷電池性能分析 37
4-2-2 甲烷下之鎳鈷電池性能分析 49
4-3 鎳鈷電池穩定性 63
五、結論 68
參考文獻 69

參考文獻

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指導教授

曾重仁(Chung-jen Tseng)

審核日期

2021-8-18

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