加濕效應對加壓型甲烷固態氧化物燃料電池碳沉積影響

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王稚元(Chih-Yuan Wang) 查詢紙本館藏

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加濕效應對加壓型甲烷固態氧化物燃料電池碳沉積影響
(Effect of Humidification on Carbon Deposition of A Pressurized Solid Oxide Fuel Cell)

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摘要(中)

本論文量測加濕效應與壓力效應對甲烷固態氧化物燃料電池(Solid Oxide Fuel Cell, SOFC)電化學性能、碳沉積與電池穩定性之影響。採用實驗室已建立之加壓型SOFC測試平台，使用鈕扣型陽極支撐電池(Ni-YSZ/ YSZ/ LSC-GDC)，於操作壓力p = 1 atm 與3 atm和操作溫度750°C，進行四種不同濕度比例之甲烷作為陽極燃料，以steam to carbon ratio (S/C)定義，分別為(1) S/C = 0 (50 sccm CH4 + 150 sccm N2)、(2) S/C = 0.25 (50 sccm CH4 + 12.5 sccm H2O + 137.5 sccm N2) 、 (3) S/C = 0.5 (50 sccm CH4 + 25 sccm H2O + 125 sccm N2) 以及(4) S/C = 1 (50 sccm CH4 + 50 sccm H2O + 100 sccm N2)，陽極總體積流率為200 sccm；陰極則是通入200 sccm的空氣。實驗結果顯示：在p = 1 atm下，甲烷加濕效應可使SOFC功率密度提升14% ~ 26%，最大提升值發生在S/C = 0.25，這是因為甲烷蒸氣重組反應將CH4轉換成H2，得以有效地降低活化極化與濃度極化。再者，壓力效應與加濕效應結合明顯降低SOFC極化阻抗，例如加濕甲烷在p = 3 atm和S/C = 0.5條件下，其電池性能比起常壓和S/C = 0.5條件下之性能高出62%。在p = 3 atm和S/C = 0條件下，於 SEM與XRD影像觀測到有大量的碳沉積聚集於燃料進口處，這是因壓力效應加劇了甲烷與陽極鎳觸媒直接裂解的速率，提高S/C可藉由甲烷蒸氣重組，與水煤氣轉換反應抑制於燃料進口處之碳沉積，達到延長電池壽命的目的。綜合以上結果，顯示加壓型甲烷SOFC配合適度加濕，未來可與直接燃燒甲烷(天然氣主要成份)之微氣渦輪機結合，發展分散式高效率複合式發電系統。

摘要(英)

This study meassures the effect of humidification on carbon deposition for a pressurized methane-fueled solid oxide fuel cell (SOFC) using anode-supported button full cell (ASC: NiO-YSZ/ YSZ/ LSC-GDC). Experiments are conducted in high-pressure SOFC testing platform. The experimental conditions are two operating pressures p = 1 atm and p = 3 atm at T = 750 °C. The anode fuel is supplied by methane with four different steam to carbon ratio (S/C): (1) S/C = 0 (50 CH4 + 150 N2), (2) S/C = 0.25 (50 CH4 + 12.5 H2O + 137.5 N2), (3) S/C =0.5 (50 CH4 + 25 H2O + 125 N2), (4) S/C =1 (50 CH4 + 50 H2O + 100 N2) at a total flow rate of 200 ml min-1, and the cathode is supplied by air at a total flow rate of 200 ml min-1 for all four cases . Results show that steam-methane reforming can improve power density and reduce both activation and concentration polarization noticeably. Moreover, the maximum power density is formed to be at S/C = 0.5 with p = 3 atm, which significantly increase of 62% as compared with that at p = 1 atm and S/C = 0.5. The scanning electron microscope (SEM) and X-ray diffraction (XRD) images show great amount of carbon deposition at S/C = 0 with p = 3 atm. The carbon deposition can be suppressed by increasing S/C under steam-methane reforming and water-gas shift reaction, which is turn extends the cell durability. This suggests that the pressurized methane-fueled SOFC is feasible for the future development of the hybrid power system integrating with micro gas turbines.

關鍵字(中)

★ 加壓型甲烷固態氧化物燃料電池
★ 甲烷蒸氣重組
★ 水煤氣轉換
★ 穩定性測試
★ 碳沉積

關鍵字(英)

★ Pressurized Methane-fueled Solid Oxide Fuel Cell
★ Methane Steam Reforming
★ Water-gas Shift Reaction
★ Stability Test
★ Carbon Deposition

論文目次

目錄
摘要 i.
Abstract ..... iii
致謝.... ivii
目錄..... vii
圖表目錄.. viii
符號說明x
第一章前言 1
1.1 研究動機 ..1
1.2 問題所在 ..3
1.3 解決方法 ..4
1.4 論文綱要 ..5
第二章文獻回顧 ....7
2.1 SOFC介紹與運作原理 ..7
2.1.1 陽極、電解質與陰極 .7
2.1.2 SOFC運作機制 ...10
2.2 SOFC之極化現象 ..15
2.2.1 活化極化 15
2.2.2 歐姆極化 16
2.2.3 濃度極化 17
2.3 甲烷SOFC性能、阻抗與電池耐久性相關文獻 ..18
2.3.1 甲烷SOFC耐久性測試與碳沉積現象相關研究 .....19
2.3.2 甲烷SOFC中添加H2O之相關研究 .....25
2.4 SOFC壓力效應 .27
2.4.1壓力效應對於SOFC性能與電化學反應機制之影響 .27
2.4.2 壓力效應對於甲烷SOFC影響 ..29
第三章實驗設備與量測方法 35
3.1 高壓SOFC實驗量測平台 .35
3.2 實驗流程與量測操作參數設定 .....38
3.3 實驗流程與量測操作參數設定 .....41
3.3.1 SOFC標準作業流程 ....41
3.3.2 甲烷SOFC 實驗量測流程 ..42
第四章結果與討論 ....46
4.1 一大氣壓甲烷SOFC加濕效應與氫氣SOFC性能與OCV 比較 .....46
4.1.1 甲烷 SOFC加濕效應OCV量測 .....46
4.1.2 甲烷SOFC加濕效應I-V極化曲線量測 .....47
4.2 一大氣壓甲烷SOFC加濕效應與氫氣SOFC電化學阻抗頻譜比較 .....51
4.2.1 一大氣壓甲烷SOFC之加濕效應對於歐姆、活化極化的影響 .....51
4.2.2 一大氣壓甲烷SOFC之加濕效應對於濃度極化的影響 .....51
4.3 壓力效應對於加濕甲烷SOFC性能影響 .53
4.4 壓力效應對於加濕甲烷SOFC電化學阻抗頻譜比較 .....56
4.5 壓力效應對於加濕甲烷SOFC碳沉積現象與電池壽命 60
4.5.1 一大氣壓甲烷 SOFC之加濕效應對於電池壽命的影響 60
4.5.2 一大氣壓甲烷 SOFC之加濕效應耐久性測試 SEM影像與 XRD圖譜 61
4.5.3 壓力效應對於加濕甲烷 SOFC電池壽命之影響 62
4.5.4 壓力效應對於加濕甲烷 SOFC耐久性測試 SEM影像與 XRD圖譜 63
第五章結論與未來工作 ..71
參考文獻....74
圖表目錄
圖2.1 SOFC 陽極觸媒Ni/YSZ 剖面圖之Triple Phase Boundaries反應位置[27]。 .....9
圖2.2 ZrO2添加Y2O3產生電荷補償效應，形成氧空洞[7]。 .10
圖2.3 SOFC陽極使用氫氣之基本運作機制[7]。 ...13
圖2.4 SOFC 極化曲線圖及各電流密度區間所造成的電壓損失[7]。 .14
圖2.5 在不同操作溫度下使用CH4或CO經過4小時後，Ni-YSZ 顆粒表面上碳沉積的量[8]。 ....22
圖2.6 使用加濕3%甲烷在(a)初始陽極Ni-YSZ、(b) 500°C、(c) 600°C(表面)、(d) 600°C、(e) 700°C，與(f) 800°C經過4小時穩定性測試後之陽極中心SEM影像[44]。..23
圖2.7 在不同溫度、負載條件下使用加濕3%甲烷進行3-6小時的穩定性測試；(a) 650°C、(b) 700°C、(c) 750°C，與(d) 800°C [9]。 ..24
圖2.8 模擬平板型ASC(NiO-YSZ/YSZ /LSCF)溫度範圍在650°C~850°C工作壓力1 atm~10 atm甲烷蒸氣重組反應之甲烷與氫氣的濃度變化[17]。 ...30
圖2.9 壓力效應對於甲烷碳沉積之影響，於溫度750°C和負載0.8V下，不同壓力下的性能穩定性分析[22]。 .31
圖2.10 壓力效應對於甲烷碳沉積之影響，於溫度800°C和負載0.9V下，不同壓力下的性能穩定性分析[22]。 ...32
表2.1表一. 各團隊甲烷SOFC性能、阻抗與電池耐久性相關文獻 ...33
表2.2各團隊甲烷SOFC中添加H2O之相關研究 ..34
圖 3.1 高壓高溫雙腔體SOFC實驗量測平台。 .37
圖3.2 (a) SOFC陶瓷鈕扣型載具實際圖與平片剖視圖。 ..39
圖 3.2 (b) Elcogen ASC-400B實際照片(左)、電池材料厚度和尺寸示意圖(左下)和SEM拍攝圖(右)。 40
圖3.3 高壓甲烷SOFC實驗流程圖。 .....44
圖4.1 (a) 加濕效應之甲烷SOFC 與氫氣SOFC 極化曲線比較圖。 ...49
圖4.1 (b) 加濕效應對於性能與OCV 比較圖。 49
圖4.2 加濕效應之甲烷SOFC與氫氣SOFC電化學阻抗頻譜: Nyquist(下方), Bode(上方)比較圖。 ....52
圖4.3 (a)壓力效應之加濕甲烷SOFC 與氫氣SOFC 極化曲線比較圖 54
圖4.3 (b) 加濕甲烷SOFC 壓力與加濕效應對於與常壓性能比較圖 ..55
表4.1 壓力效應對於加濕甲烷SOFC 與氫氣SOFC 對電池功率密度增益。 55
圖 4.4 (a) 壓力效應之加濕甲烷SOFC 與氫氣SOFC 電化學阻抗頻譜: Nyquist(下方), Bode(上方)比較圖。 ..58
圖 4.4 (a) 壓力效應之加濕甲烷SOFC 與氫氣SOFC 電化學阻抗頻譜: 依照不同頻率所造成之相位角偏差Theta (θ)與Zreal 間所繪製之Bode 比較圖；θ 為電壓所對應初始相位角φ 與電流響應初始相位角ψ 之差(θ= φ - ψ)。 .....59
表4.2壓力效應對於加濕甲烷SOFC與氫氣SOFC對電池總極化阻抗之增益。 .....60
圖4.5 在750°C、1 atm 的實驗條件，以800 mA/cm2 定電流密度量測陽極燃料為: S/C ratio = 0 (CH4/H2O/N2= 50/0/150 sccm 電池壽命13 hr)，與S/C ratio = 0.5 (CH4/H2O/N2= 50/25/125 sccm, 電池壽命48 hr) 電池耐久性測試結果。 .65
圖4.6 在為(a)通入H2 還原後之Ni-YSZ 陽極表面；(b)、(c)分別是在在750°C、1 atm，與800 mA/cm2 定電流密度條件下；為 S/C ratio = 0 (CH4/H2O/N2= 50/25/150 sccm)加濕甲烷在48 小時耐久性測試後，(b) 陽極側視剖面圖，(c) 陽極表面俯視圖。(d)、(e)則分別是S/C ratio = 0.5 (CH4/H2O/N2= 50/0/125 sccm)乾甲烷在13小時耐久性後，(d) 陽極側視剖面圖與(e) 陽極表面俯視圖。 ....66
圖4.7 SOFC 陽極表面XRD 圖譜其電池片樣本取自: (a) 通入H2 還原後之Ni-YSZ、(b) 在750°C、1 atm 的實驗條件，以800 mA/cm2 定電流密度量測陽極燃料為: S/C = 0 (CH4/ H2O/ N2= 50/ 0/ 150 sccm 電池壽命13 hr)，以及(c) S/C = 0.5 (CH4/ H2O/ N2= 50/ 25/ 125 sccm, 電池壽命48 hr)穩定性測試後的電池片。 ...67
圖4.8 在750°C、3 atm 的實驗條件，以800 mA/cm2 定電流密度量測陽極燃料為: S/C ratio = 0 (CH4/H2O/N2= 50/0/150 sccm 電池壽命2 hr)、S/C ratio = 0.5
(CH4/H2O/N2= 50/25/125 sccm, 電池壽命5 hr) ，與S/C ratio = 1 (CH4/H2O/N2= 50/50/100 sccm, 電池壽命9 hr)電池耐久性測試結果。 .....68
圖4.9 (a)為通入H2 還原後之Ni-YSZ 陽極表面；(b)、(c)分別是在在750°C、3 atm，與800 mA/cm2 定電流密度條件下；(b)、(c)分別是 S/C ratio = 0.5 (CH4/H2O/N2= 50/25/150 sccm)加濕甲烷在5 小時耐久性測試後，(b) 陽極表面中心處俯視圖、(c) 陽極表面邊緣處俯視圖。(d)、(e)則分別是S/C ratio = 0 (CH4/H2O/N2= 50/0/125 sccm)乾甲烷在2 小時耐久性後， (d) 陽極表面中心處俯視圖，以及(e) 陽極表面邊緣處俯視圖。..69
圖4.10 SOFC 陽極表面XRD 圖譜其電池片樣本取自: (a) 通入H2 還原後之Ni-YSZ、(b) 在750°C、3atm 的實驗條件，以800 mA/cm2 定電流密度量測陽極燃料為: S/C = 0 (CH4/ H2O/ N2= 50/ 0/ 150 sccm 電池壽命13 hr)，以及(c) S/C = 0.5 (CH4/ H2O/ N2= 50/ 25/ 125 sccm, 電池壽命48 hr)穩定性測試後的電池片。 ...70

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指導教授

施聖洋(Shenqyang Shih)

審核日期

2021-10-26

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