以鐵電材料搭配非熱電漿行CO2/CH4重組反應生成合成氣之研究

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鍾瑋杰(Wei-chieh Chung) 查詢紙本館藏

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論文名稱

以鐵電材料搭配非熱電漿行CO2/CH4重組反應生成合成氣之研究
(Dry Reforming of Methane with DBD and Ferroelectrics Packed-bed DBD Reactors)

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摘要(中)

全球暖化(Global Warming)為二十世紀後半以來全球關注的重要議題，降低溫室氣體(GHGs)之排放以減緩全球暖化已成全球關注的焦點。將CO2及CH4進行重組反應可同時減少兩種主要溫室氣體之排放，且主要產物為合成氣(Syngas)可做為燃料或經由費拖反應合成碳氫化合物，為具有潛力且值得發展之技術。本研究以介電質放電進行CO2/CH4重組，並以溶膠凝膠法製備具有鐵電性質之弛緩鐵電體(BaZr0.75Ti0.25O3 (BZT, εr = 149)或BaFe0.5Nb0.5O3 (BFN, εr = 2025))填入反應床輔助進行反應，結果顯示在CH4/CO2 =1、電壓為13.6 kV、頻率為20,000 Hz及總流率為40 mL/min之條件下，未添加鐵電材料、搭配BZT填充床及搭配BFN填充床的反應器所得之二氧化碳轉化率分別為51.0%、52.7%及57.0%，甲烷轉化率分別為64.6%、66.4%及72.0%，一氧化碳選擇性分別為54.0%、55.6%及59.2%，氫氣選擇性分別為59.1%、63.6%及65.5%。能量效率方面分別為3.19 mol/kWh、3.81 mol/kWh及3.83 mol/kWh，證明介電質放電和弛緩鐵電體之間存在協同效應。另一方面，在CH4/CO2 = 3、電壓為13.6 kV、頻率為20,000 Hz、總流率為40 mL/min之條件下且搭配BFN填充床進行重組時，能量效率達5.16 mol/kWh。

摘要(英)

Global warming has been a big concern since 20th century and how to reduce the emissions of greenhouse gases (GHGs) into atmosphere has become an important issue. Carbon dioxide reforming of methane to generate syngas has the advantages of converting two major GHGs simultaneously and producing syngas to be utilized as fuel or as feedstock of Fischer-Tropsch process. This study is motivated to reform CH4 with CO2 via dielectric barrier discharge (DBD), and catalyst packed bed composed by BaZr0.75Ti0.25O3 (BZT, εr = 149) or BaFe0.5Nb0.5O3 (BFN, εr = 2025) prepared by sol-gel method. The results show that with the conditions of CH4/CO2 ratio of 1, applied voltage of 13.6 kV, frequency of 20,000 Hz and flow rate of 40 mL/min, the CO2 conversions achieved with DBD alone, BZT packed bed and BFN packed bed are 43.4%, 52.7% and 57.0%, respectively, in the meantime, methane conversion efficiencies are 64.6%, 66.4% and 72.0%, respectively. The energy efficiency achieved with plasma alone is 3.66 mol/kWh, and it increases to 3.81 mol/kWh and 3.83 mol/kWh, respectively, as BZT and BFN are used as the catalyst. The results proved the combination of DBD and relaxor ferroelectric induces synergistic effect and enhances DRM. Moreover, with feeding CH4/CO2 ratio of 3, applied voltage of 13.6 kV, frequency of 20,000 Hz, flow rate of 40 mL/min and with BFN packed bed reactor, energy efficiency reaches 5.16 mol/kWh which is significantly higher than that achieved with plasma alone.

關鍵字(中)

★ CO2/CH4重組反應
★ 非熱電漿
★ 介電質放電
★ 鐵電材料
★ 合成氣

關鍵字(英)

★ Dry Reforming of Methane
★ Dielectric Barrier Discharge
★ Non-Thermal Plasma
★ Ferroelectric Catalyst
★ Syngas

論文目次

第一章前言 ....................................................................................................1
1.1 研究緣起 ............................................................................................1
1.2 研究目的 ............................................................................................5
第二章文獻回顧 ............................................................................................6
2.1 溫室氣體的來源及特性....................................................................6
2.2 二氧化碳的減量技術及再利用........................................................8
2.2.1 前處理技術 ....................................................................................8
2.2.2 後續處理技術 ................................................................................8
2.2.3 二氧化碳再利用 ............................................................................9
2.3 甲烷重組反應 ....................................................................................9
2.3.1 水氣甲烷重組反應 ........................................................................9
2.3.2 甲烷部分氧化反應 ......................................................................10
2.3.3 二氧化碳甲烷重組反應 ..............................................................10
2.4 費托反應 ..........................................................................................12
2.5 電漿 ..................................................................................................13
2.5.1 電漿反應 ......................................................................................15
2.5.2 非熱電漿 ......................................................................................16
2.6 鐵電材料 ..........................................................................................19
2.7 甲烷二氧化碳重組之反應機制及動力學......................................21
2.7.1 未添加觸媒之反應機制 ..............................................................21
2.7.2 以觸媒進行重組之反應機制 ......................................................21
2.7.3 以電漿進行重組之反應機制 ......................................................22
第三章研究設備與方法 ..............................................................................34
3.1 研究流程及架構 ..............................................................................34
3.2 實驗藥品、氣體及設備..................................................................35
3.2.1 實驗藥品 ......................................................................................35
3.2.2 實驗氣體 ......................................................................................36
3.2.3 實驗儀器設備 ..............................................................................36
3.3 觸媒材料製備 ..................................................................................37
3.4 觸媒材料之物化特性分析..............................................................38
3.4.1 X 光粉末繞射分析儀...................................................................39
3.4.2 高解析度比表面積分析儀 ..........................................................40
3.4.3 掃描式電子顯微鏡 ......................................................................40
3.4.4 傅立葉轉換紅外線光譜分析 ......................................................41
3.4.5 三相電表 ......................................................................................41
3.5 重組實驗 ..........................................................................................42
3.5.1 反應設備 ......................................................................................42
3.5.2 重組反應 ......................................................................................44
3.5.3 實驗結果之計算 ..........................................................................44
第四章結果與討論 ......................................................................................48
4.1 輸入電壓對重組反應之影響..........................................................48
4.2 總氣體流率對重組反應之影響......................................................52
4.3 進氣比對重組反應之影響..............................................................54
4.4 結合鐵電觸媒對重組反應之影響..................................................57
4.4.1 鐵電觸媒對放電功率之影響 ......................................................57
4.4.2 鐵電觸媒對轉化率之影響 ..........................................................59
4.4.3 鐵電觸媒對選擇性之影響 ..........................................................60
4.4.4 鐵電觸媒對元素平衡之影響 ......................................................61
4.4.5 鐵電觸媒對能量效率之影響 ......................................................62
4.5 鐵電觸媒之物化特性分析..............................................................63
4.5.1 XRD..............................................................................................63
4.5.2 FT-IR.............................................................................................63
4.5.3 BET...............................................................................................63
4.5.4 LCR...............................................................................................64
4.5.5 SEM ..............................................................................................64
4.6 鐵電觸媒之活性測試......................................................................65
4.7 碳氫化合物之生成..........................................................................65
第五章結論與建議 ......................................................................................98
5.1 結論 ..................................................................................................98
5.2 建議 ..................................................................................................99
參考文獻...........................................................................................................100

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指導教授

張木彬(Moo-bene Chang)

審核日期

2014-8-28

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