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Student Number 953206023
Author Yi-Wei Wu(吳義偉)
Author's Email Address iway.wu@msa.hinet.net
Statistics This thesis had been viewed 1498 times. Download 616 times.
Department Graduate Institute of Environmental Engineering
Year 2008
Semester 2
Degree Master
Type of Document Master's Thesis
Language zh-TW.Big5 Chinese
Title Plasma modification of the Ni/γ-Al2O3 catalyst with Dielectric Barrier Discharges
Date of Defense 2009-06-09
Page Count 121
Keyword
  • Ethanol
  • Ni/γ-Al2O3 Catalyst
  • Plasma
  • Steam reforming
  • Abstract The plasma modification of the catalyst is a novel way to improve performance of catalyst. Such prepared catalyst presents a higher catalytic activity and an enhanced stability over the catalyst prepared without plasma treatment. This study aims to evaluate the characteristics of Ni/Al2O3 catalyst for steam reforming of ethanol to syngas via a DBD by different flowing gases and with different processes. DBD reactor is made of the quartz tube with the inner diameter of 10.6 mm. A stainless steel rod with the diameter of 0.1 mm is used as the inner electrode and the length of discharge region is 100.0 mm. Experimental tests are conducted at fixed applied voltage (16 kV), frequency (100 Hz), applied energy of catalyst (10800 J/g), space velocity (1498 hr-1) and temperature (25 ℃), while the flowing gases include hydrogen and oxygen, the processes include discharge before and after calcination. Steam reforming experimental tests are conducted at fixed space velocity (10602 hr-1), ethanol-water mole ratio (1:3), while the temperature vary from 446 ℃ to 736 ℃.
    The catalyst prepared with discharge before calcination exhibits lower ethanol conversion rate and hydrogen selectivity, compared to the catalyst prepared without plasma treatment. At 446 ℃, ethanol conversion efficiency of traditional, O2 plasma and H2 plasma catalyst are 82.6%, 61.9% and 57.1%, H2 selectivities of each one are 42.9%, 22.8% and 0.0%, respectively. At 736 ℃, ethanol conversion efficiency of each catalyst reaches to above 99.0%, H2 selectivities of traditional, O2 plasma and H2 plasma catalyst are 85.7%, 71.6% and 83.0%, respectively. At another case, the catalyst prepared with discharge after calcination by H2 plasma shows improved ethanol conversion rate and hydrogen selectivity, compared to O2 plasma and tranditional catalyst. At 446 ℃, ethanol conversion efficiency of O2 plasma and H2 plasma catalyst are 56.9%, 39.2% and 60.4%, the H2 selectivities of each one are all 0.0%. At 736 ℃, the ethanol conversion efficiency of each catalyst reach above 99.0%, H2 selectivities of traditional, O2 plasma and H2 plasma catalyst are 51.7%, 39.9% and 72.5%, respectively. In order to reduce the effect of coke formation, the catalyst discharged after calcination conducts steam reforming process by temperature decrease way, at 446 ℃, ethanol conversion efficiency of traditional, O2 plasma and H2 plasma catalyst are 79.0%, 66.9% and 90.6%, H2 selectivities of each one are 42.8%, 64.5%, 37.4%, respectively. At 736 ℃, ethanol conversion efficiency of each catalyst are able to reach to above 99.0%, H2 selectivities of each one are 42.8%, 64.5%, 37.4%, respectively. 87.0%, 82.3%, 92.8%.
    The present investigation confirms the DBD treatment of Ni/γ-Al2O3 catalyst with hydrogen after calcination thermally, leads to better activity and selectivity for steam reforming of ethanol to syngas.
    Table of Content 一、前言1
    1-1研究緣起1
    1-2  研究目的2
    二、文獻回顧3
    2-1 氫氣的介紹3
    2-2 乙醇5
    2-2-1 乙醇之基本介紹5
    2-2-2 乙醇在燃料電池上的應用6
    2-3 碳氫化合物重組7
    2-3-1 水蒸氣重組法8
    2-3-2 部分氧化法9
    2-3-3 自發熱重組法10
    2-4 水蒸氣重組法11
    2-4-1 以水蒸氣重組法進行乙醇產氫之機制12
    2-4-2 水蒸氣重組法之程序15
    2-5 觸媒17
    2-5-1乙醇/水蒸氣重組產氫所使用之觸媒17
    2-5-2 Ni/γ-Al2O3觸媒的簡介20
    2-6 電漿22
    2-6-1 電漿原理22
    2-6-2 電漿產生方式24
    2-6-3 電漿放電對觸媒表面特性之影響28
    三、研究設備與研究方法34
    3-1 觸媒製備34
    3-1-1 觸媒製備藥品34
    3-1-2 觸媒製備步驟34
    3-2 實驗設備35
    3-2-1 氣體供應系統36
    3-2-2 乙醇及水汽化系統37
    3-2-3 介電質放電系統37
    3-2-4 水蒸氣重組反應系統39
    3-2-5 氣體冷凝系統39
    3-2-6 最終產物鑑定系統40
    3-3 研究方法40
    3-3-1 研究規劃40
    3-3-2 主體實驗41
    3-3-3 轉化效率之表示方式44
    四、結果與討論46
    4-1介電質放電實驗46
    4-2 電漿處理前、後之觸媒活性實驗48
    4-2-1 乙醇轉化率48
    4-2-2 電漿處理前、後觸媒之各產物選擇性51
    4-2-3 各產物選擇性比較57
    4-2-4 氫氣產率73
    4-3 反應溫度對產物之影響75
    4-4 非熱電漿對觸媒表面之影響76
    4-5 積碳之影響79
    4-6 表面特性分析81
    4-6-1 A組觸媒之BET表面積分析81
    4-6-2 A組觸媒之XRD圖譜81
    五、結論與建議83
    5-1 結論83
    5-2 建議84
    參考文獻86
    附錄:選擇性實驗數據原始資料……………………………………………………….......95
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    赤崎正則, 村岡克紀,渡邊征夫, 狫原建治, 電漿工學的基礎, 復文書局, 9-44, 1990.
    阿部東彥, 加田正之, 入三欲, 電漿化學, 復文書局, 15, 1991.
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  • Moo-Been Chang(張木彬)
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    Date of Submission 2009-07-29

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