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研究生:楊國華
研究生(外文):Kuo Hua Yang
論文名稱:逆水氣轉移反應在鉀促進劑鎳氧化鋁上積碳的研究
論文名稱(外文):Study of carbon deposition on K-promoter Ni/Al2O3 using RWGS
指導教授:尤建華
指導教授(外文):J. H. You
學位類別:碩士
校院名稱:長庚大學
系所名稱:化工與材料工程研究所
學門:工程學門
學類:化學工程學類
論文種類:學術論文
論文出版年:2008
畢業學年度:96
論文頁數:104
中文關鍵詞:逆水氣轉移反應鎳觸媒鉀觸媒奈米碳管
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本實驗主旨在研究減量二氧化碳與資源化再利用以及觸媒表面上生成類似化學氣相沉積法積碳的檢測。不同比例鉀促進劑添加到Ni/Al2O3形成的高性能觸媒利用逆水氣轉移反應使二氧化碳轉換為一氧化碳不僅達到減量二氧化碳還可得到高經濟效益產物,包括觸媒表面形成的管狀碳纖維。實驗部份以不同比例的鉀-鎳觸媒在不同的進料流速的變因下,觀察一氧化碳與甲烷的產生率,並找出其積碳活性點位置。同時在反應過程中秤量積碳比較質量變化,取樣進行Raman、XRD、TEM-EDS、XPS等實驗。
實驗數據結果顯示逆水氣轉移反應在K/Ni/Al2O3觸媒反應途徑是走平行反應,混合氣當中的二氧化碳同時轉換一氧化碳與甲烷,增加鉀促進劑時會增加一氧化碳產率以及抑制甲烷的產率,也發現在7wt% K-Ni/Al2O3觸媒會有最大的積碳質量與消失的甲烷氣體有密切關係。觸媒鑑定發現有K2O物種,在積碳時發現觸媒表面的鉀原子比例有逐漸減少的趨勢,穿透式顯微鏡也看到類似管狀的碳纖維且進行EDS時完全沒有鉀原子訊號,可再度證實積碳是從鉀原子生長當有積碳生成時會遮蓋到鉀元素。
The goal of the research is to reduce ration of carbon dioxide and to
recycle of the carbon dioxide with using the reverse water gas shift reaction (RWGS) on K-Ni/Al2O3 catalysts. There are some carbon deposition on Ni-K catalysts in the course of reaction. K-promoter can induce formation of solid carbon on Ni/Al2O3 catalysts. All carbon deposition containing CNFs have been identified by using TEM ,Raman spectroscopy and XRD .
We can see the production of CO and CH4 with K-Ni/Al2O3 catalyst during the RWGS. The conversion of CO2 to CO is independent with K content, but the production of CH4 is inhibited as K adding. 7wt% K-Ni/Al2O3 catalysts has the highest activity to form carbon deposition .The carbon formation can be deduced to associate with inhibition of CH4. K covered on Ni/Al2O3 catalysts can create new sites between K and Ni, leading to production of solid carbon from CO2.
指導教授推薦書..........................................................................................
口試委員會審定書………………………………………………………..
授權書…………………………………………………………………...iii
誌謝……………………………………………………………………...iv
中文摘要…………………………………………………………………v
Abstract…………………………………………………………………..vi
目錄……………………………………………………………………..vii
圖目錄……………………………………………………………………x
表目錄…………………………………………………………………xvii
第一章序論..............................................................................................1
第二章 文獻回顧......................................................................................4
2-1 逆水氣轉移反應的研究...............................................................4
2-2 逆水氣轉移反應的反應機制.......................................................8
2-2-1 表面氧化還原反應機制...................................................8
2-2-2 中間產物甲酸基反應機制.............................................10
2-3 觸媒的介紹.................................................................................12
2-3-1 添入促進劑的影響.........................................................12
2-3-2 鎳金屬催化劑.................................................................13
2-4 CVD法製備奈米碳管.................................................................14
第三章 實驗方法與步驟........................................................................15
3-1 實驗藥品.....................................................................................15
3-2 觸媒的製作步驟.........................................................................15
3-3 氣體反應系統.............................................................................16
3-3-1 反應系統儀器.................................................................16
3-3-2 實驗步驟.........................................................................17
3-4 觸媒特性的測試........................................................................18
3-4-1 程溫還原( Temperature Programmed Reduction )……..18
3-4-2 X-ray繞射分析儀( X-ray diffraction ).............................20
3-4-3 感應耦合電漿原子發射光譜分析儀( ICP/AES )..........22
3-5 程溫脫附( Temperature Programmed Desorption )...................23
3-6 拉曼光譜儀( Raman Spetrum )..................................................24
3-7 X射線光電子能譜儀 ( XPS )....................................................26
第四章 結果與討論................................................................................31
4-1 鉀-鎳觸媒成份之鑑定...............................................................31
4-1-1 觸媒ICP/AES 元素組成分析........................................31
4-1-2 觸媒高解析電子能圖譜儀 ( XPS )...............................33
4-1-3氫氣-程溫還原 ( H2-TPR )..............................................39
4-1-4 XRD分析..........................................................................41
4-2 應用於鎳鉀觸媒的反應.............................................................44
4-2-1 鉀鎳觸媒與反應流速的影響.........................................44
4-2-2 中間產物的反應途徑推測.............................................49
4-2-3 甲烷與積碳的關係.........................................................54
4-3 積碳反應的探討.........................................................................59
4-3-1 進料流速與觸媒比例對積碳的探討.............................59
4-3-2 積碳之TEM圖................................................................61
4-3-3 拉曼光譜儀( Raman Spectrum ).....................................68
4-3-4 XPS...................................................................................75
4-3-5 積碳之XRD分析測定....................................................88
4-4程溫脫附( Temperature Programmed Desorption ).....................92
4-4-1 觸媒表面吸附二氧化碳的研究.....................................92
第五章 結論..........................................................................................101
參考文獻..............................................................................................102
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