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| 研究生： |
施易緯 Yi-Wei Shih |
|---|---|
| 論文名稱： |
二氧化碳膨脹液體中對二甲苯氫化之研究 Hydrogenation of p-Xylene in CO2-Expanded Liquid |
| 指導教授： |
談駿嵩
Chung-Sung Tan |
| 口試委員: | |
| 學位類別： |
碩士 Master |
| 系所名稱： |
工學院 - 化學工程學系 Department of Chemical Engineering |
| 論文出版年： | 2006 |
| 畢業學年度： | 94 |
| 語文別： | 中文 |
| 論文頁數： | 87 |
| 中文關鍵詞： | 二氧化碳膨脹液體 |
| 相關次數： | 點閱：1 下載：0 |
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對二甲苯(p-Xylene)為對苯二甲酸(Terephthalic Acid)之原料，而對苯二甲酸主要用途為聚對苯二甲酸二乙酯(PET)之合成。由於PET結構中含苯環，微生物無法分解其結構，若能將p-Xylene中之苯環完全氫化，再將其甲基氧化為羧基，以此化合物與乙二醇進行聚合即可得結構同PET但不含苯環之生物可分解聚合物。為達成此目的， p-Xylene氫化反應速率之提升即成為一重要課題。
在文獻中已證實，若在液相中加入高壓二氧化碳，可使溶液膨脹而形成二氧化碳膨脹液體(CO2-Expanded Liquid)，增加反應物氣體如氫氣或氧氣於液體中之溶解度，並降低溶液之黏度，對物質在觸媒內部或液相中之質傳速率有所助益，進而增加反應速率。本研究在一連續式固定床反應器中進行p-Xylene液相氫化反應，並於系統中加入高壓二氧化碳以形成CO2-Expanded Liquid，觀察在不同二氧化碳含量下p-Xylene轉化率、產物Cis/trans比及反應選擇率的變化。
研究發現以Pt/γ-Al2O3、Pd/γ-Al2O3、Ru/γ-Al2O3及Ru/SiO2為觸媒時，在系統中加入二氧化碳後觸媒皆有明顯失活的現象。為了解觸媒的失活是否與二氧化碳有關，我們在反應物通入系統前先通入二氧化碳，使觸媒與二氧化碳接觸後，停止二氧化碳進料並通入反應物，結果發現觸媒已失活，故可知觸媒的失活為二氧化碳所造成。由於以γ-Al2O3及SiO2為擔體時，觸媒皆有失活的現象，故我們再將擔體改為Carbon，以商用Pd/C觸媒進行測試。實驗發現在CO2/H2莫耳比為0.1時轉化率確實有提升，觸媒無失活。由以上實驗可知觸媒的失活與擔體有關，以γ-Al2O3及SiO2為擔體時有失活的現象，但以Carbon為擔體時則無。推測是因金屬擔載於γ-Al2O3及SiO2時，二氧化碳會吸附於觸媒表面，影響氫氣之吸附而使觸媒失活。使用Carbon時則因金屬於擔體上散布型態的不同；使用Carbon時則因金屬於擔體上散布型態的不同，而不會產生此現象。未來可使用不同分析方式進一步地確認觸媒失活之原因，以求在CO2-Expanded Liquid之研究中能選擇一最佳之觸媒擔體。
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