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研究生:蔡嘉瑩
研究生(外文):Chia-Ying Tsai
論文名稱:非均相觸媒之乙酰丙酸乙酯合成反應動力行為研究
論文名稱(外文):Kinetic Behavior Study on the Synthesis of Ethyl Levulinate over Heterogeneous Catalyst
指導教授:李明哲李明哲引用關係
指導教授(外文):Ming-Jer Lee
口試委員:李明哲
口試委員(外文):Ming-Jer Lee
口試日期:2014-06-23
學位類別:碩士
校院名稱:國立臺灣科技大學
系所名稱:化學工程系
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:2014
畢業學年度:102
語文別:中文
論文頁數:159
中文關鍵詞:乙酰丙酸乙酯吸附強度模式關聯
外文關鍵詞:ethyl levulinateadsorption strengthsdata fitting
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本研究使用批式反應器探討由乙酰丙酸與乙醇合成乙酰丙酸乙酯合成反應之非均相反應動力行為,反應中使用酸性陽離子交換樹脂Amberlyst 39為觸媒。實驗操作於328.15 K至348.15 K之間,此外,並探討(醇/酸)進料莫耳比、觸媒質傳阻力以及觸媒添加量之效應。
反應動力實驗結果顯示,反應速率隨著反應溫度、(醇/酸)進料莫耳比、觸媒量以及轉速提高而加快,而昇高反應溫度與(醇/酸)進料莫耳比也會提升酸之平衡轉化率。經由吸附平衡實驗結果得知,乙酰丙酸乙酯之合成反應中各成分於Amberlyst 39之吸附強度依序為水 > 乙醇 > 乙酰丙酸 > 乙酰丙酸乙酯。
乙酰丙酸乙酯合成反應動力數據分別以理想溶液擬均相模式(IQH)、非理想溶液擬均相動力模式(NIQH)、Eley-Rideal(ER)模式、Langmuir-Hinshelwood-Hougen-Watson(LHHW)模式以及LHHW with Ka (LHHW-Ka)模式關聯,並求得最適化的動力參數值,NRTL模式則用於計算各反應成分之活性係數,關聯的結果顯示LHHW模式為描述乙酰丙酸乙酯合成反應的非均相催化動力行為的最佳模式。
The heterogeneous kinetics behavior was investigated with a batch reactor for the synthesis of ethyl levulinate from levulinic acid and ethanol over cation-exchange resins, Amberlyat 39. The experiments were conducted at tempertures from 328.15 K to 348.15 K. Additionally, the effects of molar ratio of ethanol to acid in the feed stream, the mass transfer resistances on the catalytic reaction, and the different levels of catalyst loadings were also observed.
The reaction rate of acid increased with increase of reaction temperature, molar ratio of ethanol to acid in the feed stream, catalyst loading, and rotational speed. Moreover, the equilibrium conversion of acid increased with increase of reaction temperature and molar ratio of methanol to acid in the feed stream. The relative adsorption strengths of the reacting species were determined by adsorption experiments. The results indicated that the magnitude of adsorption strengths on Amberlyst 39 followed the order of water > ethanol > levulinic acid > ethyl levulinate .
The kinetic data of the synthesis of methyl levulinate were correlated with the ideal-quasi-homogeneous (IQH), the non-ideal-quasi-homogeneous (NIQH) the Eley-Rideal (ER), the Langmuir-Hinshelwood-Hougen-Watson (LHHW) and the Langmuir-Hinshelwood-Hougen-Watson with Ka (LHHW-Ka) models, respectively. The optimal values of the kinetic parameters were determined from the data fitting. The NRTL model was used to calculate the activity coefficients for each reacting species. The LHHW model yielded the best representation for the kinetic behavior of heterogeneous catalytic synthesis of ethyl levulinate.
第一章 緒論
1-1 前言
1-2文獻回顧
1-3 本研究之重點
第二章 反應動力實驗
2-1 酯化反應動力數據量測
2-2 藥品
2-3 實驗步驟
2-4 組成分析
2-5 數據處理
2-6 動力反應實驗結果
2-7 結果與討論
第三章 等溫吸附平衡實驗
3-1 雙成份系統吸附平衡測量
3-2藥品
3-3實驗步驟
3-4數據處理
3-5吸附實驗結果
3-6 吸附實驗數據關聯結果
第四章 動力模式
4-1 動力模式
4-2理想溶液擬均相動力模式
4-3非理想溶液動力模式
4-4 速率常數與吸附常數的訂定
4-5乙酰丙酸乙酯之動力模式關聯結果
4-6 非理想溶液之平衡常數
4-7 Langmuir-Hinshelwood-Hougen-Watson with Ka (LHHW-Ka)動力模式
第五章 結論與建議
5-1 結論
5-2 建議與注意事項
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