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研究生: 林士熙
Shih-Shi Lin
論文名稱: 合成碳酸二苯酯的高溫高壓反應動力行為研究
Kinetics Behavior Study of the Synthesis of Diphenyl Carbonate at Elevated Temperatures and Pressures
指導教授: 李明哲
Ming-Jer Lee
口試委員: 李豪業
Hao-Yeh Lee
王聖潔
San-Jang Wang
學位類別: 碩士
Master
系所名稱: 工程學院 - 化學工程系
Department of Chemical Engineering
論文出版年: 2014
畢業學年度: 102
語文別: 中文
論文頁數: 93
中文關鍵詞: 反應動力學碳酸二苯酯高溫高壓合成反應
外文關鍵詞: kinetics behavior study, diphenyl carbonate, elevated temperatures and pressures synthesis
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本研究以高溫高壓連續式反應器探討碳酸二乙酯與乙酸苯酯的均相轉酯化反應動力行為,以有機鈦化合物鈦酸四乙酯為本實驗的觸媒,實驗操作於438.15 K ~ 468.15 K之間,壓力介於20 bar~ 30 bar之間,進料乙酸苯酯/碳酸二乙酯莫耳比為6、4及3以及進料碳酸二乙酯/乙酸苯酯莫耳比為6。實驗結果顯示碳酸二乙酯的反應速率隨溫度增加而提高,但在本實驗之溫度範圍內的平衡轉化率差距不大,亦即一轉酯化反應的熱效應不顯著。另外,當進料莫耳比增大時,平衡轉化率有顯著地提高。
本研究分別以兩種理想溶液均相動力模式關聯所量取之動力數據,以求得模式中的動力參數值。關聯的結果顯示,以整體來說動力模式二為最適合描述碳酸二乙酯與乙酸苯酯之轉酯化反應動力行為,其完成量測的系統提供相關製程模擬與設計使用。


The kinetic behavior of homogeneous transesterification of diethyl carbonate with phenyl acetate over an catalyst, titanium ethoxide, was investigated with a continuous tubular reactor. The tranesterification was performed te between
438.15 K to 468.15 K and the molar ratios of feed (phenyl acetate to diethyl carbonate) at 6, 4, 3 and the molar ratios of feed(diethyl carbonate to phenyl acetate) at 6, respectively. The reaction rate was found increase with increasing temperature, but the equilibrium conversions of diethyl carbonate were close over the entire range of experimental conditions. It means that the heat effect is minor. In addition, the equilibrium conversions of diethyl carbonate was found increase obviously with increasing molar ratios of feed.
The kinetic data were correlated with two different ideal solution quasi-homogeneous kinetic models. The model parameters were determined by fitting the kinetic data to these models. Generally, the second model yielded better representation for kinetic behavior of transesterification of diethyl carbonate with phenyl acetate. This model can be applied to the process simulation and process design.

英文摘要 I 中文摘要 II 誌謝 III 目 錄 IV 表目錄 VII 圖目錄 VII 第一章 緒論 1 1-1 前言 1 1-2 碳酸二苯酯的物理化學性質 2 1-3 碳酸二苯酯合成研究進展 4 1-3-1 光氣法 4 1-3-2 苯酚氧化羰基化法 5 1-3-3 轉酯化法 7 1-3-3-1 碳酸二甲酯與苯酚反應合成DPC 7 1-3-3-2 草酸二甲酯與苯酚轉酯化反應合成DPC 9 1-3-3-3 羧酸酯和碳酸二甲酯轉酯化反應合成DPC 10 1-4 轉酯化法合成DPC的反應製程發展 12 1-4-1 DPC合成及DMC/MeOH分離製程 12 1-4-2 分區反應製程 12 1-4-3 分區反應及萃取分離製程 13 1-4-4 反應精餾法合成DPC製程 14 1-5 研究動機 15 第二章 反應動力實驗 22 2-1 反應動力裝置之主要設備 22 2-2 實驗藥品 23 2-3實驗操作步驟 25 2-4 氣象層析儀校正 26 2-5 數據處理 27 2-6 動力反應實驗結果 32 2-7 結果與討論 33 第三章 理想溶液均相動力模式 55 3-1 動力模式 55 3-1-1 動力模式一 55 3-1-2 動力模式二 57 3-2 動力模式之關聯結果 60 3-2-1 動力模式一之關聯結果 60 3-2-2 動力模式二之關聯結果 60 第四章 結論與建議 86 4-1 結論 86 4-2 建議 87 參考文獻 88 符號說明 91

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