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標題: | 高壓下含有二氧化碳、醇類及酯類混合物汽液相平衡之研究 Vapor-Liquid Equilibria at High Pressures for the Mixtures of Carbon Dioxide, Alcohols and Esters |
作者: | Chen-Hsi Cheng 鄭承熙 |
指導教授: | 陳延平(Yan-Ping Chen) |
關鍵字: | 汽液相平衡,雙成分,三成分,四成分,二氧化碳,醇類與酯類混合物, VLE,binary,ternary,quaternary,high pressure,carbon dioxide,alcohol and ester mixture, |
出版年 : | 2006 |
學位: | 博士 |
摘要: | 超臨界流體技術為一新興的分離技術,而高壓相平衡實驗數據與熱力學理論,乃為發展此一製程的重要關鍵所在。本研究利用一套靜態式具可見視窗之相平衡裝置,量測三組酯類 (isopropyl acetate , diethyl carbonate , ethyl butyrate)與二氧化碳於高壓下之汽液相平衡系統。量測溫度範圍為308.15至318.15 K,壓力範圍為3.1至8.9 MPa,共77個新的實驗數據。本研究利用Soave-Redlich-Kwong (SRK)和Peng-Robinson (PR)狀態方程式配合不同混合規則,關聯三組高壓二成分系統,由結果可知,狀態方程式配合凡得瓦二參數混合規則,對於本研究系統之適用性最高,可以得到令人滿意之結果。
此外,本研究利用此設備量測三組醇類與酯類混合物 (ethanol - ethyl acetate ; 1-propanol - propyl acetate ; ethanol - 1-propanol - ethyl acetate)與二氧化碳於高壓下三成分和四成分之汽液相平衡系統,測量溫度範圍在303.15至318.15 K,壓力範圍在4.0至10.0 MPa,總共獲得123個三成分和45個四成分新的實驗數據。在特定之溫度與壓力條件下,三成分及四成分混合物系統於高壓二氧化碳中,乙醇或正-丙醇易存於汽相而與其它混合物相互分離。利用modified Soave-Redlich-Kwong (MSRK)和Peng-Robinson (PR)狀態方程式搭配混合規則或液體模式,直接進行實驗數據之關聯和預測。對於三成分系統之計算結果得知,使用PR狀態方程式及Huron-Vidal混合規則搭配NRTL液體模式計算之迴歸與預測結果為最佳。 理論計算模式亦為設計超臨界流體程序之重要關鍵,本研究利用具理論基礎之計算與預測方式,對於高壓二氧化碳-醇類-水三成分汽液相平衡之系統作詳盡討論。將計算結果應用於半導體工業之晶圓製造上,使用超臨界流體輔以共溶劑 (醇類)之清洗及水分去除是有益的。對於不同共溶劑進行水分去除之效果,在相同的溫度與壓力條件下,以乙醇為共溶劑時,去除水分效果最佳。對於不同共溶劑之殘留量與水分去除量之比例而言,乙醇在T = 318.15 K及P = 20.0 MPa之條件下有最小值。這些結果與建議,可提供相關工業界使用超臨界流體清洗或乾燥之參考。 The application of supercritical fluids (SCF) as an alternative solvent in industrial processes has attracted more and more attention in recent years. The key points for the design of process and selection of optimal operating condition are the equilibrium solubility data in supercritical fluids and appropriate thermodynamic models for calculation. A static type with visual windows apparatus was used to measure the vapor-liquid equilibria (VLE) of CO2 with isopropyl acetate, diethyl carbonate, ethyl butyrate binary mixtures at 308.15 to 318.15 K over the pressure range from 3.1 to 8.9 MPa. New VLE data for CO2 with esters are presented. These VLE data were also correlated using the Soave-Redlich-Kwong and the Peng-Robinson equations of state with various mixing rules. It is shown that both equations of state with the van der Waals mixing rules and two adjustable parameters gave satisfactory correlation results. The apparatus was also used to measure the VLE of CO2 with ethanol - ethyl acetate, 1-propanol - propyl acetate ternary mixtures, and ethanol - 1-propanol - ethyl acetate quaternary mixture at 303.15 to 318.15 K over the pressure range from 4.0 to 10.0 MPa. New VLE data for CO2 with mixed solvents are presented. It was observed that, at specific temperature and pressure, ethanol or 1-propanol can be separated from mixed solvent into the vapor phase at all concentrations in the presence of high pressure CO2. These ternary VLE data were also correlated and predicted using the modified Soave-Redlich-Kwong (MSRK) and the Peng-Robinson (PR) equations of state with mixing rule or liquid model. The PR equation of state by the Huron-Vidal mixing rule with the NRTL activity coefficient model gave satisfactory correlation and prediction results. Calculation of liquid solubility in supercritical fluids is very important for design purpose. In this research, correlation and prediction for the VLE of CO2 with alcohol - water ternary systems at high pressures were discussed. It is useful for the cleaning and the removal of water in the semiconductor industry for wafer production. At the same condition of temperature and pressure, ethanol showed the best effect for water removal. The ratio of the co-solvent residual to water removal is minimum at T = 318.15 K and P = 20.0 MPa. These results and discussion provide the information of cleaning and drying processes using supercritical fluid. |
URI: | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/34268 |
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顯示於系所單位: | 化學工程學系 |
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