本研究利用一套具有視窗的靜態式裝置，量取恆溫汽液液平衡性質，其量測溫度介於313.24 K至373.15 K之間。本研究實驗量測了水+丙二醇甲醚醋酸酯、水+醋酸甲酯、水+丙酸甲酯及水+丙酸異丙酯的雙成份汽液液平衡性質。本研究也分別量測水+丙二醇甲醚醋酸酯+丙二醇甲醚、水+醋酸甲酯+甲醇、水+丙酸甲酯+甲醇、水+醋酸甲酯+丙酸甲酯及水+丙酸異丙酯+異丙醇的三成份汽液液平衡性質。分別以NRTL及UNIQUAC模式搭配Hayden-O’Connell (HOC) 模式，並採用與溫度線性關係的參數，能夠把雙成分水溶液系統的相互溶解度數據關聯得很好。對於type-I LLE 類型的三成份系統，預測結果證實使用關聯雙成分配對的VLE或VLLE數據所得的參數，無法準確地估算其三成份汽液液平衡性質。在本研究裡，三成份汽液液平衡數據也用於檢驗多種版本之UNIFAC模式的合適性。以同時調整NRTL及UNIQUAC模式中的模式參數的方式關聯三成份汽液液平衡數據，可大幅地改善對三成份汽液液平衡性質的描述。
本研究使用體積立方型的Soave-Redlich-Kwong (SRK)狀態方程式估算酯化反應混合物系統之汽液及汽液液平衡性質，研究中分別採用三種α函數來描述吸引力項能量參數a的溫度效應，並搭配van der Waals (vdW)單一流體混合律或Chung-Twu (CT)混合律。計算結果顯示以SRK-T/CT-UNIFAC-Lyngby模式(SRK狀態方程式搭配T型α函數及引入UNIFAC-Lyngby模式的CT混合律)具有較佳的預測能力，此種方法不但可準確地預測雙成份汽液平衡性質，亦能合理預估三成份水溶液混合物之汽液液相平衡行為，此法僅需純質成份之蒸汽壓數據。另外，SRK-T/CT-UNIFAC-LL模式，則對type-II液液平衡系統有不錯的預測效果。

A static-type apparatus equipped with a visual cell was utilized in the present study to measure isothermal vapor-liquid-liquid equilibrium (VLLE) data over a temperature range of 313.24 to 373.15 K. The binary VLLE properties were determined experimentally for mixtures of water + propylene glycol methyl ether acetate (PGMEA), water + methyl acetate, water + methyl propionate and water + isopropyl propionate. The ternary VLLE properties were also measured for mixtures of water + PGMEA + propylene glycol monomethyl ether (PGME), water + methyl acetate + methanol, water + methyl propionate + methanol, water + methyl acetate + methyl propionate and water + isopropyl propionate + isopropanol. The mutual solubility data of the binary aqueous systems could be correlated well by the NRTL and the UNIQUAC models accompanied with the Hayden-O’Connell (HOC) model over a wide temperature range as linearly temperature-dependent parameters were adopted. The predicted results proved that the ternary VLLE properties are unable to be estimated accurately by using the parameters determined from the phase equilibrium data of the constituent binaries for the type-I LLE systems. The ternary VLLE data were also used to test the validity of various versions of the UNIFAC model. The representation of the ternary VLLE properties was substantially improved as the parameters of the NRTL and the UNIQUAC models were determined simultaneously from the ternary VLLE data.
In the present study, the Soave-Redlich-Kwong (SRK) equation, a cubic equation of state, was utilized to calculate VLE and VLLE properties of mixtures of esterification by using three types of α function that accounts for the temperature dependence of the energy parameter (a) in the attractive term. The selected mixing rules in this study are the van der Waals (vdW) one-fluid mixing rules and Chung-Twu (CT) mixing rules. The calculated results showed that SRK-T/CT-UNIFAC-Lyngby (the SRK equation with the T type α function and the CT mixing rules embedded the UNIFAC-Lyngby model) model, in general, not only predicted accurately the binary VLE properties, but also represented the ternary VLLE phase behavior reasonably well. The vapor pressure data of the pure substances are the only required property for SRK-T/CT-UNIFAC type model. Moreover, the predicted results of the SRK-T/CT-UNIFAC-LL model were satisfactory for the type-II LLE systems.

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