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Excess Thermodynamic Functions of Methyl Acetate-Methanol and Methyl Acetate-Ethanol Systems*

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Excess Thermodynamic Functions of Methyl Acetate-Methanol and Methyl Acetate-Ethanol Systems* EXCESS THERMODYNAMIC FUNCTIONS OF METHYL ACETATE-METHANOL AND METHYL ACETATE-ETHANOL SYSTEMS* ISAMU NAGATA, TATSUHIKO OHTA AND TAKESHI TAKAHASHI** Department of Chemical Engineering, KanazawaUniversity, Kanazawa, Japan Isothermal vapor-liquid equilibrium data are presented for methyl acetate-methanol system at 35° and 45°C and for methyl acetate-ethanol system at 45° and 55°C. Excess enthalpy data for the two systems are obtained at 45°C. Simultaneous fit of these thermodynamic quantities was successfully accomplished by using the NRTL equa- tion whose parameters were assumed to be a linear function of temperature. Table 1 Physical properties of compounds Introduction Compound Bp[-C] Density at Refractive The work presented here forms part of a programme 25-C index at 25-C to determine excess Gibbs functions and excess nD Methyl acetate 56.8 0.9273 1.3588 enthalpies for mixtures of alcohols with esters. 56.9 (ll) 0.9279 (ll) 1.3587 (5) Methanol 64.7 0.7865 1.3265 Experimental 64.65(1) 0.78653(ll) 1.32663(12) Ethano1 78.3 0.7852 1.3591 Material. Methanol was distilled twice in a 78.3 (ll) 0.7851 (ll) 1.35929(ll) glass column packed with McMahon packings. s Ethanol was refluxed over calcium oxide and then fractionated in the same column. Methyl acetate mined by density or refractive index measurements. was refluxed with acetic anhydride for six hours and Densities of methyl acetate-ethanol mixture were then distilled through a packed column. The distil- obtained by using Sprengel-Ostwald phycnometers late was shaken with anhydrous potassium carbonate (capacity ca. 10 cm3) fitted with capillary arms of and redistilled. The physical properties of purified internal diameter 1 mm. The temperature of a materials are compared with the literature values water thermostat was controlled at 25° i 0.1°C. in Table 1. The pycnometers were calibrated using distilled water. Procedure. Isothermal vapor-liquid equilibrium Weighingwas done on a Shimadzubalance within data was obtained using a Jones still4). The boiling i 0.0001 g of observed value. The vapor and liquid temperature was maintained within +0.05°C of samples of methyl acetate-methanol were analyzed designated temperature and measured with a copper- by refractive index measurements at 25° ^ 0.1°C. constantan resistance thermometer, which was cali- A Shimadzu Pulfrich refractometer was used for this brated against a standard mercury thermometercali- purpose. The tolerance of the measurements was brated by the National Research Laboratory ofMetrol- less than ± 0.0001. ogy5 Tokyo. The equilibrium pressure was measured Calorimetry. A calorimeter consists of a glass using a mercury manometer. The height of the mixing cell with two compartments in its upper half mercury level was read off by a cathetometer with and a side arm. The two liquids to be mixed are an accuracy of i 0-1 mm.The atmospheric pressure confined separately, and in the complete absence of and room temperature were recorded for each ex- vapor spaces in the compartments since mercury perimental run and necessary corrections were added filled the rest of the cell and the arm. The cell was to observed reading of pressure4}. In all cases mounted in a sealed plastic cylinder immersed in a measurements were taken only after the boiling tem- water thermostat with inner and outer baths controlled perature had remained constant for at least one hr. separately. Mixing was brought about by inverting The composition of equilibrium mixtures was deter- the cylinder. The temperature of the cell was kept ＊ Received on March3，1972 within ^ 0.005°C of specified temperature. The ＊＊ Department ofNuclear Englneerlng，Nagoya Uni－ temperature change was detected from graphical VerSlty，Nagoya extrapolation of resistance values obtained from a VOL. 5 NO. 3 1972 :i3: 227 Table 2 Vapor-liquid equilibrium data for the binary systems X , 2/i P [m m H g ] A 7 i g E Zh /* Z/P * * [% ] [c a l/m o l] M e t h y l A c e t a t e ( l ) - M e t h a n o l ( 2 ) a t 3 5 - C 0 .0 1 1 0 . 0 5 4 2 1 8 . 4 3 .2 6 2 1 .0 0 0 0 .9 8 1 0 .9 8 1 7 .8 7 - 0 . 0 0 2 1. 2 1 0. 0 2 4 0 . 1 0 3 2 2 9 .6 2 . 9 9 5 1 . 0 0 9 0 . 9 8 0 0 . 9 8 0 2 1 .4 3 - 0 . 0 0 9 1. 2 7 0 . 0 5 0 0 . 1 8 1 2 4 8 . 9 2 .7 3 4 1 .0 2 4 0 .9 7 8 0 .9 7 8 4 4 . 6 7 - 0 . 0 1 8 1. 2 6 0 . 2 0 8 0 . 43 1 3 1 0. 6 1 . 9 4 3 1 . 0 5 9 0 . 9 7 4 0 . 9 7 3 1 1 2 .3 2 - 0 . 0 1 2 - 0 . 9 4 0 .3 2 2 0 . 5 2 2 3 3 4 .3 1 . 6 3 3 1 . 1 1 6 0 . 9 7 2 0 . 9 7 1 14 2 .14 0 . 00 1 - 0 . 7 9 0 . 3 8 9 0 . 5 5 0 3 4 4 .6 1. 4 6 7 1. 2 0 0 0 .9 7 1 0 .9 7 0 1 59 . 5 3 - 0 . 0 0 7 - 0 . 4 5 0 . 4 52 0 . 5 8 5 3 5 2. 8 1. 3 7 4 1. 2 6 2 0 .9 7 0 0 .9 6 9 16 6 . 0 7 - 0 . 0 0 1 0 . 00 0 .5 2 5 0 . 61 9 35 9 . 0 1. 2 7 3 1 .3 6 0 0 .9 7 0 0 .9 6 8 1 6 6. 9 1 0 . 0 0 0 0 . l l 0. 6 5 1 0 .6 8 2 3 6 5 . 8 . 1 5 2 1 . 5 7 3 0 . 9 7 0 0 . 9 6 8 1 5 3 . 04 0 . 00 3 0. 3 7 0 .7 2 2 0 .7 1 7 36 5 . 2 1 . 0 9 0 1 . 7 5 4 0 . 9 7 0 0 . 9 6 8 1 3 3. 7 6 0 . 0 0 0 0. 01 0 .7 8 0 0. 7 5 2 3 6 3 . 0 1. 0 5 2 1 .9 3 1 0 .9 7 0 0 .9 6 8 1 1 2 . 88 - 0 . 0 0 2 - 0 . 2 8 0. 8 6 1 0 .8 2 3 35 8 . 9 1 . 0 3 2 2 . 1 5 7 0 . 9 7 0 0 . 9 6 8 8 1. 9 0 0 .0 0 5 0 .0 4 0 .9 0 5 0 . 8 6 0 3 5 3. 0 1 . 0 0 9 2 . 4 5 6 0 . 9 7 1 0 . 9 6 8 5 7 . 46 - 0 . 0 0 2 - 0 . l l 0 . 9 3 3 0 . 8 9 3 3 4 4 .7 0 . 9 9 4 2 . 6 0 1 0 . 9 7 1 0 . 9 6 9 3 5 .5 1 - 0 . 0 0 2 - 1. 1 8 M e t h y l A c e t a t e ( l ) - M e t h a n o l ( 2 ) a t 4 5 - C 0 . 02 1 0 . 0 9 6 3 6 0 . 7 3 . 3 5 9 0 . 9 9 4 0 . 9 7 3 0 . 9 7 3 1 2 .5 3 0 . 0 0 7 2 . 00 0 . 0 4 9 0 . 1 7 1 3 8 5. 6 2 . 7 3 6 1 . 0 0 1 0 . 9 7 1 0 . 9 7 1 3 2 .0 4 - 0 . 0 0 7 0 . 87 0 . 0 8 9 0 . 2 45 4 1 6 . 8 2 .3 2 8 1 .0 2 7 0 .9 6 9 0 .9 6 9 6 2 . 61 - 0 . 0 2 2 0 .3 8 0 . 1 6 7 0 . 3 5 9 4 5 9 . 0 1 . 9 9 6 1 . 0 4 6 0 . 9 6 6 0 . 9 6 6 9 6 . 6 2 - 0 . 0 1 8 - 0 . 3 1 0 . 2 3 5 0 . 4 33 4 8 8 . 8 . 8 1 7 1 . 0 7 0 0 . 9 6 4 0 . 9 6 3 12 1.5 7 - 0 . 0 0 6 0 . 40 0 . 3 4 5 0 . 5 1 0 5 1 7 . 4 1 . 5 4 0 1 . 1 4 1 0 . 9 6 2 0 . 9 6 1 14 8 . 6 7 0 . 0 0 0 0 .4 9 0 . 41 7 0 . 5 4 8 5 3 0. 7 1. 4 0 3 1 .2 1 1 0 .9 6 1 0 .9 6 0 15 9 . 8 4 0 . 0 0 0 0 .6 8 0 .4 9 1 0 . 5 89 5 4 0. 7 1 . 3 0 4 1 . 2 8 4 0 . 9 6 1 0 . 9 5 9 16 2 .7 8 0 . 0 05 0 .8 2 0 . 5 6 9 0 . 6 23 5 4 8. 7 .2 0 7 1 .4 10 0 .9 6 0 0 .9 5 8 16 1. 3 7 0 . 00 1 1. 0 9 0 . 65 5 0 . 6 6 6 5 5 1. 9 1 . 1 2 7 1 . 5 6 9 0 . 9 6 0 0 . 9 5 8 14 7 .9 1 0 .
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