Vapor–liquid equilibria and excess properties for methyl tert-butyl ether (MTBE) containing binary systems

Fluid Phase Equilibria 200 (2002) 399409

Vaporliquid equilibria and excess properties for methyl tert-butylether (MTBE) containing binary systems

So-Jin Park a,, Kyu-Jin Han a, J. Gmehling ba Department of Chemical Engineering, College of Engineering, Chungnam National University,

Daejeon 305-764, South Koreab Technische Chemie FB9, Universitt Oldenburg, Postfach 2503, D-26111 Oldenburg, Germany

Received 18 December 2001; accepted 12 February 2002

Abstract

Methyl tert-butyl ether (MTBE) is recently widely used in the chemical and petrochemical industry as a non-polluting octane booster for gasoline and as an organic solvent. The isobaric or isothermal vaporliquid equilibria(VLE) were determined directly for MTBE + C1C4 alcohols. The excess enthalpy (HE) for butane + MTBEor isobutene + MTBE and excess volume (VE) for MTBE + C3C4 alcohols were also determined. Besides, theinfinite dilute activity coefficient, partial molar excess enthalpies and volumes at infinite dilution (, HE,, VE,)were calculated from measured data. Each experimental data were correlated with various gE models or empiricalpolynomial. 2002 Elsevier Science B.V. All rights reserved.

Keywords: Methyl tert-butyl ether (MTBE); Vaporliquid equilibria; Activity coefficient; Excess molar property; Infinitedilution; Correlation

1. Introduction

Accurate representation of the chemical activities is not only essential for the design of fluid phaseseparation equipment but also helpful information to describe the mixing rules and the extension of thedatabase for thermodynamic models. The thermodynamic behaviors at infinite dilution have become asubject of considerable interest in the chemical, petroleum, food and pharmaceutical industries. However,accurate measurement and prediction of infinite dilute properties still have some problems because it treatsthe mixtures containing a very low amount of one component. Sometimes, the simple extrapolation of themeasured physical properties is suggested as a rapid and convenient method, giving reasonable values ofinfinite dilute properties; , HE,, VE,, etc.

Corresponding author. Tel.: +82-42-821-5684; fax: +82-42-823-6414.E-mail address: [email protected] (S.-J. Park).

0378-3812/02/$ see front matter 2002 Elsevier Science B.V. All rights reserved.PII: S0378-3812(02)00047-X

400 S.-J. Park et al. / Fluid Phase Equilibria 200 (2002) 399409

Tertiary-alkyl ethers are low toxic and low polluting oxygenated petrochemical compounds, used as anoctane booster for lead-free or low-leaded gasoline and also increasingly valued as a solvent and a chemicalreactant [1,2]. They are usually being produced by the conversion of alkanol with isoalkene. Therefore,the fluid phase equilibria, thermodynamic properties and infinite dilute properties for systems containingtertiary-alkyl ether, alcohols and hydrocarbons are of interest to optimize the manufacturing process orusing them as additives for gasoline. Some investigations were carried out for the methyl tert-butyl ether(MTBE)+ alcohol systems previously [3], but more data are required to develop thermodynamic modelsand to understand solution behaviors.

We have carried out a systematic study of phase equilibria and the fundamental thermophysical prop-erties for binary and ternary mixtures for tertiary-alkyl ether compounds, MTBE, tert-amyl methyl ether(TAME) and ethyl tert-butyl ether (ETBE) [47]. This work is a part of the systematic study for thesystems of MTBE with alcohols or with butane and isobutene, since MTBE is usually synthesized frommethanol and isobutene. The vaporliquid equilibria (VLE) and two different excess properties (HE, VE)were experimentally determined. These experimental properties were correlated with common gE mod-els or RedlichKister polynomial [8]. The activity coefficient at infinite dilution () was calculated bysecond order extrapolation from the calculated activity coefficient, and excess molar properties at infinitedilution (HE,, VE,) were also calculated using RedlichKister parameters. The extrapolated activitycoefficients at infinite dilution were compared with the directly measured values by using differentialebulliometry [9] or calculated values using UNIFAC equation [10].

2. Experimental

2.1. Materials

Commercial grade MTBE and alcohols from Aldrich and Merck were used. They were carefully driedwith Union Carbide type 3 molecular sieves (from Fluka) and then distilled and degassed using a ca. 20theoretical staged fractionating column. Their purities were more than 99.9 wt.% by gas chromatographicanalysis. Butane and isobutene were supplied from Messer Griesheim GmbH. Their purities were betterthan 99.5%. The observed densities () of liquid pure components at 298.15 K are given in Table 1, alongwith the published values [1113] for comparison.

2.2. VLE measurement

Recirculating still [14] is a conventional apparatus to determine isobaric VLE. A recently developedmodified headspace gas chromatographic method [5] allows the rapid and precise determination methodsfor isothermal VLE. In this work, isobaric VLE for MTBE+methanol and MTBE+ethanol systems weremeasured at 101.33 kPa using a Sieg & Rck type recirculator, which is shown in Fig. 1. Isothermal VLEfor systems of MTBE+ 1-propanol and MTBE+ 1-butanol at 313.15 K were measured with the help ofHewlett-Packard (HP) 19395A headspace sampler and the HP 5890 gas chromatograph. In the isobaricmethod, ca. 250 ml liquid mixture was introduced to the still and a Baratron pressure regulating systemwas used to regulate pressure with an accuracy of 0.1 kPa. For the headspace analysis method, about3 ml of the liquid sample mixture for known composition was added to the glass vial with an accuracy of1105 g by Mettler Balance. The glass vials were sealed with a teflon/rubber septum and aluminum cap,

S.-J. Park et al. / Fluid Phase Equilibria 200 (2002) 399409 401

Table 1Experimental densities () with literature values and Antoine constants of pure componentsChemicals Supplier Density () at 298.15 K Antoine constantsa

Observed values Literature values A B C

MTBE Aldrich 0.73533 0.73530b 7.12997 1265.40 242.517Methanol Merck 0.78645 0.78640c 8.08097 1582.27 239.970Ethanol Merck 0.78503 0.78500c 8.11220 1592.86 226.1841-Propanol Merck 0.79948 0.79957c 7.74887 1440.74 198.8062-Propanol Aldrich 0.78101 0.78082c 8.00308 1505.50 211.6001-Butanol Merck 0.80583 0.8060d 7.92484 1617.52 203.2962-Butanol Merck 0.80256 0.8026d 7.47429 1314.19 186.500

a Data from Dortmund Data Bank (DDB, version 1998).b [11].c [12].d [13].

and then kept in the thermostat, the temperature of which was regulated with an accuracy of 0.1 K. Afterthe equilibrium was achieved, the liquid and vapor phase (in the head space analysis, vapor phase only)components were then analyzed by gas chromatography. Highly pure He gas (99.9999%) and TCD wereused for analysis. Determination methods and operating procedures have been described previously [57].

2.3. Excess molar enthalpy measurement

The excess molar enthalpies (HE) for butane+MTBE and isobutene+MTBE mixtures were measureddirectly at 363.15 K under 2 103 kPa using the Hart Scientific isothermal flow calorimeter. This flowcalorimeter was equipped with syringe pumps capable of delivering accurately small pulse-free flows. Italso has several advantages over batch calorimeters with which most currently available HE data havebeen measured. This flow calorimeter works by monitoring the power required by the control heater tokeep the flow cell under isothermal conditions. The operating procedure is described elsewhere [6].

Fig. 1. Schematic diagram for the recirculating still (Sieg & Rck type).


2.4. Excess molar volume measurement

The vibrating tube digital densitometry (Anton Paar DMA 602) was employed to determine the densitiesof the pure compound and the binary mixtures. The densitometry was calibrated for each measurementusing doubly distilled water and dried air at atmospheric pressure. About 3.5 ml of sample mixtures wereprepared by weight with precisions of 1105 g. To minimize the experimental error due to evaporation,4 ml small glass vials were used as mixture vessels. The experimental systematic error was estimatedto be less than 1 104 g/cm3. All the measurements were carried out under atmospheric pressure.The temperature of the vibrating U tube was regulated by Lauda thermostat of which the temperaturewas calibrated against a HP resistance thermometer with an accuracy of 0.01 K. The time interval ofmeasurements was chosen to be 15 min to attain a constant temperature and stability in oscillation.Apparatus and operating procedure are described elsewhere [6,7].

2.5. Calculation of the thermodynamic properties at infinite dilution

The , HE, and VE, are calculated from calculated or measured thermodynamic properties ( ,HE, VE). The value was obtained by using second order extrapolation program and HE,, VE, werecalculated by the correlated parameters of RedlichKister polynomial [8].

3. Results and discussion

For the VLE determination, the simplified VLE Eq. (1) and Antoine Eq. (2) were used. For the headspaceanalysis method, true liquid mole fraction must be calculated. The calculation procedure has been previ-ously described [5].

y1P = x11P s1 (1)

logP si (mmHg) = AB

T (C)+ C (2)

The excess molar volume of mixing, VE, is defined asH E = Hm x1H1 x2H2 (3)

V E =[x1M1 + x2M2

m

] x1M1

1 x2M2

2(4)

The RedlichKister polynomial function was used to correlate the experimental excess molar properties,ME(HE, VE).

ME = x1x2ni=1

Ai(x1 x2)i1 (5)

Standard deviation of the fits, S.D., for excess molar properties is then defined as

S.D. =[

i(MEcalculated MEexperimental)2i

N n

]1/2(6)


Table 2Vaporliquid equilibria for MTBE with methanol and ethanol mixtures at 101.33 kPa

T (K) x1 y1 T (K) x1 y1 T (K) x1 y1MTBE + methanol

334.95 0.0378 0.1311 326.15 0.3543 0.5321 324.45 0.6560 0.6785333.05 0.0694 0.2153 325.95 0.3765 0.5581 324.45 0.7052 0.7038331.45 0.1077 0.2850 325.65 0.4051 0.5571 324.55 0.7659 0.7346330.25 0.1438 0.3389 325.45 0.4312 0.5714 324.65 0.7414 0.7212329.05 0.1807 0.3903 325.15 0.4637 0.5905 324.85 0.8289 0.7763328.15 0.2217 0.4213 324.95 0.4998 0.6085 325.35 0.8520 0.8002327.15 0.2772 0.4789 324.85 0.5316 0.6219 325.45 0.8967 0.8386326.65 0.3061 0.5042 324.65 0.5700 0.6368 326.25 0.9461 0.9000326.35 0.3279 0.5184 324.55 0.6098 0.6563 327.55 0.9915 0.9807

MTBE + ethanol351.25 0.0027 0.0130 335.75 0.2980 0.5892 330.75 0.5801 0.7610348.95 0.0283 0.0952 335.15 0.3221 0.6209 330.35 0.6045 0.7754346.05 0.0685 0.2473 334.65 0.3394 0.6350 329.85 0.6505 0.7937343.35 0.1090 0.3479 334.05 0.3460 0.6548 329.45 0.6992 0.8133341.05 0.1478 0.4114 333.55 0.3831 0.6651 329.05 0.7451 0.8326339.35 0.1902 0.4730 333.05 0.4108 0.6812 328.65 0.7880 0.8520337.95 0.2213 0.5120 332.55 0.4434 0.7044 328.35 0.8261 0.8724337.65 0.2354 0.5416 332.15 0.4615 0.7163 328.05 0.8738 0.8982337.05 0.2520 0.5628 331.55 0.5109 0.7361 327.85 0.9173 0.9263336.45 0.2550 0.5801 331.25 0.5433 0.7434 327.75 0.9611 0.9613

whereMEcalculated is the excess molar property, which is calculated by Eq. (5) andMEexperimental is the experi-mental excess property. From the experimental values, the properties at infinite dilution arecalculated.

The partial molar excess enthalpy and volume at infinite dilution were calculated with the adjustableparameters of the RedlichKister polynomial. The partial molar excess properties at infinite dilution arethe limit of the partial molar excess properties, as shown in Eqs. (7) and (8). In this work, we usedfive adjustable parameters of the RedlichKister polynomial.

ME,1 = lim

x10ME1 = A1 A2 + A3 A4 + A5 (7)

ME,2 = lim

x11ME2 = A1 + A2 + A3 + A4 + A5 (8)

The experimental isobaric or isothermal VLE compositions of MTBE + C1C4 alcohol systems arelisted in Tables 2 and 3, respectively. The activity coefficients were correlated using common gE models(Margules, van Laar, Wilson, NRTL, UNIQUAC). The correlation results of the various model equa-tions were almost the same. The best-fitted model parameters and the mean deviations in the vaporphase, y are given in Table 4, with the extrapolated activity coefficient at infinite dilution. Extrap-olated activity coefficients at infinite dilution agreed well with directly measured values by differen-tial ebulliometry [14] or calculated values by UNIFAC equation [10]. The mean deviation, y means|yexperimental ycalculated|/N , and the parameters Aij for the Wilson, NRTL, and UNIQUAC equations are


Table 3Vaporliquid equilibria for MTBE systems with 1-propanol and 1-butanol at 313.15 K

P (kPa) x1 y1 P (kPa) x1 y1 P (kPa) x1 y1MTBE + 1-propanol

7.65 0.0078 0.1461 28.80 0.2476 0.8170 51.74 0.7994 0.95508.58 0.0159 0.2443 33.43 0.2980 0.8535 52.56 0.8384 0.95979.26 0.0219 0.3043 36.45 0.3506 0.8722 55.47 0.8890 0.9758

10.00 0.0280 0.3592 37.46 0.3998 0.8782 57.65 0.9473 0.986410.74 0.0351 0.4075 38.75 0.4419 0.8858 57.89 0.9559 0.987911.24 0.0422 0.4276 42.11 0.5222 0.9047 58.40 0.9669 0.991112.31 0.0489 0.4907 43.65 0.5699 0.9129 58.48 0.9723 0.991713.21 0.0568 0.5291 43.97 0.5826 0.9146 58.61 0.9749 0.992617.92 0.0972 0.6682 46.76 0.6453 0.9290 59.02 0.9858 0.995622.89 0.1491 0.7527 47.87 0.6832 0.9346 59.31 0.9922 0.997727.13 0.2013 0.8012 49.31 0.7365 0.9421 59.62 0.9987 0.9997

MTBE + 1-butanol3.19 0.0072 0.2455 24.55 0.2473 0.9229 51.83 0.7989 0.98484.48 0.0164 0.4689 27.84 0.2965 0.9354 53.49 0.8454 0.98754.62 0.0205 0.4851 29.62 0.3483 0.9413 55.35 0.8935 0.98975.59 0.0292 0.5784 33.09 0.3920 0.9511 54.98 0.9194 0.99046.59 0.0389 0.6459 36.50 0.4615 0.9589 57.49 0.9555 0.99546.89 0.0425 0.6624 38.74 0.5021 0.9636 57.96 0.9670 0.99647.28 0.0482 0.6816 44.25 0.5482 0.9727 58.22 0.9705 0.99698.15 0.0566 0.7182 43.99 0.5925 0.9723 58.46 0.9768 0.9974

13.07 0.1006 0.8330 46.09 0.6478 0.9757 58.96 0.9864 0.998517.17 0.1484 0.8786 47.92 0.6944 0.9785 59.17 0.9908 0.999021.14 0.1947 0.9061 49.70 0.7598 0.9814 59.56 0.9979 0.9998

expressed as

Wilson Aij = ij ii (cal/mol) (9)NRTL Aij = gij gii (cal/mol) (10)UNIQUAC Aij = uij uii (cal/mol) (11)

Table 4Fitted gE model parameters and mean deviations of the vapor phase mole fraction and the extrapolated activity coefficient atinfinite dilution

System gE model A12 A21 y 1 1 2 2

MTBE + methanol Wilson 375.56 1090.11 0.0050 3.114a 3.208b 3.526a 3.421bMTBE + ethanol NRTL 492.82 288.76 0.3 0.0068 2.677a 2.850b 3.097a 2.983bMTBE + 1-propanol UNIQUAC 769.76 283.93 0.0053 2.315a 2.304c 2.751a 2.912cMTBE + 1-butanol Wilson 272.90 958.50 0.0030 1.720a 1.940c 2.958a 2.529c

a Calculated values by extrapolation.b Unpublished data obtained by differential ebulliometry [14].c Calculated values by UNIFAC equation [10].


Fig. 2. Isobaric VLE data at 101.33 kPa and isothermal VLE data at 313.15 K for the systems of MTBE + n-alcohols(C1C4),(x: liquid phase, y: vapor phase).

All the measured VLE data were thermodynamically consistent by the RedlichKister integral method.Fig. 2 shows the isobaric VLE compositions for MTBE + methanol and MTBE + ethanol systems andisothermal VLE for MTBE+ 1-propanol and MTBE+ 1-butanol systems. Solid lines represent the datacalculated with the NRTL parameters for MTBE + ethanol system and with UNIQUAC parameters forMTBE+ 1-propanol system and with Wilson parameters for MTBE+methanol and MTBE+ 1-butanolsystems. The MTBE+methanol system has a minimum boiling azeotrope, while the other systems do notshow azeotropic behavior. As shown in the figure, MTBE+ 1-propanol and MTBE+ 1-butanol systemsshow relatively large positive deviations from Raoults law.

Table 5 gives the experimental HE data of butane+MTBE and isobutene+MTBE. They were smoothedby the least-square method to RedlichKister equation. Parts of these data were reported in the Inter-national Data Series [15]. Fig. 3 shows the excess molar enthalpies of these binaries. Continuous linesrepresent the calculated data by means of Eq. (5). The mixing enthalpies of butane+MTBE mixture showpositive values and are almost symmetric while the isobutene + MTBE mixture show negative valuesand the minimum is slightly shifted in the MTBE rich region. Table 6 shows the fitted parameters of the


Table 5Excess molar enthalpies of the butane+MTBE and isobutene+MTBE systems at 363.15 Kx1 HE (J/mol) x1 HE (J/mol) x1 HE (J/mol) x1 HE (J/mol)Butane + MTBE

0.0588 39.18 0.3370 165.63 0.6402 178.05 0.9143 63.270.1164 73.83 0.4415 185.66 0.7346 151.47 0.9143 63.090.1731 104.13 0.5425 191.61 0.8259 114.50 0.9575 32.820.2287 130.42 0.5425 190.31 0.8705 90.06 0.9894 8.19

Isobutene + MTBE0.0157 2.81 0.2398 41.13 0.5579 74.65 0.8346 57.090.0623 11.59 0.3510 56.05 0.6543 75.70 0.8773 47.160.1230 22.34 0.4569 68.18 0.7465 69.90 0.9191 34.000.1821 32.99 0.5579 75.47 0.7465 70.85 0.9600 18.11

Fig. 3. Excess molar enthalpies of the butane+MTBE and isobutene+MTBE systems at 363.15 K.

RedlichKister equation for each binary and S.D., related to Eq. (6), with the calculated partial excessmolar enthalpy at infinite dilution.

The volume changes of mixing of MTBE with C3C4 alcohols are given in Table 7 and the values offitted RedlichKister parameters Ai and S.D. are presented in Table 8 with the calculated partial excess

Table 6Fitted parameters, standard deviations (S.D.) and partial excess molar enthalpies at infinite dilution (J/mol) for the butane+MTBEand isobutene+MTBE systems at 363.15 KSystem A1 A2 A3 A4 A5 S.D. (J/mol) H E,1 H E,2Butane + MTBE 762.0684 45.6986 13.9318 10.5542 18.2889 0.8188 710.1727 822.6783Isobutene + MTBE 285.9552 142.7336 59.4911 12.4489 5.4356 0.4519 195.6994 506.0644


Table 7Excess molar volumes of the MTBE systems with C3C4 alcohols at 298.15 K

x1 VE (cm3/mol) x1 VE (cm3/mol) x1 VE (cm3/mol) x1 VE (cm3/mol)MTBE + 1-propanol

0.0246 0.0807 0.3006 0.5902 0.5503 0.7100 0.8001 0.50670.0636 0.1782 0.3481 0.6402 0.6008 0.7037 0.8486 0.40900.0993 0.2611 0.4067 0.6856 0.6500 0.6784 0.8903 0.32520.1493 0.3653 0.4507 0.7103 0.7009 0.6254 0.9343 0.22000.1994 0.4550 0.5030 0.7050 0.7366 0.5927 0.9747 0.10770.2482 0.5324

MTBE + 2-propanol0.0243 0.0378 0.2495 0.2201 0.4997 0.2929 0.7505 0.23090.0597 0.0768 0.3004 0.2480 0.5509 0.2911 0.7943 0.19760.0996 0.1160 0.3484 0.2681 0.5991 0.2727 0.8511 0.16090.1312 0.1408 0.4015 0.2722 0.6490 0.2657 0.8968 0.12630.1898 0.1824 0.4480 0.2804 0.7009 0.2522 0.9420 0.0889

MTBE + 1-butanol0.0208 0.0736 0.3002 0.6460 0.5535 0.7494 0.7997 0.58400.0717 0.2049 0.3685 0.7153 0.5977 0.7429 0.8516 0.48930.1004 0.2785 0.4031 0.7442 0.6485 0.7295 0.9004 0.37150.1497 0.3834 0.4490 0.7551 0.6948 0.6967 0.9325 0.28020.2005 0.4837 0.4962 0.7737 0.7479 0.6726 0.9808 0.10430.2507 0.5713

MTBE + 2-butanol0.0322 0.0530 0.3008 0.3243 0.5500 0.3732 0.7962 0.26700.0788 0.1214 0.3481 0.3362 0.5981 0.3700 0.8542 0.21490.1507 0.2094 0.4043 0.3629 0.6503 0.3596 0.9023 0.15470.2015 0.2429 0.4489 0.3762 0.6970 0.3379 0.9395 0.10820.2530 0.2844 0.4994 0.3706 0.7499 0.2929

molar volume at infinite dilution. Fig. 4 shows the fitted VE curves, together with the experimental points.In all the systems, measured VE appear to be negative over the entire range of MTBE concentration.The curves are approximately symmetric with a minimum at a mole fraction at about 0.5. The negativedeviations from the linear volumetric behavior are assumed to be caused by strong hydrogen bonding orthe different molecular sizes.

Table 8Fitted parameters, standard deviations (S.D.) and partial excess molar volumes at infinite dilution (cm3/mol) for the MTBEsystems at 298.15 K

System A1 A2 A3 A4 A5 S.D. (cm3/mol) V E,1 V E,2MTBE + 1-propanol 2.8648 0.1977 0.1925 0.1433 0.4748 0.0068 3.1911 3.8731MTBE + 2-propanol 1.1600 0.0101 0.0134 0.0839 0.4340 0.0048 1.5134 1.7014MTBE + 1-butanol 3.0653 0.1687 0.7008 0.8906 0.2977 0.0097 3.0045 5.1231MTBE + 2-butanol 1.5100 0.0916 0.1570 0.0165 0.2490 0.0054 1.8409 1.9911


Fig. 4. Excess molar volumes of the MTBE systems with C3C4 alcohols at 298.15 K.

4. Conclusion

Isobaric or isothermal VLE for systems of MTBE+C1C4 alcohols were measured and correlated. Thenon-ideality was decreased with increasing carbon number of alcohols wheres the MTBE+methanol sys-tem shows azeotropic behavior. Extrapolated infinitely dilute activity coefficients were relatively agreedwell with measured or estimated values by UNIFAC equation. Mixing process of butane+MTBE systemwas endothermic while that of isobutene + MTBE system was exothermic. Excess molar volumes ofMTBE+C3C4 alcohol systems show negative deviation from the ideality because of hydrogen bondingof alcohols. Partial excess molar properties at infinite dilution were also successively calculated using thecorrelated RedlichKister.

List of symbolsA, B, C Antoine constantsAi parameter in the smoothing equationAij parameter used in Margules, van Laar, Wilson, NRTL, UNIQUAC equationgij interaction energy in the NRTL equationHE excess molar enthalpy (J/mol)ME excess molar propertyMi molecular weight of component in number of parameters AiN number of experimental valuesP total pressure (kPa)P si vapor pressure of pure component i (kPa)S.D. standard deviationuij interaction energy in the UNIQUAC equation


VE excess molar volume (cm3/mol)xi liquid phase mole fraction of component iyi vapor phase mole fraction of component i

Greek letters non-randomness parameter in the NRTL equation i activity coefficient of component iij interaction energy in the Wilson equation (cal/mol)i density of component i (g/cm3)m density of the binary mixture (g/cm3)

Acknowledgements

This work was supported by grant no. 2000-1-30700-011-2 from the Basic Research Program of theKorea Science & Engineering Foundation.

References

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Vapor-liquid equilibria and excess properties for methyl tert-butyl ether (MTBE) containing binary systemsIntroductionExperimentalMaterialsVLE measurementExcess molar enthalpy measurementExcess molar volume measurementCalculation of the thermodynamic properties at infinite dilution

Results and discussionConclusionAcknowledgementsReferences

Documents

Vapor–liquid equilibria and excess properties for methyl tert-butyl ether (MTBE) containing binary systems