Volume 1 No.

2, August 2011

International Journal of Science and Technology

©2010-11 IJST Journal. All rights reserved http://www.ejournalofsciences.org

A Volumetric and Viscosity Study for the Binary Mixtures of Dimethylsulfoxide with Benzene, Ethyl benzene, Chlorobenzene and Bromobenzene at Temperatures of (303.15, 308.15 and 313.15) K and a Pressure of 0.1MPa
1

S. Parthasarathi, K.Saravanakuamr, 3R.Baskaran ,4T.R. Kubendran

2

1,4

Department of Chemical Engineering, Alagappa College of Technology, Anna University, Chennai-600025, India. 2 Department of Chemical Engineering, Sathyabama University, Chennai-600119. India. 3 Department of Chemical Engineering, St.Joseph’s College of Engineering, Chennai-119. India.

ABSTRACT
Viscosities () and densities () of binary mixtures of dimethylsulfoxide with benzene, ethylbenzene, chlorobenzene and bromobenzene have been measured as a function of mole fraction at atmospheric pressure and at different temperatures of (303.15, 308.15, and 313.15) K. Using the experimental data, excess volumes (VE) and deviations in viscosity () have been calculated. McAllister's three-body-interaction model, Krishnan and Laddha model and Jouyban Acree model were used to correlate the kinematic viscosity of the systems. The excess volume data was fitted by means of the Redlich-Kister equation. It was found that in all cases the experimental data obtained fitted with the values correlated by the corresponding model very well.
Keywords: Viscosity; Density; Molecular Interactions; Deviations; Binary Mixture

1. INTRODUCTION
Binary liquid mixtures due to their unusual behavior have attracted considerable attention [1]. In chemical process industries materials are normally handled in fluid form and as a consequence, the physical, chemical, and transport properties of fluids assume importance. Thus data on some of the properties associated with the liquids and liquid mixtures like density and viscosity find extensive application in solution theory and molecular dynamics [2]. Such results are necessary for interpretation of data obtained from thermo chemical, electrochemical, biochemical and kinetic studies [3]. Dimethylsulfoxide is used as an Anti-inflammatory agent and analgesic. Dimethylsulfoxide + benzene mixture is used as insecticides, pesticides and comprising gel formations for vapor producing systems. Dimethylsulfoxide + ethylbenzene, chlorobenzene, bromobenzene mixture is used in dyes, pigments, perfume and pharmaceutical industry. The present study is a continuation of our earlier studies [4, 5] on understanding the thermodynamic properties of binary mixtures whose component has relevant industrial applications. In the present paper, we have re-ported density (ρ) and viscosity (η) of pure dimethylsulfoxide and benzene, ethylbenzene, chlorobenzene and bromobenzene as well as for the binary system constituted by these two chemicals at temperatures of 303.15 K, 308.15 K and 313.15 K. The viscosity values have been fitted to McAllister [6] model and Krishnan and Laddha [7] model. The Jouyban –Acree model [8] has also been extended to density and viscosity of binary mixtures. The deviation values have been fitted to Redlich-Kister type [9] equation. Literature survey showed that no measurements have been previously reported for the

mixture studied in this paper.

2. MATERIALS AND METHOD 2.1 Materials
The chemicals used were of analytical reagent grade obtained from lobo chemicals and purified by standard procedures [10]. All the components were dried over anhydrous calcium chloride and fractionally distilled [11]. Binary solutions were prepared on percentage basis (v/v) by dissolving known volume of dimethylsulfoxide in appropriate volume of benzene, ethylbenzene, chlorobenzene and bromobenzene and measuring their masses on a Shimadzu Corporation Japan Type BL 2205 electronic balance with an uncertainty of 0.01%. All the measurements described below were per-formed at least three times and the results were averaged to give the final values.

2.2 Apparatus and Procedure
Densities were determined by using a 25 cm3 bicapillary pycnometer and calibrated with deionized double distilled water with a density of 996.0 kg ·m-3 at a temperature of 303.15 K. The pycnometer was thermostatted in a transparent walled water bath (maintained constant to ± 0.01 K) for 15 min to attain thermal equilibrium and the liquid level in the two arms was obtained with a traveling microscope which could read to 0.01 mm. The Kinematic viscosities were measured at the desired temperature using Ostwald viscometer. The 96

2. 308. and n is the number of coefficients.ejournalofsciences. All rights reserved http://www. (2) Accommodation of molecules 97 . If the factors dominate the contraction factors. the VE becomes positive. ethylbenzene chlorobenzene and bromobenzene at temperatures of (303. 3. The sign of excess volume of a system depends on the relative magnitude of expansion/contraction on (4) causing expansion mixing of two liquids. After the mixture had attained bath temperature (Technico India. ethylbenzene.T =f1 ln y1+f2 ln y2 + f lf2 [AJ (f1-f2)J ⁄ T] (6) Where Ym. The excess molar volume and viscosity deviations were fitted to a Redlich. M1 and M2 refer to the molecular weight of the two components respectively. Coefficients Ai were obtained by fitting equation (7) to experimental results using a least square regression method. RESULTS AND DISCUSSION Measured values of densities and viscosities of dimethylsulfoxide with benzene. AJ is the model constant.8. which gives: ln  = x1 ln 1+x2 ln 2 + x1 ln M1+x2 ln M2+ln(x1M1+x2M22.15) K are represented in figures. 2.15. but for the other binary mixtures containing ethylbenzene. 1.01sec. The excess molar volume of dimethylsulfoxide with benzene is positive (12. (3) Steric hindrance. Madras).15 and 313. and 323. chlorobenzene and bromobenzene at (303. In the calculation of viscosity.)) (5) where B and C are interaction parameters. then VE become negative. 313. the optimum number of coefficients is ascertained from an examination of the variation in standard deviation(S) was calculated using the relation S(Y) = [(Aexp-Acal)2/(N-n)]1/2 (8) where . The calculated values of coefficients (Ai) along with the standard deviations (S) are given in table. which does not allow fitting of one component into other component.0001. On the other hand if the contraction factors dominate the expansion factors. two constants a and b of the viscometer in the relation ν = (at) – (b/t) (1) The kinematic viscosity was correlated by means of the Krishnan and Laddha model for a two component mixture. The flow measurements were made with an electronic stopwatch with a precision of 0. The values of the parameters are given in Table-6. which for two-component mixtures gives lnν = x13 lnν1 + 3x12 x2 lnν12 + 3x1 x22 lnν21+ x23 lnν2− ln(x1+ x2 M 2 / M1)+ 3x12 x2 ln((2 + M 2 / M1 ) / 3) + x23 ln(M 2/ M1) +3x1 x22 ln((1+ 2M 2 / M1 ) / 3) (4) where  refers to the kinematic viscosity of the mixture of components 1 and 2 having mole fractions x 1 and x2 respectively 1 and 2 refers to the kinematic viscosity of pure liquids 1 and 2 respectively 12 and 21 represent the interaction parameters obtained by multiple regression analysis. The values of the parameters and standard deviations are given in Table-7. and m refer to the density of components 1 and 2 and the density of the mixture. ln Ym.Volume 1 No.15) K are listed in Table 2-5. The variation of excess volumes with the mole fraction of dimethylsulfoxide with benzene. The density values have been used to calculate excess molar volumes VE using the following equation VE=(x1M1+x2M2) ⁄ m-(x1M1/1+ 2M2 ⁄ 2) (2) where x1 and x2 refer to the mole fraction of components 1 and 2. and y2. flow time has been measured. respectively. The negative VE values arise due to dominance of the following factors. (1) Loss of dipolar association (2) The geometry of molecular structure.org viscometer was calibrated using water.9.T.15.15. In each case. 1..The viscosity deviations  were calculated from the viscosity values using =-(x11+x22) (3) Where Y is either VE or  and n is the degree of polynomial. Jouyban et. (1) Chemical interaction between constituent chemicals.. The liquid mixture was charged into the viscometer. The kinematic viscosities were correlated by means of the McAllister model considering a three-bodyinteraction model. The values of the parameters and standard deviations are given in Table. respectively.T. chlorobenzene and bromobenzene is negative over the whole range of mole fraction. The factors that are responsible for expansion in volume are as follows.1-4.30x1x2(B+C(x1-x2). y1.Kister equation of the type Y= x1x2 Ai(x1-x2)i (7) It is obtained by measuring the flow time with high purity benzene at the working temperature. (1) and constants were determined. 13). and 2 are the viscosity of the mixture and the viscosity of pure components 1 and 2.T are the viscosity of the mixture and solvents 1 and 2 at temperature T. The calculated viscosities were fitted in Eq. respectively. where N is the number of data points. al proposed a model for correlating the thermal properties of liquid mixtures at various temperatures. The uncertainty in the calculation of VE from density measurements was estimated to be ±0. August 2011 International Journal of Science and Technology ©2010-11 IJST Journal. which opposes the proximity of the constituent molecules.

8272 0.15) K and 0.15K 1.3279 1.5983 4.5810 308.0873 1.0436 1.7824 1.1 MPa x2 η/ (mPa·s 3 ) 303.15K as displayed in figure 5-8 show negative deviations (14) over the entire range of mole fraction.9514 0.1076 0. chlorobenzene and bromobenzene system were found out as a function of mole fraction at atmospheric pressure and at temperatures of 303.7666 1.9784 1.0105 1.2227 0.9560 1.1003 0.0811 1.1015 0.15K.5457 1. (3) Geometry of the molecular structure that favors fitting of the component molecules with each other.3620 1.1 MPa x2 ρ/ g ·cmη/ (mPa·s) ρ/ g ·cm-3.1537 1.0989 1.6364 0.7824 1.1100 0.8480 1 303.0731 1.0477 1. η/ (mPa·s) ρ/ g ·cm3 3 η/ (mPa.0580 1. 308.15K. ethylbenzene.0828 1.0721 0.9720 0.5704 0.8665 1.8311 0.9359 0.4136 1. 308.15.1053 1.0520 1.3327 1.8629 0.15.1064 1.8520 0.0948 1.15K.8406 0.0464 0.Volume 1 No.7620 0. All rights reserved http://www.1011 1.0234 1.9796 0.4118 0. and 313.3668 0. The excess molar volume and viscosity deviation data were fitted by means of the Redlich-Kister equation.0604 0.1088 0.5621 1.0124 1.1989 0.0230 1.9003 0.15K 1.9091 0.15.5122 0.15K.8691 0.8755 1.1036 1. and 313.0261 1.2098 0.8630 1 303.8828 0.9609 0.6986 0.6203 0.6390 98 . which is related with liquid’s structure and enthalpy.5770 0.4018 1.5412 1.0013 1.15 K 1.2382 1.5810 0. 308. Consequently with the molecular interactions between the components of the mixtures.1040 0.1100 1.0913 0.1095 1.9427 0.15K 1.1689 1.0639 1.9570 0.7050 308.1009 1. Table-2: Densities ρ and viscosities η for the dimethylsulfoxide (1) + benzene (2) mixture at T= (303.7050 0.2513 1. ) 313.4709 1.0899 1.5748 0.9199 0.1230 0. 308.9242 0.5329 1.15K.0928 1.0603 1.5827 1.7368 0.9206 0.8672 0.15K 1.7409 0. Therefore the viscosity deviation depends on molecular interactions as well as on the size and shape of the molecules.5890 0.9652 1.7484 0. and 313.5631 ρ/ η/ g (mPa·s ·cm-3.1604 0. the values of excess molar volumes (VE) and the viscosity deviations () were determined at 303. The results of variation in viscosity deviations of binary systems consisting of dimethylsulfoxide with benzene.7119 0.5412 1.0899 1. Table-3: Densities ρ and viscosities η for the dimethylsulfoxide (1) + ethylbenzene(2) mixture at T= (303.1005 0.9716 1.15 K 1. Table 1: Comparison of experimental density and viscosity of pure liquids with literature values at 303.2786 0.9348 0.5630 0.0811 1.5288 0 0.8672 0.0427 1. matches with the McAllister model and Redlich-Kister equation with a high degree of precision.6648 1.1080 0.7053 0 0.9704 0.9988 1.0899 0.0813 0.6648 1.8527 0.1034 0.4434 0.1063 1.0629 1. CONCLUSIONS Viscosities () and Densities () for the binary liquid mixture of dimethylsulfoxide with benzene.1 MPa x2 ρ / g ·cm-3 η/ (mPa·s) ρ/ g ·cm-3 η/ (mPa·s) ρ/ η/ g (mPa.9017 0. and 313.8238 1.7476 0.8390 0. η/ (mPa· s) 308.5486 0 0. Excess molar volumes (VE) and the viscosity deviations () were used to predict the intermolecular interactions in the mixtures.7608 0.6843 1. lit Exp 1.15) K and 0.8910 0.15K 1.0731 1.15K 1. KrishnanLaddha model and Jouyban-Acree model were used to correlate the kinematic viscosity of the systems.1378 1.7076 0.1105 1.1002 0.7960 1.8740 0.0219 0.0811 1.6720 0.4077 1.1042 1.1446 0.7880(16) 0.0962 1.4736 1.8997 0. 308.8682 0.8975 0.0644 0. 308.15.8544 0.15 K 1.9481 0.0619 1.0303 1.1839 0.5412 1.9437 0.0905(16) 0.2435 1. The viscosity of the mixture strongly depends on the entropy of mixture.org of one component into the interstitials of the molecules of the other component.2953 1.9751 1.s) lit η/(mPa · s) Exp 1.7163 1.3182 0.8471 0.0924 1.2752 1.0020 1.0431 1.9784 0. McAllister's three-body-interaction model.8391 1 ACKNOWLEDGEMENT The authors thank the University authorities for providing the necessary facilities to carry out the work.15) K and 0.0564 0.0006 1.6761 0.7824 0.s) ·cm-3 313. 2.15.8513 1.4239 1.15K.3683 1.6637 313.6648 1.1000 (17) (5) (4) Table-4: Densities ρ and viscosities η for the dimethylsulfoxide (1) +chlorobenzene (2) mixture at T= (303.0731 1.0712 1.8670 1.1265 0.5890 ρ/ g ·cmρ/ g ·cm-3.0989 0.9215 0.0985 1. From the density () and viscosity () data.7050 (17) (5) (4) 1.0337 1.1681 0. August 2011 International Journal of Science and Technology ©2010-11 IJST Journal.0221 1.3234 0.3014 0.3790 1.8601 0.2179 1. It was found that in all cases the experimental data obtained. and 313.2308 0.15K.9957 0.3344 1.ejournalofsciences.15 K Pure liquids Dimethylsulfoxide Benzene Ethylbenzene Chlorobenzene ρ / g ·cm-3. The negative VE values in the mixtures under study indicate that interactions between molecules of the mixtures are stronger than interactions between molecules in the pure liquids and that associative force dominate the behavior of the solution.6300 1.7824 1.1489 0.9361 1.0953 0.7585 0.0417 1.5811 1.15.4832 1.8788 0. ethylbenzene.15K.6428 0.8799 0.8513 0.0899 1.6313 0.9863 0. and 313.9453 0.9619 0.0922 1.4650 0.4824 1.9886 1.0354 1. chlorobenzene and bromobenzene at temperatures of 303.

15 308.87 52.15 0.Parameters of the Redlich Kister constants and standard deviations S for viscosity Deviation T /K 303.3085 1.15 303. Densities ρ and viscosities η for the dimethylsulfoxide (1) + bromobenzene (2) mixture at T= (303.5639 1.599 -26.3409 0.4493 η/ mPa·s 1.188 0.2417 1.9260 ρ/ g ·cm-3 1.0038 0.0287 -1.3039 -0.2 0.24 201.0353 Dimethylsulfoxide(1) +Chlorobenzene(2) 303.7431 1.194 0.4033 0.4205 1.9443 0.2987 1. 99 .906 Dimethylsulfoxide(1) +Bromobenzene(2) 178.5 0 0 0.0159 308.4823 Dimethylsulfoxide(1) +Chlorobenzene(2) -177.8762 0.9389 0.0025 0.8588 1 308.0747 0.0687 0.15 313.3578 1.66 35.0974 -0.7 -46.15 313. Parameters of the Jouyban Acree model Constants and standard deviations S for the viscosity T /K 303.5412 1.0087 0.1703 -0.15 0.4551 1.15 313.15 303.0186 -0.1205 1.1227 0.9078 0.9097 0.1169 0. 313.4135 -0.294 -12.8600 -0.1491 0.0975 -1.8.6648 1.1 MPa x2 ρ/ g ·cm-3 1.15 308.949 -74.1309 -1.15K Table.0.0511 0.5034 0.547 18.4011 1.24 -52.2554 1.0353 308.624 -89.15 303.78 -190. August 2011 International Journal of Science and Technology ©2010-11 IJST Journal.776 35.0184 0.9079 Table.3383 1.3551 1.0633 -0.7 Parameters of the Krishnan and Laddha Constants and standard deviations S T/K 303.65 -153.32 -145.15 A4 A1 A2 A3 Dimethylsulfoxide(1) + Benzene(2) 210. ■.15 303.8209 0.4024 0.23 146.1262 1.3781 -0.411 194.521 Dimethylsulfoxide(1) +Bromobenzene(2) .0159 FIGURES 3 2.1222 -01250 0.4091 0.9502 0.0095 0.1059 84.9146 0. 2.8566 1.0176 0.1151 1.661 -0.15 313.0. 308.1345 1.9942 0.2478 -0.0811 1.4401 0.0276 .4931 1.569 -76.2672 1. and 313.8154 -0.15 0.677 16.339 -219.7470 2.15 308.3135 1.3406 S 0.1035 -0.15 K 0 0.1076 -0.6556 0.848 -10.3558 1.1401 Dimethylsulfoxide(1) + Ethylbenzene(2) 0.1518 0.0293 0.064 -15.0065 0.0748 -5.15 308.065 10.275 -9.7121 1.15 308.176 Dimethylsulfoxide(1) +Bromobenzene(2) -0.1009 0.1185 -0.1753 0.327 227.0514 0.63 -22.0164 313.15 0.710 160.2202 1.0669 2.0899 1. Excess molar volume (VE) for dimethylsulfoxide(1)+benzene(2) at ♦.15 A2 A3 A4 A5 Dimethylsulfoxide(1) + Benzene(2) -1.11 8.0698 0.15 308.8241 0.870 Dimethylsulfoxide(1) + Ethylbenzene(2) 269.15.0070 0.15 0.8139 1.15 0.0047 313.3029 -0.2 -59.388 -0.1485 Dimethylsulfoxide(1) +Chlorobenzene(2) -0.15 303.0731 1.1796 0.5935 1.15 308.4747 0.9573 0. 1.0.4267 η/ mPa.0616 1.3513 1.1628 0.1745 1.0913 -0.7303 -0.8631 0.1675 Dimethylsulfoxide(1) +Chlorobenzene(2) -0.15 313.0122 0.0665 Table.1316 .15 K 0.1366 -0.185 0.4240 1.4862 η/ mPa·s 1.1.8961 -1.15 308.1374 0.0079 0.515 -231.0151 0.7391 Dimethylsulfoxide(1) + Ethylbenzene(2) -0.195 1.3106 0.6801 -0.0.15 0.0204 0.3906 1.15 308. ▲.7517 0.6706 0.026 0.15 308.0031 0.0062 0.4 X2 303.0286 -0.0439 0.5243 0.3029 -0.2021 0.2491 -0.1106 0.2 0.6 Parameters of McAllister constants and standard deviations S T /K A B S Dimethylsulfoxide(1) + Benzene(2) 303.15 313.15.3082 1.0021 Dimethylsulfoxide(1) +Bromobenzene(2) 303.0083 0.15 308.3781 -0.2491 1.1174 -0.7100 1.0624 -0.15 308.394 -13.1314 1.0654 0.0257 313.0869 0.5 1 0.ejournalofsciences.717 S 0.9621 0.15 313.4294 1.835 -170.414 -26.278 -0.175 -0.1883 -0.0039 0.org Table-5.9319 0.0122 0.15 303.2631 1.2776 1.2688 -0.15 313.36 -56.3783 0.224 47.1445 0.2870 -1.15 303.0188 0.15 k.7229 0.6706 0.3718 1.15 303.6482 0.5789 0.7342 -0.7431 .6331 1.Volume 1 No.0575 0.6120 0.15 0.1689 1.0118 0.15 308.6273 0.48 -32.2112 -0.8 1 Figure.15 313.15 K 308.1817 .15 313.2246 0.19 53.0545 0.15 0.7517 0.3236 1.1905 0.0165 0.3880 -0.15 A1 A2 A3 A4 Dimethylsulfoxide(1) + Benzene(2) 0.1521 -.015 0.15 k.0331 0.2210 -1.6 0.1227 ρ/ g ·cm-3.1589 -0.8144 142.2 -6.15 k.1856 1.0566 0.5 V E cm 3 mol -1 2 1.0106 -0.3847 1.4345 1.7824 1.15 313.0626 0.2455 .0532 0.3154 1.15 313. 303.2123 1.0235 Dimethylsulfoxide(1) + Ethylbenzene(2) 303.024 0.2873 1.0069 303.3881 0.8552 0.15 0. All rights reserved http://www.3222 0.0081 0.0034 0.0438 0.5127 1.579 -118.8924 0.2299 .3820 1.5664 1.15 303.561 165.0655 0.27 218.514 A1 S 0.037 0.0071 0.15 313.s 1.4527 1.15) K and 0.2009 1.15K 313.0.6731 0.7875 0.2041 1.4094 1.2481 1.0082 308.7300 0.15 K 313.28 276.9319 0.0022 0.0416 -0.0.0034 Table.3783 0.1614 1.1091 .0.1737 1. 308.9.0555 -0.1885 0.837 99.

6 0.15 k.6 0. 313.5 V E cm 3 mol -1 0 0 0.15 k. 303.s) 0.2 -1.15 k. 303.6 -0.15 k. 0 0 -0.2 0.8 1 Figure. 313.4 X2 -0.15 K 308.15 k.6 0.08 -0.15 K 308. 313. 303.12 303.et al.15 K 308.15 K Figure. August 2011 International Journal of Science and Technology ©2010-11 IJST Journal.02 0 Δη/ /(mPa. ■. ■.15 k.ejournalofsciences.3 X2 Figure.15 k.8 1 -2.4 0.2 0. .4 0. 308.75 V E cm 3 mol -1 X2 0.15 k. REFERENCES [1] [2] Ewing.Volume 1 No.15 k.15 K 313. ▲.. Viscosity deviation (∆η) for dimethylsulfoxide(1)+ethyl benzene(2) at ♦.8. ▲. ■.15 k. ■.et al.4 0. 308.s) -0. 0 0 303. Journal of Chemical Thermodynamics.15 K Figure.04 -0. 308. Viscosity deviation (∆η) for dimethylsulfoxide(1)+benzene(2) at ♦.15K 313.8 1 Δη/ /(mPa. M. ■.5 -2 -2. ▲.15 k.12 303. Fluid Phase Equilibria.15 k.15 K 308.15 K 313.25 0 -0.06 -0.15 K 313. 2.7. 313. ■.15 K 313.5. 308.B.15 -0. 0 -0.2 -0. ▲.2 -0.8 1 Figure.org 0 -0.6 0.15 K -1.15 K 313.4 303.8 -1 -1.04 -0. 313.15 K 308.4: Excess molar volume(VE) for dimethylsulfoxide(1)+bromobenzene(2) at ♦. 308. Viscosity Deviation (∆η) for Dimethyl sulfoxide(1)+ Chlorobenzene(2) at ♦. 100 Figure. -0.2 0.1970.15 k.15 K X2 -1.224.15 k.15 K 303. Viscosity deviation (∆η) for dimethylsulfoxide(1)+bromobenzene(2) at ♦.1 -0.25 0.15 k.4 0. 303. X2 Figure.08 -0. 303.2.15 k. 313.4 0. All rights reserved http://www.s) -1.75 Δη/ /(mPa.6. 157P.8 1 -1 303. 308.6 0.05 0 -0.8 1 V E cm 3 mol -1 -0. ▲. ▲. 308. Mchaweh A.25 -2. 313.6 0. ▲.75 -0.15 k.2.2 0.15 K 0.3: Excess molar volume (VE) for dimethylsulfoxide(1)+chlorobenzene(2) at ♦.1 -0. 303.15 k.2 0.15 K 308. 303. Excess molar volume (VE) for dimethylsulfoxide(1)+ethylbenzene(2) at ♦.15 k.2 0.15 k.15 k.689p.25 0.5 X2 -0.4 0. 2004. ■.

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