Indian Journal of Pure & Applied Physics

Vol. 46, August 2008, pp. 545-551

Experimental and predicted viscosities of binary mixtures of benzene and

chloroalkanes at different temperatures using Isdale’s group contribution method
Anwar Ali*a, Mohammad Tariqb & Firdosa Nabia
a
Department of Chemistry, Jamia Millia Islamia (Central University), New Delhi 110 025
b
Laoboratory of Molecular Thermodynamics;
Instituto de Tecnologia Quimicae Biologia, Universidade de Nova De Lisboa, Oeiras, Portugal
Received 7 November 2007; revised 23 April 2008; accepted 15 May 2008
Experimental viscosities, η of pure benzene, 1,2-dichloroethane (DCE), 1,1,2,2-tetrachloroethane (TCE) and those of
their binary mixtures, having benzene as a common component, have been measured over the whole composition range at
298.15, 303.15, 308.15, 313.15 and 318.15 K. The experimental η data were then fitted to standard polynomial against
composition. Using η values, the deviations in viscosities, ∆η , excess Gibbs free energies of activation of viscous flow,
∆G*E, entropies, ∆S* and enthalpies, ∆H* of activation of viscous flow have been calculated. The sign and magnitude of
these parameters were found to be sensitive towards interactions prevailing in the studied systems. Further, the excess molar
volumes, VE were calculated using data for both the binary mixtures. Moreover, Grunberg–Nissan and Isdale’s group
contribution methods have been used to calculate the viscosities of mixtures and the results were discussed in terms of
average percentage deviations (APD) in experimentally and theoretically calculated viscosities.
Keywords: Viscosities, Interactions, Liquid mixtures, Correlations, Group contribution

1 Introduction 2 Experimental Details

Viscosity is the ratio of tangential stress and velocity
gradient and provides a measure of the internal friction
of a fluid. It is an important non-equilibrium transport
property closely related to self-aggregation in liquids1.
Viscosity data provide a valuable insight into the
structure and interactions in mixed solvents and are
needed to evaluate mass transport and heat transfer,
among others2,3. These considerations led us to
undertake the present study in continuation to our
research programme on the thermodynamic behaviour
of binary liquid mixtures4-6.
Benzene is a versatile compound and widely used
in chemical and technological processes. Benzene is a
non-polar and unassociated liquid, whereas DCE and
TCE are polar but practically unassociated7,8.
Therefore, interesting results may be obtained
regarding the molecular interactions between the
unlike molecules in these binary mixtures.
Using the experimental data, ∆η, ∆G*E, ∆S* and
∆H * have been calculated. An attempt has also been
made to calculate excess molar volumes, VE using
∆ η data. Further, the Grunberg-Nissan9 and Isdale’s
group contribution10 methods have been used to
obtain viscosities of binary mixtures theoretically.
_________________________
*E–mail: anwar_jmi@yahoo.co.in
The chemicals used in the present study were of
AR grade. Benzene (E. Merck, Germany), DCE and
TCE (Qualigens Fine Chemicals, India) were purified
by the methods described in the literature11,12. Before
use, the chemicals were stored over 0.4 nm molecular
sieves to reduce water content, if any. Mixtures were
prepared by mass using a Precisa XB-220 A (Swiss
make) electronic balance with a precision of ± 0.1 mg.
The densities of the pure liquids and their mixtures
were measured pycnometrically as reported
previously in the literature4. Viscosities were
determined with an Ubbelohde type suspended level
viscometer, thermostated in an electronically
controlled water bath (Julabo, Germany), with a
temperature stability of ± 0.02 K, for about 30 min so
that the thermal fluctuation in the viscosity was
minimized. The uncertainties in the measured
viscosities were not more than ± 2⋅10-3 mPa.s. The
observed viscosities of pure benzene, DCE and TCE
at 298.15 K are 0.6080, 0.7790 and 1.4388 mPa.s,
respectively, which compare well with the literature
values 0.6038(Ref.13)/0.6025(Ref.14), 0.7790 (Ref.15)
and 1.4560 (Ref.12)/1.4554 (Ref.16), respectively.
3 Results and Discussion
The experimental values of viscosities, η of pure
benzene, DCE and TCE and those of their binary
546 INDIAN J PURE & APPL PHYS, VOL 46, AUGUST 2008

mixtures over the entire composition range expressed ∆G *E were calculated by using the standard relations2
as a function of mole fraction, x1 of benzene at and were smoothed by Redlich-Kister polynomial19.
different temperatures ,are presented in Table 1. The The values of coefficients Ai of the polynomial19
dependence of η of the mixtures on x1 has been
together with the standard deviations σ (Y E ) are
established using a polynomial equation of the form:
given in Table 3. The variations of experimental and
calculated values, using Redlich-Kister polynomial19
4
η = ∑ηi x1i … (1) of ∆η and ∆G *E with mole fraction x1 of benzene are
i=0 graphically presented in Figs 1–4, respectively.
From Figs 1 and 2, it is clear that the ∆η values are
The coefficients ηi of Eq. (1) along with the standard negative over the whole composition range of both
deviations σ (η ) at each investigated temperature are the systems investigated at each temperature.
presented in Table 2. The significance of data fitting Negative deviations in viscosity occur where
using similar polynomial equations have also been dispersion or weak dipole-dipole forces are primarily
reported by others17,18. The values of ∆η and responsible for the interaction between component
molecules20,21. Negative ∆η values may also be
Table 1—Values of experimental viscosities of binary liquid
observed due to the difference in the molecular size of
mixtures at different temperatures the component molecules22,23. The magnitude of ∆η
values (Figs 1 and 2) follows the sequence: DCE >
x1 298.15 303.15 308.15 313.15 318.15
TCE. This is also the sequence in the difference in the
η (mPa.s) molar volume of benzene and chloroalkanes in the
Benzene + DCE present study. Furthermore, the ∆η values become
0.0000 0.7790 0.7350 0.7010 0.6741 0.6311 more negative as the temperature of the mixture
0.1028 0.7503 0.7041 0.6671 0.6355 0.5902 increases, i.e., the system shows non-ideal behaviour
0.1899 0.7229 0.6765 0.6396 0.6067 0.5634
with rise in temperature. This suggests that the
interactions between molecules become weaker as a
0.2975 0.6929 0.6465 0.6105 0.5776 0.5359
consequence of rise in temperature.
0.3910 0.6695 0.6225 0.5867 0.5541 0.5138 The variation of the excess Gibbs free energy of
0.5003 0.6431 0.5955 0.5615 0.5291 0.4901 activation of viscous flow, ∆G *E with mole fraction,
0.6019 0.6246 0.5775 0.5433 0.5105 0.4725 x1 of benzene for both the binary mixtures at different
0.7018 0.6115 0.5637 0.5305 0.4965 0.4594
0.8006 0.6041 0.5555 0.5218 0.4872 0.4509 Table 2—Coefficients of viscosities fitted to the polynomial (1)
against composition at different temperatures
0.8955 0.6015 0.5535 0.5205 0.4845 0.4492
1.0000 0.6080 0.5630 0.5330 0.5011 0.4711 T/K η0 η1 η2 η3 η4 σ (η)
Benzene + TCE Benzene + DCE
0.0000 1.4388 1.4302 1.3607 1.2258 1.0891 298.15 0.7793 -0.2860 -0.0777 0.2358 -0.0437 0.0008
0.1222 1.3256 1.3096 1.2422 1.1168 0.9902 303.15 0.7353 -0.3149 0.0345 0.0554 0.0524 0.0008
0.1956 1.2588 1.2392 1.1756 1.0585 0.9401 308.15 0.7012 -0.3579 0.2225 -0.2152 0.1819 0.0008
0.3028 1.1676 1.1451 1.0851 0.9794 0.8726 313.15 0.6744 -0.4298 0.5000 -0.6259 0.3817 0.0012
0.3862 1.1000 1.0742 1.0173 0.9199 0.8222 318.15 0.6312 -0.4595 0.6907 -0.9300 0.5380 0.0014
0.4960 1.0105 0.9814 0.9285 0.8426 0.7567 Benzene + TCE
0.5936 0.9315 0.8985 0.8504 0.7746 0.6992 298.15 1.4390 -0.9730 0.3397 -0.2904 0.0927 0.0007
0.6890 0.8557 0.8188 0.7742 0.7076 0.6425 303.15 1.4303 -1.0453 0.4689 -0.4689 0.1783 0.0009
0.8079 0.7611 0.7207 0.6807 0.6268 0.5747 308.15 1.3606 -1.0291 0.5458 -0.5738 0.2298 0.0006
0.9020 0.6861 0.6434 0.6082 0.5642 0.5222 313.15 1.2255 -0.9567 0.6702 -0.7613 0.3237 0.0006
1.0000 0.6080 0.5630 0.5330 0.5011 0.4711 318.15 1.0887 -0.8804 0.7845 -0.9203 0.3990 0.0008
 ALI et al.: VISCOSITIES OF BINARY MIXTURES 547

Table 3—Coefficients of Redlich-Kister equation for the binary liquid mixtures along with standard deviations at different temperatures

T/K A1 A2 A3 A4 A5 σ(YE)
Benzene + DCE
∆ η (mPa.s)
298.15 -0.1999 0.0682 0.0210 0.0331 -0.0092 0.0003
303.15 -0.2114 0.0714 0.0236 0.0383 -0.0552 0.0005
308.15 -0.2215 0.0640 0.0084 0.0414 -0.0875 0.0000
313.15 -0.2333 0.0544 -0.0343 0.0605 -0.1097 0.0001
318.15 -0.2435 0.0599 -0.0458 0.0539 -0.1691 0.0001
∆G*E (kJmol-1)
298.15 -620.7228 354.7228 52.3982 82.4031 -42.2639 1.2790
303.15 -719.2885 413.1853 73.2461 128.8229 -235.4530 1.9354
308.15 -814.6482 420.8769 23.4260 176.9581 -391.0945 0.3964
313.15 -916.9812 427.0885 -178.9781 329.0854 -518.6594 0.6647
318.15 -1062.5453 500.1239 -268.6752 376.6488 -821.5198 0.6004
Benzene + TCE
∆η (mPa.s)
298.15 -0.0653 -0.0557 -0.0318 0.0182 0.0322 0.0004
303.15 -0.0785 -0.0547 -0.0647 0.0028 0.0561 0.0002
308.15 -0.0864 -0.0526 -0.0636 -0.0158 0.0251 0.0003
313.15 -0.0939 -0.0468 -0.0915 -0.0347 0.0197 0.0002
318.15 -0.1026 -0.0474 -0.0949 -0.0475 -0.0148 0.0002
∆ G*E (kJmol-1)
298.15 718.0968 -280.6028 18.0444 12.1205 81.6127 0.8357
303.15 845.9568 -326.8931 -68.9754 -18.3128 166.4595 0.5952
308.15 827.2768 -326.2755 -75.2511 -30.1629 79.6855 0.4822
313.15 694.2770 -275.3872 -197.0146 -26.2600 35.3841 0.7484
318.15 520.1513 -237.6426 -286.6083 -18.8703 -46.0321 0.7898

Fig. 1—Variation of ∆η with x1 for binary mixtures of benzene Fig. 2—Variation of ∆η with x1 for binary mixtures of benzene
+ DCE at different temperatures. Points show experimental values + TCE at different temperatures. Points show experimental values
and curves show smoothed values using Redlich-Kister equation19 and curves show smoothed values using Redlich-Kister equation19
548 INDIAN J PURE & APPL PHYS, VOL 46, AUGUST 2008

temperatures are shown in Figs 3 and 4. The values of
∆G *E are found to be negative over the whole range
of composition and temperature investigated for the
mixtures of benzene + DCE (Fig. 3), while reverse
trends are observed for benzene + TCE mixtures (Fig.
4). In general, the positive contribution to the
∆G *E values may be attributed to the presence of
specific interactions whereas negative contributions
may be ascribed to the dispersion forces21,24. Thus, the
observed positive ∆G *E values for the mixtures of
benzene + TCE suggest that the specific interactions of
donor-acceptor type are prevailing in the system,
whereas in case of benzene + DCE dispersion forces
are dominant which supports ∆η trends. Thus, the
observations are in accordance with the previously
reported volumetric and ultrasonic studies4 on the
present systems.
Further, by using the temperature dependence of
viscosity data the activation parameters for viscous
flow have been investigated. The Eyring viscosity
equation 25,26 is given as:
 hN   ∆G* 
η =  exp   … (2)
 V   RT 
where h is Planck’s constant, N is Avagadro’s
constant and ∆G * E is the Gibbs energy of activation
of viscous flow. Combining Eq. (2) with
∆G* E = ∆H * − T ∆S * gives the equation:

 ηV   ∆H 
*
*
RIn  =
   − ∆S … (3)
 hN   T 

where ∆H * and ∆S * are the enthalpy and entropy of

*E
Fig. 3—Variation of ∆G with x1 for binary mixtures of
benzene + DCE at different temperatures. Points show
experimental values and curves show smoothed values using
Redlich - Kister equation19
*E
Fig. 4—Variation of ∆G with x1 for binary mixtures of
benzene + TCE at different temperatures. Points show
experimental values and curves show smoothed values using
Redlich - Kister equation19
activation of viscous flow, respectively. The plots of
 ηV 
the left hand side of Eq. (3), i.e., RIn   against
 hN 
1
for both the binary mixtures at different
T
compositions were found to show a quite linear trend
for each composition of the system under study. This
indicates that ∆H * values are almost constant in the
investigated temperature range, i.e., ∆H * is
independent of temperature.
Thus, the values of ∆H * and ∆S * were obtained as
the slopes and intercepts of the linear plots of
 ηV  1
RIn   against by using a linear regression
 hN  T
procedure.
The values of ∆H * and ∆S * along with the linear
correlation factor, r of Eq. (3) are given in Table 4. A
close perusal of Table 4 indicates that for both the
binary mixtures, the values of ∆H * and ∆S * are
positive, showing an increase in ∆H * values and an
opposite trend in ∆S * values with mole fraction x1 of
benzene for the mixture benzene + DCE. In case of
benzene + TCE, both ∆H * and ∆S * tend to decrease
as the amount of benzene increases in the mixture. It
 ALI et al.: VISCOSITIES OF BINARY MIXTURES 549

Table 4—Values of enthalpy and entropy of activation of viscous mole fraction of benzene, which again supports our
flow for the binary liquid mixtures at each composition along with earlier view.
the linear correlation factor
3.1 Theoretical Analysis
x1 * * r 3.1.1 Correlation of excess volumes with viscosity
∆H -1
(kJ.mol ) ∆S -1 -1
(JK mol )
The excess volumes were calculated using the
Benzene + DCE
deviation in viscosity data by a correlation proposed
0.0000 7.169 7.532 0.995 by Singh27.
0.1028 8.285 7.139 0.997 According to the relation, the deviations in
0.1899 8.647 6.997 0.997 viscosity, ∆η and excess molar volumes, V E are
0.2975 8.951 6.871 0.998 related to each other as:
0.3910 9.218 6.762 0.998
∆η = KV E … (4)
0.5003 9.485 6.649 0.998
0.6019 9.787 6.533 0.998 where K is a fitting parameter. The values of K for the
presently investigated mixtures were evaluated by
0.7018 10.035 6.442 0.999
using the ∆η and experimentally reported V E data4 at
0.8006 10.339 6.338 0.999
x1 = 0.5 (equimolar fraction). The values of K for
0.8955 10.320 6.350 0.999
benzene + DCE and benzene + TCE are found to be-
1.0000 8.883 6.847 0.999 209.2 and - 353.3 Nsm-5mol, respectively. From the
Benzene + TCE
experimental ∆η data, the V E values at various mole
0.0000 10.267 7.278 0.936
fractions were calculated. The V E values calculated
0.1222 10.800 7.012 0.945
from viscosity data using Eq. (4) were compared with
0.1956 10.785 6.963 0.949
our earlier reported V E values4, obtained
0.3028 10.732 6.901 0.954 experimentally for both the mixtures at 298.15 K, and
0.3862 10.717 6.842 0.959 are shown in Figs 5 and 6. A reasonable good
0.4960 10.591 6.795 0.967 agreement has been found between the experimentally
0.5936 10.465 6.752 0.973 calculated and theoretically predicted values. Thereby,
it emphasizes the effectiveness of the present approach.
0.6890 10.435 6.673 0.982
0.8079 10.163 6.645 0.991 3.1.2 Prediction of mixtures viscosity
0.9020 9.776 6.669 0.996 A number of mixing rules are available in the
1.0000 8.883 6.847 0.999 literature28 for prediction of viscosities of liquid
17
has been suggested earlier that the enthalpy of
activation of viscous flow may be regarded as a
measure of the degree of cooperation between the
species taking part in viscous flow. In a highly
structured liquid, there will be considerable degree of
order and, hence, for cooperative movement of
entities, a large heat of activation, with relatively high
value of entropy of activation is needed for the flow
process. Therefore, a perusal of Table 4 indicates that
the formation of activated species necessary for
viscous flow seems to be easy in the DCE rich region,
owing to the low values of ∆H * , and become
difficult as the mole fraction of benzene in the
mixture increases, whereas, a reverse trend is E
Fig. 5—Comparison of V between reported values (—)4 and
observed in case of benzene + TCE mixtures. The
the calculated values obtained by using viscosity data (----) of
∆S * values are positive and decrease with increase in binary mixtures of benzene + DCE at 298.15 K
550 INDIAN J PURE & APPL PHYS, VOL 46, AUGUST 2008

where N i and N j are the number of carbon atoms in

component i and j, respectively. If either of the
component (i, j) contains atom other than carbon and
hydrogen, W = 0 (as in our case). Now, ∆ can be ∑
calculated for i and j from the group contributions
given elsewhere28 at 298.15 K. For benzene, DCE and
TCE, ∑ ∆ comes out to be 0.192, 0.854 and 0.444,
respectively. For mixtures of benzene + DCE/TCE,
Gij at 298.15 K can be calculated from Eq. (7).
Gij is supposed to be a mild function of
E temperature. Isdale et al10. suggested that if this is the
Fig. 6—Comparison of V between reported values (—)4 and the
calculated values obtained by using viscosity data (----) of binary case then at subsequent temperatures G could be
mixtures of benzene + TCE at 298.15 K calculated as:
mixtures theoretically. Among them probably the 573 − T
Gij (T ) = 1 − 1 − Gij (298.15)  … (9)
most extensively examined relation is the Grunberg - 275
Nissan (G-N) method.
Adopting the above two methods, viz., linear
According to this procedure, the liquid mixtures
regression analysis and group contribution method,
viscosity is given as:
the interaction parameters, Gij have been obtained for
1
Inη = ∑ xi Inηi + ∑∑ xi x j Gij … (5) both the liquid systems at each investigated
i 2 i≠ j temperature and presented in Table 5. Using the
Gij obtained from both methods, the viscosities of the
for a binary mixture of component 1 and 2, the
equation takes the form: binary mixtures were calculated at each investigated
temperature and the results were given in terms of
Inη = x1 Inη1 + x2 Inη 2 + x1 x2G12 … (6) average percentage deviations (APD) between
Table 5—Interaction parameters of Grunberg - Nissan equation
where x is the mole fraction and G12 is an interaction and Isdale’s group contribution approach for the binary liquid
parameter, which is a function of the components as mixtures at different temperatures along with the average
well as temperature. The interaction parameter Gij can percentage deviations (APD) from the experimental logarithmic
viscosity
be calculated by using a linear regression procedure.
Isdale et al.10 proposed a group contribution Benzene + DCE
method to estimate the binary interaction parameter T/K Grunberg- APD Isdale APD
Gij at 298.15 K. According to them: Nissan
298.15 -0.265 -0.450 -0.662 32.95
Gij = ∑ ∆ i − ∑ ∆ j + W … (7) 303.15 -0.310 -0.525 -0.650 -13.19
308.15 -0.258 -0.579 -0.638 -9.88
By following the priority rules, first of all, assign the 313.15 -0.420 -0.752 -0.626 -6.93
number viz., i and j to the components. We have
318.15 -0.493 -0.865 -0.614 -4.08
assigned benzene and chloroalkanes as i and j,
respectively (as per the priority rule). Then, the Benzene + TCE
parameter W can be determined using: 298.15 0.301 -6.072 -0.252 24.50
303.15 0.345 -5.247 -0.247 -79.64
(0.3161)( N i + N j ) 2 308.15 0.330 -9.452 -0.243 64.33
W= − (0.1188)( N i − N j )
( Ni + N j ) 313.15 0.263 0.268 -0.238 -70.73
… (8) 318.15 0.183 15.70 -0.234 -70.83
 ALI et al.: VISCOSITIES OF BINARY MIXTURES
Fig. 7—Comparison of Inη with the calculated values using
Grunberg - Nissan and Isdale’s approach for the binary mixtures
of benzene + DCE at 298.15 K
Fig. 8—Comparison of Inη with the calculated values using
Grunberg - Nissan and Isdale’s approach for the binary mixtures
of benzene + TCE at 298.15 K
experimentally reported and theoretically calculated
viscosities (Table 5). It is clear from Table 5 that the
APD in case of both the mixtures is quite low, when
Gij is taken from G–N method, while large deviations
are observed when Gij is taken from Isdale’s group
contribution method. It is interesting to note that for
benzene + DCE mixtures both Gij and APD obtained
by G–N method decrease with increase in
temperature, while they show an opposite trend when
obtained by using Isdale’s method. Whereas in case of
benzene + TCE no definite trends are observed with
variation of temperature.
Further, for the sake of comparison, logarithmic
viscosities, ln Inη obtained experimentally and from
G–N and Isdale’s approaches are plotted against x1
(Figs 7 and 8) for both the mixtures studied. It is evident
551
from Figs. 7 and 8 that Inη values calculated from G–N
approach are in excellent agreement with the
experimental values, whereas, Isdale’s approach shows
significant deviations between theoretical and
experimental Inη values for both the systems studied.
Thus, the present study further supports the effectiveness
of a simple, yet accurate, G–N method over the Isdale’s
group contribution approach.
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