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Karbala International Journal of Modern Science 2 (2016) 211e218
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Activity coefficients and excess Gibbs energy functions of

acetophenone with 1,2-dichloroethane and 1,1,2,2-tetrachloroethane
binary mixtures by using NRTL, UNIQUAC, UNIFAC and
VAN LAAR models at a local atmospheric pressure of 95.3 kPa
P. Anila a, K. Rayapa Reddy a,**, G. Srinivasa Rao b, P.V.S. Sai Ram b,
D. Ramachandran c, C. Rambabu c,*
a
Department of Chemistry, Andhra Loyola College, Vijayawada, Andhra Pradesh, India
b
Department of Physics, Andhra Loyola College, Vijayawada, Andhra Pradesh, India
c
Department of Chemistry, Acharya Nagarjuna University, Guntur, Andhra Pradesh, India
Received 11 February 2016; revised 3 July 2016; accepted 4 July 2016

Abstract

Bubble point temperatures of pure liquids (Acetophenone, 1,2-dichloroethane and 1,1,2,2-tetrachloroethane) and their liquid
mixtures were measured over complete composition range at a local atmospheric pressure of 95.3 kPa using a Swietoslawski-type
ebulliometer. The data were then correlated with Antoine's equation. From the data activity coefficients and Gibbs energies were
calculated. The systems showed a positive deviation from Raoult's law which suggests the presence of the dispersal forces acting
between component molecules in the liquid mixture. NRTL, UNIQUAC, UNIFAC and VAN LAAR models have also been applied
and good results were obtained. Molecular interactions between the unlike molecules in the binary liquid mixtures are discussed.
© 2016 The Authors. Production and hosting by Elsevier B.V. on behalf of University of Kerbala. This is an open access article
under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

Keywords: Antoine equation; Ebulliometer; Activity coefficients; Gibbs energy; Molecular interactions

1. Introduction necessary to meet the industrial scale needs of the

Knowledge of physicochemical properties such as
vapor pressures, boiling point, and vaporization
enthalpy of all of the components and mixtures is
* Corresponding author.
** Corresponding author.
E-mail addresses: krreddy.seshi@gmail.com (K. Rayapa Reddy),
crbpublications@gmail.com (C. Rambabu).
Peer review under responsibility of University of Kerbala.
chemical processes (design and optimization). Vapore
liquid phase equilibrium (VLE) calculations forecast
the PTx behavior of the mixture (where P is the system
pressure, T the temperature, and x denotes the com-
positions of the coexisting phases) and subsequently
the thermo physical properties of the coexisting fluids.
Those properties include heat capacity, enthalpy, en-
tropy, and density of the coexisting fluids. VLE in-
formation is extremely useful to control the distillation
column for practical distillation process.

http://dx.doi.org/10.1016/j.kijoms.2016.07.001
2405-609X/© 2016 The Authors. Production and hosting by Elsevier B.V. on behalf of University of Kerbala. This is an open access article under
the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
 Author's Personal Copy
212 P. Anila et al. / Karbala International Journal of Modern Science 2 (2016) 211e218

The study of mixtures containing an aromatic
compound with a polar functional group is interesting
due to the intermolecular interactions between the
phenyl ring and a polar functional group (np in-
teractions) [2,3]. Thermodynamic properties of highly
polar compounds with chloroethanes have received
increasing attention because they serve as model
compounds in biochemical considerations [4e7]. The
present work is a continuation of our research which
investigates VLE and thermodynamic properties of
binary mixtures of polar solvents [8e14]. This paper
presents the vaporeliquid equilibrium data at 95.3 kPa
for binary mixtures of acetophenone with 1,2-
dichloroethane and 1,1,2,2-tetrachloroethane. Aceto-
phenone, an aromatic ketone is an important industrial
chemical. It is used as a precursor to resins which are
components of coatings and inks. Its derivatives are
being developed as therapeutics in the treatment of
Alzheimer's disease [1]. Equilibrium data on the binary
mixtures of acetophenone with selected chloroethanes
have not been reported to the best of our knowledge.
We report the VLE profile of acetophenone mixtures
and correlate those observation with those generated
with NRTL, UNIQUAC, UNIFAC and VAN LAAR
methods.
packed column of height equivalent to 30 theoretical
plates, and enough care is taken to prevent the oxida-
tion or absorption of moisture. The pure liquids used in
the present work have a mole fraction purity of >0.999
based on the absence of multiple significant peaks in
the gas chromatograms. Table 1 reports the specifica-
tion of chemicals.
2.2. Methods
2.2.1. Density and VLE measurements
Densities (r) of the pure components were
measured at T ¼ 303.15 K and atmospheric pressure
using a DMA 4500 densitometer. Densities of the pure
components and their boiling points are presented
together with the literature data in Table 2 [16e20].
Boiling point of the pure components and their binary
mixtures were measured by a Swietoslawski ebulli-
ometer as described by Hala et al. [21]. The description
of apparatus used in our studies has been described
previously [9].
3. Results and discussion
3.1. Pure components

2. Experimental The boiling point temperature (Tb) of all the pure

liquids were measured at different pressures (P) using
2.1. Materials

Acetophenone (S. D. Fine Chemicals, India) is dried Table 2

over anhydrous potassium carbonate for 3 days, Densities of pure components at 303.15 K and boiling points (Tb/K) at
a pressure of 95.3 kPa along with the literature values.
filtered, and then distilled. The middle fraction of the
distillates is retained [15]. Analytical reagent grade Substance r/kg m3 Tb/K
1,2-dichloroethane (BDH Chemicals, Mumbai, India) Exp Lit Exp Lit
is further purified by washing with dilute potassium Acetophenone 1019.86 1019.9 [16] 472.30 475.2b [17]
a

hydroxide solution and water, dried over phosphorus 1,2-dichloroethane 1238.42 1238.41 [18] 354.86a 355.15c [19]
pentoxide, and fractionally distilled twice. Spectro- 1238.6 [20]
1,1,2,2- 1578.59 1578.59 [18] 418.06 418.35 [18]
scopic grade 1,1,2,2-tetrachloroethane (S. D. Fine
tetrachloroethane
Chemicals, India) is steam-distilled from calcium hy-
Standard uncertainties u are: u (T) 0.05 K, u (r) ¼ 0.00001 gm.cm3,
droxide slurry. The final step fractional distillation of u (p) ¼ 0.05 kPa.
all of the liquids was carried out within few hours to a
At a pressure of 95.3 kPa.
b
the commencement of the phase equilibrium experi- At a pressure of 101.3 kPa.
c
ment. Fractional distillation was carried out on a At a pressure of 95.6 kPa.

Table 1
Materials.
Component CAS Reg. No Source Mole fraction purity Purification method
Acetophenone 98-86-2 S.D. Fine, India 99.9 Distillation
1,2-dichloroethane 107-06-02 BDH, India 99.8 Fractional distillation
1,1,2,2-tetrachloroethane 79-34-5 S.D. Fine, India 99.9 Steam distillation
 Author's Personal Copy
P. Anila et al. / Karbala International Journal of Modern Science 2 (2016) 211e218 213

Table 3 through well-established procedures [23,24]. The

Experimental saturated vapor pressure (P/kPa) e boiling point (T/K) objective function Q is the sum of the squared absolute
data of pure components.
deviations in pressure. The non-ideality of the vapor
P/(kPa) Acetophenone 1,2-dichloroethane 1,1,2,2- phase is taken into account with the virial equation of
tetrachloroethane
state, truncated after the second term. Second virial
28.1 428.32 314.45 378.2 coefficients are calculated by the Hayden and O'Con-
31.1 432.15 317.51 380.1
38.5 439.38 323.5 386.5
nell method [25] using the parameters reported by
47.5 446.56 330.42 393.4 Dymond and Smith [26]. The values of the molar
57.8 453.65 336.54 399.5 excess Gibbs free energy GE are estimated from a
63.4 457.30 339.65 402.5 third-order RedlicheKister equation:
70.1 460.74 343.45 406.1
84.5 468.65 349.80 412.3
X
m
GE ¼ x1 ð1  x1 Þ RTGj ð2x1  1Þ ð3Þ
j1
95.3 472.30 354.86 418.06
j¼1

Table 4 The coefficients Gj are determined by regression

Antoine's constants obtained from vapor pressure temperature data. through minimization of the sum of deviations in vapor
A B C Tmin/K Tmax/K pressures. Vapor phase deviations are accounted in
Acetophenone 62.688 8088.8 5.5434 250 500 terms of the second molar virial coefficients, estimated
1,2-dichloroethane 16.24 3781 81.15 250 500 by the method of Tsonopoulos [27,28].
1,1,2,2- 16.24 2927.2 50.22 250 500 The vapor phase compositions are calculated from:
tetrachloroethane xi gi pi
yi ¼ ð4Þ
p
the same method as that for obtaining VLE data and
listed in Table 3. The measured vapor pressure (P) and where p the total equilibrium pressure, Pi the vapor
boiling point (T) of the pure liquids are correlated pressure of pure component i, xi the mole fraction in the
using the Antoine equation: liquid phase of component i, and gi the activity coef-
ficient of ith component in the liquid phase. The non-
ln ½P=ðkPaÞ ¼ fA  B=½T=ðKÞ þ Cg ð1Þ
random parameter (alpha) in the NRTL equation has
where A, B and C are Antoine coefficients determined been fixed to 0.3 for all cases. The fitting parameters (bij
from the experimental vapor pressure and boiling point and bij) reported in Table 5 along with the UNIQUAC
data of the pure liquids over temperature range and parameters U12U 22 and U 21U 11
presented in Table 4. The objective function Q is the The liquid phase composition x1 and vapor phase
sum of the squared relative deviations in pressure: composition y1 for the mixtures of (Acetophenone þ
1,2-dichloroethane), and (Acetophenone þ 1,1,2,2-
Xpcal  pexp 2 tetrachloroethane), along with the activity coefficients
Q¼ ð2Þ
pexp g1 and g2, and the values of the excess molar Gibbs
functions GE calculated by Barker's methods are pre-
sented in Tables 6 and 7. No literature data is found for
3.2. Binary systems the comparison with the present study. The two
investigated systems do not show azeotropic behavior
Regarding the two binary mixtures, data measured as can be seen from the plots of x-y with boiling
in the experiment consists of the liquid composition point, T.
and temperature. Reduction of the data for the binary The NRTL [29] and UNIQUAC [30] equations are
mixtures is done using the method of Barker [22] also used to correlate the experimental VLE data and

Table 5
Binary interaction parameters for both the binary systems using NRTL and UNIQUAC models at a pressure of 95.3 kPa.
NRTL UNIQUAC
b12 b21 U12U22 U21U11
Acetophenone þ 1,2-dichloroethane 52.84 50.74 1588.25 2255.27
Acetophenone þ 1,1,2,2-tetrachloroethane 51.81 50.26 1587.27 2252.94
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214 P. Anila et al. / Karbala International Journal of Modern Science 2 (2016) 211e218

Table 6 estimate the liquid phase activity coefficients. The

Temperature (T/K), vapor phase composition, activity coefficients and Simulis thermodynamic software developed by Prosim
excess Gibbs energy (GE/J.mol1) for the binary system, acetophe-
none (x1) þ 1,2-dichloroethane (1x1) at a pressure of 95.3 kPa.
(France) is used to correlate the data and to fit the
parameters.
x1 Texp Tcal y1 g1 g2 ln (g1/g2) GE
Additionally, prediction of VLE for the systems
0.0000 354.86 354.86 0.0000 1.1490 e 0.0839 0.00 studied has been carried out by the Modified UNIFAC
0.0579 355.16 355.20 0.7514 1.1326 1.0000 0.0759 6.19
0.1094 356.20 356.35 0.8862 1.1068 1.0008 0.0658 10.80
(Do) group contribution method [31] using the same
0.1556 357.16 357.25 0.9352 1.0922 1.0026 0.0554 14.26 software. It is observed that the descriptions of the
0.1972 358.16 358.11 0.9572 1.0806 1.0051 0.0448 16.87 systems by the Modified UNIFAC (Do) method are
0.2349 358.56 358.45 0.9689 1.0708 1.0079 0.0347 18.84 very good for both the systems under examination.
0.2692 359.05 358.75 0.9755 1.0624 1.0109 0.0250 20.32 Furthermore, predictions of VLE for the systems
0.3006 359.16 359.05 0.9797 1.0562 1.0138 0.0161 21.43
0.3294 359.65 359.85 0.9827 1.0504 1.0168 0.0078 22.25
studied have been carried out by the van Laar equation.
0.3559 361.36 361.95 0.9877 1.0414 1.0198 0.0011 22.84 The data obtained by this model is fairly in good
0.4031 362.16 363.05 0.9899 1.0289 1.0225 0.0211 23.51 agreement with the other models used for the predic-
0.4815 365.20 365.05 0.9913 1.0245 1.0278 0.0351 23.65 tion of the VLE data.
0.5149 367.16 366.90 0.9923 1.0200 1.0371 0.0443 23.36 The expressions for activity coefficients are given
0.5532 370.15 370.05 0.9934 1.0154 1.0412 0.0546 22.78
0.5977 374.45 374.25 0.9945 1.0110 1.0459 0.0666 21.79
for NRTL by:
0.6500 382.16 381.86 0.9955 1.0068 1.0513 0.0802 20.22 Pn 0Pn 1
0.0963 tji Gji xj x t G
0.7124 393.15 393.54 0.9967 1.0034 1.0574 17.81 X
n
xj Gij B
k kj kj
C
0.7879 410.10 410.34 0.9978 1.0009 1.0642 0.1153 14.14 In gi ¼ P
j
 B j C ð5Þ
n P
n @ P n A
0.8814 433.15 432.94 0.9989 1.0000 1.0717 0.1381 8.57 Gki xk j Gkj xk Gkj xk
1.0000 472.30 472.30 1.0000 e 1.0800 0.1654 0.00 k k k
Standard uncertainty in temperature u (T) ¼ 0.05 K, combined stan-
dard uncertainty in composition u (x) ¼ 0.0001, u (y) ¼ 0.0001 and where
Pressure u (P) ¼ 0.05 kPa at a confidence level of 95%. gij  gjj
tij ¼ ð6Þ
RT
Table 7 gij  gjj ¼ Cij0 þ CijT ðT  273:15Þ ð7Þ
Temperature (T/K), vapor phase composition, activity coefficients and
excess Gibbs energy (GE/J.mol1) for the binary system, acetophe-
none (x1) þ 1,1,2,2-tetrachloroethane (1x1) at a pressure of
aij ¼ a0ij þ aTij ðT  273:15Þ ð8Þ
95.3 kPa.  
Gij ¼ exp  aij tij ð9Þ
x1 Texp Tcal y1 g1 g2 ln (g1/g2) GE
0.0000 418.06 418.06 0 e 1.0000 0.1125 0.00 And for UNIQUAC by:
0.0760 418.16 418.82 0.2826 1.1250 1.0009 0.0948 8.13
0.1413 420.16 420.27 0.4424 1.1052 1.0030 0.0793 13.95 In gi ¼ In gcomb þ In gres ð10Þ
0.1980 422.16 422.25 0.5449 1.0895 1.0058 0.0657 18.14
0.2476 425.15 425.13 0.6172 1.0777 1.0089 0.0537 21.18 fi z qi f Xn
In gcomb ¼ In þ qi In þ li  i xi li ð11Þ
0.2915 428.15 427.96 0.6696 1.0670 1.0122 0.0429 23.37 i
xi 2 fi xi j
0.3305 430.86 431.05 0.7101 1.0587 1.0155 0.0333 24.95
0.3654 433.20 433.28 0.7424 1.0519 1.0187 0.0246 26.05 !
0.3969 434.85 434.35 0.7675 1.0463 1.0219 0.0166 26.81
X
n X
n
q'j tij
In gRes ¼ q'i  q'i In qj tji  q'i Pn '
k¼1 qj tij
0.4254 437.25 437.11 0.7881 1.0415 1.0250 0.0094 27.29 i
j¼1 j¼1
0.5252 440.75 440.65 0.8483 1.0273 1.0370 0.0160 27.57
0.5544 443.12 443.12 0.863 1.0238 1.0410 0.0236 27.23 ð12Þ
0.5871 445.15 445.35 0.8783 1.0201 1.0456 0.0321 26.64
0.6239 448.25 448.65 0.8942 1.0165 1.0509 0.0417 25.69 Z
0.6637 451.15 451.35 0.9107 1.0128 1.0572 0.0527 24.27
li ¼ ðri  qi Þ  ðri  1Þ ð13Þ
2
0.7134 454.16 454.65 0.9277 1.0092 1.0649 0.0654 22.19
0.7684 458.15 458.34 0.9448 1.0059 1.0742 0.0800 19.21 where ri and qi are molecular volume and surface area
0.8327 462.85 462.25 0.9625 1.0030 1.0859 0.0900 14.94 dimensionless structural parameters, called Van der
0.9087 466.16 466.54 0.9807 1.0009 1.0050 0.1169 8.83
1.0000 472.30 472.30 1.0000 1.0000 e 0.1404 0.00
Waals volume and area structural parameters, which are
estimated using the group contribution values of Bondi.
Standard uncertainty in temperature u (T) ¼ 0.05 K, combined stan-
dard uncertainty in composition u (x) ¼ 0.0001, u (y) ¼ 0.0001 and The coordination number Z is equal to 10. The inter-
Pressure u (P) ¼ 0.05 kPa at a confidence level of 95%. action parameters are as follows:
 Author's Personal Copy
P. Anila et al. / Karbala International Journal of Modern Science 2 (2016) 211e218 215

   
Uij  Ujj Sa Sb 
tij ¼ exp  ð14Þ 
D¼   100 ð18Þ
RT Sa þSb 
 0  T
DUij ¼ Uij  Ujj ¼ Uij  Ujj þ Uij  Ujj $T ð15Þ where Sa is the area of ln (g1/g2)  x1 above the x-axis,
and Sb is the area of ln (g1/g2)  x1 under the x-axis.
van Laar equation used to find the activity coefficients  
Tmax  Tmin 
  
2 J ¼ 150    ð19Þ
In g1 ¼ A1 1 þ A1 x1 þ B1 x2 ð16Þ T 
min

  
2
In g2 ¼ B 1
1 þ A1 x 1 þ B1 x 2 ð17Þ where Tmax and Tmin are the maximum and minimum
temperatures of the system, respectively. If D < J, the
where the van Laar coefficients A1 and B1 are equal to isobaric VLE data can be considered to confirm the
the logarithmic limiting activity coefficients g∞ ∞
1 and g2 thermodynamic consistency test [33]. Both the binary
respectively. systems under investigation passed the thermodynamic
For the binary systems under investigation, the consistency test.
Herington's method [32] is used to verify the quality The calculated activity coefficients with the liquid
and consistency of all experimental data. mole fraction of acetophenone (x1) are presented in

Fig. 1. Plot of boiling point against mole fraction x1 acetophenone for the binary mixture {x1 acetophenone þ (1-x1) 1,2-dichloroethane},
(a) NRTL model, (b) UNIQUAC, and (c) UNIFAC model.
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216 P. Anila et al. / Karbala International Journal of Modern Science 2 (2016) 211e218

Tables 6 and 7. It is apparent from the data that the
activity coefficients values are very close to unity for
the binary systems under study indicating a closeness
to ideal behavior [34]. Additionally, very weak repul-
sive molecular interactions could be another contrib-
uting factor. The boiling point (Tb) versus mole
fraction curves in both liquid (x1) and vapor phases (y1)
for both investigated mixtures are presented in Figs. 1
and 2 as well as the results of correlation using NRTL
and UNIQUAC. The NRTL, UNIQUAC and VAN
LAAR models fit the experimental results of the sys-
tems very well. It has also been observed from the
figures that no azeotropic mixtures are formed in both
the binary mixtures. The positive deviations from
Raoult's law observed in the systems perhaps due to the
presence of dispersal forces over the whole composi-
tion range at constant pressure of 95.3 kPa. Similar
type of results are reported by Hasdemir et al. [35,36]
for the binary mixtures of 1,2-dichloro ethane with
toluene and acetic acid. Carlson et al. [37] explained
the positive and negative deviations for non-ideal so-
lutions from vaporeliquid equilibrium studies. Both
the binary mixtures passed the Herington's thermody-
namic consistency test.
A plot of Gibbs energy (GE) versus mole fraction of
acetophenone has been presented in Fig. 3. Both the

Fig. 2. Plot of boiling point against mole fraction x1 acetophenone for the binary mixture {x1 acetophenone þ (1-x1) 1,1,2,2-tetrachloroethane},
(a) NRTL model, (b) UNIQUAC, and (c) UNIFAC model.
 Author's Personal Copy
P. Anila et al. / Karbala International Journal of Modern Science 2 (2016) 211e218
Fig. 3. Plot of the change in Gibbs energy GE against mole fraction
x1 acetophenone for the binary systems {x1 acetophenone þ (1-x1)
1,2-dichloroethane} and {x1 acetophenone þ (1-x1) 1,1,2,2-
tetrachloroethane}.
binary systems under examination exhibit positive
values for (GE). It can be inferred from this observation
that the molecular interactions are weak which may be
due to the presence of dispersal forces between the
dissimilar molecules on mixing. Garcia-Mardones
et al. [38] have observed positive excess Gibbs en-
ergies and interpreted that the positive nature is due to
the rupture of bonds between the unlike molecules of
the binary liquid mixtures. Ming-Jer Lee et al. [39]
have observed the positive excess Gibbs energy
values and expressed their results in terms of positive
deviation from Raoult's law. The present investigated
binary systems also exhibit positive deviation from
Raoult's law. It is observed that the excess Gibbs
values are higher for acetophenone with 1,1,2,2-
tetrachloroethane than with 1,2-dichloroethane sys-
tem. Acetophenone, 1,2-dichloroethane, and 1,1,2,2-
tetrachloroethane are self associated liquids due to
the presence of dipoleedipole interactions in their pure
states. When chloro compounds are added to aceto-
phenone, incompact molecular structure may possibly
form due to dispersion forces operating between the
dissimilar molecules. In addition to dispersal forces the
geometrical mismatching of the structures between the
unlike molecules in the binary system could also play a
role.
4. Conclusions
VLE data are reported for Acetophenone þ
1,2-dichloroethane and Acetophenone þ 1,1,2,2-
tetrachloroethane. No azeotropic behavior is
observed. The experimental VLE data are correlated
with the NRTL, UNIQUAC, UNIFAC and VAN LAAR
models. The activity coefficients are found to be nearer
to unity value. Thermodynamic consistency test
217
presents that the data are consistent. Both the binary
systems are found to be non-ideal liquid mixtures.
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