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Fluid Phase Equilibria
Fluid Phase Equilibria
a r t i c l e i n f o a b s t r a c t
Article history: In this study, we report a temperature-dependent prediction model without arbitrary parameters for the
Received 8 August 2018 coefficient of surface tension of homogeneous liquid, and then validate it by the available experimental
Received in revised form data of fifteen kinds of pure liquids. Very small maximum deviation or absolute average deviation be-
18 November 2018
tween predicted and experimental results has been obtained. The prediction model uncovers the
Accepted 21 November 2018
Available online 23 November 2018
inherent relationship between the coefficient of surface tension, boiling point, heat of evaporation, heat
capacity, and coefficient of linear expansion. Furthermore, it reveals that the decrease of cohesion energy
determines the decline of coefficient of surface tension and can analyze the variation of coefficient of
Keywords:
Coefficient of surface tension
surface tension with increasing temperature.
Temperature-dependent © 2018 Elsevier B.V. All rights reserved.
Homogeneous liquid
Prediction model
https://doi.org/10.1016/j.fluid.2018.11.024
0378-3812/© 2018 Elsevier B.V. All rights reserved.
54 H. Kou et al. / Fluid Phase Equilibria 484 (2019) 53e59
gL ðT0 Þ gL ðTB Þ ¼ K 6
4
7
Cv ðtÞdt þ DHvap 5 (5)
2. Theoretical derivation
T0
of liquid materials, and EBul(L) denotes their bulk cohesion energy. Substituting Eqs. (4) and (6) in Eq. (3), it becomes:
H. Kou et al. / Fluid Phase Equilibria 484 (2019) 53e59 55
gL ðT0 Þ Cv ðTB TÞ þ DHVap
ðT gL ðTÞ ¼ (10)
gL ðT0 Þ 1 þ aðT T0 Þ Cv ðTB T0 Þ þ DHVap
gL ðT0 Þ gL ðTÞ ¼ ð TB Cv ðtÞdt (7)
Cv ðtÞdt þ DHvap T0 In this way, a new temperature-dependent coefficient of surface
T0
tension prediction model without any arbitrary parameter is
developed. It reveals the inherent relationship between the coef-
which can also be presented as:
ficient of surface tension, boiling point, heat of evaporation, heat
ðT capacity, and coefficient of linear expansion. If one of the above
Cv ðtÞdt parameters is harder to be obtained than surface tension, then the
gL ðTÞ T0 surface tension can be used to calculate other material parameters.
¼ 1 ðT (8)
gL ðT0 Þ B In the following section, available experimental data of fifteen
Cv ðtÞdt þ DHvap kinds of pure liquids are found to validate the model. Furthermore,
T0
the model can also help analyze the variation of coefficient of
In addition, surface tension is a macro reflection of intermo- surface tension with increasing temperature.
lecular or interatomic forces. Definition of coefficient of surface
tension indicates it has the dimension of force per unit length. We 3. Results and discussion
hold the point that the force per unit length is generally affected by
two parts, the force between each molecule or atom and the 3.1. Surface tension of compounds
quantity of molecule or atom per unit length. Eq. (8) reflects the
force between molecules or atomics but does not include the The surface tension experimental data of tetrachloromethane
quantity change of them per unit length with increasing temper- (CCl4) [41], trichloromethane (CHCl3), benzene (C6H6), phenol
ature. Let a0 denotes the bond length at reference temperature T0, (C6H5OH) [42], and water (H2O) [21,41,43] are found and corre-
RT
then bond length at temperature T is a0 ð1 þ T0 aðtÞdtÞ, where aðtÞ sponding values are predicted by the model. The reference
is the temperature-dependent coefficient of linear expansion. Then, temperature, boiling point, and heat of evaporation of these
the ratio of quantity of atoms or molecules per unit length at calculated materials are shown in Table 1. Their temperature-
RT dependent coefficient of volume expansions are shown in
temperature T and T0 can be easily obtained as 1=ð1 þ T0 aðtÞdtÞ.
Table 2, and the coefficient of linear expansion can be taken as
Researches also show that thermal expansion is an influence factor
one third of it [39]. The molar heat capacity of CCl4 is 133.9
that has effects on the surface tension of liquids [35e37]. Consid-
J=ðmol$KÞ [39]. The specific heat capacity of other compounds are
ering the above analyses, this part should be multiplied in Eq. (8).
shown from Table 3 to Table 6.
Then a temperature-dependent coefficient of surface tension pre-
Comparisons between experimental and predicted coefficient of
diction model for liquids can be obtained:
surface tension of CCl4 (a), CHCl3 (b), C6H6 (c), C6H5OH (d), and H2O
0 1 (e) are shown in Fig. 1. One can see that good agreement has been
ðT obtained. The maximum deviations between experimental and
B C
B C predicted results are listed in Table 1, those of CCl4, CHCl3, C6H6, and
B Cv ðtÞdt C
gL ðT0 Þ B C C6H5OH are rather small. As for H2O, there is a relatively large
gL ðTÞ ¼ ðT B 1 ð TB
T0 C (9)
B C maximum deviation (2.40%) between the experimental data and
B C
1þ aðtÞdt B Cv ðtÞdT þ DHVap C predicted results. This is resulted from the facts that the variation
T0 @ T0 A
with temperature of the quantity of hydrogen bond is ignored in
the model. To our knowledge, water has a higher surface tension
For a large amount of materials, the coefficient of linear because of the relatively high attraction through hydrogen bonds
expansion and molar heat capacity are constant in a large tem- [45]. And the quantity of hydrogen bonds decreases with increasing
perature range between the melting point and boiling point temperature [46]. However, in the presented model, decreasing of
[38e40]. Thus, the model can also be expressed as: the quantity of hydrogen bond is not sufficiently considered, which
makes the predicted results higher than experimental data.
Table 1
The physical parameters of calculated materials and maximum deviation between Table 3
experimental and predicted results [42e44]. The specific heat capacity of CHCl3 at different temperatures [42].
Materials CCl4 CHCl3 C6H6 C6H5OH H2O Temperature (K) 273.0 293.0 313.0 333.0
Reference temperature (K) 288.1 273.0 293.0 333.0 273.0 Specific heat capacity (J/(gK)) 0.958 0.963 0.968 0.976
Boiling point (K) 349.9 334.2 353.1 454.8 373.0
Heat of evaporation (J/g) 195.1 244.9 393.2 489.0 2257.0
Number of experimental points 3 4 4 6 37
Maximum deviation (%) 0.39 1.35 0.35 0.40 2.40 Table 4
The specific heat capacity of C6H6 at different temperatures [42].
Table 6
The temperature-dependent heat capacity and coefficient of linear expansion of H2O [43].
Temperature (K) 273.0 283.0 293.0 303.0 313.0 323.0 333.0 343.0 353.0 363.0 373.0
Specific heat capacity (J/(gK)) 4.218 4.192 4.182 4.178 4.179 4.181 4.184 4.189 4.196 4.205 4.216
Coefficient of linear expansion (mm/(mK)) 23.0 29.3 69.0 102.3 130.0 153.3 176.0
3.2. Surface tension of pure metal liquids recommend values and predicted coefficient of surface tension of Al
(a), Co (b), Cu (c), Fe (d), Ni (e), Mn (f), Sn (g), Ti (h), Zn (i), and Hg (j).
In this section, the coefficient of surface tension of ten kinds of It is obvious that good agreement has been obtained. The maximum
pure metal liquids at different temperatures were predicted and deviations between predicted and experimental data of Al, Co, Cu,
compared with experimental data. The thermophysical property Fe, Ni, Mn, Zn, and Hg are shown in Table 7, which are very small. As
parameters used in prediction are presented in Table 7 and Table 8. for Sn and Ti, their absolute average deviations (AAD) are 0.37% and
Comparisons between the predicted and experimental data are 0.23%, respectively. The temperature-dependent coefficient of
shown in Fig. 2. surface tension prediction model without arbitrary parameters has
Fig. 2 shows the comparisons between experimental data or been validated. In Fig. 2 (g), White [16] experimentally measured
Fig. 1. Comparisons between predicted results and experimental data of surface tension of CCl4 (a) [41], CHCl3 (b), C6H6 (c), C6H5OH (d) [42], and H2O (e) [21,41,43] as function of
temperature.
H. Kou et al. / Fluid Phase Equilibria 484 (2019) 53e59 57
Table 7
The physical parameters used in the coefficient of surface tension prediction and the maximum deviation of pure metal liquids [38e40,44,47].
Pure Reference temperature Molar heat capacity (J/ Coefficient of linear expansion (mm/ Boiling point Heat of evaporation (J/ Maximum deviation
metal (K) (molK)) (mK)) (K) mol) (%)
the temperature-dependent surface tension of Sn and gave a linear the temperature-dependent coefficient of surface tension without
equation as Eq. (1) to describe its variation with temperature. One any arbitrary parameter. Furthermore, as can be seen in Fig. 2,
can see that both White's equation and our model reach good although there have been many experimental attempts to deter-
agreement with the experimental results. However, White's equa- mine the accurate values for surface tension, there is still poor
tion is a phenomenological formula and lacks physical bases. The agreement among the existing experimental results [13]. And the
model developed in this study has a significant value of predicting variation tendencies of the experimental data with increasing
temperature given by different researchers are also different. In this
Table 8 condition, the model developed in this study can also be used to
The specific heat capacity of Hg at different temperatures [42]. evaluate which of the experimental results are more convincing to
Temperature (K) 298.0 350.0 400.0 450.0 500.0 600.0 some extent.
Up to now, there have been many attempts to correlate surface
Specific heat capacity (J/(gK)) 0.140 0.138 0.137 0.136 0.136 0.135
tension of pure metals with material properties (e.g. heat of
Fig. 2. Comparisons between experimental data or recommend values and the predicted results of Surface tension of Al (a) [7,48e51], Co (b) [7,10,52e55], Cu (c) [7,10,55e59], Fe (d)
[10,55,56,60e63], Ni (e) [10,56,60,61,64,65], Mn (f) [10], Sn (g) [16], Ti (h) [10,54,65e68], Zn (i) [10], and Hg (j) [10] as function of temperature.
58 H. Kou et al. / Fluid Phase Equilibria 484 (2019) 53e59
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