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Pergamon Chemical Emlineerinq Science. Vol. 52, No. 8. pp 1243 1251.

1997
1997 Elsevier Science Ltd. All righls reserved
Printed in Great Britain
PII:

A new correlation for thermal conductivity


of liquids
Q u n f a n g Lei,** Y u - C h u n H o u * a n d Ruisen Lin*
*Chemical Engineering Thermodynamics Laboratory, Zhejiang University, Hangzhou 310027,
People's Republic of China; *Department of Chemistry, Zhejiang University, Hangzhou
310027, People's Republic of China

(Received 6 February 1996)

Abstract--On the supposition that liquid is composed of a mixture of microcrystallites and


vacancies, and on the basis of significant structure theory and analysis of the radial distribution
function of liquids, a new two-parameter model is presented for correlating thermal conductivi-
ties of liquids and liquid mixtures. The thermal conductivities of inorganic compounds,
paraffins, olefins, cycloparaffins, aromatic hydrocarbons, alcohols, ethers, aldehydes, ketones,
esters, organic acids and some refrigerants over wide ranges of temperature are calculated using
the new model and compared with data reported in the literature. The method is extended to
mixtures by using simple mixing rules. Calculated results show that the new model can be used
for the correlation of the thermal conductivities of systems consisting of nonpolar and polar
compounds and also for those of aqueous solutions. Especially, for pure compounds such as
inorganic compounds, nitrogen- or sulfur-containing materials and aldehydes, and for mixtures
consisting of alcohols and aqueous systems, the proposed correlation shows better agreement
with experimental data than the models recommended by Reid et al. (1987, The Properties o!
Gases and Liquids, 4th Edition. McGraw-Hill, New York). ~ 1997 Elsevier Science Ltd. All
rights reserved

Keywords: Correlation; thermal conductivity; transport property.

INTRODUCTION In this paper, a new correlation for thermal conduc-


Thermal conductivities of liquids and liquid mixtures tivities of liquids, which may be used over wide ranges
are required in many heat transfer calculations, but of temperature, is proposed on the basis of the signifi-
reliable data are not abundant due to experimental cant structure theory and analysis of the radial distri-
difficulties in measurement. Since it is impractical to bution function of liquids.
measure thermal conductivities for all the liquids and
liquid mixtures of interest, especially when data over DERIVATION OF THE CORRELATION EQUATION FOR
wide ranges of temperature and pressure are involved PURE COMPOUNDS
in process calculations (Lakshimi and Prasad, 1992), According to the significant structure theory of
methods for predicting liquid thermal conductivities liquid (Eyring, 1967), a liquid is treated as a mixture of
are necessary in practice. solid- and gas-like molecules. Therefore, the thermal
Since theoretical methods have not yielded suffi- conductivity of the liquid may be expressed as
ciently accurate and simple expressions for calculating
1~ v-v~.
thermal conductivities of liquids, correlations based ~o= -iv/,., + ~ V - - ~.~ (1)
on empirical or semi-theoretical methods are widely
employed over wide ranges of temperature (Reid et al., where 2, ,;~ and 20 are the thermal conductivities of the
1987). Recently, a correlation based on the significant liquid, the solid- and the gas-like molecules, respec-
structure theory was proposed by Hildwein and tively, and V, V, are the volumes of the liquid and the
Stephan (1993), yielding satisfactory result, though the solid-like molecules, respectively.
computation process was somewhat difficult. The distribution of molecules in a liquid is non-
random at close range and random at long range.
Suppose that the liquid consists of microcrystallites
*Correspondence address: Department of Chemistry, and vacancies, and that the thermal conductivity of
Zhejiang University, Hangzhou 310027, People's Republic of the liquid is the sum of the contributions of those
China. microcrystallites and vacancies. Equation (1) may
1243
1244 Qunfang Lei et al.
then, by analogy, be used to express the liquid thermal tallite can be expressed as
conductivity, where ),~ and 2~ now represent the ther-
mal conductivities of the microcrystallites and va- ),, = Cvvl (10)
cancies, respectively.
where Cv is the heat capacity of microcrystallites,
The partition function of this liquid can then be
v the average velocity of phonons and I the mean free
written as
path of the phonons.
Q = (Q~), QO (2) By considering the scattering of phonons, the mean
free path of the phonons may be written (Saksena and
where Q* and QO are the partition functions of micro- Prabhuram, 1981; Klemens, 1951) as
crystallites and vacancies, respectively, and n is the
number of microcrystallites. For microcrystallites, Y
1 aK 2 (11)
T 3
where K is the wave vector, a is the lattice constant,
Y is a constant dependent on the size of the crystal
where fl = 1/kT, k is the Boltzmann constant, T the and is inversely proportional to the equilibrium num-
temperature, n' the number of molecules in a micro- ber of microcrystallites. Then,
crystallite, and 0 and E~ are, respectively, the Einstein
temperature and the sublimation energy of the solid. Y = D'T -3/7 (V -- Vs) -2/7 (12)
The total number of molecules in the liquid is N, and
then N = nn'. where D' is a proportionality constant.
Because the movement of vacancies in the liquid is According to Debye's theory (Kittel, 1976), the in-
related to the movement of microcrystallites, Qg can ternal energy of the microcrystallite is
be expressed as the translational partition function of
the microcrystallites v27z2
~ eho,/~--- 1 do (13)

Q._Qt.=F(2nmn'kT~3/2[_\_ In,
-hg ) V--n"~V'I" (4) where o) is the vibration frequency of the phonon,
~o = vK and h = hi2 zt.
Then, eq. (2) becomes Hence,

Cv = " ~ v = 21tZV3k r 2 (eho,/kr _ 1)2d

x(\-
~(2.mn'kT~'/2
.)
V -. V~}"/ (5)
3 V, h 2 ,/',o 014 eh~,/kv
-2rc2v3kT2 Jo (e~T)/do)
(14)
By using the Stirling formula for n!, eq. (5) reduces
to where ~ODis the maximum vibration frequency of the
phonon.
"
Combining eqs (10)-(14), we have

2s = Vs h 2 y fO ) (2)2ehO'/kT
(v - 2" -rcZ
- - ~k 2T a ( e ~ ) 2 de)
(\ h2 } n2 j. (6)
V~Y ~" O) 4 e h'/kT

At any given temperature and pressure, the Helm- ,,~ D' T 2 J 0 (e~ 7"1)2 d(D
holtz free energy of the liquid is minimized when the
system is at equilibrium (Saksena and Prabhuram, T4/TVs
1981), so that -- D (V - Vs)2/7" (15)

F = - k T In Q (7) Because the number of vacancies in the liquid is


very small, thermal conductivity of vacancies in the
C-~n) =kT[ 31n2rtrnNkT-lnV-V*+~] liquid can be calculated by using the kinetic theory of
r,v -- 2 - - - -nhT - - --7- =0 dilute gases (Reid et al., 1987):
(8)
( 2 n m N k T ) 3/7 20 ac a~2~yM (16)
n = \- --h2 ) ( v - vA 2,7 e -5/7. (9)
where T is the temperature, M the molecular weight,
According to the theory of solid state physics (Kit- a the characteristic dimension of molecule and f~o the
tel, 1976), the thermal conductivity of the microcrys- collision integral. Then a and f~0 in eq. (16) can be
A new correlation for thermal conductivity of liquids 1245
calculated by the method recommended by Reid et al. that eqs (25)-(33) reduce to the correlation for pure
( 1987): liquids when one of the component's mole ~action is
zero.
~ = Ao{T') B~ + Cg exp ( - DyT') + E0 e x p ( - FoT')
(17) RESULTS AND DISCUSSION
The thermal conductivities of 86 pure liquids in-
T'= 1.2593T, (18)
cluding inorganic compounds, paraffins, olefins,
a ~c V(!'3 (19j cycloparaffins, aromatic hydrocarbons, alcohols,
ethers, aldehydes, ketones, esters, organic acids and
.4~ = 1.16145, B u = 0.14874, Cg = 0.52487 (20) some refrigerants were calculated from eq. (23j over
wide ranges of temperature, and are shown in Table 1.
D, = 0.7732, E~ = 2.16178, Fa = 2.43787. (21) The reference data of thermal conductivities are from
Then, Vargaftik (1975), Mukhamedzianov and Usmanov
{1971), Touloukian et al. (1970), and Nieto de Castro
V@-/M (22)
et al. (1986). For 920 data points, the overall average
L, = C V~2/3f2--~. absolute deviation of the correction is 0.98%.
All estimation techniques for thermal conductivities
Combining eqs (1), (15) and (22), we have of pure liquids as listed by Reid et al. (1987), are
empirical, with only limited exceptions. Of these the
T 4~ Vs2 V -- V~ % / T 7 ~
),=D + C - - (23) Latini method shown below appears to be better than
( V - - Vs)2/7 V V Vc2/3~~ O the many tested:

where D and C are two parameters characteristic of .4(1 -- Tr) 3s


a liquid, which should be determined from experi- ). - (34)
7-,k.~
mental data. For a liquid, the data over the investi-
gated temperature range are used to make a least- ,4* T~
A= (35)
error fit. Then, the values of D and C can be obtained. M ~ T(~'
In eq. (23), V, the volume of the microcrystallites,
can be taken as the volume of the solid at the melting T~ = T / T c {36)
point, which may be estimated from the liquid volume where Tb is the normal boiling temperature, Tc the
at the melting point by the following relation (Sagara critical temperature, M the molecular weight, and
et al., 1975): values of the parameters A*, ~, fl and 7 vary for the
(24) different classes of organic compounds. Table 1 shows
V~ = 0.89V,,.
also the calculated results by the Latini method for 75
of the 86 liquids listed (816 data points), with an
CORRELA'FION FOR LIQUID MIXTURES
average absolute deviation of 3.73%. Although the
The correlation developed for pure liquids is ex- Latini method is a one-parameter method, it cannot
tended to the calculation of thermal conductivities of treat inorganic, nitrogen- or sulfur containing com-
liquid mixtures by utilizing the following simple mix- pounds and aldehydes, while the present method
ing rules: which is a two-parameter method can treat all the
compounds listed.
D,. = ~ ~ xixiDii (25) Table 2 shows the calculated and experimental
i i thermal conductivities of 67 binary mixtures. The
mixtures chosen are representative of systems with
D ~, = , v / ~ D~ (26) nonpolar + nonpolar, nonpolar + polar, polar + po-
(27} lar as well as aqueous systems. The overall average
Cm = E xiCi
absolute deviation of the correlation results from the
v,.~ = Z Z .,,x~v~,j (28) experimental data for all the binary systems with 725
i i data points was found to be 1.29%.
(29) Among the many correlation methods for the ther-
Vsi.i = is(1 -- kifl (Vs'i/3 + Vslj/3)3
mal conductivities of liquid mixtures (Reid et al.,
Mm = E x i M i (30) 1987), the Baronicini correlation (Baronicini et al.,
1984) shows below is chosen to test our method:
v,.,o = Y~ ~ xzx~ v,.,j (31)
i )
Zm = (AIx~ + A2X~ + n v f A 1 A 2 x 1 x 2 ) (1 - Tr,,) - ~
Vcfj = 18(V(~./3 -[- Vclj/3)3 (32) T ,',,/'
[37}
Tcm = ~ xi Tci (33)
where x~ and x2 are the mole fractions of components
where k~j is a binary interaction coefficient which must 1 and 2, A~ and A 2 a r e parameters of the two compo-
be determined from experimental data. It is obvious nents, respectively, with the same definition as in
1246 Qunfang Lei et al.

Table 1. Calculated results for pure compounds

Present work Latini method


No. of Temp. range
No. Compound points (K) D C x 104 Deviation (%t Deviation(%)

1 Hydrogen 15 16.00-30.00 28.0943 1.2543 1.03


2 Neon 5 25.00 29.00 34.4031 0.3390 2.90
3 Sulfur dioxide 21 200.00-400.00 10.3855 -- 0.2609 1.37
4 n-Butane 9 143.15-273.15 6.4193 -- 7.1173 1.85 2.77
5 iso-Butane 9 133.15 253.15 6.0283 - 5.4954 2.57 13.12
6 n-Pentane 9 153.15-293.15 5.9846 - 8.2518 1.79 7.67
7 n-Hexane 9 183.15 333.15 3.6990 -- 6.2928 1.62 2.97
8 n-Heptane 19 190.00 370.00 3.2029 - 6.1832 1.58 3.10
9 n-Octane 8 233.15 373.15 2.5992 -- 7.4423 0.94 2.45
10 n-Nonane 9 233.15-393.15 2.3626 -- 5.8503 2.12 1.39
11 n-Decane 10 253.15 433.15 2.0038 -- 4.8578 0.78 0.57
12 n-Undecane 11 253.15-453.15 1.8743 -- 4.9949 0.86 0.81
13 n-Dodecane 11 273.15-473.15 1.5280 - 2.8242 0.23 1.61
14 n-Tridecane 12 273,15 493.15 1.4570 -- 2.4958 0.25 3.68
15 n-Tetradecane 12 293,15-513.15 1.3631 - 2.0896 0.29 4.23
16 n-Pendecane 13 293,15 533.15 1.3265 -- 2.0765 0.25 4.84
17 Cyclohexane 6 283,15-353.15 2.3350 0.3233 0.12 4.08
18 Cycloheptane 6 273,15 373.15 2.3526 0.0028 0.14 1.27
19 Benzene 16 283.15-433.15 3.2603 -- 1.0831 0.23 0.61
20 Toluene 14 230.00-360.00 4.1933 - 6.2030 0.86 1.48
21 Ethyl benzene 11 193.15-393.15 3.5769 - 5.7389 1.92 0.51
22 n-Propyl benzene 12 193.15-413.15 2.3096 - 4.9275 0.58 2.50
23 iso-Propyl benzene 12 193.15-413.15 3.0123 - 6.6337 2.12 2.26
24 n-Butyl benzene 14 193.15-493.15 1.9226 - 1.1892 1.02 2.62
25 m-Xylene 6 273.15-398.15 2.1980 -- 0.5312 0.56 1.02
26 p-Xylene 7 273.15 393.15 2.2734 -- 2.0436 0.09 0.06
27 o-Xylene 9 253.15-413.15 2.7030 -- 3.8019 0.76 0.72
28 Propene 7 93.15 213.15 10.7021 -- 6.9362 0.84 4.60
29 1-Butene 8 113.15-253.15 5.8035 - 5.8793 0.63 4.87
30 1-Pentene 9 133.15 293.15 5.1139 - 7.3234 1.68 4.96
31 1-Hexene 10 153.15-333.15 4.8399 -- 7.1729 2.07 1.84
32 1-Heptene 11 173.15 373.15 3.2395 - 5.2189 1.62 2.16
33 l-Octene 11 193.15-393.15 3.0096 -- 6.0530 1.70 2.20
34 1-Nonene 11 213.15-413.15 2.3735 -- 5.2840 1.12 5.97
35 l-Decene 12 213.15 433.15 1.9316 -- 4.6107 0.48 10.54
36 1,2-Dibromoethane 6 293.15-393.15 2.3005 -- 3.6541 0.21 2.01
37 Chloroethane 4 213.15 273.15 6.2009 -- 3.1617 0.57 1.66
38 lodoethane 9 173.15-333.15 3.6698 - 4.5368 1.49 9.97
39 l-Ch loro butane 9 173.15 333.15 3.8143 -- 4.7314 1.14 2.57
40 1-Chloropropane 8 173.15-313.15 4.0352 -- 2.3118 0.43 6.82
41 Bromoethane 7 173.15-293.15 4.1583 - 2.7694 0.49 6.78
42 Carbon tetrachloride 23 253.15-473.15 2.4599 -- 1.3266 1.48 1.14
43 Chloroform 21 200.00 400.00 3.6528 -- 0.6703 0.87 3.01
44 Difluorodichloromethane 16 203.15-353.15 3.8561 -- 1.2568 2.54 2.19
45 Fluorodichloromethane 17 213.15-373.15 3.5859 -- 2.3226 1.90 1.72
46 Tetrafluorodichloro-
methane 24 180.00-400.00 1.8385 -- 0.7005 1.30 1.87
47 Triflurot richloroethane 12 253.15 363.15 1.6318 - 1.3661 0.12 1.12
48 Chlorodifluoromethane 35 173.15 343.15 4.3492 - 0.7192 0.90 3.41
49 Fluorodichloromethane 15 233.15-373.15 4.3451 -- 1.8256 1.13 5.45
50 Trifluorochloromethane 9 193.15 273.15 5.3091 - 1.0271 1.01 4.52
51 Methanol 9 183.15-333.15 11.8461 - 1.2395 0.76 2.87
52 Ethanol 11 163.15-333.15 9.0339 3.6309 0.85 2.43
53 1-Propanol 14 153.15-373.15 6.4557 -- 2.0895 0.54 5.81
54 iso-Propanol 10 183.15-353.15 5.1089 -- 2.1661 0.73 4.48
55 n-Butanol 10 193.15-373.15 4.7528 -- 2.6352 1.14 3.66
56 iso-Butanol 13 173.15-373.15 4.3984 -- 2.5075 2,10 6.51
57 n-Pentauol 11 193.15-393.15 4.0372 - 3,5740 0.29 4.61
58 n-Hexanol 10 233.15-413.15 3.0877 - 0,1951 0.53 5.29
59 n-Dodecanol 11 293.15-493.15 2.1214 2.8166 0.29 18.10
60 Glycerol 6 298.15-423.15 6.2519 6,3629 0.15
A new correlation for thermal conductivity of liquids 1247
Table 1. (contd.)
Present work Latini method
No. of Temp. range
No. Compound points (K) D C 10 4 Deviation (A,) Deviation{%)

61 Ethyl ether 6 193.15 296.15 5.3788 - 4.1946 0.66 1.26


62 Methyl butyl ether 8 193.15 333.15 3.61 l0 3.0464 0.28 6.76
63 Dibutyl ether 11 213.15 413.15 2.7304 - 5.0184 1.68
64 Acetaldehyde 6 193.15-293.15 8.6677 1.4874 0.19
65 n-Propionaldehyde 8 193.15-333.15 5.4837 - 3.1372 0.87
66 Acetone 7 193.15-313.15 6.8034 - 1.9502 0.63 0.84
67 Methyl ethyl ketone 9 193.15 353.15 5.0747 - 2.5331 1.06 1.18
68 Diethyl ketone 8 233.15-373.15 3.4760 1.9379 0.35 1.25
69 Propiorlic acid 9 253.15 413.15 3.8617 1.2606 0.05 5. l I
70 n-Butyric acid 9 273.15 433.15 3.0803 0.9931 0.11 4.90
71 Methyl formate 5 213.15--293.15 9.3722 - 3.5799 0.42 1.04
72 Ethyl formate 6 213.15-313.15 5.9618 - 2.7361 0.38 1.84
73 n-Propyl formate 8 213.15-353.15 4.7135 - 3.3(185 1.07 1.25
74 n-Butyl formate 9 213.15 373.15 3.9481 - 3.2975 1.03
75 Methyl acetate 6 213.15-313.15 6.4865 - 3.3981 0.52 1,38
76 Ethyl acetate 7 213.15-333.15 4.7625 39617 0.68 0.63
77 n-Propyl acetate 9 213.15 373.15 3.9144 2.3850 1.10 2.37
78 n-Butyl acetate 10 213.15 393.15 3,1968 - 1.9912 1.02 1.74
79 Methyl propionate 8 213.15 353.15 4,5286 - 2.2416 1.9(I 1.7l
80 Ethyl propionate 8 213.15 353.15 3,6170 - 1.4826 1.01 1.20
81 Chlorobenzenc 9 233.15 393.15 3.1949 - 3.6428 0.57 4.46
82 Bromobenzene 9 253.14 413.15 2,2874 - 2.6454 0.28 3.66
83 Aniline 7 273.15 423.15 4.0529 - 1.7120 0.45
84 Nitrobcnzene 6 273.15-398.15 2.9337 - 0.5732 0.40
85 Diphenyl 28 330.00-600.00 1.7356 - 0.9443 0.54 12.46
86 Water 10 273.15 363.15 31.2798 9.4816 1.20
Tolal 920 0.98 3.73

eq. (34), Tr,, is the reduced temperature of the mixture, characteristic parameters D and C are determined
n is an adjustable constant characteristic of each mix- (Lei, 19951. We shall report on these results in a n o t h e r
ture. The relation between n and the ratio ALIA2 may paper.
be of the type, n = 2.20A1/A2 (At < A2), so that the
above correlation becomes

CONCLUSIONS
)~m:(Alx~+A2x2+2.20~2xlx2 ) In this paper, a liquid is s u p p o s e d to be c o m p o s e d
of a mixture of microcrystallites and vacancies. A new
correlation for liquid thermal conductivities over wide
(1 -- Trm)0"38 ranges of temperature is p r o p o s e d on the basis of
x (Al -~< A2). (38)
T r~6 significant structure theory and analysis of the radial
distribution function of liquids. This correlation,
Table 2 also shows the correlation results according a t w o - p a r a m e t e r method, can be used to treat inor-
to eq. (37) and the prediction results according to eq. ganic c o m p o u n d s , paraffins, olefins, cycloparaffins,
(38). F o r 52 of the 67 liquid binary mixtures listed (513 aromatic h y d r o c a r b o n s , alcohols, ethers, aldehydes,
data points), the overall average absolute deviations ketones, esters, organics acids and some refrigerants.
for eqs (37) and (38) are 2.76% and 4.41%, respec- F o r pure c o m p o u n d s such as inorganic c o m p o u n d s ,
tively. nitrogen- or sulfur-containing materials and al-
One additional advantage of the present correla- dehydes, and for mixtures consisting of alcohols and
tion needs to be emphasized. According to eq. (23), the aqueous systems, the present correlation shows better
correlation may be applied to calculate the thermal agreement with experimental data than the models
conductivities of liquids under pressure so long as the r e c o m m e n d e d by Reid et al. (1987).
1248 Qunfang Lei et al.

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i.
ooooo ooo oooooo ooo oo ooooooo
~o
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A new c o r r e l a t i o n for t h e r m a l c o n d u c t i v i t y of liquids 1249

. . . . . . . . . . . . . . . . . . . . . . . . . ~C ~ .~ ~ - - -

~ggg g g g g g g g g g g g g g g ~ g g g g ~ ~ ~ =

q q q q q q q q q q q q q q ~ q ~ q q q q q q q ~ ! q q - - q - - q q q q q q q q ~
c ~ o o o o o ~ o ~ o o o o ~ o o o o o o o o o o o o o o ~ o ~ o ~ c c ~ o
I Ill I l l l l Ill I li I

.-~ o .~ _o .-~ _~ .~ o ~ ~.

~ ~ o o o o ~ = = ~ - o ~
1250 Qunfang Lei et al.

~ 0 0 ~ 0 0 o 0 0 o o 0 0 o 0 0 0 o 0 0 0 o 0 0 0
I I I I I I I I

e,i
e-~

b-


A new correlation for thermal conductivity of liquids 1251
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