Journal of Molecular Liquids 224 (2016) 234–239

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Journal of Molecular Liquids

journal homepage: www.elsevier.com/locate/molliq

A new model for the viscosity of liquid short chain (C1–C4) 1-alcohols
over density and temperature based on Lennard-Jones potential
Xiaohong Yang ⁎, Weiling Zhu
Department of Chemistry and Environmental Engineering, Wuhan Polytechnic University, Hankou, Wuhan, 430023, PR China

a r t i c l e i n f o a b s t r a c t

Article history: This work attempts to develop a new model for the viscosity of liquid short chain (C1–C4) 1-alcohols based on
Received 29 August 2016 the Lennard-Jones potential. The model derived a novel equation as the mixed power and exponential function
Received in revised form 13 September 2016 of density and temperature. When the Lennard-Jones potential took the (11.91-6) pattern, the derived equation
Accepted 26 September 2016
was found in good agreement with reliable experimental data reported in literature. The R squared for the equa-
Available online 30 September 2016
tion fitting to the 279 gathered data points that distributed in the ranges: 223.15–476.2 K and 0.1–472.8 MPa, was
Keywords:
≥0.9973. Comparing to other famous theoretical models mentioned, the new model was accurate, simpler, and
Alcohol had theory background and physical meanings for the main terms. All these advantages suggested the success
Viscosity of the developed new model and showed its practical application potentials in the industry associating the
Model alcohols.
Temperature © 2016 Elsevier B.V. All rights reserved.
Density
Lennard-Jones potential

1. Introduction
Short chain 1-alcohol is the most commonly encountered liquid
today, and has gained practical applications in broad areas. Theoretical-
ly, it belongs to the polar small organic molecule system which is inter-
esting for investigating complicated molecular interactions. Its viscosity
has importance in many physical and chemical processes, as well as the
design of unit operation equipment and calculations dealing with alco-
hol flow and reservoir behavior. In order to obtain the knowledge on the
alcohol viscosity, experimental measurement is always the most direct
and effective method. Following this route, a number of tests have
been carried out with advanced instruments in recent decades. In
1980, the interests once were in the alcohol-water mixtures [1,2]. In
1990, the attentions turned to the pure alcohols [3,4]. In recent years, re-
searchers had conducted experiments on the viscosity and relating
properties for more complicated systems [5–9].
As a result of these measurements, considerable viscosity data has
been reported, which quantitatively deepens the knowledge on the al-
cohol. However, there is neither always a possibility to find the desired
data in the literature, nor a method to overcome the disadvantages of
measurement (such as high expense, time consuming, and availability
of appropriate instrument that can carry out test at reservoir condition),
consequently many researchers have developed models to predict the
viscosities of different homologous series. The reported models can be
classified into two categories: the empirical correlation over a range of
⁎ Corresponding author.
E-mail address: yangxhong88@163.com (X. Yang).
temperature and pressure [10,11], and the model based on existing the-
ories [12].
In fact, the correlations can only tell about statistical analysis results
from data. Causation should be inferred from theory. If there is no theo-
ry for a model, it is not clear what is the mechanism for results by the
model. In consideration of the importance of theory, three well-
known theories about viscosity have been established. They are the
free volume theory [13,14], the friction theory [15–17] and the hard-
sphere model [18,19]. In the free volume theory, the viscosity (η) is sep-
arated into two terms: the viscosity in the zero density limit and the re-
sidual viscosity as in other models,
η ¼ η0 þ Δη ð1Þ
The viscosity in the zero density limit (η0) can be approximated by
the viscosity of dilute gas (ideal gas), the residual viscosity (Δη) is calcu-
lated based on the free-volume concept, an approach has been proposed
in order to model the viscosity of Newtonian fluids in the gaseous and
dense states [13,14]. By this concept, the derived equation for the resid-
ual term is
 2  "  3 #
αρ þ PMw αρ2 þ PMw 2
Δη ¼ ι pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi exp B ð2Þ
3RTMw RTρ
where, ρ, P, T, R, Mw denote density, pressure, absolute temperature,
universal gas constant and molecular weight, respectively. B, α and l
are physical parameters, which are characteristics of the molecule. The
free volume theory was shown to accurately represent the viscosity

http://dx.doi.org/10.1016/j.molliq.2016.09.117
0167-7322/© 2016 Elsevier B.V. All rights reserved.
 X. Yang, W. Zhu / Journal of Molecular Liquids 224 (2016) 234–239 235

equations of this model for the viscosity were expressed as:

Nomenclature
   X
ηexp 7
A coefficient ln ¼ aηi ð1=V r Þi ð4Þ
B parameter or coefficient Rη i¼0
C coefficient
F net force  1 =
1
ηexp V =3
2 2

fb binary force ηexp ¼ 6:035  108 ð5Þ

MRT
k Boltzmann's constant
l parameter where, aηi are universal coefficients, independent of the chemical nature
m molecular mass of the compound, and only V0 and Rη are adjustable parameters. The Rη
Mw molecular weight for alkanes [20] and aromatics [21] given by Assael et al. was indepen-
N number of the molecules dent of pressure and temperature, while V0 depended only on
NA Avogadro constant temperature.
P pressure These three theoretical models for viscosity have established rela-
R universal gas constant tionship among the viscosity and thermophysical parameters. However,
Rη adjustable parameters none of them can offer information about the link between viscosity and
r radius intermolecular interaction potential. Knowledge of intermolecular po-
T absolute temperature tential is not only crucial to both understanding and predicting chemical
u potential field thermodynamical properties, but also interesting and important for
U shear velocity many fields ranging from fundamental molecular science to widespread
uw depth of potential well industrial applications. Alcohol is one of the most polar molecules, and
v molar volume its intermolecular potential determines macroscopic properties, includ-
V volume ing the viscosity which behaves the most sensitive to molecular poten-
V0 adjustable parameters tial as it varies over 23 orders of magnitude from the least viscous gas to
vx, vy, vz x, y, z components of molecular velocity the most viscous solid. As a result of these reasons, the development of a
α parameter or coefficient new model upon intermolecular potential for alcohol ought to become
β parameter or coefficient one of the key problem in its fields.
ζ geometrical factor In present work, the authors will firstly adopt a different theoretical
Δη residual viscosity approach from others, which bases upon molecular interaction poten-
η viscosity tial; and then develop a new model so as to derive a mathematical ex-
η0 viscosity in the zero density limit pression for the viscosity of short chain (C1–C4) alcohol; finally,
κr friction coefficient evaluate the accuracy and explanatory ability of the new model with re-
κa friction coefficient liable experimental data from literature.
κrr friction coefficient
ρ density 2. Theoretical approach
σ Lennard-Jones' constant
φ molecular binary potential 2.1. Averaged intermolecular separation
φσ Lennard-Jones' constant
In a liquid, the averaged intermolecular separation between two
molecules alters with volume V or density ρ. When the volume occupied
by each molecule is considered as the sphere of radius r, the following
equations are able to estimate the averaged site-to-site intermolecular
behavior of various hydrocarbons over wide temperature and pressure
separation 2r from the macroscopic volume V or density ρ,
ranges in the gaseous, liquid and dense states.
The friction theory (f-theory) for viscosity modeling is based on
4
principle of mechanics and thermodynamics [15]. In this theory, the vis- V ¼ N πr 3 ð6Þ
3
cosity in the zero density limit (η0) is treated the same as the free vol-
ume theory, but the residual viscosity comes from mechanical friction, Nm m
which is related to the van der Waals attractive pressure (pa) and repul- ρ¼ ¼ ð7Þ
V 4π 3
sive pressure (pr). For a simple molecular structure hydrocarbon, it was r
3
shown that the f-theory models [16] consisting of a linear relation to pa
and a quadratic relation to pr can accurately represent the viscosity over where, m denotes the molecular mass. N is the total number of the mol-
wide ranges of temperature and pressure, ecules contained in volume V.

Δη ¼ κ a pa þ κ r pr þ κ rr p2r ð3Þ

where κr, κa, and κrr are the temperature dependent friction coefficients.
The f-theory has also been applied to the viscosity of alcohols [17].
The hard-sphere model was developed [18,19] for simultaneously
correlating self-diffusion, viscosity and thermal conductivity of dense
fluids. The viscosity of the fluid expressed in reduced form of Vr = V/
V0 with V0 the close-packed volume and V the molar volume, was as-
sumed to be directly proportional to the value given by the exact
hard-sphere theory. The proportionality, called roughness factor Rη, ac- Fig. 1. A molecule in uniform liquid accepts symmetric forces from its neighbors around it,
counts for molecular roughness and departure from sphericity. The and unsymmetric forces from its half neighbor at boundary.
236 X. Yang, W. Zhu / Journal of Molecular Liquids 224 (2016) 234–239

Table 2
The fitted coefficients and the R squared for Eq. (17) to the gathered data from relevant
references.

Alcohol Points A B C R2

Methanol 118 2.102 × 10−5 1.686 × 10−3 6.259 × 10−10 0.9974

Ethanol 57 1.142 × 10−5 2.813 × 10−3 1.573 × 10−9 0.9973
l-Propanol 55 6.997 × 10−6 3.135 × 10−3 1.318 × 10−9 0.9981
1-Butanol 49 2.087 × 10−6 4.447 × 10−3 2.574 × 10−9 0.9995

At the boundary, the unsymmetric force normal to the boundary

surface is able to be approximated to the summation of the binary forces
from the nearby molecules, then the following equation can be
obtained,

Fig. 2. The surface of alcohol viscosity as function of density and temperature by Eq. (17).
F ¼ ζ fb ð9Þ

where, fb denotes the binary force of molecules, the ζ is a geometrical

2.2. Symmetric molecular interactions
For a spatially uniform liquid at thermodynamic equilibrium, it is
usually too complex to analytically express the potential field (u) of in-
termolecular interactions due to the huge number of molecules. Consid-
erable approximations must be made during the derivation of the
relation between physical parameter and intermolecular interaction. In-
side the liquid, it can approximate that the molecule accepts symmetric
forces around it due to the uniformity, therefor the total force (F) are ap-
proximately zero (Fig. 1) [22]. At the boundary, however, the molecule
receives unsymmetric forces from its half neighbor to restrict it inside
the liquid. According to F = −▽u, the potential field on each molecule
in the liquid is thus simplified as a variable independent of molecular
spatial coordinates, and a step function at the boundary. This property,
just like a potential well of flat bottom, is expressed by the following
factor. For example, for the geometry presented in Fig. 1, ζ ≈
2cosθ + √3cos2θ. Here, θ is the angle between the nearby binary and
net force.
Integrating Eq. (9) across the boundary using spatial coordinates as
integral variables, it yields.
uw ¼ −ζ φinside ð10Þ
where, φinside is the amount of the binary potential in the liquid that has
an average molecular separation distance 2r. If the binary potential has
been mathematically modeled, φinside then equals the value of the model
at 2r.
A famous model for the binary potential as a function of molecular
separation is the Lennard-Jones [23], which has the following form for
the 3β–3α pattern,
 3β  3α

equation. σ σ
φ ¼ φσ − ð11Þ
d d
 
−uw within liquid
u¼ ð8Þ where, d presents the intermolecular separation, φσ and σ are the
0 without liquid
Lennard-Jones' constants. This equation is based on the site-to-site
that ignores the effects of molecular configuration and compound.
where, u denotes the potential field on molecule, uw is the variable pre- When α = 2 and β = 4, it returns to the standard 12–6 pattern
senting the depth of the potential well. Lennard-Jones potential.

Table 1
The sources of experimental alcohol viscosity data.

Alcohol Temperature (K) Pressure (MPa) Density (Kg/m3) Author No. of points

Methanol 295.00–323.193 0.1–27.05 762.7–810.6 Assael et al. [3]. 26

298.18–323.15 0.1–472.8 762.77–965.2 Isdale et al. [1] 36
303.13–318.15 0.1 769.2–782.3 Peshwe et al. [6] 4
350.7–476.2 10–40 576.84–777.36 Ono et al. [9] 12
293.15–323.15 0.1 770.1–793.9 Dikio et al. [8] 4
303.15–373.15 Saturated 711–783 Perry [24] 8
293.15–353.15 0.1–100 732–858 Zeberg [5] 24
273.15–333.15 0.1 753.2–809.7 Kumagai [25] 4
Ethanol 298.17–323.129 0.1–27.56 763.1–804.0 Assael et al. [3]. 27
293–323 0.1 760.5–791 Khattab et al. [7] 7
350.7–476.2 10–40 582.85–775.75 Ono et al. [9] 8
273.15–333.15 0.1 754–806.1 Kumagai [25] 4
273.15–373.15 Saturated 716–806 Perry [24] 11
l-Propanol 298.17–323.17 0.1–27.86 779–818.5 Assael et at. [3]. 28
350.7–373.2 10–40 741.54–789.02 Ono et al. [9] 8
293.15–323.15 0.1 773.0–804.5 Dikio et al. [8] 4
273.15–333.15 0.1 770.7–819.6 Kumagai [25] 4
273.15–373.15 Saturated 743–819 Perry [24] 11
1-Butanol 298.2–323.2 0.1–28.27 786.2–823.9 Assael et al. [3]. 29
293.15–323.15 0.1 787.6–811.5 Dikio et al. [8] 4
223.15–373.15 Saturated 753–845 Perry [24] 16
Overall 223.15–476.2 0.1–472.8 576.84–965.2 9 references 279
 X. Yang, W. Zhu / Journal of Molecular Liquids 224 (2016) 234–239 237

shear surface. Therefore, only the part of molecules nearest the shear
surface interchanges molecular momentum through random motion
in the y-direction perpendicular to the shear surface. Upon these con-
siderations, the net shear stress from the momentum transfer is
expressed as.

2r ∞
τ≈ fdvx dvy dvz ∫ 0 mUvy
b rffiffiffiffiffiffiffiffiffiffi ð14Þ
ζφ mkT Ur
¼ n exp −
kT 2π b

Here, U denotes the shear velocity to the liquid layer considered, b

the thickness of the layer, r the radius of the averaged volume occupied
by each molecule in the liquid.
Realizing that the shear rate between the layer equals the ratio of U
to b,

• U
Fig. 3. Measured viscosity against calculated viscosity for the 279 data points of methanol γ¼ ð15Þ
(Circle), ethanol (Diamond), 1-propanol (Cross), and 1-butanol (Triangle). b

the following equation of viscosity (η) for the liquid is obtained,

As mentioned above, the averaged intermolecular separation is 2r in
rffiffiffiffiffiffiffiffiffiffiffiffiffi  
the liquid, which means d = 2r in the case. When the density is chosen 2mkT ζφ
as independent variable through Eq. (7), the Lennard-Jones potential at η¼ exp − nr ð16Þ
π kT
averaged intermolecular separation is written as
" β  α # This equation indicates that the viscosity is as an exponential func-
ρ ρ tion of the averaged intermolecular potential, and that the correlation
φ ¼ φσ − ð12Þ
ρσ ρσ for the viscosity of the liquid is able to be construct under the guidance
of the intermolecular potential models. Inversely, if the viscosity as
where, ρσ = 6m/(πσ3), denotes a characteristic density at which the po- function of density and temperature is given, the potential could be es-
tential equals zero. timated via this equation. By this means, the viscosity points out a new
way to understand the molecular potential in the liquids.
2.3. Distribution function for the symmetric liquid Substituting the density dependent Lennard-Jones' potential Eq.
(12) into Eq. (16) and absorbing the geometrical factor into the coeffi-
For the above mentioned symmetric liquid under the potential well cients, it yields,
(Eq. (8)), a molecule in it can moves freely just like in the ideal gas, since
pffiffiffi 2

1 α 
the net force is considered as zero. Therefore, the following formula of η ¼ A T ρ =3 exp Bρ −Cρβ ð17Þ
Maxwell-Boltzmann distribution function in thermal equilibrium was T
proposed,
where A, B, C are coefficients independent of density and temperature.
2 3
1  2  In this equation, two core mechanisms have been involved: the mo-
 m 32 m vx þ v2y þ v2z  uw mentum transfer due to molecular transportation which is achieved
6 2 7
f ¼n exp4− 5 ð13Þ through the term in the form of root square of temperature multiplying
2πkT kT
2/3th power of density, and the statistical effect of molecular potential
realized via the exponent of the ratio of averaged intermolecular poten-
where n = N/V denotes the molecule density of the system, k is tial to averaged kinetic energy. This equation also represents a new
Boltzmann's constant, T is absolute temperature. vx, vy, vz are the x, y, model of viscosity as a function of temperature and density, which is ex-
z components of molecular velocity. pected to be applicable to the liquid short chain 1-alcohols.

2.4. Viscosity for the symmetric liquid 3. Results and discussion

Based on the above Maxwell-Boltzmann distribution function and
following Yang's approximation [22], the shear stress in the liquid is cal-
culated by the momentum transfer across shear surface. In the liquid,
the steric resistance forbids most molecules to get across the shear sur-
face through Brownian random motion except the ones nearby the
3.1. Viscosity surface
According to Eq. (17), the alcohol viscosity as function of density and
temperature was numerically calculated as Fig. 2, when the coefficients
took the values A = exp(−10.77) = 2.102 × 10−5, B = 1.686 × 10−3,

Table 3
Characters of author's new model comparing to the three famous ones.

Theory Required equations Fitted coefficients Required inputs Bases

This work 1 3 T, ρ Distribution function and LJ potential function

Free volume theory 1+ 3+ T, ρ, p, Mw Viscosity in the zero density limit, free-volume concept, and EoS
Hard-sphere theory 2 ≥2 T, V, Mw Hard-sphere theory
Friction theory 4+ 7+ T, p, Mw Viscosity in the zero density limit, mechanical friction, and EoS

+ presents the additional requirements of either equations or constants in the zero density limit.
238 X. Yang, W. Zhu / Journal of Molecular Liquids 224 (2016) 234–239
C = 6.259 × 10−10, α = 2 and β = 3.970, as well as T and ρ varied from
220 to 470 K and 570 to 970 Kg/m3 respectively. It showed that the vis-
cosity increased with density at fixed temperature but decreased with
temperature at fixed density.
3.2. Evaluation
In order to evaluate the new model in broader temperature and
pressure ranges, the authors of this paper gathered experimental viscos-
ity data from references. They were summarized in Table 1, which over-
all had 279 data points covering temperature and pressure ranges:
223.15–476.2 K, 0.1–472.8 MPa for the four short chain 1-alcohols:
methanol, ethanol, l-propanol, and 1-butanol.
For quantitatively presenting evaluation result, numerical fitting
method was employed in the procedure: at first Eq. (17) was fitted to
the experimental data obtaining the coefficients via least square meth-
od, and then theoretical data were calculated with the fitted coefficients
and Eq. (17), finally the statistic coefficient R squared between calculat-
ed and measured data was determined to evaluate the model. In the
case of this work, the value of the R squared demonstrates the goodness
of the fit, and R2 = 1 means the 100% of the variation of the experimen-
tal viscosity data is explained by the fitted trend line of the new model.
The above procedure was executed using the software named
TableCurve 3D v4.0. It was empirically found that an optimal fit can be
achieved as α = 2 and β = 3.97 for all the four short chain 1-alcohols.
These amounts means that a (11.91–6) pattern Lennard-Jones' potential
suits the C1–C4 short chain 1-alcohols. This pattern is very close to the
commonly used 12–6 pattern.
The finally fitted results for the gathered data to Eq. (17) were listed
in Table 2, which indicated that the R squared for the four alcohols very
closely approached 1, suggesting not only the good fits to the experi-
mental data, but also a satisfactory explanation to the variation of the
viscosity. The goodness can also be illustrated by the plot (see Fig. 3)
of calculated viscosity against measured viscosity of the 279 data points
for methanol, ethanol, l-propanol, and 1-butanol. All the points fairly lo-
cated along the diagonal line, certifying the success for the new model
to describe the gathered experimental data.
The goodness may also propose that the new model remained the
core intrinsic mechanisms and laws that govern the variation of viscos-
ity over temperature and density while deriving the formula. As stated
above, the intrinsic mechanisms reveal themselves as the exponent of
the ratio of averaged intermolecular potential to kinetic energy, and
the term of root square of temperature multiplying 2/3th power of den-
sity in Eq. (17).
In addition to the above quantitative evaluation, a comparison of
major characters of the new model of this work with the aforemen-
tioned three famous theories was also indicted in Table 3. The compar-
ison clearly showed the simplicity and theoretical background of the
author's model with least required equations and input variables.
In review of the evaluation and comparison, the author's new model
has been demonstrated the good agreement with the experimental data
from literature, the high explanatory ability, the simplicity comparing
with other models in question, and the theoretical background. All
these advantages suggest the success of the author's new model apply-
ing to the short chain 1-alcohols.
3.3. Limitation
It has been showed that the developed new model suits the viscosity
of the short chain 1-alcohol in the temperature and pressure ranges:
223.15–476.2 K, 0.1–472.8 MPa. In addition, authors of this paper may
also expect that it would be applicable to other small molecule organic
liquids by altering the model's coefficient. However, it cannot hope
that the model is applicable to the fluids composed of macro molecules
since the Lennard-Jones potential bases on the site-to-site assumption.
4. Conclusion
In summary of this work, a new model for the viscosity of liquid
short chain (C1–C4) 1-alcohols has been developed based on the
Lennard-Jones potential. In the model, a novel equation for the viscosity
of alcohol was derived as the mixed power and exponential function of
density and temperature, by means of introducing the Lennard-Jones
potential into the calculation of the averaged intermolecular potential
function. When the Lennard-Jones potential took the (11.91-6) pattern,
the derived equation was found in good agreement with reliable exper-
imental data gathered from literature. The R squared for the model
fitting to the 279 gathered data points that distributed in 223.15–
476.2 K temperature and 0.1–472.8 MPa pressure ranges, was
≥0.9973, the value very close to 1, implying the accuracy and high ex-
planatory power of the new model. Comparing to other famous theoret-
ical models in question, the new model of this paper was simpler, and
had theoretical background and physical meanings for the main terms.
All these advantages suggest the success of the developed new model
and show practical application potentials in the industry associating
alcohols.
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