Fuel 85 (2006) 107–113

www.fuelfirst.com

An empirical approach in predicting biodiesel viscosity

at various temperatures
Kanit Krisnangkuraa,*, Tawatchai Yimsuwanb, Ratanachai Pairintraa
a
Biochemical Technology Division, School of Bioresources and Technology, King Mongkut’s University Thonburi, Toongkru, Bangkok 10140, Thailand
b
The Joint Graduate School of Energy and Environment at King Mongkut’s University Thonburi, Toongkru, Bangkok 10140, Thailand
Received 21 November 2003; received in revised form 15 February 2005; accepted 15 February 2005
Available online 9 June 2005

Abstract
A thermodynamic model is proposed for the determination of kinematic viscosities of saturated fatty acid methyl esters (FAMEs) of
various chain lengths at different temperatures. The linearity of the natural logarithm of viscosity-carbon number, plot is limited to a narrow
carbon number range. The predicted viscosities of FAMEs of C12:0–C18:0, which are commonly found in vegetable oils and used as
biodiesels, agree well with the experimental values. The highest difference is 0.354 cSt (5.60%), for methyl stearate at 40 8C. When the
proposed method for viscosity calculation of saturated FAMEs are used in combination with the methods for viscosities of biodiesel
the mixtures, the predicted viscosities agree well with the values reported in the literatures and the measured values. The differences between
the predicted viscosities and those reported in the literatures (at 40 8C) are 1.08 to 8.56% (for eight different vegetable oil methyl esters). The
differences between the predicted viscosities and the measured values for coconut methyl esters, at 25, 40 and 50 8C are 9.20, 5.53 and 5.57%,
respectively. The differences are slightly higher than those of palm oil methyl esters (4.48, 2.06 and 2.48%, respectively).
The proposed method can also be applied to predict the viscosities of free fatty acids and it is speculated it may be applied to other
homologous series as well.
q 2005 Elsevier Ltd. All rights reserved.

Keywords: Biodiesel; Fatty acid methyl ester; Temperature; Viscosity

1. Introduction
Viscosity (m) has been used extensively in the petroleum
industry for the calculation of liquid transportation through
the pipeline. Due to the complexity of each petroleum
fraction whose composition cannot be determined at present
time, several empirical methods were proposed for viscosity
prediction of different petroleum fractions [1 and ref. there
in]. Viscosities of hydrocarbon mixtures, at a specified
temperature, can be estimated from their densities and
average molecular weights [1,2]. Riazi and Al-Otaibi [3]
proposed a method (Eq. (1)) for estimation of viscosity of
liquid hydrocarbons and petroleum mixtures at various
temperatures from its refractive index (I).
* Corresponding author. Tel.: C66 470869399; fax: C66 470869399.
E-mail address: kanitkrsnk@yahoo.com (K. Krisnangkura).
0016-2361/$ - see front matter q 2005 Elsevier Ltd. All rights reserved.
doi:10.1016/j.fuel.2005.05.010
1 B
ZAC (1)
m I
where A and B are constants specific for each compounds.
Although Eq. (1) looks simple, methods for obtaining the
values of A and B in Eq. (1) are complicate. They vary with
molecular weight, specific gravity, boiling temperature and
refractive index of the compound.
Due to the diminishing reserves and soaring price in
petroleum fuel, attempts are being made to find alternative
fuels for both diesel and gasoline engines. Neat vegetable
oils were primarily considered as alternatives for diesel fuel
but their very high viscosity, at room temperature, made
them unsuitable in diesel engines. Methyl esters (or esters of
lower alcohols) of plant or animal oils (known as biodiesel)
are very much lower in viscosities, than the neat oils, are
promising alternatives and have been commercialized in
many countries around the world. One of the most
conspicuous differences between vegetable oil and biodiesel
is viscosity. Its effect on the atomization process is
described by Msipa et al. [4]. Atomization is the first
stage of combustion in the diesel engine. Oxygen in the air
108 K. Krisnangkura et al. / Fuel 85 (2006) 107–113
will react rapidly with fuel on the outer surface of the oil
droplet and releases a tremendous amount of heat to the
surrounding. This will initiate other competitive reactions,
such as charring or coking and polymerization. Thus, higher
viscous liquids, which tend to form larger droplet size, may
enhance the polymerization reaction, especially oil of high
degree of unsaturation. The problems of using high viscosity
oil in diesel engine have long been recognized [5,6].
Although, viscosity is an important factor for biodiesel,
methods for estimation of biodiesel viscosities are few
[7–10] compared to those for petroleum.
There were several methods for predicting the viscosity
of fatty acids but few for fatty acyl esters (see Ref. [7] and
references there in). Viscosity of individual saturated fatty
acid methyl ester (FAME) and the mixture, at 40 8C, are
estimated according to Eqs. (2) and (3), respectively [7].
m Z 1:05 !10K4 M 2 K 0:024M C 2:15 (2)
X
n
ln m Z yi ln mi (3)
iZ1
where yi is the mass fraction.
The relationships between viscosity and carbon number
of fatty acids or their derivatives were only reported by
Fisher [8]. Although, Fisher was very successful in
predicting several physical properties of n-fatty acids on
their limiting properties, his method was not very accurate
on predicting the viscosity.
As pointed out earlier, viscosity has been used
extensively in the petroleum industries, and there are
several methods that correlate viscosities of different
petroleum fractions with temperature [1 and ref. there in].
The best known equation that correlates liquid viscosity and
temperature is the Andrade Equation (Eq. (4)) [9].
B
m Z Ae T (4)
where A and B are constants. T is absolute temperature. Eq.
(4) can be used for predicting viscosity up to approximately
the normal boiling point of the liquid. Comparing Eq. (4) to
the reaction rate, an equation (Eq. (5)) similar in form to Eq.
(4) has been proposed by Eyring [10].
NA h KDGvis
mZ e RT (5)
V DGvis
where NA, V, h and R are Avogadro’s number, molecular
volume, Plank’s and gas constants, respectively. DGvis is the
free energy of activation for flow.
Several modifications of Eq. (4) have been made to
extend the temperature range [1,11 and ref. there in].
Makhija and Stairs [12] modified Eq. (4), for associated
liquids, by adding a third variable parameter as shown in
Eq. (6).
B postulated that this phenomenon will also be applied to the
ln m Z m C (6)
T K T0
where m, B and T0 are constants with obscure meanings
[13]. Liew et al. [13] modified Hildebrran’s equation to Eq.
(7) to calculate the fluidities (f, reciprocal of viscosity) of
FAMEs (C7:0–C12:0).
 
E=T M
f Z Ae K1 (7)
ðk C lTÞV0
where k and l are the correlation coefficients of density with
respect to temperature. V0 and M are intrinsic volume and
molecular mass. A and E are related to Eyring’s equation of
activation for flow (Eq. (5)).
The effect of temperature on viscosity was also proposed
by Liew et al. [14] as shown in Eq. (8).
log m Z a C bT (8)
where a and b are constants. Latter work, Liew et al. [13]
abandoned Eq. (8) and used Eq. (6) to predict the viscosity
of FAMEs. Although, Liew et al. [13] are the first group to
correlate fluidity (viscosity), molecular mass and tempera-
ture in the same equation, Eq. (7), there are five parameters
in the equation. Furthermore, these parameters have to be
determined independently.
In this study, DGvis in Eq. (5) is assumed to be linearly
related to the carbon number (of the same homologous
series) and it is expanded to determine viscosity of saturated
fatty acid methyl esters at different temperatures.
2. Hypothesis
In general, viscosity may be considered as the integral
of the interaction forces of molecules. When the
interactions among molecules are very strong, they tightly
hold together and are unable to slide over each other, and
the compound is called a solid. When energy or heat is
applied up to a certain level, molecules can then slide
over each other or become melted. Initially, they slide
over each other very slowly. If the amount of heat or
temperature greatly exceeds the melting point, they move
pass each other very rapidly and the liquid becomes less
viscous. The effect of temperature on the viscous flow or
viscosity of liquid is described in Eq. (9) or its
logarithmic form.
m Z AeK RT (9)
where AZNAh/V in (5).
As aforementioned, molecular motion or flowing of
liquid depends on the interactive force among molecules, it
is speculated that, for n-alkanes or any other functional
homologous series, the molecular interactive force will
increase as the chain length is increased. This phenomenon
is widely observed in the melting point, boiling point, and
retention time in gas and liquid chromatography. Thus, it is
viscosity of liquid as well and it can be described
 K. Krisnangkura et al. / Fuel 85 (2006) 107–113 109

mathematically as follows: 3.1.3. Determination of the four constants of Eq. (13)

At constant T, Eq. (13) is reduced to Eq. (14).
DGvis Z DGo C zdG (10)
ln m Z a 0 C b 0 z (14)
where DGo is the free energy of activation for viscous flow
of the hypothetical molecule of zero carbon atom, DG is the where
increment in free energy per carbon atom and z is the c
number of carbon atom of the homologous series. a0 Z a C (15)
T
In basic thermodynamics, DG can be expanded to:
and
DG Z DH K TDS (11) d
b0 Z b C (16)
Combining Eqs. (9)–(11) gives Eq. (12). T
DHo DSo zdH zdS Thus, a and c are the intercept and slope of the a 0 KTK1
ln m Z ln A K C K C (12) plot. Similarly, b and d are the intercept and the slope of the
RT R RT R
b 0 KTK1 plot.
or Alternatively, if z is constant, Eq. (13) is reduced to Eq.
c zd (17)
ln m Z a C bz C C (13)
T T c 00
where ln m Z a 00 C (17)
T
DSo dS where
a Z ln A C ; bZ ;
R R
a 00 Z a C bz (18)
DHo dH
c ZK ; d ZK
R R and
c 00 Z c C zd (19)
00
The a and b values are obtained by a -z plot and the c
3. Experimental and d values are obtained by the c 00 -z plot.

3.1. Materials
4. Results and discussion
Refined palm oil and coconut oil were obtained from
supermarket in Bangkok. Sodium methoxide was purchased 4.1. Data in the literature
from Sigma Chemical (St. Louis, Mo). Anhydrous methanol
was purchased from LabScan Asia Co. (Bangkok, Thailand) As it was mentioned in the hypothesis section that the
. molecular interactive force increases as the chain length is
increased. The relationship can be described mathemat-
ically, at a constant temperature, as shown in Eq. (14), In gas
3.1.1. Transmethylation of vegetable oils chromatography, it is observed that the linear free energy
Transmethylation was carried out as described by
Srimamahannop and Krisnangkura [15] with a slight 4.00
modification. The molar ratio of oil to methanol was 20°C
3.50
increased to 1:20. The reaction was allowed to proceed 30°C
slightly longer to be sure that there was no trace of 3.00
Viscosities (cSt)

triglyceride left in the reaction mixture. The final product 2.50 40°C
was checked by TLC plate coated with siliga gel G (eluted 2.00
50°C
with hexane-ethyl acetate-acetic acid, 90:10:1). 60°C
1.50 70°C
80°C
1.00
3.1.2. Gas chromatographic analysis
Fatty acid methyl esters (FAMEs) compositions of the 0.50
oils were determined on an Rtx-2330 capillary column 0
(30 m!0.25 mm id. Film thickness 0.25 mm, Restex Co., 4 6 8 10 12
Ca) connected to a Shimadzu Model 17A gas chromato- Carbon numbers of the acids
graph (Shimadzu Corp., Tokyo, Japan) with a flame Fig. 1. Kinematic viscosities of short chain FAMEs (C4:0–C12:0) at different
ionization detector. Data were recorded on CR4-A data temperatures. Solid lines are kinematic viscosities obtained from Liew et al.
processor from the same company. [13] and dash lines are values generated by using Eq. (20).
110 K. Krisnangkura et al. / Fuel 85 (2006) 107–113

relationship in Eq. (10) is limited to a narrow range of

K0.001
0.007
0.017
0.026
0.016
carbon numbers and the lowest number is 5 or higher[16],
but there is no report on the free energy relationship in the

80
viscosity of liquid. As it was mentioned above, it is
speculated that linear free energy relationship should be

K0.003
0.005
0.013
0.021
0.002
observed in the viscosity of liquid as well and the

75
relationship may also be limited to a narrow carbon chain
length. Thus, FAMEs are divided into two groups,
K0.008
0.003
0.011
0.012
K0.009
C6:0–C12:0 and C12:0–C18:0. Because viscosity of a liquid
can be expressed in several units, the kinematic property
70

agree well with Eq. (13). Therefore, centistroke (cSt) is used

in this study. The complete data of FAMEs densities and
K0.011
0.004
0.007
0.005
K0.026
dynamic viscosities are converted to kinematic viscosities
The differences between the calculated viscosities (cSt) of short chain FAMEs (by Eq. (20)) and the values reported by Liew et al. [13] at different temperatures

65

by dividing the dynamic viscosity by the density. The four

numeric constants of Eq. (13) are determined by solving
K0.014
K0.002
0.004
0.023
K0.042

Eqs. (15) and (16) or Eqs. (18) and (19) or as described by

Krisnangkura et al. [17]. The R2 values of the intercept and
60

slope are 0.9956 and 0.9978, respectively. Substituting these

four numeric values into Eq. (13), Eq. (20) is obtained and it
K0.016
K0.013
0.003
K0.006
K0.058

is used for calculation of viscosity of short chain FAMEs at

55

different temperatures.
K0.019
K0.016
0.002
K0.011
K0.072

492:12 108:35z
ln m Z K2:915 K 0:158z C C (20)
T T
50

The kinematic viscosities of FAMEs generated by Eq.

K0.019
K0.005
0.002
K0.014
K0.084

(20) at different temperatures are agree well with those

reported by Liew et al. [13] as shown in Fig. 1. All the
45

differences between the calculated viscosities and the

experimental values reported by Liew et al. [13] are
K0.021
K0.012
K0.004
K0.024
K0.106

summarized in Table 1. The highest viscosity differences

40

for FAMEs of C6:0, C7:0, C8:0, C10:0, and C12:0 are K0.026,
K0.016, 0.107, 0.095 and K0.116 cSt, respectively. Results
K0.025
K0.010
0.002
K0.023
K0.115

in Table 1 suggest the linear relationship between ln m and z

(C6:0–C12:0) as described by Eq. (14).
35

For FAMEs of longer chain length (C12:0–C18:0) which

are widely found in vegetable oils, the available viscosity
K0.026
K0.009
0.013
K0.015
K0.116

data at different temperatures are scarce.

30

The data reported by Swern [18], although not complete,

are sufficient for determination of the numeric values of the
K0.016
K0.009
0.010
K0.006
K0.096

four constants. The missing viscosities of FAMEs from

C16:0–C18:0 at 20 8C are generated by Eq. (14) from the data
25

of C12:0–C15:0. The numerical values for a 0 and b 0 values of

Eq. (14) at 20 8C are K0.8141 and 0.1747, respectively. The
K0.023
K0.005
0.031
0.011
K0.054

numeric values of Eq. (13) (a, b, c and d) are solved as

described by Krisnangkura et al. [17]. The R2 values of the
20

intercept and slope are 0.9834 and 0.9921, respectively.

K0.022
0.003
0.061
0.043
0.001

Substituting these numeric values into Eq. (13) yields Eq.

Temperature (8C)

(21), which is used to predict the viscosity of saturated

15

FAMEs at different temperatures.

K0.008
0.013
0.107
0.095
0.086

403:66 109:77z
ln m Z K2:177 K 0:202z C C (21)
10

T T
The kinematic viscosities of long chain FAMEs (at 20,
FAMEs
Table 1

40 and 70 8C) generated by Eq. (21) agree well with those

(z)

10
12

reported by Swern [18].

6
7
8
 K. Krisnangkura et al. / Fuel 85 (2006) 107–113 111

Table 2 less accurate but it encloses both temperature and carbon

Predicted viscosities (cSt) of FAMEs of C12:0 to C18:0 at 20, 40 and 70 8C number of fatty acid in the same equation. Furthermore, they
z 20 8C 40 8C 70 8C are directly related to basic thermodynamic parameters
12 3.559 (0.041) 2.446 (0.017) 1.513 (K0.013) which may allow further refinement of the equation. It is
13 4.228 (0.082) 2.838 (K0.058) 1.702 (0.018) speculated that Eq. (13) may be extended to cover other
14 5.024(0.086) 3.292 (K0.062) 1.915 (0.035) functional homologous series.
15 5.970 (0.120) 3.819 (K0.069) 2.155 (0.075)
16 – 4.431 (K0.111) 2.424 (0.076)
17 – 5.140 (K0.210) 2.728 (0.062) 4.2. Viscosities of FAMEs of vegetable oils
18 – 5.964 (K0.354) 3.069 (0.041)

The differences from those reported by Swern[18] are given in the Vegetable oils generally contain both saturated and
parentheses. unsaturated fatty acids. Attempts to assign the equivalent
carbon number similar to that used in gas chromatographic
Table 2 shows the calculated viscosity values of FAMEs system were unsuccessful. This is probably due to the
by Eq. (21). The different values to those published by different forces or mechanistic interaction between these
Swern [18] are included in parentheses. The highest two systems. Therefore, for unsaturated FAMEs, Eq. (9) or
difference is K0.354 cSt for methyl stearate at 40 8C. Eq. (17) is used to predict the viscosity of individual
Results in Table 2 suggest the linear relationship between FAMEs. Using the viscosity data reported by Swern [18],
ln m and z (C12:0–C18:0) as described by Eq. (14). the four unsaturated FAMEs, which are widely found in
The form of Eq. (13) can also be applied for nature can be described by Eqs. (23–26).
determination of the viscosity of fatty acids. By using the
available viscosity data (50, 60 and 70 8C) of Liew et al. 2051:5
ln m18:1 Z K5:03 C (23)
[14], the numeric values of the four constants of Eq. (14) are T
solved according to Krisnangkura et al. (17). The R2 value
of the intercept and slope are 0.7883 and 0.9091, 1822:5
ln m18:2 Z K4:51 C (24)
respectively. After substitution of these numeric constants T
into Eq. (13), Eq. (22) is obtained and is used for
1685:5
determination of free fatty acid viscosities at different ln m18:3 Z K4:18 C (25)
temperatures. T

657:12 173:31z
ln m Z K2:496 K 0:326z C C (22)
T T
The percent differences between calculated viscosities
and those reported by Liew et al. [14] at temperatures
20–70 8C are summarized in Table 3. Higher differences are
found at lower temperature limit except those of dodecanoic
acid. The highest difference is 3.8% for tetradecanoic acid at
60 8C.
Although viscosity of a liquid can be determined by
Makhija and Stairs’ equation (Eq. (6)), which uses only
three parameters and is speculated to be more accurate than
the values obtained by using Eq. (13), Eq. (6) only correlates
individual FAMEs with temperature and each FAME has its
own numeric constants. In addition, it was pointed out by
Liew et al. [13] that the physical meanings of the three
parameters are obscure. The proposed method is slightly
Table 3
Percent differences between calculated viscosities of free fatty acids by Eq. (22) and those reported by Liew et al. [14]
2326:2
ln m22:1 Z K5:42 C (26)
T
For non-associated liquid mixture, its viscosity can be
calculated according to Eq. (3) [7].
Tables 4 and 5 summarize the viscosities of coconut and
palm oil methyl esters calculated from their components.
The experimental values were determined with the kind
service of the Science Department, Ministry of Science,
Technology and Environment. The differences between the
calculated and experimental values are relatively fluctuated
for coconut methyl esters (about 5.53–9.20%) while those of
palm oil methyl esters are slightly lower (2.06–4.48%). The
differences are higher for coconut methyl esters, especially
at 25 8C. This might be due to the high solidification point of
the esters. Also the average errors were higher for coconut
methyl esters than those of palm oil methyl esters. Allen
et al. [7] also founded that the differences between

Fatty 20 8C 25 8C 30 8C 35 8C 40 8C 45 8C 50 8C 55 8C 60 8C 65 8C 70 8C
acids
z
8 K2.79 0.47 K1.24 K K1.10 – K0.62 – K1.73 – K1.00
10 – – – 1.59 1.27 0.76 0.96 1.19 1.81 0.51 K0.32
12 – – – – – – 0.01 0.50 1.38 2.65 3.65
14 – – – – – – – – K3.80 K2.99 K1.21
112 K. Krisnangkura et al. / Fuel 85 (2006) 107–113

Table 4
Predicted viscosities of coconut oil methyl esters at different temperatures

FAMEs 25 8C 40 8C 50 8C
xi ln mi xi lnmi ln mi xi lnmi ln mi xi lnmi
8:0 0.048 0.506 0.024 0.300 0.014 0.174 0.008
10:0 0.062 0.838 0.052 0.597 0.037 0.449 0.028
12:0 0.527 1.171 0.617 0.894 0.471 0.724 0.382
14:0 0.175 1.503 0.263 1.192 0.209 1.000 0.175
16:0 0.074 1.836 0.136 1.488 0.110 1.275 0.094
18:0 0.024 2.168 0.052 1.786 0.043 1.550 0.037
18:1 0.076 1.847 0.140 1.517 0.115 1.314 0.100
18:2 0.014 1.604 0.022 1.311 0.018 1.131 0.016
Sxilnm 1.000 1.307 1.018 0.840
m 3.696 2.767 2.316
Measured 4.035 2.929 2.453
% Differences 9.20 5.53 5.57

Table 5
Predicted viscosity of palm oil methyl esters at different temperatures.

25 8C 40 8C 50 8C
xi ln mi xilnmi ln mi xilnmi ln mi xilnmi
12:0 0.003 1.171 0.004 0.894 0.003 0.724 0.002
14:0 0.009 1.503 0.014 1.192 0.011 1.000 0.009
16:0 0.380 1.836 0.698 1.488 0.565 1.275 0.485
18:0 0.061 2.168 0.132 1.786 0.109 1.550 0.095
18:1 0.439 1.847 0.811 1.517 0.666 1.314 0.577
18:2 0.108 1.604 0.173 1.311 0.142 1.131 0.122
Sxilnm 1.000 1.831 1.495 1.289
m 6.240 4.461 3.631
Measured 6.533 4.555 3.723
% Differences 4.48 2.06 2.48

experimental and the measured viscosity of coconut methyl
esters was slightly higher than other esters and it was
attributed to impurities, especially the glycerides. The
presence of mono- di- or triglyceride would increase
the viscosity of the esters. It was observed that the measured
viscosities of the esters from both vegetables oil methyl
esters, coconut and palm oil, are higher than the predicted
values.
The viscosities of biodiesels which were reported in the
literatures with their fatty acid compositions were compared
to the predicted values and are summarized in Table 6. The
viscosities of soybean oil and palm oil methyl esters were
reported in the kinematic units by Graboski and McCor-
micks et al. [19]. The percent differences between the
Table 6
Comparison of predicted viscosities of vegetable oil methyl esters to those reported in literatures at 40 8C
predicted and experimental values are 3.75 and 5.00%,
respectively. Similarly, the percent differences for 6
vegetable oil methyl esters reported using the rolling
ball viscometer by Allen et al. [7] are between 3.73 and
8.56%, assuming all the esters have the same density of
0.85 g cmK3. These differences may be lower or higher than
the present figures if the densities of the esters deviate from
0.85 g cmK3.
5. Conclusion
The viscosity of saturated FAME is shown to be directly
related to the basic thermodynamic parameters. The

FAMEs Allen et al. [7] Graboski and McCormick

[19]
Palm Rapeseed Soybean Canola Coconut Peanut Soy bean palm
Predicted viscosity (cSt) 4.411 5.885 4.005 4.229 2.746 4.285 4.037 4.438
Viscosity (cP) 3.590 4.700 3.260 3.450 2.150 3.510
Conversion into cSta 4.224 5.529 3.835 4.059 2.529 4.129 4.08 4.45
% Difference K4.44 K6.43 K4.42 K4.19 K8.56 K3.77 1.05 0.27
a
cStZcP/0.85 (assuming density of all esters Z0.85 g cmK3).
 K. Krisnangkura et al. / Fuel 85 (2006) 107–113
proposed method can be used to determine the viscosities of
saturated FAMEs at different temperatures, within a narrow
limit of 20–80 8C. Viscosity predicted outside this tempera-
ture range may be possible but accuracy may be lower. The
advantage of the proposed method is, it is directly related to
the basic thermodynamic parameters. This would allow
further refinement of the method for prediction of viscosities
of FAMEs and it may be extended to other functional
homologous series.
Acknowledgements
This work was supported by Thailand Research Fund and
The Joint Graduate School of Energy and Enviroment,
KMUTT.
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