Separation and Purification Technology 48 (2006) 7884

Free fatty acid separation from vegetable oil deodorizer distillate

using molecular distillation process
P.F. Martins , V.M. Ito, C.B. Batistella, M.R.W. Maciel
Laboratory of Separation Process Development (LDPS), School of Chemical Engineering, State University of Campinas,
Sao Paulo, CP 6066, CEP 13081-970, Brazil

Received 2 December 2004; received in revised form 10 July 2005; accepted 15 July 2005

Abstract

Distillates of the vegetable oil deodorization are composed of free fatty acids (FFA), sterols, tocopherols, sterol esters, hydrocarbons and
breakdown products of fatty acids, aldehydes, ketones and acylglycerols. The content of free fatty acids in deodorizer distillates varies between
25 and 75%. Due to its high content, free fatty acid separation from deodorizer distillate is an important step to concentrate tocopherols to
high purity. Tocopherols are valuable natural substances used in food, cosmetic and pharmaceutical industries. In this work, separation of
free fatty acids from soybean oil deodorizer distillate (SODD) was investigated through molecular distillation, using different operating
conditions. Evaporator temperature from 100 to 180 C and feed flow rate in the range of 1.523.0 g min1 were used in the experiments.
FFA and tocopherols contents were monitored in each stream generated by the molecular distillation process (distillate and residue streams).
The intention is to determine the best operating conditions to produce a material with minimum FFA content and to minimize tocopherol
losses during the process. Removal of FFA in the distillate stream resulted in a preliminary concentration of tocopherols, which is removed
in the residue stream of the molecular distillation. The results showed that an efficient FFA separation from SODD with the lowest loss of
tocopherols requires specific operating conditions. It was possible to obtain a material with 6.4% of FFA and 18.3% of tocopherols from a
raw material composed by 57.8% of FFA and 8.97% of tocopherols, using 160 C of evaporator temperature and 10.4 g min1 of feed flow
rate. These results represent FFA elimination of 96.16% and tocopherol recovery of 81.23%.
2005 Elsevier B.V. All rights reserved.

Keywords: Separation process; Molecular distillation; Free fatty acids; Tocopherols; Deodorizer distillates

1. Introduction tries. It is suggested that Vitamin E decreases the occurrence

There is a growing trend of consumer preference for
natural products. The recent interest in formulate and com-
mercialize phytochemical-based nutraceutical products has
evidenciated the importance of process development to con-
centrate natural substances.
Natural tocopherols are recovered from vegetable oil
deodorizer distillates (VODD), a valuable by-product
obtained during the deodorization of vegetable oil refining.
Tocopherols, which are physiologically active as Vita-
min E, are considered natural antioxidants and find extensive
applications in food, cosmetics, and pharmaceutical indus-
Corresponding author. Tel.: +55 19 3788 3971.
E-mail address: patricia@lopca.feq.unicamp.br (P.F. Martins).
of several age-related degenerative diseases [1].
Vegetable oil deodorizer distillate from the last step of fats
and oil refining, which is sold on the basis of tocopherols and
sterols [2], is one of the richest sources of tocopherols [3].
Deodorizer distillate can have significantly different char-
acteristics, uses, and value. Depending on fats and oils, it
can be a good raw material for the production of Vitamin E,
sterols [4] or only for fatty acid production [5].
VODD is considered a complex mixture due to the great
number of its components. It is composed of free fatty
acids (FFA), sterols, tocopherols, sterol esters, hydrocar-
bons, breakdown products of fatty acids, aldehydes, ketones
and acyl glycerol [4]. Free fatty acids constitute 2575%
of the distillate depending on the raw material, the type
of VODD and conditions of the refining process. Due to

1383-5866/$ see front matter 2005 Elsevier B.V. All rights reserved.
doi:10.1016/j.seppur.2005.07.028
 P.F. Martins et al. / Separation and Purication Technology 48 (2006) 7884
Table 1
Molecular weights and vapor pressures of FFA and tocopherols
Component Molecular weighta Vapor pressure at
(g mol1 ) 200 Ca (Pa)
FFA 180 533.28
Tocopherols 415 20.00
a Ref. [5].
its high content, FFA separation from VODD is one of the
steps that can be followed to concentrate tocopherols to high
purity.
FFA elimination from SODD through molecular distil-
lation to tocopherol concentration is technologically viable
due to the differences between molecular weights and vapor
pressures of FFA and tocopherols (Table 1).
Due to the values of molecular weights and vapor pres-
sures, it is expected that FFA, which are the lighter sub-
stances, be removed from SODD in the distillate stream and
tocopherols be concentrated in the residue stream, preferen-
tially.
Different combinations of physical and chemical treat-
ments have been proposed in the literature to eliminate FFA
and purify tocopherols. Most of them include a preliminary
chemical treatment step. Chu et al. [6,7] recommended the
use of alkali neutralization and washing to remove free fatty
acids as a preconcentration step prior the batch adsorption of
Vitamin E from palm fatty acid distillate. Ramamurthi and
McCurdy [4] studied the pretreatment of deodorizer distillate
using a lipase-catalyzed esterification reaction to convert
FFA into methyl esters, followed by vacuum distillation
to remove them and concentrate tocopherols. Chu et al.
[3] proposed an enzymatic hydrolysis using a commercial
immobilized Candida antarctica lipase, followed by alkali
neutralization and washing to remove FFA from the mixture.
Buczenko et al. [8] performed the saponification of the
raw material and the extraction of unsaponifiable matter as
pretreatment of VODD before the procedure of Vitamin E
concentration, using liquefied petroleum gas extraction. The
enzymatic hydrolysis and saponification reactions convert
fatty acids associated with acylglycerol molecules into
FFA. These mentioned procedures are laborious and require
close attention to prevent the exposure of tocopherols to
molecular oxygen, to light and to temperature in order to
avoid its decomposition. Therefore, the search for alternative
approaches is continuing in an attempt to overcome the
drawbacks of the aforementioned processes (e.g. laborious
procedures and tocopherol decomposition). In this way,
this work proposes the elimination of FFA from VODD
through molecular distillation as a first step for tocopherol
concentration.
The molecular distillation process is useful in the separa-
tion and purification of materials of high molecular weight,
as well as for those that are thermally sensitive, such as
vitamins, by minimizing losses by thermal decomposition.
It is characterized by high vacuum in the distillation space,
short exposure of the distilled liquid to the operating tem-
79
peratures, and a small distance between the evaporator and
the condenser (2050 mm) [9]. Furthermore, this process has
advantages over other techniques that use solvents as the sep-
arating agent, avoiding problems with toxicity.
The combination of a small distance between the evapo-
rator and the condenser (about 2 cm) and a high vacuum in
the distillation gap results in a specific mass transfer mech-
anism with evaporation outputs as high as 2040 g m2 s1
[10]. Under these conditions (e.g., short residence time and
low temperature), distillation of heat-sensitive materials is
accomplished without or only negligible thermal decompo-
sition. Therefore, molecular distillation shows potential in the
separation, purification and/or concentration of natural prod-
ucts, usually constituted by complex and thermally sensitive
molecules such as tocopherols.
Molecular distillation has also been used for heavy
petroleum characterization, demonstrating the potential of
this separation process in other applications [11].
The objective of this work is to study free fatty acid elimi-
nation from VODD by molecular distillation, using different
evaporator temperatures and feed flow rates as a preliminary
step to concentrate tocopherols.
2. Experimental
2.1. Materials
Deodorizer distillates originating from industrial refining
of several vegetable oils (soybean, canola and sunflower)
were obtained from Bunge Alimentos S.A. (Sao Paulo,
Brazil). All samples were stored in the refrigerator at 4 C
until analysis.
A tocopherol kit consisting of -, -, - and -tocopherol
(purity 95%) were obtained from Calbiochem (San Diego,
CA, USA) and used as reference standards for quantitative
and qualitative tocopherol chromatographic analysis.
The reagents used for the free fatty acids analysis were
ethyl alcohol, phenolphthalein and sodium hydroxide. These
reagents were of analytical grade.
The solvents, hexane and isopropanol, for tocopherols
analysis were of HPLC grade.
2.2. Molecular distillation equipment
The distillation of free fatty acids was performed using a
laboratory wiped film molecular distillation model KDL 5,
GmbH UIC (Alzenau, Germany) which is a variation from
falling film molecular distillation with agitation. The major
part of the equipment was constructed from glass. The heat-
ing of the evaporator was provided by a jacket circulated with
heated oil from an oil bath. The vacuum system included
a diffusion and a mechanical pump. The surface area of
the evaporator is 0.048 m2 and the surface area of internal
condenser is 0.065 m2 . The roller wiper speed inside the evap-
orator was fixed at 350 rpm.
80 P.F. Martins et al. / Separation and Purication Technology 48 (2006) 7884
Fig. 1. Auto-scaled chromatogram of soybean oil deodorizer distillate for tocopherols analysis.
2.3. Tocopherols analysis
The composition of tocopherol was determined by nor-
mal phase high performance liquid chromatography [12]
using a modular equipment composed by Waters 515 HPLC
pump (Mildford, MA), equipped with a fluorescence detec-
tor (Waters model 2475 multi fluorescence). The separation
was conducted in a porasil column 125 A, with particle
size of 10 m and 3.9 300 mm of dimension (Waters, Ire-
land). The mobile phase used was hexane: isopropanol (99:1).
The feed flow rate of mobile phase was set at 1.0 ml min1 .
The data processing was done by the Millenium software
2010 Chromatography Manager Software (Waters, Mildford,
MA). The SODD and samples of distillate and residue were
dissolved in hexane (1 mg ml1 ) and injected in the equip-
ment. Each chromatographic run took about 10 min. A typical
chromatogram obtained can be seen in Fig. 1. This method
determines -, -, - and -tocopherol individually. The
tocopherols detected in the chromatograms of SODD were
identified comparing the retention time of these compounds
with the retention time of standards tocopherols. Quantifi-
cation of each type of tocopherol was done using calibration
curves. Standard deviation of the measures (S) was calculated
considering the difference between the concentrations of a
sample of known tocopherol content, X, and the tocopherol
concentration determined by the calibration curve, Mi , using
the formula

i
(X Mi )2
S2 = 1 , bar, the feed temperature at 50 C, the condenser temperature
N 1
where N is the number of injections. The total tocopherol
content was obtained by summing up the individual compo-
nents. In this case, the sum of the standard deviation is given
by the sum of the individual tocopherol standard deviations.
2.4. Free fatty acid determination
The free fatty acids were determined by titration with
NaOH [13] using phenolphthalein as an indicator. The sam-
ples were dissolved in hot neutralized alcohol and the acids
groups of FFA were neutralized with NaOH solution (1 N).
The sample mass and the volume of the alkali of each deter-
mination were used to calculate the amount of free fatty acids.
The percentage of FFA in most types of fats and oils is cal-
culated as oleic acid (C18:1 ) using the formula in which N
corresponds to the normality of the sodium hydroxide solu-
tion:
mL of alkali N 28.2
FFA (%) = ,
mass (g of sample)
2.5. Elimination of free fatty acids
The experiments were organized according to the follow-
ing way: samples were melted to obtain a liquid and homoge-
nous mixture necessary to feed it inside the equipment. The
evaporator temperatures selected in this work were between
100 and 180 C. First, the evaporator temperature was fixed,
and then the feed flow rate was varied ranging from 1.5 to
23.0 g min1 . For temperatures below 160 C, the maximum
feed flow rate used was 12 g min1 , because the same quantity
of distillate was obtained with increased feed flow rate. For
each process condition, samples of both streams (distillate
and residue) were collected and submitted to FFA and toco-
pherols analysis. After that, another evaporator temperature
was adjusted; 15 min was necessary to stabilize the system in
this new condition, and the procedure was repeated. For all
distillation runs, the process pressure was maintained at 106
at 60 C, and the stirring at 350 rpm. The collected samples
of the distillate and residue stream were kept in a freezer at
18 C, for further analysis.
3. Results and discussion
3.1. Raw material characterization
Table 2 lists the characteristics of some deodorizer dis-
tillate samples analysed in this work. The VODD used are
 P.F. Martins et al. / Separation and Purication Technology 48 (2006) 7884 81

Table 2
Raw material characteristics
Analysis SODD SuODD CODD
FFA (wt% acid oleic) 57.80 1.2 55.30 1.2 49.80 1.2
-Tocopherol (%) 2.91 0.29 7.71 0.29 3.41 0.29
-Tocopherol (%) 0.14 0.07 0.14 0.07 a

-Tocopherol (%) 4.66 0.19 1.53 0.19 3.61 0.19

-Tocopherol (%) 1.25 0.08 0.10 0.08 0.27 0.08
Total tocopherols (%) 8.97 0.63 9.48 0.63 7.28 0.63
SODD, soybean oil deodorizer distillate; SuODD, sunflower oil deodorizer
distillate; CODD, canola oil deodorizer distillate.
a Not quantifiable.

brownish and semi-solid at room temperature. In general, the

free fatty acids content of deodorizer distillates is high, so that
VODD is known, also, as fatty acid distillates. Among the
analyzed samples, canola oil deodorizer distillate (CODD)
had the lowest content of tocopherols and free fatty acids,
7.28 and 49.8%, respectively. Sunflower deodorizer distil-
late (SuODD) had the highest tocopherol content (9.48%),
followed by soybean oil deodorizer distillate (SODD) with
8.97%. SODD had 57.8% and SuODD 55.3% of free fatty
acids.
3.2. Molecular distillation process
From the three VODD analysed, SODD was chosen as
a case study due to its higher content of FFA and due to the
importance of volume of soybean oil production in the world.
Fig. 2 shows the profiles of distillate flow rates when
SODD was submitted at different evaporator temperatures
and feed flow rates. It can be seen that, considering the evap-
orator temperature constant at 100 C, the distillate flow rate
is, practically, constant for the range of feed flow rate used.
At 140 C, the distillate flow rate increases with the feed flow
rate until reach the maximum capacity of processing of the
equipment. From this point, the distillate flow rate remains
constant due to heat transfer limitation. At 160 and 180 C,
this limit was not reached for the feed flow rate range con-
sidered.
When the raw material is submitted to the molecular dis-
tillation, it is split in two streams, part of the feed material is
collected in the distillate stream (D) and part in the residue
Fig. 2. Profiles of distillate flow rates using different operating conditions
of evaporator temperature and feed flow rate.
stream (R). The split ratio D/R is an important parameter to
evaluate the process of molecular distillation. It is calculated
as:
mass of distillate
split ratio, D/R = .
mass of residue
Increasing the feed flow rate, the split ratio decreases
(Tables 3 and 4). When the feed flow rate increases, the mate-
rial volume inside the evaporator is higher, the efficiency
of heat transfer between the material and the evaporator is
reduced due to poor contact with walls of evaporator, so split
ratio declines.
3.3. Free fatty acid elimination
The FFA concentration in the residue stream is a function
of feed flow rate and evaporator temperature. Fig. 3 shows
that the FFA remains in the residue stream with relatively
high concentration using lower temperatures. This means that
great part of FFA is not eliminated from SODD. Higher tem-
peratures decrease the FFA content in the residue stream, but,
eliminate a significant part of tocopherols as will be shown
in the next section.

Table 3
Results obtained when the SODD was submitted to molecular distillation using 140 C of evaporator temperature
Feed flow rate (g min1 )

1.87 3.63 5.74 7.61 8.76 10.57 11.84

Split ratio, D/R 2.60 1.84 1.81 1.36 0.95 0.71 0.57
FFA content in the distillate (%) 81.37 88.45 87.11 89.85 90.61 88.21 86.19
FFA content in the residue (%) 2.3 5.02 6.17 21.25 28.77 38.12 43.18
FFA recovery in the distillate (%) 98.92 97.00 96.24 85.22 74.88 62.27 47.51
Tocopherol content in the distillate (%) 4.39 2.22 1.5 1.42 1.16 1.29 0.9
Tocopherol content in the residue (%) 12.92 14.98 16.39 13.74 12.77 11.53 12.38
Tocopherols recovery in the residue (%) 53.4 78.4 85.5 87.5 92.0 92.5 96.1
82 P.F. Martins et al. / Separation and Purication Technology 48 (2006) 7884

Table 4
Results obtained when the SODD was submitted to molecular distillation using 160 C of evaporator temperature
Feed flow rate (g min1 )
2.00 6.02 7.18 8.76 10.42 12.43 18.81 22.75
Split ratio, D/R 4.55 2.54 2.49 2.17 1.86 1.74 1.02 0.76
FFA content in the distillate (%) 70.59 79.27 83.85 83.65 86.51 86.96 88.88 88.46
FFA content in the residue (%) 2.7 1.63 1.67 4.14 6.43 9.61 29.83 38.32
FFA recovery in the distillate (%) 99.17 99.19 99.99 97.77 96.16 94.04 75.25 63.84
Tocopherol content in the distillate (%) 9.21 5.27 3.94 3.03 2.28 2.47 2.21 1.31
Tocopherol content in the residue (%) 3.96 15.06 16.4 16.79 18.33 17.8 14.13 12.7
Tocopherols recovery in the residue (%) 8.6 52.64 63.0 72.3 81.2 80.2 86.0 92.8

The recovery of a substance is calculated through the equa-

tion:
sample mass (%) content of the
substance in the sample (%)
recovery = 100
raw material mass (%) content of the
substance in the raw material (%)

Analysing Fig. 4, it can be seen that to eliminate FFA effi-

Fig. 3. Dependence of residue FFA concentration on operating conditions
of evaporator temperature and feed flow rate.
The best way to evaluate FFA elimination in the distillate
stream is to consider its recovery (Fig. 4). The recovery cor-
responds to the percentage of FFA present in the raw material
which is present in each stream. Higher FFA recoveries were
found in the distillate stream.
Fig. 4. Recovery of FFA in the distillate stream in function of operating
conditions.
ciently in the distillate stream, temperatures higher than
140 C must be employed in the process. Using 140 C and
feed flow rates below 6 g min1 , more than 96% of FFA were
eliminated from SODD in the distillate stream. For 160 C
and feed flow rates below 11 g min1 , more than 96% of
FFA were eliminated from SODD in the distillate stream. At
180 C, the elimination of FFA was higher than 90% for all
range of feed flow rate explored.
3.4. Tocopherols concentration and recovery
For the distillate stream, the tendency is that the concentra-
tion of tocopherols decreases increasing the feed flow rate at
the same temperature. On the other hand, tocopherol concen-
tration changes widely with the feed flow rate in the residue
stream (Tables 3 and 4).
The maximum concentration of tocopherols obtained in
the residue stream was 18.3% (more than twice the toco-
pherols concentration present in the SODD raw material)
using 160 C of evaporator temperature and 10.4 g min1 of
feed flow rate. In these conditions, the residue stream showed
6.4% of FFA, what means that 96.16% of FFA were elimi-
nated in the distillate stream and 81.2% of tocopherols were
recovered in the residue stream.
Fig. 5 shows the recovery of tocopherols in the
residue stream of the molecular distillation. The recovery
corresponds to the percentage of tocopherols present
in the raw material that is present in each stream.
Higher tocopherols recoveries were found in the residue
stream.
Analyzing Fig. 5, it can be seen that at 180 C and
2 g min1 , approximately, all the initial tocopherol amount
(96.6%) was recovered in the distillate stream and at 100 or
120 C and feed flow rate above 5 g min1 , the tocopherol
was recovered in the residue stream (99.6%).
 P.F. Martins et al. / Separation and Purication Technology 48 (2006) 7884 83

Fig. 6. Operating conditions relationship. (a) Linear regression of distil-

Fig. 5. Recovery of tocopherols in the residue stream in function of operating
conditions.
In general, conditions that result in a higher tocopherol
content in the residue stream lead to considerable losses of
tocopherols in the distillate stream. Here, the loss of toco-
pherols is characterized by the quantity of tocopherol that
goes to the distillate stream, because tocopherols are to be
concentrated in the residue stream. In the distillate stream,
the tendency is that the loss of tocopherols decreases with
the increase in the feed flow rate (Tables 3 and 4).
3.5. Comparison of the operating conditions
The molecular distillation operating conditions that lead
to the higher tocopherols concentration from SODD in the
residue stream are reported in Table 5.
Comparing different operating conditions, it can be noted
that, to reach approximately the same tocopherol concentra-
tion, if higher temperatures are used, higher feed flow rates
should be used too. This operation, however, decreases the
recovery of tocopherol in the residue stream, while increases
its productivity. The FFA content was lower for 140 and
160 C due to FFA elimination higher than 96%. The tem-
peratures of 120 and 180 C are not sufficient to eliminate
all FFA present in the sample. As can be seen in Table 5,
late data Y = 0.04766 + 0.62682 X, with correlation coefficient of 0.9996
and standard deviation of 0.1981. (b) Linear regression of residue data
Y = 0.053 + 0.37419 X with correlation coefficient of 0.99883 and stan-
dard deviation of 0.20274.
86.30 and 90.23% of FFA were removed from SODD in the
distillation stream at 120 and 180 C, respectively.
Experimental results also show limits of fractionation in
one-stage operation. To achieve higher tocopherol enrich-
ment, the change of the concept of fractionation would be nec-
essary, e.g. the use of more complicated multistage scheme
with recycling of selected fractions, perhaps with chemical
modification of FFA to more volatile methyl esters.
Other interesting point to take into consideration in this
work is the relationship among the operating conditions to
obtain higher tocopherol content. As can be seen in Fig. 6,
if the distillate and residue flow rates are plotted in function
of feed flow rates and temperatures selected in Table 5, it
can be observed a linear dependency. This is an important
feature. The best combination of operating conditions of feed
flow rate and temperature seems to be near to the point of
maximum capacity of processing discussed in earlier section.
Therefore, if it is desired to work at 170 C, for example,
a feed flow rate to carry out the experiments can be estimated
in 17 g min1 approximately, which would be the point of
maximum capacity of processing at 170 C.

Table 5 4. Conclusions
Best operating conditions to concentrate tocopherols from SODD in the
residue stream This study has demonstrated that preliminar tocopherol
Temperature ( C) concentration from SODD can be achieved by utilizing
120 140 160 180 molecular distillation. It was found conditions which lead
Feed flow rate (g min1 ) 1.86 5.74 10.42 22.92
to higher free fatty acids elimination in the distillate stream
Tocopherols (%) 16.5 16.4 18.3 17.0 and, consequently, higher tocopherol concentrations in the
FFA (%) 18.9 6.2 6.4 15.2 residue stream.
Elimination of FFA (%) 86.30 96.24 96.16 90.23 In addition, the behaviours of free fatty acids and toco-
Recovery of tocopherols (%) 93.3 85.5 81.2 74.1 pherols as function of operating conditions, such as evapora-
Productivity (g tocopherols min1 ) 13.4 33.4 66.7 146.0
tor temperature and feed flow rate, were verified in this work.
84 P.F. Martins et al. / Separation and Purication Technology 48 (2006) 7884
This showed that the best operating conditions to perform free
fatty acids elimination from SODD by means of molecular
distillation as a preliminary step to concentrate tocopherols
were found near to the maximum capacity of processing.
Acknowledgements
The authors are grateful for the financial support of the
Fapesp (Fundacao de Amparo a Pesquisa do Estado de Sao
Paulo) and Capes (Coordenacao de Aperfeicoamento de Pes-
soal de Nvel Superior).
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