MEASUREMENT AND PREDICTION OF ASPHALTENE

PRECIPITATION FROM LIVE OILS

B. Edmonds, R. A. S. Moorwood, R. Szczepanski, X. Zhang
(Infochem Computer Services Ltd, South Bank Technopark,
90 London Road, London, SE1 6LN, U.K.)
M. Heyward, R. Hurle
(Expro North Sea Ltd., Fluid Analysis Centre, 2/4 Cremyll Road,
Reading, RG1 8NQ, U.K.)

1. ABSTRACT
Recently developed experimental techniques permit reliable quantitative
measurement of asphaltene precipitation direct from live crudes. An exten-
sive database of such data has now been assembled. Using these data, a
new model has been developed which can reproduce not only the
asphaltene precipitation envelopes but also the amount precipitated at
given conditions of temperature and pressure. It also gives reasonable
predictions for the effect of gas removal and gas injection. Details of the
experimental methods are described, which can be applied to all types of
fluid under almost any experimental conditions together with the charac-
terisation methods.
The model is based on a cubic equation of state with additional terms to
describe the association of asphaltene molecules and their solvation by
resins. The physically based model is able to represent a wide range of data
with minimal adjustable parameters. The ideal input is a compositional
analysis of the oil, SARA characterisation and a limited amount of
asphaltene precipitation measurements. If extensive precipitation data are
available the model can be tuned to match them accurately. However, if
data are not available the model can be run in predictive mode. A standard
characterisation method has been developed for the equation of state that
automatically adds the necessary information for performing asphaltene
calculations.
The new model is a validated practical engineering model which can be
used to devise production strategies that will minimise the risk of
asphaltene deposition. Coupled with a multi-phase equilibrium solver it can
simultaneously predict the fluid phase behaviour and the asphaltene
precipitation.
2. INTRODUCTION
Almost any form of solid formation during the production and processing
of oil and gas streams represents an operational problem and has unfa-
vourable economic consequences. Modelling solid precipitation allows the
engineer to carry out a variety of tasks from screening for potential prob-
lems through to examination of possible remediation strategies should they
occur.
The aims of this work are to develop a set of complementary experimental
and modelling methods that will allow engineers to make reliable predic-
tions of the phase behaviour of petroleum fluids. Although we consider all
types of phases including hydrates, waxes and diamondoids as well as fluid
phases (Edmonds et al., 1999) this article focuses on asphaltenes.
The necessary ingredients are: the appropriate laboratory measurements; a
characterisation procedure to set up a compositional fluid model; suffi-
ciently accurate and predictive models for all the phases of interest;
techniques for solving the multiphase equilibrium problem; and convenient
means for the engineer to access the procedures. We will first describe the
experimental methods, especially the recent novel techniques that allow
measurements on live oils and then show how the measurements can be
used in the fluid characterisation and modelling procedures we have
developed.

3. ASPHALTENE ANALYSIS

3.1 Sample Restoration and Validation

In all of the experimental measurements, single-phase bottom hole samples
were used. This ensured - as far as practicable - that the natural asphaltene
originally present in the oil remained in solution. As a further precaution,
the samples were also restored at reservoir temperature and at greater than
reservoir pressure, with intermittent mixing, for 4 or more days in their
original shipping vessels.

3.2 Measurement of Total Asphaltene Content

Once restoration was complete, the shipping vessels were inverted and left
for some time. Approximately 30 cm3 of the hot, pressurised sample was
then flashed through a heated manifold without any filtration and a further
30 cm3 was flashed through a 0.5 µm filter. The sub-samples of flashed oil
were analysed for heptane insolubles and pentane insolubles by filtration
according to IP143. If, within experimental error, the asphaltene
concentration of the filtered and unfiltered samples were the same, this
indicated that no irreversible asphaltene flocculation had occurred within
the shipping vessels. These samples were used to calibrate a
spectrophotometric method for determining changes in asphaltene content
as described in more detail below. The method is a development of a
technique described by Zerlia, Pinelli and co-workers (Zerlia et al., 1990,
1992). Note that allowance is made for the maltenes present in the oil, thus
facilitating a direct determination of the true asphaltene concentration.

3.3 Determination of Asphaltene Concentration as a Function of Pressure

A high pressure cell immersed in a thermostat (see Figure 1) was heated to
the experimental temperature and pressurised to the same pressure as the
restored sample (greater than reservoir pressure). A heated manifold
containing a 0.5 µm sieve was connected between the cell and shipping
vessel so that the required quantity of fluid could be transferred at single
phase conditions from the shipping vessel into the pressure vessel. After
the transfer was completed, the filter was checked for solid asphaltene as a
precaution against the use of invalid sample for the experiments.

FIGURE 1. Experimental arrangement

The pressure of the sample was set at the first pressure (slightly higher
than reservoir pressure) and allowed to stabilise for at least 24 hours. A
manifold containing a 0.5 µm filter was attached to the top of the pressure
vessel and immersed in the thermostat. At the other end of the manifold a
high pressure syringe valve was attached.
The sample was displaced at constant pressure and temperature out of the
pressure vessel into the manifold until it was full. A further manifold
volume was displaced and the products discarded. This was to purge the
system and ensure that the manifold contained a representative sample. A
glass flask with a septum attachment was evacuated and weighed. This
flask was secured to the manifold via the syringe. A known volume
(nominally 2 cm3) of sample was flashed into the glass flask and the flask
re-weighed to determine the mass of sample. The fluid in the flask was
then processed to determine the asphaltene content.
The remaining sample in the pressure vessel was depressurised to the next
pressure step and allowed to stabilise for 24 hours. The above process was
then repeated at a new pressure.
Dead oil, flashed from the pressure vessel through the 0.5 µm filter at each
pressure step, was analysed for asphaltenes by a UV spectrophotometric
method. This technique allows the measurement of dissolved asphaltene at
each pressure, since flocculated asphaltene is retained by the filter. A
typical series of measurements is illustrated in Figure 2.

FIGURE 2. Asphaltene precipitation isotherm

3.4 Calibration and Quantification of Asphaltene Content
Because every petroleum fraction has different UV absorption character-
istics, a calibration must be carried out for each oil and – ideally - for each
sample bottle of fluid. This is undertaken by flashing a small portion of the
reservoir oil and flocculating the bulk asphaltenes by the addition of an
excess of suitable solvent (typically pentane or heptane). The deposited
asphaltenes are then recovered by filtration and dried. Calibration solutions
are prepared by dissolving the asphaltene at known concentrations in
chloroform and determining the absorbance of these solutions at 3 to 5
wavelengths as shown in Figure 3. Typically, these absorbance calibrations
will be carried out at wavelengths in the visible region thus avoiding
interference effects from aromatic components such as toluene. Three to
five wavelengths are chosen so that a change in the nature of asphaltene
being deposited will be reflected by an alteration in it’s absorption
characteristics. This will then manifest itself through different responses at
each wavelength and alert the experimentalist to a potential problem.
To correct for residual background absorption from the oil itself, the cali-
bration filtrant from which the asphaltenes were flocculated is also taken
up in chloroform to a dilution matching that of the samples from the main
experiments. The absorbance of this solution is then subtracted from all
subsequent absorption measurements in order to correct for the absorption
effects of remaining components in the oil.

1
A
0 .9 400nm
0 .8 500nm

0 .7 600nm

0 .6
0 .5
0 .4
0 .3
0 .2
0 .1
0
0 10 20 30
µ g ( a s p h )/g r a m (s o lv e n t )

FIGURE 3. Calibration of UV absorbance

4. FLUID CHARACTERISATION
The aim of the characterisation procedure is to make the optimum use of
available experimental data relating to fluid composition to construct an
equation of state model of the fluid. The model must be sufficiently de-
tailed to describe accurately the phase behaviour of interest but simple
enough for practical engineering calculations. Although we are primarily
concerned here with asphaltene precipitation it is essential that the same
set of real components and pseudocomponents can be used simultaneously
with models for all phases of interest (fluid and solid).
We take as a starting point a typical modern fluid analysis as provided by a
PVT laboratory. The laboratory will depressurise the reservoir fluid to
obtain separate liquid and gas samples. The gas-oil ratio (GOR) is
recorded in one way or another. The samples are analysed by gas chroma-
tography (GC) to obtain their compositions. For the gas, the components
will be real discrete components of known molecular weight, so the com-
position can be expressed in mole or weight fractions with equal validity.
The GC analysis of the liquid also identifies some discrete components, but
mostly the individual hydrocarbons cannot be identified. Conventionally,
the analysis is expressed as a series of single carbon number (SCN) cuts
terminating with a plus fraction which gives the remainder. The liquid GC
analysis measures the weight fractions not the mole fractions. In addition
some properties of the liquid sample such as density and molecular weight
can be measured.
There are a number of steps in the characterisation of a petroleum fluid
which are interrelated but can also be separated out. Our recommended
procedure, for example, is:
1. The SCN weight fractions in the liquid, including the plus fraction, in
the liquid are correlated against carbon number using a distribution
function.
2. By extrapolating the distribution function, the plus fraction can be split
into a number of pseudocomponents of varying molecular weight as
required. Some SCN cuts can also be grouped into pseudocomponents
as required.
3. Molecular weights and specific gravities are assigned to each compo-
nent from a suitable correlation against carbon number.
4. The molecular weights and specific gravities of the components are all
adjusted to match the measured values for the whole liquid sample.
5. The liquid weight fractions are converted to mole fractions using the
molecular weights of the components.
6. The gas and liquid mole fractions are combined in the correct propor-
tions to give the mole fractions of the total recombined fluid.
7. Using established correlations, the critical properties and acentric
factors of the SCN cuts and pseudocomponents can be estimated from
the values of molecular weight and specific gravity for that component.
8. For asphaltenes we use the information from a SARA characterisation
to split off an asphaltene component and one or more resin compo-
nents from the fluid.
This procedure can be used to set up an equation of state model for any
petroleum fluid. Different correlations can, of course, be used for each
step of the process. We have adapted Whitson’s gamma function distri-
bution (Whitson, 1983) to fit the SCN concentrations; Riazi and Al-Sahhaf
(Riazi and Al-Sahhaf, 1996) give correlations for molecular weight and
specific gravity as a function of carbon number. To obtain critical proper-
ties and acentric factors we use the Lee-Kesler correlations (Kesler and
Lee, 1976). However, other choices would be equally good.

5. ASPHALTENE MODEL
Asphaltenes are polar compounds which are stabilised in crude oil by the
presence of resins. If the oil is diluted by light hydrocarbons, the concen-
tration of resins goes down and a point may be reached where the
asphaltene is no longer stabilised and it flocculates to form a solid phase.
Because the stabilising action of the resins works through the mechanism
of polar interactions, their effect becomes weaker as the temperature rises,
i.e. flocculation may occur as the temperature increases. However, as the
temperature increases further the asphaltene becomes more soluble in the
oil. Thus, depending on the temperature and the composition of the oil, it
is possible to find cases where flocculation both increases and decreases
with increasing temperature.
The first effective model for asphaltene flocculation was the work of
Hirschberg et al. (Hirschberg et al., 1984). Although they recognised that
the asphaltenes in crude oils are present in the form of a colloid, they
treated the oil phase as though it was a homogeneous liquid and modelled
flocculation as a thermodynamic problem of the formation of a new phase
of pure asphaltene. For practical reasons, most subsequent attempts to
model asphaltene flocculation have also treated the process
thermodynamically. Of the thermodynamic models, some treat flocculation
as a phase change in which a second liquid forms (Rydhal et al., 1997) or
else one in which a solid phase forms (Chung, 1992). It is our experience
that either type of model is capable of correlating measurements given
enough effort in adjusting model parameters. However we have found that
both approaches can result in a model that requires too many adjustable
parameters and is very sensitive to small changes in parameter values. This
means that the model must be refitted to a large quantity of experimental
data for each fluid.
Recent work of Firoozabadi and collaborators (Wu, Prausnitz and
Firoozabadi, 1998; Pan and Firoozabadi, 1997) has proposed a detailed
molecular-thermodynamic framework for understanding asphaltene pre-
cipitation. They take into account explicitly the strong interactions
between asphaltene and resin molecules and between asphaltene molecules
using the SAFT association theory in a model where the asphaltene
precipitation is treated as a liquid-liquid equilibrium with the oil. We have
used the same physical basis for our own asphaltene model but with con-
siderable simplification of the mathematical treatment in order to obtain a
practical engineering approach.
The new model is based on the RKS cubic equation of state with addi-
tional terms to describe the association of asphaltene molecules and their
solvation by resin molecules. The interactions between asphaltenes and
asphaltenes-resins are characterised by two temperature-dependent
association constants: K AA and K AR . The remaining components are de-
scribed by the van der Waals 1-fluid mixing rule with the usual binary in-
teraction parameters k ij so the new model is completely compatible with
existing engineering approaches that are adequate for describing vapour-
liquid equilibria. The new model is a computationally-efficient way of in-
corporating complex chemical effects into a cubic equation of state. This is
an important factor for practical applications and our implementation
requires only slightly longer to execute than a normal cubic equation so it
is suitable for use in engineering studies.

6. MODEL PARAMETERISATION
Experimental measurements of asphaltene phase behaviour for live oils
reported in the open literature are scarce, often limited to a flocculation
point at just one temperature. There are few examples where there are
enough data to parameterise and test a model. The collaboration between
Infochem and Expro has allowed us to build up a database with more-or-
less detailed information for over 20 different asphaltenic fluids ranging
from heavy oils to quite light oils with widely different asphaltene
contents. Typically the data includes full compositional analysis, SARA
characterisation and measurements of the amount of asphaltene in the live
oil for a range of temperatures and pressures. This database has enabled us
to compare different modelling approaches quantitatively and to
parameterise the new model.
It is our objective to make the asphaltene model as predictive as possible.
To achieve this it is important to reduce the number of adjustable
parameters to the minimum and to identify the important experimental
measurements that are needed for reliable results. The main quantities that
we wish to predict are: the asphaltene precipitation envelope ( the locus of
points in PT space at which asphaltene is first deposited from the oil); the
amount of asphaltene precipitated; and the effect of gas removal
(depressurisation below the bubble point) or gas injection.
As described above the model has two temperature-dependent association
constants and hence a minimum of four adjustable parameters. Clearly the
best results are obtained by fitting all parameters simultaneously to the
experimental datasets for a particular fluid but this requires data over a
range of conditions. Extensive comparisons on the whole database have
demonstrated that it is possible to use the same form of asphaltene-
asphaltene association constant K AA for all cases with excellent results.
Figure 4 shows the asphaltene precipitation envelopes for a number of oils.
The experimental data are the points and the curves are the result of
applying our characterisation procedure and using the asphaltene model
with the universal K AA and fitting two parameters for the asphaltene-resin
association K AR . This requires a minimum of two measurements at
different temperatures on the precipitation envelope and can give excellent
results for a wide range of different types of precipitation envelopes as
Figure 4 clearly shows. Fitting two parameters for K AR would be our
recommended procedure whenever possible.
For cases where only one precipitation point is available we have devel-
oped a correlation for one parameter for K AR and the other parameter can
be fitted to the data. This still gives good results (see below) but is obvi-
ously less reliable than the recommended procedure.
 12000

10000

8000
Pressure ( psia )

6000

4000

2000

0
-20 80 180 280 380 480
Temperature /F

FIGURE 4. Asphaltene precipitation envelopes for live oils. Experimental

data are shown by symbols and model calculations are shown by lines.

7. ADE PREDICTIONS
In this section we report a case study that shows how the model can be
applied to predict the asphaltene precipitation envelope and amount of as-
phaltene in the oil using different quantities of experimental data.

7.1 Input data

The ideal input data for the model are:
• A compositional analysis of the reservoir fluid.
• The amount of asphaltene in the oil and the ratio of resin to asphaltene,
often determined from the SARA characterisation.
• One or two sets of precipitation conditions for the asphaltene
flocculation.
• Bubble point (optional) to “tune” the petroleum fraction properties.
For cases where the complete data set we recommend is not available we
have developed correlations to assign the required parameters. The
minimum set of data in this case are:
• A compositional analysis of the oil.
• Reservoir conditions.
• Bubble point (optional) to “tune” the petroleum fraction properties.
Obviously the more data available the better the model predictions.

7.2 Case study

The case study is based on a fairly difficult case. The fluid is a very light
oil, fluid MW 68. It has a low asphaltene content of <0.1 wt% and a
resin/asphaltene ratio of 20 but exhibits flocculation. We have available a
full set of data for this fluid, including measurements of the amount of as-
phaltene deposited over a range of pressures for two isotherms.
In all cases we took the fluid analysis and characterised it in the same way.
The characterisation splits the fluid from C6+ into 15 pseudocomponents
but we find that the predictions of asphaltene precipitation are not sensitive
to the number of pseudocomponents. The specified amount of asphaltene
is split off from the fluid and the specified resins are taken from the
heaviest pseudocomponents. The pseudocomponent physical properties
were adjusted to match the measured bubble point. For light oils matching
the bubble point is an important part of the procedure. The equation of
state interaction parameters k ij were fixed using standard correlations and
were not adjusted to match any data.
Four cases were examined
Case 1
Measured data: minimum.
Estimated: wt% asphaltene; R/A (resin/asphaltene ratio); precipitation
point.
Asphaltene model parameters fitted: one K AR parameter (to estimated
precipitation point).
Case 2
Measured data: case 1 plus wt% asphaltene.
Estimated: R/A; precipitation point.
Asphaltene parameters fitted: one K AR parameter (to estimated point).
Case 3
Measured data: case 1 plus SARA characterisation.
Estimated: precipitation point.
Asphaltene parameters fitted: one K AR parameter (to estimated point).
Case 4
Measured data: case 1 plus SARA characterisation and one precipitation
measurement.
Estimated: -
Asphaltene parameters fitted: one K AR parameter (to measured point).
The results for the asphaltene precipitation envelope and for the amount of
asphaltene deposited at 150 oF are compared with experimental data in
Figures 5 and 6. For cases 1-3 the position of the asphaltene precipitation
envelope (APE) is estimated from the reservoir conditions and the one
adjustable model parameter is fitted to the estimated point. The predicted
APE is quite sensitive to the amount of asphaltene present. When this is
unknown it must be estimated based on the molecular weight and
aromaticity. The predictions are less sensitive to the R/A ratio. When
unavailable it must be estimated from the fluid properties in a similar
manner to the asphaltene content.
For this example, the predicted APE is very close to the experimental data
once the correct wt% of asphaltene in the oil is used as input data. This is
also true for the precipitation isotherm where the predicted wt% of asphal-
tene in the oil is almost identical for Cases 2 to 4.
7000

6000

5000
Pressure / psia

4000

3000

Exp. APE
Exp. Bubble
2000
Predicted bubble pt
Case 1
Case 2
1000 Case 3
Case 4

0
-100 -50 0 50 100 150 200 250 300 350 400

Temperature / F

FIGURE 5. Case studies: asphaltene precipitation envelopes.

 0.12
Isotherm at 150 F
0.10
asphaltene in oil (wt%)

0.08

0.06

Exp. data
0.04 Case 1
Case 2
0.02 Case 3
Case 4

0.00
0 2000 4000 6000 8000
Pressure (psia)

FIGURE 6. Case studies: amount of asphaltene in oil.

7.3 Heavy oil

Heavy oils often have a high asphaltene content but this does not neces-
sarily mean that the risk of asphaltene flocculation is high. One of the
heavy oils in the database has a fluid MW 206, and contains 8.5 wt%
asphaltene. The fluid does not exhibit flocculation at either reservoir con-
ditions or in laboratory measurements at 120 oF. Figure 7 shows the
predicted APE which is consistent with the measurements.
4000

Heavy Oil (Fluid MW 206, 8.5 wt% asphaltene)

3000
pressure /psia

2000
Reservoir conditions

Bubble point line

1000 Predicted ADE

0
100 120 140 160 180 200 220 240
Temperature / F

FIGURE 7. Calculated asphaltene precipitation envelope for heavy oil.

8. EFFECT OF GAS INJECTION ON THE APE
Gas injection is one of the techniques that may be used to maintain or im-
prove recovery from a reservoir. However, it is well known that addition
of light gases to an asphaltenic oil will usually result in precipitation of
asphaltenes if enough of the gas is used. Predicting the effect of gas
injection on the APE is therefore an important application of an asphaltene
model. We have used the measurements of Sirvastava et al. (Sirvastava et
al., 1995) on asphaltene precipitation from the Weyburn reservoir fluid A2
when mixed with varying amounts of CO2 . Figure 8 shows the experi-
mental measurements and our predictions. We used essentially the same
component split as Pan and Firoozabadi (Pan and Firoozabadi, 1997) and
compared two different asphaltene-CO2 interaction parameters. The value
of 0.075 which we would normally use for a petroleum fraction with the
molecular weight of the asphaltene is evidently too small. We find that the
value of 0.26 used by Pan and Firoozabadi gives much better results.

9. SCREENING
A valuable application of the new asphaltene model is for screening pur-
poses. The object is to estimate whether asphaltene flocculation is likely to
be a problem for an oil for which no direct measurement of asphaltene
3

W e y b u r n f l u i d A 2 a t 1 6 0 b a r a n d 3 3 2 .15 K
w t % a s p h a lte n e f l o c c u l a t e d

2.5

1.5 E xp .

c a l c . B IP = 0 .2 6
1

c a l c . B IP = 0 .0 7 5

0.5

0
0 10 20 30 40 50 60 70 80
C O 2 m o l% in flu id

FIGURE 8. Effect of CO2 injection on asphaltene precipitation.

flocculation has been made. We do assume as a minimum that the weight
percent of asphaltene has been measured, typically by a SARA charac-
terisation.
We have applied a screening procedure to our asphaltene model that was
originally proposed by workers at Shell (De Boer et al., 1995). The proce-
dure is as follows:
1. Assume a worst case scenario, which is that the oil in the reservoir is
saturated with asphaltenes.
2. At reservoir temperature, lower the pressure to the bubble point, as
this is the point of maximum flocculation. Calculate the oil-asphaltene
equilibrium. Note the asphaltene concentration in the oil phase.
3. Calculate the supersaturation ratio, the ratio of asphaltene in the oil at
reservoir conditions to that at the bubble point.
Table 1 gives the results for a number of oils. De Boer suggested that
when the supersaturation ratio rises above 1.1, flocculation may occur in
practice. Our results so far confirm this rule. The procedure appears par-
ticularly useful because it can be seen from Table 1 that flocculation is not
directly related to either the percentage of asphaltene in the oil or to the
average molecular weight of the oil.

TABLE 1. Screening procedure for asphaltene flocculation

asphaltene C7+ Super- Asphaltene

Sample weight % molecular saturation flocculation
weight ratio
Oil 1 0.073 175 1.37 Yes
Oil 2 0.32 218 1.08 No
Oil 3 0.19 212 1.08 No
Oil 4 4.9 365 1.28 Yes
Oil 5 0.49 183 23.6 Yes
Oil 6 0.7 209 2.49 Yes
Oil 7 3.9 253 1.11 Yes
(borderline)
Oil 8 8.5 266 1.10 No
10. CONCLUSIONS
We now have available both the experimental techniques and computer
modelling methods to allow asphaltene precipitation from live oils to be
handled effectively. A new model for asphaltene precipitation has been de-
veloped using a large database of measurements on live oils. The
recommended input data for our procedure includes a full extended com-
positional analysis, a SARA characterisation, a bubble point and at least
one measurement of the asphaltene precipitation envelope. It is still possi-
ble to make good predictions if some of the information is not available.
An asphaltene screening technique has also been evaluated and shown to
give reasonable indications of whether asphaltene precipitation is likely to
be a problem. The effect of gas injection on asphaltene precipitation can be
reproduced quite well but it is important to use appropriate binary
interaction parameters for asphaltene-light gas components.

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Equilibria. 158-160:481.
Hirschberg, A., de Jong, L.N., Schipper, B.A., and Meijer, J.G., 1984.
SPE11202.
Kesler, M.J. and Lee, B.I, 1976. Hydrocarbon processing. 53:153.
Pan, H.Q. and Firoozabadi, A., 1997. SPE38857.
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Rydhal, A.K., Pedersen, K.S., Hjermstad, H.P., 1997. Presentation at the
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