Académique Documents
Professionnel Documents
Culture Documents
Yildiz Technical University, Faculty of Civil Engineering, Department of Environmental Engineering, 34220 Davutpasa, Esenler, Istanbul, Turkey
Spill Science, 1717 Rutherford Point, S.W. Edmonton, Alberta, Canada T6W 1J6
Emergencies Science and Technology Division, Environment Canada, Ottawa, Ontario, Canada K1A 0H3
a r t i c l e
i n f o
Article history:
Received 18 May 2011
Received in revised form 28 August 2011
Accepted 30 August 2011
Available online 7 September 2011
Keywords:
Water-in-oil emulsion
Stability
Adaptive neuro-fuzzy inference system
Regression model
a b s t r a c t
Oil composition and properties including density, viscosity, asphaltene, saturate, aromatics and resin
contents are responsible factors for the formation of water-in-crude-oil emulsions. These factors can be
used to develop an stability index which determines states of water-in-oil emulsion in terms of either
an unstable, entrained, mesostable or stable conditions. It is important to note that most of the regression models cannot capture the non-linear relationships involved in the formation of these emulsions.
This study deals with the prediction of water-in-oil emulsions stability by an adaptive neuro-fuzzy inference system (ANFIS) with basic compositional factors such as density, viscosity and percentages of SARA
(saturates, aromatics, resins, and asphaltenes) components.
In the computational method, grid partition and subtractive clustering fuzzy inference systems were
tried to generate the optimum fuzzy rule base sets. The stability estimation was conducted by applying
hybrid learning algorithm and the model performance was tested by the means of distinct test data set
randomly selected from the experimental domain. The ANFIS-based predictions were also compared to
the conventional regression approach by means of various descriptive statistical indicators, such as root
mean-square error (RMSE), index of agreement (IA), the factor of two (FA2), fractional variance (FV),
proportion of systematic error (PSE), etc.
With trying various types of fuzzy inference system (FIS) structures and several numbers of training epochs ranging from 1 to 100, the lowest root mean square error (RMSE = 2.0907) and the highest
determination coefcient (R2 = 0.967) were obtained with subtractive clustering method of a rst-order
Sugeno type FIS. For the optimum ANFIS structure, input variables were fuzzied with four Gaussian
membership functions, and the number of training epochs was computed as 21. In the computational
analysis, the predictive performance of the ANFIS model was examined for the following ranges of the
clustering parameters: range of inuence (ROI) = 0.450.60, squash factor (SF) = 1.201.35, accept ratio
(AR) = 0.400.55, and reject ratio (RR) = 0.100.20. Results indicated that ROI, SF, AR and RR were obtained
to be 0.54, 1.25, 0.50 and 0.15, respectively, for the best FIS structure.
It was clearly concluded that the proposed ANFIS model demonstrated a superior predictive performance on forecasting of water-in-oil emulsions stability. Findings of this study clearly indicated that the
neuro-fuzzy modeling could be successfully used for predicting the stability of a specic water-in-oil
mixture to provide a good discrimination between several visual stability conditions.
2011 Elsevier B.V. All rights reserved.
1. Introduction
Water-in-oil emulsions or mixtures are an important part
of oil or petroleum products spill behaviour and control. These
Corresponding author. Tel.: +90 212 383 5376; fax: +90 212 383 5358.
E-mail addresses: yetilmez@yildiz.edu.tr (K. Yetilmezsoy), Fingasmerv@shaw.ca
(M. Fingas), Ben.Fieldhouse@ec.gc.ca (B. Fieldhouse).
1
Tel.: +1 780 989 6059; fax: +1 780 433 6444.
2
Tel.: +1 613 998 9622; fax: +1 613 991 9485.
0927-7757/$ see front matter 2011 Elsevier B.V. All rights reserved.
doi:10.1016/j.colsurfa.2011.08.051
K. Yetilmezsoy et al. / Colloids and Surfaces A: Physicochem. Eng. Aspects 389 (2011) 5062
ascertain what types form and how these might be predicted from
the available starting oil properties [2].
Fingas and Fieldhouse [2] published a paper on oil spill emulsion formation in which more than 300 oils or petroleum products
were studied. These oils were samples of commonly produced
and transported oils. It was found that four clearly dened waterin-oil types were formed by oil when mixed with water. This
was shown by water resolution over time, by a number of rheological measurements, and by the water-in-oil products visual
appearance, both on the day of formation and one week later.
Some emulsions were observed for a year or more, with the
identical results. The types are named stable water-in-oil emulsions, meso-stable water-in-oil emulsions, entrained, and unstable
water-in-oil emulsions or those oils which do not form a waterin-oil type. The differences among the four types are large and
are based on appearance, water content measurements and rheological measurements. In a recent study, Ghosh and Rousseau [3]
explored several factors related to crystal-stabilized water-in-oil
emulsion formation and stability. It was reported that emulsier
efcacy and the crystallization behaviour of incorporated lipids
could be signicantly impacted by surfactant interaction with
other components in the continuous oil phase or at the interface
of an emulsion. In another study, Drelich et al. [4] investigated
several properties of emulsions, such as water droplet size distribution, oilwater interfacial tension, and rheological stressstrain, to
better understand the role of particles in the formation and stabilization of water-in-oil emulsions. It was concluded that the process
of droplet formation during emulsication were impeded since
the fragmentation of water into droplets required more energy
in absence of surface-active emulsiers. Moreover, based on the
high-resolution Fourier transform ion cyclotron resonance (FT-ICR)
mass spectrometry data, Czarnecki [5] reported that the composition of the surface material collected from emulsied water
droplets was different from asphaltenes, resins, and the parent
oil. In another study, El Gamal et al. [6] evaluated the role of
asphaltene, carbonate (calcite, magnesite, and dolomite), and clay
contents (kaolinite and montmorillonite) on the stability of waterin-oil emulsions and water cut determination was via both FT-IR
spectra and physicochemical properties (API gravity, kinematic viscosity) of the tested samples. The study concluded that API gravity
slightly decreased with the increase of asphaltene content from
0.1 to 0.7 wt.%, indicating that asphaltene had a little effect on the
emulsion density in comparison with that of water. In addition,
the increase of the asphaltene content caused a slight decrease
in kinematic viscosity due to formation of mechanical barriers
via hydrogen bonding around the water droplets. Furthermore,
results of the study indicated that the acid number increased with
increasing asphaltene content due to the increase of donating protons.
The literature reports that water-in-oil types are stabilized by
both asphaltenes and resins [2,7], but excess resin content (asphaltene resin ratio, A/R > about 0.6) destabilizes the emulsion [2]. A
high asphaltene content (typically >10%) increases the viscosity of
the oil such that a stable emulsion will not form. Viscous oils will
only uptake water as entrained water and will slowly lose much of
this water over a period of about one week. Viscous oils (typically
>1000 mPa s) will not form stable or meso-stable emulsions. Oils of
low viscosity (typically <100 mPa s, i.e. Cusiana, Mississippi Canyon
72, Jet A1, etc.) usually have low amounts of asphaltenes and resins
and thus will not form any water-in-oil type and will retain less
than about 6% water. For the sake of convenience, these types are
called unstable, however, such oils do not uptake water to any signicant degree. Oils of very high viscosity (typically >10,000 mPa s,
i.e. Heritage HE 05, Point Arguello Comingled, Orinoco, etc.) will also
not form any of these water-in-oil types and thus are also classied
as unstable. Previous studies have found that the most important
51
0.58
14
24
490,000
0.96
1
1
<7
0.2
1
5
70
0.86
1
1
<6
like starting oil
Like starting oil
Oils with insufcient asphaltenes and
viscosity
5
8
12
9
16
18
300
1300
60,000
0.9
0.9
0.97
850
5
1
400
7
2
75
60
45
>30 days
<7 days
<2 days
Viscosity
increase
from
starting oil
(one day)
Typical
water
content (%)
Duration
Appearance
Color
solid
viscous liquid
shiny, viscous
The articial neural network-based methods have been successfully used in various disciplines for modeling, however, the lack
of interpretation is one of the major drawbacks of its utilization.
Wieland et al. [22] reported that one of the major shortcomings
Water-in-oil type
Table 1
Properties and characteristics of the different water-in-oil types [2].
Viscosity
increase
from
starting oil
(one week)
Stable emulsions
Red-brown
Red-brown
Meso-stable emulsion
Black
Entrained water
Oils that do not form any water-in-oil mixture or Unstable
Viscosity
(mPa s)
Resin
content
(%)
Aphaltene
content
(%)
A/R
ratio
emulsion stability based on the empirical data and the corresponding physical knowledge of water-in-oil emulsion formation under
various visual stability conditions; (2) to compare the proposed
articial intelligence-based model with the conventional multiple
regression-based approach by means of various descriptive statistical performance indicators such as R2 , MSE, MAE, RMSE, IA, FV, FA2,
etc.; and (3) to verify the prediction performance of the proposed
neuro-fuzzy model by several testing data randomly selected from
the experimental domain.
0.6
0.5
0.75
K. Yetilmezsoy et al. / Colloids and Surfaces A: Physicochem. Eng. Aspects 389 (2011) 5062
Density
(g/mL)
52
K. Yetilmezsoy et al. / Colloids and Surfaces A: Physicochem. Eng. Aspects 389 (2011) 5062
53
Rule 1 : If x is A1 and y is B1 ,
then f1 = p1 x + q1 y + r1
(1)
Rule 2 : If x is A2 and y is B2 ,
then f2 = p2 x + q2 y + r2
(2)
where Q2,i denotes the output of Layer 2. Each node output represents the ring strength of a rule [23,29].
The third layer is the normalized layer, whose nodes are labelled
N. The ith node calculates the ratio of the ith rules ring strength
to the sum of all rules ring strengths. Its function is to normalise
the weight function in the following process [19,23,28,29]:
(3)
(4)
Ai (x) =
(5)
or
x ci 2
(6)
ai
i =
Q3,i = w
(7)
wi
, for i = 1, 2
w1 + w2
(8)
where Q3,i denotes the output of Layer 3. The outputs of this layer
are called normalized ring strengths.
The fourth layer is the defuzzy layer, whose nodes are adaptive.
Every node i in this layer is an adaptive node with a specic func i (pi x + qi y + ri ), where pi , qi and ri
tion. The output equation is w
denote the linear parameters or so-called consequent parameters of
the node. The defuzzy relationship between the input and output
of this layer can be dened as follows [19,23,28,29]:
i fi = w
i (pi x + qi y + ri ), for i = 1, 2
Q4,i = w
(9)
i
wi fi
i fi = i
w
i
wi
(10)
54
K. Yetilmezsoy et al. / Colloids and Surfaces A: Physicochem. Eng. Aspects 389 (2011) 5062
A1
B1
w 1 f = p x + q y + r1
1
1
1
X
A2
f=
Y
B2
w 2 f 2 = p x + q y + r2
2
2
w f +w f
1 1
2 2
w 1+ w 2
=w f +w f
11
2 2
A1
x
A2
w1
w f
11
f
B1
y
w2
w f
2 2
w2
B2
x y
Forward pass
Backward pass
Fig. 1. A two input rst-order Sugeno FIS model with two rules and (b) equivalent ANFIS architecture.
are xed, the overall output can be expressed as a linear combination of the consequent parameters (Fig. 1a). The output f in Fig. 1b
can be expressed as follows [29]:
f =
w1
w2
f1 +
f2
w1 + w2
w1 + w2
(11)
1 (p1 x + q1 y + r1 ) + w
2 (p2 x + q2 y + r2 )
f =w
(12)
1 yq1 + w
1 r1 + w
2 xp2 + w
2 yq2 + w
2 r2
1 xp1 + w
f =w
(13)
K. Yetilmezsoy et al. / Colloids and Surfaces A: Physicochem. Eng. Aspects 389 (2011) 5062
rst cluster centre in order to determine the next data cluster and
its centre location and iterates on this process until all of the data
is within radii of a cluster centre. There are four algorithm parameters of subtractive clustering. These are range of inuence, squash
factor, accepted ratio and rejected ratio [19,32,33].
In this work, the stability estimation was conducted by applying
hybrid learning algorithm and the model performance was tested
by the means of distinct test data sets randomly selected from the
experimental domain. In this work, no pretreatment to the raw
data or elimination of the model results were performed, as implemented by Erdirencelebi and Yalpir [34]. The oil emulsion data were
divided randomly into two subsets as training and testing purposes,
respectively. Cakmakci [14] reported that more data must be used
in the training phase because ANFIS is more adapted nonlinear
functional dependency between input and output variables. It is
noted that using a large number of training data is also important
to avoid overtting problem which causes high testing error since
it can lead to predictions that are beyond the range of the training
data [29]. Considering these facts, the measured data were split at
random into two randomly selected groups: the rst group of 224
data was used as a training set (about 86.8% of the overall data), and
the remaining 34 data was used for testing the robustness of the
ANFIS-based prediction model. The performance index, the Root
Mean Square Error (RMSE), was measured at each step, and the
optimal model structure of 6 variables with the minimum RMSE
was chosen to predict the stability. The predictions by the ANFIS
model were compared with those from the conventional regression
model conducted in the scope of this work. Finally, conclusion was
made based on the ability of the models in achieving the highest
level of prediction accuracy.
55
descriptive statistics including training and testing sets are summarized in Table 2.
2.4. Conventional regression approach
Since a stability index has been established, this can be used
as the target of the relationship [2]. This regression approach
used a multi-regression program directly by using various multifunctional transformations of the input oil property data. However,
a transformation is needed to adjust the data to a singularly increasing or decreasing function. Most parameters have an optimal value
with respect to stability. The arithmetic applied converts values in
front of the peak to values behind the peak, thus yielding a singular declining or increasing function as described in a previous
paper [7]. The optimal value of this manipulation was found by
using a peak function. The arithmetic to perform the transformation is: if the initial value is less than the peak value, then the
adjusted value is the peak value less the initial value; and if the
initial value is more than the peak value, the adjusted value is
the initial value less the peak value. It should be noted that the
exponential of density was used and the natural logarithm of the
viscosity as noted earlier in the previous paper [7]. The values used
to correct oil property input parameters and the arithmetic to perform the multi-functional transformations (indicated with t indice)
are summarized in Table 3.
Using the transformed values, a multiple linear equation was
applied directly to the data [2]. The choice of functions was achieved
by correlating the stability function directly with the data and taking the best of the functions (i.e. square, log (natural of base 10),
etc.) further into the regression process. The Gaussian expansion
approach was used in which one correlates expanded values of the
inputs (i.e. exponentials) and compacted values (e.g. logarithms)
[2]. The functionalities of square, logarithmic or exponential curves
are achieved by correlating the nominal value of the input properties plus the expanded values, taken here as the cube of the starting
parameter as well as the square of the exponential of the starting
value; and their compacted values, the natural logartihm (ln) and
the logarithm (base 10) of parameter divided by the square of the
respective value. Each parameter was correlated with the stability
index in ve sets of mathematical statements. In this method, the
regression was expanded to functionalities above and below linear until the entire relationship is optimized. For example, a linear
function would be included, then a square and then a square root
and so on until tests of the complete regression show that there are
no more gains in increased expansions. Using this technique, six
input parameters: exponential of density (Exp(Dt )), the natural logarithm (ln) of viscosity (ln(Vt )), saturate content (St ), resin content
(Rt ), asphaltene content (At ) and the asphaltene/resin ratio ((A/R)t )
were found to be optimal. Thus with 4 transformations (indicated
with t indice) and the original values of these input parameters,
there are six times ve or 30 input combinations.
Using a multiple regression software package (DataFit V8.1.69,
Copyright 19952005 Oakdale Engineering, PA, RC167), containing 298 two-dimensional (2D) and 242 three-dimensional (3D)
non-linear regression models [37], a maximum of 20 of these could
be taken at a time to test the goodness-of-t. Values that yield
Prob(t) factors of greater than 0.9 were dropped until all remaining
factors could be calculated at once [2]. The Prob(t) is the probability that input can be dropped without affecting the regression
or goodness-of-t. The water-in-oil emulsion data was imported
directly from Microsoft Excel used as an open database connectivity data source, and over twenty regressions were carried out
until the resulting model was optimal. The R2 , the determination
coefcient, was 0.731, which is acceptable considering the many
potential sources of error, etc. along with the parameters to create the model. In the study, the resulting regression model showed
56
K. Yetilmezsoy et al. / Colloids and Surfaces A: Physicochem. Eng. Aspects 389 (2011) 5062
Table 2
Data statistics of model variables considered in the ANFIS modeling.
ANFIS subsets
Data statistics
Input variables
Output variable
Transformed variables
Minimum
Maximum
Average
Range
Minimum
Maximum
Average
Range
Minimum
Maximum
Average
Range
Exp(Density)
ln(Viscosity)
2.150
2.767
2.471
0.617
2.244
2.737
2.468
0.493
2.150
2.767
2.471
0.617
0.000
17.454
5.723
17.454
0.693
14.634
5.434
13.940
0.000
17.454
5.685
17.454
Saturates (%)
Aromatics (%)
Resins (%)
Asphaltenes (%)
Stability
11.200
98.000
56.480
86.800
24.000
96.000
56.668
72.000
11.200
98.000
56.505
86.800
2.000
67.700
26.196
65.700
3.000
55.000
27.535
52.000
2.000
67.700
26.372
65.700
0.000
50.800
11.493
50.800
1.000
38.300
9.903
37.300
0.000
50.800
11.284
50.800
0.000
37.500
5.855
37.500
0.000
23.100
5.926
23.100
0.000
37.500
5.864
37.500
19.500
29.100
7.732
48.600
18.400
21.000
8.465
39.400
19.500
29.100
7.829
48.600
(14)
Stability = 60.78 (0.294)A
- (0.778)B
- + (98.51)C+ (0.0286)D
- + (0.000902)E- (0.000143)F- + (26.49)G
7
(4.635)H
- (2.48)I- (47.44)J- (3.096 10 )K-
(5.957)L- (0.596)M
- (39.102)N
-
(15)
Table 3
The values used to correct oil property input parameters and the arithmetic to perform the multi-functional transformations [35].
Oil property input parameter
Mathematical form
Correction value
Density
Exponential (Exp)
2.5
Viscosity
5.8
Saturates
Standard (%)
45
Resins
Standard (%)
10
Asphaltenes
Standard (%)
Standard
0.6
K. Yetilmezsoy et al. / Colloids and Surfaces A: Physicochem. Eng. Aspects 389 (2011) 5062
57
58
K. Yetilmezsoy et al. / Colloids and Surfaces A: Physicochem. Eng. Aspects 389 (2011) 5062
3,6
3,2
3,0
Testing RMSE
Testing RMSE
3,4
3,2
3,0
2,8
2,6
2,8
2,6
SF = 1.20 - 1.35
ROI = 0.54
AR = 0.50
RR = 0.15
Minimum testing RMSE = 2.1666
(SF = 1.25)
2,4
2,4
2,2
2,2
2,0
0,44
0,46
0,48
0,50
0,52
0,54
0,56
0,58
0,60
2,0
1,18
0,62
1,20
1,22
3,5
3,0
2,5
2,0
1,5
1,0
0,44
1,26
1,28
1,30
1,32
1,34
1,36
3,2
AR = 0.45 - 0.55
ROI = 0.54
SF = 1.25
RR = 0.15
Minimum testing RMSE = 2.1666
(AR = 0.50, others have no effect)
Testing RMSE
Testing RMSE
3,0
1,24
2,8
RR = 0.10 - 0.20
ROI = 0.54
SF = 1.25
AR = 0.50
Minimum testing RMSE = 2.1666
(RR = 0.15)
2,6
2,4
2,2
0,46
0,48
0,50
0,52
0,54
2,0
0,08
0,56
0,10
0,12
0,14
0,16
0,18
0,20
0,22
Table 4
Parameters of Gaussian membership functions (MF1MF4) for the optimum ANFIS structure (ROI = 0.54, SF = 1.25, AR = 0.50, RR = 0.15, epoch number = 21).
Gaussian membership functions: f(x, ,
c) = exp ( (x c)2 /2 2 )
MF1
MF2
MF3
MF4
Input 6, asphaltenes
0.1421
0.1469
0.1047
0.0882
2.377
2.438
2.641
2.416
3.365
3.292
3.331
3.339
2.782
6.618
10.03
4.494
16.57
16.57
16.57
16.57
73
44
28
50
12.54
12.55
12.55
12.54
21
37
32
38
9.699
9.699
9.698
9.7
5
12
23
10.8
7.158
7.157
7.161
7.158
0.9992
7
17
0.9992
Table 5
Fuzzy rule base of the optimum rst-order Sugeno type ANFIS structure (ROI = 0.54, SF = 1.25, AR = 0.50, RR = 0.15, epoch number = 21).
Rule number
If exp(density) is exp(density)MF1 and In(viscosity) is ln (viscosity)MF1 and saturates is saturatesMF1 and aromatics is aromaticsMF1 and
resins is resinsMF1 and asphaltenes is asphaltenesMF1 then stability = 12.12 *
exp(density) + 0.349 ln (viscosity) 0.5194 saturates 0.5119 aromatics + 0.2484 resins + 1.15 asphaltenes + 59.53
If exp(density) is exp(density)MF2 and ln (viscosity) is ln (viscosity)MF2 and saturates is saturatesMF2 and aromatics is aromaticsMF2 and
resins is resinsMF2 and asphaltenes is asphaltenesMF2 then
stability = 273 exp(density) 0.3048 ln (viscosity) + 2.699 saturates + 2.818 aromatics + 3.657 resins + 4.855 asphaltenes 1022
If exp(density) is exp(density)MF3 and ln (viscosity) is ln (viscosity)MF3 and saturates is saturatesMF3 and aromatics is aromaticsMF3 and
resins is resinsMF3 and asphaltenes is asphaltenesMF3 then stability = 30.42 exp(density) + 0.2781 ln (viscosity) 0.9714 saturates 0.8273 aromatics 0.7427 resins 0.4864 asphaltenes + 148
If exp(density) is exp(density)MF4 and ln (viscosity) is ln (viscosity)MF4 and saturates is saturatesMF4 and aromatics is aromaticsMF1 and
resins is resinsMF4 and asphaltenes is asphaltenesMF4 then stability = 196.8 exp(density) + 12.86 ln(viscosity) 10.66 saturates 9.464 aromatics 9.934 resins + 5.094 asphaltenes + 1448
K. Yetilmezsoy et al. / Colloids and Surfaces A: Physicochem. Eng. Aspects 389 (2011) 5062
2,20
Testing RMSE
2,18
2,16
2,14
ROI = 0.54
SF = 1.25
AR = 0.50
RR = 0.15
Number of training epochs = 1 - 100
(Minimum testing RMSE = 2.0907)
(Optimum number of epoch = 21)
2,12
2,10
2,08
0
10
20
30
40
50
60
70
80
90
100
110
membership function, a few attributes were assigned the maximum degree of compatibility when they should have been assigned
lower degrees. To overcome the above limitation and linearity, it
was proposed to use continuous Gaussian membership function
[48]. The effectiveness of using Gaussian membership function was
highlighted in several other studies [4952]. Based on the abovementioned facts, in this study, the Gaussian membership function
was considered for modeling as it is more popular and simple. In
the present case, input variables were fuzzied with four Gaussian membership functions, which were labelled as MF1MF4. The
parameters of these membership functions are given in Table 4.
The rule base of rst-order Sugeno inference system reecting the
physical property of the proposed model along with the respective
membership functions is given in Table 5, with the optimum consequent parameters obtained after the ANFIS training. The output
variable is the linear function of the input variables.
inputs inputmf
EXP(Density)
59
In this study, the proposed ANFIS model was tested with 34 different experimental data used as the testing set randomly selected
from the overall water-in-oil emulsions data set. To verify the prediction performance of the proposed the ANFIS model, predicted
stability values were also evaluated for different visual stability conditions, such as oils that form water-in-oil mixtures (i.e.
entrained, meso-stable and stable conditions) and oils that do not
form water-in-oil mixtures (i.e. unstable conditions including oils
with insufcient asphaltenes and insufcient viscosity, and highly
viscous oils). For different visual stability conditions and the overall
testing data, ANFIS-based predicted results with the corresponding
descriptive statistics are summarized in Table 6.
As seen in Table 6, the proposed ANFIS model demonstrated a
very satisfactory prediction performance for different visual stability groups with very high determination coefcients ranging from
about 0.88 to 0.97. This can be ascribed to the capability of articial
intelligence-based models capturing the dynamic behaviour and
complex interactions between multi-input and output variables
in a highly non-linear system, such as formation of water-in-oil
mixtures. Based on the obtained results, it is also concluded that
MATLAB environment seems to be quite promising and gives
insight into the generalization capability of the ANFIS-based model.
Testing results showed that the major inaccuracy lies only with oil
types that do not form water-in-oil mixtures (Table 6). This is due
to the fact that there are several distinct types of oils or fuels in this
class (i.e. oils with insufcient asphaltenes and insufcient viscosity, and highly viscous oils), and each very different, and because
of the possible presence of emulsion breakers or asphaltene suspenders in these oils indicating unstables conditions.
rules
outputmf
and
MF1
LN(Viscosity)
rule 1
MF2
Saturates
rule 2
Aggregated
output
output
Stability
Aromatics
rule 3
MF3
rule 4
MF4
Resins
Asphaltenes
Fig. 4. Optimum ANFIS model structure for estimation of water-in-oil emulsions stability (ROI = 0.54, SF = 1.25, AR = 0.50, RR = 0.15, epoch number = 21, number of Gaussian
MFs = 4).
60
K. Yetilmezsoy et al. / Colloids and Surfaces A: Physicochem. Eng. Aspects 389 (2011) 5062
Table 6
ANFIS predicted results for different visual stability conditions (responses for 34 different experimental data used as the testing set).
Visual stability condition
Measured stability
R2
Min
Average
Max
Min
Average
Max
9.70
18.40
18.40
+1.10
15.10
8.50
+21.0
5.90
+21.0
9.40
19.70
19.70
+2.10
15.70
8.40
+22.20
6.30
+22.20
0.937
0.878
0.967
y = 0.9575 x + 1.0737
y = 0.9149 x 1.8602
y = 1.3024 x + 0.3610
Table 7
Descriptive performance indices for the overall testing data.
Performance indice
R
R
MAE
RMSE
RMSES
RMSEU
PSE
MSE
IA
FV
FA2
a
ANFIS model
MRMa
ANFIS model
MRMa
ANFIS model
MRMa
0.937
0.968
2.374
2.775
1.117
2.541
0.193
7.702
0.981
0.0111
1.153
0.595
0.771
5.089
7.056
4.143
5.193
0.636
49.781
0.855
0.135
8.889
0.878
0.937
1.152
1.437
0.654
1.279
0.261
2.066
0.962
0.0238
0.960
0.447
0.669
2.988
4.238
1.729
2.615
0.437
17.959
0.769
0.324
1.237
0.967
0.983
1.657
2.091
0.359
2.064
0.0303
4.387
0.991
0.0489
1.039
0.731
0.855
3.854
5.573
2.891
4.765
0.368
31.062
0.916
0.156
4.388
30
20
10
0
-10
-20
Oils (entrained, meso-stable
and stable emulsions) that
form water-in-oil mixture
-30
0
10
15
20
25
30
35
40
20
Oils (entrained,
meso-stable and
stable emulsions)
that form water-in-oil
mixture
ANFIS residuals
Multiple regression model residuals
15
10
4. Conclusions
5
0
-5
0
10
15
20
25
30
35
40
K. Yetilmezsoy et al. / Colloids and Surfaces A: Physicochem. Eng. Aspects 389 (2011) 5062
ANFIS model that could make a reliable prediction on the waterin-oil emulsions stability. The results of this study may be drawn
as follows:
Six independent variables, such as resins, saturates, asphaltenes,
aromatics, viscosity and density, were used as input parameters and the ANFIS model results showed a very good agreement
with the measured values for various visual stability conditions
(R2 = 0.880.97).
Descriptive performance indices (i.e. MAE, RMSE, IA, FV, FA2,
etc.) obviously showed that the proposed neuro-fuzzy model
produced very small deviations and exhibited superior predictive performance on forecasting of the water-in-oil emulsions
stability values compared to the multiple regression-based models. The proposed ANFIS model demonstrated a very satisfactory
prediction performance for different visual stability groups with
very high determination coefcients (R2 = 0.8780.967) and correlation coefcients (R = 0.9370.983). For overall testing set,
descriptive statistics indicated that only 3.3% of the total variations were not explained by the ANFIS model in prediction
of the water-in-oil emulsions stability. On the other hand,
multiple regression-based model showed a poor prediction performance for different visual stability groups with reasonable
determination coefcients (R2 = 0.4470.731) and correlation
coefcients (R = 0.6690.855). For the multiple regression-based
model, about 26.9% of total variations did not t the experimental
data in estimation of the water-in-oil emulsions stability.
The applicability of the proposed ANFIS model is very simple and
there is no need to dene the complex reactions and tedious
mathematical equations for the prediction of the stability values.
Due to high capability of the ANFIS model in capturing the
dynamic behaviour and non-linear interactions, it was demonstrated that a complex system, such as formation of water-in-oil
mixtures, could be easily modeled.
References
[1] NAS, Oil in the Sea III, Inputs, Fates and Effects, National Research Council,
National Academies Press, Washington, DC, 2002.
[2] M. Fingas, B. Fieldhouse, Studies on crude oil and petroleum product emulsions:
water resolution and rheology, Colloids Surf. A Physicochem. Eng. Aspect. 333
(2009) 6781.
[3] S. Ghosh, D. Rousseau, Fat crystals and water-in-oil emulsion stability, Curr.
Opin. Colloid Interface Sci. (2011), doi:10.1016/j.cocis.2011.06.006.
[4] A. Drelich, F. Gomez, D. Clausse, I. Pezron, Evolution of water-in-oil emulsions
stabilized with solid particles Inuence of added emulsier, Colloids Surf. A
Physicochem. Eng. Aspect. 365 (2010) 171177.
[5] J. Czarnecki, Stabilization of water in crude oil emulsions. Part 2, Energy Fuels
23 (2009) 12531257.
[6] M. El Gamal, A.-M.O. Mohamed, A.Y. Zerki, Effect of asphaltene, carbonate, and
clay mineral contents on water cut determination in wateroil emulsions, J.
Petrol. Sci. Eng. 46 (2005) 209224.
[7] M. Fingas, B. Fieldhouse, Special SessionEnvironmental Forensics, Physical
and Chemical Properties and Behaviour of Oil, Water-in-oil emulsions: formation and prediction., in: Proceedings of the Thirty-fourth Arctic and Marine
Oil spill Program (AMOP) Technical Seminar, on Environmental Contamination
and Response, Alberta, Canada, October 04, 2011.
[8] J.-H. Tay, X. Zhang, A fast predicting neural fuzzy model for high-rate anaerobic
wastewater treatment systems, Water Res. 34 (2000) 28492860.
[9] S.A. Abdul-Wahab, S.M. Al-Alawi, Assessment and prediction of tropospheric
ozone concentration levels using articial neural networks, Environ. Model Soft
17 (2002) 219228.
[10] A.M. Domnanovich, D.P. Strik, L. Zani, B. Pfeiffer, M. Karlovits, R. Braun, P. Holubar, A fuzzy logic approach to control anaerobic digestion, Commun. Agric.
Appl. Biol. Sci. 68 (2003) 215218.
[11] M.M. Hamed, M.G. Khalafallah, E.A. Hassanien, Prediction of wastewater treatment plant performance using articial neural networks, Environ. Model Soft
19 (2004) 919928.
[12] A. Altunkaynak, M. Ozger, M. Cakmakci, Fuzzy logic modeling of the dissolved
oxygen uctuations in Golden Horn, Ecologic. Model 189 (2005) 436446.
[13] F. Karaca, B. Ozkaya, NN-LEAP: A neural network-based model for controlling
leachate ow-rate in a municipal solid waste landll site, Environ. Model Soft
21 (2006) 11901197.
[14] M. Cakmakci, Adaptive neuro-fuzzy modeling of anaerobic digestion of primary
sedimentation sludge, Bioproc. Biosyst. Eng. 30 (2007) 349357.
61
[15] A.K. Srivastava, A.K. Nema, Forecasting of solid waste composition using fuzzy
regression approach: A case of Delhi, Inter. J. Environ. Waste Manage. 2 (2008)
6574.
[16] S. Bayar, I. Demir, G. Onkal-Engin, Modeling leaching behavior of solidied
wastes using back-propagation neural networks, Ecotoxicol. Environ. Saf. 72
(2009) 843850.
[17] F.I. Turkdogan-Aydinol, K. Yetilmezsoy, A fuzzy logic-based model to predict biogas and methane production rates in a pilot-scale mesophilic UASB
reactor treating molasses wastewater, J. Hazard. Mater. 182 (2010) 460
471.
[18] K. Yetilmezsoy, Modelling studies for the determination of completely mixed
activated sludge reactor volume: steady-state, empirical and ANN applications,
Neural Network World 20 (2010) 559589.
[19] M. Cakmakci, C. Kinaci, M. Bayramoglu, Y. Yildirim, A modeling approach for
iron concentration in sand ltration efuent using adaptive neuro-fuzzy mode,
Expert Syst. Appl. 37 (2010) 13691373.
[20] K.P. Singh, N. Basant, A. Malik, G. Jain, Modeling the performance of up-ow
anaerobic sludge blanket reactor based wastewater treatment plant using
linear and nonlinear approaches a case study, Anal. Chim. Acta 658 (2010)
111.
[21] S.O. Olatunji, A. Selamet, A.A. Abdul Rahem, Predicting correlations properties
of crude oil systems using type-2 fuzzy logic systems, Expert Syst. Appl. 38
(2011) 1091110922.
[22] D. Wieland, F. Wotawa, G. Wotawa, From neural networks to qualitative models
in environmental engineering, Comp. Aided Civ. Infra. Eng. 17 (2002) 104118.
[23] J.S.R. Jang, ANFIS Adaptive-network-based fuzzy inference system, IEEE Trans.
Syst. Man Cybern. 23 (1993) 665685.
[24] J.S.R. Jang, C.T. Sun, Neuro-fuzzy modeling and control, vol. 83, in: Proceedings
of the IEEE, 1995, pp. 378406.
[25] H. Atmaca, B. Cetisli, H.S. Yavuz, The comparison of fuzzy inference systems
and neural network approaches with ANFIS method for fuel consumption data,
in: Second International Conference on Electrical and Electronics Engineering
Papers ELECO2001, Bursa, Turkey, 2001.
[26] Y. Tsukamoto, An approach to fuzzy fuzzy reasoning method, Advances in fuzzy
set theory and applications, North-Holland, Amsterdam, 1979, p. 137149.
[27] T. Takagi, M. Sugeno, Fuzzy identication of systems and its applications to
modeling and control, IEEE Trans. Syst. Man Cybern. 15 (1985) 116132.
[28] X.-X. Li, H. Huang, C.-H. Liu, The application of an ANFIS and BP neural network
method in vehicle shift decision, in: 12th IFToMM World Congress, Besancon,
France, 2007.
[29] J. Jeon, M.S. Rahman, Fuzzy Neural Network Models for Geotechnical Problems, Final report Research project FHWA/NC/2006-52, Department of Civil
Engineering, North Carolina State University, 2008, p. 411.
[30] J.S.R. Jang, C.T. Sun, E. Mizutani, Neuro-Fuzzy Soft Comput, Prentice Hall, New
Jersey, 1997, pp510514.
[31] MATLAB V7.0, ANFIS Editor GUI, Fuzzy Logic Toolbox, Copyright 19841997,
The MathWorks, Inc., MA, USA, R14.
[32] S. Chiu, Fuzzy model identication based on cluster estimation, J. Intell Fuzzy
Syst. 2 (1994) 267278.
[33] R. Yager, D. Filev, Generation of fuzzy rules by mountain clustering, J. Intell
Fuzzy Syst. 2 (1994) 209219.
[34] D. Erdirencelebi, S. Yalpir, Adaptive network fuzzy inference system modeling
for the input selection and prediction of anaerobic digestion efuent quality,
Appl. Math. Model. 35 (2011) 38213832.
[35] M. Fingas, A new generation of models for water-in-oil emulsion formation, in:
Proceedings of the Thirty-second Arctic and Marine Oil Spill Program Technical
Seminar, Environment Canada, Ottawa, Ontario, 2009, pp. 577600.
[36] K. Yetilmezsoy, M. Fingas, B. Fieldhouse, Modeling Water-in-oil emulsion formation using fuzzy logic, J Multiple-Valued Logic Soft Comp, Manuscript ID
178i-MVLSC, 2011, in press.
[37] DataFit V8.1.69, Description and Capabilities of DataFit, Copyright 19952005,
Oakdale Engineering, PA, USA, RC167.
[38] A. Akkoyunlu, K. Yetilmezsoy, F. Erturk, E. Oztemel, A neural network-based
approach for the prediction of urban SO2 concentrations in the Istanbul
Metropolitan Area, Inter. J. Environ. Pol. 40 (2010) 301321.
[39] M.K. Kolehmainen, Data exploration with self-organizing maps in environmental informatics and bioinformatics, PhD Thesis, Department of Computer
Science and Engineering, Helsinki University of Technology, Espoo, Finland,
2004.
[40] G. Ibarra-Berastegi, A. Elias, B. Barona, J. Saenz, A. Ezcurra, J.D. de Argandona, From diagnosis to prognosis for forecasting air pollution using neural
networks: air pollution monitoring in Bilbao, Environ. Model Soft 23 (2008)
622637.
[41] E. Agirre-Basurko, G. Ibarra-Berastegi, I. Madariaga, Regression and multilayer
perceptron-based models to forecast hourly O3 and NO2 levels in the Bilbao
area, Environ. Model Soft 21 (2006) 430446.
[42] J. Gomez-Sanchis, J.D. Martin-Guerrero, E. Soria-Olivas, J. Vila-Frances, J.L. Carrasco, S. del Valle-Tascon, Neural networks for analysing the relevance of input
variables in the prediction of tropospheric ozone concentration, Atmos. Environ. 40 (2006) 61736180.
[43] K.W. Appel, A.B. Gilliland, G. Sarwar, R.C. Gilliam, Evaluation of the Community
Multiscale Air Quality (CMAQ) model version 4.5: sensitivities impacting model
performance Part I ozone, Atmos. Environ. 41 (2007) 96039615.
[44] K. Yetilmezsoy, S. Demirel, R.J. Vanderbei, Response surface modeling of Pb(II)
removal from aqueous solution by Pistacia vera L.: BoxBehnken experimental
design, J. Hazard. Mater. 171 (2009) 551562.
62
K. Yetilmezsoy et al. / Colloids and Surfaces A: Physicochem. Eng. Aspects 389 (2011) 5062