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Ntambwekambuyi 2019
Ntambwekambuyi 2019
Ntambwekambuyi 2019
ABSTRACT
Response surface methodology (RSM) is used to optimize the electrocoagulation/electro-flotation T. Ntambwe Kambuyi (corresponding author)
F. Eddaqaq
process applied for the removal of turbidity from surface water in an internal loop airlift reactor. Two A. Driouich
B. Bejjany
flat aluminium electrodes are used in monopolar arrangement for the production of coagulants. H. Mellouk
K. Digua
The central composite design is used as a second-order mathematical model. The model describes A. Dani
the change of the measured responses of turbidity removal efficiency and energy consumption Laboratory of Process Engineering and
Environment, FST of Mohammedia,
according to the initial conductivity (X1), applied voltage (X2), treatment time (X3) and inter-electrode University Hassan II,
Casablanca – Morocco, Hay Yasmina, B.P. 146,
distance (X4). The evaluation of the model fit quality is done by analysis of variance (ANOVA). Fisher’s Mohammedia, 20650,
Maroc
F-test is used to provide information about the linear, interaction and quadratic effects of factors. E-mail: toussaint_ntambwe@yahoo.fr
Multicriteria methodology, mainly the desirability function (D), is used to determine optimal
B. Lekhlif
conditions. The results show that, for a maximal desirability function D ¼ 0.79, optimal conditions Equipe de recherche Hydrogéologie, Traitement et
Epuration des Eaux et Changements
estimated are X1 ¼ 1,487 μS/cm, X2 ¼ 5 V, X3 ¼ 6.5 min, X4 ¼ 14 mm. The corresponding turbidity Climatiques,
Ecole Hassania des Travaux Publics,
removal rate and energy consumption are 84.15% and 0.215 kWh/m3 respectively. A confirmation
Km 7, Route d’El Jadida, B.P. 8108, Oasis,
study is then carried out at laboratory scale using the optimal conditions estimated. The results show Casablanca,
Maroc
a turbidity removal rate of 72.05% and an energy consumption of 0.210 kWh/m3.
Key words | airlift reactor, desirability function, electrocoagulation/electro-flotation, response
surface methodology (RSM), surface water
INTRODUCTION
Surface waters are used for the production of drinking alum). This method has some drawbacks like handling
water. However, the presence of many undesirable agents large quantities of chemicals, proper assessment of require-
such as silts, clays, and algae causes them to become ments, feeding of chemicals and production of a large
turbid and makes them unsuitable for human consumption. volume of sludge causing a disposal problem and loss of
These particles have a small size ranging from 0.1 to 0.01 μm water (Paul ). The regulations for drinking water, as
(Moussa et al. ; Naje et al. ) and remain suspended well as for wastewater discharge, and new environmental
in water. Therefore, agglomeration of particles into a considerations have allowed electrochemical technologies
larger floc is a necessary step for their removal by flotation to gain an important place worldwide during the past two
or sedimentation. A chemical coagulation/flocculation decades (Chen ). These technologies are characterized
(CC/F) process is often used for destabilization and agglom- by low sludge production, and do not require the addition
eration of suspended particles by the addition of salts (i.e. of chemical reagents.
doi: 10.2166/ws.2019.129
Electrocoagulation/electro-flotation (EC/EF) is an now increasing recognition that the OFAT approach is not
electrochemical technology which allows the generation of efficient and ought to be replaced by soundly based chemo-
coagulants in situ by electrodissolution of a soluble anode. metric methods such as response surface methodology
Metal ions (Al3þ, Fe2þ or Fe3þ) are generated at the anode (RSM) based on statistical design of experiments (DOEs).
while hydrogen gas bubbles are produced at the cathode. RSM is a multivariate analysis technic. It is based on the fit
EC/EF has numerous advantages and some drawbacks as of a polynomial equation to the experimental data, which
reported by many authors (Mouedhen et al. ; Zaroual must describe the behaviour of a data set with the objective
et al. ; Khandegar & Saroha ). The electrode of making statistical previsions (Bezerra et al. ).
arrangement can be in a monopolar or bipolar mode In this paper, a chemometric approach, especially RSM,
(Kobya et al. ). Chemical reactions when aluminium is is used to model and optimize turbidity removal efficiency
used as an electrode material are as follows: (TR) from surface water using the EC/EF process in an
internal loop airlift reactor (ILAR) as a function of initial
• At the anode (oxidation of the metal):
conductivity (X1), applied voltage (X2), treatment time
Al(s) ! Al3þ þ 3e (1) (X3), and inter-electrode distance (X4).
(aq)
2H2 O þ 2e ! H2 þ 2OH (3) particles are first ground and then sieved in order to
remove particles exceeding 45 μm. Surface waters contain
colloidal particles with a size ranging from 1 to 103 μm
EC/EF efficiency is a function of three fundamental
(Mickova ). In order to approach this characteristic, we
processes: electrochemical (electrolytic reactions at the sur-
study the sedimentation velocity of an isolated spherical par-
face of electrodes), coagulation (formation of coagulants
ticle in water (refer to Appendix A for the full survey results).
in aqueous phase and adsorption of soluble or colloidal
The reconstituted solution is characterized by an initial
pollutants on coagulants), and flotation process (solid/
turbidity (Ti) of 107 NTU, which is the approximate turbidity
liquid separation). The results of these processes and
value for surface waters (Bejjany et al. ), and pH ¼ 7.3.
their interactions within the EC/EF reactor allow the removal
The initial conductivity value is adjusted using sodium
of pollutants. However, their performance depends on some
chloride (NaCl) as the electrolyte. An HI 99300 portable
parameters such as pH, initial conductivity, treatment time,
conductivity meter is used to measure the initial conductivity
and applied voltage. To improve EC/EF efficiency, operating
value. Turbidity is measured using a HACH series 2100 N
parameters have to be at their optimum values.
brand turbidimeter. Tests are carried out in an ILAR with a
Most of the studies dealing with kinetics optimization
volume capacity of 1 L. A sample of 850 mL from reconsti-
make use of the traditional one-factor-at-a-time (OFAT)
tuted solution is used for each test. Two flat aluminium
approach, examining the effect of one parameter on response,
electrodes are used in monopolar configuration and placed
while holding all others constant. The result of this univariate
in a riser (refer to Appendix D) for the production of coagu-
analysis shows inadequate optimization towards response(s)
lants. TR is given by:
(Sakkas et al. ). Indeed, the OFAT approach is time con-
suming, does not provide interaction effects and requires a Ti Tf
TR (%) ¼ × 100 (4)
large number of experiments (Zaroual et al. ). There is Ti
where Ti and Tf represent initial and final turbidity The second-order model can be expressed as follows:
respectively.
X X X
The energy consumption (WC) in electrocoagulation is Y ¼ β0 þ β i Xi þ β ij Xi Xj þ β ii X2i þ ε (7)
calculated from:
Optimization approach
Statistical analysis
The Derringer or desirability function is the most important
and most current technique of optimization used when the
Mathematical model
optimal values for each response are located in different
regions (Bezerra et al. ; Sakkas et al. ). The scale
Central composite design (CCD) is used as a second-order
of the individual desirability function ranges from d ¼ 0,
response surface model in order to take into consideration
for a completely undesirable response, to d ¼ 1 for a fully
extreme values. This design consists of three types of
desired response, above which other improvements would
points: cube points that come from factorial design (2k),
have no importance (Bezerra et al. ). The overall desir-
axial points (2k) and central points (C0). The central
ability is calculated as follows:
points are used to calculate experimental error (Sakkas
et al. ). The experiment number is given by the following p ffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
expression: D¼ n
d1 d2 . . . dn (8)
Factor coding
as follows: 250–2,150 μS/cm, 2–10 V, 0.5–8.5 min, 6–22 mm, Applied voltage is a key parameter in EC/EF, which
for X1, X2, X3 and X4 respectively. controls the amount of Al3þ dissolved, as well as hydrogen
Figure 1 shows the prediction profiler for TR and WC. gas bubble production within the reactor (Bande et al.
The prediction profiler is often used to show how the predic- ). When X2 increases, the amount of Al3þ dissolved,
tion model changes as the settings of individual factors as well as the amount of hydrogen gas bubbles, increases
change. According to Figure 1, TR and WC increase with in the reactor, which leads to the destabilization of sus-
X1, X2 and X3. On the other hand, when X4 increases, TR pended particles and their agglomeration.
and WC decrease. TR and WC are strongly influenced by X3. A longer X3
Mouedhen et al. () reported that the amount of leads to improved TR and to increased WC.
3þ
Al released in the aqueous solution is a function of the During the EC/EF process, a very fine film of metal
NaCl concentration of the electrolyte (conductivity). hydroxides would get formed on, the anode, generating an
Indeed, the increase in X1 leads to the breakdown of the extra resistance (Ghosh et al. ). The inter-electrode dis-
anodic passive film. This allows the amount of Al3þ dis- tance is one of the parameters on which this resistance (IR)
solved in the reactor to be increased, and therefore, strongly depends. The IR refers to the resistance of the
suspended particles are quickly destabilized (Mouedhen media during the flow of electrical current through the
et al. ). This result corresponds to those reported by cell. When X4 increases, resistance to mass transfer becomes
Bejjany et al. (). In addition, the increase in X1 larger, therefore there is a smaller amount of Al3þ cations at
during EC/EF is known to increase the production of the anode, leading to slower formation of coagulants in the
hydrogen gas bubbles. In ILAR, electrodes are placed middle (Ghosh et al. ). The rate of clay particle
in a riser. Thus, hydrogen gas bubbles produced at the aggregation and adsorption of clays becomes lower, which
cathode are located in the riser. The increase in the explains the decrease in TR. Nasrullah et al. () and
amount of hydrogen gas bubbles leads to the creation of Khaled et al. () report the same results.
a density difference between the riser and downcomer WC is defined as the electrical power consumed per unit
(ρriser < ρdowncomer), which allows recirculation movement. volume. WC is a function of X1, X2, X3 and X4 as shown in
This phenomenon properly disperses Al3þ dissolved in the Figure 1. According to Figure 1, WC increases with X1, X2
reactor and allows mixing of the suspension. Therefore, the and X3 as reported by Bejjany et al. (), Bazrafshan
collision of particles is promoted, which leads to the et al. () and Zaroual et al. (), respectively. Inter-
agglomeration of destabilized particles and their removal electrode distance has an opposite effect in comparison with
by flotation. other factors. Indeed, when X4 increases, WC decreases.
Table 2 shows experimental and predicted data for two Figure 2 comes from linear regression between observed
responses. ANOVA is used to test the statistical significance (experimental) and predicted values. It shows the fit of the
of the ratio of mean square variation due to regression and predicted model to the experimental data. According to
mean square residual error. The P-value is used to estimate Figure 2, the P-values for the TR and WC regressions are
whether the F-ratio is large enough to indicate statistical sig- lower than 0.05 (P-value < .0001). This result means that
nificance. The model is statistically significant when the at least one of the terms in the regression equation has
P-value is lower than 0.05 (Yi et al. ). a significant correlation with the response variable. In
conclusion, the form of model used in this study to explain
Table 2 | Experimental and predicted values for TR and WC the factors and response relationship is correct.
Furthermore, model precision is evaluated by a determi-
TR (%) WC (kWh/m3)
nation coefficient (R 2). The R 2 values for TR and WC are
Standard Experimental Predicted Experimental Predicted
Run values values values values
0.92 and 0.98, respectively. These results imply that 92%
and 98% of the sample variation for TR and WC, respect-
1 0 4.229 0.0296 0.03216
ively, are attributed to the four factors. Only about 8% and
2 0 18.15 0.0174 0.08764
2% of the total variation for TR and WC, respectively,
3 50.99 46.29 0.081 0.05749
cannot be explained by the model. This indicates that the
4 11.98 29.15 0.0466 0.02024
accuracy and general ability of the polynomial model
5 0.99 21.43 0.142 0.13959
are good.
6 0 5.549 0.0831 0.04634
The ANOVA table also provides a term for residual
7 87.62 76.84 0.3754 0.40204
error, which measures the amount of variation in the
8 66.13 57.75 0.207 0.21607
response data left unexplained by the model. The root-
9 12.94 23.72 0.0604 0.03779
mean-square error (RMSE) is 13.554 and 0.037 for the TR
10 0 14.77 0.0359 0.01624
and WC model, respectively.
11 72.64 71.08 0.1664 0.21014
Unlike one-factor-at-a-time methodology, RSM also
12 76.96 58.92 0.08 0.09587
provides information about the interaction and quadratic
13 75.88 62.71 0.3327 0.36604
effects of factors. This analysis is done by Fisher’s F-test. In
14 44.7 51.8 0.1858 0.19577
general, the smaller the value of P-values (<0.05), the larger
15 94.42 114.97 0.8593 0.77552
the magnitude of the F-ratio, and the more significant is the
16 92.62 100.85 0.5081 0.51253
corresponding coefficient term. The estimated regression
17 0 4.736 0.0347 0.02169
coefficients, F-ratio and P-values for all the linear, quadratic
18 86.92 75.78 0.3042 0.32377
and interaction effects of the parameters are given in Tables 3
19 1.92 7.09 0.0113 0.00139
and 4 for TR and WC, respectively. In Table 3, it is observed
20 86.25 74.68 0.509 0.52547
that the linear effect of X1, X2, X3, and X4, and the quadratic
21 2.88 5.46 0.018 0.00261
effect of X1 (X21), X2 (X22) and X3 (X23) are significant model
22 92.16 94.11 0.3123 0.33947
terms. The corresponding P-value of all linear effects is
23 72.4 66.93 0.2923 0.30204
<.0001, while the P-values of the quadratic effects are
24 39.8 38.88 0.0977 0.09452
0.0127, 0.0144 and 0.0287, respectively. All other model
25 73.84 68.277 0.1783 0.167986
terms (all interaction effects and quadratic effect of X4) can
26 65.67 68.277 0.1613 0.167986
be said to be not significant (P-values > 0.05).
27 71.05 68.277 0.1647 0.167986
In addition, X3 is the most significant model term with
28 69.32 68.277 0.1743 0.167986
an F-ratio equal to 78.2564. The corresponding estimated
29 67.78 68.277 0.1669 0.167986
coefficient value is 24.475. Based on the F-ratio values, the
30 57.88 68.277 0.1658 0.167986
ranking of the significant model terms for TR is as follows:
31 72.4 68.277 0.1646 0.167986
X3 > X1 > X2 > X21 > X22 > X4 > X23.
In the same way, estimated regression coefficients, effects of X1 (X21), X3 (X23) and X4 (X24) are not significant
F-ratio and P-value results of WC are indicated in Table 4. model terms. Based on F-ratio values, X2 is the most signifi-
It shows that all linear effects of X1, X2, X3 and X4 are cant model term (F-ratio ¼ 300.5864, estimated coefficient ¼
significant model terms (P-value < .0001). The two-level 0.131). The ranking of significant model terms according to the
interaction effects of X1*X2, X1*X3, X2*X3, X2*X4 and F-ratio values for WC is as follows: X2 > X3 > X1 > X4 >
X3*X4 are significant model terms. Their corresponding X2*X3 > X1*X2 > X2*X4 > X1*X3 > X22 > X3*X4.
P-values are <.0001, 0.0011, <.0001, 0.0010 and 0.0235, The regression model equations (second-order poly-
respectively. Only the quadratic effect of X2 (X22) is a nomial) relating TR and WC are developed and given in
significant model term with a P-value ¼ 0.0033. Thus, the Equations (9) and (10), respectively. These equations only
two-level interaction effect of X1*X4 and the quadratic contain the significant model terms associated with their
estimated coefficients. The regression model equations are in Figure 3(a) (or Figure 4(a)), for a constant initial conduc-
written as follows. tivity value (with X2 ¼ 6 V and X4 ¼ 14 mm), increase in
TR model: treatment time leads to improvement in TR. On the other
hand, Figure 3(b) (or Figure 4(b)) shows that at a constant
TR ¼ 68:277 þ 17:345X1 þ 17:313X2 þ 24:475X3 value of applied voltage, increase in treatment time leads
7:429X4 7:108X21 6:952X22 6:093X23 (9) to increase in WC (with X1 ¼ 1,200 μS/cm and X4 ¼
14 mm). Thus, changes in the level of a factor can improve
WC model: one specific response and have a very negative effect on
another one. Multicriteria methodology, especially the desir-
WC ¼ 0:6179 þ 0:0755X1 þ 0:131X2 þ 0:0855X3 0:052X4 ability function, is used to overcome this problem. Table 5
þ 0:0552X1 X2 þ 0:036X1 X3 þ 0:059X2 X3 shows the scale of the individual desirability function for
0:037X2 X4 0:023X3 X4 þ 0:0238X22 (10) TR and WC. The scale of the individual desirability function
ranges from d ¼ 0.01, for a completely undesirable response
Figures 3 and 4 show two-dimensional contour plots and (low TR or high WC) to d ¼ 0.98, for a fully desired response
three-dimensional response surface plots of TR and WC, (high TR or low WC). The overall desirability (D) close to 1
respectively. These figures show interaction effects for two fac- expressing the maximum of TR and the minimum of the
tors (the factors with most effect) when others are kept WC is equal to 0.79. The optimum conditions relating to
constant in their central values. These representations this value for each factor in coded values are 0.6046869
are often used to search optimal conditions of parameter (X1 ¼ 1,487 μS/cm), 0.5 (X2 ¼ 5 V), 1 (X3 ¼ 6.5 min) and
process, especially when optimal values are located in the 0 (X4 ¼ 14 mm). The corresponding estimated values for
same region. TR and WC are 84.15% and 0.215 kWh/m3, respectively.
According to Figures 3 and 4, the optimum values of These values are used at the laboratory scale for the confir-
each response are located in different regions. For example, mation study as shown in Table 6.
Figure 3 | 2D contour plot of (a) TR (X2 ¼ 6 V and X4 ¼ 14 mm) and (b) WC (X1 ¼ 1,200 μS/cm and X4 ¼ 14 mm).
Figure 4 | 3D response surface plot of (a) TR (X2 ¼ 6 V and X4 ¼ 14 mm) and (b) WC (X1 ¼ 1,200 μS/cm and X4 ¼ 14 mm).
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First received 20 March 2019; accepted in revised form 29 August 2019. Available online 12 September 2019