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Application of Box-Behnken design with response surface methodology for

modeling and optimizing ultrasonic oxidation of arsenite with H2O2

Article  in  Central European Journal of Chemistry · February 2014

DOI: 10.2478/s11532-013-0360-y

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 Cent. Eur. J. Chem. • 12(2) • 2014 • 164-172
DOI: 10.2478/s11532-013-0360-y

Central European Journal of Chemistry

Application of Box–Behnken design with response

surface methodology for modeling and optimizing
ultrasonic oxidation of arsenite with H2O2
Research Article

Pengpeng Qiu1, Mingcan Cui1, Kyounglim Kang1, Beomguk Park1,

Yonggyu Son2, Eunkyung Khim1, Min Jang3, Jeehyeong Khim1*
School of Civil Environmental and Architecture Engineering,
1

Korea University, Seoul 136-701, Republic of Korea

y
Department of Environmental Engineering,
2

op
Kumoh National Institute of Technology,
Gyungbuk 730-701, Republic of Korea

Department of Civil Engineering, Faculty of Engineering,

3

University of Malaya, Kuala Lumpur 50603, Malaysia

rc
Received 1 January 2013; Accepted 3 September 2013

Abstract: A combined ultrasound (US)/H2O2 process was used to oxidize arsenite to arsenate, yielding a synergistic effect value of 1.26. This
showed that the combined process could be an effective method of oxidizing arsenite, instead of using either ultrasonic or H2O2
oxidation processes. This combined process was successfully modeled and optimized using a Box–Behnken design with response
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surface methodology (RSM). The effects of the US power density, the initial concentration of arsenite, and the H2O2 concentration
on the sonochemical oxidation efficiency of arsenite were investigated. Analysis of variance indicated that the proposed quadratic
model successfully interpreted the experimental data with coefficients of determination of R2 = 0.95 and adjusted R2 = 0.91. Through
this model, we can predict and control the oxidation efficiency under different conditions. Furthermore, the optimal conditions for the
oxidation of arsenite were found to be a US power density of 233.26 W L-1, an initial arsenite concentration of 0.5 mg L-1, and an H2O2
concentration of 74.29 mg L-1. The predicted oxidation efficiency obtained from the RSM under the optimal conditions was 88.95%. A
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confirmation test of the optimal conditions verified the validity of the model, yielding an oxidation efficiency of 90.1%.
Keywords: Sonochemical Oxidation • Synergy • Kinetics • Mathematical modeling
© Versita Sp. z o.o.
A

1. Introduction process for oxidizing As(III) to As(V) is therefore required.

Arsenic is commonly present in two oxidation states,
As(III) and As(V), in aqueous environments, and
these states exhibit different chemical behaviors,
bioavailabilities, and toxicities. As(III) is more toxic and
mobile than As(V), which makes up nearly 58% of the
total As in groundwater systems [1]. In addition, the
Water Quality Association (2004) reported that As(V) is
preferentially selected in activated aluminum adsorption
processes compared with As(III). Furthermore, a thin-
film composite reverse-osmosis membrane can easily
remove As(V), but has problems with As(III) [2]. In order
to increase the efficiency of As removal, a pretreatment
Until now, many processes have been used to oxidize
As(III) to the less toxic As(V), such as chemical oxidation
processes using hydrogen peroxide (H2O2) [3], potassium
permanganate (KMnO4) [4], ozone (O3) [5], hypochlorous
acid (HOCl) [6], or a Fenton reagent (Fe2+/H2O2) [7],
photocatalytic oxidation processes, or photochemical
oxidation processes [8]. In addition, ultrasound (US),
a type of wave energy, has proven to be effective for
the oxidation of As(III) since it generates hydroxide
radicals (∙OH), with a redox potential of 2.8 eV [9,10].
Furthermore, combined processes that can increase
the oxidation efficiency have caught many researchers’
interest. Neppolian et al. [11] evaluated the sonochemical

* E-mail: hyeong@korea.ac.kr
164
P. Qiu et al.
Figure 1. Schematic of the experimental reactor setup: (a) cooling system, (b) transducer, (c) reactor, (d) thermometer, (e) ultrasound generator,
and (f) power meter.
oxidation of arsenite using potassium peroxydisulfate
as an oxidizing agent. Lee et al. [12] investigated the
op
synergy between US and ultraviolet processes for
oxidation of As(III). However, the combination of US
and an H2O2 oxidant for arsenite oxidation has not been
studied so far. It is suggested that more ∙OH radicals
will be generated in the US/H2O2 process because of
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the pyrolysis of H2O2 through cavitation phenomena. In
addition, H2O2 itself has a redox potential of 1.77 eV and
can also oxidize arsenite.
Response surface methodology (RSM), which
is based on factorial design, is a mathematical and
statistical technique for designing experiments,
ho
fitting models, and determining the optimal operating
conditions for a target response [13]. It is usually used
to optimize and understand the performance of new and
complex systems whose mechanisms are not clearly
defined [14]. Recently, RSM has been widely used in
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the optimization of operating parameters in combined
systems [15-17].
In this work, the US/H2O2 process was used to
oxidize arsenite to arsenate in a batch study. The
A
kinetics of the H2O2, US, and US/H2O2 processes were
compared. Then, a Box–Behnken design with RSM was
used to optimize and develop the US/H2O2 process.
The oxidation efficiency was measured as a function of
power density, initial concentration of arsenite, and H2O2
concentration, and a quadratic model was proposed.
2. Experimental procedure
2.1. Materials
Sodium arsenite (NaAsO2, 94%) was purchased from
Sigma-Aldrich. H2O2 (34.5%) was purchased from Sam
Chung Chemicals. Purified water was obtained using
a Milli-Q system (Millipore) and had a resistivity of
18.2 MΩ.
y
2.2. Method
The experimental setup is shown in Fig. 1. The
sonoreactor consisted of a glass-cup–horn-type reactor
of capacity 2 L (Φ12.5 × 22 cm) equipped with a cup–
horn-type ultrasonic transducer (Mirae Ultrasonic
MEGA-100). The frequency was 300 kHz, and the
maximum power (100 W) was applied using a single
piezoelectric transducer (Tamura). The temperature in
the solution was measured using a thermometer (Tecpel
DTM-318) and maintained with a water jacket.
The power densities were 160, 200, and 240 W L-1,
respectively. The range of initial arsenite concentrations
was 0.5 mg L-1 to 1.5 mg L-1, based on the distribution of
As in groundwaters around the world [18]. The selection
of the H2O2 concentration range was based on pretests.
Fig. 2 shows the changes in the kinetic constants for
different H2O2 concentrations (20, 60, 120, 240, and
1000 mg L-1) at a fixed power density of 160 W L-1 and a
fixed initial arsenite concentration of 1 mg L-1. A pseudo-
first-order reaction was assumed. The chosen H2O2
concentration range was from 20 mg L-1 to 100 mg L-1.
2.3. Analysis
An anion cartridge (Supelclean LCSAX SPE 3 mL)
filter was used to separate the As(III) and As(V). The
mechanism for this method is clearly described in
Johnson’s study [19]. The As(III) concentration was
measured using an inductively coupled plasma atomic
emission spectrometer (Perkin Elmer 5300DV).
2.4. Experimental design using a Box–Behnken
design with RSM
RSM is an empirical optimization technique for
evaluating the relationship between experimental
outputs (or responses) and factors called X1, X2, X3,
etc. This method is usually used in combination with
factorial design methods such as Box–Behnken designs
and central-composite designs. Adopting Box–Behnken
165
 Application of Box–Behnken design with response surface
methodology for modeling and optimizing
ultrasonic oxidation of arsenite with H2O2

Table 1. Minimum and maximum levels of three factors in terms of coded and uncoded symbols.

Variable Symbols Levels

coded uncoded -1 0 1

Power density (W L-1) x1 X1 160 200 240

Initial concentration (mg L-1) x2 X2 0.5 1 1.5

H2O2 concentration (mg L ) -1

x3 X3 20 60 100

where η is the oxidation efficiency, which is used as the

As(III) oxidation kinetic constant (10-2 min-1)

dependent variable; it is defined as

2.0

(5)

y
1.5

where C0 is the initial concentration of arsenite and C is

the concentration of arsenite at t = 60 min.

op
1.0
In this model, xi (i = 1, 2, and 3) and xj (j = 1, 2, and
3) are independent variables, and β0, βi, and βii (i = 1,
0.5
2, and 3), and βij (i = 1, 2, and 3; j = 1, 2, and 3) are
the coefficients of the model obtained using polynomial
0.0 regression. Finally, ε is the random error. Design Expert
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1 10 100 1000 10000 V 8.0.6 (US, Stat-Ease Inc.) software was used to
H2O2 (mg L-1) evaluate this relationship.

Figure 2. Pretest for the determination of the H2O2 concentration

range. The ultrasound power density was 160 W L-1, and 3. Results and discussion
ho

the initial concentration of arsenite was 1 mg L-1.

designs can sharply reduce the number of experimental 3.1. Comparison of kinetics of each process
sets without decreasing the accuracy of the optimization Fig. 3 shows comparisons of the kinetics of the
compared with traditional factorial design methods. The H2O2, US, and US/H2O2 processes. It is clear that the
minimum and maximum ranges for the three factors are US/H2O2 process has the highest oxidation rate, when
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illustrated in terms of coded and uncoded symbols in each process was carried out separately. The oxidation
Table 1. The relationship between the coded variables rate in the US process is higher oxidation than that in the
and uncoded variables is described by the following H2O2 process because of the generation of ·OH radicals.
equations: The oxidation rate in the combined US/H2O2 process
A

is not just a simple summation of those in the US and

(1) H2O2 processes, and the synergistic effect is defined by
Eq. 6 [12]:
(2)
(6)
(3)
where, kUS/H2O2, kUS, and kH2O2 are the pseudo-
where X1, X2, and X3 are the uncoded variables and x1, first-order kinetic constants for the H2O2, US, and
x2, and x3 are the coded variables. Obviously, all three US/H2O2 processes, respectively; the values are
uncoded factors have their own units. By introducing 0.0007 min-1, 0.012 min-1, and 0.016 min-1, respectively.
coded variables, we make the factors dimensionless. In the present study, the synergistic effect value of the
The effects of these three variables on the oxidation US/H2O2 process is 1.26, indicating that the combined
efficiency can be approximated using a second-order process is more effective for oxidizing arsenite to
polynomial model, as shown in Eq. 4 [20]: arsenate than the individual ultrasonic or H2O2 oxidation
processes are. This synergistic effect can be explained
(4) by a proposed mechanism in which addition of H2O2

166
P. Qiu et al.
1.1
1.0
0.9
0.8
C/C0
0.7
0.6
0.5 H2O2 process
0.4
US process
US/H2O2 process
0.3
0 10 20 30 40 50 60 70
Time/min
Figure 3.
Comparison of the kinetics in each process. H2O2
process: H2O2 concentration, 60mg L-1; US process: US
power density, 160 W L-1; US/H2O2 process: US power
density, 160 WL-1 and H2O2 concentration, 60 mg L-1.
promotes the generation of ·OH radicals through
the decomposition of H2O2, which is caused by the
extremely high temperatures and pressures formed in
collapsing cavitation bubbles. It has been reported that
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the dissociation energy of the O–O bond (213 kJ mol-1)
in H2O2 is less than that of the O–H bond (418 kJ mol-1)
in water [15]. H2O2 is therefore more easily decomposed
than water. Furthermore, changes in the power density
and H2O2 concentration affect the synergistic effect [16].
ho
When the power density increases, not only the number
of cavitation bubbles, but also the temperature and
pressure inside the bubbles, will be increased. As the
number of cavitation bubbles increases, the amount of
H2O2 diffused into the bubbles increases, therefore more
ut
radicals will be generated. However, the increases in the
temperature and pressure inside the bubbles will intensify
the cavitation effect, leading to a higher decomposition
rate of H2O2. Finally, the H2O2 concentration also affects
A
the oxidation rate. It is necessary to choose an optimal
concentration of H2O2 because a lower amount of H2O2
would not have a great effect on the oxidation process
and too much H2O2 would lead to a scavenging effect.
A Box–Behnken design with RSM was therefore
used to evaluate the effects of power density, initial
arsenite concentration, and H2O2 concentration on the
efficiency of sonochemical oxidation of arsenite in the
following scheme. First, Box–Behnken design with RSM
is used to propose a model to describe the relationships,
considering interaction effects, with which we can predict
and control the oxidation efficiency under different
conditions. Secondly, using the response surface, the
influencing tendency of each factor is explored. Finally,
the optimal conditions are determined for engineering
use.
3.2. Optimization using a Box–Behnken design
with RSM
In general, the application of a Box–Behnken design
with RSM includes four main steps.
1) An experimental plan is provided based on the
chosen conditions.
2) Statistically designed experiments are performed.
3) The coefficients in the mathematical model are
estimated and the accuracy of the model is checked.
4) Response analysis is performed to predict the
optimal conditions, and these predictions are confirmed
experimentally.
3.2.1. Model determination
y
Table 2 shows the statistical summary for each model
that was output by Design Expert V 8.0.6. A quadratic
model was suggested, even though it has lower R2 and
op
adjusted-R2 (Adj-R2) values than a cubic model. This is
because the cubic model is aliased, which means that
the effects of each variable that cause different signals
become indistinguishable. For a linear relationship,
the R2 and Adj-R2 values are 0.6362 and 0.5370,
respectively. It is clear that the linear relationship is
not adequate for the experimental data. The quadratic
model was therefore selected to fit the experimental
data.
3.2.2. Model fitting and analysis of variance (ANOVA)
Experiments were performed using the Box–Behnken
experimental design. The experimental and predicted
oxidation efficiencies are shown along with the
experimental conditions in Table 3.
Based on the model analysis in the first part,
a quadratic model was chosen to fit the data. The
relationship between the oxidation efficiency and the
three chosen factors is shown in Eq. 7:
(7)
The coefficient of determination (R2) is defined as
the ratio of the explained variation to the total variation,
and is a measure of the degree of fit [21]. Joglekar et
al. [22] suggested that a good model fit should yield an
R2 of at least 0.8. This means that the response model
evaluated in this study can explain the reaction very
well, with an R2 of 0.9581 and an Adj-R2 of 0.8826 at
a confidence level of 95%. In addition, the model is
very significant, as is evident from its F-value (Fmodel
= 12.7) and very low probability value (p = 0.006).
A p-value lower than 0.05 indicates that the model is
statistically significant, whereas a value higher than
0.1000 indicates that the model is not significant [16].
167
 Application of Box–Behnken design with response surface
methodology for modeling and optimizing
ultrasonic oxidation of arsenite with H2O2

Table 2. Statistical summary for each model.

Source Sum of R2 Adjusted F-value Suggestion

squares R2

Linear vs Mean 808.54 0.6362 0.5370 6.41 Not adequate

Quadratic vs 566 345.63 0.9581 0.8826 10.81 Suggested

Cubic vs Quadratic 53.27 1.000 1.000 5327.06 Aliased

Table 3. Experimental and predicted oxidation efficiencies under different conditions.

Run Coded Real Response

variables variables
x1 x2 x3 X1 X2 X3 Experimental Predicted

y
1 -1 -1 0 160 0.5 60 71.6 69.5

2 1 -1 0 240 0.5 60 85.1 88.0

op
3 -1 1 0 160 1.5 60 64.6 61.6

4 1 1 0 240 1.5 60 74.8 76.9

5 -1 0 -1 160 1.0 20 55.2 58.0

6 1 0 -1 240 1.0 20 69.7 67.5

7 -1 0 1 160 1.0 100 53.6 55.8

rc
8 1 0 1 240 1.0 100 83 80.2

9 0 -1 -1 200 0.5 20 75.9 75.2

10 0 1 -1 200 1.5 20 63.2 63.4

11 0 -1 1 200 0.5 100 78.3 78.2

ho

12 0 1 1 200 1.5 100 70.2 70.9

13 0 0 0 200 1.0 60 79.2 79.2

14 0 0 0 200 1.0 60 79.1 79.1

15 0 0 0 200 1.0 60 79.2 79.2

ut

Table 4 shows the ANOVA results for the acquired the effect of cavitation increases, more H2O2 tends to
model. ANOVA is an analytical technique that is used to be decomposed, which significantly affects the optimal
identify the importance of the model and its parameters, concentration of H2O2. This result corresponds to the
A

using Fisher’s F-test and Student’s t-test [23]. Student’s
t-test was used to determine the significance of the
regression coefficients using a p-value standard. In
general, larger F-values and smaller p-values indicate
more significant coefficient terms [24]. The coefficients
for the quadratic terms for the US power density and
H2O2 concentration are shown to be very significant,
which means that these factors have very large effects
on the removal efficiency. However, the initial arsenite
concentration is only very significant in terms of its linear
effect, whereas its quadratic effect is very small. For the
interaction effects, only the interaction between power
density and H2O2 concentration is significant. This is
because the size of the reaction zone increases with
increasing power density, thereby increasing the amount
of cavitation occurring per volume [25]. However, when
discussion in the chapter 3.1.
3.2.3. Model modification
After the significance of the parameters has been
evaluated, the model can be improved by eliminating
the terms that are not very significant. The final model
for describing the relationship between the oxidation
efficiency and the US power density, initial concentration
of arsenite, and H2O2 concentration is shown in Eq. 8:
(8)
Although the R2 value of 0.9505 has decreased
slightly, the Adj-R2, which is a more important factor for
determining the fit of a regression model, has changed

168
P. Qiu et al.

Table 4. Analysis of variance results for acquired model.

Source Sum of Degrees of Mean F-value p-value Characteristics

squares freedom square

Model 1217.57 9 135.29 12.70 0.0060 Significant

X1 571.22 1 571.22 53.61 0.0007 Significant
X2 181.93 1 181.93 17.07 0.0091 Significant
X3 55.39 1 55.39 5.20 0.0715 Slightly significant
X1X2 2.72 1 2.72 0.26 0.6347 Not significant
X1X3 55.50 1 55.50 5.21 0.0713 Slightly significant
X2X3 5.18 1 5.18 0.49 0.5169 Not significant
X12 125.37 1 125.37 11.77 0.0186 Significant
X22 1.73 1 1.73 0.16 0.7033 Not significant
X32 234.22 1 234.22 21.98 0.0054 Significant

y
Residuals 53.28 5 10.66

R = 0.9581; Adj-R = 0.8826.

op
2 2

90
from 0.8826 to 0.9134 [16]. Furthermore, the p-value
of less than 0.0001 indicates that the model is more
Predicted oxidation efficiency

85
significant.
80
rc
75 3.2.4. Model accuracy check
To obtain an adequate model, an accuracy check
70
is necessary. The model accuracy was checked by
65
comparing the predicted and experimental oxidation
60 efficiencies. Fig. 4 shows the linear relationship between
ho

55
the predicted and experimental oxidation efficiencies. In
addition, a normal plot of residuals between the normal
50
50 55 60 65 70 75 80 85 90 probability (%) and the internally studentized residuals
Experimental oxidation efficiency was also obtained. In this way, the residuals can be
checked to determine how well the model satisfies the
Figure 4. Comparison of predicted and experimental oxidation
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efficiencies. assumptions of ANOVA, and the internally studentized

residuals can be used to measure the standard
deviations separating the experimental and predicted
values [26]. Fig. 5 shows the relationship between the
A

normal probability (%) and the internally studentized

residuals. The straight line means that no response
transformation was required and that there was no
apparent problem with normality.

3.2.5. Response analysis

Figure 5. Normal plot of residuals showing the relationship
between normal probability (%) and internally
studentized residuals.
The relationships between the arsenite oxidation
efficiency and these three factors are shown in
Figs. 6–8. Each plot shows the effects of two variables
within their studied ranges, with the other variable fixed
to the zero level. The response surface better visualizes
the tendency of each factor to influence the arsenite
oxidation efficiency. The shape of the contour plot shows
the natures and extents of the interactions between
factors. An elliptical contour plot indicates a prominent
interaction, whereas a negligible effect appears as a
circular contour plot [27].

169

(a)
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(b)
ho
Figure 6. Effect of power density and initial concentration of
arsenite on the arsenite oxidation efficiency with the H2O2
concentration at the zero level: (a) response surface and
(b) contour plot of the predicted oxidation efficiency.
As can be seen from the plots, the oxidation
ut
efficiency increased with increasing power density.
However, increases in the power density beyond a
certain value did not lead to any further increase in
oxidation efficiency, and even caused a small decrease.
A
This result is supported by Sivakumar and Pandit,
who state that there is always an optimal power
density beyond which there are no more benefits [28].
Furthermore, Andaluri et al. [29] proposed that there is
an optimal power density of 87 W L-1 for degradation of
estrogen using US in the range 70–95 W L-1. Finally, the
oxidation efficiency clearly increased with decreasing
initial concentration of arsenite.
With respect to the effect of H2O2 concentration,
it is clear that the oxidation efficiency increases with
increasing H2O2 concentration from 20 to around
70 mg L-1. However, beyond this concentration, the
oxidation efficiency begins to decrease. The can be
explained by the scavenging effect of H2O2. When H2O2
is added to the US system, the ultrasonic irradiation
may promote the generation of additional ·OH radicals
170
Application of Box–Behnken design with response surface
methodology for modeling and optimizing
ultrasonic oxidation of arsenite with H2O2
(a)
y
op
(b)
Figure 7. Effect of power density and H2O2 concentration on the
arsenite oxidation efficiency with the initial concentration
of arsenite at the zero level: (a) response surface and
(b) contour plot of the predicted oxidation efficiency.
from H2O2, thereby increasing the oxidation efficiency.
However, an overdose of H2O2 may inhibit radical-
induced oxidation, because H2O2 itself can serve as an
·OH radical scavenger. The ·OH-radical-scavenging
reaction can be explained by Reactions 9 and 10
[16,30]):
(9)
(10)
There was therefore an optimal H2O2 concentration
of 74.29 when the sonochemical process was used to
oxidize arsenite.
3.2.6. Condition optimization and confirmation tests
The optimization function in the Design Expert software
was used to obtain the optimal conditions for the
sonochemical oxidation of arsenite at a power density
of 233.26 W L-1, an initial arsenite concentration of
0.5 mg L-1, and an H2O2 concentration of 74.29 mg L-1.
P. Qiu et al.
(a)
rc
ho
(b)
Figure 8. Effect of initial concentration of arsenite and H2O2
concentration on the arsenite oxidation efficiency with
the power density at the zero level: (a) response surface
and (b) contour plot of the predicted oxidation efficiency.
The corresponding oxidation efficiency is 88.95%. To
ut
confirm the validity of the predicted optimal response,
three additional experiments were carried out under
the optimal conditions. The average removal efficiency
among the three repeated experiments was 90.1%.
A
The good agreement between the experimental and
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tool for optimizing individual factors in a new process.
4. Conclusions
In this study, a combined US/H2O2 process was used to
oxidize arsenite to arsenate, yielding a synergistic effect
value of 1.26. This indicates that the combined process
is an effective process for oxidizing arsenite, instead of
using either ultrasonic or H2O2 oxidation processes. A
Box–Behnken design with the RSM was successfully
applied to the sonochemical oxidation of arsenite in the
presence of H2O2. A quadratic model was proposed to
y
describe the relationship between the sonochemical
arsenite oxidation efficiency and the US power density,
op
initial concentration of arsenite, and H2O2 concentration.
The model fitted the experimental data well, with a
coefficient of determination, R2, of 0.9501 and an Adj-R2
of 0.9134. In addition, the p-value of this model was
less than 0.0001, which indicates that the model is very
significant. The optimal conditions for the sonochemical
oxidation of arsenite were a US power density of
233.26 W L-1, an initial arsenite concentration of
0.5 mg L-1, and an H2O2 concentration of 74.29 mg L-1.
The optimal response obtained from the RSM was
88.95%, which is very close to the experimental value
of 90.1%.
Acknowledgements
This work was supported by the Basic Science Research
Program through a National Research Foundation of
Korea (NRF) grant funded by the Ministry of Education,
Science and Technology (KRF-2009-0092799) and
supported by a NRF (2013R1A1A2006586).
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Application of Box–Behnken design with response surface
methodology for modeling and optimizing
ultrasonic oxidation of arsenite with H2O2
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