ENVIRONMENTAL TECHNOLOGY

https://doi.org/10.1080/09593330.2020.1746409

Treatment of slaughterhouse wastewater using high-frequency ultrasound:

optimization of operating conditions by RSM
Arwa Abdelhaya, Abeer Abu Othmana and Abeer Albsoulb
a
Civil and Environmental Engineering Department, German Jordanian University, Amman, Jordan; bDepartment of Chemical Engineering, Al-
Huson University College, Al-Balqa Applied University, Irbid, Jordan

ABSTRACT ARTICLE HISTORY

Slaughterhouse processes produce substantial amounts of high organic strength wastewater due to Received 6 December 2019
high COD level. A fundamental work had been carried out to explore the removal of COD from Accepted 15 March 2020
actual poultry slaughterhouse wastewater by ultrasound irradiation. The effect of applied
KEYWORDS
frequency, power density, irradiation time, pH, and adding H2O2 on COD removal was Advanced oxidation process
investigated. The COD removal reached ultimate levels after irradiation time of 180 min. The (AOPs); ultrasonication;
COD removal percentage increased from 2% to 43% and from 2% to 49% when the power slaughterhouse wastewater;
density increased from 160 to 1200 W/L at working frequencies of 1142 and 578 kHz, COD removal
respectively. Increasing the pH from 7 to 9 reduced the COD removal from 51% to 13%. At low
power densities, the high frequency (1142 kHz) was more efficient in COD removal than low
frequency (578 kHz) and vice versa at high power densities. A combined system of US and H2O2
was more effective in removing COD than US standalone system. Finally, the kinetics of the COD
decay using sonication was found to obey the first-order model. In conclusion, the US can be
used efficiently at least to pretreat slaughterhouse wastewater with a COD removal of about 50%.

1. Introduction blockages in drainage systems, scum formation and

Slaughterhouse wastewater (SWW) is classified by the
United States Environmental Protection Agency (US
EPA) as one of the most detrimental industrial waste-
waters to the environment due to its high organic
strength and high nutrients content. It has a complex
composition of different organic and inorganic pollu-
tants such as blood residues, proteins, fibers, fats,
heavy metals and detergents used for cleaning purposes
[1]. The presence of such complex mixture contributes
effectively in increasing the organic matter (Chemical
Oxygen Demand COD), which induces the deoxygena-
tion of rivers and contamination of groundwater [2].
Blood is a major problematic contaminant in SWW
since it has a chemical oxygen demand (COD) of
375,000 mg/L [3]. Furthermore, fat can cause physical
problems in wastewater treatment plants, such as
may eventually cause clogging and shutdown of treat-
ment plant units.
Slaughterhouse processes need substantial volumes of
water, most of it for non-consumptive uses, and generate
a significant amount of high strength wastewater [4].
Thus, the discharge of untreated SWW into the environ-
ment is objectionable and appropriate treatment prior
to disposal is indispensable [5]. In other words, the treat-
ment and final disposal of SWW are a public health neces-
sity. Several technologies have been cited in the literature
to treat slaughterhouse wastewater; including biological,
physical, and physicochemical treatment [6–8]. However,
each treatment process has different advantages and
operational difficulties depending on the SWW character-
istics and the desired degree of treatment. Biological treat-
ment is the most frequently used for SWW. However, it
does not offer an optimal option in all operational

CONTACT Arwa Abdelhay arwa.abdelhay@gju.edu.jo Civil and Environmental Engineering Department, German Jordanian University, Amman 11180,
Jordan
© 2020 Informa UK Limited, trading as Taylor & Francis Group
2 A. ABDELHAY ET AL.

conditions. On one side, aerobic treatment requires high 2.2. Experimental setup
amount of energy for aeration, applicable only in the
The experiments of this research were conducted in 1 or
case of low strength wastewater [4], and it produces
1.5-L cylindrical shape Plexiglas reactor (Meinhardt Ultra-
large amount of sludge [5,9] On the other side, anaerobic
sonics) with an internal diameter of 6.925 cm, operated
treatment of SWW is usually a preferred method. None-
in a fed-batch mode (Figure 1). The reactor has a
theless, it is hindered by the accumulation of suspended
double-jacketed vessel filled with water for temperature
solids and fat [10] and it requires post-treatment to
control purposes Ultrasound waves were produced by
comply with discharge standards [11,2]. Whereas, physico-
piezoelectric ceramic transducer (Meinhardt Ultrasonics)
chemical processes such as chemical coagulation or dis-
placed at the base of the reactor. The transducer can
solved air flotation (DAF) produce large volumes of
provide the system with three different working frequen-
bulky sludge that need special handling and further treat-
cies (578, 800 and 1142 kHz) and a maximum power
ment [12,13]. In this perspective, many researchers have
output of 240 W that can be controlled and varied
developed innovative advanced technologies having a
using an ultrasonic multi-frequency generator (Mein-
potential to destroy complex persistent organics. Among
hardt Ultrasonics) operating in continuous mode.
these technologies are the advanced oxidation processes
The temperatures of both the transducer and the gen-
(AOPs) which received recently considerable attention.
erator were monitored through sensors.
Ultrasound irradiation is one of the novel AOPs that has
emerged as a response to a growing need for environ-
mental remediation of recalcitrant pollutants because it 2.3. Sonication treatment procedure
leads to their rapid degradation [14]. Ultrasonic irradiation
relies on the formation of highly concentrated free rad- The sonication experiments were performed using
icals mainly the hydroxyl radicals (HO˙) by acoustic cavita- different frequencies (1142 or 578 kHz), power densities
tion to destroy the pollutants [15]. It does not rely on (from 160 to 1200 w/L), pH (7 and 9), and initial COD
adding chemical additives to achieve significant organic values (609, 304, 203 mg/L). Preliminary experiments
degradation rates. prevailed that 180 min is the time needed to reach
In this study, an investigation was focused on the steady-state COD readings. Thus, for each experiment,
treatment of an actual slaughterhouse wastewater the reactor was loaded with the required volume and
using high-frequency ultrasonication and without pre- then operated in a fed-batch mode for 180 min. The
treatment or dilution. The effect of different operating samples were sonicated using continuous sonication
conditions such as power density, applied frequency, mode at different frequencies and power densities.
initial COD concentration, pH, ultrasonication time, and Samples with a volume of 2 mL were withdrawn on a
adding H2O2 on COD removal efficiency was experimen- regular basis in sealed and clean 20 mL glass vials
tally examined. and the COD was analysed immediately afterwards.
All sonochemical experiments were conducted twice.
2. Materials and methods
2.1. Poultry slaughterhouse wastewater 2.4 Analytical procedures
Poultry slaughterhouse wastewater was collected from a The COD values of the initial and treated samples were
local plant (Al Tahooneh Chicken Company-union for determined according to dichromate standard method
agricultural development and slaughtering) located at [16]. The COD was measured using a Hach digester
Alzarqa, Jordan. The sample was collected after being
filtered using a screen filter. The SWW characteristics
from the selected poultry processing plants are summar-
ized in Table 1. After collection, the samples were main-
tained in a refrigerator at 4 °C.

Table 1. Characteristics of poultry slaughterhouse wastewater.

Characteristic Value
pH 7.4
Colour Reddish brown
TSS (with no pretreatment) 13,750 mg/L
COD 4000–5000 mg/L Figure 1. Ultrasound treatment setup: (1) glass reactor, (2) water
Turbidity 33.2 NTU jacket, (3) water circulation, (4) transducer, (5) electrical
Conductivity 3.15 ms
generator.
 ENVIRONMENTAL TECHNOLOGY 3

(DRB 200-Germany) and a Hach spectrophotometer (DR/ 2.6. Combined US/H2O2 system
2010-Germany). The pH and conductivity of raw samples
In this part, the influence of combining US and H2O2 was
were measured using a digital calibrated Jenway
explored by conducting the following three experiments:
3540 pH/conductivity meter. Total suspended solids
were analysed as per procedures detailed in Standard
(a) A sample of SWW having a volume of 300 mL and
Methods [16]. The turbidity of the raw samples was
H2O2 concentration of 0.1 M was sonicated at a fre-
measured using Hach 2100P portable turbidity meter.
quency of 1142 kHz and power density of 800 W/L
for 1 h.
2.5. Kinetic study (b) A sample of SWW was sonicated at a frequency of
1142 kHz and power density of 800 W/L for 1 h
The kinetic study consists of following up the COD
without adding H2O2.
removal percentage versus the sonication time at the
(c) A sample of SWW was treated by adding only H2O2
determined optimal operating conditions (578 kHz and
(0.1 M).
480 W/L) for samples having different initial COD con-
centrations (203, 305, 609 mg/L). Then, the first- and
At the end of each experiment, Absorbance was
second-order models were tested by nonlinear
measured to avoid H2O2 interference with the COD
regression techniques to describe the kinetics of the
test. The absorbance was measured at a wavelength
COD removal during sonication.
interval from 300 to 700 nm using UV/Vis spectropho-
The relevant equations are:
tometer (UV-3600/UV-VIR spectrophotometer
Shimadzu).
(a) First-order model

First-order model rate can be described by the follow- 2.7. Design of experiments (DOE) with response
ing equations: surface methodology (RSM)
dC(t) Different batch assays were carried out to explore the
r= − = k1 C(t) (1)
dt effect of three process variables (design factors)
C(t) = Co e−k1 t (2) namely, the time (A), power density (B), and working fre-
quency (C) on the ultimate COD removal response.
The normalized form of Equation (2) can be arranged However, to determine the optimum factors that maxi-
as follows: mize the ultimate COD removal, DOE was applied
lnCo using Design-Expert software (Version 12) for regression
= k1 t (3) and statistical analysis. The two-level fractional factorial
C(t)
design (FFD) was employed where each variable has
where C(t) is the COD of the treated sample in (mg/L) at two levels, the maximum which corresponds to (+1)
regular time interval t (min), Co is the initial COD of the and the minimum to (−1) as shown in Table 2. The
raw sample. k1 is the first-order rate constant (1/s). RSM was also used to compute and validate statistically
an empirical model that relates the response with the
(a) Second-order model three process variables.

Second-order model can be described by the follow-

ing equation 3. Results and discussion
dC(t) 3.1. Effect of power density on COD removal
r= − = k2 C(t)2 (4)
dt percentage at different working frequencies
The normalized form of this equation can be arranged as The effect of power density on the COD removal was
follows: investigated. The experiments were carried out at
1 1
= k2 t + (5)
C(t) Co Table 2. Experimental values of coded parameters chosen in the
DOE.
where C(t) is the COD of the treated sample in (mg/L) Factor (A) Factor (B) Factor (C)
at regular time interval t (min), Co is the initial COD of Coded values Time (h) Power density (W/L) Working frequency (kHz)
the raw sample. k2 is the second-order rate constant (L/ −1 0 160 578
mg s). +1 3 1200 1142
4 A. ABDELHAY ET AL.

Figure 2. (a) COD removal percentage versus sonication time at 1142 kHz and various power densities (T = 40°C, pH = 7). (b) COD
removal percentage versus sonication time at 578 kHz and various power densities (T = 40°C, pH = 7).

power densities ranging from 160 to 1200 W/L in two
batches sonicated at 1142 and 578 kHz (Figure 2(a,b)).
It follows from the data obtained in Figure 2 that the
COD removal depends on the sonication time regardless
of the power density value. This could be attributed to
the fact that the concentration of hydroxyl radicals gen-
erated will increase with increasing the sonication time
and will participate more in the COD removal and this
is consistent with the work done by [17] proved that
the removal efficiency of ammonia continued to increase
during the first 120 min. The similar proof was provided
by [18] on the degradation of Methylene Blue (MB)
where they found that degradation continued to
increase during the sonication time (60 min). Figure 2
(a) depicts that the removal percentage of COD at
1142 kHz frequency was found to increase from 2% to
43% with increasing the power from 160 to 480 W/L.
This could be justified by the logic that increasing the
power dissipated per treated volume will increase the
number of cavities generated and the amount of (OH˙)
free radicals released. However, it was noticed that the
COD removal started to decline when the power
density exceeded 480 W/L. This drop in the COD
removal was less pronounced at sonication time longer
than 120 min. From the present observation, it can be
said that the optimal power density in the tested interval
is 480 W/L. Isariebel et al.[19] stated that that the
enhancement of degradation rates can be achieved by
increasing the power input until an optimum power
value, beyond which the rates of degradation start to
decline.
Figure 2(b) shows a similar trend as in Figure 2(a). It
can be observed that the COD removal increased from
2% to 49% as the power density increased from 160 to
480 W/L. Further increase in the power density above
480 W/L resulted in a slight decrease in the COD
removal. This finding is in accordance to the results
reported by [20] where the decolourization efficiency
of textile wastewater increased with increases in
ultrasound power up to a certain point, beyond which
no appreciable increase in efficiency was observed.
3.2. Effect of ultrasound frequency on COD
removal percentage at different power densities
The effect of frequency on the ultimate percentage of
COD removal was investigated at different power den-
sities, maintaining the sonication time at 180 min
(Figure 3). It is clear that the optimal percentage of
COD removal was higher for samples sonicated at 1142
than at 578 kHz at power densities ranging from 160 to
400 W/L. However, when the power density was
greater than 400 W/L, the sonication process undertaken
at 578 kHz showed superior COD removal percentages.
This suggests that at low power densities, the high fre-
quency (1142 kHz) was more efficient in COD removal
than low frequency. On the other hand, sonication at
low frequency (578 kHz) resulted in higher removal of
COD at high power densities.
As mentioned earlier, low number of cavities is gener-
ated at low power dissipation. Thus, at these conditions,
the high frequency might promote the production of
(OH˙) radicals by violent and rapid collapse of the exist-
ing cavities. On the other side, high power densities
Figure 3. The ultimate percentage of COD removal at different
power densities and frequencies (pH = 7).
 ENVIRONMENTAL TECHNOLOGY 5

regions of the collapsing cavitation bubble may also

result in a decrease of the COD removal rate when pollu-
tant concentration increases [23].
However, it is important to point out that the amount
of COD removed increased with an increase of initial con-
centration [19]. As an example, the amount of COD
removed at 609 mg/L is as much as 1.5 times higher
than that removed at 204 mg/L.
A kinetic study was performed to determine the rate at
which the COD was removed from SWW during soni-
cation. The first- and second-order models were tested
in the analysis of the sonication data of SWW treatment.
The normalized form of the two models at the three
Figure 4. COD removal percentages versus time by sonication at different concentrations is depicted in Figure 5. The
various initial concentrations (pH = 7, 578 kHz, 480 W/L). kinetic parameters, rate constants and regression coeffi-
cients are summarized in Table 2. Figure 5 and Table 3
might lead to intensive cavity generation, which could show that, the time profile of the COD removal percen-
be intensified by the low frequency. tage fitted appropriately by first-order kinetics (R 2 > 0.98)
at all initial COD concentrations. Similar results have
3.3. Effect of initial concentration on COD been obtained in previous studies [19,21]. In addition, it
removal percentage at a constant frequency and should be mentioned that the first-order rate
power density constant decreased with increasing the initial COD con-
centration. This fact is in accordance with the work of
The effect of initial COD concentration on the COD [24] and [25].
removal percentage was explored at pH 7, 578 kHz,
480 W/L and three initial COD concentrations 204, 305,
3.4. Effect of initial pH on ultimate COD removal
609 mg/L. The results in Figure 4 revealed that the
percentage
COD removal percentage depends on the sonication
time. The ultimate COD removal rates after a sonication In this part of the study, batch sonication experiments
time of 180 min were found to decrease from 56% to were carried out to investigate the effect of initial pH
27% when increasing the initial COD concentration
from 204 to 609 mg/L. This finding compared well with Table 3. Kinetic parameters for COD removal during sonication
results reported by [21] where the decolourization treatment of SWW at different initial COD concentrations.
efficiency of wastewater decreased with increasing First order Second order
initial Rhodamine B dye concentration. This may be Initial
due to the decreased cavitation effects at higher COD concentration (mg/ k1 (L/ Correlation k2 (1/ Correlation
L) mg h) factor R 2 h) factor R 2
load and insufficient generation of hydroxyl radicals to
204 0.7526 0.9801 0.006 0.9434
destroy the organic pollutants [22]. The limited 305 0.2406 0.9895 0.0009 0.9867
diffusion of hydroxyl radicals out of the interfacial 609 0.2150 0.9993 0.0004 0.9969

Figure 5. (a) The first-order kinetic of COD removal during SWW sonication (pH = 7, 578 kHz, 480 W/L). (b) The second-order kinetic of
COD removal during SWW sonication (pH = 7, 578 kHz, 480 W/L).
6 A. ABDELHAY ET AL.
Figure 6. Effect of pH on ultimate COD Removal at 1142 kHz,
800 W/L, and 300 mL.
on the COD removal percentage. By increasing the pH of
the treated sample, it was clear, as can be seen in
Figure 6, that increasing the pH has greatly affected
the ultimate COD removal percentage. The sample
showed a COD removal percentage of 51% and 13%
after 3 h sonication time and at a pH of 7 and 9,
respectively.
3.5. Effect of adding h2o2 on the efficiency of
sonication process
In this part, several runs were conducted to study the
effect of combined sonication and H2O2 (US/H2O2) on
the COD removal percentage. Expectedly, the COD
measurement in these runs was challengeable due
to the interference of hydrogen peroxide with the
chemical kits used to carry out the COD measure-
ment. Therefore, at this stage, the comparison
between the four samples was based on the UV
absorbance measurement (Figure 7). The four
Figure 7. Change in the absorption UV–visible spectra of SWW at 1142 kHz, 0.1 M H2O2.
samples are namely, untreated sample, US treated
Sample, H2O2 (0.1 M) treated sample, and H2O2
(0.1 M)/US treated sample. Figure 7 shows the
measured absorbance for the latter samples. It can
be obviously seen that the absorbance peak at
420 nm has decreased in the following order:
untreated sample, US treated sample, H2O2 treated
sample, and finally US/H2O2. In other words, the
best removal efficiency was obtained when the com-
bined system US/H2O2 was used. It is logical that
COD removal by sonodegradation would be enhanced
by adding H2O2 which decomposes into (OH˙) radicals
under the effect of sonication [24]. However, it is sub-
stantial in further work to optimize the H2O2 since the
COD removal increases as the H2O2 concentration
increases until an optimal concentration is achieved.
An excess amount of H2O2 could hinder the sonode-
gradation by scavenging (OH˙) radicals formed
during sonication [21].
3.6. Optimization of ultimate COD removal
percentage using DOE with RSM: effect of time,
power density, and working frequency
After running all the DOE runs (56 runs) according
to the actual design shown in Table 4, the
optimum levels of the three process variables were
obtained using the RSM. The RSM relies on solving
the regression equation and analysing the response
surface contour and the 3D plots. Figure 8(a,b)
shows the effect of sonication time and power
density on the ultimate COD removal percentage
represented as surface contour and 3D plot respect-
ively. It can be noticed from Figure 8 that the COD
removal increases as the power density increases
 ENVIRONMENTAL TECHNOLOGY 7

Table 4. DOE matrix for three process variables with actual COD removal percentage.
Factor A Factor B Factor C
Time (h) Power density (W/L) Working frequency (kHz) Response 1 COD removal (%)
Run
1 0 160 578 0
2 1 160 578 0.24
3 2 160 578 0.48
4 3 160 578 1.43
5 0 240 578 0
6 1 240 578 1.82
7 2 240 578 1.82
8 3 240 578 2.05
9 0 320 578 0
10 1 320 578 3
11 2 320 578 5.46
12 3 320 578 5.22
13 0 400 578 0
14 1 400 578 18.33
15 2 400 578 19.76
16 3 400 578 20.24
17 0 480 578 0
18 1 480 578 30.07
19 2 480 578 47.02
20 3 480 578 49.17
21 0 800 578 0
22 1 800 578 25.42
23 2 800 578 43.57
24 3 800 578 47.05
25 0 1200 578 0
26 1 1200 578 29.50
27 2 1200 578 46.27
28 3 1200 578 49.63
29 0 160 1142 0
30 1 160 1142 0.73
31 2 160 1142 1.46
32 3 160 1142 1.70
33 0 240 1142 0
34 1 240 1142 3.25
35 2 240 1142 11.60
36 3 240 1142 13.23
37 0 320 1142 0
38 1 320 1142 0.73
39 2 320 1142 11.17
40 3 320 1142 11.65
41 0 400 1142 0
42 1 400 1142 13.22
43 2 400 1142 21.30
44 3 400 1142 21.30
45 0 480 1142 0
46 1 480 1142 43.00
47 2 480 1142 42.87
48 3 480 1142 42.87
49 0 800 1142 0
50 1 800 1142 32.33
51 2 800 1142 41.31
52 3 800 1142 41.31
53 0 1200 1142 0
54 1 1200 1142 19.66
55 2 1200 1142 39.49
56 3 1200 1142 40.17

until a peak value is reached then the COD removal
starts to decline. This observation is in accordance
with the experimental results depicted in Figure 3.
Within the investigated range, the maximum COD
removal percentage (49.2%) was obtained at the
optimum time, power density, and frequency of
3 h, 1200 W/L, respectively. The statistical
significance of the results was checked through
F-test of variance ANOVA at the 95% confidence
level (p < .05). As it can be noticed from Table 5,
the model used to represent the 3D plot was
statistically valid as evident from the F-value, the
low probability p value and the correlation coeffi-
cient R2.
8 A. ABDELHAY ET AL.
Figure 8. (a) Contour surface plot of ultimate COD removal % as a function of sonication time and power density at working frequency
of 578 kHz. (b) 3D surface plot of ultimate COD removal % as a function of sonication time and power density at working frequency of
578 kHz.
Table 5. Statistics used to test the adequacy of the reduced
models.
Response F-value p-value R2
Ultimate COD removal % 42.16 <.0001 0.7891
4. Conclusion
The results obtained in this study show that ultrasonic
irradiation is an effective technique to be used for pre-
treating slaughterhouse wastewater. High-frequency
ultrasonication can support the conventional treatment
methods by promoting the initial oxidation of recalcitrant
organic pollutants. However, it can be used as a standa-
lone treatment unit by optimizing the process parameters.
In the experimental part of this work, different operating
variables such as the power density, frequency, initial
COD concentration, pH, and H2O2 addition were tested.
The COD removal increased with increasing the power
density until an optimum power was achieved. The
highest COD removal percentage (49%) was obtained at
a frequency of 578 kHz and a power density of 480 W/L.
At power densities exceeding 400 W/L, samples sonicated
at 578 kHz showed higher COD removal. The COD
removal decreased with increasing the initial COD con-
centration and pH. The kinetic study revealed that the
COD removal during SWW sonication followed the first-
order model. Finally, a combined US/ H2O2 system
efficiently improved the COD removal from SWW.
Disclosure statement
No potential conflict of interest was reported by the author(s).
Funding
This work was financially supported by the German Jordanian
University (GJU) through a seed grant (SNRE (17/2015)).
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