Biomass and Bioenergy 152 (2021) 106198

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Biomass and Bioenergy

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Effect of the ozonation pretreatment on biogas production from waste

activated sludge of tehran wastewater treatment plant
Mahdi Hodaei a, Shahnaz Ghasemi b, *, Arash Khosravi c, d, Manouchehr Vossoughi e
a
Department of Civil Engineering, Sharif University of Technology, Tehran, Iran
b
Sharif Energy, Water and Environment Institute, Sharif University of Technology, Azadi Avenue, Tehran, P.O.Box 11365-8639, Tehran, Iran
c
Sustainable Membrane Technology Research Group, Department of Chemical Engineering, Persian Gulf University, P.O.Box 75169-13817, Bushehr, Iran
d
Sustainable Energy Research Group, Persian Gulf University, P.O.Box 75169-13817, Bushehr, Iran
e
Department of Chemical and Petroleum Engineering, Sharif University of Technology, Tehran, Iran

A R T I C L E I N F O 1 . A B S T R A C T

Keywords: In this study, the ozonation impact on anaerobic digestion of wasted thickened activated sludge of Tehran
Anaerobic digestion wastewater treatment plant has been investigated. Regarding that, the thickened activated sludge, a final solid
Biogas production waste of treatment plants, was subjected to ozonation pretreatment to evaluate its characteristics. Three major
Dewatering
sludge characteristics were considered for investigating ozonation effects on anaerobic digestion. A comparison
Ozonation pretreatment
of two different ozone doses, i.e., 0.05 and 0.1 gO3 g− 1TS was performed for short-term (10 days) and long-term
Thickened activated sludge
(30 days) sludge retention times. Furthermore, biogas production, sludge composition, dewaterability, and en­
ergy balancing, were studied during the periods mentioned above. The results show that the lower ozone dose
has an acceptable performance in a short-term operation for all parameters except energy balance which was
negative in all the scenarios. Higher ozone dosage not only decreased biogas production and volatile solids
reduction but also significantly increased the energy demand of the system. In addition, a longer retention time
reduced the effectiveness of the ozone pretreatment during that time. Eventually, the feasibility of ozone pre­
treatment capacity for sustainable management of different sludge from economic and technological perspectives
can be evaluated by further assessing this case study.

1. Introduction organic solids of sludge have been transformed into biogas containing
CH4, CO2, and a trace amount of other gases [5]. In particular, biogas
Industrial development and ongoing urbanization in recent years, includes 60–70 % methane, 30–40 % carbon dioxide, and a trace amount
along with expansions of the sewage and refining networks, have led to a of nitrogen, hydrogen sulfide, and water [3,6]. Methane gas generated
significant enhancement in sludge production. Stringent regulations for by anaerobic digestion is used to produce electrical energy and reduce
sludge reuse or disposal have forced both public and private sludge the operating cost of treatment plants [6]. Furthermore, this approach
generators to administer their own sludge management strategies [1]. decreases methane leakage through natural routes from landfills and
There are currently three main ways for sludge disposal, including reduces CO2 production by utilizing methane instead of using fossil fuels
incineration, landfilling, and ocean disposal. However, in most cases, as a treatment plant’s energy source [3]. However, the production of a
strict landfilling criteria and a ban on dumping sludge in the oceans considerable amount of digested materials, and the high content of the
made reusing sludge more attractive [2]. In addition, anaerobic diges­ degradable organic compounds in the digested matter, can result in a
tion of waste-activated sludge has been widely considered as an envi­ significant increase in soil microbial activity. Recycled materials in
ronmentally friendly wastewater treatment due to the sludge sludge technically and economically can be divided into two categories,
stabilization as well as a reliable source of renewable energy for materials for nutrients (i.e., Nitrogen & Phosphorus) and materials for
wastewater treatment plants [2,3]. energy (Carbon) [7]. The presence of non-biodegradable components
Besides, anaerobic digestion is considered the most effective and that are relatively resistant to decomposition as well as complicated
accessible energy recovery from sludge [4]. Applying this method, organic matter (i.e., proteins and lipids) leads to a decrease in anaerobic

* Corresponding author. ,
E-mail addresses: [email protected] (M. Hodaei), [email protected] (S. Ghasemi).

https://doi.org/10.1016/j.biombioe.2021.106198
Received 4 February 2021; Received in revised form 24 June 2021; Accepted 18 July 2021
Available online 23 July 2021
0961-9534/© 2021 Elsevier Ltd. All rights reserved.
M. Hodaei et al. Biomass and Bioenergy 152 (2021) 106198

digestion’s efficiency [8]. In this regard, simultaneous hydrolysis of calculated in order to assess the ozonation efficiency and sustainability.
organic substances and bacterial cells inhibit anaerobic digestion per­
formance [9]. Sludge pretreatment is one of the practical approaches to 2. Materials and methods
enhance anaerobic digestion efficiency, helps destroy bacteria’s cell
wall. Furthermore, pretreatment techniques accelerate the decomposi­ 2.1. Sludge composition and dewatering capacity measurement
tion of complex organic components into smaller and simpler ones
which in turn can increase the sludge hydrolysis rate [10]. Three different sludges, including raw primary sludge, activated
Accelerating the whole digestion process, reducing sludge retention thickened sludge, and digested sludge, were provided from the South
time, and increasing biogas production rates are mentioned as other Tehran wastewater treatment plant as the largest and most advanced
benefits of sludge pretreatment [11,12]. All pretreatment methods aim wastewater treatment plant in Iran. These sludge types are typical in
to speed up the digestion process and increase sludge dewaterability. conventional wastewater treatment plants, and their analysis could
However, the research results demonstrated that pretreatments signifi­ show the performance of the anaerobic digestion facility. Volatile solids
cantly affect active sludge digestion rather than primary sludge [13]. (VS) and total solids (TS) content of the different types of sludges were
Pretreatment methods are categorized into three main categories, measured by standard methods [32].
physical, chemical, biological, or a combination of these categories [14]. Sludge dewatering capability as the most critical parameter of sludge
Chemical pretreatment techniques utilizing acids, bases, and strong quality was determined using centrifugation with 3000 rpm for 5 min
oxidation agents such as ozone are considered more popular due to their after solids were settled. Remained solid volume was considered as
simple operation and high efficiency. However, chemical oxidation dewatered sludge, followed by measuring the dry solid content; Volu­
pretreatment with ozone is more effective than acids or bases because metric Dewatering Percentage (VDP) was calculated volumetrically by
ozone does not change sludge salt concentration. Besides, ozone can the following equation [33]:
decompose a wide range of organic and inorganic materials [15]. As a
V0 − VSludge
powerful oxidizing agent, ozone reacts with the bacteria’s cell walls VDP = × 100 (1)
V0
rapidly, killing microorganisms in the sludge and oxidizing complex
organic matter to a simpler compound [16–18]. In a closer look, it reacts where V0 is the initial sludge volume (30 ml for each test), and VSludge is
with polysaccharides, proteins, and lipid membranes of the cell, con­ the dewatered sludge volume after centrifuge.
verting them into simpler molecules that have a higher biodegradation
rate. As a result, it could enhance biogas production in the anaerobic
digestion process compared with raw sludge [19–21]. On the other 2.2. Ozonation and anaerobic digestion systems
hand, if the ozone concentration would be high enough, it can convert
cell components into minerals like H2O and CO2 and consequently The experimental setup consisted of two ozonation and anaerobic
reduce biogas production [22]. For the balance of cost and efficiency, digester reactors. The ozonation reactor was constructed from two cy­
the amount of ozone should be optimized gO3 per gTS. The optimum lindrical glass chambers with a volume of 2 L. The first chamber was
amount of ozone depends on the sludge characteristics and the test utilized for sludge ozonation, while the second cylindrical glass chamber
condition [23,24]. Ozone dose varies according to its application in containing water was used to neutralize the residual ozone coming out
wastewater treatment because ozone is being used in a broad range of from the first cylindrical chamber. A flow controller was installed on the
applications in wastewater treatment processes like disinfection as first chamber to control the ozone generator flow (PCM5 model, made in
advanced treatment or pretreatment for increasing the degradability of Iran, the production rate of 5 g h-1, the discharge rate of 5 L min− 1, 100
organic substances [24–26]. Therefore, the ozone dose depends on the W). An anaerobic digester reactor (ADR), as a batch-type reactor, was
purpose of the ozonation and waste type and varies from few micro­ constructed from a 5-Liter cylindrical glass container equipped with a
grams to several milligrams per carbon content of the sludge, as dis­ heater and thermometer to adjust the temperature. A scheme of the
cussed in the previous studies [27,28]. Most of the earlier researches on experimental set-up has been presented in Fig. 1.
the ozonation pretreatment mainly focused on ozone dose and its effects The sludge inlet was on the top of the reactor, and the sludge outlet
on sludge composition and biogas production [29–31]. However, a was on the bottom, which was used for sampling without any gas
comprehensive study that evaluates all aspects of ozonation pretreat­ leakage from the digester. The gas outlet of ADR was connected to the
ment, including retention time, dewatering, and energy balance in pressure gauge and flow meter to measure biogas pressure and volume.
addition to conventional parameters, is missing from the literature. The ozonation process was carried out in four steps. The first to third
In this study, the ozonation pretreatment impact on experimental steps were performed with the volume of 0.5 L sludge, while the final
parameters of anaerobic digestion and sludge deposal was thoroughly step was fulfilled by 0.3 L sludge. Overall, 1.8 L ozonated sludge was
investigated. Regarding that, three categories of experimental parame­ prepared for the ADR. Through all these steps, the ozone dose and
ters that are very useful in an actual wastewater treatment plant for contact time were carefully controlled. The short-term sludge retention
sludge management have been investigated. The first category of pa­ time was considered ten days because of the similarity to the actual
rameters consisted of the chemical composition of the sludge, particu­ sludge retention time of digesters in the South Tehran wastewater
larly volatile solids and total solids concentration. The second category treatment plant, while the long-term retention time was determined to
is the dewaterability of sludge, which is very important for sludge be 30 days. The temperature of the digestion process was set at meso­
disposal management according to the high cost of sludge transmission philic conditions (35 ◦ C). Therefore, all experiments were carried out in
to the landfill. Finally, the third category is referred to energy balance, the same qualitative and quantitative conditions, and the only variable
including biogas production and ozonation energy demand, which is was the ozone dose and sludge retention time. For the first experiment as
essential for assessing the sustainability of the ozonation pretreatment. a control test, ADR was fed with untreated waste thickened activated
Considering these parameters, sludge pretreatment has been performed sludge (WTAS). For the rest of the experiments, ADR was supplied by
using two ozone doses of 0.05 and 0.1 g of O3 per total solid (TS) (g O3 ozone-pretreated WTAS. The operating conditions of each test have been
g− 1 TS). The effect of ozonation on the performance of anaerobic summarized in Table A1 in supporting information.
digestion, including biogas production, sludge chemical composition
(particularly total solids (TS) and volatile solids (VS) concentration), 2.3. Biogas production
and digested sludge dewatering (which causes high sludge transition
cost), was evaluated in a short and long time sludge retention time. The biogas production rate was measured through both pressure
Eventually, the energy balance of the ozonation approach was measurement using a gauge and volume measurement using a flow

2
M. Hodaei et al. Biomass and Bioenergy 152 (2021) 106198

Fig. 1. A scheme of the experimental setup.

meter connected to the ADR gas outlet. It should be noted that the sol­ pressure. Generated biogas energy was calculated considering the
ubility of CO2 and CH4 in the sludge was neglected due to insignificancy. composition of 65 % methane and 35 % carbon dioxide identified using
In the current research, the maximum degradation rate (L biogas. kg− 1 gas chromatography analysis, which has the same composition as the
VS. d− 1) and cumulative biogas production (L biogas. kg− 1 VS) were previous studies [36]. The total produced biogas energy was derived
considered as two main factors for comparison. The maximum degra­ from the following equations:
dation rate was derived from the slope of the curve during the meth­
VCH4
anogenesis stage of the anaerobic digestion process. The cumulative Hu.act = × ρact
CH4 × Hu,n (6)
VTotal
biogas production (CBP) was determined using equation (2) [34]:
∑
Vt,biogas Ebiogas = Hu.act × Vbiogas (7)
CBP = (2)
VSin
where Hu,n is the normal calorific value of biogas equal to 50,000 kJ
where Vt, biogas is the volume of produced biogas in time of t (day), and kg− 1, Hu,act is the actual calorific value of given biogas ( kJ
kg ), and Vbiogas is
VSin is the initial volatile solids concentration in ADR. The impact of the biogas volume (L). Eventually, energy balance was measured by the
ozonation on the conversion of volatile solids to biogas was evaluated by following equation.
calculation of the biogas production yield by the following equation:
(Bioassay for monitoring biochemical methane potential and anaerobic Energy balance = Eozonation − Ebiogas (8)
toxicity)
3. Results and discussion
PB
BPY = (3)
VSreduced Three types of sludges, such as waste thickened activated sludge,
primary sludge, and digested sludge, were considered in this study. The
where BPY is the biogas production yield [L biogas. kg− 1 VSreduced], PB
moisture and the volatile solid concentration of these sludge types have
stands for the produced biogas [L], and VSreduced is the amount of vol­
been shown in Fig. A1 in supporting information. Therefore, comparing
atile solids that are converted to biogas [kg].
the chemical characteristics of these sludge types helps us estimate the
performance of the anaerobic digestion process of the treatment plant.
2.4. Energy balance measurement
As the results in Fig. A1 demonstrated, the removal of volatile solids
in the anaerobic digester of the treatment plant is not sufficient. The
The energy consumed to produce ozone for each test was calculated
reason for this problem is that the ten days retention time for sludge in
using the following equations:
the digester is not enough time to complete the hydrolysis process due to
Eozonation = W × t (4) its complexity. Besides, pretreatment of waste thickened activated
sludge is more efficient than primary sludge due to less degradable
where W is the ozone generator power (100 W), t is the ozonation period substances in this sludge than primary sludge [37]. Therefore, the
in seconds. Since the energy consumption of the heater was the same for ozonation impact on the anaerobic digestion of waste-thickened acti­
all tests, therefore it was ignored in this estimation. Therefore, only vated sludge was investigated in this study. The characteristics of the
ozonation energy was considered as consumed energy. The produced waste thickened activated sludge has been shown in Table A2 in sup­
energy through the anaerobic digestion process was calculated using the porting information.
ideal gas law. For this reason, at first, methane density was calculated at
the pressure and temperature of each test conditions [35] as follow:
3.1. Effect of ozonation dosage on biogas production
Pact Tstd
ρ act
=ρstd
× × (5)
CH4 CH4
Pstd Tact The pretreatment of the waste-thickened activated sludge was car­
ried out using two doses of 0.05 and 0.1 g of O3 per total solid (g O3 g− 1
whereρact
CH4 is the methane density at standard temperature and pressure TS). The impact of ozonation on cumulative biogas production for
(0.72 kg m− 3), Tstd is the standard temperature (273 K), Pstd is the retention times of 10 and 30 days has been depicted in Figs. 2 and 3,
standard pressure (101.325 kPa), the Tact is the gas temperature (303 K), respectively. As Fig. 2 shows, the produced biogas was significantly
and Pact is the total pressure equal to the gauge pressure plus air increased for ozone-treated sludges compared to untreated sludge for

3
M. Hodaei et al. Biomass and Bioenergy 152 (2021) 106198

composition section and Fig. 3.

As indicated in Fig. 3, different behavior was observed for the effect
of varying ozone dose in biogas production in the long-term retention
time of 30 days. Furthermore, it was demonstrated that ozonation made
not only CBP curves stepper (MDBP of untreated sludge increased from
5.01 biogas. kg− 1 VSin.d− 1 to around 6.26 biogas. kg− 1 VSin.d− 1 using
ozonation) but also decreasing main methanogenesis phase starting
point, which means ozonation successfully could accelerate AD process
both in shortening hydrolysis phase and providing more degraded
organic matter for methanogenic bacteria. However, the maximum daily
biogas production was equal for both ozone doses, which means the
higher ozone dose forms non-biodegradable by-products that cannot be
destroyed by anaerobic bacteria, suggesting that longer time or higher
ozone doses could be unnecessary.
Despite these promising consequences, some quantitative compari­
sons deserving of increasing sludge retention time need to be investi­
gated. First, the difference between the CBP ratio of untreated sludge
and the average of the ozonized sludge decreased from 22.86 L biogas.
Fig. 2. Variation of cumulative biogas production in the retention time of
kg− 1 VSin to 14.626 L biogas. kg− 1 VSin over time, which means the
10 days.
difference between cumulatively produced biogas of the untreated
sludge and ozonized sludge decreased at the end of the 30 days. Besides,
the CBP difference increased from − 3.57 L biogas. kg− 1 VSin to 1.67 L
biogas. kg− 1 VSin at the end of the 10th compared to the end of the 30th
day for ozonized sludges with different ozone doses that indicate higher
ozone dose has a negligible effect on the final produced biogas amount
in a long time.
Secondly, the main methanogens phase for untreated sludge started
on the 12th day, and CBP gradually increased till the 14th day, which
reached its maximum value. It continuously increased till the 24th day.
All the CBP variations were smooth, corresponding to the typical
exponential growth of the anaerobic bacteria [40]. On the other hand,
the methanogenesis phase for ozonized sludge started earlier. It ceased
on the 21st day, which means no more degradable organic matter was
left in the sludge for methanogenic bacteria on that day. It might be due
to the fact that ozonation pretreatment significantly affected the accel­
eration of degrading organic matter and overall anaerobic digestion
process rather than exceeding degradable organic matters or even
higher ozone dose caused mineralization of organic matters [41].
In conclusion, investigating biogas production in the long term vs.
Fig. 3. Daily cumulative biogas production in 30 days. short term can indicate the importance of the sludge retention time in
biogas production. According to acquired data from the experiment,
the retention time of 10 days. In particular, cumulative biogas produc­ ozonation pretreatment positively affected biogas production in the
tion (CBP) increased to 169 % for 0.05 g O3 g− 1 TS and 140 % for 0.1 gO3 short-term retention time of sludge in the anaerobic digestion process.
g− 1 TS ozonized sludge. However, its effectiveness faded away in higher retention time. As a
Maximum daily biogas production (MDBP) increased from 2.08 L result, higher sludge retention time not only has a limited influence on
biogas. kg− 1 VSin.d− 1 for untreated sludge to 6.26 L biogas. kg− 1 VSin. biogas enhancement but also drastically increases the operational cost of
d− 1 for ozone-treated sludges, indicating the ozonation pretreatment the wastewater treatment plant when ozonation is used as sludge pre-
accelerated methanogenesis mechanism. The biogas production volume treatment. Therefore, optimization of the sludge retention time (SRT)
reached its maximum (which can be considered as the main methano­ should be performed to maximize biogas production and minimize
genesis period) on the 6th and 7th days for 0.05 gO3. g− 1TS and 0.1 operation costs when ozonation pretreatment is implemented for the
gO3g− 1TS ozonated sludges, respectively. The main methanogenesis anaerobic digestion process. Determining optimum SRT depends on the
stage begins when the biogas production curve reaches the upward factors such as the ozonation method (i.e., micro bubbling, macro
linear zone. Considering Fig. 2, the linear zone started on the 6th and 7th bubbling, etc.) and anaerobic digestion operational parameters (i.e.,
days for 0.05 gO3g− 1TS and 0.1 gO3g− 1TS, respectively. It can be temperature, pH, CperN ratio, etc.). It may vary from sludge types and
concluded that a higher amount of the ozone concentration not only treatment plants as well. Besides biogas production, other ozone con­
decreases the CBP at the end of the 10th day but also delayed the sequences, particularly in sludge composition, dewaterability, and en­
beginning of the main methanogenesis stage while triggering the CBP for ergy balance, need to be considered in determining the most appropriate
the first day. The obtained results are consistent with the findings of the SRT and ozone dose.
previous study, which indicated higher ozone doses (0.08 and 0.10
gO3g− 1TSS) adversely affected biogas production [38]. The CBP rate is 3.2. Effect of ozonation pretreatment on sludge composition
increasing linearly after the 3rd day for 0.05 gO3. g− 1TS ozonated sludge
till the end of 10 days, while the CPB of the higher ozone dosage was 3.2.1. Impact of ozonation pretreatment on TS and VS reduction
decreased between 5th and 7th. The reason for that is the effects of Fig. 4 shows the concentration of TS and VS of each test after the
higher ozone dose on the sludge composition parameters, especially pH, retention time of 10 and 30 days.
which led to the formation of by-products less biodegradable than un­ As shown in Fig. 4 (a), at the end of the 10th day, the total solids
treated substrate [39]. This fact was elaborated in the sludge concentration decreased from 38.8 gl-1 to 32.8 gl-1 and 34.2 gl-1 for 0.05

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M. Hodaei et al. Biomass and Bioenergy 152 (2021) 106198

Fig. 4. The effect of the ozonation pretreatment on TS and VS reduction. (a) Total solids, (b) Volatile solids.

g O3g− 1 TS and 0.1 g O3g− 1 TS ozonized sludges, respectively.

Comparing these values with the initial TS concentration of 49.3 gl-1, the
calculated TS reduction rate increased from 21.3 % for untreated sludge
to 33.4 % and 30.6 % for 0.05 g O3g− 1 TS and 0.1 g O3g− 1 TS, respec­
tively. Obtained results from the long-term operation of the anaerobic
digestion revealed that the effectiveness of the ozonation on TS reduc­
tion is decreasing over time. For instance, the TS reduction rate at the
end of the 30th day for untreated sludge was 59.6 %, which increased to
62.2 % and 62.6 % for ozonized sludge, respectively. As demonstrated in
Fig. 4 (b), the same trend was observed for VS reduction because the
main reason for the TS removal was VS degradation and conversion to
biogas. Since mineral concentration was approximately constant during
the experiment (around 10 gl-1); therefore, the only parameters that can
alter total solids are the amount of the volatile solid.
As Fig. 4(b) elucidated, the volatile solids concentration at the end of
the 10th day decreased from 29.4 gl-1 for untreated sludge to 22.6 gl-1
for 0.05 g O3g− 1 TS and 23.5 gl-1 for 0.1 g O3g− 1 TS ozonized sludge. It
should be noticed that the higher ozone dose slightly decreased VS
reduction, which is in line with the decrease in biogas production in
higher ozone dose in 10 days of AD operation. The evaluation of the
ozonation effect on VS reduction shows the same variations as the last
part. The final VS concentration in both untreated and ozonized sludges
was close at the end of the 30th day.
Reduction in volatile solids degradation rate in higher ozone dose is
similar to previous research that volatile solids reduction by 0.063 g O3
g− 1 TS ozonation increased to 65 % while increasing the amount of
ozone to 0.083 g O3 g− 1 TS and 0.1 g O3 g− 1 TS, the amount of volatile
solid reduction dropped to 55 % and 57 %, respectively [38]. This
phenomenon occurred for two reasons. The first possibility is that the
organic materials were converted to minerals due to high ozone con­
centration [41–44]. Since the mineral concentration was approximately
constant with increasing ozone dose during all tests (about 10 gl-1), this
reason is not acceptable. The second reason could be acidic pH, which
inhibited the methanogenesis process. The acidity of the anaerobic
digestion process will be evaluated by the biochemical activity of bac­
teria. The methanogenic bacteria converted volatile fatty acids to
methane and carbon dioxide and stabilized the pH of the anaerobic Fig. 5. (a) The effect of ozonation pretreatment on pH variation (b) the impact
digestion process is which can effectively balance anaerobic digestion of ozone dose and pH variation on biogas production during the AD process in
acidity [45]. It is evident that ozonation accelerates the hydrolysis rate 10 days.
of organic matter, and higher ozone doses would increase it.
Consequently, 0.1 g O3 g− 1 TSozonation dose, speeding up hydro­ 7.2 to 6.45 for 0.05 g O3 g− 1 TS ozonized sludge. Increasing ozone dose
lysis, increases the concentration of volatile fatty acids while meth­ to 0.1 g O3g− 1 TS, the pH dropped to 6.45 on the 5th day, which, as
anogenic bacteria do not be able to convert them to biogas. Therefore, demonstrated in Fig. 5(b), biogas production was at the minimum rate,
system acidity will be increased, and pH will drop below the optimum and then it rose again along with the enhancement of biogas production.
pH of methanogenesis bacteria, which is between 6.5 and 7.2 [46–49]. Hence, this evidence proved that higher ozone dosage speeds up the
In particular, a pH lower than 6.7 will reduce methanogenic activity hydrolysis process with the rate that methanogenesis bacteria cannot
[50]. To prove this hypothesis, pH variation during the first 10 days was cope with that in a short time; therefore, biogas production would be
measured, and the results were demonstrated in Fig. 5(a). The effect of decreased.
ozone dose and pH variation on biogas production has been depicted in Despite the different ozone effects on sludge composition in the short
Fig. 5(b). Considering Fig. 5(a), pH varies from 7.2 to 7 untreated sludge retention time, it has a constant impact in a long time. In particular, TS
and 7.2 to 6.9 for 0.05 g O3 g− 1 TS ozonized sludge, while it ranges from and VS decreased as the ozone dose increased. However, the difference

5
M. Hodaei et al. Biomass and Bioenergy 152 (2021) 106198

between the final TS and VS concentration after 30 days was the same and 36 % for 0.05 g O3 g− 1 TS and 0.1 g O3 g− 1 TS ozonized sludge,
for each test. It shows that ozonation efficiency will be decreased over a respectively in 10 days (Fig. 6(a)), which is higher than the average dry
long time, as observed in the previous part. solids concentration of filtered sludge (20–25 % dry solids). These re­
sults are along with previous studies in which ozonation effectively
3.2.2. Effect of ozonation pretreatment on biogas production yield (BPY) enhanced sludge amount after dewatering [55,56]. However, after 30
BPY is an essential factor that implies converting the rate of organic days of digestion, dry solids reached 48 % for untreated sludge and up to
matters into biogas. Table 1 shows the BPY values for each test. As ob­ 50 % for ozonized sludges indicating that ozonation has less influence on
tained results show, the ozonation pretreatment significantly increased dewaterability in long-term digestion (Fig. 6(a)).
sludge BPY by 62.23 % for 0.05 g O3g− 1 TS and 53.12 % for 0.1 g O3g− 1 These results are conflicts with previous researches about ozone
TS in the retention time of 10 days, which is correlated to previous pretreatment effect on sludge dewaterability, indicated low ozone dose
studies that proved ozonation pretreatment successfully enhance biogas (<400 mgO3g− 1 TS) decreases sludge dewaterability [57,58] due to
yield [51,52]. Otherwise, these values drastically dropped to 7.760 % enhancement of SRF (sludge resistance to filtration) and CST (capillary
and 6.940 % for ozonized sludge after 30 days of the AD operation, suction time) by producing more fine particles [36]. Ozonation can
which is not directly pointed in the previous studies. In fact, ozonation significantly affect the physicochemical properties of the sludge, which
enhances the degradation rate of complex organic matters, which aided is directly related to sludge dewaterability. Many researchers utilized
biogas production as well as VS reduction. However, no significant ef­ belt filter press or similar methods for sludge dewatering. The perfor­
ficiency has been observed for ozonation in long sludge retention time, mance of these methods can be quantified by optimizing variables like
resulting from the sludge type and characteristics. CST, hydrophobicity, etc. However, these parameters depend on some
specific sludge properties, including available particle surface area to
3.3. Effect of ozonation on sludge dewaterability contact with water-bound, protein content, EPS concentration, and
dissolved matter that ozonation pretreatment can efficiently improve
As one of the essential parts of the wastewater treatment plant, the them in a higher dose [53]. The centrifuge method, independent of
digested sludge dewatering process has the highest operational costs. It available particle surface area and more effective for separating water
is critical decreasing sludge volume to minimize the cost of transporting from a residual part of sludge in low ozone dosage, was implemented for
sludge to the landfill, especially for the South Tehran wastewater plant dewatering in the current research. It may be because ozone first dis­
due to the high production of sludge volume and lack of available rupts the aggregated flocs, destroys the bacteria cell’s wall, emits
landfills. The dewatering process has been carried out by various intercellular water, and destroys complex matter into simple structures
physical methods such as vacuum filter, centrifuge, belt press, etc. In the [53]. In other points of view, fine particles could retard filtration by
filtration approach as a typical technique for dewatering, capillary clogging filter porous media while the centrifuge process is not influ­
suction time (CST) and sludge resistance to filtration (SRF) are consid­ enced by fine particles [59–61].
ered as quantitative indexes for the evaluation of the dewatering per­
formance [53]. In the current study, the centrifuge was utilized for 3.4. Energy balance of ozonation pretreatment
dewatering, and VDP (Volumetric Dewatering Percentage) and dry
solids (DS) were considered as evaluation factors of dewaterability The significant factors affecting the total cost of the scaling up
performance. Three samples were performed for each experiment. The ozonation pretreatment for treatment plants are energy production and
obtained results for VDP and dry solids for different retention times were consumption. Therefore, the produced and consumed energy for ozone
demonstrated in Fig. 6. pretreatment as well as energy balance have been calculated here. The
As the results of Fig. 6 depicted, the ozonation pretreatment with results were summarized in Table 2. It should be noted that because of
different dosages increases the sludge dewaterability and obtained dry the ideal condition assumption, energy loss is supposed to be negligible
solids in short and long retention times compared to untreated sludge; during ozonation and sludge digestion; consequently, it was not entered
therefore, it has a great impact on the reduction of residual sludge into the calculation. On the other hand, energy balance measurement is
volume as well as its water content. In particular, VDP increased from a comparative analysis between ozonation energy demand and final
50 % for untreated sludge to 58 % and 61 % for 0.05 g O3 g− 1 TS and 0.1 produced energy to reveal the sustainability of ozonation pretreatment.
g O3g− 1 TS ozonized sludges respectively in 10 days (Fig. 6(a)). More­ As indicated, values of consumed energy in comparison with pro­
over, the conversion of organic substances to biogas decreases sludge duced energy for ozonized sludge are very high. In particular, 0.05 g O3
content [23]; therefore, VDP has increased over time, and consequently, g− 1 TS and 0.1 g O3 g− 1 TS ozonized sludges could provide only 37.8 %
sludge dewatering has become easier. However, Fig. 6(b) revealed that and 28.5 % of their consumed energy for ozonation in 10 days. These
the differences between the dewaterability of various ozone doses values were increased over time because of more biogas production
decreased in the long retention time due to changes in sludge texture. during the anaerobic digestion process. Besides, the energy balance for
Moreover, the sludge residue will become very thick in the higher all ozone pretreatment tests is negative in the short and long retention
dewatering process, and the DS increased above 50 % for ozonized time, which indicates ozonation has high energy demand as a pre­
sludge after 30 days. Besides, it indicates that sludge dewaterability treatment method. Still, it should be considered that ozonation has other
increased in higher ozone dosage because ozonation in low doses causes benefits, including reducing organic carbons, increasing sludge dew­
particle size reduction, which deteriorates sludge dewaterability [54]. atering, and also reducing methane leakage through landfills. Therefore,
Dry solids for untreated sludge was 20 % and increased up to 28 %, rather than energy demand, other comprehensive economic analyses are

Table 1
Effect of ozonation pretreatment on Biogas Production Yield.
Short-Retention time (10 days) Long-Retention time (30 days)
− 1 1
Ozone dosage (g O3g TS) Ozone dosage (g O3g− TS)

Untreated 0.05 0.1 Untreated 0.05 0.1

Biogas Volume(L) 1.050 2.820 2.520 6.450 7.440 7.560

Reduced VS(kgl− 1) 0.0104 0.0172 0.0163 0.0293 0.0314 0.0322
BPY 100.6 163.15 153.98 219.5 236.5 234.6
Difference (%) – +62002E23 +53.12 – +7.760 +6.940

6
M. Hodaei et al. Biomass and Bioenergy 152 (2021) 106198

Fig. 6. Ozonation pretreatment effects on sludge dewaterability and obtained Dry Solids for the retention times of (a) 10 days (b) 30 days.

Acknowledgments
Table 2
Effect of ozonation on energy balance.
The authors are grateful to the Sharif University of Technology. This
Short-term (10 days) Long-term (30 days) research did not receive any specific grant from funding agencies in the
Ozone dose [g O3g− 1 0 0.05 0.1 0 0.05 0.1 public, commercial, or not-for-profit sectors.
TS]
Ozonation Energy [kJ] 0 324 388.8 0 324 388.8
Appendix A. Supplementary data
Produced Energy [kJ] 44.4 122.7 110.9 272.7 323.7 332.7
Energy Balance [kJ] 44.4 − 201.3 − 277.9 272.7 − 0.3 − 56.1
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.biombioe.2021.106198.
needed to evaluate whole aspects of ozone pretreatment, which is out of
the scope of this research, and it is strongly recommended for further Data availability
investigation. Nevertheless, we believed that the obtained results could
provide useful information about the feasibility of ozone pretreatment The raw data will be available based on request.
capacity for sustainable management of different sludge from economic
and technological perspectives. All obtained results in this study are References
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