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Applied Radiation and Isotopes 130 (2017) 270–275

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Applied Radiation and Isotopes


journal homepage: www.elsevier.com/locate/apradiso

Radiotracer investigation and modeling of an activated sludge system in a MARK


pulp and paper industry
Metali Sarkara, Vikas Kumar Sangala, Vijay Kumar Sharmab, Jitendra Samantrayb,

Haripada Bhuniaa, Pramod Kumar Bajpaia, Anil Kumarc, Anil K. Naithanic, Harish Jagat Pantb,
a
Department of Chemical Engineering, Thapar University, Patiala 147004, Punjab, India
b
Isotope and Radiation Application Division, Bhabha Atomic Research Centre, Mumbai 400085, Maharashtra, India
c
Shreyans Paper Ltd., Ahmedgarh, Sangrur, Punjab 148021, India

H I G H L I G H T S

• ARTDs
radiotracer investigation was carried out in an activated sludge process system.
• Mean ofhydraulic
an aeration tank and secondary clarifier were measured.
• The measured RTDsresidence times and dead volumes were determined.
• were simulated using suitable models.

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

Keywords: A radiotracer investigation was carried out in an activated sludge process (ASP) system of an effluent treatment
Activated sludge process, Aeration tank plant in a pulp and paper industry. The system consists of an aeration tank and a secondary clarifier connected in
Secondary Clarifier series. The primary objective of the investigation was to measure mean hydraulic retention times (MHRTs) of
Radiotracer wastewater and investigate the hydraulic performance of the ASP. Residence time distributions (RTD) of the
Iodine-131
wastewater were measured in an aeration tank and a secondary clarifier of the system using Iodine-131 as a
Residence time distribution
Mean hydraulic residence time
radiotracer. The measured RTD data was treated and MHRTs were estimated. No bypassing was found to exist in
Bypassing the aeration tank and the secondary clarifier. However, the dead volume in the aeration tank and the secondary
Dead volume clarifier was found and estimated to be 2.34% and 4.6%, respectively. The treated curves were further simulated
Tanks-in-series with backmixing model using suitable hydraulically representative mathematical models and detailed flow patterns in the aeration tank
Axial dispersion model and the secondary clarifier were deciphered.

1. Introduction bodies, causes an adverse effect on human health and the environment.
The adverse impact such as excessive solid accumulation, eutrophica-
Pulp and paper industry is a water intensive industry that uses water tion, oxygen depletion in the receiving bodies and chemical accumu-
for most of its processes. Water is used in all stages of the paper pro- lation in aquatic food web caused by discharge of wastewater from the
duction, including washing of raw materials, pulping, bleaching and pulp and paper industries on aquatic system has been studied and re-
operation of various machines. Water is also used for cooling of ported by many researchers (Afroz and Singh, 2014; Ali and
equipment, cleaning of systems and generation of steam for process use Sreekrishnan, 2001; Andersson et al., 1988; Owens, 1991). Over the
and on-site electricity production. Although most of the process water is years the growing concern about the environment has led water in-
recycled, still a significant amount of wastewater is generated during tensive industries such as pulp and paper industry to implement ne-
the pulp washing. The quality and quantity of wastewater generated cessary treatment processes to treat wastewater to predefined standards
vary according to the process adopted by specific industry (Kamali and before final disposal in the open atmosphere.
Khodaparast, 2015; Thompson et al., 2001). The untreated effluent or Various wastewater treatment technologies comprising of a combi-
wastewater contains a considerable amount of organics and toxic pol- nation of primary, secondary and tertiary treatment processes are ap-
lutants, which when discharged in the open atmosphere or water plied depending on the degree of treatment required (Bajpai, 2001). As


Corresponding author.
E-mail address: hjpant@barc.gov.in (H.J. Pant).

http://dx.doi.org/10.1016/j.apradiso.2017.10.016
Received 12 April 2017; Received in revised form 20 July 2017; Accepted 7 October 2017
Available online 10 October 2017
0969-8043/ © 2017 Elsevier Ltd. All rights reserved.
M. Sarkar et al. Applied Radiation and Isotopes 130 (2017) 270–275

the wastewater produced in the pulp and paper industry contains a


substantial amount of organics, biological treatment becomes an es-
sential part of the treatment process. Activated sludge process (ASP)
developed in early 1900 remains one of the most widely used and ef-
ficient process for biological treatment of wastewater produced in the
pulp and paper (Metcalf & Eddy et al., 2003). The process involves
mixing and aeration of suspended microbe culture in a tank to maintain
the aerobic conditions to breakdown the dissolved organic pollutants in
the effluent wastewater into biomass. The biomass formed is separated
from the treated effluent in a secondary clarifier (Peavey et al., 2013;
Metcalf & Eddy et al., 2003). The system (aeration tank and secondary
Fig. 1. Schematic diagram (front view) for radiotracer experiment in ASP system.
clarifier) in which the process is carried out is called as activated sludge
process (ASP) system. The aeration tank used in an ASP consumes
around 45–75% of the total energy required to operate a wastewater mixing of wastewater and air in the aeration tank. The secondary
treatment plant (WWTP) in a pulp and paper industry resulting in high clarifier is a circular settling tank having a diameter of 18 m, height of
operating cost (Karpinska and Bridgeman, 2016; Rieger et al., 2006). 3.71 m and capacity of 944 m3 with a peripheral feed mechanism. The
Therefore, the optimum functioning of an ASP is essential both from the treated wastewater from the aeration tank flows into the secondary
environmental and economic point of view. clarifier which acts as a settling tank where biomass settles at the
The efficient operation of an ASP depends upon parameters of the bottom. About 20% (1.04 m3/min) of the under flow from the sec-
wastewater i.e. mean hydraulic retention time (MHRT), degree of ondary clarifier is recycled back to the aeration tank to maintain the
mixing (flow pattern) and occurrence of flow abnormalities within the mixed liquor suspended solids (MLSS) concentration of 3500 mg/l in
system such as bypassing, channeling, recirculation and dead volume the aeration tank. A part of settled biomass is subsequently removed
etc. Measurement and analysis of residence time distribution (RTD) of from the bottom of the clarifier and used as organic manure. The
wastewater in the ASP can provide insight to its hydrodynamic per- treated wastewater is obtained from the secondary clarifier overflow.
formance. Conventional tracers such as dyes, salts and chemicals have
been used to measure the RTD of wastewater and investigate flow 2.2. Radiotracer experiments
characteristics of various systems in WWTPs (Bode and Seyfried, 1985;
Burrows et al., 1999; Gresch et al., 2011; Makinia and Wells, 2005; The radiotracer experiments were performed in an ASP meant for
Kjellstrand et al., 2005). However, there are many disadvantages are wastewater treatment at M/s Shreyans Paper Ltd, Ahemedgarh, India.
associated with the use of conventional tracer, such as cumbersome and The experimental setup is shown in Fig. 1. Stimulus-response approach
manual offline monitoring of tracer data and relatively higher degree of was used to measure the RTD of the wastewater in the aeration tank and
inaccuracy in measurement and analysis. All these disadvantages are the secondary clarifier. Iodine-131 (half-life: 8 days, gamma energy:
overcome by using radiotracer techniques (IAEA, 2008, 2011). Several 0.36 MeV) as NaI aqueous solution supplied by Board of Radiation and
authors have used these techniques for measurement of RTD in various Isotope Technology (BRIT) Mumbai, India,was used as a radiotracer to
systems in wastewater treatment plants (Ambrose et al., 1957; Burrows measure RTD of the wastewater. Although, Bromine-82 (half-life: 36 h
et al., 1999; Farooq et al., 2003; Debien et al., 2013; Jung et al., 2004; and gamma energies: 0.55, 0.62, 0.70, 1.48 MeV) and Technitium-99 m
Kim et al., 2005; Kasban et al., 2010; Kumar et al., 2012; Makinia and (half-life: 6 h, gamma energy: 0.14 MeV) are more suitable radiotracers
Wells, 2005; Pant et al., 2000, 2009, 2012; IAEA, 2008, 2011). Al- for tracing the wastewater in WWTPs, but in the present investigation,
though radiotracer experiments have been performed on various sys- Iodine-131 was used because of its easy availability, ease of transpor-
tems in wastewater treatment plants but the results obtained in a par- tation and relatively longer half-life thus facilitating the measurements
ticular system cannot be generalized as every single system uses at a far remotely located wastewater treatment plant (~1700 km) from
different raw material and process, design parameters and operating the nuclear reactor. Two different RTD runs were carried out and about
conditions. The available literature also indicates that no activated 1 GBq of the radiotracer was used in each run. In first run, the radio-
sludge process of wastewater treatment plant in pulp and paper in- tracer (activity: 1 GBq in volume 5 ml) was diluted in about 2 l of
dustry has been investigated using radiotracer technique. The present wastewater and instantaneously injected at the inlet of the aeration
paper describes a radiotracer investigation for measurement and ana- tank as shown in Fig. 1. The radiotracer was monitored at the several
lysis of RTD of wastewater in an ASP of a wastewater treatment plant in locations along the aeration tank and the secondary clarifier using NaI
a pulp and paper industry with a primary objective to examine its hy- (TI) scintillation detectors D1, D2, D3, D4, D5 and D6 as shown in
draulic performance. Fig. 1. Whereas, in the second run, the radiotracer was injected at the
inlet of the secondary clarifier and monitored at the inlet and outlet of
2. Experimental the secondary clarifier. Since monitoring locations were quite far from
each other and therefore it was not possible to connect all the detectors
2.1. Activated sludge process to one common data acquisition system (DAS) due to the limited length
of the detector and DAS connecting cables. Thus, the detectors were
The schematic diagram of the ASP system is shown in Fig. 1. The connected to two independent DASs and set to record the radiotracer
system consists of an aeration tank connected in series with a secondary concentration with a sampling time of 5 min. Both the DASs were
clarifier. The aeration tank is 76 m long, 18 m wide, 4 m deep with a synchronized and started at the same time to acquire the data. The
capacity of 5472 m3. The effluent from a primary clarifier enters into background radiation levels were measured prior to conducting each
the aeration tank with a flow rate of 5.21 ± 1% m3/min. The aeration run.
tank contains a predefined population of active microorganisms. These
microbes consume the organic pollutants in the wastewater as a food 3. Data treatment and analysis
and convert them into biomass under aerobic conditions. Dissolved
oxygen (DO) concentration is maintained between 1.5 and 2.0 mg/l The measured radiotracer concentration data usually contains many
with the help of diffused aeration system fitted with fine bubble undesired influences and thus needs to be treated before drawing any
membranes connected to a centrifugal blower. Six mechanical surface useful information and modeling the data. The data treatment involved,
aerators are installed in the tank to homogenize and ensure adequate zero-shift, background correction, tail correction and normalization

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using an RTD analysis software (Thyn and Zitny, 1996; IAEA, 2008;
Kasban et al., 2010). Thus the normalized RTD curves at the outlets and
other locations in the aeration tank and secondary clarifier were ob-
tained using the following equation:
C(t)
E(t) = ∞
∫0 C(t)dt (1)

where C(t): concentration at time t and E(t): normalized RTD curve. For
a perfect impulse injection of radiotracer, the first moment (M1) of the
RTD curve will directly provide the experimental MHRT (τExp) of the
wastewater in the system. Thus:

τExp = M1 = ∫0 tE(t)dt (2) Fig. 2. Phenomenological model for the aeration tank.

The theoretical MHRT (τThe) of wastewater in a system without any


recycle is the ratio of the geometric volume (V) of the reactor to the
total volumetric flow rate (Q) fed into the system. But if a fraction R
(Qr/Q) of the inlet flow is recycled back to the inlet of the system, then
the τThe considered at the time of the design of the system under normal
operating conditions is given as (Battaglia et al., 1993):
V
τThe =
Q + Qr (3)

where Qr is the recycle flow rate of the wastewater. Under normal


operating conditions, the theoretical and experimentally measured Fig. 3. Phenomenological model for the secondary clarifier.
MHRTs should be equal to each other. In case, if the theoretical MHRT
is lesser than the experimental MHRT, this implies either that a fraction (Farooq et al., 2003; Leclerc et al., 1995) was used for simulation of the
of the radiotracer is held back in the system due to adsorption and is RTD data measured in the aeration tank and the secondary clarifier. The
released gradually or the values of flow rates and volume used for de- software offers the possibility for the users to build any physically re-
termination of τThe could be erroneous. The adsorption of radiotracer presentative model for the system under investigation and subsequently
within the system is ruled out if one uses a suitable radiotracer. So the use the same to simulate the experimentally measured data. The hy-
other source of error could be errors in the values of the flow rate and draulically representative phenomenological models proposed and used
volume and thus needs to be rechecked. In case, if the value of ex- for the simulations in the present investigation are shown in Figs. 2–4
perimentally determined MHRT is lesser than the theoretical MHRT, and the results of the simulation are shown in Figs. 5–9.
then there exists possibility of dead volume i.e. the volume which is not
utilized for the flow of wastewater in the system. The presence of the
dead volume decreases the hydraulic efficiency of the system. The ex- 4. Results and discussion
tent of dead volume in the system can be estimated by comparing the
experimental and theoretical MHRTs of the system (IAEA, 2008). Thus: Usually, the radiotracer experiments are carried out with steady
τExp ⎞ state flow conditions i.e. the feed flow rate is equal to exit flow rate.
% Vd = ⎛1 − ⎜ ×100 ⎟ However, in the present investigation, the activated sludge system did
⎝ τThe ⎠ (4)
not strictly operate at the steady state condition as it was not possible to
The values of dead volumes estimated within the aeration tank and maintain exactly the same feed rate during the RTD measurements due
the clarifier are given in Table 1. to the inherent requirement of the water in different production pro-
In order to obtain detailed information about flow structure of cesses in the paper industry. It was observed that the variation in the
wastewater within the aeration and secondary clarifier, the measured feed rate was not significant enough to cause any appreciable variation
RTD data was modeled using suitable and representative mathematical in the measured RTDs. In addition to this, the duration of the experi-
models. Initially many combinations of different models (tank-in-series, ment was long enough and volume of the system was large enough to
axial dispersion, tank-in-series with backmixing and tank-in-series with equalize the flow rate due to the variations.
dead volumes etc.) were used for simulating the measured RTD curves
(Levenspiel, 2001; Fogler, 2011). After repeated attempts eventually,
most hydraulically representative models were arrived at and used for
simulation. The RTD software DTSPRO-V4.21 developed by PROGEPI

Table 1
Mean hydraulic retention times and dead volumes.

Sr. No. System V (m3) Q(m3/ τThe (Min.) τExp (Min.) % Vd


Min.)

1 Aeration tank 5472 6.25 875.5 855 2.34


2 Secondary clarifier 944 6.25 151 145 4.00
3 ASP System 6655 5.21 1277 1175 8.00
(Aeration tank
+clarifier
+connecting
pipelines)
Fig. 4. Phenomenological model for the entire activated sludge processing system.

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M. Sarkar et al. Applied Radiation and Isotopes 130 (2017) 270–275

Fig. 5. Comparison of experimentally measured and model simulated RTDs at location D2 Fig. 8. Comparison of experimentally measured and model simulated RTD curves at the
within the aeration tank (run 1). outlet of the clarifier (run 2, D6).

Fig. 9. Comparison of experimentally measured and model simulated RTD curves at the
Fig. 6. Comparison of experimentally measured and model simulated RTDs at location D3
outlet of the ASP system (run 1, D6).
within the aeration tank (run 1).

simulation are shown in Fig. 5. The bypass stream in the model is re-
presented by a plug flow (PF) component. The model parameters i.e.
number of tanks (N), model predicted MHRT (τM), fraction of bypass
(fbp) and retention time in bypass stream (tbp) obtained after simulation
corresponding to the best fit are given in Fig. 5. The results of simu-
lation indicate that the section of the tank between D1 and D2 behaves
as an ideal continuously stirred tank reactor (CSTR) with a small frac-
tion (3%) of wastewater bypassing the main flow within a very short
time i.e. 3 min at location D2. The RTD curve measured at the second
axial location (D3) was simulated using a simple tank-in-series model
(TISM) and the results of model simulations are shown in Fig. 6. The
results indicate that the section of the aeration tank between D1 and D3
behaves as an ideal CSTR (N = 1).
The treated RTD curve measured at the outlet of the aeration tank
by the detector D5 is shown in Fig. 7. The curve shows no bypassing and
Fig. 7. Comparison of experimentally measured and model simulated RTD curves at the parallel flow paths within the tank. The initial part of the curve contains
outlet of the aeration tank (run 1, D5). three distinct peaks superimposed on the RTD curve. These peaks could
be due to lumped flow or recirculation currents produced by the me-
chanical aerators and will not cause any significant effect in the aera-
4.1. Aeration tank
tion process. Since only a small fraction (20%) of the radiotracer is
recycled back to the tank, there can not be any significant change in the
The run 1 was carried out to measure the RTD of the wastewater in
shape of the RTD curve due to the recycling stream. However, the re-
the aeration tank. The RTD curves were measured at three locations i.e.
cycling stream might cause extension in the tail of the curve. The ex-
at two axial locations within the tank (D2 and D3) and at the outlet of
perimental MHRT of the wastewater within the aeration tank was de-
the tank (D5). The RTD curves monitored within the tank provided
termined to be 855 min (Eq. (2)). Since the volume of the tank and total
information about local flow patterns, whereas the RTD curve measured
volumetric flow rate to the aeration tank during the experiment were
at the outlet provided information about the overall flow behavior of
known, the theoretical MHRT of the wastewater within the tank was
the wastewater within the aeration tank. The RTD curve measured at
estimated to be 875.5 min. Based on the comparison of the theoretical
first axial location (D2) within the tank was simulated using a tank-in-
and experimentally measured MHRTs the dead volume present within
series with bypassing model (TISBPM) and the results of the model
the tank was estimated to be about 2.34% (Table 1). The amount of

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dead volume in the tank is negligibly small and within the experimental (Levenspiel, 2001; Fogler, 2011). The hydraulically representative
error. This implies that all most of the geometric volume of the tank is phenomenological model is shown in Fig. 3. The model has three
utilized for flow and hence available for the aeration process. parameters i.e. retention time in axially-dispersed component (tad),
The radiotracer concentration curve monitored by the detector D4, Peclet number (Pe) and retention time in recycle stream (tr). The
mounted on the recycle pipeline close to the inlet of the tank, indicated parameter Pe defines the degree of axial mixing within a system and
that the radiotracer takes about 50 min to get recycled back to the tank tends to zero for maximum mixing and infinity for minimum mixing.
after injection. The recycled fraction of the radiotracer will mix within The comparison of the experimental and model simulated curves cor-
the tank and may contribute to the RTD curve measured at the outlet of responding to the best fit is shown in Fig. 8. The model parameter i.e.
the tank. Pe corresponding to the best fit was estimated to be 1.3, which in-
The impulse response i.e. RTD curve measured in run 1 at the outlet dicated a significant degree of back-mixing or non-symmetrical dis-
of the aeration tank (D5) was simulated using a hydraulically re- persion in the clarifier. This could be due to the combined effect of
presentative phenomenological model as shown in Fig. 2. The model recycling and exchange of radiotracer between the active and dead
consists of three components i.e. a plug flow (PF) component connected volume (sludge) at the bottom of the clarifier leading to an extended
in series with a tanks-in-series with backmixing (TISBM) and a PF tail in the measured RTD curve.
component in recycle stream. The PF component in the beginning of the
model represents a minor time-shift or time taken by radiotracer to 4.3. Activated sludge process system
appear at the outlet of the tank without any mixing, whereas the TISBM
component represents mixing within the aeration tank. The recycle In the preceding sections, the results of the RTD measurements in
stream is also represented by a PF component. The model has six the aeration tank and the secondary clarifier were discussed. This sec-
parameters i.e. overall retention time predicted by the model (τM), re- tion discusses the results of the RTD measured at the outlet of the entire
tention time in PF component in the beginning (t1), retention time in ASP system. The total geometric volume of the system includes the
TISBM component (tbm), number of tanks in TISBM component (N), volume of the aeration tank, secondary clarifier and associated pipe-
back-mixing ratio (α) and retention time in PF component in recycle lines and was calculated to be 6655 m3 from the available drawings of
stream (tr). The back-mixing ratio is defined as the ratio of the back- the system. Since the volumetric flow rate of the wastewater through
ward flow to the forward flow between the two tanks. The proposed the system during the investigation was 5.21 ± 1% m3/min, the theo-
model was used to simulate the RTD measured at the outlet of the tank retical MHRT of wastewater in the entire system was estimated to be
(D5) and the comparison of experimental and model simulated RTD 1277 min (Table 1). Based on the comparison of the theoretical and
curves corresponding to the best fit is shown in Fig. 7. The values of the experimentally determined MHRTs, the dead volume within the system
five model parameters i.e. t1, tbm, N, α and tr corresponding to the best was estimated to be about 8% (Table 1). The sum of the dead volumes
fit were found to be 10 min, 828 min, 2, 2 and 20 min, respectively. It is within the aeration tank and the secondary clarifier is found to be ap-
observed that the retention times of wastewater in the two PF compo- proximately same as the dead volume existing within the entire ASP
nents is negligibly small as compared to the TISBM component. The system.
MHRT predicted by the model is in good agreement with the experi- During the run 1, the radiotracer injected at the inlet of the aeration
mentally measured MHRT. The obtained value of N indicates that the tank and measured at the outlet of the clarifier using detector D6 as
aeration tank behaves equivalently to two ideal CSTRs with a low de- shown in Fig. 1. The measured curve provides RTD of the entire system
gree of backmixing (α = 2) between them. For intense back-mixing, the and was independently modeled. Based on the a priori knowledge of the
value of back-mixing ratio tends to be infinity. systems and results of the RTD modeling of the aeration tank and the
secondary clarifier, a hydraulically representative phenomenological
4.2. Secondary clarifier model to simulate the RTD of the ASP system was proposed and is
shown in Fig. 4. Fig. 9 shows a plot comparing the experimental and
During the run 1, the radiotracer concentration curve was also model simulated RTD curves corresponding to the optimum values of
monitored at the outlet of the secondary clarifier in addition to the the model parameters. The optimum values of the model parameters i.e.
outlet of the aeration tank. In principle, the two curves can be used for total MHRT predicted by model (τM), retention time in the PF compo-
characterizing the flow within the secondary clarifier, as the curve nent (tp), number of tanks in TISBM component (N), backmixing ratio
monitored at the outlet of the tank will serve as an input for the in the TISBM component (α), Peclet number (Pe) of the axially-dis-
clarifier. However, in the run 1, the curve monitored at the outlet of the persed component, retention time in axially-dispersed component (tad)
secondary clarifier was significantly dispersed and could lead to errors and retention time in the recycle stream (tr) are shown in Fig. 9. The
in the determination of MHRT and model parameters, if used. total MHRT predicted by the model was in agreement with the ex-
Therefore, an independent experiment was conducted (run 2) to mea- perimentally determined value. The values of the other model para-
sure the RTD of the secondary clarifier. In run 2, the radiotracer was meters corroborated with the values of model parameters obtained in
instantaneously injected at the inlet of the clarifier and monitored at its the individual simulations of the aeration tank and secondary clarifier.
outlet using detector D6 (Fig. 1). The treated RTD curve measured at This validates the results of the RTD analysis of the aeration tank and
the outlet of the clarifier is shown in Fig. 8. From the measured RTD secondary clarifier.
curve, the experimental MHRT (τExp) of wastewater in the clarifier was
determined and found to be 145 min. Since the volume of the secondary 5. Conclusions
clarifier and flow rate through it were known, the theoretical MHRT
was determined to be 151 min (Table 1). The comparison of experi- A radiotracer investigation was successfully conducted to study the
mental and theoretical MHRTs indicates that about 4.0% of the geo- hydraulic behavior of an ASP system in a pulp and paper industry in
metric volume of the secondary clarifier is stagnant. This is justified as India. The flow behavior of the individual sub-systems i.e. the aeration
the sludge (biomass) settles down at the bottom and reduces the active tank and the secondary clarifier as well as the entire ASP was in-
volume of the clarifier. vestigated. The investigation revealed that there were no major flow
For efficient operation of the process, the secondary clarifier is ex- abnormalities such as bypassing and parallel flow paths inside the
pected to behave as a perfect plug flow reactor (no backmixing). In aeration tank and the secondary clarifier. The dead volume inside the
order to evaluate whether the secondary clarifier behaves as a plug flow aeration tank was negligibly small. Therefore, the aeration tank oper-
reactor or not, the measured RTD was simulated using a hydraulically ates at its designed hydraulic efficiency. The modeling of the measured
representative model i.e. axial dispersion model (ADM) with recycle RTD of the wastewater in the aeration tank revealed that the hydraulic

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Acknowledgement
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