Journal of Cleaner Production 242 (2020) 118544

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Journal of Cleaner Production

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

Techno-economical evaluation of coupling ionizing radiation and

biological treatment process for the remediation of real
pharmaceutical wastewater
Rahil Changotra a, Himadri Rajput a, Jhimli Paul Guin b, **, Shaik Abdul Khader c,
Amit Dhir a, *
a
School of Energy and Environment, Thapar Institute of Engineering and Technology, Patiala, 147004, India
b
Radiation Technology Development Division, Bhabha Atomic Research Centre, Mumbai, 400085, India
c
Isotope & Radiation Application Division, Bhabha Atomic Research Centre, Mumbai, 400085, India

a r t i c l e i n f o a b s t r a c t

Article history: Pharmaceutical manufacturing industries produce a vast range of substances by using organic and
Received 6 February 2019 inorganic compounds as raw material thereby gives rise to huge volume of toxic and complex organic
Received in revised form liquid effluents comprised of high levels of dissolved solids. High and low strength wastewater streams
20 September 2019
originating from manufacturing unit often contains different types of contaminants, including organic
Accepted 21 September 2019
Available online 22 September 2019
compounds which can be difficult to treat with conventional methods of treatment. In this study, the
sequential treatment process of coagulation, electron beam (E-beam) irradiation and biological treat-
Handling EditorProf. S Alwi ment was employed on real pharmaceutical industrial wastewater to study the impact of combined
treatment on remediation and detoxification of the wastewater. Combined treatment was performed on
Keywords: low (LOSW) and high (HOSW) organic strength wastewater collected from representative pharmaceutical
Electron beam industry. Operational parameters like pH, absorbed dose and use of oxidants were systematically
Real pharmaceutical wastewater investigated to achieve the enhanced treatment of wastewater streams using E-beam irradiation. Bio-
Activated sludge process logical treatment was carried out using activated sludge process at laboratory-scale reactor by utilizing
Cytotoxicity
acclimatized consortia in the experiments. Sequential hybrid coagulation, E-beam irradiation and bio-
Cost evaluation
logical treatment lead to synergistic degradation and detoxification of both the recalcitrant wastewater
streams with overall chemical oxygen demand (COD) removal of 94% and 89% for LOSW and HOSW,
respectively. Cytotoxicity assessment revealed that the combined treatment of wastewater was effective
in eliminating the toxicity when tested against the selected microorganisms. The treatment cost of E-
beam radiolysis alone, biological treatment alone and E-beam þ biological treatment for LOSW was found
to be 0.50, 2.35 and 2.85 USD m3; whereas, for HOSW, it was found to be 0.67, 0.7 and 1.37 USD m3,
respectively. The overall cost of the set-up of an E-beam unit and the treatment cost for real pharma-
ceutical wastewater was evaluated to establish the applicability of the E-beam technology at industrial
scale. The feasibility of E-beam irradiation for wastewater remediation may ensure future smart cities
with sustainable resource management.
© 2019 Elsevier Ltd. All rights reserved.

1. Introduction increasing population and urbanization growth. The adverse effect

of wastewater discharges are generally related to human health,
The problems associated with the wastewater generation and its environmental, food quality and security, socio-economic and
disposal has become an impending problem to the world due to esthetic impacts from wastewater contaminations (WHO, 2003;
Hossain et al., 2018). In this context, wastewater generated from
pharmaceutical manufacturing activity has been classified as a “red
category” owing to the enormous volume, complexity, and haz-
* Corresponding author.
** Corresponding author. ardous waste it produces, which are generally characterized by high
E-mail addresses: paul.jhimli@gmail.com (J.P. Guin), amit.dhir@thapar.edu BOD, COD, solids, auxiliary chemicals, low BOD:COD ratio, and
(A. Dhir).

https://doi.org/10.1016/j.jclepro.2019.118544
0959-6526/© 2019 Elsevier Ltd. All rights reserved.
2 R. Changotra et al. / Journal of Cleaner Production 242 (2020) 118544
presence of various pharmaceuticals or their metabolites in active
or inactive form. Although considerable amount of studies have
been reported for the pharmaceutical wastewater treatment by
various physicochemical methods, but the research is still under-
way to find a realistic and potential approach to treat actual
wastewater generated during pharmaceutical manufacturing
(Ziylan and Ince, 2011; Gadipelly et al., 2014). In some cases,
chemical coagulation/flocculation, adsorption by activated carbon
and membrane filtration have been considered as possible alter-
native methods to enhance the quality of pharmaceutical waste-
water (Rivera-Utrilla et al., 2013). However, these methods have
been proved as less efficient towards the degradation of stable
pharmaceutical compounds and they only transfer the pollutants
from one phase to another phase instead of removing them. In
addition to this, conventional wastewater treatment plants
(WWTPs) are unable to remove the recalcitrant, non-biodegradable
and toxic pharmaceutical pollutants from wastewater streams as
they are designed to eliminate the biodegradable and easily
removable organic pollutants; thereby augmenting the overall
organic load of discharged wastewater (Zhou et al., 2009; Luo et al.,
2014). More effective treatment technology is required in order to
reduce the environmental impact and potential threats related to
pharmaceutical wastewater discharges. Radiation technology is
recognized as an environmental friendly technique under the
transfer of radiation processing applications when compared to
other chemical processes. In this regards, high energy E-beam ac-
celerators have been well developed in terms of larger capacity,
wider range applications, reliability and cost reduction. In the last
few decades, E-beam technology has substantially gained impor-
tance in the mitigation of various pollution problems (Woods and
Pikaev, 1994; Hossain et al., 2018). E-beam radiation based treat-
ment plants have been successfully installed in several countries for
sludge and wastewater treatment at pilot and commercial scale
(IAEA, 2008). Radiation technology is also regarded as a special
advanced oxidation process (AOP) which generates oxidative spe-
cies (HO) and reductive species, such as hydrated electrons (e aq Þ
and hydrogen atoms (H) (Spinks and Woods, 1990; Bhuiyan et al.,
2016). E-beam radiation with high ionization energy (4.5 MeV) is
not easily perturbed or scattered by insoluble solids, where UV
radiation with low energy can be attenuated (Cantwell and
Hofmann, 2011). It has been reported that enhancement in biode-
gradability has been achieved with the combined treatment of E-
beam and biological process for textile wastewater (He et al., 2016);
polyvinyl alcohol (Jo et al., 2006); azo dyes solution (Paul et al.,
2011) and wastewater from governmental WWT plant (Duarte
et al., 2000). Due to the wider range of E-beam applications, the
first full scale E-beam based treatment plant was installed in Daegu
(S. Korea) for treating 10,000 m3 day1 of textile wastewater and it
has showed that the irradiation based treatment process is a cost
effective technology when compared to the conventional treatment
methods (Capodaglio, 2017). Bumsoo et al. (2011) found the in-
crease in removal efficiency of textile industry wastewater using E-
beam radiolysis due to the transformation of poorly bio-degradable
or refractory compounds with an overall treatment cost, including
interest and depreciation of investment, to be 0.3 USD m3 of
treated wastewater. Sparse studies have demonstrated the effec-
tiveness of radiation technology, gamma or E-beam alone, or in
combination with oxidants and biological treatments to further
improve the removal efficiencies of wastewater (Kim et al., 2015;
Wang and Chu, 2016). But these studies showed different results
related to coupling approach for different wastewaters and, most of
the available studies are related to synthetic or model compound
wastewater rather than actual industrial wastewater. In order to
overcome the economical limitation and taking into account that
biological treatment is one of the most desirable remediation
technique in terms of environmental impact, a synergistic approach
of coupling E-beam and biological treatment might be an effective
treatment route. In this study, efforts have been made to combine
the information of physicochemical characteristics, biodegrad-
ability and toxicity analysis to study the feasibility of the combi-
nation of coagulation, E-beam and biological treatment on real
pharmaceutical industrial wastewater. The prime aim was to ach-
ieve the effective overall reduction in organic content of waste-
water in a sequential treatment process. For E-beam treatment,
effect of operating parameters like absorbed dose, pH and different
oxidants were examined to achieve the maximum removal effi-
ciency. For biological treatment, an attempt has been made to
evaluate microbial performance when fed with E-beam treated
wastewater of different organic load in a laboratory scale activated
sludge process. The mixed consortium of microorganisms was
acclimatized with the pharmaceutical waste initially and then the
treatability study was performed.
2. Experimental
2.1. Chemicals and reagents
Hydrogen peroxide 30% (w/v), potassium persulfate (98%) and
phosphoric acid (88%) were obtained from Merck. Sodium hy-
droxide (>99%), calcium hydroxide (95%), aluminium sulphate
(98%), ferric chloride (99%), sulphuric acid (95%), hydrochloric acid
(37%), ammonium sulphate (99%) and potassium phosphate (99%)
were obtained from SD Fine Chemicals Pvt. Ltd., India. The Muller
Hinton Agar (MHA) culture media was purchased from Himedia
Laboratories Pvt. Ltd., India. The microbial strains of Escherichia coli
(DH5-a strain), Pseudomonas aeruginosa (MTCC-647) and Bacillus
subtilis (MTCC-441) were arranged from the Department of
Biotechnology, Thapar Institute of Engineering and Technology,
Patiala (India). Milli-Q water was used to prepare the reagents used
in the present study. Tap water was used for preparing the dilutions
of real pharmaceutical wastewater.
2.2. Wastewater collection and its pre-treatment
The wastewater was collected from equalization tank of effluent
treatment plant (ETP) of pharmaceutical manufacturing industry
located in Derabassi, Punjab and all the physicochemical charac-
teristics of collected wastewater are summarized in Table 1. The low
(LOSW) and high (HOSW) organic strength wastewater samples were
collected by grab sampling of mixed wastewater taken at three
different locations from the respective equalization tanks of the ETP
(Fig. SM-1) of the industry. Due to the presence of high solids
content in wastewater, the LOSW and HOSW were given pre-
treatment using different types of chemical coagulants including
ferric chloride (FeCl3), calcium hydroxide (Ca(OH)2) and aluminium
sulphate (Al2(SO4)3 to obtain better results among these
coagulants.
2.3. Irradiation treatment
E-beam treatment to wastewater samples was given under
linear electron beam accelerator unit (ILU-6) supplied by Budker
Institute of Nuclear Physics, Russia and having beam energy of
4.5 MeV, 4 Hz pulse frequency and average beam current of 0.3 mA.
The experiments were carried out in a 25 mL glass petri-plate laden
having 15 mL volume of wastewater samples at a dose rate of
25 kGy min1. The wastewater samples were placed at an approx-
imate 40 cm distance beneath the irradiation window and then
subjected to dose ranging in between 25 and 100 kGy at room
temperature (30 ± 2  C). The effect of operational parameters such
 R. Changotra et al. / Journal of Cleaner Production 242 (2020) 118544 3

Table 1
Physicochemical characteristics of LOSW and HOSW before and after pre-coagulation treatment with FeCl3.

S.No. Parameters Raw LOSW Treatment of LOSW with 3 g L1 FeCl3 Raw HOSW Treatment of HOSW with 4 g L1 FeCl3

Mean ± S.D. Mean ± S.D. Mean ± S.D. Mean ± S.D.

1 pH 7.76 ± 0.35 12.6 ± 0.26 7.12 ± 0.35 12.8 ± 0.35

2 Color Light brown Light brown Dark brown Dark brown
3 BOD5 6,180 ± 170 5,285 ± 190 25,650 ± 245 23,980 ± 220
4 COD 11,940 ± 215 8,345 ± 230 52,856 ± 365 37,460 ± 325
5 BOD5/COD 0.51 ± 0.04 0.63 ± 0.05 0.48 ± 0.06 0.64 ± 0.06
6 TOC 2,898 ± 85 2,270 ± 140 12,440 ± 146 8,160 ± 158
7 TSS 7,130 ± 165 3,980 ± 120 10,560 ± 278 6,570 ± 180
8 TDS 18,430 ± 255 14,460 ± 175 39,890 ± 580 20,750 ± 560
9 TKN 965 ± 120 612 ± 96 3,450 ± 140 2,980 ± 134
10 Nitrate 17 ± 1.25 11 ± 0.95 23 ± 1.10 20 ± 1.78
11 Nitrite 27 ± 1.50 15 ± 1.55 69 ± 3.2 43 ± 1.45
12 Sulfates 3,898 ± 110 2,121 ± 165 10,254 ± 275 3,860 ± 280
13 Chloride 2,345 ± 115 1,525 ± 85 9,020 ± 260 6,020 ± 128
14 Phosphate <0.005 <0.005 1.9 ± 0.32 0.2 ± 0.03

Note: All the values are expressed in mg L1 except pH, color and BOD5/COD. All the values are provided as the mean of three values.

as pH of wastewater, absorbed dose and addition of oxidants like
potassium persulfate (K2S2O8) and hydrogen peroxide (H2O2) were
examined to analyze their contribution towards the removal of
organic matter present in wastewater samples. All the irradiation
experiments were performed in a shielded remote chamber under
a non-contact mode. All the LOSW and HOSW samples were irradi-
ated parallel by placing the petri-plates in stainless steel tray. After
the attainment of a particular absorbed dose, glass petri-plates
were removed from the tray and irradiated samples were syringe
filtered (0.22 mm) for COD, TOC and toxicity analysis. The samples
after irradiation treatment were stored at 4  C temperature till their
further analysis. Under the obtained optimized conditions of E-
beam treatment of LOSW and HOSW, 20 L of each wastewater samples
were placed in a stainless steel tray of dimensions 80 60 2 cm
and was irradiated with given dose. The irradiated samples of LOSW
and HOSW were then given biological treatment using activated
sludge process.
2.4. Activated sludge process reactor
Aerobic degradation of irradiation treated wastewater was
performed in laboratory scale stainless steel fabricated activated
sludge process (ASP) unit as shown in Fig. 1. The reactor consists of
aeration tank with 9 L capacity and settling chamber of 2 L capacity.
The sludge recirculation provision was made to maintain the mixed
liquor suspended solids (MLSS) in the reactor. In the aeration tank,
mixed liquor was provided with submerged aeration using air
spargers. A storage tank of 3 L capacity was provided for the
collection of treated wastewater from the settling chamber’s
overflow drainage assembly. The potential for ASP treatment of
wastewater samples was evaluated by feeding diluted/raw waste-
water samples of LOSW and HOSW, which were pre-treated by E-
beam irradiation. At regular intervals, aliquot of samples were
withdrawn and subsequently centrifuged at 14,000 rpm for a time
span of 10 min to separate the sludge. The separated supernatant
was syringe filtered (0.22 mm) and characterized for COD, TOC and
toxicity analysis.
The reactor was inoculated by the activated sludge obtained
from the aeration tank of ETP of industry from where wastewater
was collected. The sludge was transferred to the reactor and was
retained in it, allowing the build-up of MLSS concentration. Before
startup of the reactor, gradual introduction was applied for the
acclimatization of activated sludge to the pharmaceutical waste-
water. The initial 500 mg L1 COD load wastewater was taken for
the acclimatization of sludge in a continuous reactor. The accli-
matization of sludge was done for 25 days. The reactor was
continuously fed with air to maintain 2.0e3.0 mg L1 dissolved
oxygen (DO) concentration. The pH and nutrients amount were
maintained in the range of 7.0e8.0 and COD:N:P ratio at 100:5:1,
respectively (Metcalf and Eddy, 1995). The experiments were

Fig. 1. Schematic diagram of experimental setup for activated sludge treatment of wastewater. P1: Peristaltic pump for sludge recirculation; P2: Peristaltic pump for influent of
wastewater.
4 R. Changotra et al. / Journal of Cleaner Production 242 (2020) 118544
carried out by gradually increasing the COD at 500 mg L1 rate for
every 5 days till the COD value reaches 2,000 mg L1. The reactor
was monitored on daily basis for the outlet COD and MLSS con-
centration to understand the activity of reactor. The rate of sub-
strate utilization during the acclimatization period was analyzed in
the terms of COD uptake. The ratio of COD uptake increased from 1
to 20 days of reactor operation at a rate of 100 ± 25 mg day1. The
COD uptake of reactor reached 2,000 mg day1 on 20th day and
observed to be constant thereafter. The variation in MLSS concen-
tration during the reactor operation was also assessed. The initial
MLSS concentration was 1,000 mg L1 and till 20th day it gradually
reaches the value 3,000 mg L1. When the MLSS concentration
maintained a constant value of 3,500 ± 120 mg L1, the biomass
was considered to be acclimatized. On complete acclimatization of
wastewater to sludge, the reactor was fed with wastewater with an
initial COD load of 1,000 mg L1 and 4,000 mg L1 for LOSW and
HOSW, respectively, in separate experiments.
2.5. Analytical techniques
The COD analysis of wastewater samples was performed using
Merck® Spectroquant kits and closed reflux colorimetric method
(APHA, 1998). COD removal (%) was calculated by using the
following equation (Eq. (1)):
DCOD
COD removal ð%Þ ¼  100
CODi
Where DCOD ¼ CODf  CODi ; CODf and CODi is the final and initial
COD of wastewater sample, respectively.
All the samples containing H2O2 were boiled for 10 min to
remove its interference prior to COD analysis. The 5-days biological
oxygen demand (BOD5) was measured using OxiTop® Single
Measuring System (WTW Weilheim, Germany). The chemical
analysis of other parameters including pH, total dissolved solids
(TDS), total suspended solids (TSS), mixed liquor volatile suspended
solids (MLVSS), mixed liquor suspended solids (MLSS), total Kjel-
dahl nitrogen (TKN) and concentrations of chlorides, sulphates,
phosphates, nitrates and nitrites was performed using standard
methods (APHA, 1998a). pH and absorbance of wastewater samples
was analyzed using Cyber Scan PCD 650 multiparameter analyzer
and UVeVis spectrophotometer (Shimadzu, UV-2450, Japan),
respectively. The total organic carbon (TOC) concentration was
evaluated by multi N/C 2100 TOC analyzer (Analytikjena, Germany)
with 50 mL of injected volume. Cytotoxicity potential of wastewater
samples before and after the irradiation treatment was determined
through disk diffusion method (commonly known as Kirby-Bauer
test) against clinical isolates of three microbial species: E. coli,
P. aeruginosa and B. subtilis by following the procedure reported in
the previous study (Changotra et al., 2019).
3. Results and discussion
3.1. Chemical coagulant treatment of wastewater and its
characterization
The wastewater characteristics of raw LOSW and HOSW presented
in Table 1 indicates that the generated wastewater samples from
the pharmaceutical manufacturing unit contains high organic load
as represented by high BOD5, COD values, suspended solids, dis-
solved solids, total Kjeldahl nitrogen (TKN), chlorides and sulfates.
Due to the high load of organic matter, pre-coagulation treatment
was given to wastewater with various chemical coagulants
including Ca(OH)2, FeCl3 and Al2(SO4)3 to separate some extent of
organic content in the form of sludge. All the coagulants were
added to 100 mL of LOSW and HOSW with their respective concen-
tration and were allowed to mix for 2e3 h followed by the
adjustment of pH to 8.0. After sludge formation, samples were
allowed to settle down for 60 min and supernatant was filtered for
COD analysis. During pre-treatment analysis, the concentration of
coagulant was optimized to be 3 g L1 and 4 g L1 for LOSW and
HOSW, respectively (Changotra et al., 2019). The physicochemical
analysis revealed that among the used coagulants, FeCl3 produced
better results for both LOSW and HOSW of representative pharma-
ceutical industry. Table 1 shows the results of physicochemical
characteristics of LOSW and HOSW obtained with the addition of FeCl3
as a coagulant. The result indicated that 30% of COD removal was
achieved for LOSW with 3 g L1 of FeCl3 at pH 8.0 after 180 min of
contact time, whereas 25% of COD removal was obtained for HOSW
at pH 8.0 after 120 min contact time and 4 g L1 of coagulant dose.
The pre-coagulant treated wastewater samples were subjected to
independent E-beam irradiation treatment followed by biological
treatment.
3.2. Irradiation treatment
The pre-coagulant treated wastewater samples of LOSW and
HOSW were subjected to independent E-beam irradiation treatment
under two stages. Firstly, the wastewater samples were treated in
25 mL glass petri-plates to optimize the parametric conditions like
pH, absorbed dose and type of oxidant in terms of COD and TOC
(1)
removal. Secondly, the optimized conditions were utilized to treat
wastewater samples with 20 L of volume in stainless steel tray
under E-beam irradiation.
The E-beam radiolysis of LOSW and HOSW was carried out at
different absorbed doses ranging from 25 to 100 kGy. Fig. 2(a) and
(b) demonstrate the effect of solution pH on the COD removal of
LOSW and HOSW under E-beam radiolysis, respectively. Results
showed that acidic pH of reaction solution was slightly favorable for
effective COD removal of LOSW and HOSW when compared to neutral
and alkaline pH. 52.3, 46.3 and 43.8% COD removal of LOSW was
achieved at pH 3, 7 and 11, respectively, whereas 48.1, 43.3 and
44.3% COD removal were achieved for HOSW at pH 3, 7 and 11,
respectively at an absorbed dose of 100 kGy. It is well understood
that E-beam radiolysis of water produces three primary reactive
species viz. HO radicals, hydrated electrons ðe aq Þ and hydrogen
atom (H) in the pH range 3e11 (Spinks and Woods, 1990). The
overall radical concentration increased with increase in absorbed
dose, though the higher dose rate of E-beam would rapidly deplete
oxygen in the solution. Therefore, in acidic condition, e aq pre-
dominantly reacts with Hþ through parallel reactions with the
organic molecules present in the wastewater to generate H. Thus,
 
it inhibits the recombination of e
aq and HO to form OH , providing
opportunity to HO to react with organic content of wastewaters
(Guo et al., 2012). On the other hand, HO transforms to O- with
increase in pH (pka (HO) ¼ 11.9) and therefore COD removal
decreased with increase in pH. The increased COD removal in acidic
solution and decreased COD removal in neutral and/or alkaline
solution indicates the importance of HO radicals for effective COD
removal during E-beam radiolysis of wastewater. The concentration
of radicals generated during radiolysis of water is fixed at a
particular dose. These radicals react with the pollutants present in
the wastewater through a diffusion controlled process. However,
the probability of reaction between the radicals and pollutants
increases in HOSW due to the presence of high concentration of
pollutant molecules and thus DCOD removal values increased
(Fig. 2b). On the other hand, high initial COD value in the denom-
inator of Eq. (1) results in decrease in COD removal (%) for HOSW.
Hence, both LOSW and HOSW exhibited almost similar COD removal.
The results also revealed that COD reduction was not much
 R. Changotra et al. / Journal of Cleaner Production 242 (2020) 118544
Fig. 2. Effect of solution pH on the COD removal of (a) LOSW and (b) HOSW under E-beam irradiation treatment.
significant even with high absorbed dose of 100 kGy which might
be due to the presence of dissolved solids in the wastewater sam-
ples at higher concentrations. The presence of dissolved solids is
the measure of salinity due to salts like carbonates and bi-
carbonates, sulphates, chlorides, phosphates and nitrates of po-
tassium, calcium, magnesium, manganese and iron which
contributes to high level of TDS. At high TDS levels, the degradation
efficiency by irradiation treatment or other AOPs (generating HO
radicals) is expected to decrease as HO radicals are scavenged by
these salts present in wastewater (Buxton et al., 1988). To investi-
gate the effect of different types of oxidants on E-beam radiolysis of
wastewater, H2O2 and K2S2O8 were added to LOSW and HOSW at
different concentrations to study their influence on COD and TOC
removal efficiency. The H2O2 concentration was varied in between
0.01 and 0.5 mol L1, while K2S2O8 concentration was varied in the
range of 0.01e0.15 mol L1 for LOSW. For HOSW, H2O2 concentration
was varied from 0.025 to 0.75 mol L1, while K2S2O8 concentration
was varied from 0.05 to 0.2 mol L1. The effect of different con-
centration of oxidants on COD and TOC removal efficiency of LOSW
and HOSW is shown in Fig. SM-2 (supplementary information).
Fig. 3(a) and (b) show the optimized results of oxidant on COD and
TOC removal efficiency on LOSW and HOSW, respectively. Results
revealed that addition of 0.05 mol L1 H2O2 and K2S2O8 in LOSW led
to 62.6 and 60.4% of COD removal (Fig. 3a), respectively, whereas
66.9 and 61.5% of COD removal of HOSW was achieved with addition
of 0.5 mol L1 H2O2 and 0.1 mol L1 K2S2O8, respectively (Fig. 3b).
H2O2 is considered as a HO promoter, and consequently it was
expected that its addition to wastewater could augment the
degradation of organic pollutants (Changotra et al., 2018). The ef-
ficacy of E-beam radiolysis to treat wastewater is not only
Fig. 3. Effect of oxidants on COD and TOC removal of (a) LOSW and (b) HOSW under E-beam irradiation treatment.
5
determined by the COD removal, but also by the mineralization
extent of recalcitrant organic compounds present in wastewater
and the generated intermediates/by-products. The mineralization
extent of irradiated wastewater samples was assessed to analyze
the influence of different concentrations of H2O2 on the TOC
removal (Fig. SM-2, supplementary information). Results indicated
that addition of 0.01 mol L1 H2O2 led to 43.1% of TOC removal
which enhanced to 55.8% with initial H2O2 concentration of
0.5 mol L1 in the case of LOSW, whereas TOC removal efficiency
enhanced from 37.1 to 55.0% with the increased H2O2 concentration
from 0.025 to 0.75 mol L1 in case of HOSW. The enhanced TOC
removal of LOSW and HOSW with increasing H2O2 concentration

might be due to the fact that H2O2 readily reacts with e aq and H
during E-beam radiolysis, and increases the concentration of HO
radical in the aqueous solution which mineralizes the organic
compounds and generates by-products during radiolysis process.
However, the presence of excess H2O2 may produce peroxyl radical
ðHO:2 Þ species which are less reactive in comparison to HO radical
species (Buxton et al., 1988). Fig. 3(a) and (b) depict that 0.5 and
0.75 mol L1 H2O2 leads to 55.8 and 55.0% TOC removal of pre-
coagulant treated LOSW and HOSW, respectively under E-beam
radiolysis. The remaining TOC in the wastewater samples is prob-
ably due to the remaining recalcitrant organic compounds or
radiolytically generated by-products during E-beam radiolysis of
wastewater (Changotra et al., 2019).
Irradiation treatment of pre-coagulant treated wastewater
samples was also performed in the presence of K2S2O8 as an
oxidant. During E-beam radiolysis of wastewater in the presence of
K2S2O8, sulphate radical anion SO: 
4 are produced on reaction of eaq
and H with S2 O2
8 ions according to reactions (2) and (3) (Boukari
6 R. Changotra et al. / Journal of Cleaner Production 242 (2020) 118544
et al., 2011; Paul et al., 2014).
 
 : 1 1
S2 O2 2 10
8 þ eaq / SO4 þ SO4 ::: k ¼ 1:2  10 Lmol s
 
: :  1 1
S2 O2 7
8 þ H / SO4 þ HSO4 :::: k ¼ 2:5  10 L mol s
Like HO, SO:4 is an oxidizing species with redox potential of
2.43 V and is reactive towards many organic as well as inorganic
compounds. Thus, degradation of organic compounds is expected
to enhanced due to the presence of both SO: 
4 and HO radicals. In
2
present study, addition of S2 O8 ions did not exhibit any significant
reduction in COD and TOC of wastewaters when compared to H2O2
addition. It is well established that both SO: 
4 and HO are partially

scavenged by the reactions with Cl ions present in the real
wastewater in addition to the parallel reactions with the organic
pollutants present in the wastewater (Lian et al., 2017). Reactions of
both HO and SO: 
4 radicals with Cl ions result into the generation
of Cl atom intermediate specie which again can dissociate back to
HO and subsequently to Cl: 2 radical anion by protonation reaction
as shown by Eqs. (4)-8) (Liao et al., 2001). It can be hypothesized
:
that more selective nature of SO: 4 and Cl2 radical anion than non-

selective HO radical lead to lesser degradation of the pollutants
resulting into lower COD and TOC removal efficiency of the solu-
tions in presence of K2S2O8 than H2O2 (Lian et al., 2017).
 
SO:  2 : 8 1 1
4 þ Cl /SO4 þ Cl k ¼ 3:1  10 Lmol s
 
HO: þ Cl /HO þ ClOH : k ¼ 4:3  109 Lmol1 s1
 
ClOH: / HO: þ Cl k ¼ 6:1  109 Lmol1 s1
 
ClOH: þ Hþ /Cl: þ H2 O k ¼ 2:1  1010 Lmol1 s1
Cl: þ Cl  /Cl:
2 (8)
It can be considered that E-beam radiation technology has a
potential to treat real industrial wastewater with high organic load
and the simultaneous integration of E-beam with biological treat-
ment could further eliminate the organic matter, thereby achieving
the complete removal of organic matter from wastewater. Overall,
results of oxidant presence in E-beam radiolysis of pharmaceutical
wastewater achieved enhanced removal efficiency of COD with the
addition of H2O2 when compared to K2S2O8. Under the optimized
conditions, 20 L of each LOSW and HOSW sample were irradiated in
stainless steel tray with the addition of 0.05 and 0.5 mol L1 H2O2,
respectively, in separate experiments. The final COD values of LOSW
and HOSW samples with an absorbed dose of 100 kGy were
observed to be 3,175 ± 120 mg L1 and 12,570 ± 205 mg L1,
respectively. The samples after irradiation treatment were stored in
refrigerator at 4  C temperature till the post-biological treatment
using activated sludge process was employed.
3.3. Biological treatment
Irradiated and un-irradiated samples of LOSW and HOSW were
subjected to aerobic biological degradation in laboratory scale
reactor using acclimatized sludge obtained from the aeration tank
of ETP of pharmaceutical manufacturing unit (Derabassi, India). The
pH of wastewater samples was adjusted between 7.0 and 8.0 ± 0.2
using H2SO4 and NaOH solutions. Due to the deficiency of nutrients
in irradiated wastewater samples, nitrogen and phosphorous were
added to the wastewaters to maintain the COD:N:P ratio to be
100:5:1 depending upon on the feed wastewater COD. The nutri-
(2) ents are required to support the growth of microbial population
and securing that removal of organic load would be only limited by
carbon content of wastewater. According to Symons et al. (1960),
(3) the biodegradability index (BOD5/COD ratio) should be > 0.6 for
wastewater to be amenable for biological degradation, while 0.4 is
believed to be minimum value for biological degradation to be
effective. It is important to mention that the BOD5/COD values of
the LOSW and HOSW after coagulation were determined to be 0.63
and 0.64, respectively as discussed in section 3.1. However, upon
irradiation of the pharmaceutical wastewater at an absorbed dose
of 100 kGy, BOD5/COD values were found to increase to 0.77 and
0.74 for LOSW and HOSW, respectively. Thus it can be inferred that
radiation pre-treatment of the pharmaceutical wastewater helped
in decreasing the concentration of the organic load of the water
significantly as evidenced from the decrease in COD values and also
helped to increase the biodegradability of the pharmaceutical
wastewater (Paul et al., 2013; Shah, 2017). The potential of bio-
logical treatment of LOSW and HOSW was examined by feeding the
diluted or raw pharmaceutical wastewater to ASP reactor that has
been previously fed and acclimatized to wastewater. Wastewater
samples were continuously fed into the ASP reactor with a feed rate
ðQfeed Þ of 0.15 L h1 using peristaltic pump (Cole Parmer, Masterflex
L/S® Model-7720062 and L/S 14 tubing). The wastewater hydraulic
retention time (HRT) in the reactor was 2 days. The operation and
(4) performance of the ASP reactor was monitored in continuous mode
by keeping constant Qfeed and HRT for both LOSW and HOSW indi-
vidually, and variable feed COD. Biological treatment of un-
(5) irradiated wastewater was studied, in sequel, using pre-coagulant
treated LOSW dilutions with feed COD of 4,000 and 8,200 mg L1;
whereas for HOSW, feed COD was maintained to 12,000, 24,000 and
(6)
36,000 mg L1. For the varying organic load, the COD and TOC
removal efficiency was determined for LOSW and HOSW, and the
(7) results are represented in Fig. 4. The removal efficiency of COD was
found to be 60.1 and 55.1% for initial feed COD of 4,000 and
8,200 mg L1, respectively, whereas TOC removal efficiency was
41.4 and 46.1%, respectively for a given feed COD. On the other
hand, the removal efficiency of COD was found to be 42.5, 30.2 and
24.3% for initial feed COD of 12,000, 24,000 and 36,000 mg L1,
respectively, whereas TOC removal efficiency was 41.3, 25.4 and
28.5%, respectively for a given feed COD. These results indicated
that pre-coagulant treatment of samples have ability to remove
organic substance present in the wastewater to some extent by
making wastewater sample susceptible for subsequent microbial
degradation, thereby leading to enhanced COD and TOC removal
efficiency. The COD removal decreased with the increased feed COD
to the reactor. The higher organic load with increasing feed COD
poses inhibitory effect on the treatment efficiency (Fewson, 1988).
It was observed that the MLSS concentration increased with in-
crease in feed COD and obtained saturation (Fig. 6). Higher MLSS
concentration provides insufficient supplementation of dissolved
oxygen as well as its inefficient dissolution to the solution. This
ultimately results into the incomplete mineralization of the pol-
lutants and hence COD removal efficiency of the wastewater
decreased (Changotra et al., 2019). The results showed in Fig. 4
indicated that final COD values of raw LOSW and HOSW were
reduced to 3,680 ± 120 mg L1 (Figs. 4a), 27 and 240 ± 235 mg L1
(Fig. 4b) from initial COD values of 8,200 ± 175 mg L1 and
36,000 ± 215 mg L1, respectively due to sequential treatment of
coagulation and biodegradation of the waste water.
Biological treatment of E-beam treated wastewater was studied,
in sequel, using irradiated LOSW dilutions with feed COD of 1,000,
2,000 and 3,000 mg L1; whereas for HOSW, feed COD was main-
tained to 4,000, 8,000 and 12,000 mg L1. During the operations,
 R. Changotra et al. / Journal of Cleaner Production 242 (2020) 118544
Fig. 4. Profile of COD and TOC concentration at the effluent of ASP reactor operating under continuous mode at constant Qfeed of 0.15 L h1 for pre-coagulant treated (a) LOSW and (b)
HOSW.
parameters like pH, COD, TOC, MLVSS, MLSS and SVI of mixed liquor
were monitored regularly. For the organic load varying from 1,000
to 3,000 mg L1, the pH, COD and TOC removal efficiency was
determined for LOSW and the results are represented in Fig. 5. The
removal efficiency of COD was found to be 88.2, 87.2 and 78.9% for
initial feed COD of 1,000, 2,000 and 3,000 mg L1, respectively,
whereas TOC removal efficiency was 52.8, 62.4 and 66.8%, respec-
tively for a given feed COD. These results indicated that pre-
treatment of samples by E-beam irradiation have ability to
convert recalcitrant non-biodegradable organic substance present
in the wastewater to easily removable biodegradable substances
which are removed by subsequent microbial degradation, thereby
leading to enhanced COD and TOC removal efficiency. However, the
COD reduction for feed COD of 3,000 mg L1 was observed to be
lesser when compared to feed COD of 2,000 mg L1, which might be
due to the inhibitory effect of the higher concentration of organic
pollutant with increasing organic load (Suman Raj and Anjaneyulu,
2005). The significant reduction of COD and TOC for LOSW was
supported by considerable production of MLSS and MLVSS. The
values of MLSS and SVI were monitored on daily basis to under-
stand the ongoing biochemical activity and variation of feed COD
concentration and results are shown in Fig. 6(a). As a result, con-
centration of MLSS increased from 3,500 to 3,932 mg L1 till 9th
day of biological treatment, whereas about 87.2% of COD reduction
was achieved for initial feed COD of 2,000 mg L1. On 9th day, with
the addition of high concentration of feed COD (3,000 mg L1),
MLSS concentration decreased and became consistent
to z 3,900 mg L1. The gradual increase in MLSS concentration and
Fig. 5. (a) Profile of pH and COD concentration at the effluent of ASP reactor (b) TOC profile at the effluent of ASP reactor operating under continuous mode at constant Qfeed of
0.15 L h1 and feed COD (I) 1,000 (II) 2,000 and (III) 3,000 mg L1 for LOSW.
7
insignificant decline at a specified HRT can be due to the auto
oxidation of the microbial population and food to mass ratio dy-
namics (Sastry and Thambirajah, 1995; Raj et al., 2004).
For HOSW, the organic load was varied from 4,000 to
12,000 mg L1 and results of the pH, COD and TOC removal effi-
ciency are depicted in Fig. 7. The removal efficiency of COD was
found to be 72.1, 60.1 and 52.3% for initial feed COD of 4,000, 8,000
and 12,000 mg L1, respectively, whereas TOC removal efficiency
was 60.1, 65.6 and 65.3%, respectively for a given feed COD. Fig. 6b
shows that maximum MLSS concentration was observed to be
4,110 mg L1 on 10th day and after that declining trend in con-
centration of MLSS was observed. From these observations, it can
be considered that the reduction in MLSS concentration can be
ascribed to the production of secondary metabolites and interme-
diate products during the aerobic biological degradation of phar-
maceutical wastewater (McCabe and Eckenfelder, 1958).
It was observed that for aerobic degradation of LOSW and HOSW,
the pH of effluent initially increased and then remained consistent
between 7.0 and 8.0 indicating that the active biomass was able to
cope effectively with the imposed change of the feed composition
along with the effective COD removal during this transient period.
It is believed that rate of organic matter consumption in the aerobic
biotransformation increases with the increase in concentration of
microbial population in the aeration chamber. The rise in MLVSS
concentration indicated the active phase of aerobic biotransfor-
mation (Metcalf and Eddy, 1995). In this study, the maximum
MLVSS of 3,895 mg L1 and 3,345 mg L1 were observed for reactor
operation for LOSW and HOSW, respectively. SVI is indicator of the
8 R. Changotra et al. / Journal of Cleaner Production 242 (2020) 118544
Fig. 6. Variation of MLSS and SVI during continuous mode operation of ASP reactor at constant Qfeed of 0.15 L h1 and varied COD concentration for (a) LOSW and (b) HOSW.
Fig. 7. (a) Profile of pH and COD concentration at the effluent of ASP reactor (b) TOC profile at the effluent of ASP reactor operating under continuous mode at constant Qfeed of
0.15 L h1 and feed COD (I) 4,000 (II) 8,000 and (III) 12,000 mg L1 for HOSW.
settling characteristics of activated sludge and also specifies the
extent of aerobic biotransformation (McLachlan, 1986). In the case
of aerobic treatment of LOSW, SVI ranged from 68 to 82, whereas it
ranged between 80 and 110 in case of HOSW, indicating that the
sludge was of good quality. These results show that SVI increased
with high concentration of feed COD which indicates that settling
characteristics of sludge reduced due to the inhibitory effect of high
strength pharmaceutical wastewater (Arcivala and Asolekar, 2007).
Thus, inhibition of aerobic biotransformation at higher feed COD is
attributed to the decline in the activity of the microbial populations
in the oxidative treatment of real pharmaceutical wastewater.
Microscopical inspection of the used sludge indicated the presence
of a vast variety of bacterial populations which are either freely
dispersed in aqueous phase or aggregated in sludge flocs.
The overall results indicated that sequential treatment of LOSW
with pre-coagulant treatment followed by E-beam treatment and
subsequent biological treatment led to final COD value of
710 ± 105 mg L1 from the initial COD value of 11,940 ± 215 mg L1.
In case of HOSW, final COD value of 5,721 ± 170 mg L1 was achieved
when the initial COD value was 52,856 ± 365 mg L1. Based on the
obtained outcomes, the aerobic biological treatment of pharma-
ceutical wastewater of variable organic load after the pre-coagulant
and irradiation-based treatment, more specifically E-beam treat-
ment could be a gateway in integrated wastewater management
scheme at industrial or commercial scale. In the present study,
wastewater was collected from a single pharmaceutical
manufacturing unit, thus a comprehensive study of integrated
system by taking mixed wastewater from cluster of manufacturing
industries could be helpful in attaining the actual representation of
existing wastewater treatment problems and signifies the practical
viability of combined E-beam irradiation and biological treatment
for a common effluent treatment plant.
3.4. Toxicity analysis
The efficiency of employed treatment does not only depend on
the degradation efficiency of complex organic compounds present
in the wastewater, but also on the generated intermediates or
products which are lesser or non-toxic. The cytotoxicity of un-
irradiated and irradiated wastewater samples were tested against
the clinical isolates of E. coli, P. aeruginosa and B. subtilis using zone
of inhibition test. E. coli is a low-cost, fast growing and major
constituent of humans and animals intestinal micro-biota (Nataro
and Kaper, 1998). It is an extensively utilized microbial popula-
tion platform due to wider range of accessible genetic tools
(Planson et al., 2012). P. aeruginosa is a wide group of Gram-
negative free-living bacteria that are readily found in the various
water bodies including lakes, rivers and sea. It has the ability to
persist in distilled water (Warburton et al., 1992). B. subtilis is
frequently reported microorganism in the upper layers of soil
(Wolff et al., 2007). Toxicity assessment was conducted for the
treated LOSW and HOSW through H2O2-mediated E-beam irradiation
(100 kGy of absorbed dose) followed by post-biological treatment
and the results obtained are depicted in the Fig. 8. Results showed
that in almost all the petri-dishes, strong zone of inhibition was
observed for raw LOSW and HOSW, indicating the presence of toxic
organic pollutants in the wastewater. However, with E-beam irra-
diation treatment of wastewater followed by biological, inhibition
zone almost disappeared for LOSW, and small zone was observed for
E-beam irradiated HOSW indicating the presence of some toxic
 R. Changotra et al. / Journal of Cleaner Production 242 (2020) 118544
Fig. 8. Cytotoxic potential of (a: E. coli, b: B. subtilis and c: P. aeruginosa) LOSW and (d: E. coli, e: B. subtilis and f: P. aeruginosa) HOSW treated with H2O2-mediated E-beam irradiation
followed by post-biological treatment.
compounds or secondary products after irradiation treatment of
HOSW. These results showed that when E-beam irradiation was used
as pre-treatment technology to treat wastewater with different
organic loads, almost complete detoxification of wastewater was
achieved indicating that E-beam irradiation has a potential to
eliminate cytotoxicity from real wastewater. Since the toxic nature
was only tested against the clinical isolates of selected microbes, a
comprehensive study dealing with toxicity analyses of actual
wastewater using different bioassays test methods could exhibit
more reliable and viable results.
3.5. Cost analysis and environmental implications
Most of the reported studies associated with AOPs deals with
the degradation of organic compound without considering the cost
of the treatment and in case of real wastewater treatment, litera-
ture lacks the knowledge on overall cost associated with the
treatment of real pharmaceutical wastewater using single stage
oxidation or combined treatment technology. In actual, there are
number of expenses associated with the complete treatment pro-
cess that must be taken into account while deciding the economic
viability of process. Real costs of the process must include the
reactor, reagents, chemicals, electricity consumption and operating
costs. The overall cost associated with the E-beam treatment of
LOSW and HOSW wastewater is illustrated in Table 2 and Table 3.
Table 4 represents the total operating cost of E-beam þ ASP treat-
ment of LOSW and HOSW wastewater. In this study, efforts were made
to evaluate the overall cost of treatment at field-scale and the
9
results are represented in Table 5.
The efficiencies of E-beam radiolysis alone and E-beam þ H2O2
radiolysis were determined in the terms of cost of electrical energy
consumed and other auxiliary inputs. The cost involved due to
electrical energy employed in the E-beam radiolysis of wastewater
samples was calculated using Eq. (9) and the results obtained are
explained in Tables 2 and 3
EEC ¼ P  ðt=60Þ  ð1; 000=vÞ (9)
where EEC (in kWh m3) is the consumption of electrical energy
(kWh) to degrade a pollutant in 1 m3 of volume, t is the time of
treatment (min), P is the rated power of the E-beam (kW), and v is
the treatment volume of wastewater (in L). The volume of waste-
water treated was 9.6 L as calculated using the dimensions of
stainless steel tray (80  60  2 cmÞ. The rated power of E-beam
unit was 1.35 kW. The costs involved during E-beam radiolysis of
LOSW and HOSW were calculated on the basis of COD removal effi-
ciency of 50%. The total cost of E-beam radiolysis alone and E-
beam þ H2O2 radiolysis for LOSW was found to be 0.50 and 7.87 USD
m3; whereas, for HOSW, it was found to be 0.67 and 11.48 USD m3,
respectively.
Results indicated that treatment cost of E-beam radiolysis alone,
biological treatment alone and E-beam þ biological treatment for
LOSW was found to be 0.50, 2.35 and 2.85 USD m3; whereas, for
HOSW, it was found to be 0.67, 0.7 and 1.37 USD m3, respectively.
The higher operating cost of ASP treatment and E-beam
radiolysis þ ASP treatment of LOSW could be due to the higher
10 R. Changotra et al. / Journal of Cleaner Production 242 (2020) 118544

Table 2
The treatment cost of energy involved in E-beam radiolysis of low strength pharmaceutical wastewater.

S.No. Treatment Average treatment time (min) Cost of H2O2 used (INR m3) Cost of treatment (INR m3) with INR 5/kWha Cost of treatment (USD m3)
Employed

1. E-beam alone 3 NIL 35.15 0.50

2. E-beam þH2O2 2.04 523 546.9 7.87

Average treatment time required for 50% COD removal was calculated by considering the dose rate of 25 kGy min1
a Considering the average cost of INR 5/kWh (0.072 USD/kWh) for industrial sector in India.

Table 3
The treatment cost of energy involved in E-beam-radiolysis of high strength pharmaceutical wastewater.

S.No. Treatment Average treatment time (min) Cost of H2O2 used (INR m3) Cost of treatment (INR m3) Cost of treatment (USD m3)
Employed With INR 5/kWha

1. E-beam alone 4.02 NIL 47.1 0.67

2. E-beamþH2O2 1.08 785 797.6 11.48

Average treatment time required for 50% COD removal was calculated by considering the dose rate of 25 kGy min1
a Considering the average cost of INR 5/kWh (0.072 USD/kWh) for industrial sector in India.

Table 4
The total operating cost involved in E-beam radiolysis þ biological treatment of pharmaceutical wastewater.

(A) Costs involved during E-beam radiolysis alone of LOSW (60 L) ¼ 0.50 USD m3
(B) Operating cost of lab-scale ASP treatment of LOSW
 Total volume of LOSW treated ¼ 60 L (0.06 m3)
 Cost of activated sludge ¼ 0 USD
 Energy consumed during operation of ASP process (pumping through peristaltic
pumps, air spargers, stirrer etc.) ¼ 3,270 Wh
 With 50% degradation, COD removal ¼ 1,660 mg L1 (1.66 kg m3)
 Energy consumed during per kg of COD removed ¼ 3,270/1.66 ¼ 1.96 kWh
 Electricity price in India ¼ 0.072 USD/kWh
 Cost of electricity consumption ¼ 1:96  0.072 ¼ 0.141 USD/kWh
 Cost per m3 of wastewater treated ¼ 0.141/0.06 ¼ 2.35 USD m¡3
Total operating cost of E-beam radiolysis þ ASP treatment of LOSW ¼ (A) þ (B)
¼ 2.85 USD m¡3
(1) Costs involved during E-beam radiolysis alone of HOSW (60 L) ¼ 0.67 USD m3
(2) Operating cost of lab-scale ASP treatment of HOSW
 Total volume of LOSW treated ¼ 60 L (0.06 m3)
 Cost of activated sludge ¼ 0 USD
 Energy consumed during operation of ASP process (pumping through peristaltic
pumps, air spargers, stirrer etc.) ¼ 3,495 Wh
 With 50% degradation, COD removal ¼ 5,940 mg L1 (5.94 kg m3)
 Energy consumed during per kg of COD removed ¼ 3,495/5.94 ¼ 0.588 kWh
 Electricity price in India ¼ 0.072 USD/kWh
 Cost of electricity consumption ¼ 0:588  0.072 ¼ 0.042 USD/kWh
 Cost per m3 of wastewater treated ¼ 0.042/0.06 ¼ 0.7 USD m¡3
Total operating cost of E-beam radiolysis þ ASP treatment of HOSW ¼ (1) þ (2)
¼ 1.37 USD m¡3

Table 5
Evaluation of total cost of E-beam facility for industrial applications of wastewater treatment.

Installation Treatment application Total cost of E- Shielding and Capital Treatment Cost of
capacity beam unit (M USD) maintenance cost (M requirement capacity treatment (USD
USD) (kUSD) (m3day1) m3)

E-Beam Pharmaceutical wastewater treatment with an average 1.25 0.3 4,500 10,000 0.6
(20 MeV, COD of 10,000e12,000 mg L1 by E-Beam
100 kW)

energy consumption during per kg of COD removal for LOSW when
compared to HOSW as explained in Table 4.
The use of radiation technology has been considered as an
emerging tool to treat groundwater, surface water, wastewater and
sludge. High energy E-beam radiation based pilot and commercial
sludge treatment plants have been successfully installed in India,
USA, New Mexico, Argentina, Korea and Germany (Haji-Saeid,
2007; IAEA, 2008). E-beam machine involves only one time
installation and nullifies the use of any auxiliary chemicals for the
treatment which further strengthen the potential applicability of E-
beam irradiation as a clean, cost-effective and productive tool for
water and wastewater treatments. Thus, radiation technology
particularly the use of E-beam accelerators could play an impera-
tive role in near future for the treatment of real pharmaceutical
wastewater at pilot as well as commercial scale.
4. Conclusion
Hybrid sequential treatment process of coagulation, E-beam
irradiation and biological treatment was investigated for the
treatment of real pharmaceutical industrial wastewater. The impact
of combined treatment was investigated on physicochemical
characteristics, biodegradability and toxicity analysis of the treated
wastewater. Sequential treatment route from coagulation to E-
beam irradiation and subsequent biological degradation lead to
synergistic degradation and detoxification of the pharmaceutical
wastewater streams with overall improved COD and TOC removal
efficiencies. Cytotoxic evaluation revealed that E-beam irradiated
wastewaters did not exhibited toxicity against the selected micro-
organisms. The cost of electrical energy consumed during E-beam
irradiation treatment of wastewater was calculated. The overall
cost of the set-up of E-beam unit and treatment cost for real
pharmaceutical wastewater was evaluated to establish the appli-
cability of the E-beam technology at industrial scale. This study
suggests that E-beam technology could soon become a final strat-
egy for the remediation of generalized wastewater contamination,
and if used with traditional treatment technologies, it may achieve
best possible treatment goals at lowest cost possible.
 R. Changotra et al. / Journal of Cleaner Production 242 (2020) 118544
Declarations of interest
None.
Acknowledgement
Authors are thankful to the Department of Atomic Energy
(DAE)-Board of Research in Nuclear Sciences (BRNS), Government
of India [Project Sanction No. 35/14/48/2014-BRNS]. Authors are
sincerely thankful to Dr. Y.K. Bhardwaj, RTDD, Bhabha Atomic
Research Centre, India for his support to initiate this work. Author
also likes to thank Shri K.S.S. Sharma, Shri Ravindra Patkari, EBPS,
BARC and Dr. Lalit Varshney for their support in carrying out
electron beam irradiation.
Appendix A. Supplementary data
Supplementary data to this article can be found online at
https://doi.org/10.1016/j.jclepro.2019.118544.
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