Environmental Technology & Innovation 23 (2021) 101757

Contents lists available at ScienceDirect

Environmental Technology & Innovation

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

Removal of emerging micropollutants originating from

pharmaceuticals and personal care products (PPCPs) in water
and wastewater by advanced oxidation processes: A review
Radhakrishnan Yedhu Krishnan a , Sivasubramanian Manikandan b ,
∗
Ramasamy Subbaiya c , Muniyandi Biruntha d , Muthusamy Govarthanan e , ,
∗
Natchimuthu Karmegam f ,
a
Department of Food Technology, Amal Jyothi College of Engineering, Kanjirappally, Kottayam – 686 518, Kerala, India
b
Department of Biotechnology, Saveetha School of Engineering, Saveetha Institute of Medical and Technical Sciences
(SIMATS), Saveetha Nagar, Thandalam, Chennai – 602 105, Tamil Nadu, India
c
Department of Biological Sciences, School of Mathematics and Natural Sciences, The Copperbelt University, Riverside, Jambo Drive,
P O Box 21692, Kitwe, Zambia
d
Vermitechnology Laboratory, Department of Animal Health and Management, Alagappa University, Karaikudi 630 003, Tamil
Nadu, India
e
Department of Environmental Engineering, Kyungpook National University, Daegu 41566, Republic of Korea
f
Department of Botany, Government Arts College (Autonomous), Salem-636 007, Tamil Nadu, India

article info a b s t r a c t

Article history: Because of their intrinsic potential to produce metabolic effects on the human body
Received 19 May 2021 at smaller concentrations, pharmaceuticals and personal care products (PPCPs) are
Received in revised form 20 June 2021 a distinct category of emerging environmental pollutants. Due to their widespread
Accepted 27 June 2021
intake, limited metabolic capacity, and indecorous disposal, PPCPs pollutants are com-
Available online 30 June 2021
monly found in water supplies and wastewater treatment plants. If partly oxidized
Keywords: PPCPs are introduced into wastewater treatment plants, they will disrupt biological
Advanced oxidation wastewater treatment procedures. As a result, traditional wastewater treatment plants
Electrochemical oxidation are inadequate for PPCPs elimination. PPCPs have been effectively eliminated using
Ionizing radiation advanced oxidation methods such as electrochemical oxidation, ultrasonication, and
Personal care products ionizing radiation. This review summarizes recent studies on the removal of PPCPs by
Pharmaceuticals advanced oxidation processes, as well as knowledge useful for applying these processes
Ultrasonication
in water and wastewater treatment. The degradation of different classes of PPCPs
has been reviewed to analyze (i) significant factors — initial concentration of PPCPs,
ultrasonication power, radiation dose, current density, temperature, pH, time, and effect
of catalysts; (ii) degradation efficiency of the processes when applied in combination
with other advanced oxidation methods; (iii) key factors that affect the removal of
PPCPs based on their properties. In addition, suggestions for future studies on advanced
oxidation methods and their limitations were discussed. Overall, this review could aid
in providing an in-depth understanding of the current research trends concerning PPCPs
and advanced oxidation processes.
© 2021 Elsevier B.V. All rights reserved.

∗ Corresponding authors.
E-mail addresses: gova.muthu@gmail.com (M. Govarthanan), kanishkarmegam@gmail.com (N. Karmegam).

https://doi.org/10.1016/j.eti.2021.101757
2352-1864/© 2021 Elsevier B.V. All rights reserved.
R.Y. Krishnan, S. Manikandan, R. Subbaiya et al. Environmental Technology & Innovation 23 (2021) 101757

1. Introduction

In many diverse fields such as livestock farming, medicine, aquaculture, personal hygiene products and cosmetics,
pharmaceutical, and personal care products (PPCPs) are extensively used. PPCPs form an integral part of the daily lives
of humans and their extensive use and poor removal by conventional biological wastewater treatment facilities make
them omnipresent in the environment. Due to their continued presence in aquatic environments, PPCPs have become
recognized in recent decades as pollutants of emerging concern (Fabbri et al., 2017; Mille et al., 2020). The acronym
‘PPCPs’ generally refers to products for human or animal health or their medical purposes. While in many developed and
developing countries, water treatment is now compulsory to minimize pollution, many pollutants are not eliminated in
wastewater treatment plants effectively (Baena-Nogueras et al., 2017; Brunsch et al., 2019; Delli Compagni et al., 2020).
These agents may constitute a threat to water supplies and could pose serious health risks that are specifically related to
estrogen activity and could also cause effects on the endocrine system (Zhang et al., 2017). The report that PPCPs have
been found even in Antarctic waters is really alarming (Emnet et al., 2015). A large number of recent studies on the control
of PPCPs have been recently reported (Kumar et al., 2019; Kim and Homan, 2020; Hamid et al., 2021; Hena et al., 2021).
These include strategies to control their emissions (Li et al., 2021; Chen et al., 2021), characterization of these pollutants
(Rashid and Liu, 2021; Wu et al., 2021), and degradation of these compounds into non-toxic intermediates (Atugoda et al.,
2020; Hassani et al., 2020; Keerthanan et al., 2020). These products are used daily by most people around the globe and
then they get subsequently released into our water sources.

1.1. General classes of PPCPs

Table 1 summarizes the general classification of PPCPs and their examples. PPCPs may be grouped into several
classes based on their specific properties and use. The personal care products generally include fragrance ingredients,
sunscreen UV protectors, preservatives from multiple sources, general classes of disinfectants, mosquitoes, and other
insect repellents, and soaps and shampoos. The pharmaceuticals are majorly grouped as analgesics, antibiotics, anticancer,
anticonvulsant, antidepressants, antiseptics, hormones, β -blockers, non-steroidal anti-inflammatory drugs, barbiturates,
and lipid regulators (Esplugas et al., 2007; Huerta-Fontela et al., 2011; Dodson et al., 2012).

1.2. Sources and emission of PPCPs

After being utilized, most PPCPs get released into our surroundings in many ways. Untreated domestic effluents and
treated wastewater from factories, industrial houses, and hospitals that include both refractory and partly degraded PPCPs
can get discharged directly into different water sources with no prior treatment protocols (Suppes et al., 2017; Wang et al.,
2015). The primary source of environmental PPCPs is landfill leachates and both treated and untreated sewage water. Both
wastewater treatment plants and sewage treatment plants are active contributors of PPCPs micropollutants (Daughton
and Ternes, 1999). The drugs for both human and veterinary needs get released through both direct and indirect routes.
Any of the pharmaceutical constituents which are not metabolized or disintegrated are defaecated from the body by urine
or feces and then discharged into sewers. However, in some cases, such waste materials do not get released directly into
the environment, but are treated before their release. But, after treatment of these wastes, the biosolids and wastewater
gets utilized as fertilizers in farmlands and results in the exposure of PPCPs to the nearby water sources through run-
off. Moreover, leaching of the PPCPs micropollutants occurs from the soil and they eventually reach the groundwater.
Similarly, when liquid or solid animal wastes are used as fertilizers, the veterinary drugs already administered to those
animals find their way into the soil. All these micropollutants along with their metabolic products create soil pollution
and have the potential to penetrate the food chain.
Other important local points of possible pollution include improper disposal of discarded or expired products, which
get directly discarded in lavatories or culminated in landfills, and pharmaceutical contaminants from manufacture or
industrial spill occurrences (Klavarioti et al., 2009). Other pollutants from personal care products such as sunscreens and
cosmetics also get released as a result of daily human activities like swimming, bathing, and other activities related to
hygiene. Since PPCPs are used in all parts of the world, the importance of various exposure pathways, therefore, varies
geographically as well. When released into the environment, certain PPCPs can get transported over long distances based
on the physical and chemical properties of the compound and its receptor characteristics. In general, the PPCPs are
hydrophilic, low in volatility, and strongly polar and thus are mainly distributed throughout the ecosystem via water
transport and distribution through the food chain (Caliman and Gavrilescu, 2009). The different routes through which
PPCPs get released into the environment are shown in Fig. 1.

1.3. Environmental, biological hazards and toxicity of PPCPs

PPCPs in trace quantities have been shown to have possible harmful effects on both human and animal lives resulting
in both chronic and acute toxicity, including disruption of several biological processes as well as development and
reproduction inhibition (Crane et al., 2006; Ma et al., 2018; Ren et al., 2021b). The failure to remove PPCPs from wastewater
treatment facilities presents a potential danger to public health and marine organisms. The widespread use, combined with
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R.Y. Krishnan, S. Manikandan, R. Subbaiya et al. Environmental Technology & Innovation 23 (2021) 101757

Fig. 1. Sources and emissions of PPCPs.

Table 1
General classification of PPCPs and their examples.
Class Description Examples References
Personal care Fragrances Eugenol, musk ketone, limonene, methyl Dey et al. (2019),
products salicylate, musk xylene Ebele et al. (2017),
Preservatives Methyl, ethyl and butyl paraben, Figueiredo et al.
2-phenoxyethanol, ethyl 4-hydroxybenzoate, (2016), Liu and
Butylated hydroxyanisole Wong (2013)
Sunscreen agents Octyl-triazone, Oxybenzone, Octinoxate,
Octocrylene, Benzophenone
Mosquito and insect N,N-diethyl benzamide, N,N-diethyl-m-toluamide
repellants
Disinfectants Triclosan, 2-Phenylphenol, Chloroprene,
Methyltriclosan
Soaps and shampoos Sodium Lauryl Sulfate, Ammonium Lauryl Sulfate,
Salicylic acid
Pharmaceuticals Analgesics Ketoprofen, Acetaminophen, Naproxen
Antibiotics Amoxicillin, Doxycycline, Cefalexin, Erythromycin
Anticancer drugs Cytarabine, Ifosfamide, 5-Fluorouracil
Cincinelli et al.
Anticonvulsant Phenytoin, Carbamazepine, Valproic acid
(2015), Guo et al.
Antidepressants Imipramine, Oxazepam, Doxepin
(2020), Jamil (2019),
Antiseptics Chlorhexidine, Hexachlorophene, Acridine
Liu and Wong
Anti-inflammatory Ibuprofen, Diclofenac, Aspirin, Piroxicam
(2013), Rienzie et al.
Hormones Estrone, Estriol, Testosterone, Estradiol
(2019)
β -blockers Bisoprolol, Sotalol, Atenolol
Non-steroidal Celecoxib, Aspirin, Indomethacin, Paracetamol
anti-inflammatory drugs
Barbiturates Amobarbital, Secobarbital, Pentobarbital
Lipid regulators Pravastatin, Clofibric acid, Atorvastatin,
Gemfibrozil

the rapid launch of new PPCPs or their active metabolites, significantly contribute to the proliferation of these substances
in the aquatic environment. Moreover, PPCPs are considered to be pseudo-persistent. Pseudo-persistent micropollutants
are proposed to be more environmentally persistent than other organic micropollutants such as surfactants and pesticides.
This is because, even though environmental processes such as biodegradation are involved, their sources are continuously
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R.Y. Krishnan, S. Manikandan, R. Subbaiya et al. Environmental Technology & Innovation 23 (2021) 101757

replenished (Houtman et al., 2004). PPCPs have also been known to possess negative cumulative effects on terrestrial and
marine habitats. Ecosystems are affected by the antagonistic effects of PPCPs because PPCPs deposits are found in our
food chain, including our water sources and the vegetables and fruits we consume (Kinney et al., 2020; Liu et al., 2020b).
There are also reports about hydrophobic micropollutants being critical in the food chain and certain antibiotics affecting
the long-term water quality (Bai and Acharya, 2017).
When biosolids and sewage-treated water is made use in irrigation, PPCPs residues can be discovered in plants,
particularly in their edible tissues (Rajapaksha et al., 2015). The primary concern about pharmaceutical toxicity stems from
the fact that they are explicitly engineered to enhance biological activity even at very low doses and to target specific cell-
signaling, enzymatic, and metabolic pathways. From a pharmacological point of view, these engineered molecular targets
increase the risk of pharmaceutics becoming active in non-intended organisms. In fish and other marine living organisms,
certain PPCPs bioaccumulates, eventually leading to numerous unforeseen interferences. Enlargement of fish livers owing
to the continuous exposure to PPCPs in water (Gunnarsson et al., 2009), impact on reproductive capacities, and negative
histopathological effects in zebra fish (Galus et al., 2013) are some indications of the toxicity effects of PPCPs. The presence
of PPCPs in the marine environment is a major concern because PPCPs can interact with the endocrine system and cause
unintended effects and disturbances of homeostasis. Also, the toxicity caused by complex blends of micropollutants at
comparatively trace concentrations can result in synergistic interactions (Brooks et al., 2003; Cleuvers, 2003). Another
major problem posed by the incidence of PPCPs micropollutants in the environment is the possibility for the emergence
of antibiotic-resistant strains of bacteria (WHO, 2015). Therefore the need of the hour is to control the effects of such
persistent pollutants in our environment both through regulations and through proven scientific methods (Hodges et al.,
2018; Geetha et al., 2021).
Owing to the serious threat posed by PPCPs pollutants, different countries have planned and enacted regulations to
control their release into the environment. The National Take-Back Initiative by the United States Drug Enforcement
Administration is one such effort to help the residents in disposing of unwanted or unused drugs. As a result of the
initiative, around 300 tons of drugs were collected and safely disposed of in 2010 (Straub and Hutchinson, 2012). A priority
list of pollutants has been developed both by US Environmental Protection Agency and by the European Union which
identifies PPCPs chemicals that pose serious health risks when released into the environment (Ebele et al., 2017). When
new pharmaceuticals or chemicals recognized by relevant policies are launched, they are required to pass the established
environmental risk assessment for pharmaceuticals (ERA) regulations (Straub and Hutchinson, 2012). The risk assessment
of various chemicals is determined by calculating their risk quotient (RQ) (Kosma et al., 2014) or hazard quotient (HQ)
(Prosser and Sibley, 2015). RQ or HQ is calculated based on the ratio of measured or predicted maximum environmental
daily concentration of a pollutant to the no-risk concentration of that pollutant to humans or other organisms based on
available experimental data. Therefore, the potential risk of a pollutant to pose threat is considered low when RQ or HQ <
0.1, and high when RQ or HQ >1 (Kosma et al., 2014). But these regulations are not yet fully institutionalized by different
world countries.

1.4. Water treatment processes concerning PPCPs

The PPCPs used daily are discharged into sewer pipes along with the wastewater from wash and defecation. Not just
PPCPs, but different organic and inorganic pollutants are getting discharged daily posing a huge risk to the environment
(Bhavya et al., 2021; Paidi et al., 2021). They are then eventually transported for traditional/conventional treatment at
the sewage/wastewater treatment plants and the residual PPCPs gets ultimately released into the general water system.
As a result, the elimination efficacy of PPCPs in the sewage water treatment plant is critical for the protection of water
resources. When PPCPs exit the sewage/wastewater treatment plants, their concentration is too meager and therefore is
considered less risky. This might be one of the reasons for micropollutants in PPCPs not being regulated by maximum
discharge limits (Lant, 2018). But, due to the pseudo-persistent nature of these pollutants, trace concentrations in the
range of 1 ng/L–100 µg/L in the aquatic environment can be detrimental to both animal and human life in the long
run (Yap et al., 2019). The primary processes for sewage/wastewater treatment include grit removal, sedimentation, and
filtration. The primary processes of sewage/wastewater treatment have varying efficacies for the removal of PPCPs due
to the disparity in partition coefficients between solids and liquids. The secondary process includes biological treatment
procedures and its efficacy is related to biodegradation and sorption. The elimination efficacy of most PPCPs is low in
a conventional sewage/wastewater treatment plant (Liu et al., 2020a; Kumar et al., 2021). The treatment protocols in a
conventional water treatment plant include aeration, coagulation, and flocculation, sedimentation, filtration and ozone,
chemical or ultraviolet disinfection process before it is used for human consumption.
To eliminate PPCPs effectively and to minimize human health risks from PPCPs, unconventional control techniques
and approaches are vital. These unconventional or advanced control techniques include membrane filtration, sorption,
and advanced oxidation processes. One of the most frequently used methods for eliminating pollutants from water is
membrane filtration (Shanmuganathan et al., 2017). Reverse osmosis, nanofiltration, ultrafiltration, and microfiltration
are all examples of membrane filtration (Yoon et al., 2007; Wei et al., 2020; Ren et al., 2021a). Both reverse osmosis and
nanofiltration are effective in removing PPCPs from wastewater (Lin and Lee, 2014; Song et al., 2020; Xu et al., 2020).
Another approach for removing PPCPs from water is sorption. The most commonly used sorbent in treating wastewater is
activated carbon (Rodriguez et al., 2016; Jeirani et al., 2017). For PPCPs, activated carbon has high porosity, surface area,
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R.Y. Krishnan, S. Manikandan, R. Subbaiya et al. Environmental Technology & Innovation 23 (2021) 101757

Fig. 2. Outline of advanced oxidation process in PPCPs biodegradation pathway.

and adsorption capacity. Granular activated carbon and powdered activated carbon are various forms of activated carbon
that can be used in the water treatment process. Carbon nanotubes and graphene oxide are also used as sorbents for the
removal of PPCPs in aqueous solutions and are proved to be of high efficiency (Delhiraja et al., 2019; Kurwadkar et al.,
2019).
Another advanced strategy for the removal of PPCPs in waste/sewage water treatment plants and conventional water
treatment plants is the advance oxidation process (AOP). AOP is employed either independently or in a blend with other
chemical or biological processes for the removal of PPCPs.

1.5. Advanced oxidation process in PPCPs removal

Recently, AOP has established itself as one among the most promising technologies for removal of pollutants from water
with extensive applicability, near to compete for degradation of pollutants, and high mineralization efficiency (Khasawneh
and Palaniandy, 2020; Van et al., 2020; Amor et al., 2021; Nguyen et al., 2021). These processes were initially utilized for
the treatment of potable water (Glaze, 1987). AOP is focused on the development of materials with robust oxidation power
and poor selectivity of the reaction. Such substances degrade certain PPCPs that are difficult to be extracted into simple
short chain molecular compounds. Free radical species or reactive oxygen species (like OH› or O›2− ) are potent oxidants
capable of initiating the AOP to break down contaminants into non-toxic simpler molecules. The specific advantage of
hydroxyl radical (OH› ) is their unusually high reaction potential and oxidizing capacity (Eo = 2.8 V) (Andreozzi et al.,
1999). AOPs have the potential to alter the functional groups, their characteristic properties and polarity of the targeted
PPCPs (Papageorgiou et al., 2014). When AOP is used, the organic molecules present in PPCPs get degraded into inorganic
ions, H2 O and CO2 due to the effect of hydroxyl radicals. Other reactions of hydroxyl radicals with organic molecules
can either be radical–radical interactions, hydrogen abstraction or direct electron transfer (Legrini et al., 1993). When
OH› reacts with organic groups, it results in the formation of R› or R› -OH (carbon-centered radicals) (Huang et al., 1993).
In addition, the non-selective behavior of OH› aids in its rapid reaction with different chemical species with reaction
rate constants in the range of 108 –1010 M−1 s−1 (Deng and Zhao, 2015). Another important factor affecting the oxidizing
potential of OH› is the affinity of organic molecules present in PPCPs to these oxidizing agents (Patel et al., 2019).
The different approaches for AOP include ozonation, UV-based oxidation, Fenton and Fenton-like approach, electro-
chemical methods, ultrasonication, photocatalysis, ionizing radiation, and other combined processes. A significant amount
of literature is available on the removal of PPCPs through ozonation, Fenton, and UV-based oxidation methods (Wang and
Xu, 2012). Of these methods with limited focus have been the approaches by electrochemical oxidation, ultrasonication,
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R.Y. Krishnan, S. Manikandan, R. Subbaiya et al. Environmental Technology & Innovation 23 (2021) 101757

Fig. 3. General mechanisms involved in free radicals generation by ultrasonication and ionizing radiation.

and ionizing radiation. Hence, in the following sections, major advancements related to these three AOPs are discussed
in detail. Fig. 2 illustrates the brief pathway of AOPs in PPCPs biodegradation. The objective of this review was a detailed
analysis of the principle, applications, and limitations of advanced oxidation methods, viz., ultrasonication, ionizing
radiation, and electrochemical oxidation in the removal of PPCPs. Also, the efficiency of these advanced methods when
used in combination with other AOPs has been discussed.

2. Ultrasonication

Ultrasonication has long been recognized as a sophisticated treatment method for removing complex inorganic and
organic contaminants from both wastewater and water. Ultrasonication has demonstrated significant benefits, such
as low secondary emissions, safety, and energy savings. During ultrasonication, multiple reaction zones with varying
concentrations of reactive oxygen species and temperatures are developed. These include — a gaseous zone, a zone of
gas–liquid interphase and a zone of bulk liquid (Park et al., 2011). The general mechanisms involved in the degradation
by ultrasonication are shown in Fig. 3 (Pang et al., 2011). It is at this bulk liquid zone, cavitation process results in the
formation and collapse of bubbles. Therefore, ultrasonication processes can lead to the oxidation and thus obliteration of
different pollutants with diverse physicochemical characteristics (Makino et al., 1983; Adewuyi, 2001).

2.1. Effect of sonication conditions on PPCPs removal efficiency

Ultrasound power, ultrasound frequency, temperature, pH, and the presence of certain promoters influence the
sonodegradation of PPCPs. During ultrasonication, ultrasonic waves in the range of approximately >20 kHz are transmitted
in the liquid medium to produce acoustic cavitation. The size of the cavitation bubble is determined by the ultrasound
power and frequency (Serpone and Colarusso, 1994; Joseph et al., 2009). In general, at higher frequencies, hydroxyl radical
production is likely to be boosted due to relatively increased temperature and pressure, as well as increased decavitation.
Furthermore, in such circumstances, hydroxyl radicals may be formed more aggressively and get transferred into the
liquid medium before merging in the bubble cavity (Belgiorno et al., 2007). Im et al. (2014) studied the degradation of
pharmaceuticals — naproxen and acetaminophen, using ultrasonication. When 28, 580, and 1000 kHz frequencies were
studied, the most effective frequency based upon both the rate of PPCPs degradation and hydrogen peroxide output
was found to be 580 kHz. Furthermore, increasing the solution temperature and ultrasound power density boosted the
degradation of PPCPs at 580 kHz.
With increasing solution temperature, the bubbles generated as a result of cavitation and the generation of reactive
hydroxyl radical increases. This leads to an increase in the vapor pressure of the liquid and a dense accumulation of
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R.Y. Krishnan, S. Manikandan, R. Subbaiya et al. Environmental Technology & Innovation 23 (2021) 101757

chemical species in the cavitation bubbles (Chiha et al., 2011; Anandan et al., 2020). With varying temperatures of 15 to
35 o C during ultrasonication, the rate of degradation of naproxen and acetaminophen was found to be increasing with
increasing temperature. However, at a frequency of 1000 kHz, a temperature higher than 35 o C resulted in a decrease in
the rate of degradation of these PPCPs. This indicated that increasing the temperature beyond an optimum level would
result in the decrease of free radicals and net energy in the reaction media (Im et al., 2013). Similarly, higher degradation
rates of naproxen and acetaminophen were observed under acidic pH conditions, and this was due to the increased
generation of hydroxyl radicals under these conditions (Golash and Gogate, 2012).
The rate of hydrogen peroxide formation influences the rate of PPCPs degradation. On studying the ultrasound-
induced degradation of diclofenac using three ultrasonic bath systems at 216 kHz, 617 kHz, and 850 kHz, the maximum
degradation of diclofenac was observed at 617 kHz. This was a result of the generation of a higher concentration of
hydrogen peroxide in the reaction medium (9 µM/min). The rate of hydrogen peroxide formation was also found to be
increasing with increasing ultrasound power (Hartmann et al., 2008). Similarly, the presence of carbon tetrachloride (a
volatile oxidation compound) in the reaction medium is believed to promote the degradation efficiency of PPCPs. This
increase in the rate of degradation is due to the decreased level of H› (Mahamuni and Pandit, 2006). Another factor that
can enhance PPCPs degradation is gas injection. The presence of saturating gases, viz., oxygen, argon, and air alter the
effectiveness of reaction by enhancing cavitation. Since cavitation enhances the presence of radical species, the increasing
concentration of oxygen, in turn, promotes the rate of sonochemical degradation (Serpone et al., 1994; Pétrier et al., 2007).

2.2. Effect of catalysts and other combined processes in PPCPs removal efficiency

To speed up the degradation rate, various heterogeneous catalysts are used to improve the formation of cavitation
bubbles. These include several carbon-based and non-carbon-based catalysts. Carbon-based catalysts include engineered
biochar (Sajjadi et al., 2020), carbon nanotubes (CNTs) (Zhang et al., 2019), and activated carbon (Secondes et al., 2014)
based approaches. On the sonocatalytic degradation experiments conducted on ibuprofen and sulfamethoxazole using
single-walled carbon nanotubes, hydrogen peroxide formation showed an increase from 10 µM (without CNTs) to 31 µM
(with CNTs) at a frequency of 28 kHz, and from 82 µM (without CNTs) to 111 µM (with CNTs) at a frequency of 1000 kHz
(Al-Hamadani et al., 2016). Increased adsorption capacity and free hydroxyl radical formation due to the influence of
ultrasonication is also another factor that helped in the accelerated degradation of ibuprofen and sulfamethoxazole.
Similarly, biochar along with ultrasonication provides the simultaneous effect of hydroxyl radicals and adsorption,
providing nucleation sites to the adsorbent particles (Im et al., 2014). These simultaneous effects result in the rapid
degradation of PPCPs.
Various non-carbon-based catalysts that can be used to increase the degradation efficiency of PPCPs include nanocom-
posites of TiO2 (Awfa et al., 2018), stainless-steel wire mesh (Bolobajev and Goi, 2017), and ZnO nanoparticles (Khataee
et al., 2015). The sonocatalytic activity of Sm-doped ZnO nanoparticles in the degradation of phenazopyridine was studied
by Eskandarloo et al.(Eskandarloo et al., 2016). The Sm-doped ZnO nanoparticles with 0.4 mol% concentration of Sm
showed an increased activity of 59%. The reasons for this increased sonocatalytic activity were due to the presence of
more reactive free hydroxyl radicals due to sonolysis and the scavenging of free electrons in the ZnO conduction band. The
enhanced degradation of PPCPs due to the effect of TiO2 nanocomposites was because of the generation of free electrons
due to its exposure of high energy light when suspended in water and its reaction with O2 to form O›2 (Konstantinou and
Albanis, 2004). A combination of TiO2 nanocomposites and stainless-steel wire mesh further enhanced the sonocatalytic
activity due to the enhancement of mass transfer and reactivity on the catalyst surface, enhanced active site formation on
the catalyst surface, and the combined action of hot spot generation in liquid medium and free hydroxy radicals formation
on catalytic surface (Zhao et al., 1993; Eren and Ince, 2010; Ryu et al., 2021).
In addition to the various catalysts used, there are also certain combined processes in combination with ultrasonication
for the degradation of PPCPs. These combined/hybrid processes include the combination of ultrasonication + ozonation
(Goi and Viisimaa, 2015; Abdurahman and Abdullah, 2020), ultrasonication + UV irradiation (Adewuyi, 2005), ultrasoni-
cation + H2 O2 / S2 O28− (Price and Clifton, 1996; Upadhyay and Khandate, 2012). In ultrasonication + O3 , the mass transfer
of O3 is enhanced due to the presence of ultrasonication and aids in the formation of more free hydroxyl ions in the
liquid medium (Wu et al., 2020). In the experiments performed on the degradation of diclofenac, the ultrasonication + O3
treatment induced increased degradation of the pollutant when treated for 5–20 min due to the synergistic effect between
the two processes (Naddeo et al., 2009). In the degradation studies on 4-chlorophenol using hybrid ultrasonication + UV,
increased rate constant was observed when compared to the individual processes. This increased rate constant may be a
result of geyser effect due to sonication and direct photochemical action (Hamdaoui and Naffrechoux, 2008).

2.3. Effect of sonication on various types of PPCPs and their removal

Different classes of PPCPs are effectively degraded and removed from water and wastewater. Table 2 summarizes
experiments and their results on degradation of PPCPs by sonication. Use of catalysts along with ultrasonication process
has been found to enhance the degradation efficiency in most cases (Hassani et al., 2017). It is also to be noted that in
most cases, pure water was used as the matrix (Savun-Hekimoğlu and Ince, 2017; Lianou et al., 2018). The ultrasonication
power required to achieve complete degradation depended upon the initial concentration of pollutants and the nature of
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Table 2
Summary of selected PPCP removal by ultrasonication.
PPCPs Conditions
Ampicillin and Initial concentration: 30 µM;
Nafcillin Ultrasonic power: 24.4 W;
Frequency: 375 kHz; pH: 6.5;
Time: 60 min; UV light: 4W; Fe2+
concentration: 5 mg/L; Water
from waste water treatment plant
was used as the matrix
Trimethoprim Initial concentration: 500 µg/L;
Ultrasound power density: 60
W/L; Time: 90 min; pH: 3;
Ultrapure water, bottled water,
wastewater and 50% wastewater
was used as the matrix.
Methyl paraben Catalyst: Sepiolite; Initial
concentration: 10 mg/L; pH:
neutral; Time: 30 min; Ultrasonic
power density: 0.19 W/L;
Temperature: 25 o C; Pure water
was used as the matrix.
Salicylic acid Catalyst: Zero-valent ion (ZVI): 24
mg/L; Ultrasonic Power: 120 W;
pH: 2; HPLC grade water was
used as the matrix.
Ciprofloxacin Catalyst: Nanocomposites of
TiO2 /Montmorillonite (MMT);
Ultrasonic power density: 650
W/L; pH: 6; Initial concentration:
10 mg/L; Distilled water was used
as the matrix.
Piroxicam Initial concentration: 320 mg/L;
Temperature: 20 ◦ C; Ultrasonic
power density: 36 W/L; Time:
10 min; Ultrapure water, bottled
water and surface water was used
as the matrix.
Sulfamethoxazole, Initial concentration: 4 mg/L;
Diclofenac and Time: 10 min; Distilled water was
Carbamazepine used as the matrix.
Carbamazepine Initial concentration: 5 mg/L–40
and Diclofenac mg/L; Time: 60 min; Ultrasound
power density: 400 W/L;
Wastewater effluent was used as
the matrix.
Naproxen Catalyst: Nanocomposites of
ZnO/MMT; Initial concentration:
10 mg/L; Time: 120 min;
Ultrasonic power density: 60 W/L;
pH: 4.5; Distilled water was used
as the matrix.
Ibuprofen and Catalyst: TiO2 ; Initial
Diclofenac concentration: 10 mg/L;
Ultrasound power intensity in
sample: 8.4 W/cm2 ; Time:
120 min; Sonophotocatalysis
source: UV-A; Pure water was
used as the matrix
Degradation process Reference
Sono-photo-Fenton process was used. The Montoya-Rodríguez et al.
antimicrobial activity of ampicillin and nafcillin (2020)
was reduced to 90.5% and 96.3% respectively.
The reaction rate constants for trimethoprim Arvaniti et al. (2020)
degradation for ultrapure water, bottled water,
50% wastewater and wastewater were 0.024
min−1 , 0.0162 min−1 , 0.0106 min−1 and 0.0065
min−1 respectively.
Degradation efficiency of 100% was achieved. The Savun-Hekimoğlu and
use of sepiolite after suitable surface Ince (2019)
modifications greatly enhanced the reaction rate
and degradation efficiency.
Degradation efficiency of 100% was achieved. Savun-Hekimoğlu and
Degradation was achieved even in the absence of Ince (2017)
ZVI if H2 O2 concentration was sufficient.
Degradation efficiency of 65.01% was achieved Hassani et al. (2017)
using TiO2 /MMT. This was higher compared to
pure TiO2 .
Degradation efficiency of 96%. The reaction rates Lianou et al. (2018)
increased with the increasing ultrasound power
density.
Removal efficiency of 12, 3 and 13% respectively Fraiese et al. (2019)
for the three pollutants. The degradation
efficiency of Diclofenac was improved by
90%–94% by the combined ozonation +
ultrasonication process
55% degradation efficiency was observed for both Naddeo et al. (2013)
the pollutants. H2 O2 generation improved at
higher ultrasound power density.
The degradation efficiency using ZnO/MMT Karaca et al. (2016)
catalyst was 60%, which was higher compared to
20% achieved without catalyst.
The initial degradation efficiency with sonolysis Michael et al. (2014)
alone was 10% for ibuprofen and 80% for
diclofenac. Degradation by sonophotocatalysis
enhanced the degradation efficiency of ibuprofen
to 85% and of diclofenac to 96%.

pollutants. In the comparative treatment of benzotriazole by ultrasonication and ultrasonication + UV (Wu et al., 2016),

the degradation efficiency was 5% and 100% respectively. During the combined treatment of PPCPs with ultrasonication

and other hybrid techniques, the primary degradation pathway is dealkylation process with OH› and further reduction of

intermediate products to CO2 and H2 O.

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R.Y. Krishnan, S. Manikandan, R. Subbaiya et al. Environmental Technology & Innovation 23 (2021) 101757

3. Ionizing radiation

When water is irradiated with ionizing radiation (both e− beam and γ - ray) several chemical reactive species get
generated. In the first stage, physical changes results in the generation of hydronium ions. This is followed by further
reactive species generation in the second stage of physico-chemical changes and the third stage of chemical changes.
›
These reactive species includes hydrated electrons (e− +
aq ), hydroxyl radicals (OH ), hydronium ions (H3 O ), hydrogen atoms,
hydrogen radicals, and hydrogen peroxide (Spinks and Woods, 1990). Fig. 3 represents the general mechanism involved
in the degradation by ionizing radiation. While hydroxyl radicals contributed to the oxidation reactions, the reductive
environment is contributed by the hydrogen radicals (Chu et al., 2021; Wan et al., 2016).

3.1. Ionizing parameters affecting PPCPs removal efficiency

The main parameters influencing the removal efficiency and rate of removal of PPCPs from water and wastewater
included — initial concentration of PPCPs, solution pH, absorbed dose and dose rate, and incidence of inorganic anions
like CO23− , NO− − 2−
3 , HCO3 and SO4 . When the initial concentration of PPCPs increased, there is a decrease in the rate
and removal efficiency of PPCPs. The reason behind such an observation is because increased concentration of PPCPs
decreased the probability of collisions of free radicals with the pollutants (Guo et al., 2015). In the mineralization studies
on ciprofloxacin (Sayed et al., 2016a) and norfloxacin (Sayed et al., 2016b), it has been observed that the degradation
rate is directly dependent on the initial concentration of PPCPs. In the case of norfloxacin, when the initial concentration
increased from 3.4–16.1 mg/L, the percentage degradation decreased from 91–76.1% at a constant dose rate of 870 Gy.
Similarly, in the case of ciprofloxacin, when the initial concentration increased from 4.6–17.9 mg/L, the decay constant
showed a decrease from 0.0059–0.0016 /Gy.
The absorbed radiation dose also impacted the efficiency of PPCPs degradation. When the absorbed dose of radiation
increased, the concentration of PPCPs in water and wastewater decreased. However, the radiation chemical yield (G -
value) showed a decrease with the increase in dose of radiation (Basfar et al., 2005; Kongmany et al., 2014; Kim et al.,
2017; Alkhuraiji, 2019). When the radiation dose is increased from 0.1–5 kGy, at a dose rate of 6.69 kGy/h, and an initial
sulfadiazine concentration of 25 mg/L, the sulfadiazine mineralization and degradation also increased (Rivas-Ortiz et al.,
2017). The degradation rate also enhanced with the increasing dose of radiation and followed pseudo-first order kinetics.
Simultaneously, the decrease in G-value might be attributed to the improved competition for reactive species between
PPCPs and the intermediates formed, and the enhanced prospect for recombination between free radicals due to irradiation
(Zheng et al., 2011; Cruz-González et al., 2016). Likewise, solution pH influenced active/reactive species present during
irradiation. In basic pH, OH− reacted with hydroxyl radicals, resulting in the generation of H2 O and O− . Thus, the hydroxyl
radicals got dissociated resulting in the reduced degradation of PPCPs (Poskrebyshev et al., 2002). In comparison, under
acidic conditions, H+ undergoes reaction with hydrated electrons resulting in the formation of hydrogen radicals. This
enhanced the formation of hydroxyl radicals in the liquid medium due to the effects of recombination (Liu et al., 2014a).
2−
Presence of inorganic ions also impacted the degradation. The presence of inorganic ions like HCO− 3 , CO3 and
NO− 3 scavenge hydroxyl radicals, hydrated electrons and hydrogen radicals, thus resulting in the decreased reactivity
of hydroxyl radicals with PPCPs when subjected to ionizing radiation (Ocampo-Pérez et al., 2011; Dell’Arciprete et al.,
2012). Other inorganic ions like NO− −
2 and NO3 reacted with hydroxyl radicals, hydrogen radicals and hydrated electrons
when irradiated, resulting in the formation of HNO3 . HNO3 subsequently reduced the concentration of free radicals and
eventually lead to reduced collision frequency with PPCPs (Lopez Penalver et al., 2013). Presence of organic entities like
humic acid decreased the degradation efficiency of PPCPs in the presence of ionizing radiation (Shah et al., 2014), as
they limit the interaction of free radicals with PPCPs. Also, the presence of organic molecules like glucose and peptone
lead to the reduced rate of PPCPs removal (Chu et al., 2018; Wang et al., 2017a). However, the degradation efficiency of
glucose-containing water increased with the addition of Fe2+ .

3.2. Combined catalytic degradation of PPCPs coupled with ionizing radiation

In order to achieve a higher degradation efficiency of PPCPs, using ionizing radiation alone in the process would not
be the best choice. A very high dose of radiation is required in most cases. An absorbed radiation dose of 28 kGy in the
case of degradation of metoprolol (Slegers and Tilquin, 2006), 20 kGy in the case of iopromide (Kwon et al., 2012), and
50 kGy in the case of erythromycin (Salem I. Ben et al., 2016) are some of the examples for such higher dose of absorbed
radiation requirement. Therefore, use of catalysts and other oxidizing agents along with ionizing radiation could greatly
enhance the removal efficacy of PPCPs and reduce the overall costs involved. In the studies conducted on trimethoprim
using gamma irradiation (Zhang et al., 2016), addition of persulfate greatly boosted the mineralization and degradation
efficiency. With an increase in concentration of persulfate in the range of 0.5–2 mM, the absorbed radiation dose essential
for the degradation of trimethoprim decreased. The reason behind such an observation is attributed to the disintegration of
2,4-diaminoprimidine moiety in trimethoprim resulting in the generation of ammonium ions in increased concentrations.
Addition of Fe2+ is an alternative approach for enhancing the degradation efficiency of PPCPs in the presence of
gamma irradiation. In the studies on sulfamethazine degradation by gamma irradiation in aqueous solutions, addition
of Fe2+ in the concentration range of 0.1–0.6 mM accelerated sulfamethazine degradation (Liu et al., 2014b). Such
9
R.Y. Krishnan, S. Manikandan, R. Subbaiya et al. Environmental Technology & Innovation 23 (2021) 101757

accelerated degradation is attributed to the generation of OH› which possessed higher G-values. Alternatively, Fe-based
metal organic frameworks-derived novel Fe/C nanomaterials can also be utilized as a catalyst in the degradation studies
on cephalosporin C and sulfamethazine by ionizing radiation (Yang et al., 2020). Since more amount of OH› is generated
using Fe/C nanomaterials than with ionizing radiation alone, the enhancement in the degradation of cephalosporin C and
sulfamethazine has been observed. Introducing H2 O2 along with gamma radiation has also been reported to be highly
effective in improving the degradation efficiency of PPCPs (Csay et al., 2012; Kwon et al., 2012; Chu et al., 2015).
Combined approaches of ionizing radiation along with biological treatment methods is found to be another effective
approach for the removal of PPCPs (Chu and Wang, 2016). Biological treatment methods alone are ineffective in removing
carbamazepine, a highly persistent PPCP, from wastewater. With increasing dosage of gamma radiation from 300–800 Gy,
the degradation efficacy of carbamazepine also showed an increase (Wang and Wang, 2017). Similar results were also
reported on the degradation of triclosan using the combined irradiation–biological treatment approach (Wang et al.,
2017b). The removal efficiency of triclosan using biodegradation alone was 54%, whereas, the combined approach along
with gamma irradiation showed a removal efficiency ranging from 88%–97%. One observation was that the capacity to
dechlorinate the reaction medium increased with the increasing radiation dose. Also, the intermediates formed during
the biological treatment process were quickly dissociated during its exposure to radiation, and thus enhancing the overall
degradation rate.

3.3. Applications of ionizing radiation on for the removal of various PPCPs

Application of ionizing radiation on various PPCPs and their effectiveness is summarized in Table 3. In most studies,
gamma irradiation is used as the radiation source. Also, the initial concentration of PPCPs before the irradiation process
in the reaction media was higher and pure water was used as the matrix (Wang and Wang, 2018; Chen et al., 2019).
Even though the degradation efficiency was high in most cases, a higher dose of radiation was also used in the
degradation process. Another key point that could be observed in the studies was that a single pollutant was used. Pseudo-
first order kinetics was well suited for modeling the rate of degradation. Complete mineralization of PPCPs into CO2 ,
through the formation of intermediates required very high radiation doses and was not economically viable. However,
complete mineralization is not imperative in most cases and successive biological treatment processes could successfully
break-down the detrimental effects of most PPCPs.

4. Electrochemical oxidation

In electrochemical oxidation process, the pollutants present in the liquid medium are oxidized using electrochemical
technology. Generally, an electrochemical reactor is equipped with an anode, a cathode, and an electrolytic solution. The
electrochemical oxidation of pollutants may occur by two mechanisms — p-direct oxidation at the anodic surface or
indirect/mediated oxidation (Martínez-Huitle and Ferro, 2006; Dhangar and Kumar, 2020). During direct oxidation at
anode, contaminants initially get partially oxidized and then get converted to salts, H2 O and CO2 due to direct charge
transfer electrochemical combustion reactions. In contrast, during mediated/indirect oxidation the contaminants get
degraded due to the electro-generation of a powerful oxidizing agent at anode. Such powerful oxidizing agents like
hydroxyl radicals and chlorine get absorbed at the surface of anode as an intermediate (Garcia-Segura et al., 2018; Liu
et al., 2019); (Muñoz Morales et al., 2020).

4.1. General reactor designs of electrochemical oxidation process

The selection of electrode is crucial, as it impacts the process selectivity and performance. The chosen electrode must
have certain characteristics that it should satisfy. These characteristics includes: increased selectivity and catalytic activity;
increased electrical conductivity; increased chemical and physical stability; and lower costs (Mandal et al., 2020; Peng
et al., 2020; Feng et al., 2021). Moreover, the electrode selected can be either a three-dimensional or two-dimensional
electrode (Shokoohi et al., 2020). The electrode geometry of both two-dimensional and three-dimensional can be either
static or moving electrodes. Specifically, even though the ratio of electrode surface to the cell volume is higher in
the case of a three dimensional electrode, static parallel electrodes and static concentric cylinders are widely adopted
in the electrochemical reactors for the degradation of PPCPs (Rusling, 1998). The general experimental set-up of an
electrochemical reactor is shown in Fig. 4.
For the degradation of well-known antibiotic, amoxicillin, different electrodes were tested for its effectiveness (Sopaj
et al., 2015). Platinum, carbon-graphite, carbon-fiber, carbon-felt, boron-doped diamond, Ti/RuO2 –IrO2 and PbO were
the different electrode materials studied and among them boron-doped diamond was found to the best. Boron-doped
diamond aided in the formation of higher amount of OH› , O3 and H2 O2 . Also, carbon–graphite and carbon-fiber showed
poorer oxidation properties compared to platinum electrodes. In another study on the degradation of anti-inflammatory
drug, aspirin, electrodes such as boron-doped diamond, PbO2 and porous titanium/boron-doped diamond were utilized
(He et al., 2015). The porous titanium/boron-doped diamond electrodes exhibited the best results, with boron-doped
diamond ones aiding in both indirect and direct electrochemical oxidation. On the other hand, PbO2 electrodes facilitated
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R.Y. Krishnan, S. Manikandan, R. Subbaiya et al. Environmental Technology & Innovation 23 (2021) 101757

Table 3
Summary of selected PPCP removal by ionizing radiation.
PPCPs Conditions
Norfloxacin Source: γ -irradiation; Initial
concentration: 20 mg/L; Dose: 1.5
kGy; pH: 3.25; Pure water was
used as the matrix
Erythromycin Source: γ -irradiation; Initial
concentration: 0.1 mM; Dose: 6
kGy; pH: 5; De-ionized water was
used as the matrix
Piperacillin Source: e− beam; Initial
concentration: 2×10−3 mg/L;
Dose: 0.4–16 kGy; Experiments
were conducted on synthetic
effluent wastewater matrix.
Cephalosporin C Source: γ -irradiation; Initial
concentration: 2×10−2 –2×10−1
mM; Dose: 0.4–2 kGy; Distilled
water was used as the matrix.
Amoxicillin, Source: γ -irradiation; Initial
Doxycycline and concentration: 5×10−2 mM; pH:
Ciprofloxacin Neutral; Temperature: Room
temperature; Dose: 0.5–0.7 kGy;
Distilled water, eggs, milk and
meat was used as the matrix.
Carbamazepine Source: γ -irradiation; Initial
concentration: 4×10−2 mM; Dose:
300 Gy; De-ionized water was
used as the matrix.
Clofibric acid Source: γ -irradiation; Initial
concentration: 5×10−1 mM; Dose:
5 kGy; Milli-Q grade water was
used as the matrix.
Sulfamethoxazole Source: γ -irradiation; Initial
concentration: 1×103 –5×103
µg/L; Dose: 0–400 Gy; Distilled
water was used as the matrix.
Trimethoprim Source: γ -irradiation; Initial
concentration: 2×104 µg/L; Dose:
100–1000 Gy; pH: 6.5–8.5;
Distilled water was used as the
matrix.
Tetracycline, Source: γ - irradiation; Initial
chlortetracycline concentration: 5×10−2 mM; Dose:
and 600–2000 Gy; pH: 4–8; Ultrapure
oxytetracycline water was used as the matrix.
Degradation process Reference
Degradation efficiency of 100% was achieved. Chen and Wang (2020)
Presence of H2 O2 was favorable for the
degradation. The degradation followed pseudo
first-order kinetics.
Degradation efficiency of 100% was achieved. Chu et al. (2019)
Presence of glucose and peptone promoted the
degradation rate by 12% and 2% respectively.
Degradation efficiency of 100%. The treatment Szabó et al. (2018)
with electron beam was successful in eliminating
the antimicrobial activity of piperacillin once it
gets discarded into the environment.
Total organic carbon reduced by 5%–28%. The Chen et al. (2019)
degradation rate decreased with increasing
Cephalosporin C concentration.
More than 80% removal efficiency was observed Alsager et al. (2018)
when water was used as the matrix in the case
of all three pollutants.
Removal efficiency of total organic carbon was Wang and Wang (2018)
38.3%. The presence of hydroxyl and sulfate
radicals contributed positively in the degradation
process.
Removal efficiency of 100% was observed. Csay et al. (2014)
Complete mineralization of the pollutant was also
achieved.
Degradation efficiency of 100% was attained. The Wang et al. (2017)
degradation followed a pseudo-first order reaction
kinetic model.
Degradation efficiency of 100% was achieved. Zhang et al. (2016)
Presence of persulfate in the reaction medium
enhanced the degradation efficiency.
Degradation efficiency of 100% was observed. The Lopez Penalver et al.
lysis was found to follow pseudo-first order (2013)
reaction kinetics. The toxicity of the products
formed after degradation was found to be lower.

only indirect oxidation of aspirin. PbO2 electrodes, though inexpensive is more susceptible to corrosion and can cause
water recontamination due to the liberation of Pb2+ ions.
In the case of mediated electrochemical oxidation of PPCPs, chlorine was the most widely used. In the removal of
caffeine by indirect/mediated electrochemical oxidation, graphite — PVC composite electrode was used as the anode
material (Al-Qaim et al., 2015). The efficacy of caffeine degradation increased considerably with applied voltage, indicating
that the mediated oxidation mechanism was of great importance. Caffeine removal in chloride media was likely better,
although more intermediates were formed due to the contribution of active chlorine. The research showed that the
addition of hydrogen peroxide, compared with just NaCl in the solution, slightly inhibited the electrochemical oxidation.
Other typical mediators in the indirect electrochemical oxidation process includes Fe3+ , Ag2+ , Ni2+ , and Co3+ (Farmer
et al., 1992; Bringmann et al., 1995; Paire et al., 1997).
The cell configuration in an electrochemical reactor can be either divided cell or undivided cell (Polcaro et al., 2000). In
the case of divided cells, the anolyte is separated from catholyte using a porous diaphragm. The selection of this porous
diaphragm has marked effects on the overall efficiency of an electrochemical reactor. The operational complexity and
cost when using a divided cell can be reduced by opting for an undivided cell. Currently, most studies on degradation
of PPCPs using electrochemical oxidation process were carried out using undivided cell in batch operations as they offer
lower corrosion and other mechanical problems (Comninellis, 1994; Wendt and Kreysa, 1999; García-Montoya et al., 2015;
da Silva et al., 2019a).
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R.Y. Krishnan, S. Manikandan, R. Subbaiya et al. Environmental Technology & Innovation 23 (2021) 101757

Fig. 4. Experimental set-up of an electrochemical reactor.

4.2. Significance of general operational parameters

The general factors that influence electrochemical oxidation process in the removal of PPCPs includes — current
density, initial concentration of pollutants, temperature, electrolyte solution, pH, and others. The presence of NaCl as
a supporting electrolyte greatly enhanced the oxidation of pollutants. In the studies on the removal of caffeine using a
conductive diamond as electrode (Indermuhle et al., 2013), the presence of NaCl accelerated the degradation of PPCPs
when compared to Na2 SO4 . Also, the efficiency of caffeine degradation improved with increasing current density due to
the increased concentration of hydroxyl radicals and its quick degradation to oxygen at the anode surface. In another study
on the removal of anticonvulsant drug, carbamazepine, using boron-doped diamond anodes (Domínguez et al., 2010), the
influence of current density was observed to be of primary importance. The maximum degradation of carbamazepine
was achieved at a current density of 190 mA/cm2 , pH of 9 and an electrolytic concentration of 0.48 mol/L. In the study
conducted on the degradation of paracetamol using graphite electrode (Periyasamy and Muthuchamy, 2018), current
density of 5.1 mA/cm2 , electrolyte concentration of 0.1 mol/L and pH of 4 was determined to the optimum conditions.
Thus, the effect of pH on the degradation efficiency was observed to be minimal. The effect of temperature in an
electrochemical oxidation process varied with the process being direct or indirect. In an indirect electrochemical oxidation
process, temperature variation affected the rate of oxidation, and the oxidation rate increased with the increasing
temperature. But, in a direct electrochemical oxidation process, the process remained immune to the variations in
temperature (Canizares et al., 2006).
Other than the above-mentioned factors, initial concentration of PPCPs in water or wastewater also impacted
electrochemical oxidation efficiency. In the degradation of parabens using boron-doped diamond anodes (Domínguez
et al., 2016), the initial concentration of parabens was found to be the most important factor affecting electrochemical
oxidation. There was marked decrease in the removal efficiency of parabens when the initial concentration was increasing.
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R.Y. Krishnan, S. Manikandan, R. Subbaiya et al. Environmental Technology & Innovation 23 (2021) 101757

Similarly, in the ibuprofen degradation studies using metal–oxide-coated Ti anodes (Wang et al., 2016), the oxidation rate
decreased with increasing ibuprofen concentration. The reason for such observation might be due to the increased ratio
of hydroxyl free radicals to ibuprofen and the increased probability of such radicals freely attacking ibuprofen at lower
initial concentrations. Another factor affecting the rate of electrochemical oxidation is the distance between the electrodes
or electrode spacing. Generally, shorter electrode spacing provided higher degradation efficiency of PPCPs. The increased
electrode distances resulted in longer diffusion distances for the pollutants and lower removal efficiency.

4.3. Application of electrochemical oxidation process

Various classes of PPCPs are effectively removed by electrochemical oxidation process. Table 4 shows several case
studies of PPCPs degradation. In most cases, degradation efficiency of more than 80% was observed. Among the anodes
used, boron-doped diamond anodes were reported to be the most effective in removing PPCPs from water samples (García-
Montoya et al., 2015). Use of 3-D electrode reactors were also reported to be very effective (Shen et al., 2017). Due to the
presence of chloride ions and other electrolytes in water, the degradation of PPCPs was rapid when water after preliminary
treatment processes was subjected to electrochemical oxidation (Frontistis et al., 2017). In the study using synthetic
hospital wastewater loaded with four different pollutants, initial membrane bioreactors followed by electrochemical
oxidation as the post treatment method showed 97% removal efficiency of all pollutants (Ouarda et al., 2018). Therefore,
electrochemical oxidation process is better recommended as the final step in water treatment.

5. Future perspectives

Most of the studies on the degradation of PPCPs have been focused on the operational parameters and degradation
efficiency based on pure water systems. So, more studies which use industrial or wastewater effluents as matrix are
required. Also, the initial concentration of PPCPs used in these studies are quite high when compared to the real-world
scenarios. The standardization of analytical methods to detect and characterize the pollutants and intermediate products
in trace quantities are also required.
In the case of ultrasonication, hybrid catalysts using UV-LEDs can be an alternative for conventional lamps. Moreover,
more studies on simultaneous degradation of pathogens, microcontaminants, organic and inorganic pollutants are needed
to really understand the capability of such combined approaches. Considering ionizing radiation, detailed cost analysis
studies on the processes during radiation treatment is very limited. Also, more studies on the combination of ionizing
radiation with Fe2+ and H2 O2 are limited. Such studies could really widen the domain of PPCPs degradation using ionizing
radiation. A combination of ultrasonication and ionizing radiation and their potency to effectively degrade and mineralize
PPCPs is another broad area that can be explored. In the case of electrochemical oxidation, 3-D electrochemical oxidation
systems have proved to be more effective than conventional 2-D electrochemical oxidation systems. Therefore, such
studies could result in value generation. Hybridized electrochemical oxidation processes in combination with other water
treatment processes could significantly overcome the current limitations of electrochemical oxidation methods.

5.1. Challenges ahead

The higher current density, higher ultrasonic power density and higher radiation doses required for the degradation
and mineralization of PPCPs is a cause of concern. As a direct consequence, the costs involved with AOP are higher due
to the increased energy consumption and the higher cost of associated chemicals. The applicability of these methods in
treating large scale industrial effluents and the economic and fabrication costs that could incur in such scale-up operations
are some of the serious challenges faced by AOP. At certain cases, there might also occur the formation of unfamiliar
intractable by-products during the AOP and such by-products might exhibit unpredictable behavior and increased toxicity
than the parent compound. Moreover, AOP are heavily dosage-dependent, and therefore the amounts of free radicals
formed are critical to the efficiency of the process.

6. Conclusions

PPCPs in water systems have been identified as a significant environmental problem in recent years. While PPCPs
were present in groundwater for years, they are just lately being evaluated and analyzed as a possible danger to the
ecosystem. This is attributed to the recent advances in characterization techniques which aid in the detection of PPCPs
level even in trace quantities. Traditional water processing processes are incapable of effectively removing PPCPs, and
therefore advanced oxidation methods like ultrasonication, ionizing radiation and electrochemical oxidation are required
to eliminate the danger of PPCPs from water sources. Different classes of PPCPs like analgesics, disinfectants and antibiotics
have been removed completely by the use of ultrasonication, ionizing radiation and electrochemical oxidation process.
In AOP by ultrasonication, an acidic pH and increasing ultrasound power density favored higher degradation efficiency
of PPCPs. Taking into account AOP by electrochemical oxidation, the choice of anode and the higher current density are
the most significant factors that affected the reaction. In almost all cases, presence free radicals like OH› and control of
end products or intermediate products formed during the process accelerated the degradation process. A combination
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R.Y. Krishnan, S. Manikandan, R. Subbaiya et al.
Table 4
Summary of PPCP removal using electrochemical oxidation process.
PPCPs Conditions
Sulfadiazine Anode: Titanium suboxide mesh;
Cathode: Stainless steel plate;
0.05 mol/L of Na2 SO4 , NaNO3 and
NaClO4 ; Initial concentration: 50
mg/L; Current density: 10
mA/cm2 ; Time: 60 min; pH: 6.3
Sulfamethoxazole Anode: Boron-doped diamond;
Cathode: Stainless steel plate;
Electrolyte: 0.1 M Na2 SO4 ; Initial
concentration: 30 mg/L; Current
density: 30 mA/cm2 ; Time: 3 h;
pH: 7
Methotrexate and Anode: Ti/IrO2 -RuO2 electrode;
Capecitabine Cathode: Stainless steel plate;
Electrolyte: 200 mg/L Na2 SO4 ;
Initial concentration: 0.5 mg/L;
Current density: 30 mA/cm2 ; pH:
neutral
Naproxen Anodes: IrO2 , Pt, RuO2 ,
Boron-doped diamond; Cathode:
Air diffusion electrode;
Electrolyte: 0.05 M NaClO4 ; Initial
concentration: 40 mg/L; pH: 3;
Current density: 50 mA/cm2 ;
Time: 120 min
Atenolol Anodes: Mixed metal oxide and
Platinum electrode; Cathode:
Stainless steel with a gap of
2 cm; Electrolyte: 30 mM NaCl;
Temperature: 25 ◦ C; Current
density: 10 mA/cm2 ; Time:
40 min
Norfloxacin Anode: Boron-doped diamond
electrode; Cathode: Stainless steel
plate with a gap of 3 cm; 0.5 M
Na2 SO4 ; pH: 4; Current density:
20 mA/cm2
Iohexol Anode: Titanium/RuO2 ; Cathode:
Stainless steel with a gap of
0.05 cm; Electrolyte: 0.1 M
Na2 SO4 ; Initial concentration: 525
µg/L; Current density: 38–45
mA/cm2 ; pH: 7.1; Time: 19.8
-30 min
Estriol Anode: Titanium/IrO2 –RuO2 ;
Cathode: Titanium; Electrolyte: 0.1
M Na2 SO4 ; Initial concentration: 1
mg/L; Time: 50 min; Current
density: 20 mA/cm2 ; Batch 3-D
electrode reactor was used
Methylparaben Anode: Boron-doped diamond,
IrO2 , RuO2 and Pt; Cathode: Gas
diffusion electrode; Electrolyte:
0.025 M Na2 SO4; Time: 360 min;
pH: 3; Current density: 66.7
mA/cm2
Musk ketone Anode: Porous Titanium/SnO2 –
PbO2 /Sb2 O3 electrodes; Cathode:
Stainless copper foil with a gap of
1.5 cm; Electrolyte: 0.06 M
Na2 SO4 ; Initial concentration: 50
mg/L; Time: 120 min; pH: 7;
Current density: 40 mA/cm2
of different advanced oxidation methods, or hybrid systems could hold the key for overcoming the current limitations
faced by ultrasonication, ionizing radiation and electrochemical oxidation process in addition to the use of novel catalysts
and hybrid methods. Combining ionizing radiation with biological treatment methods and addition of Fe2+ has been
Environmental Technology & Innovation 23 (2021) 101757
Degradation process Reference
Removal efficiency of 100%. Abatement proceeded Teng et al. (2020)
by indirect oxidation mediated by OH› . The anode
demonstrated potential for high oxygen evolution
and provided a large electrochemically active
surface area.
Removal efficiency of 100%. To gain insights into Hai et al. (2020)
the intermediates formed during the process, the
toxicity studies on electrolysis solution was
performed and it revealed that the solution was
well within the safety boundaries.
Removal efficiency of methotrexate was 95%. Barışçı et al. (2018)
By-products after methotrexate transformation
showed toxicity. But capecitabine transformation
products showed no signs of toxicity but their
removal efficiency was low.
Total organic carbon removal by 78% using IrO2 , Coria et al. (2016)
80% using Pt, 76% using RuO2 and 83% using
boron-doped diamond electrodes. The degradation
followed pseudo-first-order kinetics. When
0.5 mM Fe2+ was added as catalyst, the
maximum oxidation power was shown by UVA
photoelectron-Fenton, followed by electro-Fenton
process.
85.4% removal efficiency with MMO electrode and Zhu et al. (2018)
48.2% with Pt electrode by electrochemical
oxidation method. Complete removal of Atenolol
was achieved by using a combination of
photo-electrolysis process.
Complete abatement of norfloxacin was achieved. da Silva et al. (2019b)
Control of by-products synthesized during the
process needed to be regulated for achieving
higher abatement percentage.
Removal efficiency of more than 90% was Turkay et al. (2018)
observed. The degradation was initiated with the
detachment of OH groups and then lower
molecular weight products were synthesized.
Removal efficiency of 80% was achieved for Shen et al. (2017)
pollutant estriol. Batch 3-D electrode reactor
improved the reaction rate compared to
conventional 2-D electrode reactor.
Boron-doped diamond electrode was found to be Steter et al. (2016)
the most efficient with 89% reduction in total
organic carbon. Pt electrode was found to be the
least efficient for the degradation of
methylparaben.
Removal efficiency of 99.93%. Degradation Zhao et al. (2016)
happened by indirect oxidation under mediation
by OH› .
14
R.Y. Krishnan, S. Manikandan, R. Subbaiya et al. Environmental Technology & Innovation 23 (2021) 101757

found beneficial in pollutant degradation. Also, when wastewater after preliminary treatment methods are subjected to
electrochemical oxidation process, a general increase in efficiency and degradation rate has been observed. Thus, the
integration of AOP with conventional wastewater treatment plants is conceptually viable and thus a closer association
between engineers and chemists could ensure the effective utilization of advanced oxidation methods.

Declaration of competing interest

The authors declare that they have no known competing financial interests or personal relationships that could have
appeared to influence the work reported in this paper.

Acknowledgments

Authors are thankful to the Management and Department of Food Technology, Amal Jyothi College of Engineering,
Kanjirappally, Kottayam, Kerala, India, The Management of Saveetha School of Engineering (SIMATS), Thandalam, Chennai,
Tamil Nadu, India and The Management, Vice-Chancellor, Dean of SMNS and The Head of Biological Sciences, The
Copperbelt University, Kitwe, Zambia for their constant support to complete this review article.

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