1 s2.0 S0048969717309373 Main

Science of the Total Environment 596–597 (2017) 303–320
Contents lists available at ScienceDirect
Science of the Total Environment
journal homepage: www.elsevier.com/locate/scitotenv
Review
Occurrences and removal of pharmaceuticals and personal care products

(PPCPs) in drinking water and water/sewage treatment plants: A review
Yi Yang a, Yong Sik Ok b, Ki-Hyun Kim c, Eilhann E. Kwon d, Yiu Fai Tsang a,⁎
a
Department of Science and Environmental Studies, The Education University of Hong Kong, Tai Po, New Territories, Hong Kong
b
O-Jeong Eco-Resilience Institute (OJERI), Division of Environmental Science and Ecological Engineering, Korea University, Seoul, Republic of Korea
c
Department of Civil and Environmental Engineering, Hanyang University, Seoul 04763, Republic of Korea
d
Department of Environment and Energy, Sejong University, Seoul 05006, Republic of Korea
H I G H L I G H T S G R A P H I C A L A B S T R A C T
• There is a large variation in PPCP remov-

al in STPs and WTPs (−157–100%).
• PPCP removal is dependent on com-
pound characteristics and process-
specific factors.
• Advanced treatment technologies are
effective for PPCP removal.
a r t i c l e i n f o a b s t r a c t
Article history: In recent years, many of micropollutants have been widely detected because of continuous input of pharmaceu-
Received 18 January 2017 ticals and personal care products (PPCPs) into the environment and newly developed state-of-the-art analytical
Received in revised form 5 April 2017 methods. PPCP residues are frequently detected in drinking water sources, sewage treatment plants (STPs), and
Accepted 13 April 2017
water treatment plants (WTPs) due to their universal consumption, low human metabolic capability, and im-
Available online 21 April 2017
proper disposal. When partially metabolized PPCPs are transferred into STPs, they elicit negative effects on bio-
Editor: D. Barcelo logical treatment processes; therefore, conventional STPs are insufficient when it comes to PPCP removal.
Furthermore, the excreted metabolites may become secondary pollutants and can be further modified in receiv-
Keywords: ing water bodies. Several advanced treatment systems, including membrane filtration, granular activated carbon,
Contaminants of emerging concern (CECs) and advanced oxidation processes, have been used for the effective removal of individual PPCPs. This review
Pharmaceuticals covers the occurrence patterns of PPCPs in water environments and the techniques adopted for their treatment
Personal care products in STP/WTP unit processes operating in various countries. The aim of this review is to provide a comprehensive
PPCPs summary of the removal and fate of PPCPs in different treatment facilities as well as the optimum methods for
Removal efficiency
their elimination in STP and WTP systems.
Water quality
© 2017 Elsevier B.V. All rights reserved.
⁎ Corresponding author.
E-mail address: [email protected] (Y.F. Tsang).
http://dx.doi.org/10.1016/j.scitotenv.2017.04.102
0048-9697/© 2017 Elsevier B.V. All rights reserved.
304 Y. Yang et al. / Science of the Total Environment 596–597 (2017) 303–320
Contents
1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 304
1.1. Classification of PPCPs. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 304
1.2. Pathways of PPCPs in the environment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 305
2. Environmental and health risks . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 305
3. Occurrences of PPCPs in water environments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 306
3.1. PPCPs in surface water . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 306
3.2. PPCPs in groundwater. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 306
3.3. PPCPs in STPs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 307
3.3.1. Fates of PPCPs in STPs. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 307
3.3.2. Pharmaceuticals . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 307
3.3.3. Personal care products . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 309
3.4. PPCPs in WTPs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 312
4. Removal of PPCPs in treatment plants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 312
4.1. PPCP removal in STPs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 312
4.2. PPCP removal in WTPs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 313
5. Control strategies for PPCP contamination . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 315
5.1. Membrane filtration . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 315
5.2. Granular activated carbon . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 315
5.3. Advanced oxidation processes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 315
6. Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 316
Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 316
Appendix A. Supplementary data . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 316
References. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 316
1. Introduction degradation products are very limited (Miao et al., 2005; Borova et al.,
2014).The fates and removal mechanisms of PPCPs in STPs and WTPs
In recent decades, pharmaceuticals and personal care products have not been fully understood (Stasinakis et al., 2013; Blair et al.,
(PPCPs) have been recognized as contaminants of emerging concern be- 2015). Thus, numerous analytical methods have been developed to as-
cause of their persistent presence in aquatic environments. The term sess the profiles and occurrence patterns of PPCPs during the last decade
“PPCPs” broadly refers to any product with healthcare or medical pur- (Evgenidou et al., 2015).
poses for humans and/or animals. Interest in the safety issue of PPCPs Several review articles have reported the ecotoxicological effects of
has been steadily increased over the past 30 years (Schumock et al., PPCPs (Brausch and Rand, 2011) and their occurrences in various
2014). PPCPs are known to be released into aquatic environments water bodies, including groundwater (Lapworth et al., 2012), surface
through multiple pathways, including domestic wastewater, hospital water and wastewater (Liu and Wong, 2013), and STPs (Feng et al.,
discharges, improper manufacturer disposal, sewage treatment plants 2013; Evgenidou et al., 2015). However, such studies have generally
(STPs), and water treatment plants (WTPs) (Leung et al., 2012; Liu been limited to single/few treatment plants and the removal perfor-
and Wong, 2013). Compared with domestic sewage, hospital effluents mance of the corresponding unit process. This review initially focuses
generally exhibit higher detection frequencies and concentrations of on the profiles of common PPCPs in both natural and artificial environ-
pharmaceuticals (Kosma et al., 2010; Oliveira et al., 2015). The excreted ments. It is then extended to discuss the performance of PPCP removal
PPCPs may either retain their original concentrations and structures or of different treatment systems employed at each unit process in STPs
be mobilized and converted into other active (or inactive) compounds and WTPs in different regions, and describe the advanced treatment
during their lifespan in aquatic matrices. methods available for effective PPCP removal. Findings from over 200
PPCPs are generally present in surface water, groundwater, drinking studies of 219 STPs and WTPs in the US, Asia, and Europe are summa-
water, and sewage at concentrations of parts-per-trillion (ng/L) to rized and discussed (Tables 2a–4b). Considering that differences in the
parts-per-billion (μg/L) (Dai et al., 2015). However, the removal effi- operational and experimental conditions of studies may influence the
ciency of PPCPs in conventional STPs is low (Behera et al., 2011), be- results, the detailed operating conditions of various STPs and WTPs
cause the most commonly used treatment system in secondary STPs and their relevant experimental information are presented in Supple-
(i.e., activated sludge process (ASP)) is originally designed for the re- mentary materials (Tables S1 and S2).
moval of organic matter (i.e., BOD) and suspended solids to meet the
minimum discharge standard (Hua et al., 2008; Tsang, 2015). STPs 1.1. Classification of PPCPs
have been identified as a primary source of PPCPs in the aquatic envi-
ronment (Focazio et al., 2008; Padhye et al., 2014). Although the con- PPCPs can be classified into multiple groups according to their prop-
centration of PPCPs in sewage influent is relatively low, PPCPs that are erties and purposes. Pharmaceuticals generally include antibiotics, hor-
present as either individual molecules or as complexes may exert con- mones, analgesics, anti-inflammatory drugs, blood lipid regulators, β-
siderably toxic or inhibitory effects on activated sludge bacteria, blockers, and cytostatic drugs. Personal care products (PCPs) include
resulting in deteriorated removal efficiency (Thomaidi et al., 2015, preservatives, bactericides/disinfectants, insect repellents, fragrances,
2016). and sunscreen ultraviolet (UV) filters (Kosma et al., 2010; Liu and
Regulation of PPCPs has been strictly enforced and implemented to Wong, 2013). The typical classification of PPCPs and the representative
minimize their consumptions (Daughton, 2002). However, the use of compounds are summarized in Table 1 (Esplugas et al., 2007; Liu and
these products is unlikely to be restricted because of their beneficial Wong, 2013). To date, N3000 PPCPs have been used for the medical
properties for humans and animals (Jones et al., 2005). Extensive profil- treatment of both humans and animals and for the enhancement of
ing of PPCPs has been pursued in aquatic environments (Boxall et al., their living standards (Muthanna and Plósz, 2008). Numerous drugs
2012). However, data on their metabolites, by-products, and are hydrolyzed or metabolized to form water-stabilized metabolites
Y. Yang et al. / Science of the Total Environment 596–597 (2017) 303–320 305
Table 1 swimming and other recreational activities can contribute to PCP dis-
Typical classes of PPCPs and their representative compounds. charge (Brausch and Rand, 2011).
Typical classes Representative compounds Other PPCP exposure pathways include the disposal of unused med-
A. Pharmaceuticals
icines to landfills, runoff of veterinary medicines from hard surfaces in
A1. Broad-spectrum antibiotics farmyards, disposal of the carcasses of treated animals, and irrigation
1a Levofloxacin using reclaimed water (Fick et al., 2009; Awad et al., 2014). Moreover,
1b Penicillin the management and use practices of PPCPs vary in different regions
A2. Hormones
of the world. Hence, the significance of different exposure pathways
2a 17-β-Estradiol (E2)
2b Estriol (E3) also varies geographically. For example, the connectivity of the popula-
2c Estrone (E1) tion to STPs is limited in several regions of the world. Thus, exposure
A3. Non-steroidal modeling based on a specific region may not be widely applicable.
anti-inflammatory
drugs (NSAIDs)
3a Diclofenac
3b Ibuprofen 2. Environmental and health risks
3c Naproxen
A4. β-blockers The widespread occurrence of PPCPs in receiving water bodies is a
4a Metoprolol
growing concern because of its effects on environmental and human
4b Propranolol
A5. Blood lipid regulators health. PPCPs exist widely in sewage, rivers, lakes, and groundwater.
5a Clofibric acid They can become detrimental to human and animal health because
5b Gemfibrozil their residues can eventually enter and accumulate in the food chain
B. Personal care products through effluent discharge and the reuse of treated sewage and sludge
B1. Preservatives for agricultural applications (Rajapaksha et al., 2014; Vithanage et al.,
6a Parabens 2014). Despite the low concentrations of PPCPs in WTPs, which range
B2. Bactericides/disinfectants between ng/L and μg/L, PPCP residues may have serious adverse health
7a Methyltriclosan
impacts, and human exposure to these chemicals has unknown long-
7b Triclocarban (TCC)
7c Triclosan (TCS) term effects (Boxall et al., 2012).
B3. Insect repellents Many PPCPs rapidly dissipate in the environment, but their exten-
8a N, N-diethyl-m-toluamide (DEET) sive use results in their pseudo-persistence in water environments
B4. Fragrances
and serious ecological impacts on aquatic organisms (Kostich et al.,
9a Galaxolide fragrance (HHCB)
9b Toxalide fragrance (AHTN)
2014). High-frequency detection of PPCPs in STPs, including sewage ef-
B5. Sunscreen UV filters fluent and reclaimed water (Chen et al., 2013), is caused by their univer-
10a 2-Ethyl-hexyl-4-trimethoxycinnamate (EHMC) sal consumption (Liu and Wong, 2013), low human metabolic capability
10b 4-Methyl-benzylidene-camphor (4-MBC) (Borova et al., 2014), improper disposal (Ternes et al., 2004), and biolog-
10c Octyl-methoxycinnamate (OMC)
ically active structures (McClellan and Halden, 2010). PPCPs may be
10d Octyl-triazone (OC)
partially metabolized or incompletely biodegraded in artificial water
matrices. Thus, the excreted metabolites can become secondary pollut-
(Reddersen et al., 2002). In most cases, the concentrations of these me- ants and be further modified in receiving water bodies (Cardinal et al.,
tabolites are significantly lower than the concentration of the original 2014). Several PPCPs are taken up by certain plant species when
drug, as they tend to be more effectively consumed. However, the con- reclaimed water and organic manures from sewage sludge are used.
centrations of some substances, such as pharmaceutical excipients, may The adverse effects of these PPCPs on health and the environment
remain almost unchanged (Hirsch et al., 1999). have been reported previously (Tanoue et al., 2012; Jiang et al., 2013;
Rajapaksha et al., 2015).
1.2. Pathways of PPCPs in the environment PPCP residues have been found in the edible tissues of plants when
bio-solids or manure-amended soils were used or when sewage was
PPCPs can enter the environment through several pathways (Fig. 1), used for irrigation (Rajapaksha et al., 2014). Although most individual
including STPs, industrial services, hospitals, aquaculture facilities, run- PPCPs represent a de minimis risk to human health, the additive effect
off from fields into surface waters, and runoff into soil through animal of PPCPs can potentially be hazardous. The Environmental Working
farming and manure applications (Price et al., 2010; Boxall et al., Group of the United States (EWG, 2008) found 1,4-dioxane, a known
2012; Lambropoulou and Nollet, 2014). Untreated household effluent carcinogen, in 28% of 27,000 PCPs. In addition, they conducted a survey
and treated effluents from industries and hospital services containing of 20 girls aged 14–19 years old. The EWG determined that 16 hazard-
some partially degraded and refractory PPCPs may directly discharge ous chemicals, including synthetic musk, 2-benzenedicarboxylic salt,
into various receiving water bodies without improper treatment. The and Triclosan (TCS), were present in the girls' bodies due to the use of
occurrence of PPCPs in aquatic environments, including sewage, surface cosmetic products. A study by the United States Environmental Protec-
water, groundwater, and drinking water, was reviewed recently by Luo tion Agency (USEPA) found some drug classes of concern in the US
et al. (2014). PPCP residues can also enter the environment through nat- water sources, such as antibiotics, antimicrobials, estrogenic steroids,
ural hydrologic cycle (Petrović et al., 2003; Mompelat et al., 2009). and antiepileptic drugs (EWG, 2009; USEPA, 2009).
Domestic sewage is one of the major sources of PPCPs released into Certain PPCPs can lead to bioaccumulation in fish and other aquatic
the environment. Drugs used by humans or animals can be directly or creatures, which triggers various unexpected interference on them. For
indirectly discharged into the environment. Some non-metabolized or example, chronic exposure to estrogenic pollutants in water can result
dissolved pharmaceutical ingredients (e.g., methotrexate) are excreted in the enlargement of fish livers (Gunnarsson et al., 2009). Furthermore,
from the body via feces and urine (Montforts, 1999; Kim et al., 2011) single and mixed PPCP residues have been found to cause negative re-
and finally discharged into the sewerage systems (Kimura et al., production impacts and histopathological changes in zebrafish (Galus
2007). Personal care products (PCPs), including shampoos, body et al., 2013a, 2013b; Overturf et al., 2015). PPCPs also exhibit adverse cu-
washes, toothpastes, sunscreens, cosmetics, and hand lotions, can be mulative effects on terrestrial and aquatic ecosystems (Hernando et al.,
discharged into sewerage systems and surface water through the daily 2004, 2006). The adverse effects of PPCPs on ecosystems are significant
washing activities of human beings. Additionally, sloughing during to human health because PPCP residues have been detected in our food
Fig. 1. Sources and pathways of PPCPs.

(Modified from Petrović et al., 2003; Mompelat et al., 2009)
chain, including fruits, vegetables, and drinking water (Hernando et al., PPCPs had detection frequencies of 50–100% in Beijing, China, which is
2006; Carmona et al., 2014; Awad et al., 2016). one of the most densely populated cities in the world (Dai et al.,
2015). The median concentrations of the selected PPCPs were up to
3. Occurrences of PPCPs in water environments 4200 ng/L. Wood et al. (2015) reported that the concentrations of anti-
retroviral drugs in South African surface waters were higher than in
3.1. PPCPs in surface water other countries. Kim et al. (2007) investigated the occurrences of 22
pharmaceuticals and 3 PCPs in 3 major rivers receiving effluents from
Effluent from STPs is the predominant pathway through which secondary STPs located in industrialized areas in South Korea. The target
PPCPs enter surface water in the UK (Roberts and Thomas, 2006; PPCPs were found in all of the sampling sites in upstream and down-
Gardner et al., 2012), the US (Spongberg et al., 2011), Italy (Meffe and stream, with detection frequencies from 17% to 53%. The concentrations
de Bustamante, 2014), and Africa (Wood et al., 2015) and accumulate of iopromide and caffeine were comparatively high (20–361 and 10–
in aquatic environments (Luo et al., 2014). Wang et al. (2015) evaluated 194 ng/L, respectively). In addition, several species, including tris(2-
the occurrence of 36 PPCPs in urban river water samples collected from chloroethyl) phosphate (TCEP), iopromide, naproxen, carbamazepine,
Beijing, Changzhou, and Shenzhen in China. The sum of 28 compounds, and caffeine, were frequently observed (N80%) in surface water
including sulfadimethoxine (164 ng/L), sulpiride (77.3 ng/L), atenolol samples.
(52.9 ng/L), and indomethacin (50.9 ng/L), exhibited the highest medi- Analgesic/anti-inflammatory drugs are one of the most common
an concentrations. PPCP residues in sewage because of their high consumption. Moreover,
Overall, antibiotics comprise approximately half of PPCP contamina- these drugs, such as carbamazepine, are frequently detected in surface
tion. The ratio of persistent PPCPs, such as sulpiride and carbamazepine, waters at relatively high concentrations (ng/L–μg/L) (Ashton et al.,
is useful for tracing contamination sources in rivers. Spongberg et al. 2004; Hernando et al., 2006). These findings confirm that these stable
(2011) analyzed 34 PPCPs present in 86 individual water samples col- PPCPs are difficult to remove in conventional STPs (Ashton et al.,
lected from surface water and coastal locations in Costa Rica. The sam- 2004; Ziylan and Ince, 2011). Therefore, they are expected to be present
pling sites included areas that received both treated and untreated in similar concentrations in the influent, effluent, and downstream of
sewage, and surface runoff. The four most frequently detected PPCPs the receiving water body (Feng et al., 2013).
were doxycycline (77%), sulfadimethoxine (43%), salicylic acid (41%),
and TCS (34%). The PPCPs detected at higher concentrations were doxy- 3.2. PPCPs in groundwater
cycline (74 μg/L), ibuprofen (37 μg/L), gemfibrozil (17 μg/L), acetamin-
ophen (13 μg/L), and ketoprofen (10 μg/L). The frequencies and concentrations of PPCPs are lower in groundwa-
β-Blockers are used for the treatment of bronchodilation, vasodila- ter than in surface water (Vulliet and Cren-Olivé, 2011). Of the 52 target
tion, and the relaxation of visceral smooth muscles. They were found PPCPs, erythromycin, sulfamethoxazole, fluconazole, salicylic acid,
to occur frequently in the surface waters of Switzerland, with concen- methyl paraben, TCS, and bisphenol were most frequently detected, at
trations of up to ng/L (Alder et al., 2010). Most commonly found ng/L levels, in 70 groundwater samples collected nearby 2 multiple
landfill sites in Guangzhou, China. Compared with groundwater, reser- inefficient in removing PPCPs because some PPCPs are specifically de-
voirs were significantly more contaminated, exhibiting both higher designed to achieve a biological response or are antimicrobial agents
tection frequencies and concentrations (Peng et al., 2014). Lapworth (McClellan and Halden, 2010; Parolini et al., 2013).
et al. (2012) discussed the five most commonly reported PPCPs in Most work has focused on investigating the occurrences and fates of
groundwater, based on studies conducted in 14 countries across PPCPs in sewage and STPs, and their elimination efficiency (Luo et al.,
Europe, the Middle East, North America, and Asia. The mean concentra- 2014; Evgenidou et al., 2015). However, in-depth studies of the mass
tions of carbamazepine, sulfamethoxazole, ibuprofen, caffeine, and balance and removal mechanisms of PPCPs (e.g., biotransformation,
diclofenac were 5 μg/L (n = 23), 252 ng/L (n = 15), 1.5 μg/L (n = sedimentation, adsorption, biodegradation, volatilization, and hydroly-
14), 9.8 μg/L (n = 14), and 121 ng/L (n = 11), respectively. In ground- sis, etc.) in STPs, and their inhibitory effects on biological processes
water, PPCPs do not show significant trends or seasonal variations, (e.g., ASP and nutrient removal) have not been fully established.
whereas the PPCP concentrations in reservoirs are higher during spring (Carballa et al., 2007; Gao et al., 2012; Stasinakis et al., 2013; Blair
than in other seasons. Lin et al. (2015) investigated the occurrences of et al., 2015). Therefore, it is necessary to further evaluate the effects of
contaminants of emerging concern and the correlation of their presence PPCPs on the performance of different treatment methods for different
in groundwater with possible pollution sources in Taiwan. These au- purposes (e.g., ultimate discharge or water reuse).
thors detected most of the 50 target pharmaceuticals and perfluorinated
chemicals at the ng/L level, except for 17α-ethinylestradiol, sulfameth- 3.3.2. Pharmaceuticals
oxazole, and acetaminophen (i.e., 1822, 1820, and 1036 ng/L, respec- Given the volume of prescription, toxicity, and their presence in the
tively). The results indicated that PPCPs with high detection environment, antibiotics, hormones, non-steroidal anti-inflammatory
frequencies and their corresponding concentrations in groundwater drugs (NSAIDs), β-blockers, blood lipid regulators, antiepileptics, anal-
were consistent with the results obtained in other countries. Antibiotics, gesics and anti-inflammatories, and antidepressants are the most stud-
anti-inflammatories and analgesics, lipid regulators, and N, N-diethyl- ied pharmaceutical groups (Miege et al., 2009; Jelić et al., 2012).
m-toluamide (DEET) were frequently detected in groundwater (Sui Table 2a summarizes the influent and effluent concentrations of com-
et al., 2015). Sulfonamides are one of the most extensively studied clas- mon pharmaceuticals detected in STPs in different countries.
ses of antibiotics and were found at high concentrations in several stud- Antibiotics are commonly used pharmaceuticals that protect
ies (García-Galán et al., 2010; Gottschall et al., 2012; Meffe and de humans and animals against diseases and infection caused by bacteria.
Bustamante, 2014). Van Boeckel et al. (2015) predicted that the global consumption of anti-
The most commonly detected anti-inflammatories and analgesics in biotics in livestock would rise by 67%. Many antibiotics are released into
groundwater include ibuprofen, diclofenac, salicylic acid, carbamaze- the environment even without being metabolized. Sulfonamides,
pine, and paracetamol because they are widely and frequently con- fluoroquinolones, and macrolides are persistent in sewage (Huang
sumed. Several pharmaceuticals and their metabolites, such as et al., 2011; Jelić et al., 2012). Among these antibiotics, sulfamethoxa-
diclofenac, ibuprofen, and ketoprofen, have been found at concentra- zole, ciprofloxacin, azithromycin, and tylosin are the most frequently
tions of up to mg/L. Salicylic acid was found with a detection frequency detected species in STP effluent (Huang et al., 2011). Trimethoprim
of 98% in Guangzhou, China; its concentration ranged from 43.7 to (TMP) and tetracycline (TET) exhibit high persistence in both influent
2014.7 ng/L (Peng et al., 2014). Loos et al. (2010) reported that carba- and effluent, indicating low removal efficiencies in STPs (Brown et al.,
mazepine, which is a commonly used analgesic, was detected in 42% 2006; Watkinson et al., 2007; Leung et al., 2012).
of groundwater samples collected from 164 locations in 23 European β-Blockers are common pharmaceuticals used for the treatment of
countries, with a maximum concentration of 390 ng/L. The detection cardiovascular diseases, such as angina and hypertension, and were ob-
frequencies of lipid regulators and metabolites in groundwater, such served in European waters in 1995 (Ternes, 1998). Subgroups, including
as bezafibrate (N.D.), gemfibrozil (N.D.), and clofibric acid (3%), were atenolol, propranolol, and metoprolol, were also detected in the influ-
lower than those of antibiotics and anti-inflammatories (Peng et al., ents and effluents of STPs, demonstrating that these pharmaceuticals
2014). Results of a national survey of pharmaceuticals and organic pol- are not always removed effectively by STPs (Lee et al., 2007; Vieno N.
lutants in the US indicated that DEET (35%) and sulfamethoxazole (23%) et al., 2007). For instance, the influent and effluent concentrations of
were the most frequently detected PPCPs in 47 groundwaters across 18 metoprolol in Finnish STPs were 1060 and 755 ng/L, respectively
states (Barnes et al., 2008). Holm et al. (1995) indicated that PPCP con- (Vieno N. et al., 2007). In addition, a negative growth in the concentra-
tamination and its subsequent ecological risks could be a serious con- tion of propranolol was observed in UK STPs from 60–638 ng/L to 93–
cern for groundwater near landfill sites. 288 ng/L in influent (Kasprzyk-Hordern et al., 2008, 2009; Gardner
et al., 2012, 2013).
3.3. PPCPs in STPs Hormones are a class of signaling molecules produced by glands in
multicellular organisms. They are transported by the circulatory system
3.3.1. Fates of PPCPs in STPs to distant target organs and regulate physiology and behavior. Contam-
PPCPs are mainly released into aquatic environments through STPs ination by the natural estrogens, estrone (E1), 17β-estradiol (E2), and
before they reach the receiving soil, surface water, sediment, and estriol (E3), and the synthetic contraceptive 17α-ethinylestradiol
groundwater (Leung et al., 2012; Liu and Wong, 2013). They are fre- (EE2) is of great concern (Desbrow et al., 1998). The concentrations of
quently detected at various concentrations in influent, effluent, these species are relatively low compared with previous studies. For in-
reclaimed water, and receiving water bodies in Hong Kong (Li and stance, the influent concentrations of E1, E2, E3, progesterone, and tes-
Zhang, 2010), South China (Liu and Wong, 2013; Yin et al., 2012), tosterone were 41, 8.6, 13, 10, and 7 ng/L, respectively, in Czech
Europe (Kosma et al., 2010; Jiang et al., 2013) and other regions of the Republic. The corresponding effluent concentrations were b2.5, b1,
world (Subedi et al., 2015a; Dotan et al., 2016; Wang and Kannan, b10, b0.5, and b0.5 ng/L, respectively (Vymazal et al., 2015). These re-
2016). The potential fates of PPCPs in STPs (e.g., biodegradation/bio- sults are similar to those obtained by Mailler et al. (2015). Biodegrada-
transformation, retention of solid/sludge, and release into receiving tion, discharge into the aquatic environment with secondary effluent,
water bodies) are dependent on their original chemical structures and and discharge with excess sludge are three possible elimination path-
the associated metabolites and/or transformation products (Jiang ways for hormones from different treatment units of STPs (Belhaj
et al., 2013; Maia et al., 2014). Typical PPCP removal processes include et al., 2015). In addition, biodeconjugation can be an effective method
ASP, tertiary treatment with nutrient removal, membrane bioreactors, to remove natural hormones in STPs (Liu Z.H. et al., 2015).
and advanced oxidation processes (AOPs) (Miao et al., 2005; Tsang NSAIDs are a pharmaceutical class that includes analgesic (pain-kill-
et al., 2007; Zhao et al., 2014). However, conventional STPs are usually ing) and antipyretic (fever-reducing) drugs. Acetaminophen,
Table 2a
The concentrations and removal (%) of selected pharmaceuticals in conventional STPs in different countries.
Order Representative compounds Influent (ng/L) Final effluent (ng/L) Overall removal (%) Sludge (ng/kg) Location References
A. Antibiotics
1a Amoxicillin (AMOX) ND ND NA Hong Kong, Stonecutters Leung et al. (2012)
261 ± 3 66 ± 2 74 Hong Kong, Tai Po Leung et al. (2012)
ND ND NA Hong Kong, Sha Tin Leung et al. (2012)
1b Ampicillin ND-1805 ND-498 72 Greece, Volos Papageorgiou et al. (2016)
1c Cefalexin (CFX) ND ND NA Hong Kong, Stonecutters Leung et al. (2012)
ND ND NA Hong Kong, Tai Po Leung et al. (2012)
40 ± 5 ND N90 Hong Kong, Sha Tin Leung et al. (2012)
1d Chloramphenicol (CAP) 206 ± 56 234 ± 63 −14 Hong Kong, Stonecutters Leung et al. (2012)
11 ND Spain, Valencia Carmona et al. (2014)
28 ± 3 3.3 ± 0.6 88 Hong Kong, Tai Po Leung et al. (2012)
109 ± 53 ND N99 Hong Kong, Sha Tin Leung et al. (2012)
1e Ciprofloxacin 67 NA USA (20 states) Kostich et al. (2014)
1f ERY-H2O 460 ± 224 455 ± 194 1 Hong Kong, Stonecutters Leung et al. (2012)
707 ± 35 708 ± 274 0 Hong Kong, Sha Tin Leung et al. (2012)
1g Erythromycin (ERY) ND-320 ND Greece, Volos Papageorgiou et al. (2016)
1h Levofloxacin 180 10 50–80 210 UK (160 STPs) Gardner et al. (2012, 2013)
1i Norfloxacin (NOR) 680 ± 181 364 ± 159 46 Hong Kong, Stonecutters Leung et al. (2012)
48 ± 19 33 31 Hong Kong, Tai Po Leung et al. (2012)
275 ± 11 77 ± 0.4 72 Hong Kong, Sha Tin Leung et al. (2012)
160 USA (20 states) Kostich et al. (2014)
1j Ofloxacin (OFX) 1020 ± 243 980 ± 240 4 Hong Kong, Stonecutters Leung et al. (2012)
275 ± 11 707 ± 35 −157 Hong Kong, Sha Tin Leung et al. (2012)
1k Roxithromycin (ROX) 120 120 0 Hong Kong, Stonecutters Leung et al. (2012)
ND ND NA Hong Kong, Tai Po Leung et al. (2012)
126 ± 0.4 142 ± 5 −13 Hong Kong, Sha Tin Leung et al. (2012)
1l Sulfamethazine (SMX) 110 ± 45 110 ± 36 0 Hong Kong, Stonecutters Leung et al. (2012)
39 ± 0.7 8± 3 79 Hong Kong, Sha Tin Leung et al. (2012)
ND-507 ND-80 84 Greece, Volos Papageorgiou et al. (2016)
12 USA (20 cities) Kostich et al. (2014)
1m Tetracycline (TET) 257 ± 176 152 ± 59 44 Hong Kong, Stonecutters Leung et al. (2012)
77 ± 24 ND N90 Hong Kong, Tai Po Leung et al. (2012)
1n Trimethoprim (TMP) 95 ± 23 91 ± 28 4 Hong Kong, Stonecutters Leung et al. (2012)
B. Antiepileptic drugs
2a Carbamazepine 97 NA USA (20 cities) Kostich et al. (2014)
15,780 7570 52 Spain, Murcia Fernández-López et al. (2016)
C. Blood lipid regulators

3a Gemfibrozil 420 NA USA (20 cities) Kostich et al. (2014)
D. β-Blockers
4a Propranolol 60–638 93–388 −50–44 170 UK (162 STPs); Gardner et al. (2012, 2013)
UK, South Wales
E. Hormones
5a Estrone (E1) 7 9 −28 France Mailler et al. (2015)
41 b2.5 N94 Czech Republic Vymazal et al. (2015)
5b 17β-Estradiol (E2) 1.1–1.2 USA Belhaj et al. (2015)
8.6 b1 N88 Czech Republic Vymazal et al. (2015)
Estriol (E3) 13 b10 N23 Czech Republic Vymazal et al. (2015)
F. NSAIDs
6a Acetaminophen 300 NA USA (20 cities) Kostich et al. (2014)
6b Diclofenac 1660 430 74 Spain, Murcia Fernández-López et al. (2016)
400–1500 NA Spain, Catalonia Jelić et al. (2011)
6c Ibuprofen 1681–33,764 143–4239 N80 380 UK, Bath Petrie et al. (2015)
460 NA USA (20 cities) Kostich et al. (2014)
4374 ND N99 Spain, Valencia Carmona et al. (2014)
2800 720 72 Spain, Murcia Fernández-López et al. (2016)
1100–2300 400–1000 64-56 Spain, Catalonia Jelić et al. (2011)
6d Naproxen 1180 190 84 Spain, Murcia Fernández-López et al. (2016)
4200–7200 NA Spain, Catalonia Jelić et al. (2011)
2399 102 N90 Spain, Valencia Carmona et al. (2014)
ND = not detectable; NA = not available.

Table 2b
The concentrations and removal (%) of selected PCPs in conventional STPs in different countries.
Order Representative compounds Influent Final effluent Overall removal Sludge Location References
(ng/L) (ng/L) (%) (ng/kg)
A. Bactericides/disinfectants
1a Triclosan (TCS) 892 202 77 645 India (2 states) Subedi et al. (2015a)
2300 48 N90 USA, California Yu et al. (2013)
547 112 79 Korea, Ulsan Behera et al. (2011)
300 NA 55 USA Blair et al. (2015)
1b Triclocarban (TCC) 1150 49 N80 5570 India (2 states) Subedi et al. (2015a)
540 NA 11 USA Blair et al. (2015)
B. Fragrances
2a Calaxilid fragrance (HHCB) 2560–4520 NA 61–N99 Korea, Busan Lee et al. (2010)
2b Toxalide fragrance (AHTN) 550–1210 NA Korea, Busan Lee et al. (2010)
C. Insect repellents
3a DEET 600–1200 60–624 69 ± 21 China, Beijing Sui et al. (2010)
66 40 40 China, Shanghai Wang et al. (2014)
D. Preservatives
4a Butylparaben (BuP) 15–27 3 N80 China, Guangzhou Yu et al. (2011)
160–170 1 N99 China, Guangzhou Yu et al. (2011)
4b Methylparaben (MeP) 290–10,000 6–50 N90 Spain (northwest) González-Mariño et al. (2011)
334 11 96 Spain, Valencia Carmona et al. (2014)
36.8; 97.9 0.14; 0.14 99.7; 99 41.6; 58.5 New York, USA (2 STPs) Wang et al., (2016)
4c Propylparaben (PrP) 520–2800 2–210 N90 Spain (northwest) González-Mariño et al. (2011)
1630 b5 99 Spain, Valencia Carmona et al. (2014)
E. Sunscreen UV filters
5a 4-Methyl-benzilidine-camphor (4MBC) 169 43 12 (n = 60) 49 Hong Kong (5 regions) Tsui et al. (2014)
5b 2-Ethyl-hexyl-4-trimethoxycinnamate (EHMC) 462 150 93 (n = 60) 68 Hong Kong (5 regions) Tsui et al. (2014)
309 126 59 Hong Kong (5 regions) Tsui et al. (2014)
601 347 42 Hong Kong (5 regions) Tsui et al. (2014)
5c Butyl methoxydibenzoylmethane (BMDM) 289 147 49 Hong Kong (5 regions) Tsui et al. (2014)
5d Ethylhexyl salicylate (EHS) 93 8 91 Hong Kong (5 regions) Tsui et al. (2014)
5e Homosalate (HMS) 151 31 79 Hong Kong (5 regions) Tsui et al. (2014)
5f Isoamyl p-methoxycinnamate (IAMC) 43 24 44 Hong Kong (5 regions) Tsui et al. (2014)
5g Octyl dimethyl-p-aminobenzoic acid (ODPABA) 138 56 17 Hong Kong (5 regions) Tsui et al. (2014)
5h Octocrylene (OC) 8 0 N99 Hong Kong (5 regions) Tsui et al. (2014)
5i Oxycodone (OXB) ND 41.2 1.53 India (2 states) Subedi et al. (2015a)
ND = not detectable; NA = not available.
diclofenac, ibuprofen, and naproxen are prominent NSAIDs available in studies (Miege et al., 2009; Jelić et al., 2011, 2012; Gao et al., 2012;
most countries (Paxeus, 2004; Okuda et al., 2008; Zhang et al., 2008). Gracia-Lor et al., 2012; Kosma et al., 2014).
Previous studies determined relatively high concentrations of acet-
aminophen (up to 6000 ng/L) in different countries (Jim et al., 2006;
Roberts and Thomas, 2006; Kostich et al., 2014). Diclofenac, ibuprofen, 3.3.3. Personal care products
and naproxen showed relatively low concentrations but their removal PCPs typically refer to products used for the enhancement of living
(i.e., from 40% to 80%) was also found to be ineffective standards, including preservatives (e.g., parabens), disinfectants
(Kasprzyk-Hordern et al., 2008, 2009; Jelić et al., 2011; Carmona et al., (e.g., TCS), insect repellents (e.g., DEET), fragrances (e.g., musks), and
2014; Fernández-López et al., 2016; Papageorgiou et al., 2016). As for sunscreen UV filters (e.g., 4-methyl-benzylidene-camphor (4-MBC)).
hormones, biodegradation/biotransformation is an effective mechanism To date, many studies have monitored the presence of PCPs in STPs;
in removing NSAIDs (Samaras et al., 2013). Other pharmaceuticals, in- however, information on the effects of PCPs on the operation of waste-
cluding antiepileptic drugs and blood lipid regulators, have also been water treatment processes is still lacking (Zhou et al., 2009; Lee et al.,
detected in sewage at relatively low concentrations (Roberts et al., 2010). Table 2b summarizes the influent and effluent concentrations
2006; Kostich et al., 2014). of common PCPs detected in STPs in different countries.
The concentration of pharmaceuticals in water environments varies Parabens are esters of para-hydroxybenzoic acid, containing either
from different regions and their properties significantly affect treatment an alkyl or benzyl group. They are widely used as preservatives in cos-
performance. Carmona et al. (2014) investigated the occurrences of 21 metics, foodstuffs, and pharmaceuticals (Guo and Kannan, 2013; Li
pharmaceuticals in 3 STPs in Spain. Ibuprofen, tetrahydrocannabinol, et al., 2015). Methylparaben (MeP) and propylparaben (PrP) are the
and naproxen dominated in the STP influents, with concentrations of most abundant parabens in STP influents, with concentrations of up to
4374, 2591, and 2399 ng/L, respectively (n = 21). Average removal ef- 30 μg/L and 20 μg/L, respectively (Kasprzyk-Hordern et al., 2008;
ficiency higher than 90% can be achieved in most pharmaceuticals. González-Mariño et al., 2011; Carmona et al., 2014). As they are readily
However, 11 out of 21 tested pharmaceuticals, including tetrahydrocan- biodegradable under aerobic conditions and are effectively removed in
nabinol, triclocarban, gemfibrozil, and diclofenac, were still detected in ASP, the concentrations of parabens in effluents are generally on the
the final effluents that are exceeding the regulation standard in these order of several to several tens of ng/L (Hernández Leal et al., 2010).
STPs. Moreover, some pharmaceuticals, such as diclofenac, flufenamic Daily (Carmona et al., 2014) and seasonal (Pedrouzo et al., 2009) varia-
acid, and gemfibrozil, consistently exhibited higher concentrations in tions in the concentrations of parabens in raw sewage are always ob-
effluents than in the corresponding influents. This may be attributed served because of daily consumption patterns and their widespread
to the deconjugation of metabolites, transformation products from hy- use as preservatives. These variations may lead to an underestimation
drolysis, and desorption from suspended solids/sludge during the treat- of paraben concentrations in STPs when using time-composite sampling
ment processes. These findings were in accordance with those of other methods (Guo and Kannan, 2013).
TCS is a bactericide, commonly used in healthcare products, such with TCS, there is a critical lack of information regarding triclocarban
as cosmetics, deodorants, mouth rinses, shampoos, skin-care lotions, (TCC) in STPs.
soaps, and toothpastes, at concentrations of 0.1–0.3% (w/w) DEET is the most commonly used active ingredient in insect repel-
(Thompson, 2005). TCS is frequently detected in STP influents and lents and is persistent in the aquatic environment. Although DEET has
effluents in various countries, at concentrations of 0.2–16.6 μg/L been detected globally in STPs, its concentrations in influents and efflu-
and 0.08–2.7 μg/L, respectively (McAvoy et al., 2002; Behera et al., ents are relatively low. The level of DEET is significantly decreased in
2011; Yu et al., 2013; Subedi et al., 2015a). Dissociated TCS can be winter due to reduced consumption (Knepper, 2004; Costanzo et al.,
easily decomposed under sunlight, with a half-life of less than 1 h; 2007; Sui et al., 2010; Wang et al., 2014). Brausch and Rand, (2011) re-
however, non-dissociated TCS and methyl TCS are relatively stable ported that DEET was found in 95% of analyzed samples, with a median
to photo-degradation. Approximately half of TCS is converted into concentration of approximately 0.2 μg/L. However, DEET may not accu-
unknown metabolites and/or transformation products, or strongly mulate in aquatic organisms as indicated by its low bioconcentration
bound residues (e.g., methyl TCS) through biological methylation factor (Glassmeyer et al., 2005).
and finally released into water environments through effluent dis- Fragrances have been a widely investigated group of PCPs in STPs.
charge (Lindström et al., 2002; Bester, 2007). However, compared Synthetic musks, namely nitro musks (e.g., musk ketone (MK) and
Table 3a
The concentrations and removal (%) of selected pharmaceuticals in conventional WTPs in different countries.
Order Representative Raw water Treated water Overall removal Mineral waters Tap waters Location References
compounds (ng/L) (ng/L) (%) (ng/L) (ng/L)
A. Antibiotics
1a Clarithromycin 40.1–54.4 ND N99 Spain (Northeast) Boleda et al. (2011)
1b Chloramphenicol 1 2 Spain, Valencia Carmona et al. (2014)
1c Erythromycin 21–33 1.3–2.0 N90 Spain (Northeast) Boleda et al. (2011)
1d Sulfamethoxazole 57–149 ND N99 Spain (Northeast) Boleda et al. (2011)
0.41 NA 0.37 USA, New York Subedi et al. (2015b)
4 ND N99 France (8 WTPs) Vulliet et al. (2011)
1e Sulfadimethoxine ND-8.3 ND N99 Spain (Northeast) Boleda et al. (2011)
B. Antiepileptic drugs
2a Carbamazepine 144–215 1.0–1.4 N99 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
43.2 France, Marseilles Togola and Budzinski (2008)
33 8 75 France (8 WTPs) Vulliet et al. (2011)
C. Analgesics and anti-inflammatory drugs

3b Acetylsalicylic acid 21–54 b0.1 N99 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
3c Diclofenac 9 ND N99 France (8 WTPs) Vulliet et al. (2011)
3d Ibuprofen 12 39 Spain, Valencia Carmona et al. (2014)
6.6 1.3 80 France (8 WTPs) Vulliet et al. (2011)
D. Blood lipid regulators

4a Clofibric acid 11.5–20 ND N99 Spain (Northeast) Boleda et al. (2011)
68 b0.1 N99 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
4b Gemfibrozil 187–326 ND N99 Spain (Northeast) Boleda et al. (2011)
E. β-Blockers
5a Metoprolol 2 ND N99 France (8 WTPs) Vulliet et al. (2011)
F. Hormones
7a Estrone (E1) 77–120 b0.15 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
7b 17-β-estradiol (E2) 35–101 b0.15 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
7c Ethinylestradiol (EE2) 10–97 b0.2 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
G. Non-steroidal anti-inflammatory drugs (NSAIDs)

8a Acetaminophen 163–260 3–16 Spain (Northeast) Boleda et al. (2011)
210 France, Marseilles Togola and Budzinski (2008)
7–37.1 ND-6.4 N90 China, Taihu Lin et al. (2016)
8b Diclofenac 25 18 Spain, Valencia Carmona et al. (2014)
210–316 45–68 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
8c Ibuprofen 12 39 Spain, Valencia Carmona et al. (2014)
81–230 ND Spain (Northeast) Boleda et al. (2011)
257–357 74–102 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
8d Ketoprofen 133–250 20–37 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
3 France, Marseilles Togola and Budzinski (2008)
8e Naproxen 0.9 ND USA (17 WTPs) Benotti et al. (2008)
3.1 ND France (8 WTPs) Vulliet et al. (2011)
99–152 ND Spain (Northeast) Boleda et al. (2011)
71–321 0.5–2.4 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
25 11 Spain, Valencia Carmona et al. (2014)
H. Additional pharmaceuticals
9a Florfenicol 24–111 b0.04 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
9b Flunixin 69–145 b0.03 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
9c Phenylbutazone 67–98 b0.15 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
9d pyrimethamine 21–57 b0.15 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
NA = not available; ND = not detectable.

Table 3b
The concentrations and removal (%) of selected PCPs in conventional WTPs in different countries.
Order Representative Raw water Treated water Overall removal Mineral waters Tap waters Location References
compounds (ng/L) (ng/L) (%) (ng/L) (ng/L)
A. Parabens
1a Butylparaben 36 28 Spain, Valencia Carmona et al. (2014)
1b Ethylparaben 2 ND Spain, Valencia Carmona et al. (2014)
1c Methylparaben 40 12 Spain, Valencia Carmona et al. (2014)
1d Propylparaben 23 9 Spain, Valencia Carmona et al. (2014)
1e Methyltriclosan 74 ND N99 China (polit) Zhao et al. (2014)
B. Bactericides/disinfectants
2a Triclosan (TCS) 4 ND Spain, Valencia Carmona et al. (2014)
ND ND USA, New York Subedi et al. (2015b)
3 ND N99 USA (17 WTPs) Benotti et al. (2008)
74–102 b0.1 N99 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
1230 100 92 Israel and Palestine Dotan et al. (2016)
2b Triclocarban (TCC) 12 13 Spain, Valencia Carmona et al. (2014)
7.18 5.4 USA, New York Subedi et al. (2015b)
C. Insect repellents
3a DEET 85 49 42 USA (17 WTPs) Benotti et al. (2008)
19.8–78.4 ND N99 China, Taihu Lin et al. (2016)
D. Sunscreen UV filters
4a Oxybenzone 19.4 1.39 USA, New York Subedi et al. (2015b)
musk xylene (MX)) and polycyclic musks (e.g., HHCB and AHTN), are based recreational activities and effluent discharge. Several studies con-
the most frequently used fragrance ingredients in consumer products, ducted in Switzerland found that the concentration profiles of UV filters
including deodorants, soaps, and detergents (Daughton and Ternes, in STP influents were similar with the order of EHMC N MBC; BP-3 N OC.
1999). Among these musks, HHCB and AHTN are regularly detected in UV filters were also detected in the effluents of all of the tested STPs, but
STP influents with relatively high concentrations of 0.043–13.7 μg/L. their concentrations were comparatively low and their profiles were
The detected levels of polycyclic musks exceed their toxicity limits, indi- significantly different (4-MBC N BP-3 N EHMC; OC) (Poiger et al.,
cating the importance of the removal of these fragrances in wastewater 2004; Balmer et al., 2005). A recent study found that the occurrences
treatment processes. Sun et al. (2014) investigated the occurrences and and removal of 12 widely used UV filters from five STPs in Hong Kong
statistical distribution of HHCB and AHTN in 40 STPs in the US. The mean and South China (Tsui et al., 2014). 2,4-Dihydroxybenzophenone (BP-
concentrations of HHCB and AHTN were 1.86 μg/L (0.45–4.79 μg/L) and 1), benzophenone-3 (BP-3), benzophenone-4 (BP-4), and EHMC were
0.18 μg/L (0.05–0.44 μg/L), respectively, across the US. Brausch and detected with frequencies over 80% in the STP influents and effluents.
Rand (2011) found that MK and MX were present in 83–90% of STP ef- The overall removal efficiency of these UV filters was around 50%. In ad-
fluents at comparatively low concentrations. dition, higher concentrations of UV-filters are generally found in wet
UV filters are commonly used in sunscreens, lotions, and cosmetics and summer seasons (Bester, 2007; Kasprzyk-Hordern et al., 2008;
to protect skin against UV radiation. Their increased usage is the result Tsui et al., 2014).
of growing concerns regarding the adverse health effects of UV radia-
tion. UV filters are released into water environments through water-
Fig. 2. a Flow diagram of conventional STPs (modified from Carballa et al., 2004; Metcalf and Eddy, 2014). b Flow diagram of conventional WTPs (modified from Metcalf and Eddy, 2014;
Stackelberg et al., 2004).
Table 4a
The removal (%) of PPCPs in different unit processes in STPs in different countries.
Order Representative Preliminary Primary Secondary Tertiary Location References

compounds treatment (%) treatment (%) treatment (%) treatment (%)
1a Triclosan (TCS) 77 18 Greece, Agrinio Stamatis and Konstantinou (2013)
42 97 Australia, Canberra Roberts et al. (2016)
−20 75 −25 Korea, Ulsan Behera et al. (2011)
B. Broad-spectrum antibiotics
2a Acetaminophen (AMP) 6 8 N99 N99 USA, Michigan Gao et al. (2012)
2b Carbamazepine (CBZ) −19 −42 −41 USA, Michigan Gao et al. (2012)
−36 22 NA Australia, Canberra Roberts et al. (2016)
2c Codeine 53–83.2 China (Southern and Northern) Zhao et al. (2013)
2d Chlortetracycline (CTC) 5 32 N99 N99 USA, Michigan Gao et al. (2012)
2e Doxycycline (DOC) 35 40 64 50 USA, Michigan Gao et al. (2012)
2f Lincomycin (LCM) −31 2 40 USA, Michigan Gao et al. (2012)
2g Oxytetracycline (OTC) 28 8 64 39 USA, Michigan Gao et al. (2012)
2h Sulfadiazine (SDZ) 1 2 22 27 USA, Michigan Gao et al. (2012)
2i Sulfamerazine (SMR) N99 NA N99 N99 USA, Michigan Gao et al. (2012)
2j Sulfamethoxazole (SMX) 18 17 69 89 USA, Michigan Gao et al. (2012)
2k Sulpiride (SP) 8 −33 5 China, Shanghai Wang et al. (2014)
2l Tetracycline (TC) 59 50 N99 N99 USA, Michigan Gao et al. (2012)
2m Trimethoprim (TMP) 12 10 9 China, Shanghai Wang et al. (2014)
C. Hormones
3a Estradiol NA 93 ± 14 N99 Korea, Ulsan Behera et al. (2011)
3b Estriol 45 90 ± 11 N99 Korea, Ulsan Behera et al. (2011)
D. Insect repellents
4a DEET −22 43 15 China, Shanghai Wang et al. (2014)
5 93 92 China, Beijing Gao et al. (2016)
E. Nonsteroidal anti-inflammatory drugs (NSAIDs)

5a Ibuprofen 90 25 Greece Stamatis and Konstantinou (2013)
F. Preservatives
6a Methylparaben 71.6 China (Southern and Northern) Zhao et al. (2013)
3.4. PPCPs in WTPs low concentrations of PPCPs (b100 ng/L) were found in tap and mineral
waters, and parabens were present at relatively high concentrations in
To date, most studies have reported on the monitoring of PPCPs in WTPs in Valencia, Spain. In tap water samples, naproxen and salicylic
water and wastewater treatment systems. Additionally, considerably acid were frequently detected, while diclofenac, PrP, and ibuprofen ex-
more research has focused on STPs than on WTPs. Considering that hibited the highest mean concentrations (1–39 ng/L). Methylparaben
most WTPs do not have the capabilities required for routine PPCP anal- was detected in mineral water, at a concentration of 40 ng/L. Liu J.
ysis, PPCPs are possibly present in drinking water at the concentrations et al. (2015) studied the fates and removal of six antibiotics in an
with unknown effects to humans (Padhye et al., 2014). However, the industrial-scale WTP equipped with advanced treatment processes in
fates and removal of PPCPs in WTPs and the occurrences of PPCPs in China. The influent and effluent concentrations of these antibiotics
tap water have not been extensively studied because of analytical diffi- ranged from 1 to 43 ng/L and from below the detection limit (BDL) to
culties (Mompelat et al., 2009). Tables 3a and 3b summarize the influent 6 ng/L, respectively. Currently, the information of occurrences and
and effluent concentrations of selected pharmaceuticals and PCPs, re- fates of PCPs in WTPs is very limited compared with equivalent data re-
spectively, in WTPs in different countries. In general, raw water is not garding pharmaceuticals.
highly polluted by PPCPs (Kim et al., 2007), while the concentrations
of PPCPs in treated water are typically at trace levels or below their de-
tection limits (Huerta-Fontela et al., 2011; Vulliet et al., 2011; Vulliet 4. Removal of PPCPs in treatment plants
and Cren-Olivé, 2011).
Kim et al. (2007) investigated the presence of 14 pharmaceuticals 4.1. PPCP removal in STPs
and 3 PCPs in two full-scale conventional WTPs in South Korea. In the
Seoul WTP, only 6 target PPCPs were detected in raw water, at low con- Generally, conventional sewage treatment processes (Fig. 2), includ-
centrations (i.e., 2–143 ng/L). Moreover, their concentrations were ing screening, degritting, primary sedimentation, aeration tanks, and
below the detection limits in treated water (either b1 or 10 ng/L). How- final sedimentation, are ineffective in eliminating PPCPs (Carballa
ever, in Gwangju, only oxybenzone (sunscreen) was detected, at a very et al., 2004). Minus implies that the concentration of target PPCPs in-
low level (i.e., 1.2 ng/L). Mompelat et al. (2009) summarized the occur- creases after wastewater treatment processes. Removal of PPCPs in
rence of 90 PPCPs in reservoirs, treated water, and tap water in STPs is a complicated process and depends on the chemical and biolog-
Germany, Italy, Canada, France, Finland, and the US. Among 90 target ical properties of pollutants, such as hydrophilicity, solubility
PPCPs, bezafibrate, clofibric acid, diclofenac, gemfibrozil, ibuprofen, (Evgenidou et al., 2015), volatility, biodegradability (Jones et al.,
and TCS were detected, at concentrations of 2.5–734 ng/L. Vulliet et al. 2005), and the adsorption capability of the activated sludge (Liu and
(2011) found that 25 PPCPs were present in drinking water. Salicylic Wong, 2013). Some PPCPs (e.g., parabens) can be effectively eliminated
acid was most frequently detected, while carbamazepine and atenolol in STPs, with an average removal rate of N90% (Jonkers et al., 2009;
were detected in N 30% of the contaminated water supplies but at low González-Mariño et al., 2011). However, most PPCPs are only partially
concentrations (b or = 2 ng/L). Carmona et al. (2014) reported that removed in conventional STPs equipped with primary and secondary
treatment processes. Table 4a shows the removal efficiencies of PPCPs in Several PPCPs are poorly eliminated by the secondary treatment
different unit processes in STPs in different countries. processes; therefore, the use of the tertiary treatment processes in
The capabilities of primary treatment processes (i.e., sedimentation) STPs, namely, sand filtration, AOPs, and membrane separation, is com-
in removing PPCPs are very limited because of the hydrophilic nature of monly necessitated to remove PPCPs prior to either chemical or UV dis-
most PPCPs (Carballa et al., 2005; Luo et al., 2014). The removal efficien- infection. Transformation of PPCPs was also identified in chlorination
cy of pharmaceuticals is comparatively lower than that of PCPs. For ex- process (Gómez-Ramos Mdel et al., 2011).
ample, b 28% of diclofenac and E3 was found to be removed in Similar with sedimentation, sand filtration is generally ineffective for
sedimentation tanks (Behera et al., 2011), and no considerable reduc- PPCP removal owing to the high hydrophilicities of most PPCPs. McAvoy
tion was reported for estrone, ibuprofen, and sulfamethoxazole et al. (2002) demonstrated that sand filter system in STPs was ineffec-
(Carballa et al., 2004; Gao et al., 2012). TCS removal by primary treat- tive in removing TCS. Nakada et al. (2007) evaluated the treatment per-
ment varies significantly because the high water consumption rate re- formance of 21 PPCPs in a full-scale STP equipped with sand filtration
sults in short hydraulic retention time (HRT) in sedimentation tanks and ozonation in Tokyo. The results suggested that hydrophobicity
(McAvoy et al., 2002). Adsorption is one of the main mechanisms of was the controlling factor in PPCP removal. Low removal efficiencies
PPCP removal in primary treatment processes (Suárez et al., 2008). (b50%) of PPCPs with a log/Kow b 3 were achieved during sand filtration,
Wang et al. (2014) investigated the removal of six PPCPs, namely caf- whereas PPCPs with a log/Kow N 3 exhibited over 80% removal in some
feine, DEET, carbamazepine, metoprolol, TMP, and sulpiride in an STP. cases. In addition, most of the target pharmaceuticals and all target an-
The overall removal efficiencies of these PPCPs in primary sedimenta- tibiotics were effectively eliminated (i.e., N80%) ozonation. Several stud-
tion tanks were b 20% owing to their hydrophilic characteristics ies have suggested that oxidation is the major removal mechanism of
(i.e., low water partition coefficient). Moreover, the specific size of ozonation and tertiary amino groups are susceptible to ozone attack
sludge particles suitable for adsorption of PPCPs is extremely restricted (Huber et al., 2005; Dodd et al., 2006). These findings indicate that the
(Luo et al., 2014). Therefore, primary treatment alone may be insuffi- removal of PPCPs via ozonation depends on their chemical structures.
cient to remove PPCPs efficiently. However, up to 40% of fragrances This may be attributed to the selective reaction of ozone with certain
(e.g., AHTN and HHCB) can be efficiently removed in primary treatment functional groups and the non-selective reactivity of hydroxyl radical
because of high partition coefficients between the liquid and solid (Papageorgiou et al., 2016).
phases (Stamatis and Konstantinou, 2013). Sun et al. (2014) found a It has been reported that effective removal of parabens (N 90%) can
strong correlation between the concentrations of AHTN and HHCB in be achieved in conventional STPs (Gorga et al., 2013; Haman et al.,
STP effluent (r2 = 0.71). The similar removal mechanisms of AHTN 2015). However, some parabens are still frequently detected in second-
and HHCB, namely, sorption and volatilization, in STPs resulted from ary effluents. For example, Li et al. (2015) investigated the fate and re-
their similar physiochemical properties. moval of 9 parabens and their derivatives in STPs using advanced
Secondary treatment mainly refers to biological process (e.g., ASP) and treatment processes (i.e., ultrafiltration (UF) followed by ozonation).
enables the removal of PPCPs through partition, adsorption, biotransfor- Only b1 to 10% of the target PPCPs were removed by UF, perhaps be-
mation, and biodegradation (Miao et al., 2005; McClellan and Halden, cause these PPCP molecules are smaller than the membrane pores
2010; Jelić et al., 2011). The removal efficiency of PPCPs in ASP is highly (Sahar et al., 2011). Several parabens were released from the membrane
dependent on the nature of PPCPs, HRT, sludge age, adsorption capacity during backwashing or significant pH fluctuations of the influent
on sludge, and reactor design (Lin et al., 2009; Bulloch et al., 2015; (Caliman and Gavrilescu, 2009). However, ozonation exhibited out-
Evgenidou et al., 2015). Different PPCPs in the same class can exhibit sig- standing performance (N 98–100%) in removing most of the parabens,
nificant variability in their biodegradability. McAvoy et al. (2002) report- except for di-chlorinated compounds, because of the high oxidation po-
ed that TCS was consistently eliminated, with a removal efficiency of tential of ozone. The findings were in agreement with a previous study,
N95% in ASP; however, poor and variable treatment performance was ob- in which 99% of parabens were removed by ozonation with short HRTs
served in biotrickling filters. No enrichment of the TCS biotransformation (Tay et al., 2010). Several studies have demonstrated that UV radiation
product, triclosan-OMe, was found in ASP, indicating that no persistent in- is effective in removing PPCPs. Moreover, the combination of biological
termediates were formed. Federle et al. (2002) reported that over 80% of processes and UV systems can considerably improve the overall treat-
TCS was removed in ASP through biodegradation. Caffeine, ibuprofen, and ment performance of PPCPs in STPs (Salgado et al., 2012; Wang et al.,
ketoprofen were biodegraded by up to 75–87% but b 25% of diclofenac 2014).
was removed during secondary treatment (Salgado et al., 2012; Wang Nakada et al. (2007) found that integration of ASP with sand filtra-
et al., 2014). Many studies have reported that the removal efficiency of tion and ozonation is effective in removing (N90%) most of the target
DEET is around 40% in biological treatment systems (Costanzo et al., PPCPs. Compared with the use of a single biological process, systems
2007; Sui et al., 2010; Zhou et al., 2009; Wang et al., 2014). Several combining a bioreactor and AOPs (e.g., UV/O3/H2O2) were found to no-
PPCPs with low biodegradability, such as carbamazepine and TMP, are ticeably enhance the removal efficiencies of cyclophosphamide (CP)
hardly biodegraded or incompletely removed in secondary treatment, re- and ifosfamide (IF) from 59% and 35%, respectively, to N99%. Although
gardless of the type of system used (Behera et al., 2011; Jelić et al., 2011; chemical processes, such as chlorination and ozonation, exhibit better
Wang et al., 2014). The ineffective removal of PPCPs in secondary treat- treatment performance, the chemicals introduced in these processes
ment may be attributed to the transformation of PPCPs into by-products may have certain levels of toxicity (Gerrity et al., 2011). In addition,
or metabolites (Miao et al., 2005) and the conjugation of target PPCPs chemical processes are not necessarily efficient in removing biologically
(Carballa et al., 2004; Galán et al., 2012). Exposure to antibiotics active antibiotics (e.g., clarithromycin) (Zhang et al., 2013) and light re-
(e.g., TMP), antibacterial agents (e.g., TCS), and β-blockers sistant UV filters (e.g., 4-MBC) (Brausch and Rand, 2011).
(e.g., metoprolol) can induce toxic or inhibitory effects on activated
sludge bacteria (Göbel et al., 2005; Miege et al., 2009; Dann and 4.2. PPCP removal in WTPs
Hontela, 2011) and alter the microbial community (Lubarsky et al.,
2012; Drury et al., 2013), thereby resulting in low removal efficiency. Compared with STPs, the performance and removal mechanisms of
For example, TCS is toxic to activated sludge bacteria because it inhibits PPCPs in WTPs are less well characterized because they had been com-
the enzyme enoyl-ACP reductase, which is an essential component of monly investigated in lab-scale studies. Some authors have reported
the bacterial fatty acid biosynthetic pathway in bioreactors (Drury et al., overall removal efficiencies based on the differences in concentration
2013). Thus, ASP cannot be used to reduce PPCPs to an environmentally levels of raw and treated water (Ternes et al., 2002; Stackelberg et al.,
safe level in most of the existing secondary STPs in Hong Kong, China, 2004, 2007). Table 4b summarizes the removal efficiencies of PPCPs in
and Europe (Muthanna and Plósz, 2008; Lin et al., 2009). different unit processes in WTPs in different countries. Similar with
STPs, PPCP removal in individual unit processes shows more significant (Huerta-Fontela et al., 2011; Diemert et al., 2013). The removal efficien-
variations than the overall PPCP removal in WTPs. The removal efficiencies of antibiotics in conventional WTPs are even b10% (Liu J. et al.,
cy is mainly dependent on the specific processes used in WTPs (Boleda 2015).
et al., 2011; Padhye et al., 2014). In general, conventional water treat- Advanced treatment technologies, such as ozonation, activated car-
ment processes (Fig. 2b), including coagulation/flocculation, sedimen- bon adsorption, and reverse osmosis (RO), are applicable to PPCP re-
tation, and sand filtration, are ineffective in removing PPCPs (b 30%) moval in WTPs (Heberer, 2002; Snyder et al., 2003; Lee et al., 2008;
Table 4b
The removal (%) of PPCPs in different unit processes in WTPs in different countries.
Order Representative Step 1 Step 2

compounds Coagulation and Sand filtration and Advanced treatment processes Location References
flocculation (%) chlorination (%)
GAC Ultrafiltration and reverse
(%) osmosis (%)
1a Triclosan 89 86.6 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
B. Blood lipid regulators

2a Metoprolol 8 11 N95 Finland, Helsinki Vieno N.M. et al. (2007)
2b Pravastatin 91 91 Spain (Northeast) Boleda et al. (2011)
C. Broad-spectrum antibiotics
3a Acetaminophen 96 99 Spain (Northeast) Boleda et al. (2011)
46 86 Canada, Ontario McKie et al. (2016)
3b Acetylsalicylic acid 83 NA Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
8 Finland, Helsinki Vieno N.M. et al. (2007)
3c Azithromycin 99 99 Spain (Northeast) Boleda et al. (2011)
3d Carbamazepine 7 Finland, Helsinki Vieno N.M. et al. (2007)
46 NA Spain, Llobregat Huerta-Fontela et al. (2011)
3e Chlorhexidine N99 N99 Spain (Northeast) Boleda et al. (2011)
3f Clarithromycin N99 N99 Spain (Northeast) Boleda et al. (2011)
3g Diclofenac 99 N99 Spain (Northeast) Boleda et al. (2011)
78.3 76.8 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
3h Erythromycin 95 99 Spain (Northeast) Boleda et al. (2011)
3i Lincomycin 99 N99 Spain (Northeast) Boleda et al. (2011)
3j OH-omeprazole 97 99 Spain (Northeast) Boleda et al. (2011)
3k Omeprazole 93 95 Spain (Northeast) Boleda et al. (2011)
3l Paracetamol 81.3 80.7 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
3m Phenylbutazone 79.3 95.5 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
3n Sulfadimethoxine 97 91 Spain (Northeast) Boleda et al. (2011)
3o Sulfamethazine 99 91 Spain (Northeast) Boleda et al. (2011)
3p Sulfamethoxazole N99 N99 Spain (Northeast) Boleda et al. (2011)
3q Trimethoprim 99 N99 Spain (Northeast) Boleda et al. (2011)
3r Tylosin 94 99 Spain (Northeast) Boleda et al. (2011)
D. β-Blockers
4a Atenolol 12 Finland, Helsinki Vieno N.M. et al. (2007)
4b Salicylic acid 84 85 Spain (Northeast) Boleda et al. (2011)
4c Sotalol b1 5 N96 Finland, Helsinki Vieno N.M. et al. (2007)
E. Hormones
5a Bezafibrate 98 N99 Spain (Northeast) Boleda et al. (2011)
17 27 N77 Finland, Helsinki Vieno N.M. et al. (2007)
5b Estrone 73 93.8 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
5c 17β-Estradiol 73.1 95.2 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
5d 17α-Ethinylestradiol 75 90 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
F. Nonsteroidal anti-inflammatory drugs (NSAIDs)

6a Clofibric acid 87 97 Spain (Northeast) Boleda et al. (2011)
83.8 NA Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
6b Flunixin 84 96 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
6c Gemfibrozil N99 N99 Spain (Northeast) Boleda et al. (2011)
29 NA Canada, Ontario McKie et al. (2016)
6d Ibuprofen 98 N99 Spain (Northeast) Boleda et al. (2011)
9 12 92 Finland, Helsinki Vieno N.M. et al. (2007)
6e Ketoprofen 85.1 80 Spain (one city in south-eastern) Azzouz and Ballesteros (2013)
6f Naproxen 99 N99 Spain (Northeast) Boleda et al. (2011)

Huerta-Fontela et al., 2011). However, ozonation may produce un- achieved by ozonation with initial dose of 2.25 mg/L followed by NF in
known degradation products (Westerhoff et al., 2005). Zwiener and natural waters (Watkinson et al., 2007). Although NF and RO processes
Frimmel (2000) suggested that AOPs can significantly enhance the re- exhibit efficient PPCP removal, pollutants in a highly concentrated form
moval of PPCPs, especially pharmaceuticals. However, their efficiencies remaining in the retentate require further treatment.
are often limited by the radical scavenging capacity and ozone con-
sumption of organic matter present in the water (Zwiener and
5.2. Granular activated carbon
Frimmel, 2000). Huerta-Fontela et al. (2011) reported that PPCPs with
high hydrophobicities could be effectively eliminated by GAC filtration.
Granular activated carbon (GAC) and powdered activated carbon
Lin et al. (2016) investigated the occurrences and removal of 39 PPCPs
(PAC) were investigated for the sorptive removal of PPCPs (Yang et al.,
in a WTP equipped with ozonation and GAC filtration. Most of the 14
2011; Boehler et al., 2012; Margot et al., 2013). GAC is typically used
PPCPs detected in raw water were completely removed by the advanced
in rapid filters, whereas PAC is an efficient method in removing season-
WTP. The removal efficiencies of caffeine, indomethacin, and sulfameth-
ally occurring taste and odor in WTPs (Scheurer et al., 2010; Zoschke
oxazole were 89.5%, 84.2%, and 92.2%, respectively. The results of princi-
et al., 2011). In this review, we focus on GAC because it has been used
pal component analysis also suggested that oxidation, coagulation
widely in drinking water treatment and tertiary treatment in STPs.
combined with sedimentation, and filtration were the major removal
Stackelberg et al. (2007) found that GAC facilities in a conventional
mechanisms in the advanced WTP. These findings were consistent
WTP accounted for 53% removal of the tested PPCPs, whereas disinfec-
with a previous study, in which ozonation was found to be highly effec-
tion and sedimentation accoutred for 32% and 15%, respectively.
tive for PPCP removal (Hollender et al., 2009).
In a study by Hernández-Leal et al. (2011), the removal efficiencies
Biofilters, which can be simply fabricated by converting granular
for tonalide and nonylphenol ranged from 50% to N 90% (galaxolide).
media filters, have been demonstrated to be effective for PPCP removal
Contact time was found to markedly affect the extent of carbon adsorp-
(Zuehlke et al., 2007; Meffe et al., 2010; Zearley and Summers, 2012).
tion. Short contact times resulted in low removal efficiencies. Corre-
McKie et al. (2016) performed a pilot-scale study to evaluate the PPCP
spondingly, long contact times increase surface loading and the
removal in WTPs equipped with biofilters. Compared with conventional
number of accessible adsorption sites (Bolong et al., 2009; Meinel
dual-media filtration, biofiltration systems with and without coagulant
et al., 2015). In general, adsorption by activated carbon has greater po-
addition successfully improved the PPCP removal from 13% to 39% and
tential for removal of antibiotics than coagulation and flocculation pro-
70%, respectively. The treatment performance of biofilters for PPCP re-
cesses (Choi et al., 2008).
moval may be enhanced using low doses of in-line coagulant without
Activated carbon has also demonstrated as an effective advanced
adversely affecting headloss (Azzeh et al., 2015).
treatment process in removing PPCP residues from treated effluents.
Ek et al. (2014) conducted a pilot-scale study to evaluate the perfor-
5. Control strategies for PPCP contamination
mance of activated carbon in removing pharmaceutical residues from
treated wastewater. The results suggested that activated carbon beds
5.1. Membrane filtration
with 90–98% PPCP removal may be a competitive alternative to treat-
ment with ozone. Similar conclusions were drawn by Grover et al.
Membrane filtration processes, such as nanofiltration (NF) and RO,
(2011), who studied the removal of pharmaceuticals from sewage efflu-
are promising alternatives for the elimination of PPCPs from wastewater
ent in a full-scale STP. 43–64% of steroidal estrogens were successfully
(Nghiem et al., 2004; Yoon et al., 2006; Yoon et al., 2010). UF and
removed by GAC. The elimination rates varied for different types of
microfiltration (MF) have been proven to remove PPCPs. However,
pharmaceuticals; for example, the removal efficiencies of mebeverine
their removal performances are relatively poor because membrane
and diclofenac were 84%–99%. In contrast, carbamazepine and propran-
pore sizes are considerably larger than PPCP molecules. For comparison,
olol exhibited relatively low removal rates of 17%–23%.
pressure-driven membrane processes, NF and RO, were applied to the
Paredes et al. (2016) assessed the treatment of secondary effluents
drinking water treatment (Watkinson et al., 2007). These processes
using sand and GAC biofilters. Several reactors were used to determine
generally show significant PPCP removal efficiencies; however these
the contributions of adsorption and biotransformation to the removal of
membranes are still slightly permeable to some relatively small pollut-
several PPCPs. The PPCP removal mechanisms were classified into three
ants (Schäfer et al., 2011).
different categories: (I) biotransformation and high adsorption on GAC
The removal capabilities of two different types of submerged NF flat
and sand (e.g., galaxolide, tonalide, celestolide, and TCS), (II) biotrans-
sheet modules for removal of pharmaceuticals from STPs were investi-
formation and high adsorption on GAC, but either low or null adsorption
gated (Röhricht et al., 2009). Approximately 60% of diclofenac and
on sand (e.g., ibuprofen, naproxen, fluoxetine, erythromycin,
naproxen were retained by both types of membranes, whereas only a
roxithromycin, sulfamethoxazole, TMP, bisphenol A, E1, E2, and EE2),
small proportion of carbamazepine was removed. Hence, diclofenac
and (III) adsorption on GAC alone (e.g., carbamazepine, diazepam, and
and naproxen may be obstructed by the negatively charged membrane
diclofenac). When choosing the most appropriate PPCP treatment pro-
surface, whereas carbamazepine may not (Nghiem et al., 2005).Howev-
cess, the high operating cost, the clogging problem, and the associated
er, these removal efficiencies may not be sufficient to justify the use of
hydraulic capacity limits should be considered (Ek et al., 2014).
such a system as an additional treatment step in STPs. For more polar
compounds, the NF membrane showed higher removal efficiencies
than the UF membrane. The removal of selected PPCPs by NF and RO 5.3. Advanced oxidation processes
has also been compared in previous studies (Yangali-Quintanilla et al.,
2011). The average retention efficiency of NF is 82% for neutral pollut- AOPs, such as ozonation, UV, photocatalysis, and Fenton reaction,
ants and 97% for ionic contaminants, whereas RO can achieve 85% to have been used for drinking water treatment (e.g., odor/taste control
99%. Real et al. (2012) compared the efficiencies of different system con- and disinfection) and to lesser extent in wastewater disinfection
figurations in the elimination of PPCPs from selected water sources. (Huber et al., 2003; Klavarioti et al., 2009; Gerrity et al., 2010). AOPs
When ozonation was combined with NF, the removal efficiency was sig- may change the polarity and functional groups of the target PPCPs
nificantly affected by such variables as ozone dose and treatment se- (McMonagle, 2013; Papageorgiou et al., 2014). Thus, AOPs are suitable
quences. For instance, NF followed by ozonation removed N 97% of for water reuse purposes that involve direct human contact, such as
pollutants from natural water, with an ozone dose of 2.25 mg/L and household wastewater reuse applications (Hernández-Leal et al.,
N90% from secondary effluent, with an ozone dose of 3.75 mg/L. In con- 2011). It has been reported that WTPs equipped with AOPs further elim-
trast, a high removal efficiency (N 70% in the permeate stream) was inated PPCPs. Compounds, such as caffeine, indomethacin, and
sulfamethoxazole, were removed at efficiencies of 89.5%, 84.2%, and Kong (No. DSRAF-6 SP1), and the National Research Foundation of Ko-
92.2%, respectively (Lin et al., 2016). rea (NRF) funded by the Ministry of Science, ICT and Future Planning
A study on pilot-scale experiments in a WTP was conducted by (No. 2016R1E1A1A01940995).
Borikar et al. (2015). The results indicated that conventional WTPs
equipped with either ozone/H2O2 or UV/H2O2 greatly improved PPCP Appendix A. Supplementary data
removal from 26% to 97% or 92%, respectively. Among the tested
PPCPs, carbamazepine, fluoxetine, naproxen, gemfibrozil, and TCS Supplementary data to this article can be found online at http://dx.
showed near complete removal. Diclofenac and ibuprofen were also re- doi.org/10.1016/j.scitotenv.2017.04.102.
moved by up to 97% and 98%, respectively. However, pharmaceuticals
demonstrated some resistance in that, the highest removal of atorva-
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Science of the Total Environment 596–597 (2017) 303–320

Contents lists available at ScienceDirect

Science of the Total Environment

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

Occurrences and removal of pharmaceuticals and personal care products

• There is a large variation in PPCP remov-

Fig. 1. Sources and pathways of PPCPs.

C. Blood lipid regulators

ND = not detectable; NA = not available.

ND = not detectable; NA = not available.

C. Analgesics and anti-inﬂammatory drugs

D. Blood lipid regulators

G. Non-steroidal anti-inﬂammatory drugs (NSAIDs)

NA = not available; ND = not detectable.

NA = not available; ND = not detectable.

Order Representative Preliminary Primary Secondary Tertiary Location References

E. Nonsteroidal anti-inﬂammatory drugs (NSAIDs)

NA = not available; ND = not detectable.

Order Representative Step 1 Step 2

B. Blood lipid regulators

F. Nonsteroidal anti-inﬂammatory drugs (NSAIDs)

NA = not available; ND = not detectable.

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