1 s2.0 S0301479722012762 Main

Journal of Environmental Management 320 (2022) 115703
Contents lists available at ScienceDirect
Journal of Environmental Management

journal homepage: www.elsevier.com/locate/jenvman
Review
Global groundwater vulnerability for Pharmaceutical and Personal care

products (PPCPs): The scenario of second decade of 21st century
Rahul Silori a, Vikalp Shrivastava a, Ashwin Singh b, Pradeep Sharma c, Marwan Aouad d,
Jürgen Mahlknecht e, Manish Kumar a, *
a
School of Engineering, University of Petroleum & Energy Studies, Dehradun, Uttarakhand, 248007, India
b
Discipline of Civil Engineering, Indian Institute of Technology Gandhinagar, Gandhinagar, 382355, Gujarat, India
c
Department of Environmental Science, Graphic Era Deemed to be University, Dehradun, Uttarakhand, 248002, India
d
College of Engineering, Applied Science University (ASU), Kingdom of Bahrain
e
Escuela de Ingeniería y Ciencias, Tecnologico de Monterrey, Campus Monterey, Monterrey, 64849, Nuevo Leon, Mexico
A R T I C L E I N F O A B S T R A C T
Keywords: The global production of PPCPs have increased by multiple folds promoting excessive exposure of its metabolites
Pharmaceutical and personal care products to humans via different aquatic systems. The higher residence time of toxic precursors of these metabolites pose
(PPCPs) direct human health risk. Among the different aquatic systems, the contamination of groundwater by PPCPs is
Groundwater
the most concerning threat. This threat is especially critical considering the lesser oxidizing potential of the
Global trends
Emerging contaminants
groundwater as compared to freshwater/river water. A major challenge also arises due to excessive dependency
Life-style impact of the world’s population on groundwater, which is exponentially increasing with time. This makes the identi
fication and characterization of spatial contamination hotspots highly probabilistic as compared to other
freshwater systems. The situation is more vulnerable in developing countries where there is a reported in
adequacy of wastewater treatment facilities, thereby forcing the groundwater to behave as the only available
sequestrating sink for all these contaminants. With increased consumption of antibiotics and other pharma
ceuticals compounds, these wastes have proven capability in terms of enhancing the resistance among the biotic
community of the soil systems, which ultimately can become catastrophic and carcinogenic in near future.
Recent studies are supporting the aforementioned concern where compounds like diclofenac (analgesic) have
attained a concentration of 1.3 mgL− 1 in the aquifer systems of Delhi, India. The situation is far worse for
developed nations where prolonged and indiscriminate usage of antidepressants and antibiotics have life
threating consequences. It has been confirmed that certain compounds like ofloxacin (antibiotics) and bis-(2-
ethylhexyl)phthalate are present in some of the most sensitive wells/springs of the United States and Mexico. The
current trend of the situation has been demonstrated by integrating a comparative approach of the published
literatures in last three years. This review provides first-hand information report for formulating a directive
policy framework for tackling PPCPs issues in the groundwater system.
1. Introduction toothpaste, sunscreens, etc., which are widely used in high quantities in
daily life across the world (Daughton and Ternes, 1999). The most
During the last few decades, there has been a substantial increase in common urban pathways by which these PPCPs reach the aquatic and
the production and consumption of Pharmaceutical and Personal care terrestrial environment are municipal wastewater treatment plants
products (PPCPs) to meet the requirements of modern standards of (WWTPs), pharmaceutical industries, effluent from hospitals, fecal
living and ensure better health system (Daughton and Ternes, 1999; wastes of humans and animals, landfill sites, animal husbandries and
Khan et al., 2022). PPCPs consist of a wide group of organic compounds, aquaculture (Silori and Tauseef, 2022). Their presence in aquatic envi
including pharmaceutical products from various therapeutic classes and ronment like surface water, groundwater and wastewater have raised
amalgamates of personal care products (PCPs) such as soaps, lotions, concerns for the health of humans and aquatic life due to their potential
* Corresponding author. Energy Acres, UPES, Dehradun, Uttarakhand, 248007, India.

E-mail addresses: manish.env@gmail.com, manish.kumar@ddn.upes.ac.in (M. Kumar).
https://doi.org/10.1016/j.jenvman.2022.115703
Received 8 February 2022; Received in revised form 5 June 2022; Accepted 6 July 2022
Available online 3 August 2022
0301-4797/© 2022 Elsevier Ltd. All rights reserved.
R. Silori et al. Journal of Environmental Management 320 (2022) 115703
toxic composition and degradation process (Yuan et al., 2020). The of chromatography such as conventional Gas chromatography (GC) etc.
long-term persistence and partial degradation in the environment make have been traditionally used. With the technological advancement, lat
the accumulation of PPCPs in the water bodies a viable threat (Martínez, est and more sensitive techniques such as Liquid chromatography
2008; Watkinson et al., 2009). The low-level exposure of PPCPs promote coupled with mass spectrometry (LC-MS), Ultra-High-Performance
antibiotic resistance in river base flows which further disrupts the liquid chromatography-tandem mass spectrometry (UHPLC-tandem-
groundwater system when active streamflow exchange takes place be MS) etc. have been developed for the analysis of these compounds up to
tween river and groundwater, providing an equal stress on the survival trace levels (Galindo-Miranda et al., 2019).
prospect of sub-surface microorganisms. The risk factor further am It has been generally observed that the concentration of PPCPs is
plifies in regions which are heavily dependent upon groundwater for usually maximum in WWTPs. Although, there is disparity in the pollu
meeting their needs as the sorption of these contaminants is highly tion level between a municipal WWTP and pharmaceutical production/
sensitive to pH and Ionic Strength (IS) of the solution (Chen et al., 2011). healthcare WWTPs (Balakrishna et al., 2017). Concentration for PPCPs
Further, it has been established that Karst aquifers are relatively more in WWTPs effluent treating pharmaceutical formulation facilities
vulnerable to the sorption of these contaminants due to their geologic wastewater generally lies in hundreds of μg/L to mg/L (Fick et al., 2009;
settings which promote high hydraulic conductivities and groundwater Larsson et al., 2007; Lin and Tsai, 2009; Phillips et al., 2010; Sim et al.,
velocities even under limiting adsorption of contaminants on the soil 2011) but in municipal WWTPs effluent processing domestic wastewater
(Katz et al., 2009). Based on the geomorphic and geologic settings in normally lies in ng/L (Chiffre et al., 2016; Kosma et al., 2010; Lacey
which different emerging economies are located, it becomes imperative et al., 2012; Mijangos et al., 2018; Mohapatra et al., 2016). A study
to explore the potential of groundwater susceptibility to PPCPs conducted in Greece by Kosma et al. (2014) demonstrated the difference
contamination. between PPCPs concentrations detected in municipal WWTP and that by
Studies since 1980 have been pointing out that pesticides and fer WWTP treating a hospital effluent. In the study, the maximum concen
tilizers have been intruding into the groundwater system promoted by tration of salicylic acid (analgesics) and trimethoprim (antibiotics) at a
varying recharge conditions (Hallberg, 1989). However, recent studies municipal WWTP of Arta city, Greece, reported as 4.97 μg/L and 0.0545
have confirmed that even hydrophobic agricultural chemicals, espe μg/L respectively while their maximum concentrations at a WWTP
cially atrazine have high tendencies to leach through epikarst during treating hospital effluent in Ioannina city (Greece) reported as 75.84
high flow conditions, tracing the storm pulses on the surface (Vesper μg/L and 1.866 μg/L respectively. Similarly, a study in Korea showed a
et al., 2001). Further, it has been established that groundwater in the considerable difference between concentration of PPCPs in treated
Karst aquifers, especially that in pristine state are highly susceptible to effluent of a pharmaceutical production facility and municipal WWTP
anti-inflammatory drugs (Einsiedl et al., 2010). The PPCPs risk in the (Sim et al., 2011).
groundwater is a function of residence time. Additionally, the microbe Effluent from a pharmaceutical formulation WWTP reported a
mediated processes are dependent upon the location of fractures and maximum concentration of 19.2 μg/L for diclofenac (Nonsteroidal anti-
fissures in the aquifers, where there is lower hydraulic conductivity inflammatory drug, NSAID) while maximum concentration of only 1.76
(Wilhartitz et al., 2009). Specifically, the bacteria present in the oligo μg/L for the same compound was detected in effluent of a municipal
trophic Karst aquifers could probably metabolize these pollutants. WWTP. Since, conventional WWTPs are not very efficient in treating and
However, permanent exposure of these pollutants causes adaptation and removing PPCPs, there are some alternative methods reported in the
a change in the functional genes of the bacteria, thereby promo literature to target these compounds removal. The removal methods are
ting/inhibiting the degradation of the contaminants (Herrick et al., physical, chemical and biological, notably. The rudimentary aspect in
1997). The groundwater has a functional mechanism to mitigate the volves in physical process is adsorption with carbon-based adsorptive
intrusion of the pollutants via degradation in which both hydraulic and materials such as activated carbon, graphene and carbon nanotubes
geologic factors play an important role. However, it is equal concerning (Wang and Wang, 2016). For example, removal of these PPCPs from
to evaluate the nature of pollutant and its source, which primarily is the sorption process using sustainable cotton-based adsorbent (Czech et al.,
wastewater, which ultimately decides the fate of contaminants in the 2020). Results showed that it efficiently removed triclosan (137
groundwater system. mg/gm), caffeine and naproxen from the sample.
Krishnan et al. (2021) stated that at the end of treatment, the Another innovative approach introduced by Keerthanan et al.
wastewater is converted into two products, namely biosolids and treated (2020), which again used the concept of adsorbing the PPCPs on a
wastewater effluent. Application of these biosolids on farmlands intro synthesized tea-biochar for the removal of caffeine from aqua media.
duce PPCPs to terrestrial environment. During irrigation, the pollutants Results showed the removal of 55.6 mg/gm/min of caffeine from the
present in fertilizers leach into the ground causing contamination of the media. One of other approach integrated a renovated filter filled with
vadose zone due to subsequent adsorption/desorption at the surface of poly-3-hydroxybutyrateco-hydroxyvalerate and granulated activated
soil matrix. In the study, which was carried out on emerging contami carbon (Yi et al., 2020). The promising results showed 80% of removal
nants in vadose zone in North China, PPCPs such as carbamazepine were efficiency of PPCPs along with no accumulation of ammonia and nitrite.
detected in soil samples of irrigated farmlands at a depth of 16 m from Chemical process involves ozonation, advanced oxidation process (AOP)
ground level up to the levels of 12.5 μg/kg (Ma et al., 2018). Treated which consists the use of O3/UV, UV/H2O2, gamma radiolysis and
wastewater is the other product generated from WWTPs. Generally, this electro-chemical oxidation process where contaminants are partially
treated wastewater is discharged openly into any water body like river oxidized and then converted into salts, H2O, CO2 (Krishnan et al., 2021;
or lake, which eventually introduce these PPCPs into the surface water Wang and Xu, 2012). Biological process consists of pure culture and
bodies (Gogoi et al., 2018) [A]. Sometimes treated wastewater is used mixed culture methods for the removal of such contaminants (Wang and
for irrigation in water scarce locations. Moreover, to manage the issue of Wang, 2016).
salinity in soil, wastewater is used to irrigate the lands in order to However, the presence of these compounds in water bodies are a
maintain the soil pH. Wastewater is also rich in nitrogen, potassium and testament of limitation of rules and regulations set up by the responsible
phosphorus; which are key elements required for proper growth of authority in any country. Detection of high concentration of PPCPs in
crops. However, leaching and irrigating with wastewater has its own wastewater highlights the loopholes in disposal policies. The procedures
consequences as it trickles down all the way to groundwater level with in the disposal of effluents from pharmaceutical industries and health
the contents it carries within. care facilities are not being followed as the law stipulates and they end
The traces of PPCPs are present at a very diminutive level, which are up entering in our environment. To address these challenges, some steps
hard to distinguish in the environment. To substantiate their presence in have been taken only in few countries, such as Federal and State
the environment many analytical techniques that work on the rudiments agencies of U.S.A. have formulated legislations and regulation to tackle
2
the threat posed by PPCPs and Endocrine disrupting chemicals (EDCs) to indomethacin, an anti-inflammatory drug (Lister & Van Der Kraak,
(Water Research Foundation, 2015). For instance, Clean Water Act 2008). Streptomycin, a kind of anti-microbial substance have been
(1972) stipulates the discharge of pollutants from point sources into U.S. found to retard the synthesis of protein, which causes misreading of
water as per developed standards. It also sets bar over maximum daily mRNA in duckweed plant (Brain et al., 2004). At a very low concen
loads for chlordane and atrazine. Similarly, Safe Drinking Water Act tration (<0.1 ng/L) of antibiotics, some algae cease to grow which leads
(1996) sets enforceable maximum contamination level of organic to scarcity of algal population in aquatic system which serves as a major
chemicals, radionuclides etc. from public water systems. Similar regu food source of many aquatic animals and organisms (Al-Farsi et al.,
latory and monitoring steps have been taken in Australia in the form of 2017). In case of warm-blooded vertebrates like birds, approximately
‘Western 0020 Australian project’ at Perth. This project aims to monitor 6000 Swainson’s Hawks were found dead in grassland of Argentina after
the pharmaceutical compounds in recycled wastewater (Miarov et al., feeding on the grasshoppers, which were exposed to organophosphate
2020). In any country, municipal WWTPs, as well as pharmaceutical pesticides spread in order to mitigate their outbreak (Goldstein et al.,
manufacturing WWTPs are not subjected to stringent emission guide 1999).
lines till date (Silori and Tauseef, 2022). Additionally, pharmaceutical PPCPs also pose a threat and can alter our body’s response to hostile
compounds are not regulated in drinking water in any country despite of microbes. These PPCPs keep accruing in the environment and exposure
their potential adverse effects (Bexfield et al., 2019). to those environmental components which may cause proliferation of
Moreover, as the time ensues their accumulation might become a Anti-Microbial Resistance (AMR). Humans consuming food containing
major issue for the ecosystem on this planet. Limited knowledge about antibiotic residues in them, exposure to contaminated groundwater or
these PPCPs and the ways of their handling, usage and disposal is an area surface water, household pets or any occupational area exposed to any
of environmental concern (Al-Farsi et al., 2017). Database of google contaminated work field nearby may lead to resistance or modification
scholar clearly shows a rise in the number of studies conducted or dis in human microbial activities resulting into such diseases or illness that
cussed globally on PPCPs in water environment encompassing waste cannot be easily cured (Al-Farsi et al., 2017; Alderton et al., 2021;
water, surface water and groundwater etc. The received and continuous Bhagat et al., 2020). This condition is known as AMR and knowledge
increasing data showed the interest of researchers and scholars for this about AMR is still need to be characterized properly to have its better
topic, which is a positive step. Fig. 1 elucidate that the number of studies understanding (Alderton et al., 2021). Excess mortality rate and pro
has considerably increased since last decade. The keywords used for longed stay in hospital was associated with the diseases and infections
finding the result were PPCPs and water in the database. caused by AMR bacteria (Huijbers et al., 2015).
The PPCPs can affect the metabolism of living organisms by devel It has been outlined in many studies that accumulation of such PPCPs
oping toxic effects in them or by amplification of drug-resistant strains in water environment has led to some adverse effects stretching from
(Zhu et al., 2013). PPCPs have considerably affected the biology of near annihilation of fish species to their feminization (Nordea, 2016).
aquatic animals by polluting their environment and bioaccumulating in World Health Organization (WHO) reported that high resistance in
their food chain (Hamid et al., 2021). Since groundwater receives bacteria such as ‘Escherichia Coli’, Staphylococcus aureus, ‘Klebsiella
streamflow discharge therefore it becomes equally important to under Pneumoniae’ etc. were found in the community of those people living in
stand the probable counter wise effect of PPCPs contaminated ground WHO identified sensitive regions (World Health Organization, 2014). As
water intrusion into the river water. It has been reported that exposure reported by Nikolaou et al. (2007), humans subjected to these PPCPs are
to triclosan (TCS) has resulted into physical variation in fin length and susceptible to declining fertility rate, birth defects, colon, breast and
sex ratio in fishes like Medaka (O. latipes) (Foran et al., 2000). Sexual testicular cancer. So far, no major risk has been reported on human
abnormalities in fish species have been posited in various studies living health in studies but as they say, “prevention is better than cure”. Looking
near outfall of WWTP (Bolong et al., 2009). Reduction in spawning at the data of U.S. Fish and Wildlife Service (USFWS) Threatened and
nonsteroidal rates and clutch sizes were observed in Zebrafish exposed Endangered Species Systems (TESS), there are about 370 threatened and
Fig. 1. Global year-wise trend for research studies on PPCPs in the aquatic environment including wastewater. There has been an increase of 27% in the research
from 2010 to 2015, with an almost a more than 100% increase in literary output in last 10 years (Google Scholar).
3
endangered vertebrate species. Their exposure to such contaminants being one of the primary locations for the outfall or discharge of
will be dire to their population and existence by affecting their ability to monsoon water, the river water and its life-form adversely gets affected.
recover and increase their population or it may lead to their geograph In Central America, study reported that fishes exposed to estrogenic
ical and habitat isolation (Smith et al., 2007). pollutants had an increase in their liver size (Gunnarsson et al., 2009).
Keeping in concern of PPCPs contamination tremendous rise in Spongberg et al. (2011) in river water samples of Costa Rica sampled in
environmental matrices, this review paper will primarily present (a). 2009 reported the maximum concentration of caffeine reaching up to
global prevalence of various PPCPs in groundwater environment since 1.1 mg/L while other compounds like doxycycline, ibuprofen, acet
last one and half decade, (b). current trends in occurrence of these PPCPs aminophen had their concentrations 74 μg/L, 37 μg/L and 17 μg/L
in global groundwater system from 2019 to 2021 and (c). correlation respectively. In a populous country like India, the amount of wastewater
between groundwater contamination and the countries based on their generated is way more than the capacity of WWTP’s capacity designed
development index (developed country and developing country). to treat them, hence a lot of untreated waste water is discharged into
surface water (Biswas and Vellanki, 2021). Kaur et al. (2012) highlights
2. PPCPs occurrence in wastewater and aquatic environment those major cities of India generate 38,354 MLD wastewater but the
capacity of WWTP to treat this volume is only 11,786 MLD. Such a
2.1. Wastewater scenario has been reported in Yamuna river, which is a source of
drinking water to millions in Northern India was found to be contami
WWTPs act as a junction of all the PPCPs of human settlement, be it a nated with an alarming concentration of trimethoprim and caffeine as
small town or a metropolitan city. Wastewater comes to WWTP from all 8.807 μg/L and 6.489 μg/L respectively (Biswas and Vellanki, 2021).
the possible sources such as greywater and excretion wastes from Ahammad et al. (2014) reported that banks of Ganges, which are used as
households, effluent from chemical and paper industries and medical bathing sites during pilgrimage seasons, might act as hot spot for the
facilities, discharge from community spots like swimming pools and broader exposure and proliferation of such compounds.
bathing sites, careless disposal of expired products, which include Turning towards Africa, study found the total concentration and
electronic items. These waste matters carrying all the obnoxious loads of all the PPCPs measured in the water samples of Nzoia river of
chemicals dissolved in it meet at WWTP via sewer lines. Due to the Kenya were up to 23 μg/L and 7220 g/day while the concentration and
knowledge gap about these contaminants of emerging concern, the load of pesticides in these samples were 0.343 μg/L and 2600 g/day
current WWTPs are designed to remove only targeted impurities like (K’oreje et al., 2018). Algal toxicity of clarithromycin and levofloxacin
nutrients, pathogens and particulate matters (Adeleye et al., 2022). was identified in the river at a concentration of 3.1 and 310 μg/L. The
Therefore, it is reasonable to find the maximum concentration of PPCPs aquatic organisms of Adige River in Sole valley (Italian Alps) were
in wastewater, sometimes fully or partially metabolized. As per Adeleye exposed to unacceptable risk of these PPCPs which included antibiotics,
et al. (2022), the reduction in mass of PPCPs can be seen at the effluent painkillers, surfactants and anti-bacterial agents with the maximum
of WWTPs due to the physiochemical properties of PPCPs and WWTPs abundance of artificial sweetener ‘sucralose’ reaching to a maximum
like Hydraulic Retention Time (HRT) and Surface Retention Time (SRT) abundance of 600 ng/L (Villa et al., 2020). A study conducted by Bendz
but still these WWTPs are insufficient in proper removal of PPCPs (Liu et al. (2005) reported the heavy concentrations of carbamazepine,
et al., 2020). Watkinson et al. (2009) reports about the Australian atenolol, metoprolol, gemfibrozil and propranolol compounds ranging
wastewater effluent having concentration of 3.4 μg/L of tylosin from 0.16 to 1.18 μg/L in Hoje River basin, Sweden. Looking into South
(antibiotics). American continent in the country of Brazil, caffeine (stimulant) was
In African wastewater, heavy concentration of anti-malarian drugs, found at the highest concentration of 14,050 ng/L in Jundiai River (de
artemether and lumefantrine were detected ranging from 3 to 32 μg/L Sousa et al., 2018). The Australian rivers received a huge contaminant
(Miraji et al., 2016). Such high residues of anti-malarial drug provides concentration of salicylic acid, paracetamol, carbamazepine and
the evidence of prevalence of malaria being a common disease in that caffeine with their maximum concentration of 1.53, 7.15, 0.682 and
country. In Asia, a study conducted on wastewater of an effluent at a 3.770 μg/L (Scott et al., 2014). From all these results, it can be
WWTP near Hyderabad, India by Larsson et al. (2007) reported that concluded that the presence of these contaminants and drug residues in
extremely high concentration of ciprofloxacin reaching to 31 mg/L was our river water are a grave matter of concern to us and as the time
detected which can be an indicator for the inefficiency of conventional progresses these compounds are going to accumulate only.
WWTPs. Another Asian study conducted on PPCPs’ detection in WWTPs
of Taiwan reported heavy concentration of diclofenac up to 228,000 2.3. Lakes
ng/L in effluent of WWTP treating wastewater from pharmaceutical
production facilities (Lin and Tsai, 2009). In North America, heavy Lakes are one of the primary sources of fresh water but their water
concentration of naproxen was found in the effluent of Penn state’s (U.S. have been found to be contaminated with many compounds due to the
A.) WWTP with a huge concentration of 34.719 mg/L (Kibuye et al., human activities (Katsikaros and Chrysikopoulos, 2021). Li et al. (2021)
2019a). A separate American study also highlighted the presence of investigated that the conventional drinking water treatment plants are
PPCPs in its wastewater treatment facility where 79.86 ng/L of gaba not much efficient in removing these PPCPs and pose serious health risk
pentin was detected (Oliveira et al., 2015). European treatment plants to the population consuming it. As reported by Lin et al. (2016) surge in
were also found to be infested with PPCPs contamination where 55 ng/L population and fast industrialization of Chinese societies has led to the
of ibuprofen detected in Spanish WWTP (Santos et al., 2009). discharge of these PPCPs into the surface water which acts as a source
for the water in Taihu Lake (third largest freshwater lake in China).
2.2. Rivers However, due to the lack of study about occurrence and removal of these
PPCPs, it is unsure whether any technology can eliminate these com
Extensive use of PPCPs and pesticides, inefficient treatment at pounds out of drinking water at a drinking water treatment plant that
WWTPs and disposal of wastewater into the environment has made uses Taihu Lake as its source. That led to a frequent detection of
water bodies a concoction of these compounds (Xu et al., 2019). Out of chemicals and drugs like N,N-diethyl-meta-toluamide (DEET), sulpha
all the water bodies, river is a focal point for locating such contaminants pyridine, tiamulin, caffeine, antipyrine and lincomycin in the water of
due to several common sources such as WWTPs, which generally dis Taihu lake (Lin et al., 2016).
charges the treated wastewater directly into rivers (Kumar et al., 2014, Looking at the global context, African lakes were heavily contami
2022). Monsoon water, carrying diversity of such compounds in it, nated with PPCPs, especially Victoria and Hartbeespoort lakes. Mean
collected from its entire watershed area, join river streams. Therefore, while, some common PPCPs like carbamazepine and sulfamethoxazole
4
were ubiquitous in lakes of other continents. However, efavirenz and shape the infiltration rate; larger slope leads to higher and faster run-off
nevirapine (antivirals) were only found in African lakes (Katsikaros and leading to low infiltration rate into the groundwater. However, it is
Chrysikopoulos, 2021). equally important to note that the soil mineralogy and hydraulic char
The concentration of pharmaceutical compounds in Antarctica lakes acteristics equally dictate the process. PPCPs and their metabolites are
range from <0.66 ng/L to 70 ng/L while the concentration of PCPs usually either adsorbed or absorbed in our body and later washed or
ranged from <10 ng/L to 69 ng/L in the water of Oceanian lakes (Kat excreted which end up reaching WWTP. However, their abundance
sikaros and Chrysikopoulos, 2021). comes in small quantity but they can act as endocrine disruptors and can
Asian lakes has been found to be reported with the highest amount of hinder the reproductive health of living organisms (Serra-Roig et al.,
PPCPs, where pharmaceutical compounds were 179 and PCPs were 39 2016). In a study conducted in Besos River Delta (Spain), these PPCPs
(Katsikaros and Chrysikopoulos, 2021). Similar trend appears for Eu were found at a significant concentration of 2 μg/L, namely in the form
ropean lakes where 133 pharmaceuticals and 35 PCPs were found of benzotriazole and methyl benzotriazole (Serra-Roig et al., 2016).
reaching to a maximum concentration of 1364 ng/L (Katsikaros and Since, it is known that baseline flow of rivers is of groundwater origin, so
Chrysikopoulos, 2021). Meanwhile, 117 and 22 PPCPs were detected in a river which depends upon groundwater influx instead of precipitation
the lakes of North and South America respectively. The maximum maintaining its flow is called an effluent river or an effluent stream.
concentration of these compounds were 9200 ng/L and 13,000 ng/L in These groundwater streams keep recharging the main river body along
the lakes of North and South American continents, respectively (Katsi its stretch thereby maintaining the water level in the river. Mississippi,
karos and Chrysikopoulos, 2021). Amazon and Columbia River are such big examples of effluent rivers.
There is a high possibility of contamination of such large river bodies via
2.4. Groundwater groundwater.
The presence of “contaminants of emerging concern” in groundwater 3. Global trends of PPCPs in groundwater environment
is indeed worrisome. Although, groundwater is less susceptible to
contamination by emerging contaminants such as PPCPs than surface Since the onset of this issue from last few decades it is being observed
water but residues of many PPCPs have been detected in groundwater that many studies are being conducted which are providing some
systems and they are harder to remove from the matrices such as un alarming data. Mostly, the pharmaceutical compounds which has been
saturated zone, rocks, sediments, soil etc. (Lukač Lukač Reberski et al., identified in groundwater belongs to the therapeutic classes such as
2022). Residues of PPCPs and veterinary medicines have been observed analgesics/antipyretics/NSAIDS, antibiotics, lipid regulators, beta
in groundwater (Branchet et al., 2019; Elliott et al., 2018; Kovačević blockers, antiepileptics, stimulant and metabolites. Worldwide, traces of
et al., 2017; Schaider et al., 2014; Yang et al., 2018). Some studies have these compounds have been found since last one and half decades and
revealed that the contamination of groundwater by these PPCPs have the data is presented in Table 1, which shows that no geographical zone
been a result of irrigating the fields and agricultural land with treated of this planet is unaffected with the contamination of PPCPs in their
wastewater. So many potential sources and pathways have been groundwater. The extensive data provides the knowledge about some
distinguished for this situation. Sometimes, effluent from WWTPs, general location where this contamination has been traced such as
pharmaceutical facility or hospital, leakage from any landfills, irrigating natural springs, private and community wells, aquifers etc. At some
a land with treated wastewater or irrigating an agricultural land which places where concentration of this contamination reaches to the levels of
has been fertilized with municipal biosolids acts as a major origin point μg/L and mg/L raises concern and questions on the disposal and treat
for the transport of these PPCPs and pesticide contaminants into ment policy of the respective country. In addition to that, it gives an idea
groundwater by leaching mechanism. Application of manures and of some commonly used drugs in that region. This table represents the
slurry, excretion by animals or treatment processes used in aquaculture range of concentration of PPCPs detected in groundwater in every
infuse these compounds into groundwater as well (Topp et al., 2010). corner of the world.
The presence of pesticides in groundwater can become a cause of Furthermore, it is vital to understand the global distribution and
concern for those areas which relies on groundwater as its source and occurrence of different therapeutic classes in groundwater. Henceforth,
these pesticides can remain in groundwater for as long as several de the maximum values of concentrations of PPCPs tabulated above for
cades (Berni et al., 2021). Adsorption, migration and degradation are the groundwater contamination worldwide are represented in the form of
three primary processes, which govern the fate of PPCPs transport box-plot in Fig. 2. The purpose of the box plot is to show the range/
through porous media in the groundwater (Sui et al., 2015). Moroccan spectrum of maximum concentrations of these PPCPs of all the thera
groundwater observed prominent amount of chlorothalonil, diuron, peutic classes reported in literature. Concentration of those compounds
dicofol and bifenthrin compounds (Berni et al., 2021). In a survey showing abnormally high values with respect to others within its own
conducted in France on 589 aquifers in 2013, 203 aquifers were in poor therapeutic class are represented as outlier points in the plot. Such as
chemical condition. Their abundance in groundwater can be attributed maximum concentrations for naproxen of analgesics/NSAIDs and
to several factors such as soil and active chemical properties which may ofloxacin of antibiotic classes stands at 98,390 ng/L (Kibuye et al.,
lead to the processes of sorption and degradation (Baran et al., 2021). 2019a) and 122,700 ng/L (Kibuye et al., 2019b) respectively in
Sometimes, poor wellhead protection can lead to degradation of the groundwater of United States, which represents anomalous values which
groundwater. One such example can be seen in New Zealand where are rare to be seen in other parts of the world. However, a very unusual
glyphosate was detected in a well with a concentration of 2.1 μg/L. In and high concentration has been detected for diclofenac (analge
that similar study 655 ng/L concentration of sucralose (artificial sic/NSAID) in the aquifers of India, which peaked up to 1,390,000 ng/L
sweetener) was found in groundwater (Close et al., 2021). Duttagupta due to the presence of a landfill site near groundwater sampling site
et al. (2020) reported that depth of groundwater can also play a crucial (Velpandian et al., 2018).
role for the infiltration of these compounds through natural processes In order to determine a relation between the occurrence of thera
like sorption, dispersion, biodegradation etc. Duttagupta et al. (2020) peutic classes in groundwater and the country it has been found in; it is
stated that other parameters such as aquifer media, soil media can affect necessary to know the maximum concentration of those classes recorded
the hydraulic conductivity of the infiltrate substances into groundwater. in that country. Table 2 shows the PPCP contamination scenario in the
The rate of contamination of groundwater can be rapid inside a sand groundwater of India reaching to critical threshold values. The excessive
matrix or it can be plodding for a low-conductivity clay (Fitts, 2013). In production and consumption of generic drugs in India are clearly finding
the study by Duttagupta et al. (2020), topography of the area is also a route into the groundwater systems of the major cities in India. This
considered as an important parameter, as the slope of the terrain can concentration is higher than most developed countries and emerging
5
Table 1
Groundwater concentration spectrum of various PPCPs reported globally.
Therapeutic Class Pharmaceutical Minimum Maximum Groundwater source Country Reference
Compound Concentration (ng/ Concentration (ng/
L) L)
Analgesics/ Acetaminophen 50 15,580 Wells U. S Kibuye et al. (2019a)

Antipyretics/ 9 380 Wells, springs and sumps U. S Barnes et al. (2008)
NSAIDs < 60 1890 Wells U. S Fram & Belitz (2011)
200 2200 Private wells and springs U. S Kibuye et al. (2019b)
8.8 17 Wells and Springs U. S Bexfield et al. (2019)
0.9 1036 Shallow wells Taiwan Lin et al. (2015)
1 9 Karst Springs and Swallow hole Switzerland Morasch (2013)
<1 188 Wells and boreholes Nigeria Ebele et al. (2020)
110 111 Boreholes, wells and springs Cameroon Branchet et al. (2019)
Diclofenac 1 31.7 Wells Canada Carrara et al. (2008)
< 0.2 24 Groundwater monitoring Europe Loos et al. (2010)
stations
3.6 15.4 Karst Springs Germany Einsiedl et al. (2010)
< 10 129 Monitoring wells Germany Wolf et al. (2012)
35 477 Monitoring wells Spain Teijon et al. (2010)
15b 55c Monitoring wells and Spain Cabeza et al. (2012)
Piezometers
29.5 380 Pumping wells and observation Spain López-Serna et al.
piezometers (2013)
< 0.15 2770 Monitoring wells from landfills Poland Kapelewska et al. (2018)
< 1.5 17 Monitoring wells Singapore Tran et al. (2014)
2.1 33.2 Shallow wells Taiwan Lin et al. (2015)
N.R. 113.8 Monitoring wells Taiwan Lu et al. (2016)
13 18 Wells in the immediate vicinity Serbia Kovačević et al. (2017)
of Danube, Sava, Velika Morava
and Tisa Rivers
<8 ≈8 Private wells China Yang et al. (2018)
< 10 518 Boreholes, wells and springs Cameroon Branchet et al. (2019)
<1 42 Wells and Boreholes Nigeria Ebele et al. (2020)
150 1,390,000 Borewells India Velpandian et al. (2018)
6a 48.1a Bore and tube wells India Jindal et al. (2015)
Ibuprofen 0 2 Groundwater wells United States McEachran et al. (2016)
N.R. 3110 Wells, springs and sumps United States Barnes et al. (2008)
stations
< 10 185 Monitoring wells Spain Teijon et al. (2010)
< LOD 988 Pumping wells and observation Spain López-Serna et al.
piezometers (2013)
N.R. 290 Groundwater UK Stuart et al. (2011)
N.R. 25.5 Monitoring wells Taiwan Lu et al. (2016)
10 > 50 Private wells China Yang et al. (2018)
N.R. 57.9 Wells China Peng et al. (2014)
N.R. 65 Springs and wells Jordan Zemann et al. (2015)
< 25 276 Boreholes, wells and springs Cameroon Branchet et al. (2019)
< LOD 49.4 Hand pumps along Ganges River India Sharma et al. (2019)
Naproxen 6950 98,390 Wells United States Kibuye et al. (2019a)
0 12 Groundwater wells United States McEachran et al. (2016)
< LOD 5.59 Pumping wells and observation Spain López-Serna et al.
piezometers (2013)
N.D. 128 Shallow wells Taiwan Lin et al. (2015)
Ketprofen 27.8 731.8 Groundwater Wells Bay of Puck Szymczycha et al.
(2020)
N.R. 290 Monitoring wells Taiwan Lu et al. (2016)
Codeine 106 348.3 Monitoring wells Spain Teijon et al. (2010)
< 23 214 Wells United States Fram & Belitz (2011)
Salicylic acid <1 29 Wells Canada Carrara et al. (2008)
6.55b 9.3c Monitoring wells and Spain Cabeza et al. (2012)
Piezometers
piezometers (2013)
(continued on next page)
6
Table 1 (continued )
L) L)
N.R. 2015 Wells China Peng et al. (2014)

< LOQ 2.5 Private wells Serbia Petrović et al. (2014)
Meclofenamic acid <1 43 Wells and Boreholes Nigeria Ebele et al. (2020)
Tramadol 26.4 186 Wells United States Elliott et al. (2018)
Antibiotics Doxycycline < 2.6 2000 Natural Springs Spain Gros et al. (2021)
Ciprofloxacin N.R. 596 Wells Pakistan Zainab et al. (2021)
44 14,000 Wells India Fick et al. (2009)
10 770 Wells India Rutgersson et al. (2014)
Sulphapyridine 1.3 766.1 Wells Spain Jurado et al. (2020)
Erythromycin N.D. 54.8 Shallow wells Taiwan Lin et al. (2015)
≈8 > 10 Private wells China Yang et al. (2018)
N.R. 52.2 Groundwater China (C. Huang et al., 2021)
Lincomycin N.R. 320 Wells, springs and sumps United States Barnes et al. (2008)
Sulfamethoxazole 50 27,410 Wells United States Kibuye et al. (2019a)
<5 113 Public wells United States Schaider et al. (2014)
7 965 Wells United States Elliott et al. (2018)
100 32,000 Private wells and springs United States Kibuye et al. (2019b)
N.R. 120 Wells and Springs United States Bexfield et al. (2019)
N.D. 27.7 Wells Spain Jurado et al. (2020)
N.R. 48 Groundwater Switzerland (Federal Office for the
Environment (FOEN),
2009)
0.8 17 Karst Springs and Swallow hole Switzerland Morasch (2013)
stations
0.2 1820 Shallow wells Taiwan Lin et al. (2015)
9b 46c Monitoring wells and Spain Cabeza et al. (2012)
Piezometers
< LOD 65 Pumping wells and observation Spain López-Serna et al.
piezometers (2013)
≈2 >5 Private wells China Yang et al. (2018)
0 20,060 Wells China Qin et al. (2020)
<2 1285 Boreholes, wells and springs Cameroon Branchet et al. (2019)
Sulfamethazine N.R. 360 Wells, springs and sumps United States Barnes et al. (2008)
1.6 28.9 Shallow wells Taiwan (Y. C. Lin et al., 2015)
Piezometers
14.6 29.2 Pumping wells and observation Spain López-Serna et al.
piezometers (2013)
N.D. 28.5 Wells Spain Jurado et al. (2020)
N.D. 1.2 Boreholes China Tong et al. (2014)
Trimethoprim 50 6950 Wells United States Kibuye et al. (2019a)
100 3200 Private wells and springs United States Kibuye et al. (2019b)
N.R. 14.9 Wells and Springs United States Bexfield et al. (2019)
0.869 9.41 Pumping wells and observation Spain López-Serna et al.
piezometers (2013)
N.D. 17.8 Shallow wells Taiwan Lin et al. (2015)
17 55 Wells India Fick et al. (2009)
Amoxicillin 44 6490 Wells and Boreholes Nigeria Ebele et al. (2020)
Ampicillin 200 700 Private wells and springs United States Kibuye et al. (2019b)
200 3690 Wells United States Kibuye et al. (2019a)
Ofloxacin 1500 114,940 Wells United States Kibuye et al. (2019a)
piezometers (2013)
N.D. 44.2 Wells China Peng et al. (2014)
< LOQ 9.4 Wells India Rutgersson et al. (2014)
7
L) L)

Enoxacin 80 1900 Wells India Fick et al. (2009)
Norfloxacin N.D. 9.3 Shallow wells Taiwan Lin et al. (2015)
0.3 2 Karst Springs and Swallow hole Switzerland Morasch (2013)
piezometers (2013)
< LOQ 145 Wells India Rutgersson et al. (2014)
Azithromycin 4 10 Karst Springs and Swallow hole Switzerland Morasch (2013)
piezometers (2013)
N.D. 68 Observation wells near Danube Serbia Radović et al. (2015)
River and tributaries
Beta- Blockers Metoprolol 2 9 Karst Springs and Swallow hole Switzerland Morasch (2013)
136 355 Pumping wells and observation Spain López-Serna et al.
piezometers (2013)
and Tisa Rivers
N.D. 90 Wells India Fick et al. (2009)
Atenolol 18 106 Monitoring wells Spain Teijon et al. (2010)
N.D. 3.6 Shallow wells Taiwan Lin et al. (2015)
Propanolol < LOD 9.38 Pumping wells and observation Spain López-Serna et al.
piezometers (2013)
< LOQ 4.5 Private wells Serbia Petrović et al. (2014)
Lipid Regulators Gemfibrozil <5 1.2 Public wells United States Schaider et al. (2014)
< 12 574 Monitoring wells Spain Teijon et al. (2010)
piezometers (2013)
Bezafibrate 1.42b 4.22c Monitoring wells and Spain Cabeza et al. (2012)
Piezometers
< LOD 25.8 Pumping wells and observation Spain López-Serna et al.
piezometers (2013)
Antiepileptics Carbamazepine < 30 420 Wells United States Fram & Belitz (2011)
<5 72 Public wells United States Schaider et al. (2014)
9.93 1000 Wells United States Elliott et al. (2018)
0 11 Wells United States McEachran et al. (2016)
N.R. 2325 Monitoring boreholes Europe Bunting et al. (2021)
stations
Piezometers
0.49 176 Wells Hungary Kondor et al. (2020)
N.R. 45 Groundwater Switzerland (Federal Office for the
Environment (FOEN),
2009)
< 0.3 35 Monitoring wells Germany Wolf et al. (2012)
< 0.3 9.3 Monitoring wells Singapore Tran et al. (2014)
5 3600 Groundwater United Stuart et al. (2011)
Kingdom
N.R. 890 Wells Czech Rozman et al. (2017)
Republic
N.R. 100 Springs and wells Jordan Zemann et al. (2015)
and Tisa Rivers
5 41 Observation wells near Danube Serbia Radović et al. (2015)
River and tributaries
N.D. > 10 Private wells China Yang et al. (2018)
<5 335 Boreholes, wells and springs Cameroon Branchet et al. (2019)
< 0.01 6.9 Wells Sri Lanka Do et al. (2021)
8
L) L)
0.1 67 Private or public wells India Richards et al. (2021)

Gabapentin <1 41 Wells and Boreholes Nigeria Ebele et al. (2020)
Phenytoin <5 66 Public wells United States Schaider et al. (2014)
Lamotrigine 5.18 849 Wells Hungary Kondor et al. (2020)
Antidepressant Citalopram N.R. 7.4 Wells and Springs United States Bexfield et al. (2019)
Venlafaxine < 40.6 134 Monitoring wells Spain Teijon et al. (2010)
Antihistamine Cetrizine 550 28,000 Wells India Fick et al. (2009)
Stimulant Caffeine 50 14,150 Wells United States Kibuye et al. (2019a)
6 25 Wells United States McEachran et al. (2016)
N.R. 14,770 Groundwater in WWTP Vicinity Spain Bunting et al. (2021)
10b 55.5c Monitoring wells and Spain Cabeza et al. (2012)
Piezometers
< LOD 1528 Groundwater wells Bay of Puck Szymczycha et al.
(2020)
stations
< 6.0 16,249 Monitoring wells Singapore Tran et al. (2014)
≈ 10 > 50 Private wells China Yang et al. (2018)
15 262 Hand pumps along Ganges River India Sharma et al. (2019)
Amphetamine N.R. 68.3 Monitoring wells Taiwan Lu et al. (2016)
Estrogen 17α-Ethynylestradiol N.D. 1822.2 Shallow wells Taiwan Lin et al. (2015)
Antagonist Valsartan <1 84 Wells and Boreholes Nigeria Ebele et al. (2020)
Cimetidine N.R. 23.6 Wells and Springs United States Bexfield et al. (2019)
Antifungal Clotrimazole <1 191 Wells and Boreholes Nigeria Ebele et al. (2020)
Terbinafine 90 1800 Wells India Fick et al. (2009)
Antiviral Acyclovir N.R. 5.7 Wells and Springs United States Bexfield et al. (2019)
Biguanides Metformin 75.6 206 Wells United States Elliott et al. (2018)
< 0.5 349 Wells and Boreholes Nigeria Ebele et al. (2020)
Tranquilizers Flunitrazepam N.R. 196 Monitoring wells Taiwan Lu et al. (2016)
Metabolites Para-xanthine (Caffeine) N.R. 57 Wells, springs and sumps United States Barnes et al. (2008)
N-formyl-4-amino- < 21 416 Wells and Springs United States Bexfield et al. (2019)
antipyrine (Metamizole) 27 275 Monitoring wells Spain Teijon et al. (2010)
and Tisa Rivers
N-acetyl-4-amino- 1 362 Monitoring wells Spain Teijon et al. (2010)
antipyrine (Metamizole) 5 128 Wells in the immediate vicinity Serbia Kovačević et al. (2017)
and Tisa Rivers
Clofibric acid < 10 1350 Monitoring wells Germany Wolf et al. (2012)
(Clofibrate) < LOD 7.57 Pumping wells and observation Spain López-Serna et al.
piezometers (2013)
LOD – Limit of detection.

LOQ – Limit of quantification.
N.R. – Not reported.
N.D. – Not detected.
a
Maximum Concentration in ng/mL.
b
Minimum mean concentration in ng/L.
c
Maximum mean concentration in ng/L.
future economies of the world. to conclude whether there is any relation among detection of PPCPs and
Likewise, graphical comparisons have been made among countries countries or not.
based upon the maximum concentration of these pharmaceutical com From Fig. 3 and Table 1, it can be deduced that groundwater of U.S.
pounds found in their groundwater. This graph will help to set an un A. is highly contaminated, with the maximum concentration of carba
derstanding about a country using or discharging various therapeutic mazepine belonging to the class antiepileptics, having a concentration of
class drugs. Later, from the trend of this graph an attempt has been made 1000 ng/L (Elliott et al., 2018). Even the concentration of caffeine
9
Fig. 2. Box-plot of various PPCPs therapeutic classes

with their maximum concentrations. The bottom and
top of the box represents first and third quartile,
respectively and the cross mark represents the mean
value of all the reported values in the groundwater.
Highest concentration for diclofenac (1,390,000 ng/
L) of analgesics/NSAIDs class is not shown as outlier.
Metabolites are included as one of the PPCPs thera
peutic class owing to their capability of producing the
desired therapeutic effects in active form. Metabolites
box-plot is prepared based on the spectrum of it in
groundwater since last one and half decade (included
in Table 1).
Table 2
Maximum concentration (in ng/L) of various PPCPs therapeutic classes reported in respective countries groundwater system since last one and half decade.
Therapeutic Class U.S.A. Switzerland Taiwan Nigeria Spain India
Analgesics/Antipyretics/NSAIDs 98,390 12 1036 2440 988 1,390,000

Antibiotics 122,700 48 1820 6490 2000 14,000
Beta Blockers 8.7 9 3.6 54 355 90
Antiepileptics 1000 45 37.9 50 118 67
a
Stimulants 14,150 N.R. 930.7 166 14,770 262
a a
Lipid Regulators 1.2 N.R. 172.3 730 751 N.R.
a
N.R.- Not reported.
(stimulant) was also reported at a high concentration of 14,150 ng/L in (López-Serna et al., 2013) followed by India, a developing nation having
the groundwater of Unites States (Kibuye et al., 2019a). These ostensible a maximum concentration of 90 ng/L (Fick et al., 2009) for metoprolol
data give an idea that the usage of these pharmaceutical compounds is which is way higher than the atenolol’s (beta blockers) maximum
common among the population of U.S.A. Although, the consumption of contamination found in the wells and springs of U.S.A. (8.7 ng/L)
caffeine is among the highest in India yet it showed only 262 ng/L of (Bexfield et al., 2019). Similarly, for lipid regulators, Spain was again
concentration in its groundwater (Sharma et al., 2019) as compared found to be polluted with the maximum concentration of gemfibrozil
with other countries in the given graph. Meanwhile, the maximum (751 ng/L) (López-Serna et al., 2013) closely followed by the maximum
concentration of caffeine in Spain was recorded up to 14,770 ng/L concentration in Nigerian wells and boreholes (730 ng/L) (Ebele et al.,
(Bunting et al., 2021), which is highest among all the countries 2020). The concentration of lipid regulators found in Nigeria was much
compared in this graph. higher than those of American public wells (1.2 ng/L) (Schaider et al.,
In Fig. 3 and Table 1, comparison between the analgesics/NSAIDs 2014), meanwhile no study for determination of traces of lipid regula
and antibiotics classes have been presented. U.S.A.‘s groundwater was tors in groundwater of Switzerland and India has been reported.
mostly contaminated with naproxen (analgesics/NSAIDs) with a huge Another depiction of occurrence of PPCPs in groundwater is repre
concentration of 98,390 ng/L (Kibuye et al., 2019a). Maximum con sented in Fig. 4, highlighting the range of the contaminants in above
centration of antibiotics standing at 122,700 ng/L was detected in the included 6 countries. The given figure demonstrates the minimum and
private wells and springs of U.S.A. for ofloxacin compound (Kibuye maximum range of all the six therapeutic classes included in Fig. 4 along
et al., 2019b). Even Indian wells were also found to be contaminated with the mention of sites where these classes were detected. It can be
with ciprofloxacin compound belonging to antibiotics class having a postulated that Spain and Switzerland displayed a diminutive level of
maximum concentration of 14,000 ng/L (Fick et al., 2009). Earlier, it concentration of all the therapeutic classes taken into consideration
was assumed that the compounds which were present in heavy con except for stimulants in Spain. On the other side, United States’
centrations in groundwater of developed countries like U.S.A. and other groundwater was severely infested with analgesics and antibiotics
European countries may not be present at a similar abundance in ranging from (0–98390 ng/L) and (0–122,700 ng/L) respectively. Sce
developing countries like India or Nigeria. Even Nigeria showed a high nario of Indian groundwater shows heavy prevalence of analgesics and
concentration (6490 ng/L) of amoxicillin compound of antibiotic class antibiotics in its groundwater which could range from as low as 150 and
in its groundwater (Ebele et al., 2020), which is higher than the 10 ng/L and could spike up to 1,390,000 and 14,000 ng/L, respectively.
maximum concentration of antibiotics reported in the groundwater of For Nigeria, its wells and boreholes were infested with antibiotics
other developed countries like Spain (2000 ng/L) (Gros et al., 2021), (<1–6490 ng/L) while Taiwanese groundwater showed moderate
Taiwan (1820 ng/L) (Lin et al., 2015) or Switzerland (48 ng/L) (Federal presence of every therapeutic class.
Office for the Environment (FOEN), 2009).
Similarly, in Fig. 3 comparison between the beta blocker and lipid 4. Current global trends of PPCPs in groundwater
regulator classes have been presented. Maximum concentration of
metoprolol (beta blocker) was found in the pumping wells of Spain In earlier section of tabular and pictorial representations, the
which is a developed European country, peaked at 355 ng/L occurrence of some PPCPs in global groundwater system in last one and
10
Fig. 3. Graphs comparing PPCPs in ng/L, therapeutic classes (antiepileptics and stimulant), (β-blockers and lipid regulators) in ng/Land therapeutic classes (an
algesics/NSAIDs and antibiotics) in ng/L in logarithmic scale.
half decade is demonstrated. Recently, there has been a surge in number pollution bulletin of mentioned countries encompassing almost every
of studies published on PPCPs detection in groundwater worldwide. continent of the world.
Henceforth, itis important to know that at what extent PPCPs has
reached the groundwater system in various countries of the world. The
following extent/reach has been depicted in Fig. 5(a) and (b) and 5(c) 4.1. Trend in 2019
informing about the contamination of groundwater from three major
contaminants of emerging concern (CECs) namely (a) agriculture-based Looking at the 2019 trend of contamination of groundwater with
chemicals (pesticides and veterinary chemicals), (b) PCPs and (c) agricultural chemicals, which include pesticides, West Indies has been
pharmaceutical products. adversely affected with a high concentration of 700 ng/L of hydroxy
Furthermore, Fig. 5(a), (b) and 5(c) give us an idea about the current chlorothanonil, a fungicide (Edwards et al., 2019). Alarming situation
trends and geographical extent of these compounds in groundwater. prevails in the groundwater of East China where concentration of 1,1,
These trends can also be used to determine the country which needs to 2-trichloroethane reached at 759 mg/L in its monitoring wells (Yang
be proactive into the formulation and promulgation of rules and regu et al., 2019). From this data, it can be deduced that discharge of un
lations regarding PPCPs polluting their groundwater. The information treated or partial treated effluents from chemical formulation facilities
on the type of contaminants detected in groundwater through these in the environmental compartments and excessive use of these chem
trends can explain types of chemicals and drugs being used in those icals in agriculture sector are the major sources through which these
respective countries and can give us an extent of recent groundwater chemicals leach into the groundwater system in significant amount.
Reviewing contamination of groundwater by PCPs, usual prevalence of
11
R. Silori et al.
12
Journal of Environmental Management 320 (2022) 115703

Fig. 4. Range of PPCPs’ contamination of all the therapeutic classes (analgesics, antiepileptics, β-blockers, antibiotics, lipid regulators and stimulants) in United States, Spain, Switzerland, Nigeria, India and Taiwan. The
information provided follows this sequence: Therapeutic class- (range) – maximum contamination detected site. (*)- Only maximum concentration of the given therapeutic class. AG, AB, β-B, AP. LR, ST stands for
Analgesics, Antibiotics, β-blockers, Antiepileptics, Lipid regulators and Stimulant therapeutic classes respectively.
Fig. 5. Prevalence of CECs reported in groundwater in different parts of the world for the year (a) 2019, (b) 2020, (c) 2021.
13
triclosan and triclocarbon has been detected in every corner of the • Studies specifically from African countries highlighted that major
world; stretching from India (Sharma et al., 2019), China (Wang et al., contaminated site were near rubber/asphalt processing industries,
2019) to African countries like Nigeria and Zambia (Offiong et al., sanitary landfills and hospitals. Further, triclosan, herbicides and
2019). Studies related to pharmaceutical compounds occurrence in insecticides were traced backwards to residential areas.
groundwater reveals that numerous appearances of antibiotics detected • The data present us a clear image that irrespective of country,
in China (Huang et al., 2019; Jiang et al., 2019; Liu et al., 2019) where it continent or hemisphere, the groundwater is found to be equally
has been detected at a maximum concentration of 508.6 ng/L whereas affected with the presence of these contaminants of emerging
U.S.A. witnessed a highest concentration of analgesics standing at 15, concern.
580 ng/L (Kibuye et al., 2019a). The other key observations for CECs • Our study showcases that we are seeing a surge in the contamination,
contamination in groundwater reported in other countries in 2019 are and it is only going to accumulate as the time ensues, more studies
depicted in Fig. 5(a) (Lee et al., 2019; Moreau et al., 2019; Sjerps et al., and investigations are required in this field.
2019). • It is essential to know the fate of PPCPs inside the soil and ground
water system. We suggest that development of new methodologies
4.2. Trend in 2020 encompassing the concept of mobilization through soil media by
considering several factors like porosity, void ratio, degree of satu
Hintze et al. (2020) studied the prevalence of agriculture-based ration, air content etc. and life cycle of these PPCPs would be helpful
chemicals in groundwater of Switzerland and found 2300 ng/L of in determining the fate of these contaminants in groundwater.
desphenyl-chloridazone which is a herbicide. In France, 96% of • Study of these PPCPs in groundwater can be very complicated, less
groundwater extracts were found to be contaminated with diuron, accurate, taxing and time-consuming. Most often, their detection
which is also a herbicide (Pinasseau et al., 2020). Colossal amount of Bis entails expensive and sensitive equipment and skilled personal to
(2-ethylhexyl phthalate) which is a constituent of plasticizer used as operate it.
PCPs was detected at the highest concentration of 220,000 ng/L in • Providing in-situ tracing and remediation measures such as intro
groundwater of Mexico (Cruz-López et al., 2020). For pharmaceutical ducing tracer chemicals and adsorbent materials to analyze the
contaminants, Hungarian groundwater was found to be polluted with extent and severity of contamination of groundwater would be very
carbamazepine (176 ng/L) and lamotrigine (849 ng/L) (Kondor et al., helpful in saving ample amount of time. It will be much helpful in
2020). In Nigerian groundwater, high concentration of amoxicillin providing us the desired result by-passing tedious procedures.
belonging to antibiotics group was found at 6490 ng/L (Ebele et al., • Henceforth, more studies should incorporate mineralogical charac
2020). Another antibiotic’s subclass, sulfonamides, were found to be teristics of various types of soil. Knowledge about soil property could
heavily contaminated in the groundwater of China at a concentration of be helpful in predicting the fate and extent of PPCPs mixed with
20,060 ng/L (Qin et al., 2020). The other key observations for CECs irrigation water which might be lurching downwards to meet
contamination in groundwater reported in other countries in 2020 are groundwater through vadose zone.
depicted in Fig. 5(b) (Duttagupta et al., 2020; Jurado et al., 2020;
Kotowska et al., 2020; B. B. Li et al., 2020; X. Li et al., 2020; Suciu et al., Consent for publication
2020; Szymczycha et al., 2020; Wu et al., 2020; Zambito Zambito
Marsala et al., 2020). The submitted MS is original and not published or submitted to any
other journal for publication. The publisher has the consent to publish
4.3. Trend in 2021 the paper, if accepted.
The trend of 2021 shows that DEET, an insect repellant, was ubiq Credit author statement
uitous in the European groundwater (Bunting et al., 2021). U.S.
groundwater is facing a grave concern with regards to pesticides with a RS: Original Draft, Reviewing, Editing and Data curation. VS: Orig
range starting from as low as 3 ng/L and shooting up till 3,68,00 ng/L inal Draft, Reviewing, Editing and Data curation. AS: Reviewing and
(Fisher et al., 2021). Galaxolide, which is used in fragrance and odor Editing. PS: Reviewing and Editing. JM: Reviewing and Editing. MK:
products had been commonly found in the groundwater of Spain with a Conceptualization, Project Supervision, Reviewing, Editing and Final
range of 435–3130 ng/L (Llamas-Dios et al., 2021). In 2021, concen Draft.
tration of carbamazepine (antiepileptics) and caffeine (stimulant) was
found in the groundwater of Europe at an enormous concentration of
2300 and 14,800 ng/L respectively (Bunting et al., 2021). Carbamaze Declaration of competing interest
pine was also detected in the groundwater of Patna, India at a concen
tration of 67 ng/L (Richards et al., 2021). The other key observations for The authors declare that they have no known competing financial
CECs contamination in groundwater reported in other countries in 2021 interests or personal relationships that could have appeared to influence
are depicted in Fig. 5(c) (Do et al., 2021; Gros et al., 2021; Huang et al., the work reported in this paper.
2021; Kiefer et al., 2021; Michel et al., 2021; Mooney et al., 2021;
Rusiniak et al., 2021; Zainab et al., 2021). Acknowledgements
5. Conclusion The author acknowledges the contribution of University of Petro

leum and Energy Studies, Dehradun in providing an excellent research
This study tried to summaries the circumstance of PPCPs occurrence infrastructure that helped in conceptualizing the present study.
and its expanding footholds in groundwater across the world. However,
future research into the PPCPs occurrence, fate and remediation mea
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Journal of Environmental Management 320 (2022) 115703

Contents lists available at ScienceDirect

Journal of Environmental Management

Global groundwater vulnerability for Pharmaceutical and Personal care

* Corresponding author. Energy Acres, UPES, Dehradun, Uttarakhand, 248007, India.

Analgesics/ Acetaminophen 50 15,580 Wells U. S Kibuye et al. (2019a)

N.R. 2015 Wells China Peng et al. (2014)

26 480 Wells India Fick et al. (2009)

0.1 67 Private or public wells India Richards et al. (2021)

LOD – Limit of detection.

Fig. 2. Box-plot of various PPCPs therapeutic classes

Analgesics/Antipyretics/NSAIDs 98,390 12 1036 2440 988 1,390,000

Journal of Environmental Management 320 (2022) 115703

5. Conclusion The author acknowledges the contribution of University of Petro

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1 s2.0 S0301479722012762 Main

Uploaded by

Document Information

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Copyright

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Did you find this document useful?

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1 s2.0 S0301479722012762 Main

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Copyright:

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Journal of Environmental Management 320 (2022) 115703

Contents lists available at ScienceDirect

Journal of Environmental Management

Global groundwater vulnerability for Pharmaceutical and Personal care

* Corresponding author. Energy Acres, UPES, Dehradun, Uttarakhand, 248007, India.

Analgesics/ Acetaminophen 50 15,580 Wells U. S Kibuye et al. (2019a)

N.R. 2015 Wells China Peng et al. (2014)

26 480 Wells India Fick et al. (2009)

0.1 67 Private or public wells India Richards et al. (2021)

LOD – Limit of detection.

Fig. 2. Box-plot of various PPCPs therapeutic classes

Analgesics/Antipyretics/NSAIDs 98,390 12 1036 2440 988 1,390,000

Journal of Environmental Management 320 (2022) 115703

5. Conclusion The author acknowledges the contribution of University of Petro­

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5. Conclusion The author acknowledges the contribution of University of Petro