Environmental Pollution 208 (2016) 704e713

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Environmental Pollution
journal homepage: www.elsevier.com/locate/envpol

Perfluoroalkyl substances (PFAS) in river and ground/drinking water

of the Ganges River basin: Emissions and implications for human
exposure
Brij Mohan Sharma a, *, Girija K. Bharat b, Shresth Tayal a, b, Thorjørn Larssen c,
Jitka Be
 d, Pavlína Kara
canova skova  d, Paul G. Whitehead e, Martyn N. Futter f,
g c, d, **
Dan Butterfield , Luca Nizzetto
a
TERI University, 10 Institutional Area, Vasant Kunj, New Delhi 110070, India
b
The Energy and Resources Institute (TERI), Darbari Seth Block, India Habitat Centre, Lodhi Road, New Delhi 110003, India
c
Norwegian Institute for Water Research (NIVA), Gaustadall een 21, Oslo 0349, Norway
d
Research Centre for Toxic Compounds in the Environment (RECETOX), Masaryk University, Brno 62500, Czech Republic
e
School of Geography and the Environment, University of Oxford, Oxford OX1 3QY, United Kingdom
f
Department of Aquatic Sciences and Assessment, Swedish University of Agricultural Sciences, SE-75007 Uppsala, Sweden
g
Enmosys, Glen Ellyn, IL 60138, USA

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

Article history: Many perfluoroalkyl substances (PFAS) are ubiquitous environmental contaminants. They have been
Received 17 August 2015 widely used in production processes and daily-use products or may result from degradation of precursor
Received in revised form compounds in products or the environment. India, with its developing industrialization and population
25 October 2015
moving from traditional to contemporary lifestyles, represents an interesting case study to investigate
Accepted 26 October 2015
PFAS emission and exposure along steep environmental and socioeconomic gradients. This study as-
sesses PFAS concentrations in river and groundwater (used in this region as drinking water) from several
locations along the Ganges River and estimates direct emissions, specifically for PFOS and PFOA. 15 PFAS
Keywords:
Perfluoroalkyl substances
were frequently detected in the river with the highest concentrations observed for PFHxA (0.4
Ganges River e4.7 ng L
1) and PFBS (<MQL e 10.2 ng L
1) among PFCAs and PFSAs, respectively. Prevalence of short-
Emissions chain PFAS indicates that the effects of PFOA and PFOS substitution are visible in environmental samples
Groundwater from India. The spatial pattern of C5eC7 PFCAs co-varied with that of PFOS suggesting similar emission
Human exposure drivers. PFDA and PFNA had much lower concentrations and covaried with PFOA especially in two
hotspots downstream of Kanpur and Patna. PFOS and PFOA emissions to the river varied dramatically
along the transect (0.20e190 and 0.03e150 g d
1, respectively). PFOS emission pattern could be
explained by the number of urban residents in the subcatchment (rather than total population). Per-
capita emissions were lower than in many developed countries. In groundwater, PFBA (<MQL e
9.2 ng L
1) and PFBS (<MQL e 4.9 ng L
1) had the highest concentrations among PFCAs and PFSAs,
respectively. Concentrations and trends in groundwater were generally similar to those observed in
surface water suggesting the aquifer was contaminated by wastewater receiving river water. Daily PFAS
exposure intakes through drinking water were below safety thresholds for oral non-cancer risk in all age
groups.
© 2015 Elsevier Ltd. All rights reserved.

1. Introduction

* Corresponding author. Department of Natural Resources, TERI University, 10
Institutional Area, Vasant Kunj, New Delhi 110070, India.
** Corresponding author. Norwegian Institute for Water Research (NIVA),
Gaustadalleen 21, Oslo 0349, Norway.
E-mail addresses: brijmsharma05@gmail.com (B.M. Sharma), luca.nizzetto@
niva.no (L. Nizzetto).
The environmental occurrence of perfluoroalkyl substances
(PFAS) and in particular perfluorocarboxylic acids (PFCAs) such as
perfluorooctanoic acid (PFOA), perfluorosulfonates (PFSAs) such as
perfluorooctane sulfonate (PFOS), and perfluorosulfonamides
(PFOSAs) has received particular attention by both scientists and

http://dx.doi.org/10.1016/j.envpol.2015.10.050
0269-7491/© 2015 Elsevier Ltd. All rights reserved.
 B.M. Sharma et al. / Environmental Pollution 208 (2016) 704e713
regulators because of their ubiquitous distribution (underpinning
exposure to humans and biota) and associated toxicological out-
comes (Buck et al., 2011; Corsini et al., 2014; Domingo, 2012; Houde
et al., 2006). PFAS include chemicals used in industrial processing
or as additives in consumer products. Direct emissions to the at-
mosphere and wastewater during production and consumption of
PFSA-containing articles (Prevedouros et al., 2006) and atmo-
spheric, riverine, or marine transports are the prevalent pathways
for ecosystem exposure (Ahrens et al., 2009; Castiglioni et al., 2015;
Filipovic et al., 2013; Simcik and Dorweiler, 2005).
Some PFAS such as PFOA and PFOS are resistant to biological and
chemical degradation in natural environment (Lindstrom et al.,
2011) and can accumulate in organisms. PFOA and PFOS are
found in human serum and milk (Fu et al., 2014b; Tao et al., 2008).
Laboratory tests showed that high concentrations of PFAS can
impair immune and endocrine systems, and cause cancer (Corsini
et al., 2014; Jensen and Leffers, 2008). The widespread presence
of these substances in the general population has been reported
from different regions especially in developed western countries
(Dallaire et al., 2009; Olsen et al., 2009; Steenland et al., 2010).
However, human exposure patterns have not yet been fully
elucidated.
PFAS are among the primary concerns for environmental and
health protection authorities both nationally and internationally.
PFOS and its salts have been included as new persistent organic
pollutants (POPs) by the Stockholm Convention (SC) (UNEP, 2010).
The European Chemical Agency has included ammonium penta-
decafluorooctanoate (APFO), PFOA, and C11eC14 PFCAs in the
candidate list of substances of very high concern (ECHA, 2015). The
EU Water Framework Directive had specified environmental qual-
ity standards (EQS) of 0.65 ng L
1 for PFOS (EC, 2013), and proposed
restrictions on manufacturing, use or market distribution of PFOA
(ECHA, 2014). The US Environmental Protection Agency has
established provisional thresholds of 400 and 200 ng L
1 for PFOA
and PFOS in drinking water, respectively (USEPA, 2009, 2011). The
Swedish National Food Agency has recently introduced a conser-
vative “limit of action threshold” of 90 ng L
1 for the sum of seven
PFASs (PFBS, PFHxS, PFOS, PFPeA, PFHxA, PFHpA, and PFOA) for
drinking water (Englund, 2015). Recently, the Chinese Ministry of
Environment Protection drafted a list of priority hazardous chem-
icals for environmental management including PFOS and its salts.
However, no threshold limits for PFOS or other PFAS environmental
concentrations have been specified yet (SAWS, 2015). In contrast,
India has not updated its SC National Implementation Plan for PFOS
and no specific national guidelines or EQS exist for the manage-
ment of PFAS and other priority hazardous chemicals. In addition,
the analysis of PFAS contamination status in India has been so far
hampered by the scarcity of data.
With the exception of several case studies in China (e.g. (Pan
et al., 2014; So et al., 2007; Sun et al., 2011; Wang et al., 2013;
Yang et al., 2011)), data on PFAS environmental concentrations
and emissions are generally very scarce from developing countries
as is information on human exposure (Fu et al., 2014a, 2014b;
Guruge et al., 2005; Tao et al., 2008; Yeung et al., 2009). Assess-
ments of PFAS emission, contamination and human exposure in
highly industrialized developing countries are urgently needed.
With a growing share of the population adopting new and more
sophisticated consumption habits, the enormous production of
poorly managed waste, and the ongoing delocalization of the flu-
orochemical industry from developed countries (Li et al., 2015),
some areas of developing countries may, in fact, represent impor-
tant contamination hotspots.
In recent years, various studies focused on elucidating the
emission, distribution, fate and transport of PFASs using both
monitoring and modeling approaches (Castiglioni et al., 2015;
705
Filipovic et al., 2013; Li et al., 2015; Liu et al., 2015b; Wang et al.,
2014b). In this study, we focused on Northern India as one of the
emerging industrial regions in the global economic panorama, for
which data on PFAS environmental and human exposure are still
very limited. Here, a comprehensive assessment of the occurrence
of 21 PFAS in water resources of the Ganges River basin in India is
presented. The Ganges River is one of the largest rivers in the world
supporting the livelihood of 7% of the world's population and
serving as habitat of a rich and endangered biodiversity (CPCB,
2013). The monitored matrices included surface water and
groundwater, which is used as untreated drinking water by a ma-
jority of the urban and rural population. One aim of the study was
to estimate direct discharges of selected PFAS to surface waters in
sections of the river with contrasting socioeconomic conditions and
to elaborate a framework to explain the observed variability as a
function of socioeconomic data. An additional aim of the study was
to assess exposure patterns of drinking water resources used by
local populations and derive an assessment of human exposure
through drinking water consumption.
2. Materials and methods
2.1. Study area and sample collection
The Ganges is the largest river in India with a basin of
861,452 km2 and an average annual discharge of 12,400 m3 s
1. Its
catchment includes areas with diverse climate (varying from alpine
to tropical conditions) (MoWR, 2014; UNESCO, 1971). The sampling
campaign encompassed nine locations: two along the Bhagirathi
River (the main source of the Ganges River originating from the
Gangotri Glacier in the Himalayas); one along Alaknanda River
(another major tributary of Ganges); and one in the Himalayan
Reach (HR) of the Ganges main stream after the confluence of these
two tributaries. Two locations were selected in densely populated
and industrialized areas in the Middle Reach (MR), and three lo-
cations in the Ganges Lower Reach including its estuary. In total, 14
samples of river water and 14 samples of groundwater (collected
from wells in the vicinity of the river bank) were analyzed covering
the transect of 2525 km (Fig. 1). These samples were obtained
during FebruaryeApril 2014. More details of the sampling locations
are presented in Supplementary Table S1.
The simultaneous sampling of river water and groundwater was
performed so as to obtain information on possible co-variation of
contamination of drinking water resources with surface water re-
sources receiving domestic and industrial wastewater. In addition,
we explored such a long and complex transect so as to capture
variations in exposure levels both at a regional scale (by collecting
samples along the entire course of the Ganges River and its head-
waters) and locally (by estimating the variance between PFAS
concentrations in river sections immediately upstream (U) and
downstream (D) of major cities/town (namely: Uttarkashi (UKU,
UKD), Devprayag (DBG, DAK, DGR), Kanpur (KU, KD), Varanasi (VU,
VD), Patna (PU, PD), Farakka (FU, FD)) and Gangasagar (GS).
Grab bulk water samples (1 L) were collected from each sam-
pling location using high density polyethylene (HDPE) bottles, pre-
cleaned by thorough rinsing with MilliQ water and methanol.
River water samples were collected by a boat from the middle of
the river, with the exception of locations in HR where samples were
collected directly from the river bank taking advantage of the
relatively narrow channel and high mixing of turbulent water.
Groundwater was sampled from wells located less than 5 km from
the river bank using hand-pumps. Piping and the pump itself were
flushed at high flow for 2 min before samples were collected. Prior
to sample collection, bottles were rinsed at least twice with the
same water. Samples were kept in an icebox and transported to the
706 B.M. Sharma et al. / Environmental Pollution 208 (2016) 704e713
Fig. 1. Sampling locations and population density (people km
2) in the Ganges River basin. Sampling locations in HR have been magnified in the topright corner of the figure.
TERI laboratory where they were temporarily stored frozen until
they were shipped (cooled at 4  C) to the Czech Republic. Analysis
was conducted in the RECETOX laboratory in Brno, Czech Republic.
2.2. Chemical analysis and quality assurance/quality control
A detailed description of sample extraction, chemicals, analyt-
ical methods, and quality assurance and control measures is re-
ported in the supplementary information, Text S1.
2.3. PFAS emission estimates
One aim of the study was to derive direct emission estimates of
PFAS to river water from wastewater discharges in different sec-
tions of the river by combining experimental data and calculations
from a hydrobiogeochemical multimedia fate model (Nizzetto et al.,
in review). The analysis was carried out for PFOS and PFOA. These
substances were selected for: i) being the PFAS of currently highest
concern; ii) having relatively well established modeling frames and
physical chemical data (Armitage et al., 2009a, 2009b) and available
information on atmospheric deposition and concentrations for use
as inputs to the fate model (Kwok et al., 2010); iii) and, being a good
proxy for the spatial concentration pattern of several other PFAS
(namely, PFPA, PFHxA and PFHpA for PFOS, and PFNA, PFDA for
PFOA).
Sampling points for emissions analysis were selected to reflect
subcatchment scenarios with contrasting socioeconomic condi-
tions. In total, 5 subcatchments were selected covering a very steep
gradient of land use and human presence/impact including rural
mountain areas, heavily populated and industrialized districts with
large urban populations, and heavily populated agricultural
districts with a low proportion of urban residents. Details are re-
ported in Supplementary Figure S1a, b.
In order to carry out emission estimates, the newly developed
INCA-Contaminants model was used (Nizzetto et al., in review).
This integrative model dynamically describes hydro-
biogeochemical processes and multimedia contaminant fate with
a daily time resolution and high fidelity in river water discharge
prediction. The complex hydrology of the Ganges River system and
river flow regime variability in space and time is simulated with a
high level of detail as a function of meteorology and soil/river bed
conditions. Information on performance of the hydrological module
configuration for the Ganges River can be found elsewhere (Jin
et al., 2015; Whitehead et al., 2015). Information on scenario defi-
nition and input climate data is also reported elsewhere
(Whitehead et al., 2015). Furthermore, INCA- Contaminants de-
scribes organic carbon (Futter et al., 2007), and suspended sedi-
ment (Lazar et al., 2010) dynamics using previously published and
validated equations. A thorough calibration was conducted to
ensure modeled suspended sediments and organic carbon con-
centrations were in the ranges of those published in two previous
studies (Aucour et al., 2006; Chakrapani et al., 1995). Due to their
hydrophilic properties PFOS and PFOA are expected to be little
sensitive to the influence of partitioning onto suspended sedi-
ments. In particular, pH levels measured in river water ranging
between 7 and 8 suggest that PFOA (with a pKa <4) (Armitage et al.,
2009a; Burns et al., 2008; Goss, 2008; Goss and Arp, 2009) is pre-
sent in water predominantly in the highly hydrophilic dissociated
form (PFO). In contrast, PFOS is present in the environment pre-
dominantly in the non-ionic form.
In order to simulate multimedia contaminant fate, INCA-
Contaminants model was parameterized with compound specific
 B.M. Sharma et al. / Environmental Pollution 208 (2016) 704e713
Fig. 2. Concentrations of various PFAS in the Ganges at different sampling sites (logarithmic scale, base 10).
physicalechemical properties, emission scenarios (including inputs
from the atmosphere, and direct discharges to the catchment soils
or stream water and sediments) and a set of parameters governing
exchange and reaction of contaminants within and across different
environmental phases. The set of physicalechemical properties
used by Armitage et al., were also used here (Armitage et al., 2009a,
2009b). In order to initialize the model, PFOS and PFOA atmo-
spheric concentration (0.2 pg m
3) and wet deposition (0.04,
0.21 ng L
1, respectively) inputs were specified based on available
monitoring data in the region (Kwok et al., 2010) or regions with
possibly similar characteristics (in terms of land use) (Goosey and
Harrad, 2012). This provided an approximation of the “back-
ground” concentrations expected in river water. In order to esti-
mate ranges of direct PFOS anthropogenic discharges to the river in
individual sections, the model was run in a “reverse-mode” to find
the value of direct PFOS and PFOA discharge to water (E(ng day
1))
producing river discharge outputs that best matched the 95% un-
certainty boundaries of the distribution river discharges estimated
apriori from monitored data. These distributions were assumed to
be normal and contained within the order of magnitude centered
on the measured discharge flux of the contaminants in each of the
selected river sections (obtained by multiplying measured con-
centrations and river discharge). Such an approach was used so as
to take into account (as a first approximation) the cumulative un-
certainty associated with concentration measurements and river
discharge simulations.
In order to calculate subcatchment specific PFOS and PFOA
discharges (ES) a Monte Carlo frame was used in which randomly-
drawn E values (Er,D) from the distribution pertinent to one selected
river section were subtracted from randomly extracted E values
(Er,U) from the apriori distribution of the nearest upstream section.
This operation was repeated (N ¼ 10,000) in order to derive a
distribution of subcatchment specific discharges to the river. A
conditional function was introduced that excluded any negative
estimates of ES (which were assumed to result from combined er-
rors in concentration measurements and simulated river water
discharge). This frame generated the distribution of ES estimates.
3. Results and discussion
3.1. PFAS in the surface water of the Ganges
Among the 21 analyzed PFAS, 15 compounds were detected in
one or more locations. A summary of measured river water con-
centration is presented in Fig. 2 and Supplementary Table S6. Total
PFAS concentration in the Ganges River water samples ranged
1.3e15.9 ng L
1. PFAS with C5eC8 were detected more frequently
707
than C9eC14. PFHxA, PFHpA, and PFOA were the only compounds
that were detected in all the sampling locations, while PFUnDA,
PFTeDA, MeFOSA, EtFOSA, MeFOSE and EtFOSE were not detected
in any of the river samples. Highest concentrations among PFCAs
and PFSAs were measured for PFHxA (0.4e4.7 ng L
1) and PFBS
(<MQL e 10.2 ng L
1), respectively, despite PFBS not having been
detected in most of the locations in the middle and lower reaches
due to high MQL. Concentrations of PFOA and PFOS ranged between
0.1 and 1.2 ng L
1 and <MQL e 1.7 ng L
1, respectively.
PFSAs concentrations in the Ganges were lower than concen-
trations reported in rivers from Japan, China, Italy, and North-East
Spain; while they were in the same range as those detected in
some rivers in Germany, Vietnam, and Brazil (Supplementary
Table S7 presents a detailed comparison between this study data
and data from literature).
It is generally assumed that industrial and municipal solid and
liquid waste is the major source of PFAS to the environment
(Armitage et al., 2006; Prevedouros et al., 2006). It has also been
suggested that long range atmospheric transport of volatile com-
pounds including FTOHs, FTOs, and PFOSAs, and their subsequent
degradation to mostly odd carbon chain length PFAS results in
contamination in remote regions (Li et al., 2011; Simcik and
Dorweiler, 2005). Atmospheric deposition may therefore be a
possibly relevant source for surface water contamination in remote
environments with low anthropogenic impacts. In the Ganges, due
to the large river section, huge catchment and high dilution, at-
mospheric inputs of some PFAS may be important sources espe-
cially in areas of the catchment (such as the HR) with a relatively
low anthropogenic impact.
In our study, concentrations of PFOA were lower than those of
PFHxA, PFHpA, and PFPA by a factor 1.7e16 in all river sections
(including both highly anthropic regions of the Gangetic plain). In
addition the spatial distribution of C5eC8 PFCA concentrations in
river water was strongly positively correlated (P < 0.01; R
(Spearman) ¼ 0.8e0.95) (Supplementary Table S8), and had con-
centrations measured downstream of the major conurbations
typically higher than those measured upstream. This indicates a
prevalence of direct sources from the technosphere (e.g. direct
discharge through waste water or leaching from poorly disposed
solid waste) dominating PFAS inputs, especially in the most an-
thropic parts of the river. The prevalence of compounds with
shorter alkyl chains is interpreted as a result of on-going substi-
tution strategy adopted by industry. To our knowledge, this is the
first experimental evidence of shorter chain PFCAs exceeding levels
of PFOA in river water from a country with an emerging industrial
economy. Most recent surveys of PFCAs in river waters in countries
with emerging economies consistently showed PFOA levels still
708 B.M. Sharma et al. / Environmental Pollution 208 (2016) 704e713
exceeding C5eC7 PFCAs levels (Duong et al., 2015; Liu et al., 2015a;
Lu et al., 2015; Mudumbi et al., 2014; Wang et al., 2014a; Yao et al.,
2014). In contrast, data from Europe and North America display
temporal trends in which shorter chain PFCAs tend to increase their
abundance in environmental samples in comparison to PFOA
(Heydebreck et al., 2015; Myers et al., 2012; Rostkowski et al., 2009;
Zhao et al., 2015). Direct sources of shorter chain PFCAs have been
identified as releases from degradation of 6:2 fluorotelomer-based
goods (including water/oil repellents and aqueous fire-fighting
foams) used as replacements for 8:2 fluorotelomer-based prod-
ucts (Prevedouros et al., 2006; Wang et al., 2014b).
Concentrations of PFCAs appeared to increase from HR to MR,
possibly due to the cumulative contribution from increasingly
populated regions. Such a trend was however not significant likely
due to the counteracting effect of dilution in the downstream
(Chakrapani and Saini, 2009; Whitehead et al., 2015). The influence
of local direct emission from urban areas could be clearly seen for
several PFCAs (specifically: PFPA, PFHxA, PFHpA, and PFOA) and
PFOS in relation to the relatively higher concentrations, typically
observed downstream of major conurbations compared to the
immediate upstream section (Fig. 2). This is more clearly depicted
in Supplementary Fig. S2 where the pattern is presented as the ratio
of river concentrations measured downstream vs upstream of
major cities in the Gangetic plain. Ratios ranged between >1 and 7
with the highest point source emissions typically observed for
C6eC8 PFCAs compared to PFOS and longer-chained PFCAs.
PFSAs concentrations showed a different pattern compared to
PFCAs. PFBS was the most abundant PFSA in the HR (UKU, UKD,
DBG, DAK, and DGR). High method quantification limits due to
strong matrix effects in samples collected in the MR and LR pre-
cluded quantification of PFBS in these samples. The relatively high
PFBS values in the HR (the least impacted and populated part of the
catchment) may be, at least in this part, associated with the influ-
ence of atmospheric deposition since PFBS is also an atmospheric
degradation product of volatile precursors (Chu and Letcher, 2014;
Hagenaars et al., 2011). Notably, PFBS can be derived from
Fig. 3. Distribution plots of estimated total emission (g day
1) (Upper charts) and emission per urban resident (mg day
1 person
1) (Lower charts) of PFOS and PFOA in five selected
subcatchments of the Ganges River. The grey distribution plot in the PFOA charts refers to calculations performed by considering the sample collected upstream of the Patna hotspot,
in contrast to the estimates performed considering the downstream sample.
degradation of perfluorobutansulfamide-based products. However,
relatively low population density in the HR and their mainly
traditional life style suggests that emissions from the technosphere
might be limited in this area. In contrast to this trend and consistent
with expectations, concentrations of PFOS were highest in MR and
LR (KD, VD, PU, and PD), suggesting a strong influence of direct
anthropogenic sources especially in the most densely populated
and industrialized regions (Supplementary Figure S1a, S2).
The spatial distribution pattern of PFOS and PFCAs was further
investigated using principal component analysis (Supplementary
Fig. S3). PFOA had a similar distribution pattern as PFNA and
PFDA and was essentially influenced by relatively large levels
recorded downstream of two major cities of the MR and LR (Kanpur
and Patna, respectively). Regression analysis confirmed that C9eC10
PFCA trends significantly correlated (P < 0.05) with that of PFOA
(Supplementary Table S8). In contrast, trends of C5eC7 PFCAs were
correlated (P < 0.05) with that of PFOS and distinct from those of
longer chained PFCAs. The peculiar PFAS signature downstream of
Kanpur and Patna likely reflects the influence of localized sources,
the identity of which warrant further investigation in future
studies.
3.2. Results of PFOA and PFOS direct emissions to river water
Estimates of direct anthropogenic discharge of PFOA and PFOS
are summarized in Fig. 3. This assessment directly covers a total
population of about 400 million people (7% of the current global
population). Similar analyses of PFAS emissions were conducted
before in different geographical contexts (Earnshaw et al., 2014;
Filipovic et al., 2013; McLachlan et al., 2007), nevertheless, to our
knowledge, this is the largest study of this type. The mean cumu-
lative PFOA and PFOS discharges in the whole Ganges catchment
were calculated to be in the order of 240 and 210 g day
1 respec-
tively. Estimated emissions varied by up to 4 orders of magnitude in
different subcatchments (Fig. 3). The drivers of this variability were
investigated by correlation analysis. The following descriptors were
 B.M. Sharma et al. / Environmental Pollution 208 (2016) 704e713
considered: industrial waste water production generation (CPCB,
2013), total population and total urban population in the sub-
catchment (MHA, 2011). These descriptors were not correlated
among each other (P < 0.05). Urban population displayed a strong
positive correlation with PFOS emissions (P ¼ 0.016, R
(Spearman) ¼ 0.99, adj-R2 ¼ 0.98) (The fitted linear model is pre-
sented in Supplementary Fig. S4). After scaling ES by the urban
population over 95% of the variability was resolved, suggesting a
direct relationship between PFOS emissions and the urban envi-
ronment. Importantly, a borderline significant correlation (P ¼ 0.08,
R (Spearman) ¼ 0.9) was found between PFOS emissions and total
population suggesting that rural areas may have only a minor role
as sources of this compound in India (and therefore also possibly
the compounds with spatial distribution pattern correlated to that
of PFOS such as C5eC7 PFCAs) (Supplementary Table S8). Estimates
of emission per urban resident (ES,PC_U mg day
1 person
1) are
depicted in Fig. 3. Mean values of ES,PC_U between different sub-
catchment ranged 0.1e2.5 mg day
1 person
1 for PFOS and
0.3e11 mg day
1 person
1 for PFOA. ES,PC_U of PFOA substantially
followed the same trend as PFOS when an outlier was excluded.
Such a hotspot coincided with the site downstream of Patna, pre-
viously highlighted for having PFAS signature different from the
general trend (Supplementary Fig. S3) with a higher contribution of
PFOA and C9eC10 PFCAs. At this location, PFOA ES,PC_U was over one
order of magnitude higher compared to the highest estimates for
other subcatchments. This result can only be explained by postu-
lating that sampling at this section captured the plume from a
strong local source.
Estimated emissions of PFOS and PFOA in the Ganges River were
significantly lower than estimates from Europe (Pistocchi and Loos,
2009). Similarly, PFOS per capita emissions from the present study
were lower than those reported from the Eastern Coastal Region of
China when only domestic activities (in contrast to Industrial
sources) are considered (Xie et al., 2013). Similarly, higher (up to 1
order of magnitude) per capita emissions of PFOS and PFOA were
found in many developed countries (for a comprehensive review of
literature data and comparison see Supplementary Table S9). Esti-
mated per capita emissions from this study were in the range of
those calculated for some areas in Poland (0.7 mg day
1 person
1)
and Latvia (0.4 ng day
1 person
1) (Filipovic et al., 2013). This
comparison suggests that, despite the postulated low level of
pollution emission control and waste management in India, usage
and emissions of PFAS appear to be lower in this developing region
compared to more developed/industrialized countries. A relation-
ship between per capita gross domestic product (GDP) and emis-
sions of PFAS was hypothesized and illustrated by Wang et al., in a
Fig. 4. Concentrations of various PFAS in the groundwater/drinking water at different sampling sites in the Ganges River basin (logarithmic scale, base 10).
709
review of PFAS emission data from China (Wang et al., 2015).
Outside China, emission data from developing countries are still
very scarce and it is currently impossible to assess the general
validity of this relationship. A recent report has, however, pre-
sented emission estimates for a few cities in Kenya (Chirikona et al.,
2015) which could be converted into per-capita emissions. Values
for these cities were up to 10 folds lower than those found in the
present study for densely populated and industrialized regions of
the Ganges River (Supplementary Table S9), corroborating the hy-
pothesis of a relationship between per capita GDP and PFAS emis-
sions over a global scale.
3.3. PFAS in groundwater
There is a lack of information on the concentrations of PFAS in
groundwater from India. This study is the first to analyze ground-
water samples from the Ganges River basin in relation to exposure
of surface water as receptors of wastewater inputs. Such an analysis
was strongly motivated by the fact that groundwater is used for
drinking as well as irrigation purposes in most of the Ganges basin.
Concentrations of PFAS in groundwater are shown in Fig. 4 and
Supplementary Table S10. Levels and patterns were very similar to
those observed in surface water. Out of 21 PFAS, 14 compounds
were frequently detected. PFUnDA, PFTeDA, PFHpS, MeFOSA,
EtFOSA, MeFOSE, and EtFOSE were not detected at any of the
sampling locations. Unlike river water, PFBA was detected in
groundwater only in the LR with highest concentrations among all
PFCAs (<MQL e 9.2 ng L
1). PFHxA and PFHpA were detected in all
samples at concentrations ranging from 0.8 to 4.9 ng L
1 and
0.5e3.5 ng L
1, respectively. Concentrations of other PFCAs such as
PFPA, PFOA, PFNA, and PFDA ranged between < MQL e 2.2 ng L
1,
<MQL e 0.8 ng L
1, <MQL e 0.2 ng L
1, and <MQL e 0.1 ng L
1,
respectively.
Similar to what was observed in Ganges River water, concen-
trations of PFOA in groundwater were lower than PFPA, PFHxA, and
PFHpA concentrations. As described previously, this can be indic-
ative of a shift in use to 6:2 fluorotelomer-based articles from 8:2
fluorotelomer-based articles. PFBS was the homologue with highest
concentrations (<MQL e 4.9 ng L
1) among PFSAs, followed by
PFOS (<MQL e 1.1 ng L
1), PFHxS (<MQL e 0.08 ng L
1), and PFDS
(<MQL e 0.06 ng L
1). Furthermore, concentrations of PFBA, PFPA,
PFHxA, PFHpA, and PFOA were often demonstrably higher in
groundwater than in the river.
The observed consistent contamination profile and spatial
trends of PFCAs and PFOS indicates that the occurrence of PFAS in
groundwater has similar drivers of that in surface water. Possible
710 B.M. Sharma et al. / Environmental Pollution 208 (2016) 704e713
sources of PFAS contamination to groundwater can include leach-
ing and runoff from unpaved surfaces (including leaching of
contaminated atmospheric depositions) as well as leaks from
municipal and industrial wastewater drains and landfills. Abstrac-
tion of polluted river water for irrigation and leaching from agri-
cultural soils may also contribute to aquifer contamination with
PFAS emitted through wastewater directly to the river. The use of
river water for irrigation is especially high during the dry season
which overlapped with our sampling campaign. Infiltration of river
water into the groundwater aquifer directly from the river sedi-
ment bed and banks is another potentially important process for
PFAS circulation. While, there is little knowledge about the dy-
namics of this process in the Ganges basin, it is likely that such an
exchange between groundwater and river water is highly seasonal
with a net water recharge (from groundwater to river water) during
the wet season and infiltration during the dry season. It is therefore
expected that river water directly contributed to groundwater
contamination during the period of the campaign.
The ratio CGW/CRW of groundwater concentrations to river water
concentrations was up to 9 for PFBA and tended to decrease from
PFPA > PFHxA > PFHpA > PFOA > PFOS. This behavior can provide
some insights into the origin of groundwater contamination since it
appears to be influenced by compound-specific physical chemical
properties. Water:organic carbon equilibrium partitioning co-
efficients KOC are expected to increase with length of the alkyl chain
of PFCAs while it is highest for PFOS (Milinovic et al., 2015;
Sepulvado et al., 2011). The observed trends with higher concen-
trations in groundwater compared to river water for the more
soluble substances and decreasing CGW/CRW ratio at increasing KOC
suggests that groundwater may be preferentially contaminated by
direct sources through processes that are mediated by partitioning
with soil and/or sediment. In principle, these include all the pro-
cesses mentioned above (i.e. leaching from contaminated ground,
leaks from the sewage and exchange with river water by infiltration
through the river sediment bank). The closely coupled river water/
groundwater contamination is corroborated also by the similar
trends observed for some compounds in locations upstream and
downstream of major conurbations. Concentrations of PFOS in
groundwater and river water had a similar spatial trend (Fig. 5).
Even on the local scale, and similar to patterns for river water,
higher concentrations of PFOS in groundwater were typically
observed at locations downstream of the conurbations with highest
emission estimates compared to their upstream sites (Fig. 5).
Groundwater contamination appears to be very sensitive to local
sources and river contamination levels. PFAS can therefore possibly
be regarded as markers of wastewater contamination in
Fig. 5. Concentrations of PFOS in river and groundwater samples at different sampling
sites along the Ganges River.
groundwater resources. Their presence can indicate possible
contamination from a number of other wastewater-borne con-
taminants emitted through residential and industrial effluents to
the river, although, in order to reinforce this hypothesis, data from
genuine and conservative wastewater tracers should be evaluated.
Fortunately, the groundwater PFAS concentrations measured
here were low. They were up to 4 orders of magnitude lower than
those detected in studies carried out in wells from the Netherlands
(Eschauzier et al., 2013), and up to 2 orders of magnitude lower
than those detected in some locations in Western USA (Post et al.,
2013). Concentrations of PFOA and PFOS in groundwater
measured in Northern Italy were also found to be higher than those
detected in this study (Castiglioni et al., 2015). The consistently
higher PFAS concentrations observed in developed nations con-
firms that sources from the technosphere consistent with high
industrialization levels and diffuse use of sophisticated products
can result in considerably higher contamination levels of drinking
water resources and therefore possibly higher exposure for the
human population.
3.4. Estimation of human exposure to PFAS
Several studies have shown that historical exposure of the
general population to PFAS is through multiple pathways including
ingestion of food, drinking water, and inhalation of air/dust
(Gebbink et al., 2015; Trudel et al., 2008). Despite the fact that the
dominant pathway controlling exposure of PFAS in humans has not
been fully elucidated so far, drinking water is often regarded as an
important contributor to the total intake. The approach to estimate
the exposure through drinking water was previously described
using a Scenario-based Risk Assessment (SceBRA) (Trudel et al.,
2008; Vestergren et al., 2008). In this study, low-exposure, inter-
mediate-exposure and high-exposure scenarios to PFAS for chil-
dren, adults, and senior citizens through contaminated drinking
water were estimated by the approach presented by Gebbink et al.,
(Gebbink et al., 2015). Daily exposure intakes for PFAS via drinking
water consumption (Edw) were calculated as:
Cdw  qdw
Edw ¼  Fuptake (1)
mbw
Where, Cdw is concentration of PFAS in drinking water (ng L
1), qdw
is quantity of drinking water consumed (L day
1), mbw is body
weight (kg) and Fuptake is gastrointestinal uptake fraction (unit less).
Fuptake based on rodent studies are estimated as 0.66, 0.80 and 0.91
for low-, intermediate-, and high-exposure scenarios for PFOA and
PFOS (Trudel et al., 2008). We adopted these values of Fuptake for
other PFAS in the absence of literature values, although major dif-
ferences may occur due to the broad range of PFAS phys-
icalechemical properties. Average body weights for children,
adults, and the elderly people are 24, 70, and 60 kg, respectively. On
an average, the amount of water consumed by children is approx-
imately 1.3 L day
1, while, 2.5 and 2 L day
1are consumed by adults
and seniors, respectively (EFSA, 2010).
We used groundwater contamination data (5th, 50th, and 95th
percentile of concentrations from all location for each compound)
measured here to calculate daily intakes. Results are presented in
Supplementary Fig. S5 and Supplementary Table S11. Intake of
PFHxA (up to 0.2 ng kg
1 day
1) was estimated to be the highest
among all the PFAS. Intakes of PFOA and PFOS intake were found to
be similar (up to 0.04 ng kg
1 day
1). Intakes of PFHpA
(0.2 ng kg
1 day
1) and PFPA (0.09 ng kg
1 day
1) were higher than
those observed for PFOA and PFOS. Intakes for PFNA, PFDA, PFDS
and PFOSA were very low, ranging up to 0.007 ng kg
1 day
1.
Among different scenarios, the highest PFAS intakes per kg of body
 B.M. Sharma et al. / Environmental Pollution 208 (2016) 704e713
weight were observed for children. Seniors have the lowest expo-
sure intakes of PFAS compared to other age groups in all the three
exposure scenarios. These exposure levels were 2e3 times lower
than those calculated for the adult population of Catalonia in Spain
and children from Taiwan (Chimeddulam and Wu, 2013; Domingo
et al., 2012).
Health risks based on exposure to PFAS through contaminated
water consumption were also assessed. The oral non-cancer risk,
expressed as a Hazard Index (HI), was determined by comparing
oral exposure dose (through water intake) with a Reference Dose
(Rf) for each PFAS as:
Exposure intake
HI ¼
Rf
Reference dose values for PFOA and PFOS were assumed to be
140 and 75 ng kg
1 day
1, respectively (MDH, 2007) (based on
increased liver weight, and decreased HDL cholesterol and changes
in thyroid hormones). In the absence of Rf values for other PFAS, Rf
values for PFCAs were assumed as a first approximation to be
similar to that of PFOA. Similarly, for other PCSAs, the Rf value of
PFOS was used. A summary of hazardous index values for each PFAS
is presented in the Supplementary Table S12.
For all PFAS and age groups, the exposure intake did not exceed
the Rf under any of the exposure scenarios. The estimated HI values,
therefore, were below 1, implying no considerable risks from
drinking water consumption. High values for HI were found for
PFHxA, PFHpA, PFPA, and PFOA for children (6e12 years old) under
the high exposure scenario. By comparison, HI values in this study
were 2e3 orders of magnitude lower than those detected Taiwa-
nese river water (Chimeddulam and Wu, 2013).
4. Conclusions
This study provided a first regional overview on PFAS occur-
rence in, and emissions to the water resources in the Ganges River
basin along with a preliminary first assessment of human exposure
through drinking water in this region. The enormous availability of
renewable water resources controlling dilution of wastewater ef-
fluents in the large river, relatively low per-capita emissions in a
region with an economy that is still largely based on agriculture and
a large part of the population still living a traditional lifestyle
resulted in limited environmental and human exposure levels to
PFAS. Ground/drinking water had a similar contamination pattern
(both at regional and local scale) as waste water-receiving river
water, suggesting that these compartments are sensitive to the
same diffuse and/or local sources of PFAS. Presence of PFAS in
groundwater can be interpreted as a consequence of river water
infiltration, spills from sewage, or leaching from contaminated
surface water (possibly including the use of contaminated river
water for irrigation and subsequent leaching). Despite generally
low concentrations of PFAS in drinking water, the observed
wastewater signature in groundwater samples is of concern since
other toxic substances emitted from domestic and industrial ef-
fluents may also be present, posing a risk to the human population
that consumes untreated groundwater.
Acknowledgments
The research leading to these results has acquired a financial
grant from the People Program (Marie Curie action) of the Seventh
Framework Program of EU according to the REA Grant Agreement
No. 291782. The research is further co-financed by the South-
Moravian Region. This paper reflects solely the author's views,
the European Union or the institutes which the authors represent
711
are not liable for any use that may be made of the information
contained therein. This study was also supported by the Norwegian
Research Council's NORKLIMA program through the project Climate
Induced Mobilization of Persistent OrganicPollutants (POPs) in Rivers
in India (INDNOPOP), project no: 215975/E10). MNF was funded by
the FORMAS Forest POPs project. Flow data for the Ganges was
obtained as part of the project Assessing health, livelihoods,
ecosystem services and poverty alleviation in populous deltas under
grant NE/J003085/1. This project was funded by the Department for
International Development (DFID), the Economic and Social
Research Council (ESRC), and the Natural Environment Research
Council (NERC) as part of the Ecosystem Services for Poverty Alle-
viation (ESPA) Programme.
(2)
Appendix B. Supplementary data
Supplementary data related to this article can be found at http://
dx.doi.org/10.1016/j.envpol.2015.10.050.
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