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Emerging contaminants and treatment options in water
recycling for indirect potable use
T. Wintgens, F. Salehi, R. Hochstrat and T. Melin
ABSTRACT
T. Wintgens
F. Salehi
R. Hochstrat
T. Melin
Chemical Engineering Department,
RWTH Aachen University,
Turmstrasse 46, 52056 Aachen,
Germany
E-mail: wintgens@ivt.rwth-aachen.de
Solutions to global water stress problems are urgently needed yet must be sustainable,
economical and safe. The utilisation of alternative water sources like reclaimed municipal
wastewater is one of the most obvious and promising options in integrated water resources
management. Among the various beneficial uses of reclaimed wastewater Aquifer Recharge (AR)
receives growing attention because it features advantages such as additional natural treatment,
storage capacity to buffer seasonal variations of supply and demand as well as mixing with
natural water bodies which promotes the acceptance of further uses, particularly indirect potable
use. Major concerns about the safety of this exploitation route of an alternative water source are
connected to microbial and chemical contaminants occurring in wastewater, among which are
emerging trace organics like endocrine disrupters and pharmaceuticals. This paper reviews the
current international debate about the relevance of emerging contaminants and technical
mitigation options in water recycling for indirect potable use.
Key words
|
emerging contaminants, indirect potable reuse, water recycling
INTRODUCTION
Population growth, increased industrial activities in many
parts of the world as well as the estimated impacts of
climate change will exceed various pressures on the water
supply systems (EEA 2007). Particularly in developing
countries there is a need to dramatically enlarge the access
to safe and piped water (UN 2006). Considering the growing
burden on freshwater resources, particularly the over-
abstraction of groundwater, the deterioration of ground-
water quality, and saltwater intrusion into coastal aquifers,
the utilisation of alternative water sources is a promising
option to supplement water supply and restore natural
resources (EEA 1999; Margat & Valle
´
e 2000). Among the
alternative water sources are seawater, brackish ground-
water, urban storm water, collected rain water as well as
reclaimed water which can be used for different beneficial
purposes.
Global water demand will continue to increase and is
expected to reach probably 70% of the available freshwater
resources till 2025 (UN 2006). Furthermore, these resources
are unequally distributed and often of poor quality so that
numerous regions in the world face rising water stress.
Superposed on the evolution of demand are natural and
man-made variations of water availability.
The water stress index – the ratio of a country’s total
water withdrawal to its total renewable freshwater
resources – serves as a rough indicator for the pressure
exerted on water resources. Not all water uses are causing
comparable stress. A ratio in the range of 10% to 20%
indicates that water availability is becoming a constraint
on development. A water stress index above 20% is
supposed to necessitate comprehensive water manage-
ment efforts and actions to resolve conflicts among
competing uses (OECD 2003). It is striking that approxi-
mately half of the European countries, representing
almost 70% of the population, are already facing water
stress issues today.
doi: 10.2166/wst.2008.799
99 Q IWA Publishing 2008 Water Science & Technology—WST
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57.1
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Water reclamation and reuse applications
Municipal wastewater including stormwater can be consi-
dered as an alternative water source if treated appropriately
for the intended use. This is highlighted by the Urban
Wastewater Treatment Directive (91/271/EEC) and by the
Water Framework Directive (2000/60/EC) encouraging
“reuse measures” and “artificial recharge” as supplementary
measures that can be applied to reach the fixed environ-
mental objectives for surface and groundwater bodies.
Reclamation and reuse of municipal wastewater is a
method to mitigate increasingly evident water stress arising
in many regions of the world from water scarcity and water
quality degradation. The proposed implementation of water
reclamation in integrated water resources management is
driven by sustainability issues, potential cost-advantages
and climate change conditions. The socio-cultural environ-
ment often drives and determines the appropriateness of
technical solutions (Bixio et al. 2005; Asano et al. 2006).
Indirect potable reuse
Indirect potable reuse can be regarded as any augmentation
of water bodies utilised for drinking water supplies by
wastewater treatment plant effluents or overflows from
combined sewer systems (Asano et al. 2006). One can
distinguish between unintended or de facto indirect potable
reuse which happens along major river catchments around
the world, where drinking water resources are influenced by
wastewater discharges as observed on basis of anthropo-
genic tracer substances, (Ternes & Joss 2006; Weil &
Knepper 2006; Dillon & Jiminez 2007) as well as planned or
intended indirect potable reuse. Planned indirect potable
reuse is a measure to supplement public water supply by the
utilisation of reclaimed water through introduction in a
drinking water reservoir or via managed aquifer recharge.
Managed recharge has for a long time provided means to
mitigate depletion of groundwater levels, to protect coastal
aquifers from saltwater intrusion, and to store surface water
for future use (Kanarek & Michail 1996; Mills et al. 1998;
Bouwer 2000). Aquifer storage has some advantages over
surface water reservoirs which might be more costly and
environmentally questionable. Moreover, soil percolation
and aquifer storage act as treatment steps while avoiding
evaporation as well as taste and odour problems due to algae
growth in surface storage (Dillon 2000; Asano & Cotruvo
2004). Recharge can be performed in two ways: direct or
indirect. If conducted by infiltration and percolation through
soil and subsoil, the recharge processes, e.g. by so-called Soil
Aquifer Treatment (SAT), offer an additional barrier. Mixing
reclaimed wastewater with natural groundwater prior to any
intended use also positively influences the public acceptance
of a reuse scheme.
The concept of Aquifer Recharge (AR) offers potential
for various subsequent uses like irrigation, industrial
process water and augmentation of public water supplies.
The latter, indirect potable use, is certainly one of the most
challenging water reclamation and reuse applications with a
high demand in terms of safety because of the potential use
as drinking water (whose quality criteria are fixed in
directive 98/83/EC) and the general level of protection
required for groundwater resources as laid down in the
directive on the protection of groundwater against pollution
and deterioration (2006/118/EC). Even if drinking water
supplementation is not explicitly foreseen in an aquifer
recharge project, the provision of drinking water quality in
the recovered product is a common bottom line in many
applications, e.g. in Israel where the Dan Region Recla-
mation and SAT scheme provides “accidental drinking
water quality” on a large scale (Mekorot 2003).
EMERGING CONTAMINANTS IN INDIRECT
POTABLE USE
Water quality criteria
According to a recent review conducted by Asano & Cotruvo
(2004) the main concerns in indirect potable reuse are health
risks resulting from pathogens and trace chemicals as well as
nitrate. Among the organic pollutants there is a range of so
called emerging contaminants such as endocrine disrupting
compounds (EDC), pharmaceutically active compounds
(PhAC), personal care products (PCP) and disinfection
by-products (DBP). The occurrence of these emerging
contaminants in the aquatic environment including surface
and groundwaters, and wastewater sludges as well as
drinking water has been studied (Heberer 2002; Ternes &
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Table 1
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Emerging contaminants in indirect potable reuse and aquifer recharge schemes
Scheme and sample point Compound Concentration [ng/L] Reference
North City Water Reclamation Plant San Diego (CA) – Advanced Water Treatment Pilot
V Tertiary effluent Sulfamethaxoazole 892 DeCarolis et al. 2006
V Reverse osmosis permeate Sulfamethaxoazole 2.9 DeCarolis et al. 2006
V UV þ Peroxide product Sulfamethaxoazole , 1.0 DeCarolis et al. 2006
V Tertiary effluent Iopromide 632 DeCarolis et al. 2006
V Reverse osmosis permeate Iopromide 1.4 DeCarolis et al. 2006
V UV þ Peroxide product Iopromide , 1.0 DeCarolis et al. 2006
Bolivar Aquifer Storage and Recovery Scheme (South Australia)
V Reclaimed water Atrazine 9.2 Overacre et al. 2006
V Groundwater (5 month storage) Atrazine 4.5 Overacre et al. 2006
V Groundwater (11 month storage) Atrazine 1.8 Overacre et al. 2006
V Reclaimed water Estrone 32 Overacre et al. 2006
V Groundwater (5 month storage) Estrone 24 Overacre et al. 2006
V Groundwater (11 month storage) Estrone 11 Overacre et al. 2006
Temporary Hanningfield reservoir augmentation by Chelmsford effluent (UK)
V Sewage plant effluent Estrone 8 33 Gomes & Lester 2003
V UV-treated effluent Estrone , 1-20 Gomes & Lester 2003
Infiltration of secondary effluent into groundwater via
a wetland upstream of a drinking water facility (Germany)
V Receiving surface water Carbamazepin 1,100 Bergman et al. 2003
V Wetland Carbamazepin 500–600 Bergman et al. 2003
V Groundwater (420 m from infiltration) Carbamazepin 530 Bergman et al. 2003
Irrigation of treated wastewater in Braunschweig, Germany
V Tertiary effluent Sulfamethaxoazole 620 ^ 90 Ternes et al. 2007
V Groundwater (in the irrigation area) Sulfamethaxoazole , LOQ – 110 Ternes et al. 2007
V Tertiary effluent Carbamazepine 2,100 ^ 700 Ternes et al. 2007
V Groundwater (in the irrigation area) Carbamazepine , LOQ – 570 Ternes et al. 2007
V Tertiary effluent Diatrizoate 1,700 ^ 3,300 Ternes et al. 2007
V Groundwater Diatrizoate 1,600 – 9,600 Ternes et al. 2007
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Joss 2006). A particular substance of concern is N-nitrosodi-
methylamine (NDMA) which was found to be a possible
by-product in water and wastewater disinfection (Mitch &
Sedlak 2002) and is characterised as highly carcinogenic.
In contrast to the wide range of EDCs, PhACs and
PCPs, only DBPs are currently considered in water related
pieces of regulation and supra-national recommendations,
particularly in drinking water quality requirements such as
the WHO Guidelines for Drinking-water Quality (WHO
2004), the European Drinking Water Directive and the US
National Primary Drinking Water Regulations (US EPA
2006). Guidelines for indirect potable use make regularly
reference to drinking water quality standards and add a
number of specific criteria such as absence of faecal
contamination and low TOC (. 3 mg/L) (US EPA 2004;
Salgot et al. 2006). While not formally incorporated into
Table 1
|
(continued)
Scheme and sample point Compound Concentration [ng/L] Reference
Comparing MF, RO and soil-aquifer treatment
for indirect potable reuse of water (USA)
V Tertiary effluent EDTA 35,400 ^ 27,600 Drewes et al. 2003
V Microfiltration permeate EDTA 5,600 Drewes et al. 2003
V Nanofiltration permeate EDTA , LOQ Drewes et al. 2003
V Reverse osmosis permeate EDTA , LOQ Drewes et al. 2003
V Soil-aquifer treatment EDTA 3,960 ^ 3,180 Drewes et al. 2003
V Tertiary effluent APECs 55,800 ^ 59,400 Drewes et al. 2003
V Microfiltration permeate APECs 23,400 Drewes et al. 2003
V Nanofiltration permeate APECs , LOQ Drewes et al. 2003
V Reverse osmosis permeate APECs , LOQ Drewes et al. 2003
V Soil-aquifer treatment APECs 680 ^ 1,140 Drewes et al. 2003
Water samples influenced by wastewater
in Berlin (Germany)
V Surface water p-TSA , 1,150 Richter et al. 2007
V Groundwater (directly below a former
sewage farm)
p-TSA , 40,800 Richter et al. 2007
V Drinking water p-TSA , 270 Richter et al. 2007
V Surface water BSA , 520 Richter et al. 2007
V Groundwater (directly below a former
sewage farm)
BSA , 1,220 Richter et al. 2007
V Drinking water BSA , 50 Richter et al. 2007
LOQ ¼ limit of quantification, p-TSA ¼ paratoluenesulfonamide, BSA ¼ benzenesulfonamide, EDTA ¼ ethylenediaminetetraacetic acid, APECs ¼ alkylphenolpolyethoxycarboxylates.
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national drinking water standards the Californian Office of
Environmental Health Hazard Assessment issued 2006 a
Public Health Goal (PHG) for NDMA of 3 ng/L (OEHHA
2006). The California Department of Health Services’
Division of Drinking Water and Environmental Manage-
ment (DDWEM) has established a notification level of
10 ng/L for a number of nitrosamines (DHS 2006). Without a
direct link to indirect potable use, but to guideline values for
emerging contaminants in the aquatic environment, the
European Parliament Committee on the Environment,
Public Health and Food Safety has approved a proposal in
2007 for an extension of the list of the priority substances to
be included in the Annex X of the Water Framework
Directive (EPC 2007), containing trace organics as bisphenol
A, carbamazepine, clotrimazole and diclofenac.
Occurrence and fate of emerging contaminants
The occurrence and fate of emerging contaminants has been
monitored in a number of indirect potable reuse and aquifer
recharge schemes (PUB 2002; Gomes & Lester 2003; Asano
et al.2006; Snyder et al.2007). Table 1 summarises selected
data on the occurrence and fate of emerging contaminants
obtained from monitoring of both planned and unplanned
Table 2
|
Water reclamation schemes investigated in RECLAIM WATER (www.reclaim-water.org)
Site location & capacity Scheme description
Sabadell 30 km from Barcelona,
Spain Capacity: 25,000 m
3
d
21
Secondary treated wastewater effluent discharged into a river bed where it infiltrates and is
recovered. The water is then disinfected (UV) and distributed for parks irrigation.
Nardo
`
Salento Region, south of Bari,
Italy Capacity: 12,000 m
3
d
21
Secondary treated municipal effluent is transported to aquifer injection. Recharge acts as a
salt intrusion barrier and resource is also used as drinking water source.
Shafdan Negev, Israel
Capacity: 342,000 m
3
d
21
Secondary wastewater from the Tel-Aviv area is recharged to an aquifer via a soil aquifer
treatment (SAT) system. Recovered water is primarily used for irrigation but has accidental
drinking water quality.
Gaobeidian Beijing, China
Capacity: 650 m
3
d
21
Tertiary effluent is used for aquifer recharge. Treatment is provided by coagulation, filtration
and ozonation (in test) prior to infiltration and recharge.
Adelaide Salisbury, South Australia
Capacity: 1,100 m
3
d
21
Wetland treated urban stormwater injected into a brackish aquifer. Water recovered via
separate recovery wells. Recovered water intended for drinking supplies, and until proven will
be used for irrigation.
Torrele (Wulpen) Belgium
Capacity: 8,640 m
3
/d
Infiltration: 2.5 million m
3
/ year
Tertiary treated municipal effluent is upgraded by microfiltration and reverse osmosis, and
then infiltrated via an infiltration pond to prevent salt intrusion and to recharge an aquifer
used for drinking water production.
Mezquital Valley (State of Mexico)
Mexico Infiltration:
630 million m
3
/year
Wastewater mixed with stormwater and surface water is discharged to an irrigated area of
more than 76,000 ha. About 40% of the irrigation water infiltrates into the aquifer. The water
is recovered via separate wells and springs. 206 well systems, 31 springs, and 63 waterwheels
are in operation. Recovered water is chlorinated and distributed for drinking water supply,
industrial use, irrigation and other purposes (bathing, swimming, washing).
Atlantis (Cape Town) South Africa
Capacity: 15,000 m
3
/d
Infiltration: 2.7 million m
3
/year
Urban stormwater run-off, is collected via a series of detention basins and blended with
secondary treated domestic wastewater and recharged up-gradient of the production well
field for augmenting the water supply. The blend of natural groundwater and recharged water
abstracted from the well field is used as potable water supply for the town of Atlantis.
NEWATER Singapore
Capacity: 150,000 m
3
/d
NEWATER is treated used water further purified using dual-membrane (microfiltration and
reverse osmosis) and UV treatment. Four NEWATER factories are in operation
supplementing Singapore’s water supplies, part of the product water is use to augment
drinking water reservoirs.
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indirect potable reuse as well as aquifer recharge schemes.
To overcome the limitations of compound-specific tests with
respect to the potential health hazards toxicological tests
have also been carried out with bio-assays in a number of
indirect potable reuse schemes. Both toxicological tests as
well as a limited number of epidemiological tests could not
show that a higher health risk is connected to water recycling
than to the use of the conventional sources considered (PUB
2002; Khan & Roser 2007)
TREATMENT OPTIONS IN INDIRECT POTABLE
REUSE
Wastewater is generally more polluted than most drinking
water sources and hence requires more extensive treatment
prior to indirect potable use. The treatment technology for
these ambitious goals is generally available and implemented
in full scale (e.g. in Orange County, Singapore and Wulpen/
Belgium). Examples exist where the aquifer is recharged with
secondary treated effluent only and the soil-aquifer system is
used as treatment and storage, as it is the case in economically
developed countries such as Israel, USA and Australia
(International Water and Irrigation Review 1999)aswellas
in countries with transient economies such as Mexico,
South Africa, Thailand and Peru (Dillon & Jiminez 2007).
The natural attenuation processes occurring in the soil and
sub-soil, particularly in the vadose zone, have shown to be
quite effective with respect to trace organic removal (Ternes
et al.2007). On the other hand, in the last decade the common
practice in Western Countries is rather to apply tertiary
(e.g. coagulation, filtration, disinfection) or quaternary treat-
ment (various types of double membrane systems, as it is the
case in Belgium, California, Singapore, Australia and Nami-
bia) before infiltration and potable use (Bixio et al. 2005).
The effectiveness of a range of intensive water recla-
mation technologies such as conventional and membrane
coupled (MBR) activated sludge treatment, membrane
effluent filtration with porous and dense membrane pro-
cesses, activated carbon adsorption as well as different
oxidation processes (Ozone, UV þ Ozone, UV þ Per-
oxide) have been investigated in a number of studies
(Asano et al. 2006; Ternes & Joss 2006; Snyder et al.
2007). It seems obvious from the result of these investi-
gations that an almost complete retention of a wide range of
emerging contaminants can be achieved with multi-barrier
treatment processes. Particularly difficult is the removal of
NDMA; advanced oxidation processes with UV and H
2
O
2
have been implemented in indirect potable reuse schemes in
the US to cope with this problem (Asano et al. 2006).
Technologies applied in full scale water reuse schemes
There is a number of treatment technologies applied in
indirect potable reuse projects ranging from soil application
of raw wastewater to highly engineered double membrane
systems plus advanced oxidation. Compilations of the
different treatment trains utilised in various schemes world-
wide can be obtained e.g. from Asano et al. (2006), Ternes &
Joss (2006), Dillon & Jimenez (2007). A number of different
indirect potable reuse and managed groundwater recharge
schemes are under investigation by the European Project
partnership RECLAIM WATER. The case studies investi-
gated there also with respect to the occurrence and fate of
trace organics are listed in Table 2.
Table 3
|
Nanofiltration application studies in water and wastewater applications
Application Treatment aims Source
Drinking water treatment (Groundwater) Water softening Gorenflo et al. (2002)
Drinking water treatment (Surface water) TOC removal Beros et al. (2003)
Textile industry Dye removal Van der Bruggen et al. (2004)
Desalination Salt removal Melin & Rautenbach (2007)
Water reclamation TOC removal Meier & Melin (2005)
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Emerging technologies
Among the emerging technologies for indirect potable use
nanofiltration should be highlighted as a treatment tech-
nology which can remove a wide range of microbiological
as well as chemical contaminants (Scha¨ fer et al. 2005).
Nanofiltration can be considered as an alternative to
reverse osmosis technology where a lower degree of
desalination is required. With a molecular weight cut-off
above 200 g/mol it is a promising treatment option for a
variety of emerging trace contaminants. Nanofiltration has
Table 4
|
Retention of organic micropollutants with NF and RO membranes
Compounds Substance type Membrane type Retention [%] Source
Bisphenol A EDC NF 1.9–99.7
p
Gallenkemper (2005)
Bisphenol A EDC RO 18–83 Kimura et al. (2004)
Bisphenol A EDC NF 47– . 99 Agenson et al. (2003)
Nonylphenol EDC NF 90.5–99.3
p
Gallenkemper (2005)
Estrone EDC NF/RO 13– . 80 Nghiem et al. (2004)
Estrone EDC NF 80– . 95 Scha¨ fer et al. (2003)
Estrone EDC NF 65–83 Braeken et al. (2005)
Estrone EDC NF 40– . 99 Weber (2004)
Estradiol EDC NF 20– . 80 Nghiem et al. (2004)
Estradiol EDC NF 49– . 99 Weber (2004)
Estradiol EDC RO 29–83 Kimura et al. (2004)
Diethylstilbestrol EDC NF 60– . 99 Weber (2004)
Mestranol EDC NF 90– . 99 Weber (2004)
Ethinylestradiol EDC NF 41– . 99 Weber (2004)
Atrazine Pesticide NF 59–92 Zhang et al. (2004)
Atrazine Pesticide NF 86–95 Chen et al. (2004)
Atrazine Pesticide NF . 80 Plakas et al. (2006)
Simazine Pesticide NF 45– . 80 Zhang et al. (2004)
Primidone Pharmaceutical RO 85– 87 Kimura et al. (2004)
Isopropylantipyrine Pharmaceutical RO 69–78 Kimura et al. (2004)
Carbamazipine Pharmaceutical RO 85–91 Kimura et al. (2004)
Sufamethoxazole Pharmaceutical RO 70–82 Kimura et al. (2004)
p
retentions are corrected by the effect of concentration polarisation.
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been investigated for a number of purification applications
as shown in Table 3.
The largest full scale implementation of nanofiltration
in water treatment applications is the Me
´
ry sur Oise plant
close to Paris that was built to reduce the high organic load
in the raw surface water utilised for drinking water
production. Seasonal pesticide issues were the reason to
complement the multi-barrier concept by a dense mem-
brane process (Cyna et al. 2002; Beros et al. 2003).
In a number of studies the organic micropollutant removal
capacity of nanofiltration has been investigated and compared
to reverse osmosis (Table 4). Medium to high removal rates
have been observed for endocrine disrupting compounds,
pesticides and pharmaceutically active compounds.
In a recent study conducted in Germany on the appli-
cation of dense membrane processes to treat River Rhine bank
filtrate reverse osmosis was preferred when compared to
nanofiltration due to the even higher micropollutant retention
detected in this case (Loi-Bru
¨
gger et al.2007).
ACKNOWLEDGEMENTS
The authors acknowledge the European Commission for
funding the RECLAIM WATER project on “Water recla-
mation technologies for safe groundwater recharge”, 6th
Framework Programme on Research and Technological
Development, Global Change and Eco-systems Sub-priority.
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