1

Removal of Contaminants of Emerging Concern from Wastewater

Carlos G. Dosoretz
Technion – Israel Institute of Technology, Haifa, Israel

1 Introduction (WQd ) should be at least at the same quality that at

intake (WQi ): WQd ≥ WQi .
Water is pivotal for sustainable development, but These adverse conditions of the water resources has
water shortages and deterioration due to severe or brought water reclamation and reuse issues to the front
prolonged drought conditions, added to intensive agri- scenario, especially in countries facing water scarcity
culture and urbanization are seriously threatening the [3–5]. Nowadays, the water reclamation market is esti-
ecosystem integrity, especially in arid and semi-arid mated at around 14 000 million gallons per day of water
regions of the world. The wide discharge and reuse reused worldwide [6]. Most water reclamation applica-
of conventionally treated effluents for irrigation may tions have been developed to meet nondrinking demands
further aggravate the situation. Conventional wastew- and therefore mostly tailored on sanitation/pathogens
ater treatment removes bulk organic contaminant removal. Reuse of secondary or tertiary effluents in
leaving micropollutants, better-named contaminants agricultural irrigation seems the widest application of
of emerging concern (CEC), in the effluents. CEC reclaimed water, it is a midrange priced application
include, among others, pharmaceuticals and personal characterized by seasonal consumption, thus requiring
care products (PPCP), endocrine disrupting compounds spacious storing reservoirs. The most intense application
(EDC), suspected carcinogens, and nanomaterials in agricultural irrigation nowadays is practiced in Israel
[1, 2]. To this add antibiotic-resistant bacteria (ARB) and at an annual rate of water recycle per capita around
antibiotic-resistant genes (ARG). Discharge or reuse of 70–80 m3 per person, representing approx. 85% of all
inadequately treated effluent generates a gradual deteri- treated effluents annually [7, 8]. Besides a very few cases
oration of soil and groundwater properties and environ- of high-quality water reuse such as the Water Factory
mental pollution due to the spreading and accumulation 21 Direct Injection Project in California since 1976 or
of CEC. the NeWater program for high-quality industrial water
The fate of municipal treated effluents in the envi- in Singapore since 2009 [4, 9], water reuse disregards
ronment, either by discharge or reuse, is therefore a salinity and dissolved contaminants, not removed by
cardinal issue in terms of water sustainability and public conventional wastewater treatment processes. Owing to
health considerations aimed at preventing the spread public perception issues, direct potable reuse is limited.
of salts, viruses, CEC, ARB/ARG, metals, and other A list of main water reclamation applications is presented
unknown contaminants. In terms of water availabil- in Table 1.
ity, sustainability is largely related to the increase of Added to this, “de facto reuse” worldwide increases the
human population and water consumption, ability to exposure of wide sectors of the population to different
confront adverse effects of anthropogenic pollutants levels of the dissolved fraction of treated effluents and
and particularly under the umbrella of global changes. on the opposite, in developed countries, transferring
In response to these facts, the term “sustainable water the treatment costs to the water supply segment. De
systems” describes systems engineered or managed to facto reuse refers to the discharge of treated effluents
provide sustainable water for human consumption and upstream surface water, either rivers, lakes or artificial
maintenance of natural ecosystems. A simple quanti- reservoirs, and its intake for drinking purposes down-
tative definition of water sustainability must be based stream of those sources [10]. De facto reuse is quite
on the premise that water quality at discharge or reuse common worldwide and may be particularly alarming in
Encyclopedia of Water: Science, Technology, and Society, edited by Patricia A. Maurice.
Copyright © 2019 John Wiley & Sons, Inc.
DOI: 10.1002/9781119300762.wsts0044
2 Water Technology

Table 1 Accepted types of water reclamation worldwide.

Use Constraints Quality Cost range

Agricultural irrigation Seasonal demand Low/intermediate Midrange

Landscape irrigation Seasonal demand Low/intermediate Low
Non-process industrial Constant demand/site specific Intermediate/high Low
Non-potable urban Limited volumes Intermediate/high Low
Recreation/environmental Site specific Intermediate Low
Indirect potable-groundwater recharge Requires suitable aquifer Very high High
Indirect potable-surface water Availability of reservoir sites Very high High
augmentation

Source: Modified from [3, 4].

dry periods when natural water supplies are reduced and

Agricultural Domestic Industrial
wastewater makes up a larger proportion of the water.
The continuous progress in laboratory testing, which
highlights the presence of CEC in the aquatic environ- Sewage
ment, pushes new directives regarding their presence system
and removal from wastewater effluents [11]. While the
directives do not require the implementation of specific
treatment, controls of outflows of micropollutants is Reclamation WWTP discharge

emerging in industrialized countries.

Advances in membrane technology targeted to sea-
Infiltration
water desalination increased recovery of brackish water Soil Groundwater Surface water
(BW) and started to revolutionize marginal water treat- Runoff
ment, and especially wastewater effluents, enabling
purification systems well-suited for wide distribution Figure 1 Schematic pathway of dispersal distribution of
to meet the most stringent requirements. Over recent contaminants of environmental concern throughout the water
decades, the cost of dense pressure-driven membranes consumption cycle. WWTP, wastewater treatment plant.
Reclamation options as in Table 1. Agricultural discharge includes
with emphasis on reverse osmosis (RO) has decreased both plant and veterinary uses. Direct industrial discharge refers
and fluxes have dramatically increased, making mem- principally to on-site treated wastewater effluents. Dashed lines
branes an attractive technological solution for water depict possible leaks.
and wastewater effluent treatment. RO is recognized
as the most energy-efficient desalination method [12]. reviewed during the last thirty years, along with an
Using dense membrane filtration such as RO purified increase in the sensitivity and capabilities of the ana-
water can be obtained in a fast and continuous way with lytical detection techniques [1, 13–21]. Main sources
recoveries of almost 90%, while CEC and other con- of CEC are from domestic, agricultural, and industrial
taminants are concentrated in brines of relatively small origin, entering the cycle through surface water and
volume. groundwater. A generic outlook of dispersal distribution
This article, thus, aims at discussing the application of of CEC along and across the water consumption cycle is
advanced technologies for purification of treated efflu- presented in Figure 1.
ents, with emphasis on RO, targeted to remove CEC, CEC of domestic origin comprises all range of synthetic
metal, excess salt, and ARB/ARG possibly present in organic compounds directly discharged throughout the
wastewater. This will exclude them from circulating and municipal sewage system. It includes mainly household
contribute to sustainable wastewater disposal. consumption products and emission from health care
institutions and commercial and recreational centers
such as pharmaceuticals, personal care products, clean-
2 Contaminants of Emerging Concern ing, and sanitation products, etc. Direct spills through
in the Water Consumption Cycle leaks in the municipal area (gasoline stations, trans-
portation, etc.) may directly contaminate groundwater.
Presence of CEC at the different levels of the water As seen in Figure 1, CEC of domestic origin are the most
consumption cycle has been repeatedly reported and widely distributed throughout the water cycle reaching
 Removal of Contaminants of Emerging Concern from Wastewater 3

both groundwater and surface water by reclamation contain high concentrations of bacteria and different
uses and direct discharge, respectively. The main impact types of antibiotics from different sources [38–40]. There
of industrial emission is on surface water through dis- is evidence of an increased flow of ARGs throughout
charge of on-site treated effluents or indirectly through effluent treatment facilities, suspended biomass or
the municipal sewage system or wastewater treatment biofilms [41–43]. The ambivalent mode of action of
plants (WWTPs) (Figure 1). Agricultural emission is antibiotics causes increasing antibiotic resistance, one of
characterized by a broad type of pesticides and other the major problems of the twenty-first century.
plant additives applied for crop protection and vet- Bacterial response to antibiotics, like alteration
erinary drugs for animal production, mostly entering of the expression of genes involved in metabolism,
directly the water system by runoff and leaching. Reuse regulation, virulence, DNA or stress response, are
of treated effluents for irrigation with emphasis on concentration-dependent [44]. The transmission of
agriculture also contribute to spreading of CEC in the antibiotic resistance can occur either by ARBs or ARGs.
water cycle, especially through soil infiltration into the Elements that specialize in moving DNA within and
groundwater. between genomes include plasmids, transposons, inte-
Pharmaceuticals are among the most studied CEC grons, insertion sequences, and integrative conjugative
due to their extensive use and their increasing occur- elements and these elements and the genes they carry
rence in the aquatic environment. Potential sources for are collectively known as the mobilome [45]. The col-
pharmaceutical pollution include chemical manufacture lective genes that contribute to antibiotic resistance
facilities, medical facilities, and household consumption. are referred to as the antibiotic resistome [46], which
Eventually, a portion of the pharmaceutical compounds can be subdivided into intrinsic, environmental, and
generated from various potential sources will reach nonpredictive/silent [47]. ARGs are nowadays consid-
WWTPs and due to insufficient removal may often ered as “emerging contaminants” [48] or as xenogenetic
be discharged to various aquatic environments such pollutants, but with the critical distinction that they
as rivers, groundwater, and drinking water [22, 23]. replicate rather than degrade when released to pollute
Hospital and chemical manufacture facilities wastew- natural environments [44].
aters provide a significant source of pharmaceuticals
into the environment [24, 25]. These substances may
2.1 Micropollutants Regulation
be detected at much higher concentrations in source
wastewater than in household wastewater (may reach Discharge of CEC in the environment is poorly regu-
levels as high as several mg L−1 ) due to their inten- lated. The European Union water framework directive
sive use and lower dilution. Nevertheless, the main 2000/06/CE setup a strategy to define high-risk sub-
contribution in terms of mass input is from WWTPs stances to be prioritized (Directive, 2000). A list of 33
effluents. A special emphasis among pharmaceuticals priority substances and the respective environmen-
is on antibiotics. Most hospital wastewaters are dis- tal quality standards were ratified by the Directive
charged to a municipal WWTP with no pretreatment 2008/105/EC (Directive, 2008). Moreover, in direc-
[26] or with a pretreatment that only partially removes tive 2013/39/EU, it was recommended monitoring
pharmaceutical residues [27–29]. Similarly, because of and treatment options for a group of 45 substances,
lack of specific regulation, treatment at manufactur- which includes pesticides, phthalates, and poly-
ing facilities removes pharmaceutical residues to an cyclic aromatic hydrocarbons (Directive, 2013). In
only limited extent. Removal of antibiotics by conven- addition, Decision 2015/495/EU of 20 March 2015
tional activated sludge (CAS) in municipal WWTPs published a watch list of substances for European
was reported to be only partial (e.g. ciprofloxacin Union-wide monitoring. The list includes different types
removal 54%) [30, 31]. Table 2 presents concentration of micropollutants: a pharmaceutical (diclofenac),
of some widely studied CEC in the aquatic environ- three hormones (two natural, 17-β-estradiol and
ment. estrone, and one synthetic, 17-α-ethinylestradiol), three
The potential risk associated with the presence of macrolide antibiotics (azithromycin, clarithromycin,
antibiotics in wastewater relates mostly to the possible and erythromycin), eight pesticides (acetamiprid,
development of antibiotic-resistant bacteria. Domestic clothianidin, imidacloprid, methiocarb, oxadiazon, thi-
sewage, as well as wastewater originating in hospitals, acloprid, triallate, and thiamethoxam), a UV-absorbing
nursing institutions, industries, biological, probiotics (2-ethylhexyl-4-methoxycinnamate) and an antioxidant
industries, and industries that combine heavy metals, (2,6-di-tert-butyl-4-methylphenol) commonly used as
can be a significant source of bacteria resistant to antibi- food additive [11].
otics [37]. WWTPs are reported to be a neural node Switzerland is the first country enforcing CEC removal
for developing of resistance to antibiotics because they from municipal effluents, valid as of December 2016 [49].
4 Water Technology

Table 2 Concentration of selected CEC in the aquatic environment.a)

Compound WWTPs WWTPs Source Surface water Source Groundwater Source

influent effluent (ng L−1 ) (ng L−1 )
(ng L−1 ) (ng L−1 )

Caffeine na 23–776 [32] 2.9–194 4–505

[32] [2]
Carbamazepine 1662 950 [33] 4.5–61 10–2325
Diatrizoate 330 410 [34] 230b) [34] 3b) [34]
Diclofenac 397 119 [33] 150b) [35] 0–3050
Estrone na 2.2–36 [32] 1.7–5.0 [32] 0–79 [2]
Ibuprofen na 370b) [35] 70b) [35] 0–3110
Iomeprol 160 130 100b) <LOQ
Iopamidol 430 470 [34] 490b) [34] 160b) [34]
Iopromide 750 810 100b) <LOQ
Ketoprofen na 200b) 0.5–14 [2] 2.8–2886
[35]
Naproxen na 300b) 1.8–18 1.2–263
[32] [2]
Sulfamethoxazole 49 23 [33] 1.7–36 2–1100
Triclosan 0.03–23.9 0.01–6.88 [2] 35–1023 [36] 0–118

a) Data is presented as mean concentration or interval concentration.

b) Indicates median concentration.
na, data not available; LOQ, limit of quantitation.

The program includes the elimination of 80% by average microbial activity. Thus, pharmaceuticals in wastewater
of 10 CEC from a recommended list: amisulpride, car- are not relevant for the design of conventional WWTPs.
bamazepine, citalopram, clarithromycin, diclofenac, Modern CAS WWTP are very efficient for sanitation
hydrochlorothiazide, benzotriazole, candesartan, irbe- of wastewater and nutrients removal based on their
sartan, 4+5-methylbenzotriazole. original design purposes. In contrast, discharges from
The US Environmental Protection Agency (EPA) in municipal and industrial WWTP are considered as
2009 published a contaminants list/CCL-3 in which one of the major sources of spreading anthropogenic
104 chemicals or chemical groups will be moni- compounds into the aquatic system in industrialized
tored and considered for potential regulation. In this countries (Table 2). An increasing number of anthro-
list are found three pharmaceuticals (erythromycin, pogenic chemicals is detected in treated wastewater
17R-ethinylestradiol, and nitroglycerin), eight hor- and there is increasing evidence of adverse environ-
mones (17R-estradiol, 17β-estradiol, equilenin, equilin, mental effects related to WWTP discharges [18, 51,
estriol, estrone, mestranol, and norethindrone) as well as 52]. If the requirements at the end of pipe of WWTP
pesticides, disinfection by-products among others [50]. will not be modified this situation will deteriorate, since
the number of CEC worldwide is immense, more than
100 000 individual compounds currently on the mar-
ket with thousand new compounds being added every
2.2 Fate of CEC in WWTP
year.
Conventional WWTP, most if not all based on the CAS treatment involves essentially sedimenta-
activated sludge process, are not able to eliminate phar- tion of settable solids and biological degradation
maceutical residues efficiently. The main reason for of the macro-components of the organic matter
this is that most if not all synthetic organic compounds (mg L−1 –g L−1 ), mostly natural, and nutrients, added
present in sewage in general and CEC in particular, are to pathogens removal. Sorption to biosolids is the
at negligible concentration (ng L−1 –μg L−1 ) compared to primary removal mechanism for more hydrophobic
wastewater organic matter (mg L−1 –g L−1 ) and therefore compounds (pK ow > 4), some separated at the primary
they are irrelevant to growth linked-microbial degra- clarification and others throughout secondary clarifica-
dation (heterotrophic biomass). Furthermore, many of tion. Sorption adds a point of concern regarding the fate
these synthetic organic compounds, and especially phar- of the biosolids and their further use in agriculture even
maceuticals, have been synthesized to endure metabolic following anaerobic stabilization and/or composting.
activity, and therefore display persistent to recalcitrant Although no clear data regarding the fate of CEC during
 Removal of Contaminants of Emerging Concern from Wastewater 5

anaerobic digestion of biosolids are available, recycle of 150 Low range

reject water either back to the WWTP or release through High range
120
the autotrophic anammox system should be reconsid-
ered. The CEC of lower hydrophobicity (pK ow ≤ 3–4), 90

DOC (mg L−1)

especially PPCPs and EDCs, reach the aeration tank and 60
can be available for microbial degradation. The micro- 20
bial food chain in WWTP is driven by growth-linked
biodegradation of the macro-organic components at 10
the hydraulic conditions imposed by the continuous
regime. Although some CEC are intrinsically biodegrad-
0
able, at environmental concentration (ng L−1 –pg L−1 RW TDW WW SE TEf TEd QE
for individual components) and continuous regime
their transformation is negligible and irrelevant to the Figure 2 Variations in water quality along the municipal water
design and functioning of conventional WWTP [18, cycle, from water intake through wastewater treatment to
53–57]. Photolytic degradation from sun irradiation and discharge. Data is presented as dissolved organic carbon (DOC)
concentration. RW, raw (natural) water; TDW, treated drinking
volatilization are only minor routes for disappearance of
water; WW, wastewater; SE, secondary effluents; TEf , tertiary
most CECs in WWTP. effluents-filtration; TEd , tertiary effluents-degradation; QE,
Nevertheless, WWTPs that have nearly complete quaternary effluents-desalination. Source: [5, 65–68].
biological ammonia removal through nitrification
(i.e. high solids retention time) display co-metabolic
biotransformation of some CEC, e.g. single-stage trans- Upgrading these effluents by applying advanced treat-
formation. Autotrophic co-metabolism appears as the ment, mostly destructive (TEd : advance oxidation,
main pathway for reported transformation of CEC in ozonation, soil-aquifer treatment (SAT), activated car-
WWTP [58–61]. Transformation of pharmaceuticals at bon adsorption, etc.), can considerably increase quality
trace concentrations can proceed through autotrophic but still leave residual organics, inorganic contami-
co-metabolism, such as ammonia monooxygenase nants, and salts. Safe effluents for unrestricted reuse
(AMO) in ammonia-oxidizing bacteria (AOB). However, and sustainable discharge can be achieved by quater-
and even in the case that transformation of certain nary treatment (desalination), and even for indirect
compounds occur through primary metabolism, at the potable reuse (IPR) upon polishing of the permeate.
very end primary transformation products would be A water quality diagram based on the change of the
released. Since most initial stages of microbial transfor- dissolved organic matter (DOM) fraction of water and
mation are carried out but oxygenases and hydrolases, effluents, described by the dissolved organic carbon
these product of transformation, are hydroxylated with (DOC), along the different treatment schemes is shown
increased solubility, therefore, increasing exposure to in Figure 2.
ecosystems. Moreover, very often these intermediate In the transition from water to wastewater and
products can be more harmful than the parent com- treated effluents, not only a change in concentration
pounds to the aquatic/soil ecosystem [62, 63]. Because takes place but also in composition. Indeed, organic
of their operation at relatively lower organic loading matter of raw, natural water, is composed mainly by
and consequently high solids retention times, with humic compounds better known as natural organic
capability to retain colloids including ARBs, mem- matter (NOM). Effluent released from conventional
brane bioreactors (MBRs) might display some more treatment, secondary effluent (SE), the first instance
transformation than CAS [64]. Nevertheless, MBRs of discharge, contain in addition soluble microbial
still do not resolve the threat of release of CEC or products (SMP) resulting from biomass activity and
their transformation products in the end-of-the-pipe decay during biological treatment, and CEC comprising
effluents. all forms of synthetic organic compounds introduced
Effluents purification can exclude total dissolved during use or formed during treatment, such as dis-
solids (TDS) and CEC from circulating and contribute infection by-products [66, 69–71]. Whereas CEC are
to a sustainable wastewater disposal. Actual effluents at trace amounts (0.2–0.5 mg L−1 as DOC), NOM and
quality for irrigation and discharge meets sanitary SMP constitute the macro-component fraction of efflu-
concerns (TEf : mainly filtration and disinfection) but ents organic matter (EfOM) (10–13 mg L−1 as DOC for
leaves CEC behind, namely neglecting environmental well-treated effluent). This macro-component fraction of
and public health considerations aimed at preventing EfOM interferes with most advanced treatments aimed
the spread of viruses, salts, and soluble contaminants. at removing CEC.
6 Water Technology

3 Advanced Technologies for Water two main group present in secondary or tertiary-filtered
Reclamation effluent. Several organo-modified clays [72–74] and
porous β-cyclodextrin polymers [75], no yet in commer-
Advanced technologies for water reclamation need to cial application and with relatively narrow selectivity,
cope with sustainable water reclamation challenges com- have been reported for sorption of more polar or
prising: (i) Removal of soluble macro-contaminants or ionized CEC.
TDS components (salts, metals, radionuclides, nutrients, Oxidation technologies comprising ozonation, wet,
and thermal oxidation and a range of advanced oxi-
and residual DOM); (ii) Elimination trace-contaminants
dation processes (AOP) have been described for CEC
(CEC, ARB/ARG, unknowns); (iii) High water recovery
removal from marginal water and treated effluents.
ratio (≥90%); (iv) Safe release of treatment residues.
Owing to their broad range of oxidation and ease of
Since CEC released into the wastewater stream encom-
implementation, ozonation and UV/H2 O2 have the
pass tens of thousands, or perhaps even hundreds of
actual highest potential for full-scale implementation
thousands of molecules, generic removal technologies
among the oxidation techniques, although, ozonation
with proven capabilities, even at very low concentrations,
is considered most cost-effective. Combination of both
have to be practiced.
can achieve increased elimination of a broad range of
The main advanced technologies reported for removal CEC by combined reaction of ozone and OH radicals
of soluble contaminants from treated effluents are and direct photolysis.
adsorption onto activated carbon, oxidation processes, SAT is a procedure applied in large scale for produc-
and tight membrane separation. Although other experi- tion effluents for unrestricted irrigation in Israel (Dan
mental technologies are available, these three processes Region Project) and in Tucson and Mesa, AZ or in Cali-
exist commercially and have demonstrated feasibility in fornia (USA) among other locations, releasing reclaimed
full-scale application. Nevertheless, whereas adsorption water of improved quality with DOC < 5 mg L−1 [66,
and oxidation are effective only toward the organic 76, 77]. Main mechanisms of DOM removal during
fractions, membrane separation, or desalination is infiltration are filtration, sorption, and biodegradation
active against all soluble fractions present in wastew- by the biofilm developed in the unsaturated zone. Rain-
ater effluents. A list of most often reported advanced fall infiltration increases quality by dilution. Managed
methodologies are presented in Table 3. Application may only for reclaimed water, SAT provides a storage during
include integrated processes combining technologies. nonirrigation period. Although biofilm can transform
For comparative data and details concerning advanced CEC [78], especially in oligotrophic environments, the
technologies consult reviews by Prasse et al. [51], Oulton fate of CEC and ARB/ARG during SAT is not clear.
et al. [54], Gur-Reznik and Dosoretz [56]. Since CEC are at trace concentration compared to
Adsorption on either granular activated carbon the major EfOM components, the effectiveness of both
(GAC) or powdered activated carbon (PAC) is effi- adsorption and oxidation techniques strongly depend
cient (>75% adsorption) principally toward more on contact time, background materials (type and con-
hydrophobic compounds (pK ow >4). However, it dis- centration), and above all, they leave behind inorganic
play moderate-to-low affinity (50–70%) for compounds contaminants.
with low hydrophobicity (2 < pK ow < 4) and very low to Regarding oxidation techniques, the dose applied
negligible (<25%) for hydrophilic CEC [17, 51, 56], the needs to be optimized depending on the wastewater

Table 3 Advanced water/wastewater technologies for removal of dissolved contaminants.a)

Adsorption Oxidation processes Dense membrane filtration Other emerging

(pressure driven)b) processes

Activated carbon (PAC, GAC) Advanced oxidation Reverse osmosis (RO) Enzymatic oxidation (laccase,
processes-AOP: UV/H2 O2 , peroxidase)
UV/TiO2 , UV/H2 O2 /O3
Organo-modified clays Ozonation (O3 ) Nanofiltration (NF)
Chitosan composites Non-thermal plasma (NTP)
Wet and thermal oxidation

a) Shaded background indicate commercial technologies.

b) Separate all range of dissolved contaminants, organic and inorganic. All others treat only organics.
 Removal of Contaminants of Emerging Concern from Wastewater 7

composition. Most characteristic quenchers are bicar- Furthermore, this technique does not demands extensive
bonate alkalinity, SMP, and NOM [79]. Because complete use of harmful chemicals and have small plant footprints
mineralization is not cost-effective, partial oxidation may and removes both organic and inorganic contaminants
lead to formation harmful end products such aldehydes, [91, 92].
nitrosamines, bromate, and unknown transformation Removal of CEC by tight membranes is complex
products of CECs. Therefore post-treatment is required and depends on the properties of the contaminants
before discharge. (pK ow , MW, charge), feedwater (pH, temperature,
Even though oxidation techniques and ozonation, in DOC, inorganic matrix), and membrane surface
particular, seem effective toward ARB and ARGs control (charge/zeta-potential, wettability/contact angle).
[80], appropriate dose and especially partial oxidation In general, three major interactions primarily affect
should be followed with care and a better understanding solute-membrane rejection, molecular sieving, electro-
is required. This is also relevant to the posttreatment static repulsion and van der Waals interaction [56, 93].
procedures. For example, the UV dose required to Presence of EfOM has been shown to increase efficiency
dimerize ARGs resulted at least one order of magnitude of separation of most neutral CEC by tight membranes
higher than that for inactivation of the host bacterium [94–96], whereas organic fouling layer that was estab-
[81]. Preliminary studies show that chlorination of lished over time served as an impermeable barrier for
wastewater effluents may encourage the formation of de nonionic hydrophobic solutes, such as steroid hormones,
novo antibiotic-like activity species, unknown antibiotics due to adsorption and partitioning [97]. Organic foul-
that could also enter the environment, potentially con- ing was also suggested to increase membrane surface
tributing to the growing problem of antibiotic resistance charge resulting in an increased rejection of nega-
[82]. Moreover, chlorinated transformation products tively charged organic solutes and hydrophobic organic
of compounds such as sulfamethoxazole, salicylic acid, solutes [98]. The higher selectivity regardless of feedwa-
iopamidol, and propranolol were identified during ter matrix composition make RO membranes, tighter
chlorination of water [83, 84]. than NF, the most generic core technology available
Regarding activated carbon, CEC removal capacity is for effluent purification, removing both organic and
limited by contact time, competition with background inorganic contaminants, including antibiotics and well
organic matter, contaminant solubility, and carbon type as antibiotic-resistant microorganisms to a great extent.
[17, 85, 86]. In addition, spent carbon needs to be con- Molecular sieving appears to be the dominant mecha-
stantly disposed or regenerated, i.e. incinerated in the nism for the high rejection rate of most soluble organic
case of PAC or thermally reactivated, pyrolyzed, in the compounds by RO membranes, namely low influence
case of GAC, in specialized locations. No data regarding of solute-solute and solute-membrane interaction,
fate of ARB and ARG during activated carbon adsorption regardless of the operating conditions and water matrix.
is available. Average rejection of 90–100% with a median value of 98%
The recent regulation in Switzerland, valid as of was reported for most pharmaceutical compounds with
December 2016, includes the full-scale implementation molecular weight ≥200 Da almost regardless of their
of ozonation+sand filtration or powdered activated car- chemical structure [54–56, 94]. Although some incon-
bon treatment (PACT) for CEC removal from municipal sistency may occur for highly hydrophobic molecules
effluents [87]. The program includes the 100 largest (pK ow >4), they have anyway low to negligible water
municipal WWTP, representing about 50–60% of solubility and are therefore irrelevant in effluent streams.
the wastewater treatment capacity. These plants are Rejection of CEC with MW lower than 200 Da depend
demanded to eliminate 80% by average of 12 CEC from on solute–solute and solute–membrane interaction
a recommended list [49]. The results of this experience especially for polar or dissociated compounds, with
will add light on the feasibility of these techniques to rejection values above 80%. Figure 3 depicts the capa-
reduce ecotoxicological risks of effluents discharge and bilities of CEC removal from well-treated municipal
the effect on “de facto” reuse. effluents by membrane desalination applying brackish
water type reverse osmosis membranes (BWRO). As
seen from these data, RO not only displays an effective
3.1 Effluents Purification by Dense Membrane
separation of most CEC with MW > 200 Da but in addi-
Separation/Membrane Desalination
tion shows almost constant efficiency regardless of the
Pressure driven-membrane separation, RO and nanofil- concentration in the feedwater.
tration (NF), or membrane desalination (see Table 3), is Some low-MW neutral and low polar CEC (<100 Da)
the most generic treatment technique for the reclamation are only partially removed by RO membranes, with
of municipal effluents [88–90], combining simplicity, ver- slight rejection around 70%. This includes some dis-
satility, and continuous processing of aqueous streams. infection byproducts or products of partial oxidation
8 Water Technology

Metformin MW
Acetaminophene 100

Permeate (ng L−1)

Acridine
Caffeine
10
Rejection (%)

Acridone
100 Ibuprofen
Carbamazepine
CBZ-EP
OX-CBZ 1
Sulfamethoxazole
CBZ-10OH
80 Ketoprofen
Lamotrigine
0.1
O-desmethylvenlafaxine
Dihydroxy-CBZ
Benzoylecgonine 0.01
Fluoxetine
Iopamidol
60 0.001
0 200 400 600 800 1 10 100 1000 10 000
MW (Da) Feed (ng L−1)

Figure 3 CEC removal from tertiary effluents by RO membrane desalination. Runs were performed between February and September
2016 in the 2-stage Technion pilot plant for effluents desalination with a 4–6 m3 h−1 capacity located at a commercial WWTP (consult [99,
100] for details). The pilot is fed with SE generated at the WWTP and comprises a pre-filtration stage (100 μm disk filter), ultrafiltration
(∼40–80 nm MWCO) followed by a 2-stage BWRO system. Typical product recovery 80–90% (5–10-fold concentration). Source: [101].

such as N-nitrosodimethylamine (NDMA) or chlo- easily upgradable for IPR by any oxidation technique for
roform [97]. Bromates, normally oxidation products further reinflitration into groundwater. IPR if perhaps
of AOP or ozonation, are practically fully rejected. the most sustainable reuse system since the high-quality
Application of low-pressure RO membranes and NF water reclaimed is stored under conditions that preserve
membranes, while providing approximately the same its quality.
product water quality and interaction with the polar
fraction of NOM, i.e. fulvic acids, either in the feedwater 3.1.1 Operational Conditions and Limitations
or in the concentration-polarization layer, have shown of Effluent Desalination
rejection close to 80% [102]. As dense microporous Because of operational constraints, only effluent of
membranes such very tight ultrafiltration (molecular WWTPs practicing full biological nutrient reduction
weight cutoff-MWCO < 1000 Da) are practically capable (BNR) and efficient organic matter removal are com-
of effective rejecting ARB (≥6 logs) and retain ARG patible with RO desalination, i.e. at least effluents of
TEf quality. A primary reason for low levels of nitro-
[103, 104], one may expect a complete removal in RO,
gen and phosphorous species in the feedwater to the
especially of ARGs.
RO system is due to eutrophication concerns during
High throughput RO membranes of BW type com-
brines disposal. Low phosphate is required in addition
monly applied for effluents desalination display high salt
due to scaling issues, i.e. calcium phosphate crystal-
rejection (≥99%) and effective removal of background
lization, especially at high recoveries [100]. Another
EfOM (90–95%), releasing DOC values of ≤0.5 mg L−1
consideration for efficient nitrogen removal from
with negligible levels of most individual CEC. In addi-
effluents is since nitrate rejection is relatively limited
tion, upgrading quality of effluent through membrane (93–95%) and ammonia/ammonium rejection is a strong
separation will not only reduce environmental risks function of pH. Owing to deposition or particulate
and alleviate soil and groundwater pollution but will fouling, a preparatory stage (e.g. microporous filtration,
also improve irrigation efficiency by reducing salinity coagulation-filtration) is required before effluents enter-
and emitter fouling, the main cause of uneven water ing the RO train to remove particulates and colloids.
discharge in micro irrigation, which in turn affect crop Efficient organic matter removal (meaning low concen-
yield and productivity [68, 105]. tration/low biodegradability of background DOM) is
Taking all these capabilities together, nowadays RO required to hinder biofouling issues. Membrane fouling
desalination, alone and in combination with other alters membrane surface characteristics, in addition to
advanced purification technologies, is the most generic the permeate flux decline [106–108], and may impact
and efficient means for effluents purification. Although to some extent CEC removal [98, 109]. Finally, changes
it is not feasible to desalinate all treated effluents and in surface conformation due to residues of oxidizing
quality of these effluents is by far above actual discharge biocides, such as hypochlorite, required for feedwater
regulations, it ensures to a great extent long-term sus- disinfection to ameliorate biofouling, may alter in the
tainability. In addition, desalination might decrease long run the separation of CEC in tight membranes
ecotoxicological constraints of “de facto” reuse, and in [110].
the long run, will decrease costs at waterworks plants. Finally, the resulting brines at high permeate recov-
Furthermore, since most if not all quenching compo- eries (∼90%), contain a 10-fold concentration of salts,
nents are absent in the permeate, these effluents are organics, and biological components [56, 100, 111]. This
 Removal of Contaminants of Emerging Concern from Wastewater 9

is probably the most critical issue in desalination of efflu- creating a full-cycle of treatment and releasing innocu-
ent, especially for inland plants, still not fully resolved ous brines to the aquatic environment. The continuous
and requires further research. The three main aspects price reduction and increased efficiency of membrane
to be considered for brines managements are concen- and oxidation systems faced from year to year would
tration, treatment, and disposal. Regarding discharge increase the accessibility of these technologies.
options, sea outfall is the most practical option; however, While the directives for upgrading effluent quality do
this requires transport solution and might increase eco- not require the implementation of specific treatment,
toxicological risks in the marine environment. Although control of CEC outflows is emerging in industrialized
today there are no legal regulations for brines discharge, countries. Besides upgrading existing municipal efflu-
development of low-cost-treatment technologies will ents changes in conception, management and planning
be required for wide implementation of effluent desali- of the urban water systems approach are needed [114,
nation. Owing to high concentration of quenching 115]. Intensive urbanization with continuous expansion
components, economic feasibility of advanced oxidation of big and intermediate-sized cities urge the develop-
is low [79, 112, 113]. Development of new nanomaterials ment of decentralized wastewater treatment to reduce
and lanthanides based-new oxidants or further devel- transportation to long distances, which is a decisive
opment of more “robust” oxidation processes such as factor in terms of economics and environmental safety.
wet, thermal, or supercritical water oxidation, together Furthermore, source control measures comprising
with cheaper energy sources may advance oxidation of on-site treatment of health care institutions (hospitals,
brines components. It should be noted that whereas clinics, dispensaries, nurseries, and nursing homes) and
application of these technologies for effluent treatment drug manufacturers have to be revaluated with highest
require continuous processes limited by contact time, priority.
their application in brines can be carried out in batch Although it is infeasible to remove all trace pollutants
processes, significantly simplifying the conditions of to levels below the detection limit from all wastewater
application. streams, reduction at source of synthetic chemicals
and drugs as well as antibiotic resistance determinants,
and treatment at source of concentrated streams may
be operative. Removal of dissolved organic pollutants
4 Concluding Remarks and mineral contaminants at trace levels cannot be
done without consuming energy, and therefore, the
The continuous progress in analytical laboratory testing, water–energy nexus and related life cycle analyses
which highlights the presence of organic and inorganic need to be rethought in terms of environmental and
pollutants at trace levels in the aquatic environment health risks and deterioration of water resources and
as well as antibiotic resistance determinants, pushes soils.
new directions regarding their removal from wastew-
ater effluents. Since existing technological capabilities
for upgrading effluents quality are almost unlimited, List of Abbreviations and Symbols
the optimal compromise for reclamation or discharge
management rests upon revision of planning/design of AMO ammonia monoxygenase
wastewater treatment, economical, and public health AOB ammonia oxidizing bacteria
considerations and environmental regulations. Upgrad- AOP advanced oxidation processes
ing quality of effluent will not only reduce environmental ARB antibiotic resistant bacteria
risks and alleviate soil and groundwater pollution but ARG antibiotic resistant genes
will also improve irrigation efficiency with reclaimed BWRO brackish water type RO membrane
water and decrease costs of “de facto” reuse of surface CAS conventional activated sludge
water. CEC contaminants of emerging concern
Integrated advanced processes with tight nonporous DOC dissolved organic carbon
membranes such RO as a pivotal stage are technologi- DOM dissolved organic matter
cally feasible and environmentally compatible to ensure EDC endocrine disrupting compounds
maximal removal of all trace contaminants from water EDC endocrine disrupting compounds
streams. RO membranes are nowadays the most generic SE-secondary effluents
means to remove organic and inorganic contaminants at EfOM effluents organic matter
once in compact footprint-continuous processes, easily GAC granular activated carbon
scalable and suitable for all kind of waters. Yet, brines IPR indirect potable reuse
treatment needs to be properly economically resolved for Kow octanol-water partition coefficient
10 Water Technology

LOQ limit of quantitation QE quaternary effluents

MBR membrane bioreactor RO reverse osmosis
MW molecular weight RW raw (natural) water
MWCO molecular weight cutoff SAT soil-aquifer treatment
NDMA N-nitrosodimethylamine SE secondary effluents
NF nanofiltration SMP soluble microbial products
NOM natural organic matter TDS total dissolved solids
NTP non-thermal plasma TDW treated drinking water
PAC powdered activated carbon TEd tertiary effluents-degradation
PACT powdered activated carbon treatment TEf tertiary effluents-filtration
PPCP pharmaceuticals and personal care WQ water quality (d: discharged; i: intake)
products WWTP wastewater treatment plant

Further Reading
Grandclément, C., Seyssiecq, I., Piram, A. et al. (2017). Environment, Comprehensive Analytical Chemistry, vol.
Water Res. 111: 297–317. 62. Elsevier Science. ISBN: ISBN: 9780444626578.
Petrovic, M., Perez, S., and Barcelo, D. (2013). Analysis, Stamm, V.-C., Eggen, R.I.L., Hering, J.G. et al. (2015).
Removal, Effects and Risk of Pharmaceuticals in the Environ. Sci. Technol. 49: 6374–6375.
Water Cycle: Occurrence and Transformation in the

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