Rizzo Et Al. - 2020 - Best Available Technologies and Treatment Trains T

Science of the Total Environment 710 (2020) 136312
Contents lists available at ScienceDirect
Science of the Total Environment
journal homepage: www.elsevier.com/locate/scitotenv
Review
Best available technologies and treatment trains to address current

challenges in urban wastewater reuse for irrigation of crops in
EU countries
Luigi Rizzo a,⁎, Wolfgang Gernjak b,c, Pawel Krzeminski d, Sixto Malato e,f, Christa S. McArdell g,
Jose Antonio Sanchez Perez f,h, Heidemarie Schaar i, Despo Fatta-Kassinos j,⁎
a
Department of Civil Engineering, University of Salerno, Via Giovanni Paolo II 132, 84084 Fisciano, SA, Italy
b
Catalan Institute for Water Research (ICRA), Emili Grahit 101, 17003 Girona, Spain
c
Catalan Institute for Research and Advanced Studies (ICREA), Passeig Lluís Companys 23, 08010 Barcelona, Spain
d
Section of Systems Engineering and Technology, Norwegian Institute for Water Research (NIVA), Gaustadalléen 21, N-0349 Oslo, Norway
e
Plataforma Solar de Almería (CIEMAT), Carretera de Senés, km. 4, Tabernas, Almería 04200, Spain
f
Solar Energy Research Centre (CIESOL), Joint Centre University of Almería-CIEMAT, Universitiy of Almeria, Ctra. Sacramento s/n, ES04120 Almería, Spain
g
Eawag, Swiss Federal Institute of Aquatic Science and Technology, CH-8600 Dübendorf, Switzerland
h
Department of Chemical Engineering, University of Almeria, Ctra. Sacramento s/n, ES04120 Almería, Spain
i
Technische Universität Wien, Institute for Water Quality and Resource Management, Karlsplatz 13/2261, 1040 Vienna, Austria
j
Department of Civil and Environmental Engineering and Nireas, International Water Research Center, University of Cyprus, P.O. Box 20537, CY-1678 Nicosia, Cyprus
H I G H L I G H T S G R A P H I C A L A B S T R A C T
• This work gathers the efforts of interna-

tional experts from NEREUS COST Ac-
tion.
• Advantages and drawbacks of BATs
discussed according to CECs removal
and AR control
• Possible advanced treatment options to
make wastewater reuse safer recom-
mended
• Smart combination of BATs and a suit-
able monitoring program necessary for
a safe reuse
• Further comparative studies among dif-
ferent advanced treatment methods
recommended
a r t i c l e i n f o a b s t r a c t
Article history: Conventional urban wastewater treatment plants (UWTPs) are poorly effective in the removal of most contam-
Received 5 November 2019 inants of emerging concern (CECs), including antibiotics, antibiotic resistant bacteria and antibiotic resistance
Received in revised form 21 December 2019 genes (ARB&ARGs). These contaminants result in some concern for the environment and human health, in par-
Accepted 22 December 2019
ticular if UWTPs effluents are reused for crop irrigation. Recently, stakeholders' interest further increased in
Available online 30 December 2019
Europe, because the European Commission is currently developing a regulation on water reuse. Likely,
Abbreviations: ARB, antibiotic resistant bacteria; ARGs, antibiotic resistance genes; AOPs, advanced oxidation processes; BAC, biological activated carbon; CBZ, carbamazepine; CECs,
contaminants of emerging concern; CPC, compound parabolic collector; DBPs, disinfection by products; DCF, diclofenac; DOC, dissolved organic carbon; ERY, erythromycin; FRC, free
residual chlorine; GAC, granular activated carbon; HO•, hydroxyl radical; LRV, Log removal value; MDR, multi drug resistant; MF, microfiltration; NDMA, N-nitrosodimethylamine; NF,
nanofiltration; PAC, powdered activated carbon; RO, reverse osmosis; TMP, transmembrane pressure; UF, ultrafiltration; SMX, sulfamethoxazole; UWTPs, urban wastewater treatment
plants.
⁎ Corresponding authors.
E-mail addresses: [email protected] (L. Rizzo), [email protected] (D. Fatta-Kassinos).
https://doi.org/10.1016/j.scitotenv.2019.136312
0048-9697/© 2018 Elsevier B.V. All rights reserved.
2 L. Rizzo et al. / Science of the Total Environment 710 (2020) 136312
Editor: Damia Barcelo conventional UWTPs will require additional advanced treatment steps to meet water quality limits yet to be of-
ficially established for wastewater reuse. Even though it seems that CECs will not be included in the proposed
Keywords: regulation, the aim of this paper is to provide a technical contribution to this discussion as well as to support
Activated carbon stakeholders by recommending possible advanced treatment options, in particular with regard to the removal
Advanced oxidation processes
of CECs and ARB&ARGs. Taking into account the current knowledge and the precautionary principle, any new
Antibiotic resistance
Contaminants of emerging concern
or revised water-related Directive should address such contaminants. Hence, this review paper gathers the ef-
Disinfection forts of a group of international experts, members of the NEREUS COST Action ES1403, who for three years
Ozonation have been constructively discussing the efficiency of the best available technologies (BATs) for urban wastewater
treatment to abate CECs and ARB&ARGs. In particular, ozonation, activated carbon adsorption, chemical disinfec-
tants, UV radiation, advanced oxidation processes (AOPs) and membrane filtration are discussed with regard to
their capability to effectively remove CECs and ARB&ARGs, as well as their advantages and drawbacks. Moreover,
a comparison among the above-mentioned processes is performed for CECs relevant for crop uptake. Finally, pos-
sible treatment trains including the above-discussed BATs are discussed, issuing end-use specific recommenda-
tions which will be useful to UWTPs managers to select the most suitable options to be implemented at their own
facilities to successfully address wastewater reuse challenges.
© 2018 Elsevier B.V. All rights reserved.
Contents
1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
2. Overview of the BATs for advanced treatment and reuse of urban wastewater: CECs abatement, effect on ARB&ARGs and process drawbacks . . . . . 3
2.1. Ozonation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
2.1.1. Abatement of CECs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
2.1.2. Effect on ARB&ARGs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
2.1.3. Formation of oxidation by-products . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
2.1.4. Application at full-scale as advanced treatment of urban wastewater . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
2.2. Activated carbon adsorption . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
2.2.1. Removal of CECs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
2.2.3. Application at full-scale as advanced treatment of urban wastewater . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
2.3. Chemical oxidants/disinfectants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
2.3.1. Chlorination . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
2.3.2. Disinfection with peracetic acid . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
2.4. UV radiation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
2.5. Advanced oxidation processes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
2.6. Membrane filtration . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
2.6.1. Removal of CECs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
2.7. Comparison among BATs for the removal of CECs relevant for crop uptake . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
3. Multi-barrier approach for a safe treated wastewater reuse in agriculture . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
3.1. Treatment trains for a safe reuse . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
3.2. Advantages, drawbacks and recommendations of the treatment schemes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
4. Concluding remarks . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
Declaration of competing interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
References. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
1. Introduction is related to consumption of raw or undercooked vegetables contami-

nated with pathogenic microorganisms stemming from the use of un-
Wastewater reuse is one of the most important alternatives to con- treated or poorly treated wastewater for crop irrigation (Fuhrimann
ventional water sources to address water scarcity. As a matter of fact, et al., 2016). In countries of higher income level, wastewater reuse for
around 1.2 billion people live in areas affected by serious water scarcity irrigation is regulated, at least in some of them (Paranychianakis et al.,
conditions (United Nations, 2014) and 1.8 billion people are expected to 2015), and concerns tend to shift from microbial risk (effective disinfec-
be living in countries or regions affected by water scarcity by 2025, action processes are typically included in the treatment train) to contam-
cording to United Nations reports (United Nations, 2014; FAO, 2013). inants of emerging concern (CECs), such as pesticides, pharmaceuticals,
Wastewater reuse for irrigation in agriculture is by far the most illicit drugs, synthetic and natural hormones, personal care products,
established end-use for reclaimed water (Drechsel et al., 2010a), in and resistant microorganisms (i.e. antibiotic resistant bacteria and
low-income countries as well as in arid and semi-arid ones (Drechsel genes (ARB&ARGs)). However, neither the release of CECs from urban
et al., 2010b). However, while solving water scarcity, wastewater wastewater treatment plants (UWTPs) into the environment (except
reuse can generate public health risks if treatment, storage and piping for Switzerland) nor their occurrence in wastewater for agricultural
are not adequate. The main risk, in particular in low-income countries, reuse has been regulated so far. CECs monitoring in UWTPs effluents
L. Rizzo et al. / Science of the Total Environment 710 (2020) 136312 3
to reuse for crop irrigation is one of the main debated issues among sci- risk at European Union level, but for which monitoring data are insuffi-
entists, policy makers and stakeholders at EU level (Christou et al., cient to come to a conclusion regarding the actual posed risk.
2017a; Piña et al., 2018; Rizzo et al., 2018; Deng et al., 2019) even in re- UWTPs are recognized among the main anthropogenic sources for
lation to the regulation for wastewater reuse which is about to be ap- the release of CECs and ARB&ARGs into the environment, therefore, tak-
proved by the Parliament (European Parliament, 2019). ing into account the environment and human health concerns related to
According to scientific literature, conventional treatment trains in their occurrence in UWTPs effluents and into the environment, different
UWTPs are poorly effective to comprehensively remove CECs (Petrie advanced treatment technologies have been investigated so far to find
et al., 2015; Falas et al., 2016; Krzeminski et al., 2019), which can finally effective solutions to minimize their release. In the following sub-
be released into the environment, constituting a particular concern paragraphs, the BATs for advanced treatment of urban wastewater are
when effluents are reused for crop irrigation. To be able to meet strin- introduced to evaluate their effect one CECs and ARB&ARGs. Possible
gent limits for wastewater reuse as well as to effectively remove CECs, advantages and drawbacks of these processes are also discussed accord-
advanced treatment steps should be implemented in conventional ing to the relevant scientific literature.
UWTPs (Krzeminski et al., 2019; Rizzo et al., 2019a). However, while
the effect of biological processes (Boshir Ahmed et al., 2017; Tiwari 2.1. Ozonation
et al., 2017; Krzeminski et al., 2019) and advanced treatment technolo-
gies (Miklos et al., 2018; Von Gunten, 2018; Roccaro, 2018; Marron 2.1.1. Abatement of CECs
et al., 2019; Rizzo et al., 2019a; Siegrist et al., 2019) on chemical CECs The oxidation capacity of the ozone process relies on the strong ox-
has been reviewed in different papers, less information is available idation potential of both, molecular ozone and HO radicals (HO•) (2.07
about ARB&ARGs and, most importantly, on possible treatment trains and 2.8 V against standard hydrogen electrode, respectively). While
combining several processes to successfully address these challenges. ozone reacts selectively with compounds containing electron-rich moi-
This review paper gathers the efforts of a group of international ex- eties (such as olefins, deprotonated amines or activated aromatics), HO•
perts, members of the NEREUS COST Action ES14031 “New and emerg- exhibit a low selectivity and fast reaction with a wide range of organic
ing challenges and opportunities in wastewater reuse” (Fatta-Kassinos and inorganic compounds (Von Sonntag, 2007). Ozonation and other
et al., 2015), who for three years have been constructively discussing oxidation-based processes were originally applied for disinfection pur-
the effect of the best available technologies (BATs) for urban wastewa- poses in drinking water treatment, but have been widely investigated
ter treatment on CECs and ARB&ARGs. Accordingly, the objective of this for the abatement of different CECs from urban wastewater since
paper is to introduce and discuss the BATs for advanced treatment of N10 years (Ternes et al., 2003). Based on the reaction rate constants
urban wastewater, as well as possible treatment trains to control the re- with ozone and HO•, CEC abatement can be predicted in municipal
lease of CECs, including ARB&ARGs, to produce wastewater for safe and wastewater (Lee et al., 2013). Hollender et al. (2009) and Bourgin
sustainable reuse practices in agriculture. In particular, the capability of et al. (2018) investigated the abatement of 220–550 micropollutants
ozonation, activated carbon adsorption, chemical oxidants/disinfec- at two full-scale UWTPs upgraded with ozonation (followed by sand fil-
tants, UV radiation, advanced oxidation processes (AOPs) and mem- tration). Compounds such as sulfamethoxazole, diclofenac, or carba-
brane filtration to abate CECs and ARB&ARGs are discussed including mazepine with high apparent second-order rate constants at pH 7
the advantages and drawbacks of these processes. Moreover, a compar- (kO3,pH 7 N 103) were abated by N80% at a specific ozone dose of
ison among the above-mentioned processes is performed for CECs rele- 0.4 g O3/g dissolved organic carbon (DOC). Compounds more refractory
vant for crop uptake. It is noteworthy that only results from to oxidation by ozone (kO3,pH 7 = 102–103), such as bezafibrate and ben-
investigations at pilot or full-scale on real wastewater were considered. zotriazole, were abated by 80% only at a higher ozone dose (~0.6 g O3/g
Subsequently, possible treatment trains including the above-discussed DOC). The high efficiency of ozonation in the abatement of CECs from
BATs are presented and recommended for possible application in the wastewater was also confirmed in other studies on a smaller group of
EU and other developed countries. Finally, possible advantages, draw- compounds (e.g., Antoniou et al., 2013; Magdeburg et al., 2014). After
backs and recommendations of the proposed treatment trains are ozonation, a biological post-treatment (sand filter or biological acti-
summarized. vated carbon (BAC) filter) is recommended to eliminate possible nega-
tive ecotoxicological effects or by-products generated during ozonation
2. Overview of the BATs for advanced treatment and reuse of urban (Von Gunten, 2018; Bacaro et al., 2019).
wastewater: CECs abatement, effect on ARB&ARGs and process
drawbacks 2.1.2. Effect on ARB&ARGs
Mechanisms for disinfection or inactivation of bacteria by ozone ex-
The occurrence of CECs into the environment is related to different posure include the disruption of bacterial cell walls (leading to the re-
human activities (Verlicchi et al., 2015; Bilal et al., 2019a, 2019b) and lease of intracellular constituents), damage of nucleic acids (breaking
it has been associated to biological adverse effects on living organisms aromatic structure), and breakage of carbon-nitrogen bonds of proteins
such as toxicity, endocrine disruption and antibiotic resistance in micro- leading to depolymerisation (Alexander et al., 2016; Michael-Kordatou
organisms (Manaia, 2017; López-Pacheco et al., 2019; Ma et al., 2019). et al., 2018). The inactivation efficiency by ozonation depends on the
Specifically, several CECs have been found to increase the risks for susceptibility of the target organism and ozone exposure, which is a
human-health, because they finally cause imbalance to hormonal and function of the wastewater characteristics and transferred ozone dose.
male/female reproductive systems and different disorders, namely me- Unlike CECs, the effect of ozonation on ARB&ARGs has not been investi-
tabolism, neurological, and immunological ones (López-Pacheco et al., gated systematically and thoroughly so far. Alexander et al. (2016) ob-
2019; Pedrazzani et al., 2019; Rueda-Ruzafa et al., 2019). served diverse patterns of resistances and susceptibilities of
In 2015, the European Commission established the EU Watch List opportunistic bacteria and accumulations of some ARGs during ozone
(Decision 2015/495/EU) to monitor 17 CECs in water. The target CECs treatment (0.9 ± 0.1 g O3/g DOC) of treated wastewater. Ozone affected
belong to different categories including antibiotics, estrogenic hor- microorganisms in different ways, with a high susceptibility of entero-
mones, non-steroidal anti-inflammatory compounds, pesticides and cocci (almost 99% reduction) compared to Pseudomonas aeruginosa,
herbicides, UV filters, and they were selected according to their poten- that displayed only minor changes in abundance after treatment. The
tial to cause damage to aquatic environments and to pose a significant investigated ARGs demonstrated an even more diverse pattern with 2
orders of magnitude reduction of erythromycin resistance gene
1
COST Action ES1403 New and emerging challenges and opportunities in wastewater (ermB) but a simultaneous increase in the abundance of ARGs (vanA,
reuse (NEREUS), http://www.nereus-cost.eu. blaVIM) within the surviving wastewater population. Ozonation
operated at high contact time (40 min) with an ozone dose of 0.25 g O3/ has been successfully applied as low-cost potable reuse option
g DOC was capable of inactivating total as well as antibiotic (sulfameth- (Gerrity et al., 2014; Reungoat et al., 2012; Stanford et al., 2017);
oxazole and trimethoprim) resistant Escherichia coli (E. coli), with the si-
multaneous reduction of the abundance of the examined genes 2.2. Activated carbon adsorption
(Iakovides et al., 2019). Accordingly, the studies published so far con-
firm that the ozonation process is effective in the inactivation of ARB 2.2.1. Removal of CECs
and to some extent in the removal of ARGs (Lüddeke et al., 2014; Unlike oxidation, adsorption is a separation process which does not
Zhuang et al., 2015; Alexander et al., 2016; Zheng et al., 2017; Sousa result in the formation of by-products. Activated carbon is the most
et al., 2017), but it seems that the process may also select for bacterial used adsorbent in water treatment for the removal of organic and inor-
population (Alexander et al., 2016; Sousa et al., 2017; Czekalski et al., ganic pollutants dissolved in water. Activated carbon treatment for the
2016). Regrowth of ARB during biological sand-filtration following removal of CECs from wastewater has been widely investigated
ozonation was found to partly compensate inactivation during ozona- (Boehler et al., 2012; Grassi et al., 2013; Rizzo et al., 2015; Ahmed,
tion (Czekalski et al., 2016). Moreover, mobile genetic elements may 2017; Kovalova et al., 2013; Michael et al., 2019). Packed bed adsorption
reach pre-treatment levels after some days of storage (Sousa et al., reactors with granular activated carbon (GAC) as adsorbent material are
2017), which can be of concern for wastewater reuse practice where commonly used in drinking water treatment. Due to process costs, their
treated effluents may be stored for some days before use (Iakovides application at full-scale as advanced urban wastewater treatment only
et al., 2019). recently has attracted the interest of UWTPs managers and profes-
sionals, as the concern for possible effect on human health and environ-
2.1.3. Formation of oxidation by-products ment of CECs has increased (Rizzo et al., 2019a; Siegrist et al., 2019). Its
Ozonation can result in the formation of biologically potent (e.g. advantage compared to powdered activated carbon (PAC) is that oper-
toxic, mutagenic) oxidation by-products. Among them, N- ationally it is easier to use, and it can be recovered and regenerated
nitrosodimethylamine (NDMA) and bromate are of particular concern when its adsorption capacity is exhausted. However, the process re-
for human health because they are potentially carcinogenic. Therefore, quires an adequate monitoring strategy, since adsorption competition
NDMA and bromate need to be measured to test the feasibility of ozon- results in a reduced CEC removal or even desorption of less adsorbable
ation as an option for advanced wastewater treatment at a specific loca- CECs with increasing treated bed volumes due to a decrease in available
tion (Schindler Wildhaber et al., 2015). Only if the concentrations adsorption sites. PAC can be applied as a post-treatment or dosed into
expected after dilution of discharged effluents are clearly below (poten- the biological unit in UWTPs and, due to its smaller particle size (higher
tial) drinking water standards (10 μg/L for bromate, 10 ng/L for NDMA, specific surface area), is more efficient compared to GAC in the removal
Bourgin et al., 2018), ozonation is considered suitable. Bromate results of water pollutants and specifically CECs (Nowotny et al., 2007; Boehler
from the reaction of O3 and HO• with bromide. NDMA can be formed et al., 2012).
from the reaction of amine precursors (e.g. containing hydrazine,
sulfamide, and dimethylamino functional groups) with generally low 2.2.2. Effect on ARB&ARGs
yields but that can reach up to ≥50% in exceptional cases (Kosaka Even though adsorption is not a disinfection process and not de-
et al., 2009; Schmidt and Brauch, 2008; von Gunten et al., 2010; signed to remove bacteria and mobile genetic elements, a contribution
Krasner et al., 2013; Sgroi et al., 2014). Because precursors are mostly to the reduction of antibiotic resistance in wastewater effluent can be
unknown or unidentified in wastewater, the formation of NDMA cannot expected due to possible entrapment of ARB&ARGs inside the pores of
be excluded a priori. NDMA can also already be present in the UWTP adsorbent particles (Zhang et al., 2017; Ashbolt et al., 2018; Bürgmann
influent. et al., 2018).
To minimize the release of biodegradable compounds including e.g.
transformation products of CECs formed during ozonation, a subse- 2.2.3. Application at full-scale as advanced treatment of urban wastewater
quent treatment by biologically active sand filtration (or adsorption) Activated carbon adsorption has been recently applied at full-scale
is recommended. For the evaluation of the water quality after ozonation, for advanced treatment of urban wastewater as alternative to ozona-
specific and unspecific toxicity of the treated wastewater needs to be tion, particularly in Switzerland and Germany, for the removal of CECs
measured with bioassays (Schindler Wildhaber et al., 2015). before effluent discharge into the environment (Rizzo et al., 2019a). De-
pending on DOC and operation technology, a dose of 10–20 mg/L PAC
2.1.4. Application at full-scale as advanced treatment of urban wastewater can be recommended to protect the aquatic environment (Boehler
Ozonation is well established in drinking water treatment, but only et al., 2012). A post-treatment is also needed in PAC treatment for sep-
recently has been applied at full-scale as advanced treatment of urban aration of residual PAC material. The use of GAC-packed reactors is more
wastewater in Europe for the removal of CECs before discharge into restricted since it does not allow to react to certain conditions (e.g. rainy
the environment. In particular in Switzerland, ozonation is considered periods), whereas PAC dose can be increased (Siegrist et al., 2019).
as one of the BATs to meet the requirement of the new Swiss water pro- However, GAC in combination with other treatment is used successfully
tection Act (micropollutants removal by 80% relative to the raw waste- for many years, but just for direct potable reuse application (Vaidya
water; Eggen et al., 2014, Bourgin et al., 2018), which requires an et al., 2019; Piras et al., 2020). As far as operation costs are concerned,
upgrade of selected UWTPs until 2040. A website of the Swiss Water As- feasibility studies conducted in the state of North Rhine-Westphalia
sociation provides updated information on European UWTPs that are (Germany) in the years 2009–2016 resulted in similar median costs
planning or running full-scale advanced treatment for CEC removal (0.04 €/m3) for ozonation (16 plants), PAC (11) and GAC (9) processes
(www.micropoll.ch). (Fig. SI4 in Rizzo et al., 2019a), with highest variability for GAC treat-
The occurrence of organic matter (measured as DOC) and other ment. Overall costs, including investment and operation, vary substan-
readily oxidizable compounds (such as nitrite) in the effluent of biolog- tially with the size of the UWTP. For mid-scale plants (~50,000 PE),
ical treatment affect ozone exposure and should be considered when the costs are in the range of 0.10 to 0.15 €/m3 treated wastewater, de-
defining the ozone dose for the abatement of CECs. An ozone dose in creasing further with increasing plant size even below 0.05 €/m3, with
the range of 0.4–0.6 g O3/g DOC (in the absence of nitrite) was found PAC treatment being slightly more expensive than ozonation (Fig. 4,
to be suitable to efficiently abate micropollutants (Hollender et al., Rizzo et al., 2019a). Consistently with the numbers determined in
2009; McArdell et al., 2015; Bourgin et al., 2018). Cost evaluations are Germany, overall costs for PAC (0.10–0.15 CHF/m3, 1 CHF being 0.88 €
shown later (Section 2.2.3) in comparison to treatment with activated on January 18th, 2019, for dosing 10 mg/L PAC in a large plant with
carbon. In the US and in Australia, ozonation followed by a BAC filter 590,000 p.e.) were estimated to be higher than for ozonation
(0.04–0.06 CHF/m3, for dosing 5 mg/L ozone in a large plant) in investigated, different results were observed. For example, ARGs ereA
Switzerland (McArdell et al., 2015, Abegglen and Siegrist, 2012). and ermB persisted in chlorinated (15 mg Cl2 min/L) urban wastewater
samples (Yuan et al., 2015) and chlorination was found to be effective in
2.3. Chemical oxidants/disinfectants ARGs removal (3.16 Log for sulI and 3.24 Log for tetG after 120 min treat-
ment) only at non-realistic chlorine concentration (160 mg/L) (Zhuang
Chlorination is by far the most common method of wastewater dis- et al., 2015). On the opposite, Zheng et al. (2017) observed that chlori-
infection, but the concern for human health and the environment re- nation can reduce ARGs (tetA, tetM, tetO, tetQ, tetW, sulI and sulII) abun-
lated to the formation of toxic by-products (e.g., trihalomethanes, dance to some extent (b1 Log unit for tetA) even under realistic
haloacetic acids and related contaminants) is increasing the interest to- operating conditions (5 mg/L of chlorine, 30 min contact time). More-
wards alternative chemical disinfectants, such as peracids. Among over, Yoon et al. (2017) observed 4 Log reduction of ARGs concentration
them, peracetic acid (PAA) already finds different applications at full- (two differing amplicons located in the commercially available plasmid
scale in UWTPs, particularly in Italy (Formisano et al., 2016; Di Cesare pUC4K i.e., ampR and kanR) with 33–72 (mg·min)/L chlorine dose at
et al., 2016a) and in the USA (Bell and Wylie, 2016; Stewart et al., pH 7 in urban wastewater. In particular, intracellular ARGs showed
2018). Accordingly, chlorination and PAA disinfection are discussed in lower rates of damage compared to the extracellular ARGs, possibly
the subsequent sub-paragraphs. Neither of the two technologies is ap- due to the protective roles of cellular components. However, when pro-
plied for CEC abatement as they are not economic and produce prob- cess efficiency was investigated in full-scale UWTPs, chlorination did
lematic effluents. not prove to have significant contribution to ARGs (tetA, tetW, tetO,
ermB, qnrS, blaTEM sulI) removal (Munir et al., 2011; Gao et al., 2012;
2.3.1. Chlorination Di Cesare et al., 2016b).
Wastewater disinfection by chlorine is typically performed by chlo-
rine gas (in medium – large UWTPs) or hypochlorite (either calcium or
sodium). Limited studies have focused on the abatement of CECs by 2.3.2. Disinfection with peracetic acid
chlorine, which was found to be quite poor, in particular if compared PAA is a strong and broad-spectrum disinfectant, with high
to oxidation/disinfection processes with higher oxidation potential reduction-oxidation (redox) potential and strong biocidal effects on
such as ozone and other AOPs (Anumol et al., 2016; Hua et al., 2019). bacteria. Because of the formation of toxic by-products in chlorination,
For example, Li and Zhang (2011) reported abatement of antibiotics PAA is increasingly replacing chlorine in UWTPs as it shows a broad-
during wastewater treatment with chlorine in the range of 18% spectrum efficiency and comparable way of application (Antonelli
(roxithromycin) to 40% (trimethoprim), while cephalexin and ampicil- et al., 2013; Formisano et al., 2016; Di Cesare et al., 2016a).
lin were abated by 99% and 91%, respectively. However, the chlorine In spite of no significant formation of disinfection by products
dose was not reported in this study, and cephalexin and ampicillin are (DBPs) resulting from wastewater disinfection by PAA when low
beta-lactam antibiotics that hydrolyze very quickly, so these results do doses are used (b5–10 mg/L) (Nurizzo et al., 2005), PAA was found to
not allow to discriminate hydrolysis contribution from chlorine oxida- be toxic for bacteria and crustaceans, even at concentrations lower
tion effects. Contrasting results are documented in the scientific litera- than the ones commonly used in wastewater disinfection (2–5 mg/L).
ture for sulfamethoxazole (SMX). While Gao et al. (2014) observed an But when PAA was compared to other disinfection processes, a lower
almost complete abatement of SMX (initial concentration in the range toxicity against aquatic organisms was observed. In particular Da
0.05–2 mg/L) within 15 min contact time and 2.0 mg/L of chlorine, De Costa et al. (2014) compared PAA (5 mg/L, 20 min contact time), UV
Jesus Gaffney et al. (2016) observed only 20% abatement (pH 6–7, light (average UV dose at 254 nm 670.8 mJ/cm2, 120 s contact time),
2 mg/L of free chlorine) of SMX after 2 h contact time. However, when ozone (29.9 mg/L, 5 min contact time), and sodium hypochlorite
reaction kinetics of SMX were investigated in different water matrices, (2.5 mg/L, 20 min contact time) against Ceriodaphnia silvestrii, Daphnia
the results achieved in real wastewater ([SMX]0 = 2.0 × 10−6 M, similis, Chironomus xanthus, and Danio rerio and toxicities after treat-
pH 7.3, free residual chlorine (FRC) 11 mg/L) confirmed the substantial ment were in the order of free chlorine N ozone N UV N PAA after the re-
degradation of SMX observed in deionized water (half-life of 23 s was spective disinfection treatments had been applied to secondary effluent.
measured under pseudo-first-order conditions ([FRC]0 = 20 μM Due to its lower oxidation potential compared to ozone and hy-
(1.4 mg/L))) (Dodd and Huang, 2004). This expectation is supported droxyl radicals, possible abatement of CECs in wastewater by PAA has
by existing observations at full-scale UWTPs, where 89.6% SMX abate- not attracted the interest of the scientific community. As matter of
ment was observed (Renew and Huang, 2004). Despite the fact that sin- fact, PAA effect on CECs has been investigated only as control test com-
gle compounds are degraded by chlorination, a broad abatement of pared to UV/PAA process (Rizzo et al., 2019b). Unlike carbamazepine
CECs cannot be achieved; for example, poor or no abatement of (no abatement observed even after 300 min contact time), diclofenac
diclofenac or carbamazepine was observed (Hua et al., 2019). was effectively oxidized by 2 mg PAA/L already after 60 min (80% abate-
Chlorination can result in the formation of toxic by-products, includ- ment), while SMX was abated at a lower percentage (52% after
ing trihalomethanes and haloacetic acids (Richardson et al., 2007). 300 min). As PAA effect on ARB is of concern, the limit of detection
Moreover, in effluents with incomplete nitrification, chlorine combines was achieved within 15 min treatment in groundwater inoculated
with ammonia to form chloramines or so-called combined chlorine. with an antibiotic resistant E. coli strain by 1 mg/L and 2 mg/L of PAA
Chloramine chemistry is complex and will not be discussed further (Rizzo et al., 2019b). However, the water matrix strongly affects bacte-
here, but it is noteworthy that chloramines are weaker oxidants and dis- rial inactivation efficiency. As a matter of fact, Huang et al. (2013) ob-
infectants compared to free chlorine. NDMA is a typical disinfection served lower inactivation in reclaimed water with a higher PAA initial
byproduct when chloramines are generated in wastewater effluents dose (20 mg/L). In particular, inactivation was higher for ampicillin-
(Sgroi et al., 2018). It can be concluded that chlorination is not an option resistant bacteria (2.3 Log) than for total heterotrophic bacteria
for CECs abatement and could produce an adverse effect on effluent or- (2.0 Log) and tetracycline resistant bacteria (1.1 Log) after 10 min treat-
ganic composition when used for disinfection. ment. Moreover, the regrowth of chloramphenicol-and tetracycline-
The effect of chlorination on ARB is being investigated since the 70s resistant bacteria, as well as total heterotrophic bacteria was N10-fold
(Grabow et al., 1976). Although the chlorination process was found to compared to those in the untreated wastewater sample (22 h stilling
effectively decrease antibiotic resistant E. coli in wastewater, it may se- culture after exposure to 2 or 5 mg PAA/L as for 10 min). Di Cesare
lect bacterial population by increasing antibiotic resistant E. coli strains et al. (2016a) evaluated the fate of diverse ARGs, heavy metal resistant
compared to the corresponding total population (Fiorentino et al., genes and of a mobile element (the class I integron) in three UWTPs
2015). However, when the effect of chlorination on ARGs was using different disinfection processes. In 2 (sulII and tetA) out of 4
(ermB and qnrS) of the quantified ARGs, a decrease was observed after was observed before and after UV disinfection, while for sulII even an in-
PAA treatment. crease was observed after disinfection (Di Cesare et al., 2016a).
2.4. UV radiation 2.5. Advanced oxidation processes
UV radiation (250–270 nm) is widely used for urban wastewater Advanced oxidation processes (AOPs) rely on the formation of hy-
disinfection either for effluent discharge or reuse (Munir et al., 2011; droxyl radicals that can abate a wide range of CECs (Rizzo, 2011; He
Di Cesare et al., 2016a). UV radiation can damage DNA, resulting in the et al., 2020) as well as inactivate microorganisms (Dunlop et al., 2010;
inhibition of cell replication and, in case of lethal doses, in loss of the Fiorentino et al., 2015). A possible classification of AOPs includes two
ability of reproduction. The effectiveness of a UV disinfection system de- groups: homogeneous processes (e.g., UV/H2O2, UV/Fe/H2O2, O3, O3/
pends on the characteristics of the wastewater, the UV fluence (inten- H2O2 etc.) and heterogeneous (solid semiconductors + light source,
sity × irradiation time), the type of microorganisms and reactor e.g., UV/TiO2, UV/ZnO) photocatalytic processes. Homogeneous pro-
configuration. Since turbidity and suspended solids drastically decrease cesses have been widely investigated as advanced treatment of urban
UV disinfection efficiency, conventional depth filtration should be used wastewater effluents and either are already applied at full-scale
before UV disinfection (not necessary when applied following a mem- (e.g., O3, see Section 2.1) or are characterized by short-/mid-term per-
brane biological reactor (MBR)). spective application (e.g., UV/H2O2, UV/Fe/H2O2) as opposed to hetero-
geneous photocatalytic processes (Rizzo et al., 2019a; Maniakova et al.,
2020). The main reason why heterogeneous photocatalytic processes
2.4.1. Abatement of CECs are not ready for full-scale application as advanced urban wastewater
UV radiation is not at all or is poorly effective in the abatement of treatment are related to photocatalyst preparation costs, photocatalyst
most of CECs from water and wastewater, but it can abate some antibi- quantum yield (effectiveness) and reactor configuration (Iervolino
otics and other CECs at very high UV doses (Kim et al., 2009; Rizzo et al., et al., 2020). In particular, heterogeneous photocatalytic processes can
2019b). For example, an almost complete abatement of tetracyclines be operated under two main configurations: (i) with the photocatalyst
and ciprofloxacin was achieved but only at high UV doses suspended in the reactor (i.e., slurry system) or (ii) attached to a sup-
(11,000–30,000 mJ/cm2) (Yuan et al., 2011) and high abatement effi- port (i.e., immobilized system). Due to the higher specific surface area
ciencies (86–100%) were also observed for sulfonamides (SMX and sul- available, a slurry system is more effective than an immobilized one,
fadimethoxine) and quinolones (norfloxacin and nalidixic acid) (Kim but a subsequent expensive separation process (e.g., coagulation, filtra-
et al., 2009). Iodinated X-ray contrast media were abated by N90% at tion, membrane) is necessary to recover the photocatalyst before efflu-
720 mJ/cm2 (Kovalova et al., 2013). ent discharge or reuse (Fernández-Ibáñez et al., 2003). Immobilized
photocatalytic systems have relatively lower quantum efficiency than
2.4.2. Effect on ARB&ARGs slurry ones, which results in longer treatment time and consequently
The effect of UV radiation on ARB&ARGs in urban wastewater has larger water volume to treat (Spasiano et al., 2015). Some homogeneous
been increasingly investigated in the last years at lab and full-scale photo-driven AOPs can also be operated under natural sunlight (solar/
(Munir et al., 2011; McKinney and Pruden, 2012; Rizzo et al., 2013; H2O2 or solar/Fe/H2O2) thus saving energy costs (Klamerth et al.,
Guo et al., 2013; Zhuang et al., 2015; Di Cesare et al., 2016a). Process ef- 2010; Ortega-Gómez et al., 2014; Ferro et al., 2015; Giannakis et al.,
ficiency strongly depends on the applied UV dose and target ARB&ARGs, 2016) and this can be considered as an attractive option for small
and possibly this is the main reason to explain differences between lab- UWTPs in areas with sufficient sunlight.
and full-scale evidences.
Efficient removal of heterotrophic bacteria harboring resistance to 2.5.1. Abatement of CECs
erythromycin and tetracycline was observed (Guo et al., 2013) (equiva- Due to their high redox potential hydroxyl radicals oxidize a wide
lent Log reduction being 1.4 and 1.1 at a UV dose of 5 mJ/cm2). As UV spectrum of organic contaminants, accordingly, AOPs successfully de-
dose was further increased to 20 and 50 mJ/cm2, respectively, ARB grade several organic micropollutants (Klavarioti et al., 2009; Rizzo,
were below the detection limit (1 CFU/mL). 2011). The most common AOPs studied are UV/H2O2, O3/H2O2, O3/UV,
The UV dose also affects the removal of ARGs. UV doses ranging from Fenton (Fe/H2O2), photo-Fenton (UV/Fe/H2O2) and heterogeneous
200 to 400 mJ/cm2 (at least one order of magnitude higher than those photocatalysis (e.g., UV/TiO2, UV/ZnO). Although UV/H2O2, is more effi-
for the inactivation of host bacterial cells) were required to remove 3 cient than UV alone to abate CECs, still more energy is needed compared
or 4 Log units of ARGs, namely ampC, mecA, tetA and vanA (McKinney to ozonation (Rizzo et al., 2019a). O3/H2O2 does not improve abatement
and Pruden, 2012). Actually, also lower UV doses (5–10 mJ/cm2) were of CECs compared to ozone alone in UWTP effluents, since effluent
found to be effective in the removal of ARGs (namely ereA, ereB, ermA, ozonation can be considered an intrinsically AOP due to the high HO•
ermB, tetA, tetO) but starting from lower initial ARGs copies per mL generation potential of the organic matrix (Buffle et al., 2006), at the
(Guo et al., 2013). The relative abundance of selected ARGs increased same time HO• are scavenged by the matrix (Acero and von Gunten,
with low doses of UV (Zhuang et al., 2015). Less than one order of mag- 2001; Kovalova et al., 2013). Fenton and photo-Fenton processes are
nitude removal of five tetracycline resistance genes (tetA, tetM, tetO, typically effective under acidic conditions (pH 3) and the abatement
tetQ, tetW) and two sulfonamide resistance genes (sulI, sulII) were ob- of three antibiotics, namely SMX, erythromycin (ERY) and
served in UV disinfection (UV fluence 10–160 mJ/cm2) of wastewater clarithromycin, from urban wastewater was investigated (Karaolia
samples taken from the secondary sedimentation tank of a UWTP in et al., 2017). SMX and ERY were efficiently abated from UWTP second-
Hangzhou, China (Zheng et al., 2017). The removal efficiency of the ary effluents by solar photo-Fenton in continuous flow operation with
five tet genes was between 52.0% and 73.5% at the lower fluence UV dis- N80% abatement at a hydraulic residence time of 20 min in non-
infection (40 mJ/cm2 or less), and between 79.7%, and 92.0% at high concentrating raceway pond reactors (Arzate et al., 2017). Nonetheless,
fluence (160 mJ/cm2). Lower removal efficiencies were observed for this operation mode at full-scale would result in additional process cost
sulI, sulII (78.1% and 71.1% respectively, at the higher fluence). and salinity increase because pH has to be first decreased and subse-
In full-scale monitoring (5 UWTPs in the USA), UV radiation quently neutralized before effluent discharge or reuse. However,
employed for disinfection did not prove to have a significant contribu- photo-Fenton has also been successfully investigated under almost neu-
tion to ARGs (tetw, tetO, sulI) and ARB reduction (Munir et al., 2011). tral pH conditions and solar radiation for the abatement of CECs from
These results were confirmed in a subsequent study at full-scale, urban wastewater with the addition of complexing agents. As a matter
where no significant difference in ARGs (namely, ermB, qnrS and tetA) of fact, the (solar driven) photo-Fenton process allowed to effectively
decrease CECs from urban wastewater under so-called mild conditions, driven photo Fenton processes (CPC reactor at pH 3 and raceway
i.e. under low Fe (b5 mg/L) and H2O2 (b20 mg/L) concentrations and ponds at neutral pH) did not effectively remove the target ARGs.
pH 5–6, thus avoiding the necessity for final separation of soluble iron The effect of heterogeneous photocatalysis with TiO2 on ARB&ARGs
species from the treated wastewater (Klamerth et al., 2010; De la Obra has been investigated in slurry and immobilized systems. According to
et al., 2017). The use of organic chelating agents makes the process fea- the results observed for homogenous photo-driven AOPs, even hetero-
sible and effective even under neutral pH conditions (De Luca et al., geneous photocatalytic processes, while effective in the inactivation of
2014; Fiorentino et al., 2018; Soriano-Molina et al., 2018). Unlike different antibiotic resistant bacterial populations (Tsai et al., 2010;
photo-Fenton, solar-UV/H2O2 process can be operated at neutral pH Rizzo et al., 2014a; Rizzo et al., 2014b; Dunlop et al., 2015; Zammit
without chelating agents, and it can successfully abate some CECs, but et al., 2019) may not be effective in the removal of some ARGs
longer reaction time compared to photo-Fenton is needed (Ferro et al., (Karaolia et al., 2018).
2015).
2.6. Membrane filtration
2.5.2. Effect on ARB&ARGs
AOPs can successfully inactivate ARB in urban wastewater (Karaolia
Membrane separation processes include microfiltration (MF), ultra-
et al., 2014; Rizzo et al., 2014a; Fiorentino et al., 2019). As a matter of
filtration (UF), nanofiltration (NF) and reverse osmosis (RO), which
fact, sunlight/H2O2 process resulted in a total inactivation of multi
may be operated separately or in combination with other processes as
drug resistant (MDR) E. coli (resistant to a mixture of three antibiotics:
a part of integrated technologies such as MBR. NF and RO are effective
ampicillin, ciprofloxacin and tetracycline), after 90 min of treatment
in the removal of both organic and inorganic CECs (Bellona et al.,
(Fiorentino et al., 2015). Noteworthy, longer treatment time
2004; Alturki et al., 2010; Garcia et al., 2013), while MF or UF are typi-
(120 min) was necessary to achieve a complete inactivation of the
cally used as pre-treatment of either NF or RO to control membrane
total E. coli population, despite the percentage of MDR E. coli ((total
fouling as well as for disinfection and solids removal. NF and specifically
E. coli − MDR E. coli) × 100 / total E. coli) increased as total E. coli popu-
RO provide the opportunity to reduce the effluent salinity, which can be
lation decreased with treatment time.
necessary depending on the downstream application of the treated ef-
However, the release of mobile genetic elements from bacterial cells,
fluent. However, a waste stream containing the separated salts and
that may take place after disinfection process, and the potential to trans-
other pollutants is generated as well.
fer antibiotic resistance through horizontal mechanism, have been
poorly investigated. Photo-driven AOPs have recently been investigated
to evaluate if they can be more effective in the removal of ARGs than 2.6.1. Removal of CECs
conventional disinfection processes, such as chlorination and UV radia- Removal of CECs by membrane processes is primarily based on size
tion. Ferro et al. (2016) investigated the effect of UV/H2O2 (broad-band exclusion, although electrostatic interactions between charged solutes
spectrum UV lamp with main emission in the range 320–450 nm), and negatively charged membranes typically have an important role
under realistic conditions for wastewater treatment (natural pH (7.6) in the removal (Bellona et al., 2004). Hydrophobic trace contaminants
and 20 mg H2O2/L), on antibiotic resistance transfer potential in urban have been shown to absorb to membrane surfaces reducing the rejec-
wastewater. The investigated process resulted in bacterial inactivation tion of these contaminants through both RO and NF. This has been
and a decrease of ARGs in intracellular DNA after 60 min treatment, shown to be particularly relevant in NF processes. Several other factors
but UV/H2O2 did not remove ARGs effectively. Actually, an increase up typically also affect the removal of the target CECs (such as phenolic ar-
to 3.7 × 103 copies/mL (p N 0.05) of blaTEM gene was observed in total omatic compounds) by membrane processes (Bellona et al., 2004). De-
DNA after 240 min treatment, while no difference (p N 0.05) was pending on the type of membrane, the range of rejections of CECs by
found for qnrS gene between the initial (5.1 × 104 copies/mL) and the both RO and NF is quite broad, but the rejection can be higher than
final sample (4.3 × 104 copies/mL). In UV/H2O2 process (pH 7, 99% for high rejection RO membranes (Krzeminski et al., 2017). How-
50–130 mJ/cm2), 4 Log reduction of ARGs (ampR and kanR) concentra- ever, in these membrane processes the CECs are accumulating in the
tion was observed in urban wastewater (Yoon et al., 2017). According rejected concentrate. The discharge of the concentrate to the environ-
to the results previously discussed for the chlorination process, intracel- ment can be problematic, as the original salt and pollutant load of the
lular ARGs showed lower rates of damage compared to extracellular secondary effluent, while not having increased in absolute mass, is
ARGs due to cell protective roles and significant HO• radical scavenging now concentrated typically by a factor of 3 to 7, depending on the per-
by cellular components. Zhang et al. (2016a) showed that UV/H2O2 can meate water recovery percentage of the membrane process. The pres-
effectively remove ARGs (2.8–3.5 logs removal of sul1, tetX, and tetG, ence of the contamination in concentrated form can also be an
within 30 min treatment) but only under conditions that seem unreal- opportunity for targeted treatment since pollutants are more effectively
istic for full-scale implementation (pH 3.5 and 340 mg H2O2/L), more- treated by advanced oxidation processes (usually governed by first
over UV fluence was not provided. order kinetics) as initial concentration increases (Miralles-Cuevas
Solar driven photo-Fenton process is effective in the inactivation of et al., 2016).
ARB (Karaolia et al., 2017; Fiorentino et al., 2019). When the process Full-scale applications of RO technology are reported in potable
(5 mg Fe2+/L, 50 mg H2O2/L, pH 3) was operated at pilot scale through reuse treatment trains, e.g. the Orange County Groundwater Replenish-
a compound parabolic collector (CPC) based reactor, on the effluent of ment System (California, USA), NEWater facilities at the Bedok, Kranji,
an MBR, a complete inactivation of the low initial bacterial population Ulu Pandan and Changi facilities in Singapore and the Torreele Reuse Fa-
(E. coli = 2 CFU/100 mL, P. aeruginosa = 4 CFU/100 mL, Klebsiella cility in Belgium (Raffin et al., 2013; Gerrity et al., 2013). RO is also used
spp. = 3 CFU/100 mL), including antibiotic-tolerant and susceptible in direct potable reuse treatment trains, along with MF or UF, in
bacteria, was observed, after 54 min of solar radiation intensity normal- Cloudcroft (New Mexico) and Big Spring (Texas) in USA (Gerrity et al.,
ized time (Karaolia et al., 2017). On the other hand, repair of 2013). NF typically removes CECs in the 300–1000 molecular weight
P. aeruginosa was observed, with 2 CFU/100 mL growing on the selective (MW) range, rejecting selected salts and most organic constituents
media 24 h after solar Fenton oxidation. Solar photo-Fenton process was and microorganisms, operating at higher recovery rates and lower pres-
also investigated in raceway pond reactors, at neutral pH conditions sures than RO processes. Accordingly, and when feasible, NF can be used
(20 mg Fe2+/L, 50 mg H2O2/L), in real urban wastewater and an effec- instead of RO to save some energy, chemical and concentrate disposal
tive inactivation of E. coli and Enterococcus sp. cefotaxime resistant bac- costs (Yangali-Quintanilla et al., 2010). While offering very high re-
teria was observed (detection limit (1 CFU/mL) achieved after moval efficiencies for CECs, specifically RO, on the downside these tech-
30–40 min, 3.2–4.7 kJ/L) (Fiorentino et al., 2019). However, both solar nologies exhibit high energy consumption.
2.6.2. Effect on ARB&ARGs study investigating the removal of ARGs in a full-scale wastewater treat-
As the separation principle is purely based on size, the removal of ment plant including biological and physicochemical treatment located
ARB can be expected to behave very similar to the removal of those on a swine farm showed very high removals for ARGs in both, NF and
not carrying antibiotic resistance. MF and UF are commonly applied bar- RO. The removals achieved depended on the ARG and ranged from 5
riers for pathogens, with MF being very effective against protozoa and to 8 Log removals compared to raw sewage (Lan et al., 2019).
bacteria, while due to a larger pore size, it is not very effective in remov- Above 99.2% removal of free DNA from UWTP effluent by NF mem-
ing viruses. UF removes all three classes of pathogens to a very high ex- brane in the lab-scale system was reported (Slipko et al., 2019). Similar
tent (2 to 4 Log removal values (LRV)) (Hai et al., 2014). NF and RO removal rates were observed both in water and in effluent. According to
membranes present in theory an even smaller pore size and should be the authors, besides size exclusion mechanism, electrostatic repulsion
“perfect filters”. In fact, N 6 LRV virus removal has been observed at plays also important role in removal of free DNA in NF and RO.
pilot-scale. However, due to the modular engineering approach system
breaches cannot be per se excluded and finding appropriate surrogate 2.7. Comparison among BATs for the removal of CECs relevant for crop
measurements remains a challenge to ensure disinfection during oper- uptake
ation, at least at levels beyond e.g. the removal of electrical conductivity
(Pype et al., 2016). During the last years, several classes of CECs have been proven to
The effect of membrane filtration, in particular NF and RO, on taken up through roots and translocated to the aerial parts of crop plants
ARB&ARGs, thus far, has been little discussed in the literature as the irrigated with treated wastewater, grown under hydroponic or green-
existing studies have focused mostly on MBRs and MF and UF mem- house control conditions, as well as soils irrigated with treated waste-
branes (Munir et al., 2011; Riquelme Breazeal et al., 2013; Rizzo et al., water in real agricultural systems. The uptake is largely dependent on
2013; Yang et al., 2013; Sun et al., 2016; Threedeach et al., 2016; Li CECs' bioavailability in soil pore water near the rhizosphere and thus
et al., 2019). on their physicochemical properties and the properties of the soil envi-
As previously mentioned, membranes can remove bacteria due to ronment. Once taken up, the transport of CECs within the plant vascular
membrane retention, thus contributing to reducing the spread of multi- translocation system (xylem and phloem) mainly depends on their li-
ple antibiotic resistant strains (Verlicchi et al., 2015). For example, filtra- pophilicity and electrical charge, as well as the physiology and transpi-
tion of ARGs spiked UWTP effluent through the 100, 10 and 1 kDa ration rate of crop plants and environmental conditions (i.e. drought
membranes in the lab-scale stirred ultrafiltration cell reduced vanA stress), (Nereus COST Action ES1403, Deliverable 11). Accordingly, dif-
and blaTEM ARGs by 0.9, 3.5 and 4.2 Log, respectively (Riquelme ferent crops have different potential for CECs uptake, for example, up-
Breazeal et al., 2013). The removal of plasmid-associated ARGs im- take potential is generally higher for leafy vegetables compared to
proved further at the presence of colloidal material in the water matrix fruit vegetables or cereal crops. The main biotic factors that may affect
and the colloids influence became more apparent as the membrane the uptake of CECs by plants are the plant itself (including the species,
pore size decreased. The DNA removal was attributed to membrane re- the variety and cultivar, the genotype, and the physiological state of
tention and following mechanisms: i) size exclusion of the DNA, ii) size the plant), and the soil fauna, which constitute the main cause for the
exclusion of DNA-colloid complexes, or iii) interactions with the mem- biodegradation and biotransformation of CECs within the soil (Ahuja
brane material (Riquelme Breazeal et al., 2013). et al., 2010; Goldstein et al., 2014). Climatic conditions and other envi-
Arkhangelsky et al. (2008, 2011) studied, in lab-scale dead-end ronmental perturbations (such as temperature, wind speed, UV radia-
membrane cell, penetration of plasmid DNA through UF membranes tion, salinity, drought, environmental pollution, etc.) constitute the
and demonstrated that despite electrostatic repulsion and a significant main abiotic factors that influence the potential for CECs uptake by
size difference between plasmid and pore sizes, DNA can penetrate crop plants (Dodgen et al., 2015; Zhang et al., 2016b). The majority of
through the UF membrane, indicating that UF did not provide absolute studies with regard to CECs uptake, either conducted in controlled lab-
barrier for DNA retention. Also, Riquelme Breazeal et al. (2013) ob- oratory or greenhouse conditions or under field or simulated conditions,
served that 1 kDa membrane did not completely retain plasmid and employed mostly (a) vegetables (leafy vegetables such as lettuce and
pointed out that the effective size of DNA is smaller than predicted by cabbage, fruit vegetables such as tomato and cucumber, and root vege-
molecular weight because DNA is a long, thin and flexible molecule. Al- tables such as carrot and radish) and (b) cereals and fodder crops (i.e.
though the penetration mechanism is not yet clear, Arkhangelsky et al. maize, wheat, alfalfa). Experimental results revealed that the potential
(2011) suggested that plasmid stretches into long hair-shaped flexible for CECs uptake by crop plants decreased in the order of leafy vegeta-
strands and penetrates pores based on ‘snake-like’ movement due to bles N root vegetables N cereals and fodder crops N fruit vegetables.
hydrodynamic pressure (transmembrane pressure, TMP) with gradual Though, the uptake of CECs by important crop plants, such as fruit
pore blocking. The proposed penetration mechanism is in accordance trees, has not yet been evaluated. Fruit trees, such as citrus, bananas,
with the findings of other studies on DNA (Marko et al., 2011; Travers, apple and other fruit bearing trees, have high net irrigation require-
2004). In addition, plasmid transportation levels are linearly correlated ments and evapotranspiration rates, which may render them as plants
to the TMP. with moderate to high potential for CECs uptake (similar to that of
Böckelmann et al. (2009) studied three artificial recharge systems in fruit vegetables) (Christou et al., 2019). Therefore, the recommendation
Europe. Combination of UF and RO proved to be an efficient barrier for on the BAT should consider both the soil and the type of the crop species
the elimination of ARGs. ARGs tetO and ermB detected in UWTP effluent to be irrigated by reclaimed water.
at concentrations of 1.05 × 107 ± 3.54 × 106 gene copies/100 mL and Consistently with the aim of the present review paper, a comparison
1.92 × 105 ± 1.06 × 104 gene copies/100 mL, respectively, were re- among the above-mentioned BATs was performed according to the
moved during the UF-RO process applied in the Torreele Reuse Facility. chemical CECs relevant for crop uptake by considering results from in-
Noteworthy, tetO were detected again, at low concentrations, in subse- vestigations at pilot or full-scale on real wastewater. According to the
quent sampling points: in the infiltration water before transport list compiled by NEREUS COST Action ES1403, 27 CECs are relevant for
(5.92 × 103 ± 1.39 × 103 gene copies/100 mL) and in the groundwater crop uptake (Krzeminski et al., 2019). The Action also applied selected
after infiltration (3.13 × 103 ± 1.52 × 103 gene copies/100 mL). In a re- criteria to establish a prioritised list with CECs which include the follow-
cent work, a wastewater reuse treatment train including MBR with MF ing: 1) high frequency of detection in treated effluents, which is related
membranes followed by RO provided up to 3.8 Log removal of the ARGs to high patterns of use and recalcitrance during the wastewater treat-
down to absolute abundance of 4.03 × 104 copies/mL (Lu et al., 2020). ment process, 2) environmental, agricultural and/or health concern; at
MF was capable of 2–3 Log removal of ARGs whereas subsequent RO least one of the following criteria should be met by the target CECs:
provided additionally up to 1.5 Log removal. Another recent full-scale a) DT50 (time necessary to degrade the 50% of the original contaminant
Table 1
Effect of BATs on the abatement of chemical CECs relevant for crop uptake. Only results from investigations at pilot or full-scale on real wastewater are presented (part of these data is
extracted from Table 3 and Supplementary information of “Rizzo et al., 2019a”).
CEC Process Scale of Water matrixa DOC CEC initial Comments CEC Reference
study (mg/L) concentration abatement
(%)
Sulfamethoxazole PAC Pilot/full RMW 5–10 171 ng/L (data 10–20 mg PAC/L. 0.3–1 h contact 58–64 Boehler et al., 2012;
only from 1 paper) time. Margot et al., 2013
GAC Pilot RMW 5.8 145 ng/L 7400 bed volumes treated. 14 min 59 Bourgin et al., 2018
EBCT.
O3 Pilot/full RMW 3.5–8.6 – 0.61 ± 0.04 g O3/g DOC. 94–97 Hollender et al.,
2009; Kreuzinger
et al., 2015; Bourgin
et al., 2018.
Free chlorine Full RMW – 576 ng/L Neutral pH, sample taken from the 89.6 Renew and Huang,
effluent of chlorination unit (dose 2004
not provided)
PAA Pilot RMW 24 100 μg/L 2.0 mg PAA/L, 300 min 52 Rizzo et al., 2019b
UV Pilot RMW 24 100 μg/L 4.58 kJ/L 100 Rizzo et al., 2019b
Solar Pilot RMW/SRMW 10.2–42.7 5.5 ng/L–1879 μg/L Fe: 5–10 mg/L; H2O2: 20–100 mg/L; N80–100 Klamerth et al.,
photo-Fenton pH: 2.8 or higher (5–6). 2010; Karaolia
(CPC rector) et al., 2014, 2017;
Prieto-Rodríguez
et al., 2013;
Solar Pilot RMW 40 282 ± 36.7 ng/L Continuous mode. Two liquid depths 81–100 Arzate et al., 2017
photo-Fenton (5, 15 cm) and three HRTs (80, 40,
(Raceway 20 min); Fe: 5.5 mg/L; H2O2:
pond) 30 mg/L. pH 2.8.
Photo Fenton Pilot RMW 5–7.5b 487 ng/L 30 mg H2O2/L; 2 mg Fe/L. pH 6–7 82 De la Cruz et al.,
(no chelating agents added). 5 low 2013
pressure mercury lamps (254 nm)
of 150 W each, incident light
70 W/m2.
UV/H2O2 Pilot RMW 5–7.5b 487 ng/L 30 mg H2O2/L. 5 low pressure 89 De la Cruz et al.,
mercury lamps (254 nm) of 150 W 2013
each, incident light 70 W/m2.
Sunlight/TiO2 Pilot SRMW 13 100 μg/L TiO2 immobilized on glass spheres 100 Miranda-García
(CPC reactor) (0.335 g TiO2/L). k = 0.03 1/min et al., 2011
RO Pilot Secondary treated – 56 ng/L Saehan 4040 FL, flux = 20 L/(m2·h) N98 Snyder et al., 2007
wastewater
RMW/primary 7.8 15–1800 ng/L Saehan 4040 FL, Osmonics AK4040, 94–99
treated wastewater flux = 17–20 L/(m2·h) (based on
2 studies)
Secondary/tertiary – 805–1030 ng/L Hydranautics ESPA2 N99 (based
treated wastewater on 2
studies)
RO Pilot RMW – 85–122 ng/L Filmtec TW30 25–40, 98 Sahar et al., 2011
flux = 22–31 L/(m2·h)
Filmtec BW30–400, 98
flux = 45 L/(m2·h)
RO Pilot RMW – 20–27 ng/L Ropur TR70-4021-HF N99 Dolar et al., 2012
NF Pilot RMW – 100–500 ng/L Filmtec NF90, MWCO 200 Da, 99 Mamo et al., 2018
flux = 18 L/(m2·h)
RO Hydranautics ESPA2, MWCO 100 Da, 100
flux = 18 L/(m2·h)
Diclofenac PAC Pilot RMW 7.3 1187 ng/L 10–20 mg PAC/L; 0.3–0.7 h contact 69 Margot et al., 2013
(±1.9) time.
GAC Pilot RMW 4.4 1008 ng/L 23,400 bed volumes treated. 14 min 72 Bourgin et al., 2018
EBCT.
O3 Pilot/full RMW 3.5–8.6 – 0.61 (±0.04) g O3/g DOC. 98–100 Hollender et al.,
2009; Kreuzinger
et al., 2018.
Free chlorine Full RMW – – Neutral pH 60 Anumol et al., 2016
PAA Pilot RMW 24 100 μg/L 2.0 mg PAA/L, 60 min 80 Rizzo et al., 2019b
Photo-Fenton Pilot RMW 5–7.5b 925 ng/L 20–50 mg H2O2/L; 2–4 mg Fe/L. 93–100 De la Cruz et al.,
pH 6–7. 5 low pressure mercury 2013
lamps (254 nm) of 150 W each,
incident light 70 W/m2.
Solar Pilot RMW/SRMW 10.2–36 1–5100 μg/L Fe: 5–10 mg/L; H2O2: 20–60 mg/L; 80–100 Klamerth et al.,
photo-Fenton pH: 2.8 or neutral (chelating agent 2010, 2011;
(CPC rector) used). Prieto-Rodríguez
et al., 2013;
UV/H2O2 Pilot RMW 5–7.5b 925 ng/L 20–50 mg H2O2/L. 5 low pressure 99–100 De la Cruz et al.,
(continued on next page)

Table 1 (continued)
CEC Process Scale of Water matrixa DOC CEC initial Comments CEC Reference
study (mg/L) concentration abatement
(%)
Sunlight/TiO2 Pilot RMW/SRMW 13–23 414 ng/L–100 μg/L 20 mg/L TiO2 and supported TiO2, 80–100 Miranda-García
(CPC reactor) neutral pH. et al., 2011;
Prieto-Rodríguez
et al., 2012;
wastewater
RMW/primary 7.8 1.1–38 ng/L Saehan 4040 FL, Osmonics AK4040, N93%
treated wastewater flux = 17–20 L/(m2·h) (from 2
pilots)
Secondary/Tertiary – 49–59 ng/L Hydranautics ESPA2 N98 (from
treated wastewater 2 pilots)
RO Pilot RMW – 500–580 ng/L Filmtec TW30 25–40, 95–99 Sahar et al., 2011
flux = 22–31 L/(m2·h) (from 2
Filmtec BW30–400, pilots)
flux = 45 L/(m2·h)
NF Pilot Effluent UWTP – 720 ng/L Flux = 1–2 LMH, TMP = 0.7 bar 60–65 Röhricht et al.,
2009, 2010
NF Pilot RMW – 260–440 ng/L FILMTEC NF90-4040, 200 Da 87–98 Cartagena et al.,
RO FILMTEC BW30-4040 88–96 2013
NF Pilot RMW – 100–500 ng/L Filmtec NF90 MWCO = 200 Da, 100 Mamo et al., 2018
flux = 18 L/(m2·h)
RO Hydranautics ESPA2 MWCO 100 Da, 100
flux = 18 L/(m2·h)
Carbamazepine PAC Pilot/full RMW 5–10 221–461 ng/L 10–20 mg PAC/L; 0.3–1 h contact 90–92 Boehler et al., 2012;
time; data from 3 papers. Margot et al., 2013;
Mailler et al., 2015;
Karelid et al., 2017.
GAC Pilot RMW 4.4 110 ng/L 23,400 bed volumes treated. 14 min 72 Bourgin et al., 2018
EBCT.
O3 Pilot/full RMW 3.5–7.6 – 0.61 ± 0.04 g O3/g DOC. 97–100 Hollender et al.,
2009; Kreuzinger
et al., 2018.
Free chlorine Full RMW – – Neutral pH No Anumol et al., 2016
removal
PAA Pilot RMW 24 100 μg/L 2.0 mg PAA/L, up to 300 min No Rizzo et al., 2019b
removal
Solar Pilot RMW/SRMW 10–36 70 ng/L–100 μg/L Fe: 5 mg/L; H2O2: 50–60 mg/L; pH: N24–100 Klamerth et al.,
photo-Fenton 2.8 or neutral (chelating agent 2010, 2011;
(CPC rector) used). Prieto-Rodríguez
et al., 2013;
Solar Pilot RMW 40 422 ± 54.9 ng/L Two liquid depths (5, 15 cm) and 86–96 Arzate et al., 2017
photo-Fenton three HRTs (80, 40, 20 min); Fe:
(Raceway 5.5 mg/L; H2O2: 30 mg/L. pH 2.8
pond)
Photo-Fenton Pilot RMW 5–7.5b 333 ng/L 20–50 mg H2O2/L; 2–4 mg Fe/L. 66–94 De la Cruz et al.,
pH 6–7. 5 low pressure mercury 2013
lamps (254 nm) of 150 W each,
incident light 70 W/m2.
UV/H2O2 Pilot RMW 5–7.5b 333 ng/L 20–50 mg H2O2/L. 5 low pressure 82–99 De la Cruz et al.,
Sunlight/TiO2 Pilot SRMW 13 100 μg/L TiO2 immobilized on glass spheres. 50–80 Miranda-García
(CPC reactor) et al., 2011
Sunlight/TiO2 Pilot RMW 15–50 56 ng/L 0.2 g TiO2 powder/L. 65–80 Bernabeu et al.,
(CPC reactor) 2011
wastewater
RMW/primary 7.8 181–410 ng/L Saehan 4040 FL, Osmonics AK4040, N99 (from
treated wastewater flux = 17–20 L/(m2·h) 2 pilots)
Secondary/tertiary – 237–271 ng/L Hydranautics ESPA2 N99 (from
treated wastewater 2 pilots)
RO Pilot RMW 64–99 ng/L Ropur TR70-4021-HF N99 Dolar et al., 2012
NF Pilot Effluent UWTP – 640 ng/L Flat sheet, flux = 1–3 L/(m2·h), 12 Röhricht et al.,
TMP = 0.3–0.7 bar 2009, 2010
NF Pilot RMW – 300–380 ng/L FILMTEC NF90-4040, 200 Da 78–92 Cartagena et al.,
RO FILMTEC BW30–4040 82–93 2013
NF Pilot RMW – 100–500 ng/L Filmtec NF90 MWCO = 200 Da, 79 Mamo et al., 2018
flux = 18 L/(m2·h)
RO Hydranautics ESPA2 MWCO 100 Da, 100
flux = 18 L/(m2·h)
a
RMW = real municipal wastewater; SRMW = spiked real municipal wastewater.
b
TOC.
concentration) in soil N 14 d, b) phytotoxicity at environmental relevant 3. Multi-barrier approach for a safe treated wastewater reuse in
concentrations, c) promote a selection pressure to soil microbiota, agriculture
d) potential human health effects according to threshold contaminant
concentration criteria, 3) significant uptake rate by crops (usually 3.1. Treatment trains for a safe reuse
bioconcentration factors (RCF = [root] / [growing medium]; LCF =
[leaf] / [growing medium]; FCF = [fruit] / [growing medium]) higher To make wastewater reuse safe for crop irrigation, a multi-barrier
than 1). The list of prioritised CECs includes carbamazepine (CBZ), approach to wastewater treatment is necessary. These barriers should
diclofenac (DCF), enrofloxacin, SMX, 17α -ethinyl estradiol, include typical processes for urban wastewater treatment (namely, pri-
lamotrigine and trimethoprim (Nereus COST Action ES1403, Deliver- mary mechanical pre-treatment, possible primary settling, biological
able 7; Boxall et al., 2012; Calderón-Preciado et al., 2013; Christou treatment etc.) and advanced treatments. Possible options of treatment
et al., 2017b; Goldstein et al., 2014; Miller et al., 2016; Tanoue trains (TTs) providing different effluent qualities are presented in Fig. 1.
et al., 2012; Wu et al., 2015; Zhang et al., 2016b). However, out of As matter of fact, no specific regulation on CECs (except in
27 crop relevant CECs only for 3 compounds, namely CBZ, DCF and Switzerland) and ARB&ARGs is in force that can justify a prioritisation
SMX, literature was found on their removal from wastewater matri- for these contaminants with respect to more traditional parameters
ces during different advanced technologies (Table 1). For SMX, high (in particular bacteria indicators such as total coliforms and E. coli) reg-
removal efficiencies (N80–100%) were observed during RO and NF, ulated in different countries and guidelines for wastewater reuse. In
UV radiation, chlorination (HOCl), ozonation and other AOPs, while particular, as ARB are of concern, total E. coli population was suggested
lower efficiencies (b64%) were observed for PAA and PAC treatment. to be a good indicator for the inactivation of the antibiotic resistant frac-
High DCF removal efficiencies (80–100%) were observed during RO tion (Fiorentino et al., 2015).
and NF, UV radiation, PAA treatment, ozonation and other AOPs, The minimum treatment scheme for safe reuse should include a
good removals (≅70%) for PAC, lower (60%) for chlorination. Finally, conventional depth filtration downstream of a biological process
high CBZ removal efficiencies (90–100%) were observed for PAC, (or an UF membrane as in case of MBR, Fig. 1, b), followed by a disin-
ozonation, and RO, a wide range of efficiencies (N24–100%) for fection unit with UV radiation (Fig. 1, a). This TT should effectively
AOPs and NF, depending on the process and operating conditions, allow to address typical parameters (e.g., biochemical oxygen de-
UV radiation resulted in a poor efficiency (16%), and no removal mand (BOD), chemical oxygen demand (COD), total suspended
was observed for chlorination and PAA treatment under the investi- solids (TSS), E. coli etc.) set in wastewater reuse regulation and
gated conditions. guidelines.
Fig. 1. Different options of treatment trains for urban wastewater reuse to address traditional parameters set in wastewater reuse regulation and guidelines (e.g., BOD, COD, TSS, E. coli etc.)
(a, b, c) and to effectively remove CECs in addition to the typical parameters (d, e, f, g). Advanced treatment in red lines; red dotted lines mean that process application should be evaluated
case by case. “Biological process” followed by “depth filtration” may be replaced by “MBR” for treatment trains “d” and “e”.
Chemical disinfection (in particular by chlorine) (Fig. 1, c) is cheaper 3.2. Advantages, drawbacks and recommendations of the treatment
compared to other disinfection options but the formation of DBPs schemes
should be considered, and the TT may become expensive compared to
other options if DBPs are removed before reuse. The main objective of this discussion and analysis is to suggest the
It has to be noted that, chemical disinfectants (such as chlorine and “best available technologies able to minimize the release of
PAA) as well as an MBR with UF membrane and UV radiation are poorly microcontaminants including ARB&ARGs, and biological risk, and fulfill
effective in the removal of CECs. requirements for a safe reuse for crop irrigation”. Important issues for all
Therefore, if (i) the corresponding limit for bacterial indicators is so TT discussed before are summarized in Table 2. Accordingly, and consid-
stringent that UV disinfection is not sufficient and/or (ii) CECs contam- ering that no exhaustive comparative studies addressing CECs and
ination should be effectively minimized, other, more effective treatment ARB&ARGs removal by advanced treatment methods are available in
technologies need to be considered (Fig. 1, d–g). scientific literature (Rizzo et al., 2019a), a comparative economic evalu-
Among AOPs, ozonation and photochemical processes showed ation would be questionable. In particular, advanced treatment
interesting results in the removal of CECs and ARB. In particular, in methods have been compared in terms of either CECs removal, costs,
the short term, ozonation and UV/H2O2 processes are more attractive disinfection efficiency, ARB and ARGs removal, formation of DBPs and
options (Fig. 1, d) compared to other photo-driven AOPs to abate oxidation reaction products, and final toxicity, but the whole impact
CECs as well as to effectively inactivate bacteria (Rizzo et al., on the environment through the simultaneous evaluation of all these is-
2019a) because: sues has not been investigated (Rizzo et al., 2019a). A recommendation
needs to be case-specific, taking into account possible regional regula-
1. their efficiency has been confirmed by different works available in tions on wastewater reuse for crop irrigation, intake and required
scientific literature. However, ozonation needs considerably less en- water quality, and local climate conditions, and the relative importance
ergy compared to UV/H2O2 treatment for the same CEC abatement of each aspect needs to be carefully evaluated.
level and shows full-scale application;
2. other homogeneous photocatalytic processes (such as photo-
4. Concluding remarks
Fenton) may request additional costs (e.g., pH adjustment, chelating
agents' addition) and/or have not yet been exhaustively investigated
The safety of treated wastewater to be reused for crop irrigation is
(e.g., UV/free chlorine, UV/PAA, sulfate radical based AOPs);
a relevant issue worldwide. Recently the interest has increased at EU
3. heterogeneous photocatalytic processes still have serious technolog-
level and stimulated a discussion among policy makers, scientists,
ical barriers for full-scale application.
professionals, practitioners and other stakeholders, because the
European Commission is about to approve a regulation on “Mini-
It is important to note that ozonation and AOPs typically ask for a bi- mum requirements for water reuse” (European Parliament, 2019).
ological post-treatment, i.e. a biological sand or activated carbon filtra- Accordingly, the aim of this paper is to provide a technical contribu-
tion, to remove biodegradable oxidation by-products and tion to this discussion by recommending possible advanced treat-
transformation products (Fig. 1, d). Rapid depth filtration or alterna- ment options to make wastewater reuse safer, in particular with
tively a dissolved air flotation treatment may be used as pre- regard to the removal of CECs and ARB&ARGs. Different factors affect
treatment method just before AOP in the event that residual suspended the choice of the most suitable treatment approach (i.e., water qual-
solids should interfere with subsequent processes. ity, local regulation/restrictions, process costs, type of crop, irriga-
Adsorption to GAC in packed reactors followed by UV disinfection tion method, soil type, environmental footprint, social acceptance,
(unlike O3 and UV/H2O2, adsorption is not a disinfection process) is etc.). Nevertheless, an attempt was made in this manuscript by
another option to improve the quality of effluent wastewater before discussing possible BATs for the advanced treatment of urban waste-
reuse (Fig. 1, e). In order to prevent GAC packed reactors from a fast water including their advantages and drawbacks.
clogging and increase back flushing intervals, cloth or rapid sand fil- The main conclusion of this work, that gathers the efforts of a group
tration may be used to remove suspended solids before the adsorp- of international experts, members of the NEREUS COST Action ES1403,
tion process. is that a single advanced treatment method is not sufficient to minimize
If PAC adsorption is used in combination with the biological process the release of chemical CECs and ARB&ARGs and make wastewater
(by adding PAC into the biological treatment) or as a separated unit reuse for crop irrigation safer, but a smart combination of them
thereafter, either depth filtration and/or MF/UF membrane processes (Fig. 1) and a suitable monitoring program (Table 2) would be neces-
should be used to remove residual PAC particles before discharge sary. This conclusion stems from the awareness that each treatment
(Fig. 1, f). As in GAC treatment, a UV disinfection may have to be method has its own weaknesses/drawbacks, for example:
installed.
Finally, membrane filtration with NF or RO followed by UV disin- • a biological post-treatment to remove oxidation by-products may
fection is another possible option for advanced treatment of waste- be necessary when ozonation or AOP is used as advanced treat-
water before reuse (Fig. 1, g). Pre-treatment by sand filtration can ment.;
be used to remove suspended solids to control membrane fouling, al- • ozonation and AOPs require toxicity monitoring because of possi-
though it is more common to filter settled effluent directly with MF ble formation of problematic oxidation reaction products;
or UF membranes. MF and UF membranes also provide suitable • adsorption processes should be followed by an effective disinfec-
pre-treatment for the NF or RO step (in such a case final disinfection tion process (i.e., UV disinfection) to meet the stringent limits for
by UV radiation is not necessary for crop irrigation). It is worthy to wastewater reuse;
mention that RO treatment would be additionally beneficial for • if PAC is used, a subsequent filtration or membrane process should
crop irrigation because of the removal of salts from the effluent. be applied to remove the adsorbent particles;
However, for membrane technologies to become sustainable there • chemical disinfection is not effective in the removal of CECs and
is need for a deep study of the adequate treatment and/or disposal ARGs, thus it should be coupled to other advanced treatment
of concentrates on a case by case basis. Implementation of effective methods. Moreover, possible formation of DBPs (i.e., chlorination
concentrate treatment has the potential to enhance treatment effi- by products) should be considered, and a subsequent treatment
ciency, move towards a near zero-liquid discharge and avoid un- for their removal may be necessary;
wanted discharge of CEC. • NF or RO membrane technology would require a pre-treatment
Table 2
Advantages, drawbacks and recommendations for each TT in Fig. 1.
TT (advanced treatment) Advantages Drawbacks Recommendations
a or b (UV) • Effective disinfection (including ARB inac- • If local standards for reuse are too strin- • Compliance with local residual bacterial
tivation) gent for residual bacterial density, UV density standards should be evaluated
• No DBPs formation compared to chemical may not be sufficient
disinfection • Poor/no CECs removal
• Partial removal of ARGs
c (chemical disinfection) • Effective disinfection (including ARB • Poor/no removal of CECs and ARGs • Toxicity tests recommended
inactivation) • Formation of DBPs • DBPs (depending on the disinfectants used)
• If local standards for reuse are too strin- should be monitored
gent for DBPs, some disinfectant cannot
be used (e.g., chlorine in Italy)
d (O3/AOP and biological • Effective disinfection (including ARB inac- • Formation of some DBPs (NDMA, bro- • Toxicity tests recommended
post-treatment) tivation) mate) during ozonation • NDMA and bromate should be monitored in
• CECs abatement high during ozonation • Formation of oxidation transformation O3 treatment
and (solar) photo Fenton, moderate with products during AOP and ozonation
UV/H2O2 • Partial ARGs removal
• Full-scale evidence on practicability only
for O3
e (GAC and UV) • Effective disinfection by UV • Poor/no removal of ARB&ARGs by GAC • Decreasing adsorption capacity with
• High CECs removal by GAC alone increasing bed volume should be taken into
• Full-scale evidence on practicability • For UV see above, TT a & b account
f (PAC and UV) • Effective disinfection by UV • Poor/no removal of ARB&ARGs by PAC
• High CECs removal by PAC alone
• Full-scale evidence on practicability for • For UV see above, TT a & b
CEC removal by PAC
g (NF or RO membrane filtration, • Effective disinfection for bacteria (incl. • Poor/no removal of ARGs at full-scale by • Impact of membrane characteristics on
with potential pre-treatment ARB) and protozoa for all membranes; MF (for UF some removal is expected) disinfection, ARB, ARG, and CEC removal
with MF or UF membranes) viruses well removed by UF, NF & RO • Poor CECs removal for MF and UF should be carefully considered in design
• ARGs well removed by NF and RO • High energy requirements for NF and RO • Consider AOP instead of UV disinfection if
• CECs removal from poor (MF, UF) to very • Generation of a substantial concentrate the risk of unknowns and spills is considered
good (NF, RO) depending on membrane waste stream by NF and RO high
type, • For post UV-C see TT a&b • Consider high UV doses if NDMA can be
• RO and partially also NF reduce salinity suspected in the membrane effluent (e.g.
• For post UV-C see TT a & b following prior chloramination)
(i.e., sand filtration) to prevent clogging and a sustainable solution and from the Spanish Ministry of Science, Innovation and Universities,
for the management of membrane concentrate. the State Agency of Investigation and EU FEDER program (project IN-
VEST: RTI2018-097471-B-C21). SM wishes to thank the Spanish Minis-
try of Economy and Competitiveness for funding under the
Further comparative studies among different advanced treatment ECOSAFEFARMING Project (International Joint Programming Actions,
methods on real wastewater, using different criteria (i.e., CECs removal, reference: PCIN-2017-005) and 2016 Water and FACCE JPIs Joint Call.
ARB&ARGs, toxicity, DBPs, costs) are recommended. The results will be JASP acknowledges the Spanish Ministry of Economy and Competitive-
useful to UWTPs managers to select the most suitable options to be im- ness and the European Regional Development Fund (ERDF) for funding
plemented at their own facilities to successfully address wastewater the project CTQ2016-78255-R. PK acknowledges the financial support
reuse challenges. provided by NIVA's Strategic Institute Initiative “Urban water chal-
lenges” (Research Council of Norway, contract no. 160016).
Declaration of competing interest
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Science of the Total Environment 710 (2020) 136312

Contents lists available at ScienceDirect

Science of the Total Environment

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

Best available technologies and treatment trains to address current

• This work gathers the efforts of interna-

1. Introduction is related to consumption of raw or undercooked vegetables contami-

2.4. UV radiation 2.5. Advanced oxidation processes

(continued on next page)

TT (advanced treatment) Advantages Drawbacks Recommendations

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