Emerging Pollutants - Ingenta Connect

Emerging Pollutants – Part II: Treatment Olya S. Keen1*, Katherine Y. Bell2, Carla Cherchi3, Benjamin J. Finnegan4, Meagan S. Mauter5, Austa Marie Parker6, James S. Rosenblum6, Holly A. Stretz7

ABSTRACT:

The goal of this review is to summarize

wastewater treatment, reclaimed water

new research published in the field of emerging pollutants doi:10.2175/106143014X14031280668731

in the past year. For the purpose of the review, unregulated and relatively new compounds found in wastewater, drinking water, recycled water and the environment were

Overview

considered. The review consists of two parts, with Part I

A few notes must be added on the terminology

focusing on the occurrence of the contaminants in the

associated with pollutants of emerging concern. In general,

media mentioned above, and Part II focusing on the

this class of pollutants includes compounds that have been

treatment technologies.

found in the environment, wastewater and drinking water relatively recently and are presently unregulated. Several

KEYWORDS:

emerging

pollutants,

endocrine

terms are used to denote emerging pollutants almost

disruption compounds, micropollutants, pharmaceuticals

interchangeably. Some of those terms are micropollutants

and personal care products, nanoparticles, antibiotic

and trace pollutants. There are also terms that refer to

resistance genes, trace organics, drinking water treatment,

subsets of emerging pollutants. Pharmaceuticals and personal care products (PPCPs) is an example of a term that

————————— 1*

indicates a narrower subset of emerging pollutants, as those

Civil and Environmental Engineering Department, 9201

can also include trace pesticides, insect repellents, musks

University City Blvd, University of North Carolina, Charlotte,

and fragrances, plasticizers, fire retardants, perfluorinated

NC, 28223; Tel. 704-687-5048; e-mail: [email protected] 2

compounds,

CDM Smith, Nashville, Tennessee

3

MWH Global, Chicago, Illinois

nanoparticles,

etc.

Recently,

antibiotic

resistance genes (ARGs) have also been included in the

4

CDM Smith, Chicago, Illinois

class of emerging pollutants and are believed to be related

5

Carnegie Mellon University, Pittsburg, Pennsylvania

to the trace levels of antibiotics in the environment.

6

University of Colorado, Boulder, Colorado

Another narrower subclass of emerging pollutants is 7

Tenessee Technical University, Cookeville, TN

endocrine disrupting compounds (EDCs). This term refers

2036 Water Environment Research, Volume 86, Number 10—Copyright © 2014 Water Environment Federation

to specific pollutants that have been demonstrated to have

and membranes are necessary to properly address emerging

an effect on the endocrine system of aquatic organisms or

pollutants. This appears to have driven development of

were designed with the purpose to act on a human

membrane technologies including techniques such as

hormonal system. Typical representatives are bisphenol A

functionalization and grafting of membrane materials. In

(BPA) and natural and synthetic human hormones.

chemical oxidation, advanced oxidation processes show the

Somewhat broader, but not all-inclusive terms are trace

most promise, however several studies caution regarding

organic compounds (TrOCs or TOrCs) and synthetic

the properties of the transformation products, which should

organic compounds (SOCs). Because most of emerging

be properly studied and understood. Catalytic processes

pollutants are trace synthetic organics, these terms are

have been one of the major focal points of the chemical

inclusive of the majority of the pollutants, with the

treatment technologies.

exception of metal nanoparticles, inorganic ions (e.g.

There is also a trend towards coupling various

bromate) and ARGs. Some of the less common terms in

processes which in many instances are shown to have

this category are unregulated organic compounds (UOC)

synergistic effects compared to each individual process.

and xenobiotic organic compounds (XOC).

And, multiple studies identified the differences between the

This paper provides a review of advances in the

bench-scale and synthetic wastewater research and the

field of the treatment of emerging pollutants during 2013. It

larger scale research with the more complex background

is divided into biological treatment, chemical treatment,

matrix. One of the most important research areas for future

and

focus should be on the translation of research results from

physical

treatment,

and

has

information

on

combinations and comparisons of technologies. Physical treatment

also

includes

separation

In addition to this review, several other reviews

processes, such as ion exchange and coagulation, as these

were published in 2013. Fatta-Kassinos and Michael (2013)

methods move the pollutant from one medium to another

summarized the outcomes of a workshop held in Cyprus

without changing it structurally. Some of the most

during September 2012, where the challenges of emerging

interesting trends that were noted in this review are

pollutant removal were discussed with respect to the

identification of specific organisms capable of TrOC

wastewater reuse practice. Some of the outcomes of the

biodegradation

traditional

discussion included the need of long-term (chronic)

Apart from

exposure data at sub-lethal levels, the need for a stricter

bacterial biodegradation, white rot fungus is receiving

standardization of protocols for measuring and monitoring

increased attention. Additionally, despite the improvements

emerging pollutants, the lack of effluent quality criteria and

in the biological treatment processes and their better

the

understanding, the consensus is still that chemical oxidation

cost/performance comparison evaluations.

and

physicochemical

bench-scale to pilot- and full-scale.

bioaugmentation

of

biological processes with these organisms.

identification

of

treatment

technologies


and

Other reviews focused on treatment technologies

of UOCs by coagulation/flocculation/clarification was

from conventional to advanced methods. A broad literature

limited. Air stripping was also not an effective treatment.

review on the presence and removal of pharmaceuticals in

Ozone did achieve a significant reduction of most

water

both

compounds with the exception of several phosphate-based

conventional and advanced treatment systems (Rivera-

fire retardants, N,N-diethyl-m-toluamide (DEET), caffeine

Utrilla et al., 2013). Advantages, disadvantages, important

and cotinine. Granular activated carbon (GAC) was not, in

design parameters, and key literature pertaining to the

general, effective except at one plant which did not pre-

treatment technologies were summarized. Another study

chlorinate, and the limited removal was attributed to the

(Rojas et al., 2013) provided a literature review and

possible presence of biological activity rather than

statistical analysis on the use of conventional wastewater

adsorption. Benner et al. (2013) published a critical review

treatment processes for the removal of emerging pollutants,

on the viability of biological treatment processes to remove

specifically focusing on biological processes (membrane

micropollutants from drinking water resources. The authors

bioreactors (MBRs), sequencing batch reactors, lagoons,

provided a summary of occurrence of micropollutants in

trickling filters, and activated sludge). Compound-specific

drinking water sources and in finished drinking water. A

parameters were consolidated in this review, with statistical

discussion on conventional and advanced drinking water

results showing biodegradability and hydrophobicity to be

treatment processes for micropollutant removal was also

the dominant drivers for removal. Jasper et al. (2013)

provided. Authors also proposed biological treatment and

assembled a review of TrOC removal in constructed

bioaugmentation as a potential targeted, cost-effective, and

wetlands with the effort to improve the design of the

sustainable alternative to existing processes while critically

wetland unit processes for the purpose.

examining technical limitations and scientific challenges

treatment

was

assembled

focusing

on

With respect to conventional drinking water

that need to be addressed prior to implementation.

treatment, an extensive study and report were issued by the

In the area of advanced treatment options, Feng

Water Research Foundation (2013) detailing actual

et al. (2013) reviewed the current state-of-knowledge on

performance of four full scale water treatment facilities in

the application of electrochemical advanced oxidation

New Jersey and the removal performance for 105

processes (AOPs) for the removal of widespread pollutants,

unregulated organic chemicals (UOC) found in raw water,

such

targeting chemicals with the potential to be endocrine

diclofenac,

disrupters. Additionally, the study characterized how

wastewater treatment plants (WWTPs) are not specifically

upstream inputs correlated with presence of pollutants in

designed to achieve complete removal of pharmaceuticals,

raw water. While a review of the 189 page report is beyond

electrochemical AOP has been proposed as a promising

the scope of this work, a few highlights stand out. Removal

technology

as

aspirin,

ibuprofen,

ketoprofen,

naproxen,

and

paracetamol.

Because

traditional

to

achieve

mineralization.

During


electrochemical advanced oxidation, for example, the

carbon adsorption – may be necessary to prevent the

degradation

release of trace levels of antibiotics into the environment.

of

analgesics

and

anti-inflammatory

compounds is obtained by the action of hydroxyl radicals

While physical and chemical processes were

via direct electrochemical anodic oxidation or indirectly

consistently rated as most promising in the review studies,

through Fenton’s reaction. Although largely evaluated

Ba et al. (2013) prepared a review of laccases (fungal

through

on

enzymes) in order to elucidate their catalytic mechanisms,

scalability of this technology to a greater industrial scale

immobilization techniques, and reactor design effects for

are desirable, as concluded by the authors of the review.

the

laboratory-scale

demonstrations,

studies

potential

applications

of

laccases

for

the

Other studies supported the assertion that

biotransformation of micropollutants in wastewater. Yang,

advanced technologies are necessary for treatment of

Hai, Nghiem, Price et al. (2013) also published a critical

emerging pollutants.

Boyjoo et al. (2013) conducted a

review for removal of TrOCs by white rot fungi.

literature review on greywater and found that advanced

Chemicals which are resistant to bacterial degradation

oxidation is the most promising current technology for

(including diclofenac, carbamazepine (CBZ), naproxen,

emerging pollutant treatment. Lofrano et al. (2013)

and 17α-ethynylestradiol) showed active removal by the

reviewed SOC treatment in industrial wastewater (tannery).

fungi. Three main classes of enzymes are secreted by these

The authors found that advanced oxidation and membrane

fungi:

filtration are the best treatment processes for the purpose.

peroxidases and laccase. Compounds with strong electron

Tijani et al. (2013) surveyed the existing literature on

donating groups such as hydroxyl or amines were

emerging pollutant treatment and determined that current

effectively biotransformed. Among compounds with strong

technologies, such as biological treatment, ozonation and

electron

activated carbon, were not designed to handle emerging

effectively treated. Whole cell presence was found to be

pollutants and are therefore not effective as singular

more effective for contaminant biotransformation than

processes. The authors recommend that the focus should

simple addition of enzymes.

be on AOPs in combination with other processes as the

enzymes was reported to be successful: decrease in

most promising technology.

Similarly, Michael et al.

nonylphenol (NP) and triclosan were observed using

(2013) reviewed the current knowledge base on the

laccase immobilized on silica beads. Most of the work

removal of antibiotics in conventional WWTPs and in

reviewed focused on pure culture tests and the authors

WWTPs with advanced treatment processes, and proposed

recommend more studies in continuous reactors, where it

that advanced treatments or their combinations – such as

was found that combinations of bacteria and fungi can

advanced oxidation, membrane filtration and activated

eventually limit the fungi performance as the bacteria

lignin

peroxidases,

withdrawing

groups,

manganese-dependent

triclosan

was

often

Some immobilization of

compete successfully for substrate.


Apart

from

reviews

of

actual

Enhanced Natural Systems

process

performance, a critical review of wastewater treatment models

was

conducted

to

evaluate

the

fate

This section describes natural processes that are

of

used to polish water treated in the engineered treatment

micropollutants in biological treatment processes (Pomies

works. The two most common types of enhanced natural

et al., 2012). The review provided insights into model

system treatment are subsurface treatment in-situ and

improvements including an inventory of experimental

engineered wetlands.

parameters,

In-situ and subsurface treatment. In-situ

comparison of model differences, and standardization of

biodegradation using aerobic co-metabolism of methane

calibration methodologies. Another study used the review

and benzene amended groundwater (in soil columns) was

of existing data to develop a statistically-based model for

shown to be a viable treatment for remediation of N-

removal of micropollutants in drinking water treatment

nitrosodimethylamine (NDMA) and a structural analog

(Sanches et al., 2013). Authors found that for membrane

(Weidhaas and DuPont, 2013).

methodologies

for

determining

model

rejection, the most influential parameters are alkalinity,

Burke et al. (2013) conducted a study on the

molecular size descriptors, molar volume, molecular weight

influence of aeration on the fate of wastewater derived

and its distribution coefficient. For adsorption, polar and

analgesics

electrostatic interactions were found to be more important

antimicrobial compounds from anoxic groundwater. Results

than hydrophobic interactions. Clouzot et al. (2013)

from the study showed that degradation of six phenazone

reviewed the current models developed to predict the

compounds was dependent on oxygen availability and

removal, attenuation and fate of organic and inorganic

compounds were efficiently treated under oxic conditions

micropollutants in wastewater treatment processes. The

only. The antimicrobials doxycycline and trimethoprim

review focused on the implications of these models in

were better removed during aeration, whereas a slightly

engineering design and operations, and recently on the

improved removal under anoxic conditions was observed

development of national and international regulatory

for

frameworks. Although, these predictive models can be used

demonstrating that their biodegradation is influenced by the

as benchmarking tools for comparing treatment processes

redox environment.

and

their

clindamycin,

residues

roxithromycin

Engineered wetlands.

capabilities towards the removal of specific pollutants, the

as

well

and

as

several

clarithromycin

Constructed wetlands

the

were evaluated for their ability to remove antibiotic

understanding of the ecotoxicological implications of

resistant genes (ARGs) that are introduced into the

pollutants discharges into receiving waters is still limited.

environment via treated municipal wastewater effluent. The

authors

concluded

that

their

application

for

systems were able to reduce the concentration of ARG, and the removal rate was affected by operational parameters, as


well as concentrations of nitrates, ammonia, and organic

blanket

reactor

versus

conventional

settling)

and

matter (Nolvak et al., 2013)

operational strategy (alternation of saturated/unsaturated

Hsieh et al. (2013) demonstrated that several

phases versus permanently saturated) on the removal of

phenolic endocrine disruptors including nonylphenol

various emerging pollutants in horizontal subsurface flow

diethoxylates,

and

constructed wetlands. Results showed that the occurrence

nonylphenol exhibited 55‒91% removal in freshwater

of higher redox potentials within the wetland bed promotes

constructed wetlands. Authors showed that removal was up

the elimination of conventional as well as emerging

to 30 times greater in freshwater systems when compared

pollutants, and that removal efficiencies were improved

to brackish or estuarine wetland systems.

under batch operations.

nonylphenol

monoethoxylate,

While biodegradation is one of the primary Biological Treatment Methods

mechanisms for removal of TrOCs in wetlands, photolysis can be also important and was studied by Jasper and Sedlak

While there are numerous advanced chemical and

(2013). In this study, a photolysis model was constructed

physical treatment methods that are employed to address

using steady state relationships for pollutant destruction by

emerging pollutants, conventional biological wastewater

carbonate and hydroxyl radicals to predict the required land

treatment processes are important and researchers have

area for removal of 90% of TrOCs including atenolol, CBZ,

continued to work to identify the treatment rates and

propranolol, and sulfamethoxazole (SMX). The authors

mechanisms for these systems.

concluded that for 90% removal in nitrified wastewater

Activated Sludge. The primary theme in

effluent, a land area of approximately 15 hectares is

activated sludge treatment studies was determining

required.

treatability of specific compounds either at bench- or Apart from chemical pollutants, fecal indicator

laboratory-scale, although research was also conducted at

bacteria and antibiotic resistance were studied at 7 pilot-

full-scale.

In one full-scale study, 8 micropollutants of

scale constructed wetlands and one urban WWTP treating

household origin were examined for the removal by

the same effluent. Constructed wetlands achieved greater

activated sludge. All micropollutants apart from sucralose

bacterial reductions compared to conventional activated

and PFOA were degraded or transformed by activated

sludge, although there was no significant difference

sludge (Pasquini et al., 2013). Fate and occurrence of 36

between levels of antibiotic resistant bacteria and the

emerging pollutants were investigated during primary and

treatments used (Sidrach-Cardona and Becares, 2013).

secondary treatment in a WWTP (Stasinakis et al., 2013).

Wetland configuration can also be of importance

Nine of the 36 compounds detected in influent were

for pollutant removal. Avila et al. (2013) evaluated the

removed by more than 70%; while the other compounds

influence of primary treatment (hydrolytic upflow sludge

were removed to a lesser degree or not at all, suggesting


advanced treatment processes should be included in order

in-situ data demonstrating that the expected hydrophobic

to remove the other pollutants of interest. Carvalho et al.

interaction and the modeled biological degradation from

(2013) evaluated activated sludge for the removal of

BIOWIN4 predicted removal of PPCPs from a secondary

veterinary pharmaceuticals enrofloxacin, tetracycline, and

treatment process. Additional research efforts focused on

ceftiofur from slaughterhouse wastewater in conventional

studying specific aspects of biological processes to improve

activated sludge laboratory batch reactors. Results showed

the modeling of pharmaceutical fate (Sathyamoorthy et al.,

that the major factor influencing the efficiency of pollutant

2013). A cometabolic process-based model was developed

removal was sorption to sludge and, to a smaller extent, to

to incorporate nitrification in order to improve biochemical

the organic matter present in the wastewater. The results

modeling processes for the accurate prediction of

highlighted the need to measure both the dissolved and the

pharmaceutical biodegradation in wastewater treatment.

adsorbed fraction of pharmaceuticals in the treatment

The new model may provide a good descriptor for

process. Yang, Wang and Tseng (2013) examined how an

pharmaceutical degradation in wastewater treatment due to

activated sludge mixed microbial culture could be used in a

its insensitivity to biokinetic parameters.

continuous stirred tank reactor to degrade methylamine

Some studies caution about generalizing between

(MA), a chemical used in a variety of industrial

synthetic wastewater and real wastewater for drawing

applications. The hydraulic retention time (HRT) for

research conclusions. Yang, Wang and Chen (2013) studied

complete removal of MA was measured under various

the removal of di-n-butyl phthalate from synthetic and

conditions including 600-1000 mg/L of MA, synthetic and

actual wastewater in a batch reactor using mixed microbial

actual wastewater, and batch conditions.

The optimum

cultures from activated sludge and soil from a rice paddy.

HRT was 1.16 days and the contribution of degradation

The di-n-butyl phthalate removal rates were approximately

products to change in pH was discussed.

4 times higher in the synthetic versus actual wastewater,

Some studies included the element of modeling

with the difference being attributed to lack of pH buffering

in evaluating the performance of activated sludge for PPCP

capacity in the actual wastewater.

removal. Blair et al. (2013) studied 54 PPCPs and

matrices di-n-butyl phthalate decreased by 91–100%. Some

hormones over six dates in raw influent, primary effluent,

researchers

However, in both

identified

the

dominant

secondary effluent, and final effluent of a full-scale plant.

pathways of removal for specific pollutants in activated

Results showed that the majority of the removal occurred

sludge: adsorption onto solids or biodegradation. For

across the secondary treatment process for the majority of

example, Samaras et al. (2013) identified nine emerging

the compounds. Secondary treatment removal rates were

pollutants

predicted by integrating BIOWIN4 into pseudo-first order

(ibuprofen, naproxen, diclofenac, ketoprophen, triclosan,

kinetics of PPCPs; predicted values were compared to the

BPA, and NP with two metabolites), and traced them

in

wastewater

activated

sludge

samples


through the wastewater treatment process. Nonylphenols

have been shown to be important. Gerrity et al., 2013

and triclosan showed dominant removal by adsorption to

studied the effects of SRT in a conventional full-scale

the sludge, and all other compound removal was driven by

activated sludge WWTP for removal of 33 emerging

biodegradation/biotransformation. Tang, Li et al. (2013)

pollutants. The authors observed that compounds that are

investigated the sorption and degradation of naproxen and

susceptible to biodegradation and/or sorption, such as

bezafibrate by activated sludge. Removal by sorption was

antibiotics and analgesics, are removed best at SRTs

higher for naproxen then bezafibrate, while the reverse was

ranging from 10 to 15 days. Removal of up to 100% was

true for degradation. There was no observed relationship

observed during the study for select compounds. However,

between COD removal and naproxen degradation that

other pollutants which do not exhibit susceptibility to these

could be used as a surrogate, suggesting an alternative

processes, such as recalcitrant compounds including

indicator is needed to determine the impact of natural

anticonvulsants and flame retardants, showed little removal

organic matter (NOM) on degradation of pharmaceuticals

in conventional biological treatment processes independent

by activated sludge. To elucidate the mechanism of the

of the SRT. Miller et al. (2013) also found that operational

biosorption pathway, Metivier et al. (2013) studied the

conditions, including longer SRT, significantly reduced

ability of extracellular polymeric substances (EPS) in both

ARGs. Yet another study showed that SRT is important for

their soluble (S-EPS) and bound (B-EPS) forms to bind to

biodegradable contaminants (Zeng et al., 2013).

acetaminophen and ethylsuccinate. S-EPS and B-EPS

removal of two estrogens (17β-estradiol [E2] and 17α-

presented the same affinities for each compound, both

ethinylestradiol [EE2]) was studied in an anaerobic-anoxic-

binding more easily to acetaminophen. Low ethylsuccinate

aerobic treatment. The authors found the optimal SRT that

adsorption documented in this study may explain the

achieved both contaminant degradation and nutrient

compounds relatively poor removal rates (50–80%) in

removal, and cautioned that some of the hormones

activated sludge. Sathyamoorthy, Ramsburg, et al. (2013)

partitioned into sludge, especially EE2. E2 was completely

utilized existing pharmaceutical (PhAC) sorption data in

removed from the water by anaerobic biodegradation with

order to create a predictive model for PhAC sorption. The

SRT having no significant effect. EE2 removal efficiency

study suggests separating PhAC modeling into the charge

was 65–81% by biodegradation and sorption combined, and

of the dominate species (negative or positive), depending

most of the sorption occurred in the anaerobic unit.

on the experimental pH, rather than relying on octanolwater

partitioning

coefficient

(KOW)

and

The

While most research on biological treatment

sorption

processes published in 2013 focused on mixed activated

distribution coefficient (KD) parameters alone.

sludge cultures, some studies identified the specific

Operational parameters of the activated sludge,

organisms participating in biodegradation of PPCPs. Zhou

such as solids retention time (SRT) and oxygen conditions

et al. (2013) reported bacterial isolates capable of


degrading PPCPs from 1 mg/L to 90%), compared to 5‒40% for the

anaerobic/oxic combination processes showed greater

activated sludge. The sludge however removed all four

removal efficacy. In general, more hydrophobic estrogen

compounds and fungi only removed SMX in the presence

containing compounds exhibited greater removal. Further,

of HBT mediator-enhanced laccase catalyst, and did not

increasing HRT and SRT also led to greater removal of

remove CBZ; authors discussed the mechanisms of the

hydrophobic compounds.

Nghiem,

Roddick

and

Price

(2013)

process

employed

at

the

WWTP

with

phenomena. Edwards et al. (2013) discussed the role of

In addition, the researchers showed interest in

biofilms on the bioremediation of persistent organic

comparing small decentralized system efficiencies to those

pollutants and PPCPs (e.g., biphenylol, p-chlorom-cresol,

of large centralized systems. Garcia, Clubbs et al. (2013)


compared the effluent concentrations of testosterone, E1,

were grafted with acrylic acid (AA) and N-vinyl-2-

E2 and EE2 to assess differences in endocrine activity

pyrrolidone (NVP). The pollutants investigated in this

between effluent from on-site (septic and decentralized)

study include 4-acetimiophenol, ofloxacin, ciprofloxacin,

and centralized municipal wastewater treatment systems.

tetracycline, chloramphenicol, propranolol, and diclofenac.

The effluent water quality results showed that, although on-

The authors demonstrated that the AA grafted membranes

site treatment provides an additional treatment of EDCs

were

through soil infiltration, its water quality was the lowest

ciprofloxacin, and propranolol and the degree of removal

among the alternative treatment options considered.

increased with the degree of AA grafting, up to 97%

effective

at

selectively

removing

ofloxacin,

removal of propranolol was achieved. For the NVP-grafted membranes increased removal was only observed with Physical Treatment Methods propranolol in comparison to the standard un-grafted PES Among advanced treatment processes, physical membranes. Removal of up to 82% was observed for removal is one of the most effective treatment tools propranolol at a lower degree of grafting, as the degree of available for addressing emerging pollutants. grafting increased with the NVP membranes the compound Membrane processes.

A number of research removal decreased. Functionalized membranes, using poly-

studies on membrane process applications focused on the vinylbenzyl-chloride with cyclic diamine piperazine, were membrane material. For example, Yuksel et al. (2013) used investigated for their ability to remove boron from natural six commercially available membranes to compare waters (Thakur et al., 2013). The functionalized membranes efficiency for removal of BPA at 50 mg/L. Polyamide based exhibited a maximal boron sorption of 28 mg/g at a neutral membranes exhibited good rejection (>98%) while pH, while being easy to prepare, robust and reusable, cellulose acetate (CA) membranes had low or variable demonstrating the potential application of these membranes rejection rates.

In another study, charged surface for boron removal from natural waters.

modifying

macromolecules

were

incorporated

into The material of the membrane is important for

modified CA nanofiltration (NF) membranes, and these rejection properties, and adsorption characteristics. The role modified membranes were tested against commercially of adsorption in the reverse osmosis (RO)-NF membranes available thin-film composite (TFC) membranes (Filmtec was studied by Dolar et al. (2013) using different filtration NF-270) for removal of emerging pollutants (Narbaitz et technologies

on

selected

glucocorticosteroids

and

al., 2013). The commercial TFC NF membrane showed anesthetics of different physical-chemical properties (e.g., better removals of CBZ, ibuprofen, and sulfamethazine in hydrophobicity,

water

solubility,

size,

etc.).

When

filter water effluents. Gong et al., 2013 analyzed the effect adsorption to membrane occurred for smaller and of UV-grafted polyether sulfonate (PES) membranes on hydrophobic molecules (e.g., procaine and lidocaine), the removal of select emerging pollutants. The membranes


release of this compound in permeates via diffusion

properties (e.g., active skin layer thickness). Membranes

become likely. Compounds with high dipole moments and

characterized by high mean free volume hole-radius or

poorly soluble in water showed higher likelihood to be

thicker skin layer showed higher rejection potential,

adsorbed onto membranes with larger pores.

particularly for high molecular volume compounds. The

Different types of membranes were compared in

removal of three pharmaceutically active compounds

several studies. Garcia, Moreno and al. (2013) studied the

(PhACs) was studied with a NF membrane using spiked

detectability and rejection of 22 micropollutants in a full-

surface waters from a drinking water treatment plant

scale microfiltration (MF)-RO system. Two parallel pilot

(Vergili, 2013). The bench scale study showed overall

operations using NF and RO were run independently to

rejections of 31‒39% for CBZ and 55‒61% for diclofenac

monitor the removal of two pharmaceutical compounds, NP

and ibuprofen. Moderate removals of PhACs coupled with

and ibuprofen, and resulted in a negligible role of

high organic matter removals, suggests NF as a possible

membrane selectivity on their rejection. With few

method for surface water treatment.

exceptions, the full-scale MF-RO system substantially

Other

membrane

process

improvements

removed the majority of the tested compounds (>75%), and

considered by researchers included application of an

in other cases concentrations were below detection.

electric field to the membrane or adding micelle forming

Differences in removal rates were observed from full-scale

surfactants to the process.

to pilot-scale system operations, with lower rejections in

evaluated electro-ultrafiltration (EUF) to separate 4-

the full-scale possibly due to the older age of the membrane

methylbenzylidene camphor (4-MBC) from water by

tested in the full-scale system. D’Haese et al. (2013)

applying an electric field across the membrane to remove

compared the rejection capacity of forward osmosis (FO),

this ultraviolet (UV) light filtering compound and minimize

NF and RO towards the removal of 20 different

fouling. The modification of polyvinylidene fluoride

pharmaceuticals. Modeling was conducted to determine the

(PVDF) membrane resulted in a rougher surface with

build-up of trace organics in the closed loop of a FO-RO

increased pore size which improved hydrophilicity in the

system and the result showed that high TOrC concentration

PVDF membrane; results of testing showed EUF could

develop in the draw solution of RO when compounds are

increase 4-MBC rejection and reduce filtration resistance.

transported through convection. Three RO membranes of

Exall et al. (2013) explored the improvement of

different mean free volume hole-radius and water

conventional ultrafiltration (UF) processes through micellar

permeability were tested in the study by Fujioka et al.

enhanced UF process, where the addiction of a cationic

(2013) to investigate the rejection of small solutes, such as

surfactant cetyltrimethylammonium bromide was shown to

boric acid and the disinfection byproduct NDMA as a

result in 3‒4 fold increase in membrane rejection of

function of their molecular dimension and membrane

sulfonamide antibiotics. The study also demonstrated that

Chen and Deng (2013)


the wastewater matrix plays a significant role in the

being the main factor in extraction efficiency, with the

removal of sulfonamide antibiotics, showing an increased

diluent 1-decanol having the longest lifetime of 150

rejection for increased solids content in wastewater and

minutes. While most of the studies focused on the removal

showing little to no effect in presence of DOM, due to poor interaction

between

DOM,

of organic pollutants, application of membranes for other

cetyltrimethylammonium

types of pollutants have received attention. Riquelme-

bromide micelles and the antibiotics. Among water quality parameters, NOM and

Breazeal et al. (2013) considered membranes for treatment

divalent cations have been studied for their effects on

of ARGs in WWTPs to prevent their release to receiving

membrane performance. Perfluorooctane sulfonate (PFOS)

environments. The removal of AGRs was shown to be

may be removed effectively from inlet water using NF in

successful with membranes ≤100 kDa with dependence on

the presence of calcium ions, as described by Zhao et al.

the corresponding protein, polysaccharide, and total organic

(2013). Rejection improved from 86% to 95% as pH was

carbon (TOC) colloidal fractions. Wongsawa et al. (2013)

increased from 3 to 9 with 0.1 mM Ca+2. Authors describe

presented both a design equation model and experimental

a bridging mechanism between the negatively charged

data for the removal/stripping of silver ions from

PFOS and the membrane with density functional theory

pharmaceutical wastewater by a hollow fiber supported

calculations to quantify this bridging mechanism.

liquid membrane, LIX-84-I. The model was validated by

In addition, several studies focused on the

predictions of concentrations of silver ions in the feed and

operational parameters. Chemical cleaning and temperature

stripping phases. Axial convection, axial diffusion, and

impacts on NF and its physicochemical properties, along

reactions

with its separation efficiency of inorganic salts and two

membrane-stripping interfaces were considered.

at

the

feed-liquid

membrane

and

liquid

PhACs (SMX and CBZ) were investigated (Simon et al.,

FO has been studied as a cost-effective

2013). Chemical cleaning at high temperatures resulted in a

alternative to RO technology. Researchers (Alturki et al.,

large increase in the rejection of the variables studied in

2013) investigated FO, pressure retarded osmosis (PRO),

their neutral form, while caustic cleaning at high

and RO in two commercial membranes with respect to

temperatures had no impact on the rejection of the variables

rejection of 40 compounds at pH 6. Five compounds were

studied. Sunsandee et al. (2013) examined a hollow-fiber

positively charged, 8 were negatively charged and the

supported liquid membrane (HFSLM) and its ability to

remaining 27 existed predominantly in their neutral forms.

recover (S)-amlodipine from pharmaceutical wastewater.

Results showed that in RO mode, electrostatic interactions

The HFSLM was tested under various chemical parameters

played a dominant role in governing the rejection of

(stripping

carrier

charged TrOCs; in FO and PRO modes, the rejection of

concentration), which revealed the polarity of the diluents

charged TrOCs was governed by electrostatic interaction

phase,

organic

diluent,

and


and size exclusion, while rejection of neutral compounds

Benzotriazole and 5-tolyltriazole at 30C, respectively.

was dominated by size exclusion, with rejection increasing

Jiang, Chang et al. (2013) investigated the removal of

with TrOC molecular weight. Further rejection of neutral

ciprofloxacin from aqueous solutions with bernessite, a

TrOCs in FO mode was higher than in RO mode. FO

manganese oxide. The results of the study showed uptake

transmembrane temperature changes and differences and

of

their effects on rejection of 12 TrOC was examined by Xie,

accumulation of the pollutant in natural systems. Globular

Ngheim, et al. (2013). The rejection of charged TrOCs was

organo-bentonite (GOB) was compared to powdered

higher than for neutral TrOCs (due to size and electrostatic

organo-bentonite (POB) for their abilities to remove 2-

repulsion effects), and temperature exerted only a small

naphthol during solid/liquid separation (Sun, Huang et al.,

influence on removal of these substances. A combination of

2013). GOB and POB had similar removal efficiency for 2-

low feed and high draw solution temperature produced

naphthol, but GOB was easily separated from the treated

significant enhancement in neutral TrOC rejection, notably

wastewater when compared to POB, which demonstrated

linuron and triclosan.

the potential of GOB compared to classical POB. Das et al.

ciprofloxacin

by bernessite

is

a

potential

for

Ion

(2013) performed a series of batch adsorption tests using a

Zeolites were some of the most commonly

modified palygorskite-based clay media MatCARETM to

studied mineral surface adsorption materials. Grieco and

investigate the removal of PFOS from wastewaters or its

Ramarao (2013) investigated the ability of select alumina-

fixation in contaminated soils. The natural clay exhibited

silica zeolites to adsorb tris-2-chloroethyl phosphate

faster adsorption kinetics and higher affinity to PFOS than

(TCEP) from aqueous solutions. The results demonstrated

activated carbon. X-ray diffraction (XRD) and Fourier

that a zeolite with high silica to aluminum ratio showed the

Transformed Infrared (FT-IR) spectroscopy showed that the

greatest adsorptive capabilities (103,000 microgram of

adsorption occurred at the surface level of the media

TCEP per gram of zeolite) in low pH (~pH 4.0) solutions.

through hydrophobic interactions between the long chains

However at typical environmental concentrations below

of PFOS and MatCARETM. Treatability studies using

100 micrograms per liter, adsorption of TECP was greater

MatCARETM showed its potential to exothermically fix

at a higher pH (pH ~10.0). Jiang, Yang and Yan et al.

PFOS in contaminated soils with retention capacity

(2013)

of

influenced by soil physical-chemical properties (e.g., pH,

benzotriazoles with a novel zeolitic adsorbent. The

organic content, etc.). Álvarez et al. (2013) researched the

adsorption of 1-H-Benzotriazole and 5-tolyltriazole showed

sorption characteristics of sepiolite Minclear SG36 as a

pseudo first order reaction kinetics in agreement with

low-cost alternative to traditional sorbent materials such as

Langmuir isotherm kinetics. Adsorption constants of 298.5

activated carbon, for removal of caffeine from aqueous

and 396.8 mg per gram were observed for 1-H-

solutions. Compared with activated carbon adsorbent,

Mineral Exchange.

Surface

demonstrated

the

Adsorption

adsorption

and

kinetics


sepiolite adsorbent, with small particle size and high

models. Strong-base polymeric anion exchange resins were

specific surface area, showed faster adsorption rate and

tested for their ability to remove diclofenac from both fresh

middle adsorption capacity for caffeine. The equilibrium

and ureolyzed synthetic urine (Landry, 2013). Diclofenac

adsorption capacity for caffeine by sepiolite was 20.0 mg/g,

removal was >90% for polystyrene resins, with the

and adsorption equilibrium could be reached in 10 days.

mechanism

of

removal

dominated

by

electrostatic

metallic

interactions between quaternary ammonium functional

adsorbents and resins. The ability of a metallic (zinc,

groups of resin and carboxylic acid of diclofenac and non-

copper, cobalt, and ferrite) based multi-phase adsorbent to

electrostatic interactions between resin matrix and benzene

remove select compounds including anionic (Congo red,

rings of diclofenac. The presence of competing ions (e.g.

and Orange G) and cationic (methylene blue and malachite

phosphate and citrate) did not significantly reduce

green) dyes was studied by Jacob et al. (2013). The study

diclofenac adsorption.

Other

materials

studied

included

showed rapid pseudo-first order kinetics of adsorption with

Carbon Adsorption. Carbon is still one of the

a rate constant ranging from 0.1 to 0.2 min-1. Huang and

most popular adsorbents for the treatment of emerging

Keller (2013) studied magnetic nanoparticle interactions

pollutants. SMX, caffeine, iopromide and CBZ were

with several emerging pollutants. The nanoparticles had a

studied for their removal by several types of activated

magnetite core and porous crystalline silica outer shell

carbon: powdered (PAC), and fluidized, coagulated and

filled with surfactant micelles. Relatively fast adsorption

flocculated activated carbons (FAC) (Piel et al., 2013). PAC

kinetics were observed for 2-chlorophenol, atenolol, D-

showed efficient removal of CBZ (80%), and FAC showing

gluconic,

l-3-(3,4-

consistent (80 to >95%) removal of all four compounds.

dihydroxyphenyl)alanine, methyl orange, succinic acid, and

Juan and Hoffman (2013) modeled the quantitative

SMX. Adsorption studies with methyl orange indicated that

structure activity relationship (QSAR) for 115 pollutants

almost all of the compound was removed from the water

published on the US Environmental Protection Agency

within 60 minutes, a time frame within the range of most

(EPA) Contaminant Candidate List 3. The results of the

water treatment processes. Grimmett (2013) showed that

model indicated that the majority of the compounds are

over 99% removal of sulfamethazine was observed with

treatable using activated carbon. Subsequent bench scale

three hyper cross-linked polystyrene resins, approximately

studies documented the adsorption of 17β-estradiol,

31% was observed with a fourth resin. Control tests were

ibuprofen,

conducted with glass beads and a copolymer resin which

diethoxalyate, azithromycin and tylosin with activated

showed no appreciable removal. The adsorption of

carbon in Lake Ontario water. In the bench scale tests,

sulfamethazine on a MN250 resin (the most efficient one of

breakthrough of the carbon column was only observed for

the four) compared favorably with the Langmuir isotherm

two pollutants, ibuprofen and SMX after approximately

ethylbenzene,

gemfibrozil,

diazinon,

SMX,

CBZ,

4-nonylphenol


110,000 bed volumes (consistent with 1 year of operation

was evaluated for removal of EDCs via molecular

in a conventional treatment plant). Results of bench studies

dynamics simulations and adsorption experiments (Boateng

confirmed predictions by the QSAR model.

et al., 2013). Binding free energies for adsorption of BPA

Nano-scale carbon materials have received a

and EE2 onto graphene, single-walled carbon nanotubes

great deal of interest from the research community. The

(SWNTs), and multi-walled carbon nanotubes (MWCNTs)

ability of graphene nanosheets and graphite oxide to

were computed. Computed results showed preferential

remove organic pollutants from aqueous solutions was

sorption of EE2 onto the CNMs compared to BPA and were

studied by Ji, Chen et al. (2013). The study showed three

consistent with experimental results in which higher

aromatic compounds (naphthalene, 2-naptshanol, and 1-

removal efficiencies were observed for EE2 compared to

napthylamine) and one pharmaceutical compound (tylosin)

BPA. Zhang, Fang et al. (2013) found that bisphenol AP

showed a high degree of affinity for both the grapheme

(BPAP) could be adsorbed onto MWCNT reversibly, and

nanosheets and graphite oxide nanotubes. Joseph et al.,

recharged using an ethanol/sodium hydrate solution. Ionic

2013 demonstrated the removal of estrogenic compounds

strength had no effect on adsorption and pH only led to

with carbon nanotubes and GAC adsorption. The study

lower adsorptions outside of the range of 4 to 10. A pseudo

investigated the removal of BPA and EE2 in seawater,

second order model mainly governed by external mass

synthetic landfill leachate, and natural river water. The

transfer fit experimental data the best. Zhang, Lv et al.

results of the study showed up to 90% removal of both

(2013) examined the removal of bisphenol AF (BPAF)

compounds with activated carbon adsorption. Coagulation

using adsorption onto MWCNT. The optimal pH range

with the carbon nanotubes showed minimal removal and

was 4.0 to 8.3. This adsorption was reversible by stripping

did not provide a synergistic effect at reducing the

with small amounts of ethanol.

pollutants when used in tandem with the GAC. Carbon

external mass transfer processes were involved in the

nanofibers are being investigated in a variety of

sorption process. Zhang, Pan et al. (2013) also examined

applications for water treatment currently, and Yang and

the removal of bisphenol F (BPF) from water using

Yen (2013) have described a novel process whereby

adsorption onto multiwall carbon nanotubes MWCNT.

alumina-based

on

a

Removal efficiencies were >90%, with a wide range of

into

an

effective pH (4‒10) and no effect was observed by

electrocoagulation and electrofiltration unit and then tested

variations in either ionic strength or major cation/anion

for both adsorption and removal efficiencies for caffeine,

presence. Regeneration was achieved using 10 mL

acetaminophen and SMX. Caffeine and SMX were

ethanol/1.0 M sodium hydrate solution (7:3 v/v). Removals

removed at ~95%, but acetaminophen removal was only

of EDCs in water by graphene-based composites with γ-

~80%. The adsorptive capacity of carbon nanomaterials

Fe2O3 nanoparticles were investigated (Sinha and Jana,

polyvinylchloride

carbon film

nanofibers were

grown

Both intra-particle and

incorporated


2013). The removal capacities of these graphene based

illustrating the mixture of fly ash and soil could be used as

compounds, were 360 and 680 mg/g for BPA and 1-

an adsorbent material for removing CBZ from water.

naphthol, showing substantial removal efficiencies of the

Crespo-Alonso et al. (2013) used the Langmuir

compounds studied.

isotherm model to evaluate adsorption properties of cork

In general the process of adsorption also had an

for the removal of fluoroquinolone ofloxacin, a widely used

effect on the occurrence, fate and level of mobilization of

antibiotic. The sorbing performance of cork was found to

seven selected PPCPs (e.g., ibuprofen, diclofenac, CBZ,

be independent of the particle size, and experimental pH

etc.) in a sewer catchment during dry and wet weather

seemed to have influenced the type of interactions between

conditions (Del Rio et al., 2013). The result of the field

sorbent and sorbate. The study showed that at different pH

campaign revealed the adsorption of these compounds in

protonated species and moieties of ofloxacin interacted

biofilms formed in the collector and in sediments and their

differently with the solid surface of cork.

subsequent release and mobilization through wet weather

Chitosans cross-linked with glutaraldehyde and

flows. Mobilization only occurred for compounds that are

grafted

typically removed through adsorption to solids in WWTPs,

carboxybenzyl) (CsNCB) were tested alongside non-

and excluded others, such as caffeine, that typically

modified chitosan (Cs) for their ability to adsorb

undergo degradation in secondary treatment.

pramipexole dihydrochloride (Kyzas, 2013). Tests showed

Alternative

Adsorbents.

with

either

sulfonate

(CsSLF)

or

N(-2-

Sanchez-Martin,

that CsSLF adsorbed pramipexole dihydrochloride most

Beltran-Heredia, Delgado-Regana et al. (2013) synthesized

efficiently, followed by CsNCB and Cs. Researchers

laboratory scale tannin rigid foams for emerging pollutant

proposed modified chitosan as promising, environmentally

(methylene blue, polyoxyethylene sodium lauryl ether

friendly adsorbents for use in pharmaceutical wastewater

sulfate, and trimethoprim) treatment by adsorption.

treatment. Nanofiber mats made of chitosan or cellulose

Adsorption behavior could be predicted by existing kinetic

were tested for adsorption of five trace toxic metals from

and equilibrium models; and adsorption capacities were

water (Musyoka et al., 2013). Both materials were able to

comparable to commercial adsorbents.

remove metals from river and treated water, though

Fly ash was also considered as an alternative

chitosan out-performed the cellulose.

adsorbent and fly ash-amended soil was investigated for its

Molecularly imprinted silica sorbents were

ability to remove CBZ from an aqueous solution

fabricated via an acid-catalyzed sol-gel process in the

(Swarcewicz et al., 2013). Results demonstrated a mean

presence of a templating pollutant (Morais et al., 2013).

removal of 92.8% with a soil mixture containing 30% fly

Silica with molecular cavities imprinted by chemical

ash, while soil alone had only a 33% removal of CBZ,

pollutants displayed adsorption capacities of 55‒65% when


The

used in potable and ground water, while non-imprinted silica had adsorption capacities of only 15‒20%.

ability

to

remove

an

anti-estrogenic

compound (Tamoxifen) from secondary WWTP effluents

Coagulation. The majority of the studies focused

using coagulation was investigated. Removal of the

on selecting the right coagulant and the best dose for the

compound by FeCl3 (36%) and polyaluminium chloride

purpose. Two coagulants, aluminum sulfate and pre-

(20%) were limited even as coagulant dose increased,

hydroxylyzed polyaluminum chloride (PAX-XL1, PAX-XL

suggesting anti-estrogenic fractions are difficult to remove

19), were added to contaminated water for the removal of

through coagulation (Tang, Wu, et al., 2013).

several types of PCBs and heavy metals. PAX-XL 19

Comparison of Physical Processes.

Khalaf et

showed the most removal, with the total PCB concentration

al. (2013) studied the removal of mefenamic acid with RO,

being reduced by 71%, and an 86% reduction in lead

activated charcoal and a micelle clay complex. The results

concentration (Rosinska and Dabrowska, 2013). Parmar

indicate that in wastewater spiked with the compound,

and Upadhyay (2013) utilized various doses of coagulants

activated carbon proved more effective at removing the

FeCl3, AlCl3, and FeSO4 in combination in order to

pollutant with a 97.2% removal. The Langmuir adsorption

optimize the removal of pharmaceuticals in wastewater,

capacity of activated carbon was 90.9 mg/g while the

and found that the optimal dosing of each coagulant was

micelle-clay complex exhibited a capacity of 100.0 mg/g,

dependent on the wastewater and pH.

or slightly higher than activated carbon.

The impacts of water quality on coagulation Chemical Treatment Methods

performance with respect to removal of emerging pollutants were also investigated. Diemert and Andrews

Chemical treatment methods can be used to

(2013) investigated the effectiveness of coagulation via

transform pollutant molecules rather than physically

bench-scale alum treatment for the removal of a number of

remove them; there are a number of chemical oxidants that

pharmaceutically active and EDCs from three surface

were studied in 2013.

waters in Canada. Removal mechanisms varied depending

Ozone. Ozonation of excess wastewater sludge

on the target molecule, water chemistry and on the

for the treatment of EDCs [E1, E2, estriol (E3), EE2, BPA)

complexes that these molecules established with NOM in

and NP] was investigated with results showing effective

water matrixes. In a similar experiment with alum

removal of these EDCs in ozonated activated sludge

coagulation a following study by Diemert et al. (2013)

(Qiang, Nie et al., 2013). Proper ozone dosing, the addition

looked into the role of NOM on halo-benzoquinones

of H2O2, and a possible pH adjustment were listed as

removal from the same waters and showed increased

important factors for efficient removal. SMX and EE2 were

removal efficiencies by increasing the coagulant dose.

subjected to ozonation at lower doses than generally used to treat wastewater to test whether biological treatment


would respond to match or enhance total degradation

(HO•), and HO• exposure. Reaction rate constants were also

(Larcher and Yargeau, 2013). Experimental results testing

reported for 16 common micropollutants. Hubner, Keller

ozonation as a pre-treatment to biological treatment

and Jekel (2013) showed that in a pilot-scale ozone reactor

indicated that pre-treatment enhanced the SMX removal,

the destruction of TrOCs in WWTP secondary effluent can

but decreased the EE2 removal. This variability suggests

be

that the potential for ozone pretreatment is compound-

concentration of a tracer compound. However prediction of

dependent. Other studies also demonstrated the potential

TrOC removal by direct reaction with ozone was not

for combining ozonation with biological treatment. The

feasible. The authors determined that the reaction of ozone

biodegradation of ozonation by-products of CBZ in soil

with these compounds was largely limited by mass transfer

columns was investigated by Hubner, Seiwert et al. (2013).

efficiency highlighting the importance of considering

The authors demonstrated that after ozonation of secondary

reactor design and geometry when studying compound

wastewater effluent containing 10 micrograms per liter of

destruction with ozone. Yong and Lin (2013) have

CBZ, approximately 50% of the compound converted into

developed an explicit method to determine simultaneous

a primary by-product known as BQM. Subsequent soil

rate constants for initiation, promotion and inhibition in

column tests showed this compound to be more

ozonation of NOM as it influenced the degradation of

biodegradable than CBZ itself however other by-product

ibuprofen. The model was validated using a model initiator

compounds showed no appreciable removal after 5 to 6

(hydroxide ion), model promoter (methanol) and model

days of residence time in the sand column.

inhibitor (acetate).

Other

considerations

for

ozone

predicted

by

measuring

the

relative

residual

applications

Identification of the products and determining their

included pricing and modeling the process. Shadow prices

toxicity is always an important consideration with chemical

of treating wastewater for five pharmeceuticals and

processes including ozonation.

personal care products using ozonation were estimated

(2013) detailed the effects of oxidation with ozone and

(Molinos-Senante et al., 2013). All estimated shadow prices

hydroxyl radicals on the destruction of the antibiotic

were negative, indicating that the environmental benefit of

levofloxacin. The kinetic results of these experiments

treating wastewater with these pollutants outweighs the

indicate that the destruction of levofloxacin with ozone

treatment costs. Lee, Gerrity et al. (2013) developed a

exhibits a second order decay constant of 6.0×10-4 M-1s-1 at

predictive, mechanistic model to describe the removal of

a pH of 7.2 and a temperature of 20 °C. The rate constant

micropollutants by ozonation.

Model inputs included

for destruction with hydroxyl radicals at pH 6.0 and 7.2

ozone dose normalized to the dissolved organic carbon

were 4.5×109 M-1s-1 and 5.2×109 M-1s-1, respectively. Four

(DOC) concentration, rate constants for the reaction of the

treatment by-products were identified for the reaction of

given micropollutant with ozone and hydroxyl radicals

levofloxacin with ozone. Toxicity of these constituents was

Hamdi El Najjar et al.


analyzed by inhibition of luminescence of the bacteria V.

also measured removal efficiencies of these EDCs which

fisheri and indicated that the intermediate compounds are

varied from 20 to 70%, depending on flow conditions at an

potentially more toxic than the levofloxacin. Barritaud et al.

ozone dose of 0.5 g O3 per g TOC. Biological tests showed

(2013) tested a methodology to identify the potential by-

that the oxidation stage did not significantly reduce the

products of emerging chemical pollutants generated during

estrogenicity of the effluent and revealed the presence

ozonation by testing river water samples spiked with

and/or formation of genotoxic compounds showing that

estrone sulfate.

Four main treatment by products were

poor performances recorded in this study could be

found by chromatography. Estrogen receptor-mediated

attributed to the presence of a significant industrial

chemical activated luciferase gene expression bioassays

component in the influent wastewater.

were performed to measure the estrogenic potency of

Ozone and ozone/H2O2 were studied at different

samples before and after treatment. Results of this study,

concentrations for their ability to degrade bezafibrate and

which were also reported by Bourgin, Gervais et al. (2013),

CBZ, along with characterizing the transformation products

showed that degradation of the parent compound (>80%)

(TPs) formed. CBZ was completely oxidized under both

occurred in 10 minutes. A non-targeted chemical profiling

conditions and had TPs for ozone only, while low levels or

approach derived from metabolomic profiling studies

non-detects for ozone/H2O2 were observed. Bezafibrate

revealed 11 ozonation by-products, among which 4 were

was oxidized by both (>89%) and had TPs for ozone and

predominant. While the results confirmed that ozonation

low levels or non-detects for ozone/H2O2, suggesting that

showed formation of by products, the by-products had

while ozone is great at degrading the parent compound,

significantly lower estrogenic activity. The performance of

hydroxyl radicals are still important in the transformation

a full-scale ozonation plant was investigated in order to

of TPs (Tootchi et al., 2013).

assess the removal efficiency of four target EDCs:

Antoniou et al. (2013) investigated the ozone

nonylphenol, nonylphenol monoethoxylate, nonylphenol

dosage required to remove PhACs from biologically treated

diethoxylate and BPA (Bertanza, Papa, Pedrazzani, Repice

wastewater of varying quality, originated from different

and Dal Grande, 2013). Researchers evaluated tertiary

raw wastewater and wastewater treatment processes. Test

effluent from a municipal WWTP which receives an

waters were spiked with 42 PhACs and treated with

industrial (textile) load. Results of the study showed that

different ozone doses (0.5–12.0 mg/L) in bench-scale

measured removal efficiency was lower than what could be

experiments. Fifteen of the 42 investigated PhACs could be

predicted based on literature data, because of the relatively

classified as easily degradable, while 19 were moderately

high residual content of biorefractory compounds still

degradable, and 8 were recalcitrant towards ozone

present after biological treatment. In a companion paper,

treatment. The ozone dose for 90% degradation can be

Bertanza, Papa, Pedrazzani, Repice, Mazzoleni et al. (2013)


predicted based on the target pharmaceutical and the DOC

precursors during chloramination and chlorination of

of the wastewater to be treated.

wastewaters as a function of the initial water chemistry

Chlorination, bromination and chloramination.

(e.g., dissolved organic nitrogen, DOC and bromide).

Chlorination was questioned as a potential treatment

During speciation dichloroacetamide was the most common

technology for the EDCs BPA, triclosan, and NP from

HAcAm detected during chlorination or chloramination

secondary wastewater effluent, and was not found to be

whereas bromochloroacetamide was the most abundant

completely effective (Noutsopoulos et al., 2013). NP, BPA,

species among the six bromine-containing HAcAms. Shen

and triclosan were effectively removed (60‒84%) at

and Andrews (2013b) studied the impact of pre-

moderate chlorine doses, however, ethoxylates of NP

chlorination and water matrix upon the formation of

(NP1EO and NP2EO) showed removal efficiencies of

NDMA from amine-based pharmaceuticals. In deionized

chlorophene > nortriptyline HCl >

from oxidation of aromatic double bonds. Zhang, Sun et al.

benzotriazole > DEET. Reaction rate constants for

(2013) studied how permanganate can be utilized to oxidize

bromination of the compounds ranked in the same

BPA and compared results to the existing literature on BPA

sequence. The efficiency of chlorination for the degradation

fate in other oxidative processes. The reaction rates were

of these compounds when present in surface water from a

second order (28.53 M-1s-1), the same as photo-catalytic

public reservoir, and two effluents from municipal WWTPs

degradation of BPA, though ferrate oxidation was an order

showed chlorination degraded some of the compounds but

of magnitude greater. The advantage of the process was

was not effective for all, especially benzotriazole and

selectivity of permanganate for BPA in a complex matrix,

DEET. Also, chlorination in the presence of bromide

while other oxidants can be non-selective and can suffer

revealed that low bromide concentrations enhanced slightly

from reduced efficiency in some samples. BPA removal

the reaction of the selected compounds during chlorine

was highly pH and temperature dependent, but co-existing

oxidation. Pape et al. (2013) found that the antimicrobial

solutes had no negative effects on BPA degradation.

with

compounds

were

ranked

as

triclosan transformed quickly in wastewater treatment

Photolysis. The studies in photolysis focused on

chlorination when tested in the absence of full matrices, but

two main aspects of the process: kinetics and quantum

found inconsistencies when tested in a natural water matrix,

yields, and transformation products. Ji, Zhou et al. (2013)

demonstrating

investigated

the

importance

of

influent

matrix

composition on triclosan chlorination transformation.

the

photochemcial

destruction

of

2-

phenylbenzimidazole-5-sulfonic acid, an agent present in sunscreen, by high pressure mercury vapor lamp and laser

Chlorination effects upon microbial antibiotic using

flash photolysis. In this study a quantum yield of 2.7 × 10-4

metagenomics. Results suggested that chlorination in

was reported at a pH of 6.8 in buffer solution. The results

drinking water could concentrate various ARG, as well as

of the study indicate that the principal means of destruction

plasmids, insertion sequences, and integrons, illustrating a

of the pollutant is by direct photolysis. Indirect photolysis

potential public health concern (Shi et al., 2013).

only plays a role when direct photolysis is inhibited by

resistance

were

studied

in

drinking

water,


photosensitizers such as nitrate. De Laurentiis et al. (2013)

photodegradation rates and the relative distribution of the

studied the effect of UV photolysis on benzophenone-4,

major reaction intermediates. Salgado et al. (2013)

commonly present in freshwater and seawater environment

investigated the use of medium pressure direct UV

from direct wastewater discharge or release during

photolysis on the degradation of three pharmaceuticals

sunbathing. The two deprotonated forms of benzophenone-

(ketoprofen, diclofenac, atenolol) in both laboratory grade

4, HA- and A2-, present different degradation kinetics when

water and wastewater, in order to provide insight into

exposed to direct photolysis, with the latter generally faster

wastewater discharge products when UV photolysis is

than the former. The opposite occurs for low levels of

employed. Photodegradation kinetics were followed with

DOM in the water matrix, due to the faster reaction of HA-

ketoprofen > diclofenac > atenolol, and the associated

with hydroxyl radicals. Presence of bromide and DOC in

byproducts were identified for all three compounds.

seawater environment plays a significant role in the

Apart from emerging chemical pollutants, UV was

reactivity of benzophenone-4 during photolysis. Four

also evaluated for emerging biological pollutants such as

halobenzoquinones, a class of emerging disinfection by-

antibiotic resistant bacteria. Guo et al. (2013a) elucidated

product, showed as much as 90% degradation by UV

the dose-response curves at the bench scale for nine

irradiation in both pure and tap water, and several major

antibiotic resistance strains of bacteria with ultra-violet

byproducts were identified (Qian et al., 2013). Keen et al.

(UV) disinfection. Strains of bacteria that were investigated

(2013) studied the photodegradation of diclofenac under

identified in the treatment plant included strains resistant to

UV and found that quantum yield of photolysis was

cephalexin,

independent of wavelength, and that one of the products of

vancomycin,

photolysis is a dimer of the parent molecule. Because the

chloramphenicol, and a strain resistant to both tetracycline

dimers were found only in pure water and not in

and erythromycin. The results of the study showed that

wastewater, the authors postulated that incorporation into

strains

the background organic matter may be a reaction pathway

erythromycin required a UV fluence of 50 mJ/cm2 for a 4-

for this pollutant.

log inactivation, a 2-log inactivation was achieved at a

In addition, dissolved oxygen and

ciprofloxacin,

erythromycin,

gentamicin,

rifampicin,

tetracycline,

sulfadiazine,

resistant

to

sulfadiazine,

vancomycin,

and

be

fluence of approximately 10 mJ/cm2. All other species

instrumental for the dimer formation. Another study also

required a UV fluence between 10 and 20 mJ/cm2 for a 4-

found that oxygen can affect photodegradation of some

log reduction. The authors indicated that UV treatment

compounds (Marotta et al., 2013). The photodegradation of

showed a potential for selectivity for certain strains,

aqueous solution of naproxen and its photo-products were

including those resistant to gentamicin, vanomycin,

studied under aerated and deaerated conditions. Results

rifampicin,

showed a significant influence of dissolved oxygen on

proportions of these strains in comparison to the others

intermediate epoxide formation

was shown

to

tetracycline,

and

ciprofloxacin

as


the

increased after UV treatment. In a subsequent article, Guo

in a reaction with hydroxyl radicals. Based on that, and

et al. (2013b) detailed the same effect for tetracycline and

other criteria, authors proposed using sucralose as a

erythromycin resistant bacteria. After 1-log of bacterial

performance indicator for AOP reactors for treatment of

counts reduction, the proportion of tetracycline resistant

emerging pollutants. Benitez et al. (2013a; 2013b; 2013c)

bacteria increased in proportion to that of erythromycin

performed photodegradation experiments by UV radiation

resistant bacteria.

alone, UV/H2O2 and Fenton’s reagent system on five

effects

of

Huang et al. (2013) documented the

physical

and

chemical

disinfectants

on

emerging

pollutants

(1-H-benzotriazole,

DEET,

tetracycline-resistant E. coli. The bacteria showed no

chlorophene, 3-methylindole, and nortriptyline HCI),

increased resistance to UV irradiation compared to non-

frequently found in surface waters and wastewaters. The

tetracycline resistant strains of E. coli. However, the

researchers determined quantum yields and rate constants

authors showed that after 4.3-log inactivation with chlorine

for the radical reaction between each compound and

exposure, tetracycline-resistant strains were more prevalent

hydroxyl

than non-tetracycline resistant bacteria indicating selection

photodegradation of mixtures of the selected compounds in

of these bacteria in the disinfection process.

several water matrices were conducted. A model was

radicals

(Benitez

2013b).

Simultaneous

While UV photolysis was most commonly studied,

proposed for the elimination of these compounds and

some researchers explored solar photodegradation of

compared to experimental results confirming its viability to

pollutants. Babic´ et al. (2013) studied the photolytic

predict the elimination of these compounds in various

degradation of norfloxacin, enrofloxacin and ciprofloxacin,

waters (Benitez et al., 2013b). In addition, transformation

fluoroquinolone antibacterials widely used in human and

products were identified, and the authors reported that

veterinary medicine under simulated solar irradiation in

some of the early intermediates showed higher toxicity

different

that

using a Microtox test (Benitez et al., 2013c). A variety of

and

AOPs were applied to the same five compounds in public

photodegradation followed pseudo first order kinetics;

reservoir water and two secondary effluents from municipal

researchers also identified the degradation pathways. The

wastewater plants by the same group of researchers

slowest photodegradation rate was observed in river water

(Benitez et al., 2013a) to evaluate the costs of each

for all three fluoroquinolones.

process. In general, combined oxidation processes, like

water

fluoroquinolones

matrices. degrade

The results showed very

quickly

Advanced Oxidation Processes. Because UV is

UV/TiO2, O3/H2O2 and photo-Fenton systems, resulted in

commonly as a component of advanced oxidation, multiple

greater contaminant removal than single oxidant processes.

studies compared UV with UV/H2O2 for transformation of

Researchers noted that the electrical energy required for

a variety of compounds. Keen and Linden (2013b) showed

operating UV lamps can be significant, and found

that sucralose is stable under UV to 200 nm, but degrades

traditional Fenton’s reagent to have the lowest cost of


materials and energy (Benitez et al., 2013c). Direct

90%, although high H2O2 doses were required due to bulk

iron was found not to improve removal rates and

organic and inorganic carbon in the wastewater (Schulze-

efficiencies due to increased reduction of UV transmittance

Hennings and Pinnekamp, 2013). Forty pharmaceuticals

and limited presence of dissolved iron due to Fe(III)

were compared in terms of degradation rate under

precipitation at pH of 6‒7. In another study by Keen and

UV/H2O2 treatment by Wols et al. (2013). Three different

Linden (2013a), the effectiveness of both UV and UV/H2O2

water sources and two different UV lamps were used. Most

was examined for degradation of antibacterial activity of

of

antibiotics. Representatives of 6 different antibiotic classes

monochromatic LP lamp regardless of water source. For a

were used with low pressure and medium pressure mercury

polychromatic medium pressure (MP) lamp, photolysis was

lamps, and the treatment was studied in both pure water

improved for some pharmaceuticals depending on the water

and

matrix. Degradation kinetics for several pharmaceuticals

wastewater

transformed

effluent.

Both

UV

and

UV-AOP

compounds

degraded

slowly

under

the

no

was not previously reported, including metformine,

antibiotic.

paroxetine, pindolol, sotalol and venlafaxine. In oxidation

Erythromycin formed antibacterial products at UV fluence

processes influent constituents can affect the rate at which

antibacterial

the antibiotics into products with

the

activity

for

all

but

one


acid pharmaceuticals are degraded. Yuan et al. (2013) have

compounds tested (e.g., CBZ, diclofenac, metoprolol,

investigated the effects of humic acids in influent water for

SMX, etc.) and that degradation efficiencies and rates of

UV/H2O2 treatment of six pharmaceuticals. Humic acid at

UV and UV/H2O2 treatment are increased with lower flow

1, 5 and 10 mg/L inhibited the degradation rate

rates and addition of H2O2, respectively.

significantly. The presence of several anions including Cl-,

Fenton and photo-Fenton processes are among

NO3-, and HCO3- were also shown to inhibit the reactor

other popular AOPs. Klamerth et al. (2013) investigated

efficiency of pharmaceutical degradation. Authors discuss a

the destruction of emerging pollutants (total concentration

number of other variables including temperature, H2O2

240 ng/L) in wastewater effluent using a solar photo-

concentration, pH and lab versus natural waters.

Fenton and modified photo-Fenton process. Over 95%

Several AOP studies evaluated and compared

removal of all compounds was achieved. The photo-Fenton

alternatives for generating hydroxyl radicals. Pablos et al.

process at pH 3 was more effective than the modified

(2013) explored various photochemical AOPs (UV-C/H2O2,

photo-Fenton process which was conducted at neutral pH.

UV-A/TiO2,

simultaneous

Photodegradation of a recalcitrant endocrine disruptor, 4-

removal of pharmaceuticals and inactivation of bacteria.

tert octylphenol or as promoted by Fe (III) was reported by

Pharmaceuticals were only fully eliminated using UV-

Wu et al. (2013). Complete degradation after 45 minutes at

A/TiO2, but a longer irradiation time was necessary to

365 nm was noted. 2-propanol was an effective inhibitor (a

achieve bacterial inactivation. UV/Cl2 and UV/H2O2 AOPs

mechanism was discussed).

UV-A/TiO2/H2O2)

for

the

were considered for the removal of emerging pollutants and

Some of the less common types of AOP were

taste and odor compounds in a drinking water facility, with

evaluated as well. Oncu and Balcioglu et al. (2013b)

chlorine-based AOPs showing an economic advantage, and

evaluated microwave-assisted hydrogen peroxide treatment

a reduction of MIB ranging between 45 and 90%

and microwave-assisted persulfate treatment of biological

depending on pH (Rosenfeldt et al., 2013). Potential

sludge and compared treatment methods in terms of

advantages of UV/Cl2 include minimal disinfection by-

simultaneous

product formation as a result of chlorination, performance

solubilization. Although both methods yielded nearly

at low oxidant doses, improved efficiency (site specific),

complete antibiotic degradation, the microwave-assisted

and no residual quenching. In the study by Eyser et al.

persulfate was found to be efficient at a lower temperature

(2013), oxidation of PPCPs using advanced oxidation

and oxidant dose. Additionally, it also provided more

treatment with ozone, UV and UV/H2O2 was investigated

overall metal solubilization, twofold higher improvement in

and

transformation

dewaterability, and the oxidation of solubilized ammonia to

intermediates evaluated. The results showed that ozone

nitrate occurred in a shorter treatment period. Although

alone achieves high removal efficiency (>84%) of the

most of the AOP rely on chemical addition for generation

the

formation

and

toxicity

of

antibiotic

degradation

and

sludge


of hydroxyl radicals, some of the background contituents

fluorescent lamp. In addition, the nanocomposite rods were

can do so as well. Effluent organic matter (EfOM) acts as a

easily recovered and removed due to their long axial

photosensitizer by producing reactive oxygen species,

dimensions (Lam, 2013a). Lam et al. (2013b) also

which in turn oxidize recalcitrant organic compounds. The

synthesized nano-scaled tungsten oxide (WO3) coated

study by Lee, Glover and Rosario-Ortiz (2013) reveals that

evenly on ZnO nanorods (ZNRs) to create robust WO3-

photoproduction

HO•

of

is

a

function

of

ZNR nanocomposites with a red-shifted adsorption

the

physicochemical properties of EfOM, including molecular

spectrum.

These

nanocomposites

showed

superior

size and hydrophobicity.

photocatalytic activity in the degradation of resorcinol over

Activity of the transformation products was also

pure ZNRs, as well as successful degradation of other

the focus of the study by Yu et al. (2013). The authors have

endocrine disrupting chemicals. Leshuk et al. (2013)

studied the degradation mechanisms for diclofenac reacting

synthesized

with hydroxyl radical and solvated electron. Rate constants

paramagnetic γ-Fe2O3@SiO2@TiO2 colloidal nanospheres

were reported at 9.29×109 and 1.53×109 M-1s-1 respectively.

with mesophorous TiO2 shells for use in photocatalysis for

Toxicity studies were also reported using V. fischeri

water

bioluminescent species. The advanced reduction process

photcatalytic activities to high-activity, mixed-phase titania

was found to remove toxicity more effectively.

photocatalyst (e.g. P25 TiO2, Degussa), but were recyclable

and

purification.

characterized

These

core-shell,

nanospheres

had

super-

similar

Catalysis. Many studies focused on testing novel

via magnetic recovery. Baumgartner et al. (2013) evaluated

catalysts for treatment of emerging pollutants. Xin et al.

a catalytic system with Rh/Al2O3 and H2 and found this

(2013) described a combination of water-surface discharge

system to be capable of efficiently degrading a wide range

plasma

of

of halogenated benzenes at ambient temperature and

microcystine-LR (MC-LR), a toxin from cyanobacterial

pressure. Results of this work showed slower degradation

blooms. The optimal reported removal rate was 90.2%

with increasing number of fluorine substituents and

versus 75.3% without xerogel addition.

An oxidation-

increasing degradation rates with increasing number of

adsorption kinetic model was used to analyze the system

adjacent fluorine substituents. The observed fluorinated

and indicated that catalytic oxidation was dominant in

intermediates indicated that adjacent fluorine substituents

determining rate. ZnO nanorods coated evenly with

are preferably removed. Chalasani and Vasudevan (2013)

nanoscale

ZNR-Bi2O3

evaluated water-dispersible, photocatalytic Fe3O4@TiO2

nanocomposites showed high charge-separation efficiency,

core shell magnetic nanoparticles for their ability to capture

high hydroxyl radical generation ability, and higher

and photocatalytically destroy BPA and dibutyl phthalate in

photocatalytic activities in the degradation of phenol and

water. The specially prepared nanomaterial showed that

methylparaben than pure ZnO nanorods under a compact

high removal rates could be achieved and the catalyst can

with

a

Bi2O3

xerogel

catalyst

particles

to

for

make

oxidation


be magnetically separated from the dispersion after reaction

effluent from a hybrid biological concentrator reactor.

and reused with little or no loss of catalytic activity. Chi et

Results revealed differences in removal rates depending

al. (2013) used a modified polyacrylonitrile catalyst and

upon the technique used for synthesis of the composite

dosed effluent from a conventional WWTP with hydrogen

TiO2-based catalyst. Buda and Czech (2013) evaluated

peroxide in a heterogeneous Fenton’s process to remove

mesoporous C- and C,N-codoped TiO2 in the removal of

EDCs and PPCPs. The treatment system was effective at

diclofenac from water. Results showed that the synthesized

ambient temperature and at the natural pH of the

catalysts were effective for degrading diclofenac and

wastewater. Estrogenic potency was removed by 82.77%,

enabled reduction of the COD value of the wastewater by at

91.36%, and 96.13% from three different WWTPs with

least 60%. The process of catalyst production had an

furnace dust was insolubilized by a solution of highly

ozonation > solar heterogeneous photocatalysis with TiO2.

enriched bacteria within 168 hours of culture.

Similar conclusion was drawn in another study. The

pesticides,

polychlorinated

technology

effectiveness

that

eliminates

Comparison of Chemical Processes. Several

removal of 11 pharmaceuticals in RO brine by ozonation

studies focused on comparing different processes, and the

and UV/H2O2 oxidation was studied by Justo et al., 2013.

process with the highest promise was not consistent from

In general, due to the resistance to oxidation by ozone of

one study to another and depended on the properties of the

several chemicals including atenolol and CBZ, UV/H2O2

target

Beltran-

proved to be a more efficient technology as effective

Heredia and Domingues (2013) investigated the use of UV

removal of these compounds was observed with this

photolysis, UV/TiO2, and UV/H2O2 for the removal of

treatment method.

compounds

studied.

Sanchez-Martin,


Apart from chemical pollutants, some studies

using pulsed ozonation. They found that daily pulsed ozone

compared various technologies for treating biological

doses could shorten the standard 15–30 day-long aerobic

emerging pollutants. Oncu and Balcioglu (2013a) compiled

digestion process to 4 days, while maintaining greater than

a literature review, and performed a study on the removal

85% of mixed liquor suspended solids removal and

of antimicrobial resistant elements by various oxidation-

achieving 99% removal of EDCs. Collado, Quero et al.

based

Heterogeneous

(2013) evaluated the performance of a combined wet

photocatalysis and ozonation were shown to be more

oxidation/aerobic biological process in removing phenolic

effective than conventional chlorination for the removal of

compounds (phenol and salicylic, p-hydroxybenzoic and 5-

a resistance carrier in DNA from a bacterial plasmid.

hydroxyisophthalic acids) from wastewater effluents from

Rizzo, Fiorentino and Anselmo (2013) utilized both UV

pharmaceutical manufacturing. The integrated process

radiation and chlorination for the treatment of antibiotic-

maintained high stability during fluctuations of hydraulic

resistant E. coli strains including those resistant to

and pollutant loads, and significant COD removal

amoxicillin, SMX, and ciprofloxacin (CPX). Chlorination

efficiencies (>97%) were obtained during each process

process did not cause an effect in the antibiotic-resistant

step. Yoon et al. (2013) performed bench-scale soil batch

strains, while UV was effective. UV photolysis was also

reactor studies in combination with ozonation to elucidate

able to degrade all three compounds, with the treatment

how aquifer recharge and recovery might attenuate TrOCs,

time required for each compound as follows: CPX (14 min)

generate

< amoxicillin (20 min) < SMX (25 min). The authors

biotransformation, and remove oxidation products from

conclude that conventional chlorination may not be

coupled ozonation. Seventeen target TrOCs were treated.

effective for addressing ARGs.

Fluorescence studies were used to analyze for bulk organic

water

treatment

technologies.

organic

matter

more

amenable

to

carbon attenuation. Ozonation was enacted either before or Combinations of Processes Combinations

of

biological

after aquifer recharge and recovery. Pre-ozonation was and

chemical

superior for removal of dissolved organics, while post-

oxidation processes have been a common focus of

ozonation was more effective for removal of certain

treatment research. Ozonation of amoxicillin in wastewater

fluorescing compounds and TrOCs. Nitrosodimethylamine

was tested as a pretreatment to biological degradation in an

formed in ozonation was found to be eliminated by aquifer

SBR (Lefebvre et al., 2013). Although ozonation was

recharge and recovery. A comparison of suspended

successful, performance of the SBR degraded, likely due to

activated sludge (MBBR), activated sludge, hydrodynamic

ozone byproducts, indicating that ozone may not be a

cavitation (HC)-H2O2, and UV treatment versus sequential

suitable pretreatment for amoxicillin wastewater. Muz et

treatment and the efficiency for removal of ibuprofen,

al. (2013) studied removal of EDCs in activated sludge

naproxen, ketoprofen, CBZ, diclofenac and a metabolite of


clofibric acid was reported by Zupanc et al. (2013). The

al., 2013). The vast majority of compounds were able to be

highest amount of biomass was actually determined to be in

removed by MBR followed by O3, O3/H2O2, or PAC, but

activated sludge rather than suspended on the carriers

not by MBR followed by ClO2.

(attached biomass), contrary to expectations. Removal was

studied the removal of a mixture of emerging pollutants

inconsistent for most pharmaceuticals and zero for CBZ be

(analgesics,

either biomass method. The HC/H2O2 treatment did remove

combination of ozonation, black-light photocatalysis and

CBZ and diclofenac, but featured only 40‒50% removal of

titania (supported in activated carbon and non-supported).

other TrOCs. Highest overall removals of all compounds

Processes that used ozonation achieved the highest

combined was found for a sequence of MBBR-HC/H2O2-

degradation rates compared to other processes (e.g.,

UV where CBZ and diclofenac removal was >98%. Silva et

photolysis (UVA), adsorption (TiO2 and [AC-TiO2]),

al. (2013) investigated the effect of a multitude of

photocatalytic oxidation). According to the results of TOC

treatments on biodegradability enhancement and trace

conversion profiles, ozonation-based processes are also

pollutants within

recalcitrant

most likely to achieve some degree of mineralization.

character of the leachate resulted in an initial 39%

Another research team (Zylan and Ince, 2013) compared

reduction in organic carbon utilizing biological treatment

the effectiveness of ozone-based treatments combined with

alone, but the removal increased to 70% when biological

combinations of UV, H2O2, FeSO4 and ultrasound (US) for

treatment was followed by photo-Fenton and another

abating

biological treatment after photo-Fenton.

Pharmaceutical

laboratory-scale reactor. Of the various combinations, the

wastewater containing high levels of CBZ and venlafaxine

US/UV and US/Fe+2 in combination with ozonation were

was run through biological activated sludge followed by

found to be remarkably efficient in rendering diclofenac-

ozonation to test the system’s removal efficiency (Lester et

free water and providing mineralization to reduce

al., 2013). Both CBZ and venlafaxine were recalcitrant to

disinfection byproduct production at the later chlorination

biological degradation but were degraded by ozone, with

steps. The US/Fe+2 process additionally allowed for a

degradation rates individually varying with pH. Ozonation

chemical-free coagulation step as a follow-on. Ferreira de

also increased the biodegradability of the wastewater,

Oliveira et al. (2013) observed that coupling of ozone and

which would be desired if followed by biological treatment.

activated carbon treatment enhanced the removal efficiency

One major focus area of research was the

and rates of recalcitrant pollutants, such as phthalates. The

landfill

leachate.

The

antibiotics,

diclofenac

of

and

Encinas et al. (2013)

anti-inflammatory)

using

simultaneously DOC

processes

also

achieved

in

a

a

enhancement of ozonation by coupling it with a variety of

combination

complete

other processes. PhACs in hospital wastewater effluent

mineralization of the compound as well as reaction product

were tested for removal using MBR coupled with oxidation

intermediates. The enhancement is most likely linked to the

(O3, O3/H2O2, ClO2) or adsorption technologies (Nielsen et

reaction of radicals formed via ozonation with the


functional groups at the activated carbon surface. The

draw solution, recycle of the draw solution using in-line

structure of the carbon surface is progressively modified

GAC or UV treatment could mitigate this limitation. Yet

during treatment, and shows increasing formation of

another alternative for concentrate management in tandem

carbonyl groups with longer ozone exposure times.

with membrane filtration was studied by Urtiaga et al.

Membranes coupled with other processes were

(2013) who examined an advanced tertiary treatment

studied by many research groups. Cartagena et al. (2013)

method, which included membrane technologies (UF-RO)

evaluated an MBR pilot plant using two different

and electrooxidation (boron-doped diamond electrodes) for

membrane systems. Removal efficiencies of 10 emerging

the elimination of two stimulants and ten pharmaceuticals

pollutants were determined and results were consistent with

from secondary wastewater treatment effluent. The

other previously published research showing that coupling

membranes were able to achieve 99% reduction for all

MBRs

and

target compounds with the electrooxidation utilized on the

biodegradation), and NF or RO (which provides size

concentrate stream (95% removal for most of the

exclusion),

for

compounds studied), exhibiting the potential of this

In some instances the combined

treatment train to remove emerging pollutants from

(which

provide

produces

emerging pollutants.

adsorption

high

removal

processes had a synergistic effect.

to

sludge

efficiencies

Low-pressure UV

secondary WWTP effluents.

photolysis combined with NF was investigated for the

Chon et al. (2013) evaluated the removal of seven

removal of emerging pesticides in drinking water, and

micropollutants of emerging concern performance using an

efficient removal of all pesticides was found with

integrated reclamation system (coagulation-disk filtration-

photodegradation byproducts also being removed by NF

UF and RO). The study showed that high pollutant

following UV treatment. An added benefit of disinfection

removals were achieved in the RO, with performance

can be found by coupling this process, and could perhaps

strongly influenced by the pollutants diffusion coefficient,

require a lower chlorine dose for disinfection, minimizing

molecular size cut-off and charge. The study of membrane

disinfection byproduct formation (Sanches, Penetra et al.,

foulants showed the highest affinity of RO membranes with

2013). Another study also found membrane treatment

hydrophilic fractions of pollutants, while hydrophobic

followed by UV to be a promising coupling (Xie, Price et

residuals were mainly detected in UF foulants. Diemert et

al., 2013). A combination of FO and membrane distillation

al. (2013) evaluated the production of halo-benzoquinones,

was examined for on-site use in mining of sewer effluent to

disinfection byproducts present in disinfected treated

produce recycled water. In particular the hybrid system

waters, from three different sources when alum coagulation

showed good removal of TrOCs, and membrane distillation

is followed by chlorination. The study also focused on the

could be operated with waste heat. The authors further

contribution

showed that while some compounds accumulated in the

benzoquinones and demonstrated that, in some instances a

of

NOM

in

the

formation

of


halo-

correlation exists between recalcitrant humic fraction of

BAC

water and the formation of the 2,6-benzoquinone, when a

sulfonamides. In short, authors made the same conclusion

compiled dataset with the three waters is used. Another

that a combination of technologies was necessary to

study evaluated combinations of processes and their effect

remove the mixture of antibiotics from the source water.

on unregulated disinfection by-product formation (Wei et

Yet another example of a beneficial coupling of membrane

al., 2013). Authors discussed the role of biological

filtration with other processes was demonstrated by

pretreatment and BAC in producing soluble microbial

Miralles-Cuevas (2013). Photo-Fenton treatment processes

products

experience slow reaction kinetics when the pollutant

which

serve

as

precursors

for

iodinated

treatment

was highly effective in

removing

trihalomethanes (I-THM). I-THMs were found in drinking

concentration is low.

water from Southern China after the chloramination unit.

micropollutants via NF prior to solar photo-Fenton

Model studies showed that CH2ClI levels increased with

treatment reduced H2O2 consumption and enhanced

increasing iodine content but remained low under high

degradation rates as compared to solar photo-Fenton

chlorine doses.

systems alone.

Lipids were the most reactive model

precursors of the soluble microbial products.

Pre-concentrating pharmaceutical

Another set of studies evaluated the performance

In general, most studies evaluating process

of whole plants. Occurrence and the removal of emerging

combinations concluded that a multibarrier approach is the

pharmaceuticals, personal care products, and caffeine were

key to providing treatment objectives. Combining multiple

investigated at a WWTP over a fourteen-month period in

treatment

organic

western Greece (Stamatis and Konstantinou, 2013). In

micropollutant removals was investigated, with the purpose

addition to the traditional preliminary, primary and

of suggesting treatment trains (Sudhakaran, Maeng and

secondary treatment with chlorine disinfection, the plant

Amy, 2013). This hybrid approach aimed to establish

included chemical phosphorus removal and sand filtration.

sustainable processes, and suggested the use of oxidation

All compounds investigated were detected within the

and microfiltration for pretreatment, while also suggesting

wastewater samples, with removal efficiencies of 46.3% for

NF, adsorption, and chlorination for a post-treatment

CBZ and 96.8% for naproxen. The study illustrated the

method in aquifer recharge and recovery. Conventional

ability

coagulation-sedimentation and ozone-biologically active

pharmaceuticals, although significant amounts still enter

carbon (BAC) systems were evaluated for removal of

the waterways. Ibañez et al., 2013 demonstrated the

antibiotics and organic matter in a contaminated lake in

occurrence of over 60 types of pharmaceuticals and

China (Liao et al., 2013). While coagulation and

emerging pollutants in WWTP effluent. The study showed

sedimentation was effective in removing fluoroquinolones,

that

ozonation was required for the removal of tetracycline and

conventional waste water treatment processes. Further

methods

(hybridization)

for

of

WWTPs

to

remove

some

levels

the compounds were effectively removed


of

by

treatment with ozone at a dosage of 7‒12 mg/L provided

plant investigations were not limited to WWTPs. The use

effective removal for all pollutants. The authors also

of UV/H2O2 alongside GAC and conventional surface water

documented the ineffectiveness of ultrasound treatment in

treatment in removing pesticides, endocrine disruptors,

combination with ozonation. Roccaro et al. (2013)

pharmaceuticals, solvents, and algae toxins, was tested for

proposed 10 possible upgrades to conventional WWTPs

use in full-scale water treatment plants which use water

utilizing a combination of treatment technologies in a

from Lake IJsell. It was confirmed that atrazine and diuron

multi-barrier treatment approach to aid the removal of

are degraded by photodegradation while benzatone and

EDCs and PPCPs. Data on the removal efficiency was

bromacil are degraded by hydroxyl-radical oxidation.

synthesized from existing literature in order to calculate the

Generally, it was found that this multibarrier system was

total unit cost for the upgraded facilities water for various

successful in degrading many compounds found in Lake

plant sizes. The concentrations and removal rates of trace

IJsell (Kruithof, 2013).

emerging organic pollutants were evaluated across various

In addition to the studies measuring the

stages of treatment in 16 WWTPs in UK. In this study by

performance of the whole plant, some modeled the plant

Gardner et al. (2013) a wide range of treatment

performance for specific pollutants. The preliminary design

performance was observed, and often tertiary treatment

and exploratory testing and modeling of a mineralizing

showed better pollutant removals than those achieved by

urban/suburban ambient net-zero water (UANZW) system

secondary treatment, possibly more sensitive to operating

was conceptualized by Englehardt et al. (2013) for potable

conditions (e.g., redox, HRT, SRT). Removal by adsorption

reuse applications and consequent elimination of emerging

to solid is also reported by Gardner et al. (2013) as an

compounds. The treatment train including MBR, IMA,

important removal process for TrOCs, and often not

vacuum UF, peroxone, and UV was designed to meet

functional for hydrophobic molecules. Faul et al. (2013)

potable water quality criteria through denitrification and

reviewed the quality of reclaimed water for domestic and

effluent mineralization of wastewater. EE2 was modeled as

human consumption from Gammams Sewage Treatment

a target compound and found to be completely removed

Plant (GSTP) and Goreangab Water Reclamation Plant

after treatment with peroxone at specific doses (6.7 g/h

(GWRP) in Namibia. E3, E1, testosterone, were among the

H2O2 and 22 g/h O3) and in presence of 17 mg COD/L or

EDCs under evaluation. The results showed that rainfall

NOM.

events produced seasonal patterns in the concentrations

investigated eight drinking water treatment methods for

profiles of EDCs in raw sewage entering GSTP. The GRWP

organic micropollutant removal using experimental and

has the potential to achieve complete removal of these

model studies. Multi-criteria analysis was conducted (cost,

compounds, even if partial removal is achieved in GSTP

sustainability, time, treatment, technology) which assessed

(27‒92% depending on the EDC considered). The full-scale

a slew of variables, with the model selecting river-bank

Sudhakaran,

Lattemann

and

Amy

(2013)


filtration and ozonation as the best method. A quantitative

(2013)

structure activity relationship model was used, suggesting

micropollutants in hospital wastewater using O3, O3/H2O2,

NF outranked RO for organic micropollutant removal.

PAC, and UV light with or without TiO2. They found that

compared

the

removal

efficiencies

of

the majority of wastewater micropollutants can be removed Comparison of Processes

by ozone and PAC, while some recalcitrant compounds,

While some of the studies that compared

like diatrizoate, can only be removed by high UV doses.

different methods within the biological, chemical or

Combined treatments of O3/H2O2 and UV/TiO2 did not

physical class were discussed in the corresponding sections,

improve removal efficiency over single treatments of ozone

this section summarizes the studies that compared

and UV. The efficiency of MBRs and ozonation in

processes involving different mechanisms of action. Some

removing endocrine disruptive potentials was studied for

studies focused on systems that involve a variety of

use in treatment of hospital wastewater (Maletz et al.,

processes. Abargues et al. (2013) evaluated the effect of

2013). Treatment by MBRs reduced estrogenicity of

light, oxygen and microalgae on removal of the endocrine-

sewage while ozonation efficiently removed most measured

disrupting compounds 4-(1,1,3,3-tetramethylbutyl)phenol,

compounds. Future investigation may require establishing

technical-nonylphenol, 4-n-nonylphenol, and BPA from the

whether either of these processes generates endocrine

effluent of an anaerobic MBR. Results demonstrated that

active metabolites.

the removal rates of these compounds differed with each

Yet another subset of studies in this category

post-treatment method and that aeration (oxygen) resulted

evaluated whole plants and either compared different

in the highest removal ratios indicating the importance of

treatment trains or compared processes within a single plant

an aerobic step in EDC degradation; a mass balance also

to each other in terms of effectiveness for emerging

showed that chemical oxidation was more important than

pollutant abatement. The concentrations and removal rates

sorption

compared

of ARGs were measured in three municipal WWTPs

perchlorate-selective ion exchange, biological reduction

employing conventional treatment followed by different

and catalytic treatment for perchlorate removal based on

advanced treatment systems [biological aerated filter,

the

inputs

constructed wetland, and UV disinfection] (Chen and

normalized to the mass treated, in a lifecycle analysis.

Zhang 2013). The authors reported ARG reductions of 1−3

Because resource consumption during the operational phase

orders of magnitude through three conventional activated

comprises > 80% of the total impacts of these technologies,

sludge processes. However, advanced post-treatment

the analysis indicates that ion exchange is competitive, but

systems differed with 1−3 orders of reductions in ARGs in

emerging technologies also show great promise from an

constructed wetlands, 0.6−1.2 orders in the biological

environmental sustainability perspective. Kovalova et al.

aerated filter, and no apparent decrease by UV disinfection.

processes.

environmental

Choe

impacts

et

al.

of

(2013)

consumable


Flores et al. (2013) evaluated a full-scale drinking water

upsetting biological processes were those meant to have

treatment plant and several pilot treatment systems with a

antibacterial action. In particular, silver nanoparticles and

number of conventional (prechlorination, coagulation, sand

antibiotics were of interest to researchers. Collado,

filtration and ozonation) and advanced (RO, reverse

Buttiglieri et al. (2013) studied the influence of 50 µg/L of

electrodialysis and GAC adsorption) water treatment

SMX on the bacterial community of a lab scale SBR fed

processes for their ability to remove perfluorinated

with synthetic wastewater over 2 months. COD and

compounds. Authors found the most efficient process was

nitrogen removal did not seem to be impacted by SMX.

RO, which resulted in 99% removal of the studied

SMX removal was favored during the aerobic phase of the

pollutants. Other processes that showed removal of both

SBR cycle and ranged between 20 and 50%. The bacterial

the pollutants were adsorption onto GAC and reverse

community changed after introduction of SMX, some

electrodialysis. All of the conventional processes proved to

species fading while new ones growing. Doolette et al.

be fully ineffective. Concentrations of antibacterial

(2013) investigated the toxic impact of silver and

chemicals triclocarbon and triclosan and a triclosan

polyvinylpyrrolidone coated silver nanoparticles (AgNPs)

biodegradation product methyltriclosan (MeTCS) were

to nitrifiers and methanogens cultured in bench-scale SBRs.

monitored in the liquid phase throughout a wastewater

Results showed that, in the short-term, both bacterial

plant by Lozano et al. (2013). Triclocarbon and triclosan

communities were not affected by exposure to AgNPs,

were primarily removed by sorption and settling, though

however a shift in bacterial population was observed,

concentrations of both also decreased during nitrification-

particularly for the anaerobic population. The sulfidation of

denitrification and triclosan concentration decreased during

Ag to form Ag-S species might have contributed to the

the activated-sludge stage. Ozonation followed by sand

limited toxicity observed, due to consequent reduction of

filtration and PAC followed by either sand filtration or UF

highly toxic Ag+ ions. Miller et al. (2013) studied the

were tested in parallel for removal of 70 potentially

effects of antibiotic and AgNPs on prevalence of 5

problematic substances and reduction of ecotoxicological

antibiotic-resistant genes (ARGs) in anaerobic digesters.

effects at large scale WWTPs over a year (Margot et al.,

AgNPs had no apparent effect on thermophilic digester

2013). Both technologies significantly reduced toxicity of

performance or ARG copy numbers. ARGs are the subject

wastewater, but PAC/UF technologies were both more

of increasing attention and concern. Yang, Wang, Qui et al.

costly and more effective.

(2013) showed that an RP4 plasmid can be transferred from donor strain to activated sludge in a MBR. Horizontal

Effect on Treatment transfer was indicated, and COD and nitrogen removal Biological processes at WWTPs are the most efficiency studies indicated changes in reactor performance vulnerable part of the water treatment cycle.

Some within 24 hours of inoculation and performance recovery

emerging pollutants that cause the most concern for


by day 31. In addition to inducing antibacterial resistance in the culture, some of the trace antibiotics were also shown to

Acknowledgements

affect the ability of the microorganisms to perform their

The authors would like to acknowledge the contribution of

tasks. Activated sludge was exposed to varying levels of

Sara R. Kelly from Carnegie Mellon University.

oxytetracycline to investigate changes in COD removal efficiency and microbial composition (Liu, Zhang et al.,

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