Environ. Process.

DOI 10.1007/s40710-017-0207-1

TECHNICAL NOTE

A Critical Evaluation of Advanced Oxidation Processes

for Emerging Contaminants Removal

Sara Ann Fast 1 & Veera Gnaneswar Gude 1 &

Dennis D. Truax 1 & James Martin 1 &
Benjamin S. Magbanua 1

Received: 5 October 2016 / Accepted: 31 December 2016

# Springer International Publishing Switzerland 2017

Abstract Removing emerging contaminants from waste streams has become a topic of
growing interest. The adverse effects of endocrine disrupting chemicals (EDCs) and
pharmaceutical and personal care products (PPCPs) have been well documented, but
much remains to be known about these contaminants and their removal. Their removal
with traditional methods has not been entirely successful. However, adequate degra-
dation can be achieved through the use of advanced oxidation processes (AOPs).
Multiple factors must be considered when completing an in-depth comparison; there-
fore, process engineering, environmental, and economic and social parameters were
included in a deeper analysis. This study presents a ranking system to numerically
score the performance of various AOPs (e.g., Ozonation, UV irradiation,
Photocatalysis, Fenton reaction, and integrated processes) in several categories of
parameters under engineering, environmental, and socioeconomic components. From
this preliminary assessment, it was noted that H2O2/O3 (Perozonation) presented the
highest average ranking (3.45), with other processes showing comparable performance.
TiO2 photocatalysis received the lowest ranking (2.11).

Keywords Endocrine disrupting chemicals . Pharmaceutical and personal care products .

Advanced oxidation processes . Cost analysis

* Veera Gnaneswar Gude

[email protected]

1
Civil and Environmental Engineering Department, Mississippi State University, Mississippi State,
MS 39762, USA
 S.A. Fast et al.

1 Introduction

1.1 Emerging Contaminants

Numerous pollutants and toxins have been a major concern in environmental management
throughout the history. Their removal has been fine-tuned and optimized in order to achieve
the highest percentage of contaminant removal at the lowest chemical and energy consumption
values possible. However, not all contaminants are easily removed by traditional methods, and
many remain relatively unknown. Chemicals such as these are classified as Bemerging
contaminants^ because many are not currently regulated and have the potential to cause
serious health concerns (Esplugas et al. 2002, 2007). Emerging contaminants have also the
potential to cause major adverse effects on aquatic environments, surface waters, drinking
water, and soils (Miranda-García et al. 2010). Many of these contaminants are actually
derivatives of manufactured products, making their removal particularly complicated (Guo
et al. 2009). The health threat posed to both humans and wildlife has made emerging
contaminants, such as endocrine disrupting chemicals (EDCs) and pharmaceutical and per-
sonal care products (PPCPs), topics of particular interest (Esplugas et al. 2007).

1.1.1 Endocrine Disrupting Chemicals

Endocrine disrupting chemicals have been found to disrupt the endocrine systems of both
humans and animals, which has resulted in the feminization of male fish, complications to the
reproductive system, and difficulties in egg shell breakage, among others. Human occurrences
include increases in certain types of cancers, as well as the presence of breasts in males and
reductions in sperm (Esplugas et al. 2007). EDCs have also been known to bio-accumulate in
body fat, which means that concentrations can build considerably (Rahman et al. 2009).
Known sources of EDCs include urban and agricultural runoff, landfill leachates, and con-
centrated animal feeding operations (Benotti et al. 2008). Treated wastewater and drinking
water can also contain EDCs that are not adequately removed by traditional treatment methods
(Westerhoff et al. 2005). Table 1 lists several EDCs, including a variety of pesticides,
hormones, and heavy metals (Westerhoff et al. 2005; Esplugas et al. 2007; Belgiorno et al.
2007).

1.1.2 Pharmaceutical and Personal Care Products

Pharmaceutical and personal care products (PPCPs) include pharmaceutical drugs, cosmetics,
fragrances, and food supplements, as can be seen in Table 1 (Westerhoff et al. 2005; Esplugas
et al. 2007; Belgiorno et al. 2007). PPCPs are in widespread use, making this an imperative
subject. Products such as these are used by most populations on a daily basis and can later be
inadvertently introduced into water sources. These contaminants are commonly sourced by
sewage effluents and hospital and animal wastes (Esplugas et al. 2007). In addition, it is not
certain what the chronic effects are for these contaminants (Benotti et al. 2008). Another
concern is the presence of increased amounts of antibiotics in water sources, leading to
resistance of bacteria and reducing the effectiveness of existing medications (Baquero et al.
2008). For example, the antiviral drug Oseltamivir, more commonly known as Tamiflu, is not
successfully degraded by traditional treatment methods, and even ultraviolet radiation has very
limited success (Fick et al. 2007).
Critical Evaluation of Advanced Oxidation Processes

Table 1 Examples of EDCs and PPCPs (Andreozzi et al. 1999; NWRI 2000; Azbar et al. 2004; Klavarioti et al.
2009; Dodson et al. 2012)

Contaminant (EDCs) Description Contaminant (PPCPs) Description

Bisphenol A Preservative, Acetaminophen Analgesic

Plastic
Compo-
nent
Butylated Hydroxyanisole Food Ketoprofen, Naproxen Analgesic
Preserva-
tive
DDT Pesticide Carbamazepine Anti-seizure
Atrazine Pesticide Ibuprofen Anti-Inflammatory
17β-estradiol Steroid Triclosan Antibacterial
Hormone
Estrone Steroid Ciprofloxacin Antibiotic
Hormone
Testosterone Steroid Acridine Antiseptic
Hormone
Cadmium Heavy Metal Bezafibrate Fibrate Drug
Mercury Heavy Metal Dilantin Antiepileptic
Lead Heavy Metal Nicotine Stimulant,
Insecticide
Arsenic Heavy Metal Meprobamate Anti-anxiety
Musk Ketone, Benzylacetate, Fragrances Phenytoin Anti-convulsant
Eugenol, Hexyl cinnemal, Glycol ethers - 2-Butoxyethanol, 2- Paints and cleaners
Limonene, Linalool, Methyl -Phenoxyethanol, 2,2- Biomedical and
eugenol, Methyl salicylate, -Methoxyethoxyethanol, 2,2- cosmetic products
Pinene, Terpineol, Bucinal -Butoxyethoxyethanol
Diphenyl ether DPMI HHCB Cyclosiloxanes –
Isobornyl acetate Methyl Octamethylcyclotetrasiloxane,
ionone Musk ketone Musk Decamethylcyclopentasiloxane,
xylene, Phenethyl alcohol Dodecamethylcyclohexylsiloxane,
Benzophenone, Benzophenone-1,
Benzophenone-3 Octinoxate
Hexabromocyclododecane Flame
Retardant
Caffeine Stimulant
Triclocarban, Triclosan Antimicrobial Benzophenone Benzophenone-1, UV filters
Benzophenone-3, Octinoxate
Linuron Herbicide Parabens - Methyl paraben Ethyl Preservatives
paraben Butyl paraben
Nonyl Phenol Surfactant Ethanolamines – Monoethanolamine, Detergents,
Diethanolamine emulsifiers,
polishes,
pharmaceuticals,
corrosion
inhibitors
Pthalates - Bis(2-ethylhexyl) Plasticizers Alkylphenols - 4-t-Octylphenol Detergents, and
adipate, Bis(2-ethylhexyl) Octylphenol monoethoxylate, cleaning products
phthalate, Benzylbutyl Octylphenol diethoxylate, 4-t-
phthalate, Di-cyclohexyl -Nonylphenol, Nonylphenol
phthalate, Di-isobutyl monoethoxylate, Nonylphenol
phthalate, Di-isononyl diethoxylate
phthalate, Di-n-butyl
phthalate,, Di-n-hexyl
phthalate, Di-n-octyl
phthalate, Di-n-propyl
phthalate, Diethyl phthalate
 S.A. Fast et al.

1.2 Advanced Oxidation Processes

Due to the difficulty of removing emerging contaminants, the introduction of more effective
processes is necessary.
Advanced oxidation processes (AOPs) have been proven as capable technologies
regarding the degradation of emerging contaminants (Stasinakis 2008; Sichel et al.
2011; O’Shea and Dionysiou 2012). In this process, organic compounds are fully
oxidized into carbon dioxide (CO2), water (H2O), and mineral acids (Metcalf and
Eddy 2014). Oxidants known as free hydroxyl radicals (•OH) are formed in this
process. Hydroxyl radicals react easily with organic compounds due to the unpaired
electron. Large amounts of hydroxyl radicals are produced by AOPs, improving the
degradation of difficult organic compounds. Furthermore, pollutants are degraded, or
broken down, not simply removed or altered. Theoretically, there are no resulting
products that must be removed following treatment. It follows that operational costs
are reduced due to the lack of the secondary waste stream that would be present if
other processes, such as adsorption, ion exchange, and stripping, were utilized
(Metcalf and Eddy 2014).
Common oxidizing agents used in AOPs include ozone (O3), UV, and hydrogen peroxide
(H2O2). Individual success degrading emerging contaminants has been demonstrated, but
greater removal can be achieved through processes that combine multiple oxidizing agents
(Metcalf and Eddy 2014). AOPs investigated in this research include: H2O2/O3, O3/UV, and
H2O2/UV. Several of these technologies are more widely known and well-developed, while
others are more novel, such as titanium dioxide (TiO2) photocatalysis and Fenton’s reaction.
Table 2 provides relevant data for these processes. The source water, initial contaminant
concentration in μg/L, and energy consumption in kWh/m3 is provided for each process;
however, the removal efficiencies of each process are not provided, as this data was not often
available. All the techniques discussed are considered capable technically of removing emerg-
ing contaminants; it is the remaining parameters that are of interest. Unless otherwise stated,
the constituent matrix included a large variety of emerging contaminants. Table 3 provides a
list of the process components for the advanced oxidation processes discussed in this study and
a comparison of the advantages and disadvantages for these processes. Table 3 also summa-
rizes the findings and the rationale for the ranking system developed in this study.

1.2.1 Ozonation (O3)

Due to its ability to cause cell lysis in bacteria, ozone (O3) has often been used as a
disinfectant. The production of ozone must occur on-site because it cannot be stored;
this can have a significant effect on operational costs (Reynolds and Richards 1996).
Furthermore, concentrations of ozone that are greater than 23% are potentially explo-
sive (Davis 2010). Ozonation is capable of achieving 90% emerging contaminant
removal (Huber et al. 2003), and it is the most commonly used dark oxidation method
(Esplugas et al. 2007).
Ozone is potentially hazardous because it is a compressed gas, an oxidizer, highly toxic,
and can produce carcinogenic byproducts. Aldehydes, such as formaldehyde, acetaldehyde,
glyoxal, methyl glyoxal, and bromate, are among the known byproducts. One positive effect is
the rise in effluent dissolved oxygen (DO) concentrations, which may make it easier to reach
DO standards (Metcalf and Eddy 2014).
Critical Evaluation of Advanced Oxidation Processes

Table 2 Summary of performance of some advanced oxidation processes

AOT Source/ Initial Concentration (μg/L) Specific Energy Reference

Water Consumption (kWh/m3)

Geosmin MIB Geosmin MIB

UV/O3 Fish Farm 0.0042–0.0067 0.0032–0.0087 19.00 8.00 Klausen and
(spiked) Grønborg
(2010)
UV/H2O2 Fish Farm 0.0042–0.0068 0.0032–0.0088 16.00 13.00 Klausen and
(spiked) Grønborg
(2010)
Oxalic Acid Dichloroacetic Oxalic Dichloroacetic
Acid Acid Acid
TiO2/O3 Synthetic 126 129 17.0 50.0 Mehrjouei et al.
(2014)
TiO2/UVA/O2 Synthetic 126 129 63.0 350.0 Mehrjouei et al.
(2014)
TiO2/UVA/O3 Synthetic 126 129 7.0 24.0 Mehrjouei et al.
(2014)
O3 Post MBR – – 11.93 Chong et al.
Wastewa- (2012)
ter
O3/UV Post MBR – – 6.15 Chong et al.
Wastewa- (2012)
ter
H2O2/UV Post MBR – – 0.23 Chong et al.
Wastewa- (2012)
ter
Photocatalysis Post MBR – – 7.09 Chong et al.
Wastewa- (2012)
ter
80 W 40 W Lamp
Lamp
UV/HOCl Tap Water 1.00 0.32 0.16 Sichel et al.
(2011)
UV/ClO2 Tap Water 1.00 0.32 0.16 Sichel et al.
(2011)
UV/H2O2 (UV Tap Water 1.00 0.5 Sichel et al.
mp lamps) (2011)
UV/H2O2 w/ MF/RO – – 0.62 James et al.
RO Permeate (2014)
UV/H2O2 w/ MF/RO – – 0.93 James et al.
MF Permeate (2014)
UV/H2O2 w/ MF/RO – – James et al.
AC Permeate (2014)
O3 (2 mg/l) WWTP 0.001–0.503 0.03 Kim and Tanaka
Effluent (2011)
O3 (4 mg/L) WWTP 0.001–0.503 0.06 Kim and Tanaka
Effluent (2011)
O3 (6 mg/L) WWTP 0.001–0.503 0.09 Kim and Tanaka
Effluent (2011)
O3 (2 WWTP 0.001–0.503 0.37 Kim and Tanaka
mg/l)/- Effluent (2011)
UV21.5W
O3 (4 WWTP 0.001–0.503 0.4 Kim and Tanaka
mg/L)/- Effluent (2011)
UV21.5W
 S.A. Fast et al.

Table 2 (continued)

AOT Source/ Initial Concentration (μg/L) Specific Energy Reference

Water Consumption (kWh/m3)

O3 (6 WWTP 0.001–0.503 0.43 Kim and Tanaka

mg/L)/- Effluent (2011)
UV21.5W
O3 (2 WWTP 0.001–0.503 1.06 Kim and Tanaka
mg/l)/UV65W Effluent (2011)
O3 (4 WWTP 0.001–0.503 1.09 Kim and Tanaka
mg/L)/- Effluent (2011)
UV65W
O3 (6 WWTP 0.001–0.503 1.12 Kim and Tanaka
mg/L)/- Effluent (2011)
UV65W
UV(10 W) Hospital 0.4 10.00 Köhler et al.
WW (2012)
UV(2.5 W) Hospital 0.4 6.00 Köhler et al.
WW (2012)
0.83 gH2O2L−1 Hospital 0.4 2.00 Köhler et al.
WW (2012)
1.11 gH2O2L−1 Hospital 0.4 2.00 Köhler et al.
WW (2012)
Conventional NF/GAC – 0.16 Bonton et al.
GAC Plants (2012)
Nanofiltration NF/GAC – 0.55 Bonton et al.
Plants (2012)

1.2.2 Ultraviolet Light (UV)

Ultraviolet light has been used for disinfection purposes in the past, but its applications are
extended to AOPs through the process of photolysis (Reynolds and Richards 1996). Photolysis
degrades contaminants through light exposure and the absorption of photons (Metcalf and
Eddy 2014). This absorption of photons causes the outer electrons in a compound to become
unstable, and thus they become reactive or split. UV lamps are commonly used as the light
source in this process, but the sun is also a viable source. Experiments have been completed to
determine the advantages and disadvantages of submerged versus overhead bulbs, resulting in
the conclusion that submerged bulbs produce improved effects (Reynolds and Richards 1996).
In addition, either low-pressure or medium-pressure lamps can be used. Medium-pressure
lamps require a smaller number of lamps because their intensity is greater than low-pressure
lamps (Davis 2010).
UV lamps demand periodic replacement, as well as maintenance due to fouling of the UV
lamp sleeves which causes high maintenance costs (Metcalf and Eddy 2014). Furthermore, UV
lamps often have higher energy requirements than other processes. Also, the absorbance of UV
light is reduced if large amount of compounds, such as iron and nitrate, are present (NWRI 2000).

1.2.3 Photocatalysis (TiO2)

Photocatalysis degrades a wide variety of contaminants by forming free hydroxyl radicals in

the presence of a metal oxide semiconductor and a light source (Haroune et al. 2014). Titanium
Critical Evaluation of Advanced Oxidation Processes

Table 3 Comparison of advanced oxidation processes (Pros and Cons of each process) discussed in this study
(NWRI 2000; Al-Kdasi et al. 2004; Baquero et al. 2008; Comninellis et al. 2008; Poyatos et al. 2010; Oller et al. 2011)

Process Process components Remarks

Ozonation O3 generator and diffusers + Serves as supplemental disinfectant

Contactor vessels + Established technology
Ozone off-gas catalytic decomposer + Public acceptance is moderate
Supply and discharge pumps and piping − Potential for bromate formation which may be
Monitoring and control systems controlled
− May require ozone off-gas treatment and/or per-
mitting
− Interference with chemical compounds
− Potential for trihalomethanes (THMs) due to
pre/post chlorination
Ultraviolet Ultraviolet lamps, lamp sleeves and + No potential for bromate formation
Light cleaning system + Disinfection by UV
Temperature controller + NO off-gas treatment required
Supply and discharge pumps and piping + NO mass transfer limitations
Monitoring and control systems + History of operation and regulatory acceptance with
H2O2
+ Public acceptance is high with H2O2
− Turbidity interference
− UV lamps and sleeve failures
− Interference with chemical compounds
− Potential for trihalomethanes (THMs) or HAAs due
to pre/post chlorination
Photocatalysis TiO2 slurry injection and extraction + No potential for bromate formation
system + NO off-gas treatment required
TiO2 impregnation resin fluidized bed − Pretreatment necessary to avoid biofouling of
reactor catalyst
Static mixer − Separation of TiO2 required
Supply and discharge pumps and piping − Potential loss of TiO2 activity
Monitoring and control systems − Efficiency is highly pH dependent
− Not a well-established technology
Fenton Fe II and hydrogen peroxide storage and + No potential for bromate formation
Process injection systems + Less energy requirements
Completely stirred tank reactor + NO off-gas treatment required
pH controllers − Requires iron extraction system
Iron removal system − Very low pH required to keep iron in solution
Supply and discharge pumps and piping − Operation and maintenance costs due to pH
Monitoring and control systems adjustment
H2O2/O3 H2O2 storage and injection system + Serves as supplemental disinfectant
O3 generator and diffusers + More effective than O3 or H2O2 alone
Contactor and mixing vessels + Established technology
Ozone off-gas catalytic decomposer + Field-proven history of operation and regulatory
Supply and discharge pumps and piping acceptance
Monitoring and control systems + Public acceptance is high
− Potential for bromate formation which may be
controlled
− Potential for microbial growth due to Excess H2O2
− May require ozone off-gas treatment and/or per-
mitting
O3/UV Ultraviolet lamps, lamp sleeves and + Serves as supplemental disinfectant
cleaning system + More effective than O3 or H2O2 alone
Ozone generator and diffusers + Public acceptance is high
Liquid O2 or compressed air tank − Energy and cost intensive process
Contactor and missing vessels − Potential for bromate formation which may be
Ozone off-gas catalytic decomposer controlled
Temperature controller
 S.A. Fast et al.

Table 3 (continued)

Process Process components Remarks

Supply and discharge pumps and piping − May require ozone off-gas treatment and/or per-
Monitoring and control systems mitting
− Interference with chemical compounds
− Potential for trihalomethanes (THMs) due to
pre/post chlorination
H2O2/UV H2O2 storage and injection system + No potential for bromate formation
Ultraviolet lamps, lamp sleeves and + NO off-gas treatment required
cleaning system + Established technology
Temperature controller + Public acceptance is moderate
Supply and discharge pumps and piping − Interference with chemical compounds (e.g., nitrate)
Monitoring and control system − Turbidity influence on UV light
Reactor chamber − Potential for trihalomethanes (THMs) or HAAs due
to pre/post chlorination

dioxide (TiO2) has been found to be among the most effective and can be utilized as either a
slurry or an immobilized catalyst (Belgiorno et al. 2007). Furthermore, photocatalysis has been
found to not only degrade contaminants, but also the derivatives that are produced during most
treatments (Haroune et al. 2014). Removal efficiencies for emerging contaminants have been
reported as greater than 98% in some studies (Esplugas et al. 2007).
As it is a relatively new method, there are still uncertainties relating to its novelty. These
issues can be alleviated through pilot plants and full scale studies. Disadvantages such as
fouling of the UV lamps sleeves and the TiO2 catalyst can occur. Furthermore, maintenance
during the recovery of TiO2 slurry is necessary (Metcalf and Eddy 2014).

1.2.4 Fenton Process

During the Fenton reaction, hydroxyl radicals are formed through the reaction between ferrous
iron (Fe2+) and H2O2 (Lloyd et al. 1997). It has been reported that the Fenton reaction is
capable of removing compounds, such as clofibric acid and X-ray contrast agents, which are
not removed by more common methods, such as ozonation (Esplugas et al. 2007).
Low pH conditions are required, however, for the Fenton reaction to be successful (Metcalf
and Eddy 2014). Optimal pH levels have been reported to be between 2 and 4 (Shemer et al.
2006). If the pH is too low, the scavenging of hydroxyl radicals can increase, but if the pH is
too high, the oxidation potential and degradation rates will decrease (Shemer et al. 2006).

1.2.5 H2O2/O3

The individual success of H2O2 and O3 may be limited, but the efficiency can be significantly
increased if these compounds are merged into one technique (NWRI 2000). This combination
of processes can be advantageous in some instances, such as during the degradation of
compounds that do not absorb UV well (Metcalf and Eddy 2014). Furthermore, H2O2/O3
has an advantage over UV processes because of the lack of related equipment and mainte-
nance, which can reduce energy requirements.
However, it can be difficult to maintain the proper operating conditions, including chemical
dosages and pH level (Metcalf and Eddy 2014). Ozone dosage is a particular concern because
the actual required dosage is larger than estimated through stoichiometry. An excess of ozone
Critical Evaluation of Advanced Oxidation Processes

or H2O2 can produce unwanted byproducts, such as bromate, or even the quenching of
hydroxyl radicals. Residual H2O2 can also disrupt the proper functioning and reaction of
hydroxyl radicals. While the removal of excess H2O2 is necessary, it also introduces additional
operational and maintenance costs.

1.2.6 O3/UV

Another viable integration of processes is O3/UV. Ozone photolysis first produces H2O2. The
H2O2 can then react with the O3 to produce hydroxyl radicals for use in contaminant
degradation. The multiple mechanisms simultaneously contribute to the efficacy of this
process because there are opportunities for degradation through not only the production and
reaction with hydroxyl radicals, but also through ozonation and photolysis (Metcalf and Eddy
2014).
It has been reported that O3/UV produces greater amounts of hydroxyl radicals than H2O2/
UV; however, this statement is contingent on the types of UV lamps used (NWRI 2000). The
O3/UV process shares the same disadvantages as ozonation and UV individually. This includes
the necessary destruction of ozone and potential UV lamp fouling. Once again, UV lamps tend
to be more energy intensive (Metcalf and Eddy 2014). In addition, the O3/UV process creates
H2O2, which may not be as feasible as simply introducing H2O2.

1.2.7 H2O2/UV

Hydroxyl radicals can also be produced through the photolysis of H2O2. However, high
dosages of both UV and H2O2 may be necessary. Subsequently, high amounts of H2O2 may
be present in the effluent. This can impede disinfection and requires removal. Despite this fact,
it has been found that elevated H2O2 concentrations can be used to degrade pollutants that
were not able to be degraded by UV treatment alone (Linden et al. 2005). As previously
mentioned, processes related to the use of UV lamps are subject to fouling and higher energy
consumption costs. However, the lack of the use of O3 can be considered an advantage because
there is no potential bromate production (NWRI 2000).

2 Materials and Methods

2.1 Holistic Analysis

A holistic analysis was completed to determine the AOP performance at removing EDCs and
PPCPs with respect to a broad spectrum of parameters that are essential to overall constituent
removal success. Three categories were chosen for the analysis: process engineering param-
eters, environmental parameters, and social and economic parameters. Process engineering
parameters include: mechanical reliability, process reliability, flexibility, adaptability, and
energy consumption. Environmental parameters include: contribution to climate change,
eutrophication, terrestrial and aquatic toxicity, and degradation products. The selection of
these parameters were influenced by the factors investigated during Life Cycle Analysis
studies (SAIC 2006). Social and economic parameters include: public acceptance, ease of
use, and economic feasibility. A variety of AOPs were studied, including: O3, H2O2/O3, O3/
UV, H2O2/UV, TiO2 photocatalysis, and the Fenton reaction.
 S.A. Fast et al.

2.2 Parameter Ranking Methodology

Based on a comprehensive literature review and analysis, a ranking system was developed to
assign a numerical value corresponding to the performance of each process in these parame-
ters. This system compares the processes and parameters on a uniform, numerical basis. The
ranking system has a value system ranging from 1 to 5 corresponding to descriptive variable of
Bvery low^ to Bvery high^. The highest positive value possible is represented by a ranking of
five, while a value of one indicates the poorest performance. The high rank also indicates
reduced maintenance and operating costs. Tables 3 and 4 should be referred for clarification of
the ranking system.

2.3 Comparison and Assessment

Application of the ranking system allows for comparison of each process for the individual
parameter. Average rankings were also calculated for each category of parameters, which
indicates the process that performs at the highest level in each category. The technologies that
function well in all three categories were identified by a cumulative comparison. A final
average ranking could then be calculated using the category averages, essentially indicating the
superior technologies overall.

3 Results

3.1 Process Engineering Parameters

Mechanical reliability, process reliability, flexibility, adaptability, and energy consumption

compose the process engineering parameters. Table 4 displays the rankings assigned to each
of the processes for each parameter and the average rankings for each process. These findings
are summarized in Fig. 1.

Table 4 Parametric ranking summary

AOPs

Parameters O3 H2O2/O3 O3/UV H2O2/UV TiO2 Fenton

Mechanical Reliability 4 4 3 3 2 2
Process Reliability 4 4 4 4 2 2
Flexibility 4 4 4 4 3 3
Adaptability 3 3 2 2 3 3
Energy Consumption 2 3 2 4 2 5
Average Engineering 3.4 3.6 3 3.4 2.4 3
Climate Change 2 3 2 4 2 5
Eutrophication 5 5 5 5 5 5
Toxicity 2 3 2 3 2 2
Average Environmental 2.25 2.75 2.25 3 2.25 3
Public Acceptance 4 4 4 4 2 2
Ease of Use 4 4 4 4 2 2
Economic Feasibility 5 4 4 3 1 4
Average Economic and Social 4.33 4 4 3.67 1.67 2.67
Comprehensive Average 3.33 3.45 3.08 3.36 2.11 2.89
Critical Evaluation of Advanced Oxidation Processes

Fig. 1 Process engineering parameters

3.1.1 Mechanical Reliability

The mechanical soundness of a process determines the dependability. Processes with more
mechanical pieces will inevitably have increased maintenance and replacement costs, which
can affect the successful functioning of the process as a whole. Therefore, a mechanically
simple process will be more reliable.
The selected AOPs were ranked based on their mechanical reliability. Table 4 shows that
O3, H2O2, and H2O2/O3 were given rankings of four, indicating high mechanical reliabilities,
while both O3/UV and H2O2/UV received rankings of three. Ozone generators and ozone gas
diffusers require inspection and cleaning routinely. The precipitation of carbonates can lead to
sparger fouling, which decreases the efficiency of ozone transfer (NWRI 2000). Furthermore,
UV lamps require replacement, as well as periodic inspections (Metcalf and Eddy 2014. The
processes receiving the lowest rankings were TiO2 photocatalysis and Fenton process, each
ranked two, due to high maintenance requirements relating to condition parameters such as
pH, mixing, and chemical (TiO2 and iron) addition (NWRI 2000).

3.1.2 Process Reliability

A unit is essentially useless if it cannot consistently produce a satisfactory effluent that meets
all required water quality standards. An effective technology will not only produce the required
effluent, but it will also do so steadily, despite variations in flow, influent quality, and
environmental conditions.
As can be seen in Table 4, O3, H2O2/O3, O3/UV, and H2O2/UV each received rankings of
four because they are capable of regularly producing an adequate effluent without complica-
tions and have a history of being reliable systems. Treatment processes that have been in use
for longer periods of time generally display greater process reliability (NWRI 2000). Con-
versely, newer technologies, such as TiO2 photocatalysis and the Fenton process, tend to be
less reliable due to lack of experimental and field data. In addition, these processes also require
removal of chemicals used, which will vary the quality of the effluent (NWRI 2000). TiO2
photocatalysis and the Fenton process thus received rankings of two. Despite the fact that
H2O2/O3, and H2O2/UV processes require removal of excess chemicals, their practical dem-
onstration and feasibility outweighed this drawback.
 S.A. Fast et al.

3.1.3 Flexibility

Process flexibility refers to the process capability of adjusting to changes in the influent flow
rate. A successful technology can continue to operate properly despite variations both above
and below the designed flow rate. As discussed previously, older technologies have been given
the opportunity to corroborate their flexibility, while more recent processes have not. Processes
using ozone or UV can react to changes with relative ease because chemical dosages can easily
be adjusted in response to fluctuations in flow.
Thus, rankings of four for O3, H2O2/O3, O3/UV, and H2O2/UV can be seen in Table 4.
While TiO2 photocatalysis and the Fenton reaction are newer technologies, they are also fairly
flexible. These processes are often designed in semi-batch reactors, suggesting that they can
manage flow rate fluctuations, which earns them rankings of three (NWRI 2000).

3.1.4 Adaptability

Adaptability is similar in some aspects to the previous parameter, flexibility, but it concerns
variations in water quality instead of quantity. The quality of a water source can have a
considerable impact on the efficacy of a process. Consistent water quality is not guaranteed,
but an effective process must be able to respond to changes in the constituent matrix.
Influent water having high turbidity may face difficulties in processes using a UV
light source because penetration may become limited (NWRI 2000). Adaptations to
particular constituents must also be made. The presence of nitrate and iron can reduce
the degradation efficiency of processes that utilize UV. O3 diffusers and UV lamp
sleeves are subject to scaling and fouling (NWRI 2000). TiO2 photocatalysis produces
hydroxyl radicals quickly, and may be capable of responding well to changes in water
quality; however, the UV component is still susceptible to the difficulties mentioned
previously (NWRI 2000). The Fenton reaction is expected to respond relatively well
to variations in water quality, but it should be recalled that this process is sensitive to
pH conditions. Understandably, AOPs are highly dependent on influent water quality
and all the processes require pH adjustment to be effective. As can be seen in Table 4,
all processes, with the exception of O3/UV and H2O2/UV (which received rankings of
two), were assigned rankings of three.

3.1.5 Energy Consumption

Energy consumption can easily be considered one of the most essential factors in this
study. It is currently a global goal to reduce the amounts of energy used in order to
decrease depletion of fossil fuels and alleviate other negative impacts that energy
production or use can have on the environment. One of the largest contributors to
overall process costs is energy consumption. UV lamps are one of the greatest
contributors to high energy consumption values. Table 2 presents energy consumption
values in kWh/m3.
Low rankings were assigned to processes using UV lamps; however, H2O2/UV generally
displays low energy consumption and received a ranking of 4. Due to the requirement for
on-site O3 generation, processes using O3 received lower rankings. The Fenton process
receives the highest ranking because its energy demands do not expand past simple pumping
requirements (NWRI 2000).
Critical Evaluation of Advanced Oxidation Processes

Energy consumption can also vary for one process based on the contaminant that is being
removed, however (Mahamuni and Adewuyi 2010). For example, when treating a post-
membrane bioreactor wastewater sample, O3, O3/UV, H2O2/UV, and photocatalysis reported
energy consumption values of 11.93, 6.15, 0.23, and 7.09, respectively, which indicates that
O3 requires more energy for this particular constituent matrix, while ozonation only reported
0.03-0.09 kWh/m3 for a variety of ozone dosages (Chong et al. 2012; Kim and Tanaka 2011).
These values also illustrate the significant influence of proper H2O2 dosage on lowering energy
consumption. For comparison purposes, it can be noted that for granular activated carbon
(GAC) an energy consumption of 0.16 kWh/m3 has been reported, and for nanofiltration 0.55
kWh/m3 (Bonton et al. 2012).

3.2 Environmental Parameters

Contribution to climate change, eutrophication, terrestrial and aquatic toxicity/degradation

products are environmental parameters in consideration. The rankings assigned to each of
the processes for each parameter and the average rankings for each process are presented in
Table 4. Figure 2 compares these findings graphically.

3.2.1 Contribution to Climate Change

During the development of new technologies, global climate change is a constant

concern. All efforts are made to decrease production of greenhouse gases in order to
reduce effects such as polar melt, altered wind and ocean patterns, sea level rise, and
change in seasons (SAIC 2006). Contributors to climate change include: carbon
dioxide (CO2), nitrogen dioxide (NO2), methane (CH4), chlorofluorocarbons (CFCs),
hydrochlorofluorocarbons (HCFCs), and methyl bromide (CH3Br) (SAIC 2006). CO2
emissions are directly related to the generation of electricity; therefore, the rankings
for this parameter are based on energy consumption. However, there are many other
factors contributing to climate change, such as additional resources and energy utilized
in the production of chemicals, equipment, etc.
Upon review of Table 4, it can be noted that the Fenton process and H2O2/UV, which
received high rankings for their low energy consumptions, also received high rankings for
climate change. A high score indicates a positive reflection, or low contribution to climate
change, while a low ranking signifies higher contributions. Larger energy consumption values
resulted in lower rankings.

Fig. 2 Environmental parameters

 S.A. Fast et al.

3.2.2 Eutrophication

Excess nutrients, such as nitrogen and phosphorus, can potentially be incredibly harmful to
aquatic wildlife. The process whereby the concentrations of nutrients increases to significant
levels is known as eutrophication. Operations that introduce additional nutrients into the
environment are not considered viable. The following list includes nutrients of concern:
phosphate (PO4), nitrogen oxide (NO), nitrogen dioxide (NO2), nitrates, and ammonia (NH4)
(SAIC 2006). While AOPs are practical methods for removal of emerging contaminants, they
are often preceded or followed by other technologies that target nutrients more specifically in
advanced wastewater treatment. Furthermore, the discussed nutrients are not created or released
during operation. As can be seen in Table 4, all processes received rankings of 5.

3.2.3 Terrestrial and Aquatic Toxicity

The removal of emerging contaminants to prevent harm to humans and wildlife is the ultimate
goal of these AOPs, but it is possible that other toxic materials are introduced. Chemicals used
during the treatment methods can potentially enter a waterbody. In addition, byproducts that
are formed during the progression of the process can also be problematic. A technology that
effectively removes emerging contaminants, but also releases other damaging or toxic mate-
rials is not a practical technology.
As mentioned previously, bromate and other byproducts are produced when O3 is utilized.
Bromate is carcinogenic, which merits considerable concern, but the release of bromate can be
minimized with proper care. For example, bromate production during H2O2/O3 can be
diminished with proper chemical doses (NWRI 2000). Processes that employ UV lamps have
the advantage of introducing no additional chemicals. TiO2 photocatalysis requires recovery of
the TiO2 catalyst, which poses potentially harmful effects as the inactivated catalyst itself can
serve a favorable site for microbial growth, while the Fenton process demands removal of iron.
Although iron is an essential trace element, exposure should be limited (World Health
Organization 2003) and subsequent discoloration of the reactor effluents can be problematic
when discharged to public receiving waters.
The production of degradation products from the contaminants themselves is also a
concern. It has been suggested that effluent from AOPs be treated subsequently by
biofiltration, membranes, or other techniques to remove byproducts (Snyder et al. 2003).
Some studies question whether the degradation products of AOPs are actually more harmful
than the original contaminant (Gómez et al. 2008). This is a relatively new area of study that
requires progress in analytical determination processes (Agüera et al. 2013). Acetaminophen is
one example of an emerging contaminant with known transformation products. One study
noted the removal of acetaminophen, but the pollutant was instead degraded into 4-
aminophenol (del Mar Gómez-Ramos et al. 2011). An in depth study of the degradation of
the insecticide thiamethoxam reported that a large number of byproducts were produced (Mir
et al. 2013).
Bromate formation led to lower rankings for processes utilizing ozonation, as seen in
Table 4. H2O2/O3 was ranked slightly higher because of the potential for remedy as discussed
previously. TiO2 photocatalysis and the Fenton reaction received lower scores because of the
introduction of catalyst and iron respectively. Higher scores were assigned to UV processes as
they do not directly introduce chemicals into the effluent. The score for each process was also
lowered due to the potential for transformation products.
Critical Evaluation of Advanced Oxidation Processes

3.3 Economic and Social Parameters

Public acceptance, ease of use, and economic feasibility are considered economic and social
parameters. Table 3 presents the public acceptance of the processes. Table 4 presents process
and parameter rankings, and the average rankings. A graphical comparison can be seen in
Fig. 3.

3.3.1 Public Acceptance

The extent to which the general public acknowledges and understands a treatment process is
critical. The opinions of individuals outside of the design process must be taken into account
because the well-being of the public is given a very high priority. Despite their lack of an in-
depth understanding of all water and wastewater treatment processes, the public must be given
the opportunity to be informed and give input.
Historically, the public accepts traditional, conventional, and widely used technologies.
This means acceptance of new treatment processes using novel materials and reactor config-
urations can be difficult to achieve. Another sensitive subject is the introduction of potentially
harmful substances. This is reflected in the low rankings of TiO2 photocatalysis and the Fenton
process in Table 4. Furthermore, these processes require the addition of inorganic chemicals
(TiO2 and iron) that are viewed negatively (NWRI 2000). Higher scores are given to the more
well-known processes because they are more easily accepted due to the more numerous pilot-
scale and full-scale demonstrations.

3.3.2 Ease of Use

The user friendliness of a process plays an important role when selecting and implementing a
process. A complicated process is more likely to have a greater number of errors. Higher labor
costs may also be involved if skilled personnel is necessary. It is also likely that a more
intricate system will have higher operational and maintenance costs due to unusual chemicals
or units.
Once again, conventional processes are displayed as receiving higher scores in Table 4,
while the more novel techniques received lower rankings. Older techniques have been given
the opportunity to be corrected and perfected. TiO2 photocatalysis and the Fenton process have
not had this same opportunity. Additional pilot-scale or full-scale testing are needed to give

Fig. 3 Economic and social parameters

 S.A. Fast et al.

accurate representations of daily use. Furthermore, the required catalyst recovery involved
with photocatalysis adds a level of difficultly.

3.3.3 Economic Feasibility

Economic practicality is perhaps one of the most critical features when choosing a
treatment method. The limiting factor in many situations is often available capital. A
technology immediately becomes less appealing if it cannot be easily supported
financially. High capital, maintenance, or operation costs reflect very negatively on
a method. Table 4 shows the average economic and social rankings.
Operation and maintenance costs include costs relating to part replacement, labor,
analytical methods, chemical use, and electrical requirements (Mahamuni and
Adewuyi 2010). The rankings in Table 4 directly reflect the cost estimates in Table 5
($/1000 L). Estimates were not found for H2O2/O3, so a comparison between related
technologies was used to assign ranking. Ozonation performs incredibly well in this
area, particularly in comparison to the other processes. TiO2 photocatalysis, however,
shows little strength related to economic feasibility as the reported total cost is $2285/
1000 L (Mahamuni and Adewuyi 2010). Somewhat average rankings were assigned to
the remaining methods. Ozonation received a very high score for its low cost of
$0.27/1000 L (Mahamuni and Adewuyi 2010).

4 Discussion

Figure 4 shows the comparison of parametric rankings for all processes. Throughout
this study, the comparison presented between more established processes and more
modern ones is a major issue to consider. TiO2 photocatalysis and the Fenton reaction
oftentimes received lower scores because of their relative novelty, while the more
conventional processes received higher scores. This is especially true amongst the
economic and social parameters. This may not be a fair comparison, as the general
public is becoming more open to new technology, so the negative reflection illustrated
in this study may not be accurate. Also, vastly different results could be found if this
same study was completed in the future.
It can be difficult to create an equal comparison between all of the processes discussed. One
key component for consideration is the constituent matrix of the influent to be treated. Some
pollutants are more readily degraded than others; therefore, processes removing these contam-
inants may be more likely to produce high rankings. Also, some pollutants react more

Table 5 AOP cost estimates shown in $/1000 L (Mahamuni and Adewuyi 2010)

AOP Cost ($/1000 L) Amortized Annual Capital Cost Annual O&M Costs

O3 0.32 1.99E + 04 2.42E + 04

O3/UV 10.21 2.96E + 05 1.12E + 06
H2O2/UV 81.50 6.24E + 05 1.07E + 07
TiO2 2285.02 6.63E + 07 2.51E + 08
Fenton 3.77 – 5.26E + 05
Critical Evaluation of Advanced Oxidation Processes

Fig. 4 Comparison of average rankings

positively to some processes. An examination of all processes across multiple source waters
would be advantageous.
A more detailed economic comparison was completed following the initial study, as this
can be considered one of the most essential parameters. Additional data was acquired from
Mahamuni and Adewuyi (2010) to compare the operational and maintenance costs. These
results can be viewed in Table 6 and Fig. 5. It is clear that the poor performance of TiO2
photocatalysis pertaining to economic feasibility is directly related to extremely high electrical
costs, which are significantly higher than other processes. A dramatic reduction in energy
usage and cost must occur for TiO2 photocatalysis to be a feasible process.
Degradation products created through these processes are also a concern, particularly
because they are prospectively more harmful than their parent products. Detection and
identification of transformation byproducts is essential as these could have more detrimental
effects on humans and the receiving environment (Gómez et al. 2008). Additional research is
needed to achieve a better understanding of these byproducts, as well as to determine the
correct mechanisms of removal.
All the parameters considered in the study were given equal worth, but this is not always
true. For example, economic feasibility was considered equally as important as adaptability.
Most individuals would agree that economic factors must be given priority. The ranking
method could be altered by weighting parameters according to their importance, but this does
include a certain amount of user bias. User bias is a considerable issue in this study. One
individual could assign a vastly different ranking based on that individual’s influences or
background. The introduction of a survey to obtain a variety of opinions on subjects such as
public acceptance could be very helpful.
This particular ranking system used five levels of ranking. The use of more levels of
ranking would produce a more detailed study. This also provides the potential for more

Table 6 Operational and maintenance costs (Mahamuni and Adewuyi 2010)

O&M Cost Breakdown ($/1000 L)

AOP Part Replacement Labor Analytical Chemical Electrical Total

O3 1.35E + 02 1.2E + 04 1.1E + 04 0.00 1.08E + 03 2.42E + 04

O3/UV 3.38E + 05 1.57E + 04 1.92E + 04 0.00 7.50E + 05 1.12E + 06
H2O2/UV 7.34E + 05 1.03E + 04 8.24E + 03 8.32E + 06 1.63E + 06 1.07E + 07
TiO2 7.79E + 07 1.03E + 04 8.24E + 03 4.12E + 03 1.73E + 08 2.51E + 08
Fenton 0.00 1.26E + 04 8.24E + 03 5.05E + 05 0.00 5.26E + 05
 S.A. Fast et al.

Fig. 5 O&M cost comparison for various advanced oxidation processes ($/1000 gallons)

deviation between scores, which would illustrate the advantages and disadvantages of each
process more clearly.

5 Conclusions

Advanced oxidation processes have successfully demonstrated their ability to degrade emerg-
ing contaminants. They include: O3, H2O2/O3, O3/UV, H2O2/UV, TiO2 photocatalysis, and the
Fenton reaction. A preliminary assessment of overall performance and feasibility of these
processes was demonstrated in this study. Performance based on engineering process param-
eters, environmental parameters, and economic and social parameters was examined to
complete a more robust study. A ranking system was used to compare these processes.
Ultimately, H2O2/O3 achieved the highest ranking at 3.45. O3, O3/UV, H2O2/UV, and the
Fenton process received comparable, though decreasing, average rankings (3.30, 3.08, 3.36,
and 2.89, respectively). The process receiving the lowest ranking in this study was TiO2
photocatalysis with a value of 2.11. However, these rankings are not an absolute indication of
advantage because some other parameters must be considered as more influential. Economic
and social parameters caused the most significant variation in scores due to electricity costs.
Both the strengths and weaknesses of each process were clearly displayed by the ranking
system. Overall, the need for additional research and testing was clear. This would help to
provide the additional support that newer technologies require, as well as improvements in
high electricity demands. It was also recognized that the system lacked necessary detail and
suffered from an inclusion of significant user bias. A weighted ranking system that includes
more levels of ranking, as well as the use of the opinions of multiple individuals, such as
practicing and industrial professionals, could alleviate some of these issues.
Critical Evaluation of Advanced Oxidation Processes

Acknowledgements This work was supported by the Department of Civil and Environmental Engineering
(CEE), the Bagley College of Engineering (BCoE), and the Office of Research and Economic Development
(ORED) at Mississippi State University.

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