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A R T I C L E I N F O A B S T R A C T
Keywords: To deal with the contamination of the water environment, which represents an arena for microorganisms and
Photocatalysis antibiotics, a photocatalytic process has been proposed due to its high efficiency and non-toxicity. This review
Disinfection discusses and investigates antibiotics and antibiotic-resistant bacteria (ARB) removal and inactivation with their
Antibiotics
associated genes through photocatalysis technique as an efficient and ecofriendly advanced oxidation process
Antibiotic-resistant bacteria
Wastewater
(AOP) photocatalysis. The paper summarizes recent studies that dealt with both pollutants and their process
parameters, optimal operating conditions, used semiconductor photocatalysts and their corresponding removal
efficiency. Thus, it suggests that photocatalysis can offer impressive treatment efficiencies for both organic and
microbial pollutants simultaneously. The review also states that both antibiotics and bacteria have a destroying
effect against each other, where antibiotics have antimicrobial activity and bacteria have microbial degradation.
This phenomenon creates a hybrid system for each pollutant (photocatalysis-bacteria, photocatalysis-antibiotic,
bacteria-antibiotic), which accelerates the purification and disinfection of the polluted water caused by patho
gens and hazardous pollutants using green and safe technology. Moreover, the reaction mechanism was detailed
in order to define the role of reactive oxygen species (ROS). Likewise, photocatalysis coupling with other AOP
techniques in this context was discussed to achieve more promising results. The main contribution of this review
is to explain the relationship between antibiotics, microbial contaminants and photocatalysis. It also introduces a
new area of study and concludes with an outlook on future research topics, such as viral disinfection.
1. Context of water pollution products [12]. Within this rapid development in science and technology,
and with the new industrial processes and synthetic products continu
Water is our planet’s most crucial natural resource [1]. It is essential ously being developed [13], more and more contaminants are being
for all organisms in our lives. It covers about 71 % of the earth’s surface, produced and discharged into the environment [1]. The number of these
where 2.5 % are classified as freshwater [2], including a rare amount of contaminants and their concentrations in the water are growing
0.002 % considered as humanly accessible [3]. The rarity of this continuously [14]. Earth’s freshwater is continually polluted with
resource is further intensified with the increasing demand related to the different chemicals, such as pharmaceutical compounds [15]. Adding
natural changes endured by the globe or the consumptions linked to water to a mixture of drug trace amounts is potentially a crucial
human needs/activities [1,4–11]. emerging problem and is engineered to exhibit potent physiological
Among the highest water-consuming sectors, industries have grown activity [4]. Many pharmaceuticals are not substantially absorbed into
and developed within much of the world, and the emerging chemical the subsoil due to their polar structure. Then contaminants may be
industry has synthesized a multitude of previously unknown chemical transferred from the contaminated watercourses into groundwater
* Corresponding authors.
E-mail addresses: ajery@kku.edu.sa (A. El Jery), aymen.assadi@ensc-rennes.fr (A.A. Assadi).
https://doi.org/10.1016/j.jwpe.2021.102089
Received 24 January 2021; Received in revised form 10 April 2021; Accepted 12 April 2021
Available online 31 May 2021
2214-7144/© 2021 Elsevier Ltd. All rights reserved.
O. Baaloudj et al. Journal of Water Process Engineering 42 (2021) 102089
aquifers [4,16]. Urban wastewater is also considered a substantial cause increase globally and nearly double in South Africa, Russia, China,
of water pollution [16]. It is vulnerable to contamination due to its Brazil, and India between 2010 and 2030 [33]. Annual use of about 100,
too-high pollution levels and relatively low self-purification capacity 000–200,000 tons of antibiotics worldwide has been recorded [34].
[17]. As a result, water pollution in urban rivers in many countries is Hospitals are known as primary antibiotic distribution sources in
becoming a major environmental issue. municipal urban treatment units of wastewater [30]. Data from the
The contamination of the water presents potential risks to both Centers for Disease Control and Prevention (CDC) found that 55.7 % of
human health and the environment; it has direct and indirect damage to patients received antibiotics [34]. At the same time, they stay in hos
the health of all organisms [18,19]. Polluted water is the primary cause pitals from 325 hospitals in 2010, and 37.2 % of those antibiotic pre
of infectious diseases (e.g., Malaria and Cholera, Amoebiasis, Para scriptions were unnecessary or could be changed, which is consistent
typhoid Fever, Dysentery) [3]. Epidemics from contagious agents in with previous literature research on the use of antibiotics in acute care
potable water have already developed in most countries. Waterborne hospitals. For that, the CDC has initiated many health promotion pro
pathogens are now well handled using disinfectant agents. Regrettably, grams to target antibiotic resistance [35]. Antibiotics are commonly
the control of occurrence in the wastewater of the potentially hazardous used in the treatment of bacterial infections in both humans and ani
chemicals constitutes a very challenging job from the applied perspec mals. These are used in livestock processing, fish farming additives, and
tive. The regulation of water pollution and the improvement of sus poultry industries as growth promoters [36]. They are also used to
tainable water purification technologies are therefore necessary improve the quality of feed [37]. Because of their chemical composition,
solutions. The adoption of safe technological processes and the water the commonly used antibiotics can be categorized into six kinds: β-lac
reuse for various industrial activities are core issues for our society tams, quinolones, tetracyclines, aminoglycosides, macrolides, and sul
intending to maintain water supplies [1,5,21]. This problem has fates [38–41]. Most of these substances are poorly absorbed. Mainly,
received much attention in recent years and initiated many research 80–90% of the antibiotic is excreted into the water by wastewater
efforts, political and legal activities [20], and that attention appears to effluent [41]. As shown in Fig. 1, the extensive utilization of medical and
be increasing. Environmentalists worldwide have named the pharma veterinary antibiotics has resulted in the widespread occurrence of
ceuticals “emerging contaminants” (ECs) of the environment [21]. traces of these highly stable compounds in natural aquatic habitats all
Moreover, antibiotics are a significant concern for researchers world over the world, including rivers [42–44], lakes [40,43,44], groundwater
wide compared to other drug compounds groups as they are toxic and [45,46–49], seawater [40,41], and drinking water [30,47]. These traces
non-biodegradable [22]. have been proved difficult to be removed by conventional drainage
systems [50]. Due to the continuous discharge of wastewater, antibiotics
2. Antibiotics usually occur in the surface water as mixtures at various concentrations
from a few ng/L to a high μg/L [51,52].
Antibiotics are either natural or human-made substances that can
destroy or prevent bacteria from developing [23]. They are widely used 3. Photocatalytic removal of antibiotics
for the sake of the rescue of many lives. to avoid and cure infectious
diseases and pathogens. They have substantial physical and chemical Since the late 20th century, studies have been published on sources,
properties which make it hard to remove the aquatic environment as incidents, fate, and dangers of antibiotics in aquatic environments.
their existence may increase aquatic toxicity [24,25]. They are the pri These papers typically gave a regional viewpoint, summed up world
mary concern and hazards in pharmaceutical products because they are wide studies’ data, and exposed the lack of knowledge regarding anti
extensively applied and have negative impacts on useful and nontarget biotics’ toxicological effects in ecosystems example [30,47,52–62].
microbiota of the biological system [26,27]. Their association with However, some studies introduced a critical review on removing anti
growing and rapidly growing antibiotic resistance make them one of the biotics from polluted waters through various treatment methods
three most important threats to the World Health Organization (WHO) [63–73]. The conventional approaches can not remove antibiotic resi
[28–30]. Furthermore, antibiotics can cause many genetic effects in dues in polluted waters effectively [74–76]. On the other hand,
humans, for example, allergic reactions [31]. An analytical study of advanced oxidation processes (AOPs) have shown promising results and
observational data evaluating the antibiotics’ use over the 15 years in 76 proved a suitable solution for quick deterioration of recalcitrant and
countries showed a 65 % rise between 2010 and 2015 [32]. It can also non-biodegradable substances in water, such as antibiotics. The
Fig. 1. Human and veterinary environmental sources and transportation of antibiotics by Christine Klein [53].
2
O. Baaloudj et al. Journal of Water Process Engineering 42 (2021) 102089
3
O. Baaloudj et al. Journal of Water Process Engineering 42 (2021) 102089
Table 1 (continued ) • Bacteria of streptococcal disease cause many different body in
Target pollutants Catalyst Operating conditions Degradation Ref fections, including meningitis, ear infections, pneumonia, and strep
efficiency throat [93].
initial concentration:
15 mg/L MRSA (Methicillin-resistant Staphylococcus aureus) is a gram-positive
Catalyst dosage: bacteria of the family Firmicutes [108]. It is the most well-known of
1.0 g/L the Superbugs, which caused 72 444 invasive infections in the United
pH: 5, reaction time:
States and 9194 deaths in 2014 [107]. Superbugs’ resistance to drugs
Ciprofloxacin TiO2 30 min 100 % [87]
initial Ciprofloxacin may also be based on mutation or the development of resistance genes
concentration: from other bacteria [93]. Since antibiotics are widely used, our bodies
105 mg/L no longer rely on our immune systems any longer, making us unable to
Catalyst dosage: deal with new bacteria.
1.5 g/L
pH: 10, reaction time:
Metronidazole ZnO 180 min 96.55 % [88] 5. Photocatalysis inactivation of bacteria in water
initial Metronidazole
concentration: Despite attempts to develop new antibiotics, antibacterial resistance
80 mg/L
is still growing too rapidly to keep up with drug development. However,
pH: 11, reaction time:
180 min Advanced Oxidation Processes (AOPs) have provided an acceptable rate
NF-TiO2 of bacterial inactivation. AOPs are safer and natural technology for
Oxytetracycline initial SMX 92 % [89]
film
concentration: 5 mg/ water disinfection, unlike conventional water disinfection methods like
L chlorination, ozonation, and ultraviolet irradiation [109]. They have
many disadvantages as they present high investments, maintenance
costs, large consumption of chemical reagents and environmental
problems created by disposal of the waste effluent after treatment.
Indeed, the chlorination process leads to the development of carcino
genic by-products such as trihalomethanes (THM) [110]; for ultraviolet
irradiation, many microorganisms can resist it. For ozonation, the cost
and security concerns restrict its use in practice [109]. Using these
methods can also lead to developing very undesirable and toxic disin
fection by-products [111].
Among the different AOPs, Photocatalysis has become a safe and
successful green photochemical mechanism [112]. It has long been used
to combat pathogenic bacteria [113]. Several papers verified that the
bacterial envelope is the primary target of the photocatalysis process,
leading to membrane permeability modifications and cell death
[114–116]. The photocatalytic process can also use for the inactivation
of viruses [111,112]. Semiconductors like TiO2 are known to generate
Fig. 2. A schematic diagram for the proposed mechanism of organic pollut microbicidal, reactive oxygen species in the presence of light [117]. In
ants [15]. 1985 [118], identified the first microbicidal activity study on TiO2
photocatalysis. Over the last two decades, there have been many
appealing photocatalytic applications for drinking water disinfection
new antibiotics [98]. This phenomenon caused a drastic environmental
[119]. In which process lead to the antibiotic-resistant bacteria inacti
change, a toxic shock to the bacterial world [92]. In the case of disease,
vation. Table 2 summarizes a list of bibliographical references on pho
combining antibiotics is used for controlling ABR, which is the most
tocatalytic studies for the Inactivation of ARB in water.
significant danger that threatens modern medicine [99]. Both bacteria
We can conclude from the results of the table that the catalysts have a
and viruses are responsible for some of the deadliest diseases in history
great ability to inactivate bacteria of all kinds in the water. This makes
[100]. Bacteria that are antibiotic-resistant with their genes represent
them a suitable solution to get rid of those harmful organisms. This
one of the most severe and intense challenges of the twenty-first century
mechanism can be explained in Fig. 3 which illustrated a proposed
[101]. They are well-known “easy-to-get, hard-to-lose” pollutants [102].
disinfection mechanism of the photocatalyst. As already discussed in the
They can easily be transmitted to humans and animals through the
photodegradation part that when the light of suitable wavelength is
horizontal transmission of genes in a water environment that poses a
irradiated on the catalyst, the conduction band (Cb) and valence band
significant risk [103]. Actually, a conservative estimate by the CDC in
(VB) of this photocatalyst tend to bend, and a depletion layer is formed
dicates that antibiotic resistance more than two million people in the US
around the interface. Making e− in the VB excited to move to CB
get sick from antimicrobial-resistant causes 700,000 deaths globally
simultaneously produced the same amount of h+ in the VB. The electron-
each year [104]. A study [105] suggests that the world’s foremost cause
of death will be antibiotic-resistant infections in 2050. The most com hole pairs (e− and h+ ) can interact with HO2 and OH(e− ) to create OH∗ ,
mon disease caused by ABR are: while O2 generate O2 − ∗ by electron-accepting with O2 H∗ to form H2 O2
and OH∗ . ROS (OH∗ , O2 H∗ , H2 O2 , and O2 − ∗ ) can produce high oxidative
• Mycobacterium tuberculosis infections, approximately two billion stress and interact strongly with bacterial cells and kill them by
people are infected with the bacterium that causes this disease [97]. degrading the cell wall and several types of bacterial cell contents like
• Strains of Neisseria gonorrhoeae were recently resistant to third- protein, lipids, carbohydrate, DNA and amino acids [129]. Moreover,
generation carbapenems. They lead to several untreatable gonor photocatalyst molecules can interact with bacterial cells by depositing
rhoea infections in the UK [106]. them on the surface through the mechanism of cellular proliferation and
• Staphylococcus aureus causes a range of body infections, including endocytosis, resulting in the destruction of membrane proteins or cell
boils, injury infections, toxic shock syndrome, cellulite, abscesses, membranes through the phenomenon of organ permeability. Both
pneumonia, and food poisoning [107]. semiconductor particles and ROS can disturb the transport of electrons
4
O. Baaloudj et al. Journal of Water Process Engineering 42 (2021) 102089
kansasii and
TiO2-Ag reaction time: 240 min 99.9 % [128] extremely powerful (potent) oxidants of organic pollutants because they
Mycobacterium
initial bacterial cells:
avium
5 × 108 CFU/mL
can destroy the bonds of stable and unreactive organic molecules to form
the temperature: 35 ◦ C organic intermediates that can be further degraded into CO2 and H2O
Catalyst: 2 wt % Pd/ [132]. On the other hand, they can damage microorganisms without
BiFeO3 further adding chemical oxidants by attacking and breaking the cell wall
Pd- Dose: 1 g/L
Enterococcus making microorganisms become inactive or dead and denature proteins,
loaded reaction time: 240 min 98%-100 % [79]
faecalis
BiFeO3 initial bacterial cells: finally resulting in various end-products [119]. Both mechanism pho
107 CFU/mL todegradation of organic pollutants and bacterial inactivation is illus
the temperature: 37 ◦ C trated in Fig. 4. Furthermore, Eqs. 13 to 17 suggest the basic process of
photocatalytic degradation and water pollutants’ disinfection.
5
O. Baaloudj et al. Journal of Water Process Engineering 42 (2021) 102089
Table 3
Catalysts for bacteria inactivation as well as antibiotics degradation.
Target bacteria Target pollutants Catalyst Photodegradation Photocatalytic disinfection Ref
6
O. Baaloudj et al. Journal of Water Process Engineering 42 (2021) 102089
Fig. 4. Mechanisms of the organic and microbial pollution photocatalytic removals [114].
H2 O + h+ → OH∗ + H+ (14)
O2 + e− → O2 − ∗
(15)
7
O. Baaloudj et al. Journal of Water Process Engineering 42 (2021) 102089
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