From Removal to Recovery: An Evaluation of Antibiotics Removal
Techniques from Wastewater
Xilai Ma
BASIS International School Park Lane Harbour, China
Keywords:
Antibiotics Removal, Removal Mechanisms, Biological Wastewater Treatment Technology, Membrane
Bioreactor, Bioelectrochemical System, Constructed Wetland, Microalgae.
Abstract:
Due to the potential risks to human health and ecosystems, antibiotics contamination is an emerging
environmental concern. Currently, numerous technologies have been widely explored for the removal of
antibiotics from wastewater, including membrane bioreactor, biological process, bioelectrochemical system,
constructed wetland and microalgae. In this review, the fundamental mechanisms and removal efficiency of
such technologies were discussed. Besides, current challenges and further direction of the antibiotic removal
are present, in which the recovery of antibiotics was highlighted. Thus, a shift of antibiotics from the
removal to recovery would be a focus in the future for the sustainable development of society.
Graphical abstract
1
INTRODUCTION
Antibiotics are used in farming and medicine to
reduce harmful parasites in crops, and treat diseases
by bacterial infection in domesticated animals and
humans. Since its discovery in 1928 by Alexander
Flemin (K. Gould, 2016), there are now many types
of antibiotics such as sulphonamides, macrolides,
puinolones, cephalosporins and penicillin. Since the
1950s, people are using antibiotics on a massive
scale to treat diseases in poultry and livestock
production (E.K. Silbergeld, 2008). They are used to
promote the growth of the life stocks by being used
as feed additives in reducing the chances of animals
getting sick or kills harmful bacteria during fruit or
vegetable production (E.K. Silbergeld, 2008).
However, the overuse of antibiotics results in the
production of harmful chemicals. It was reported
that from 2000 to 2010, there was a 36% increase in
antibiotics usage in developing countries (Thung,
2016) and this exploitation of antibiotics has caused
the appearance of more potent pests that are resistant
to the antibiotics, causing more expensive medical
treatment, longer treatment period, and increased
death rates (Brown, 2016); (Liu, 2016). In a study, it
shows that there are about 58% of antibiotics left in
1138
Ma, X.
From Removal to Recovery: An Evaluation of Antibiotics Removal Techniques from Wastewater.
DOI: 10.5220/0011379100003443
In Proceedings of the 4th International Conference on Biomedical Engineering and Bioinformatics (ICBEB 2022), pages 1138-1144
ISBN: 978-989-758-595-1
Copyright
c
2022 by SCITEPRESS Science and Technology Publications, Lda. All rights reserved
the feces and urine of those humans and animals that
had consumed antibiotics (Zhang, 2015). Therefore,
it is crucial to look for a proper way of treating the
wastes, so people can prevent the runoff in the
livestock industry to pollute water and soil (Ma,
2015); (Lukaszewicz, 2017). Currently, the
technologies for removing antibiotics from
wastewater include biological process, adsorption,
membrane filtration, Fenton, redoxreaciton,
photolysis (Martinez, 2013); (Molinos-Senante,
2013). To find out a practical way to remove
antibiotics, the review paper takes a deep look into
the latest technology available for the antibiotics
removal. A comparison among those antibiotics
removal techniques was conducted. Besides, we
propose a possible solution to increase the feasibility
of antibiotics removal system.
Figure 1: Schematic diagram of antibiotic delivery chain.
Adopted from Song et al. (X. Song, 2021).
2 BIOLOGICAL PROCESS
In the biological process, it relies on the oxidation
by microbes to effectively decompose antibiotics.
Conventional activated sludge (CAS) is the most
popular method for the removal of antibiotics
through sludge adsorption. However, the method has
unstable performance and its removal efficiency
ranges from 90% to a negative percentage, which
indicates the antibiotics may build up in the reactor.
In CAP, the adsorption capacity depends on the
antibiotic’s hydrophobicity and chemical structure,
and the activated sludge’s property (Suto, 2017).
Compared to the CAS, the sequencing batch reactor
(SBR) is more advantageous due to its high
flexibility and simple structure and operation.
Similar to CAS, the efficiency of SBR depends on
property of antibiotics. Besides, hydraulic retention
time (HRT), sludge retention time (SRT), condition
for redox reaction and temperature can also
influence the removal of antibiotics, where HRT and
SRT are the most crucial factor (Yang, 2011).
Neyestani et al. (Neyestani, 2017) found that the
removal efficiency of trimethoprim (TMP) increased
from 19% to 71% as the SRT increased from 2 days
to 20 days.
Apart from this, anaerobic digestion (AD) is the
most efficient way to remove the antibiotics from
wastewater due to low energy input and the absence
of human intervention. Moreover, the temperature is
the most crucial factor affecting the removal
efficiency in the anaerobic digestion; for example,
Liu et al. (Liu, 2018) reported that the removal
efficiencies of tetracyclines (TCs) and
fluoroquinolones (FQs) from pig farms were higher
in summer than that in winter. It should be noted
here that the concentration of antibiotics in the AD
system may negatively affect its performance such
as hindering the production of CH4 and COD
removal. It was reported that the biogas production
was reduced by 10% due to the presence of 130mg/L
of tylosin, which is attributed to the inhibition of
oxidizing bacteria that produce methane by
antibiotics (Mitchell, 2013).
3 MEMBRANE BIOREACTOR
(MBR)
Membrane bioreactor (MBR) is a more high-quality
method for the removal of the antibiotic than
biological process due to its long SRT, higher cell
concentration, less sludge production and more
stable environment for microbial growth, which
integrates biological process with micro-filtration
(MF) or ultrafiltration (UF) (Cecconet, 2017). The
biodegradation of antibiotics can be enhanced by
higher microbial concentration and diversity. In
MBR, the removal efficiency of antibiotics can be
over 90%, including erythromycin, ofloxacin, TC,
ciprofloxacin (CIP), and chlortetracycline
(Cecconet, 2017); (Tiwari, 2017). For example, Xiao
et al. (Xiao, 2017) found that the anaerobic MBR
can achieve 94.2 ± 5.5% of TMP and 67.8 ± 13.9%
of sulfamethoxazole (SMX) being removed. It
should be noted that higher SRT favors the removal
of the antibiotic because this facilitates the growth of
slow-growing microorganisms and raises the
biodiversity of the microbial community, which has
positive impacts on the biodegradation of antibiotics.
From Removal to Recovery: An Evaluation of Antibiotics Removal Techniques from Wastewater
1139
4 BIOELECTROCHEMICAL
SYSTEM
For bioelectrochemical system (BES), it can not
only effectively remove antibiotics from wastewater,
but also generate electricity through redox reactions
performed by anaerobic bacteria at the anode
(Logan, 2009) and aerobic bacteria in the cathode by
the cellular respiration (Kumar, 2017); (Logan,
2012). The cellular respiration by anaerobic bacteria
at the anode chamber produces protons and
electrons, in which the proton can diffuse through a
proton exchange membrane to the cathode whilst
electrons can transfer by the external circuit to react
with the electron acceptor at the cathode for the
electricity generation. Microbial electrolysis cells
(MECs) and microbial fuel cells (MFCs) are the two
typical types of BESs which can achieve effective
removal of antibiotics with simultaneous energy
recovery.
The MFC has high antibiotic removal rate due to
its high activity of microbes. It was reported that
98% of β-Lactam antibiotics can be removed in
single-chambered MFC while two-chambered MFC
achieved over 80 % of TCs, quinolones,
chloramphenicol, sulfonamides and nitroimidazoles
being removed (Zhang, 2017); (Guo, 2016); (Zhou,
2018). In contrast to the MFC, additional power can
be applied in MEC, which facilitates the removal of
antibiotics. Increasing the applied voltage from 0 to
0.9 V resulted in enhanced removal of sulfadiazine
(SDZ) (Yang, 2018), which is attributed to the
improved biofilm formation and increased microbial
activity (Liu, 2015). Guo et al. (Guo, 2017) argued
that the microbial community can be manipulated by
additional power to make the system more suitable
for a certain kind of antibiotics. Furthermore,
biocathode are more effective at removing
antibiotics than abiotic cathode since the microbes at
the biocathode can gain electrons to boost the
electrochemical process (Liang, 2013). Excessive
concentration of antibiotics may also detrimentally
affect their removal efficiency in BES (Song, 2013);
for instance, Wang et al. (Wang, 2015) found that
increasing the concentration of SMX from 20 to 200
mg/L, its half-life increased from 1 to 3 d in the
MFC reactor.
5 CONSTRUCTED WETLAND
The removal of antibiotics by constructed wetland
(CW) relies on plants, microorganisms and
substrates which work together through
photodegradation absorption, microbial
decomposition and plant uptake (García, 2020);
(Gorito, 2017). Microbial decomposition plays a
crucial role in the removal of antibiotics in CW,
which depends on many different microbes, such as
the heterotrophic and autotrophic bacteria,
protozoan, and funguis (e.g., yeast, basidiomycetes)
(Liu, 2019). Biotransformation processes in treating
antibiotics heavily depend on their physio-chemical
properties, where antibiotics that have more similar
properties to naturally occurring organic molecules
can be fairly quickly decomposed and then
consumed by bacteria (Li, 2014). Besides,
antibiotics can be also destroyed directly through
photolysis, in which the radiation from light breaks
the bond cleavage, making the molecule no longer
harmful. Light intensity is an important factor
determining the rate of photodegradation while other
influencing factors include light frequency and the
chemical property of the surrounding water such as
pH and water hardness (Batchu, 2014).
Photosensitizers such as dissolved organic matter
(DOM), nitrate and nitrite can also indirectly
influence the photolysis of antibiotics (Jiang, 2010);
(Lin, 2005). The presence of DOM may inhibit the
removal of CIP via photodegradation, but have
positive impacts on the decomposition for
chlortetracycline, roxarsone, and SMX (Mangalgiri,
2017). The removal of antibiotics by substrate
adsorption is important, in which the antibiotics can
be adsorbed to the substrate such as sludge or the
surface of biofilm (Liu, 2020). In addition, some
antibiotics in CW can be taken up by plants with the
help of some specific xenobiotic transporters in the
plant cells (Liu, 2013); (Wu, 2015). According to the
difference in water flow, there are several types of
CW, including free water surface (FWS) flow
wetland, verticle subsurface flow (VSSF) wetland,
and horizontal subsurface flow (HSSF) wetland (L.
Liu, 2013).
6 MICROALGAE
Microalgae can effectively remove antibiotics by
bioadsorption, bioaccumulation, biodegradation,
volatilization and photodegradation (SHena, 2021);
(Leng, 2020); (Sutherland, 2019). Microalgae
integrated systems generally include closed
photobioreactors (PBRs) and open ponds (Hena,
2021), where suspension-based microalgae
cultivation is always involved. The classes and
concentrations of antibiotics highly affect the
ICBEB 2022 - The International Conference on Biomedical Engineering and Bioinformatics
1140
antibiotic removal by microalgae integrated system.
When the concentrations of antibiotics are higher or
close to tolerable level of microalgae, the microalgae
growth may be inhibited by antibiotics, thus
negatively affecting the antibiotic removal (Sun,
2017). However, increasing the antibiotic
concentration within the tolerable level of
microalgae may have insignificant impacts on the
antibiotic removal (Leng, 2020). Li et al. (Li, 2015)
argued that the tolerable concentration of
amoxicillin for C. pyrenoidosa ranges from 300 to
400 mg/L. Besides, microalgae C. pyrenoidosa can
achieve 83–100% of amoxicillin and 7–23% of
cefradine being removed while the two antibiotics
are at the same level (Li, 2015). This indicates that
microalgae may have different removal efficiency
for the different antibiotic kinds even they are at the
same level (Leng, 2020). Apart from this, the
microalgae growth is influenced by microalgae
growth inhibitors, dissolved oxygen, design of the
photobioreactor, salinity, CO2 concentration,
temperature, illumination, solution pH and nutrient
concentration, which in turn affects the antibiotic
removal by microalgae (Norvill, 2016). The increase
in the nutrient concentration is beneficial for the
microalgae growth metabolisms, which also has
positive impacts on the antibiotic removal; for
instance, the removal efficiency of CIP can be
increased by over 3 times while adding 4 g/L sodium
acetate to Chlamydomonas Mexicana cultures
(Xiong, 2017). Moreover, the solution pH is a
crucial factor affecting the antibiotic removal in the
microalgae integrated system since it may determine
the hydrolysis of some ionic antibiotics. Norvill et
al. (Norvill, 2017) found that alkaline pH favors the
removal of TC by microalgae while the pH ranging
from 6.3-8.0 may have negligible effects on the
removal of 7-ACA (Guo, 2016). The removal of
antibiotics can be also enhanced by strong light
irradiation, where reactive oxygen species can be
generated (Norvill, 2017).
7 FUTURE PERSPECTIVE
Currently, the risks of antibiotics have been widely
explored and many technologies have been
developed for their effective removal. Even though
bio-based processes could achieve effective
antibiotic removal, the stability and reliability of
bacteria are still a big challenge for their full-scale
applications. Therefore, the selection of appropriate
bacteria for biodegrading certain kinds of antibiotics
may be a possible solution to increasing the removal
performance of bio-based processes. For the MBR
and BES, membrane fouling is a big barrier to
maintain their performance. This is despite the fact
that anaerobic MBR and MFC can recover energy
through biogas and electricity production. Thus,
further development should focus on improving the
properties of membranes with low synthesis costs.
The antibiotic removal by CW and microalgae is
achieved by multiple mechanisms, so it is essential
to identify the specific removal mechanism for
certain kinds of antibiotics. Overall, the antibiotic
removal requires substantial input of energy and
chemicals. Compared to the antibiotic removal from
wastewater, the antibiotic recovery is more
promising and can create a circular economy
because the recovered antibiotics can be reused in
animal feed. As shown in Table 1, Pan et al. (Pan,
2015) utilized forward osmosis (FO) process with
thin film composite membrane for the recovery of
TC. In this scenario, more than 97% TC can be
rejected in the feed side of the FO process, which
produces the TC-rich streams for further use.
Similarly, Li et al. (Li, 2017) employed eggshell
membrane (ESM)-derived MgFe2O4 to adsorb
doxycycline (DC) with the maximal adsorption
capacity of 308 mg/g, after which acid treatment and
magnetic separation were conducted for the
adsorbent regeneration and DC concentration.
However, the technologies mentioned above for the
antibiotic recovery may not achieve high-quality
stream with rich antibiotics due to the presence of
other foreign substances, which may negatively
affect the further application of recovered
antibiotics. Thus, future research should aim to
develop technologies for recovering antibiotics with
high-quality products.
From Removal to Recovery: An Evaluation of Antibiotics Removal Techniques from Wastewater
1141
Table 1: Summary of technologies for antibiotic recovery from wastewater t-SNPs: thiol functionalized silica nanoparticles.
Technology Wastewater Antibiotic Efficiency Reference
Foam separation with t-snps Pharmaceutical
wastewater
streptomycin
sulfate
recovery rate at
90.1 ± 4.5%
Shu et al. (T.
Shu, 2018)
Forward osmosis process Synthetic wastewater TC 99% of TC being
concentrated
Pan et al. (S.-F.
Pan, 2015)
Membrane (RO-UF) filtration Oxytetracycline waste
liquo
r
oxytetracycline recovery rate over 60% Li et al. (S.-z.
Li, 2004)
gradient elution preparative
chromatography
Crystallization
mother-liquor streams
ertapenem 0.6·kg·ertapenem/d·kg·s
tationary phase
Sajonz et al. (P.
Sajonz, 2006)
Electrodialysis with
ultrafiltration membrane
Synthetic wastewater penicillin G− 20.3% of penicillin
G− concentrated
Lu et al. (H. Lu,
2016)
8 CONCLUSION
The review paper demonstrated the effectiveness of
several technologies for the antibiotic removal, in
which bio-based processes have been widely used
for the antibiotic removal. However, there are still
some challenges that need to be solved to further
improve the removal efficiency, such as how to
maintain the microbial community in the removal
processes. Besides, the antibiotic recovery is
preferred compared to the antibiotic removal, but
more research are needed to make it feasibly viable.
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