Current Research Trends On Microplastic Pollution From Wastewater Systems: A Critical Review

Rev Environ Sci Biotechnol (2019) 18:207–230
https://doi.org/10.1007/s11157-019-09498-w(0123456789().,-volV)
(0123456789().,-volV)
REVIEW PAPER
Current research trends on microplastic pollution

from wastewater systems: a critical review
Yulin Hu . Mengyue Gong . Jiayi Wang . Amarjeet Bassi
Published online: 13 April 2019

Ó Springer Nature B.V. 2019
Abstract Microplastics have been widely consid- fate of microplastics during wastewater treatments and
ered as contaminants for the environment and biota. the environmental contamination of effluent to envi-
Till now, most previous studies have focused on the ronment are presented. Previous studies reported that
identification and characterization of microplastics in the advanced wastewater treatment (e.g., membrane
freshwater, sea water, and the terrestrial environment. bioreactor) is needed for improving the removal
Although microplastics have been extensively efficiency of small-sized microplastics (\ 100 lm).
detected in the wastewater, research in this area is Although the role of microplastics as transport vectors
still lacking and not thoroughly understood. To fill this for persistent organic pollutants (POPs) is still under
knowledge gap, the current review article covers the debate, they have demonstrated abilities to absorb
analytical methods of microplastics originating from harmful agents like pharmaceuticals.
wastewater streams and describes their sources and
occurrences in wastewater treatment plants (WWTPs). Keywords Microplastics Wastewater systems
Studies indicated that microplastic pollution caused by Analytical techniques Wastewater treatment plant
domestic washing of synthetic fibers could be detected Environmental contamination
in the effluent; however, most microplastics from
personal care and cosmetic products (PCCPs) can be
Abbreviations
efficiently removed during wastewater treatment.
ATR Attenuated total reflectance
Moreover, various techniques for sampling and ana-
CaCl2 Calcium chloride
lyzing microplastics from wastewater systems are
FTIR Fourier-transform infrared spectroscopy
reviewed; while, the implementation of standardized
Fe Iron
protocols for microplastics is required. Finally, the
FeSO4 Iron (II) sulfate
FPA Focal plane array
Y. Hu (&) M. Gong J. Wang A. Bassi H2O2 Hydrogen peroxide
Department of Chemical and Biochemical Engineering, HNO3 Nitric acid
University of Western Ontario, London, ON N6A 5B9, HDPE High density polyethylene
Canada KOH Potassium hydroxide
e-mail: yhu268@uwo.ca
KI Potassium iodide
M. Gong NaCl Sodium chloride
School of Food Science and Technology, Jiangnan NaI Sodium iodide
University, Wuxi 214122, Jiangsu, People’s Republic of POP Persistent organic pollutant
China
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208 Rev Environ Sci Biotechnol (2019) 18:207–230
PCCP Personal care and cosmetic product persistent organic pollutants (POPs) due to their large
PE Polyethylene specific surface areas; and (3) they may be potentially
PEST Polyester ingested by fish and other living organisms (Jiang
PVC Polyvinyl chloride 2017; Wang et al. 2018a). Previous literature has
PS Polystyrene stated that the microplastics can be detected in all
POM Polyoxymethylene environmental systems and biota, such as rivers, lakes,
PP Polypropylene oceans, sediments, marine animals, and soils (Ng and
PET Polyethylene terephthalate Obbard 2006; Vianello et al. 2013; Cheung et al. 2018;
PC Polycarbonate Pellini et al. 2018; Rodrigues et al. 2018; Scheurer and
PU Polyurethane Bigalke 2018; Xiong et al. 2018).
PEVA Poly(ethylene–vinyl acetate) Until now, most recent reviews have focused on the
PA Polyamide microplastics in the freshwater, ocean, and terrestrial
Py–GC/ Pyrolysis–gas chromatography/mass environments (Andrady 2011; Cole et al. 2011; Wright
MS spectrometry et al. 2013; do Sul and Costa 2014; Barboza and
PO Polyolefin Gimenez 2015; Anderson et al. 2016; Duis and Coors
PAH Polycyclic aromatic hydrocarbon 2016; Auta et al. 2017; Alimi et al. 2018; He et al.
PCB Polychlorinated biphenyl 2018; Li et al. 2018a; Mai et al. 2018; Rezania et al.
SPT Sodium polytungstate 2018; Wang and Wang 2018; Wang et al. 2018b;
TGA– Thermogravimetric analysis–differential Xiong et al. 2018; Castro et al. 2018; Chae and An
DSC scanning calorimetry 2018; Fahrenfeld et al. 2019; Koelmans et al. 2019;
UV Ultraviolet Stock et al. 2019; Strungaru et al. 2019; Triebskorn
WWTP Wastewater treatment plant et al. 2019; Barletta et al. 2019). Whereas, based on the
WPO Wet peroxide oxidation previous studies, a high concentration of microplastics
ZnCl2 Zinc chloride is often found in the effluent and sludge from
wastewater treatment plants (WWTPs) and the incom-
plete removal of these microplastics might cause
pollution in the receiving water (Estahbanati and
1 Introduction Fahrenfeld 2016). So far, only a few review articles
have discussed the microplastics in wastewater sys-
Microplastics, commonly defined as plastics smaller tems (Morris et al. 2017; Burns and Boxall 2018; Kang
than 5 mm in diameter, are ubiquitous in various et al. 2018; Prata 2018; Raju et al. 2018; Sun et al.
aquatic and terrestrial environments and biota (Han- 2019; Ziajahromi et al. 2016). In addition, no review
vey et al. 2017; Alimi et al. 2018). This microplastics has summarized the current analytical approaches
pollution could affect both the food chain and human including sampling, extraction, and characterization
health (Barboza et al. 2018; Carbery et al. 2018; used for microplastics present in the wastewater
Waring et al. 2018). In general, according to the routes systems. Therefore, in this article, a comprehensive
in which they are generated, the microplastics can be review of microplastics originating from wastewater
broadly classified into: (1) primary microplastics systems is presented.
originating from everyday use products (e.g., facial
cleansers, scrubbers, and tooth paste) and (2) sec-
ondary microplastics are caused by the fragmentation 2 Sources of microplastics in WWTPs
of large plastics into small debris through photo-
oxidation, mechanical, chemical, or biological inter- 2.1 Personal care and cosmetic products (PCCPs)
actions (Li et al. 2016; Auta et al. 2017).
In recent decades, the pollution by microplastics in Currently, the natural exfoliating materials such as
both aquatic and terrestrial environments is of growing walnut husk, pumice, and apricot in the facial cleanser
global concern, owing to: (1) poor degradability and have been substituted by microplastics. In the indus-
thus leads to accumulation; (2) the possibility to sorb try, the term ‘microbeads’ is usually used to describe
the existence of microplastics as ingredients in the
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Rev Environ Sci Biotechnol (2019) 18:207–230 209
PCCPs (Napper et al. 2015). Based on the American authors reported that the particle size of microbeads
Academy of Dermatology, polyethylene (PE) was in the range of 24–800 lm. In addition, it was
microbeads are often applied in the facial cleansers, observed that the average amount of microbeads
owing to their smoothness in nature and thus leads to detected was between 5219 microbeads/gproduct and
less damage and redness to the skin (Chang 2015). It is 50,391 microbeads/gproduct. Additionally, the predom-
worthwhile to mention that the majority of microplas- inant shape of the microbeads from facial cleansers
tics resulting from PCCPs can be removed by was irregular. In another study, Kalčı́ková et al. (2017)
conventional wastewater treatments and the most characterized the microbeads in the body washes and
frequently detected microplastics in the effluent are facial cleansers, and the size of most microbeads was
fibers and fragments rather than microbeads. The less than 100 lm. Besides, a higher abundance of the
images of microplastics extracted from commercially larger sized microplastics was found in the body
available PCCPs are shown in Fig. 1 (Carr et al. 2016). washes, while, in contrast, facial cleansers contained
mostly smaller sized microplastics. The average
2.1.1 Characterizations concentration of PE in the body washes (4.82 gparti-
cles/100 mL) was considerably higher than that
Fendall and Sewell (2009) identified and characterized observed in the facial cleansers (0.74 gparticles/
the microplastics from four commercially available 100 mL). Table 1 summarizes the recent studies
facial cleansers, and the size of the most extracted investigating the microplastic pollution caused by
microplastics was observed to be smaller than PCCPs.
0.5 mm. In addition, all microplastics in the facial
cleansers showed various irregular shapes. Chang 2.1.2 Estimated releasing amount
(2015) characterized the PE microbeads in the facial
exfoliating cleansers, such as size, color, and concen- Kalčı́ková et al. (2017) estimated the daily emission of
tration. The results showed that the average size of microbeads originating from cosmetics, and around
microbeads was between 60 and 800 lm in diameter. 15.2 mg/person can be released every day. Besides,
Besides, most microbeads were found to be white and based on a 52% removal efficiency of microbeads by a
opaque. Cheung and Fok (2017) extracted the biological WWTP, about 1,125,500,000 particles/day
microbeads from nine different commercially avail- of PE microbeads could be discharged to the receiving
able facial cleansers from mainland China, and the river, which leads to the concentration of microbeads
Fig. 1 Images of microplastic samples extracting from commercially available cosmetics and personal care products (Carr et al. 2016)
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Table 1 Recent studies on microplastic pollution originating from personal care and cosmetic products
Sources Size (lm) Shape Color Polymer type References
Facial \ 500 Ellipse; rod; thread; granular Blue; orange – Fendall and
cleansers Sewell
(2009)
Facial 60–800 Uniform; granular White; opaque – Chang (2015)
cleansers
Facial 80–186 Irregular (mainly granular) White; orange; dark PE; LDPE; Cheung and
cleanser blue; light blue; Wax; Luwax; Fok (2017)
opaque PVC
Facial 100 Irregular White; red; blue; brown PE Kalčı́ková
cleanser; et al. (2017)
body wash
Facial 313 ± 130 Round; spherical; ellipse; filament; White; opaque PE Lei et al.
cleanser long stripe; grape-shaped; fragment (2017)
Shower gel 422 ± 185
to be 21 particles/m3. Cheung and Fok (2017) reported when considering the large quantities of microplastic
that approximately 209.7 trillion microbeads (equiv- pollution originating from PCCPs.
alent to 306.9 tonnes) originating from facial cleanser
might be released into the aquatic environment in 2.2 Synthetic fibers
mainland China on an annual basis. van Wezel et al.
(2016) employed a mathematic model [Eq. (1)] to Microfibers as secondary microplastics that results
estimate the amount of microplastic pollution caused from the synthetic polymers in garments are consid-
by PCCPs. According to three different emission ered to be the most prevalent type of microplastic
scenarios including minimum, average, and maxi- pollution in the environment (Gago et al. 2018).
mum, the estimated concentration of microplastics Similar to microbeads, microfibers can be detected in a
was 0.2 lg/L, 2.7 lg/L, and 66 lg/L in the final variety of environmental systems. Additionally,
effluent, respectively. microfibers could accidentally be ingested by living
organism and hence enter the food chain and harm
Cmp Uprod ð1 Fwt Þ Fpen
PECeff ¼ ð1Þ human health. Except for entering the aquatic envi-
Winf
ronment, microfibers can also be discharged into the
where PECeff and Cmp represents the predicted con- terrestrial soils through the application of sludge as a
centration of microplastics in the final effluent (gmi- fertilizer (Hartline et al. 2016). During conventional
croparticle/Leffluent) and the concentration of domestic washing of synthetic fibers, thousands of
microplastics in a commercial product (gmicroparticle/ microfibers can be released and the resulting washing
gproduct), respectively. Uprod is the usage of the product effluent is either released to the soils or to WWTPs
on a daily basis (g per capita per day) and Fwt is the through sewers (Browne et al. 2011). According to
fraction of microplastics removed by wastewater previous literature, approximately 35% of the
treatments. In addition, Fpen and Winf represents the microplastics identified in the aquatic environment
market penetration of products containing plastic might be released from synthetic fibers during washing
microbeads and the amount of wastewater generated (Prata 2018). Table 2 summarizes the recent studies
on a daily basis (L per capita per day), respectively. on microplastic pollution resulting from the domestic
Although some regulations have been introduced washing of synthetic fibers.
by the government to monitor the amount of
microplastics applied as ingredients in the PCCPs,
the alternatives to microbeads must be developed
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Table 2 Recent studies on microplastics pollution resulting from domestic washing of synthetic fibers
Synthetic fabric types Main conclusions References
Polyester-cotton blend Loss of fiber decreased with increasing times of wash Napper and
Polyester Polyester-cotton blend led to the lowest fibers Thompson
(2016)
Acrylic More fibers were released when using conditioner or detergent
Plain weave polyester Woven polyester released the highest amount of microfibers De Falco et al.
Double knit jersey polyester The use of softner led to the lowest amount of microfibers release (2018)
Plain weave polypropylene Powder detergent, high temperature, higher water hardness, and
mechanical action increased microfibers release
100% polyester interlock The use of detergent was the most important factor affecting microfibers Hernandez et al.
Plain singlt kit jersey polyester and release (2017)
2% Spandex plating The length of fiber (100–800 lm) was not affected by the washing
conditions and fabric type
Polyester The highest fibers release was from polyester-elastane blend, followed Sillanpää and
Polyester-elastane blend by cotton Sainio (2017)
Cotton The thickness and length for most microfibers was 20 lm and
100–1000 lm, respectively
Polyester Polyester fleece fabrics released the highest number of microfibers (7360 Carney Almroth
Polyacrylic fibers/m-2/L-1 in one wash) et al. (2018)
Polyamide High twist yarns are preferable for reducing microfibers releasing
2.2.1 Effects of washing conditions on the estimated washing parameters (temperature, time, water hard-
releasing amount ness, and mechanical action), and industrial washes on
the release of microfibers were examined. The use of
Napper and Thompson (2016) investigated the effects detergent led to an increase in the microfibers release.
of washing temperature (30–40 °C), detergent, and Specifically, the release of microfiber considerably
conditioner on the quantity of microfibers releasing increased from 162 ± 52 microfibers/g of fabric to
from polyester (PEST), acrylic, and PEST-cotton 1273 ± 177 or 3538 ± 664 microfibers/g of fabric
during laundering. In the case of PEST, the amount when using liquid or powder detergent, respectively.
of microfiber loss gradually reduced from 2.79 mg at This increase might be due to the inorganics (i.e.,
1st wash to 1.63 mg at 5th wash, which was similar to zeolite) in the detergent, which could cause friction
the trend observed for acrylic and PEST-cotton. The with synthetic fabrics in the process of domestic
result could indicate that old garments release fewer washing. Another reason could be related to the high
microfibers than new clothing. In addition, the usage pH value of detergent, especially when using powder
of conditioner and detergent significantly affected the detergent, since the alkaline detergent is able to
amount of fibers released. Clearly, more fibers would damage the surface of PEST fabrics through slow
be released during washing in the presence of deter- surface hydrolysis. A similar observance was reported
gent and conditioner. Based on the assumption of 6 kg by Hernandez et al. (2017), in which the use of
of washing load, the authors estimated that the amount detergent was observed to be the most important factor
of microfibers caused by the washing of PEST, acrylic, affecting the total mass of microfibers released.
and PEST-cotton fabrics was 496,030, 728,789, and Besides, a greater level of microfibers releasing was
137,951 fibers, respectively. achieved by applying higher temperatures, washing
In another study, De Falco et al. (2018) quantified times, and water hardness in the washing process. The
the released microfibers from three different types of higher washing temperature may accelerate the slow
synthetic fabrics during domestic washing, and the surface hydrolysis of PEST fabrics in the presence of
highest releasing extent of microfibers was found in alkaline detergent, and this extent of chemical damage
the woven PEST. Moreover, the effects of detergents, of fabrics can be increased by using a longer washing
123
time. The utilization of hard water triggers the 3.1 Container collection and pumping coupled
abrasion to PEST during domestic laundering. Addi- with filtration
tionally, an estimation of 6,000,000 microfibers can be
generated after domestic washing when based on an Even though sampling collecting by container is easy
assumption of 5 kg wash load of PEST fabrics. to operate, only a limited amount of wastewater can be
Carney Almroth et al. (2018) evaluated the amount sampled. As a result, container collection is desirable
of microfibers released from three common synthetic for the influent of WWTPs due to the high concentra-
materials (acrylic, nylon, and PEST) under varying tion of organic materials and solids (Talvitie et al.
washing conditions, and it was observed that PEST 2017b). Magnusson et al. (2014) adopted a Ruttner
fleece fabrics produced the highest amount of micro- sampler consisting of a cylinder which is immersed
fibers during washing. The authors also reported that into the wastewater and closed with a plummet. The
the amount of microfibers shredded in laundering was wastewater sample was then transferred into a stain-
dependent on the yarn and needle gauge. Specifically, less steel filter holder with a mesh size of 300 lm,
a higher release degree of microfibers was obtained followed by vacuum filtration.
when washing tightly knitted PEST fabrics. The aging On the contrary, sampling by separate pumping
of clothing was found to be another significant factor coupled with filtration can be used for the collection of
affecting the release of microfibers in domestic hundreds liters of wastewater, thereby making it
washing, and the use of aged clothing resulted in favorable for sampling the effluent of WWTPs. A
higher masses of microfibers than that obtained from newly designed sampling method using a mobile
new clothing. pumping device was developed by Mintenig et al.
In addition, the effect of number of wash cycle on (2017), as shown in Fig. 2. This sampling device is
microplastics releasing was investigated by Sillanpää composed of a flexible PVC hose connected with a
and Sainio (2017), in which four different types of weighted end-piece, membrane pump, flow meter, and
PEST textiles and two garments of cotton were a filter housing containing stainless steel cartridge
evaluated. The authors found that the amount of filter (mesh size: 10 lm). Prior to sampling, the
released microfibers reduced from 2.1 9 105– pumping system of the device was flushed with
1.3 9 107 microfibers/kg fabrics into one tenth by wastewater for 5 min. Afterwards, the weighed end-
fifth washes, which was in agreement with the results piece was placed below the surface of wastewater
reported by Napper and Thompson (2016). (* 10 cm) to collect the sample.
In conclusion, it is very difficult to control and Ziajahromi et al. (2017) developed a sampling
monitor the releasing amount of microfibers due to device (Fig. 3) that contains four stainless steel mesh
their prevalence in our daily life. Additionally, the screens with a size of 25, 100, 190, and 500 lm,
interaction between microfibers and sediment/plank- respectively, for the identification and characterization
ton has been reported, causing accidental ingestion of of microplastics in the effluents. As depicted in Fig. 3,
microfibers by animals and thus enters the food chain all mesh screens were stacked on top of each other, and
(Gago et al. 2018). Thus, appropriate regulations for the one with the largest size was placed on the top. The
controlling the amount of microfiber released by stacked mesh screens were sheltered by a cover made
domestic washing must be established. of polyvinyl chloride (PVC), and a baffle was placed
inside the inlet to ensure an even distribution of
sampled wastewater. This sampling device has two
3 Sampling approaches main advantages: (1) provides an in-situ division of
microplastics, which is performed based on their size
Until now, different sampling methods have been distribution; and (2) a large volume of sample can be
employed for collecting microplastics-containing treated continuously. The recovery efficiency of
wastewater, including container collection, pumping polystyrene (PS) microplastics obtained by this sam-
coupled with filtration, surface filtration, and autosam- pling technique was observed to be 92% when using a
pler collection (Sun et al. 2019). Table 3 summarizes 25 lm mesh screen, and the adoption of 500 lm mesh
the sampling approaches from recent studies on screen led to a 99% recovery efficiency. This obser-
microplastics present in the wastewater streams. vance might suggest that it is effective for capturing
123
Table 3 A summary of sampling approaches adopted for collecting microplastic samples originating from wastewater systems
Methods Location Device Lowest References
mesh size
Container collection
Glasgow 10 L of steel buckets 65 lm Murphy et al.
(2016)
Derby Telescopic sampling tool 0.2 lm Tagg et al.
(2015)
Lysekil Ruttner sampler 300 lm Magnusson
et al. (2014)
Vancouver Glass jar 1 lm Gies et al.
(2018)
Kenkäveronniemi 10 L stainless steel bucket 0.25 mm Lares et al.
(2018)
South Korea 100 L UV sterilization tank 106 lm Lee and Kim
(2018)
Northern Italy Steel bucket 63 lm Magni et al.
(2019)
Pumping coupled with filtration
Lysekil Filter holder made from plankton net and a suction pump 300 lm Magnusson
et al. (2014)
Northern A set of Tyler sieves and an extraction pump 0.125 mm Mason et al.
California (2016)
Western New York
Eastern New York
Central New York
Eastern Wisconsin
Oldenburg Custom made mobile membrane pump 10 lm Mintenig et al.
(2017)
Helsinki A specific filtering assembly with an electric pump 20 lm Talvitie et al.
(2017b)
Sydney A stacked units consisting of several stainless steel mesh screens 25 lm Ziajahromi
et al. (2017)
Los Angeles A stacked units consisting of several stainless steel mesh screens 20 lm Carr et al.
County (2016)
East Bay A stacked units consisting of several stainless steel mesh screens 0.125 mm Dyachenko
et al. (2017)
Surface filtration
Los Angeles A surface filtering assembly designed for skimming the water – Carr et al.
County surface at effluent discharge outfall (2016)
Autosampler collection
Helsinki Automated sampler (ISCO 3700) 20 lm Talvitie et al.
(2017b)
Adana Endress ? Hauser ASP-Station 2000, vacuum system RPS20 55 lm Gündoğdu et al.
model sampler (2018)
123
applied during sampling period. Nevertheless, sam-

pling by surface filtration has several limitations that
are required to be addressed: (1) is only applicable at
water falls; and (2) the airborne contamination can not
be eliminated as the surface filtration unit should be
placed in an open channel. Additionally, the amount of
microplastics can be underestimated by surface filtra-
tion since skimming the water surface might only
collect the low-density microplastics (Sun et al. 2019).
In general, based on the current studies on wastew-
ater sampling, we found that the most used are
container collection and pumping coupled with filtra-
tion. In the case of collecting effluent samples,
Fig. 2 A newly designed mobile pumping system for sampling pumping coupled with filtration is a favorable sam-
(Mintenig et al. 2017) pling technique as a large amount of samples can be
taken. On the other hand, for the microplastics present
microplastics with a wide range of particle sizes. More in the sludge, the most commonly adopted method is
importantly, no contamination caused by sampling described as follows: the sludge samples can be
process can be found. directly collected in a beaker/glass jar and then stored
in a refrigerator/cooler (i.e., - 4 °C) prior to analysis
3.2 Surface filtration (Gies et al. 2018).
Surface filtration is an highly effective sampling 3.3 Contamination

technique for collecting thousands of cubic meters of
wastewater. As depicted in Fig. 4, a surface filtration It is significant to avoid contamination throughout the
unit for sampling was developed by Carr et al. (2016), whole experiment. Mintenig et al. (2017) adopted
which can be used for skimming the water surface at several steps to reduce contamination, such as: (1) all
the effluent discharge outfall. Based on the flow rate
lab materials were rinsed using ultrapure water and
and water quality, different deployment times were
Fig. 3 A stacked sampling

device with four different
mesh sizes (Ziajahromi et al.
2017)
123
Fig. 4 A surface filtering assembly used for collecting microplastics-containing wastewater system (Carr et al. 2016)
30% ethanol; (2) all samples and lab materials were Except that, other solutions like sodium poly-
covered by aluminium foil to minimize airborne tungstate (SPT) solution, zinc chloride (ZnCl2), cal-
contamination; and (3) the limited use of plastic cium chloride (CaCl2), and sodium iodide (NaI)
materials during the experiment. Additionally, the solution have exhibited their effectiveness for the
blank experiments must be conducted in order to extraction of microplastics (Corcoran 2015; Stolte
control the airborne contamination (Gies et al. 2018). et al. 2015; Coppock et al. 2017; Crichton et al. 2017).
Briefly, a membrane filter is placed in a petri dish For example, Mahon et al. (2017) adopted 1 M ZnCl2
without a cover in the area where the experimental solution to separate microplastics from three effluents
work is carried out, followed by microscope analysis. samples after treatment by lime stabilization, anaer-
obic digestion, or thermal drying. Whereas, the oily
appearance was observed in the samples obtained after
4 Pre-treatment lime stabilization, making this density separation
method undesirable for extracting microplastics. In
4.1 Density separation addition, the high cost and toxicity of the above
solutions represent barrier for their practical applica-
The extraction of microplastics from liquid is com- tions. Table 4 summarizes the different solutions
monly achieved through density separation which adopted in the density separation of microplastics
involves the mixing of a liquid of defined density with originating from wastewater systems.
the sample. The saturated sodium chloride (NaCl)
solution with a density of 1.2 kg/L is the most 4.2 Digestion
commonly used liquid in the density separation, owing
to its cheap price and non-toxic characteristics (Li Due to the complexity in the composition of wastew-
et al. 2018a). During separation, a suspension is ater, digestion is required to remove biogenic mate-
created and then vigorously shaken, followed by rials from wastewater prior to further characterizations
incubation until two clear phases are formed. The via FTIR and Raman spectroscopy. Table 4 summa-
upper layer of water contains low-density particles rizes the digestion methods adopted by analyzing the
like microplastics and high-density particles (e.g., microplastics from wastewater streams.
clay) usually separates into the bottom layer. Conse- To date, the most effective digestion approach
quently, the microplastic particles can be recovered involves the incubation of microplastics-containing
from the supernatant (Li et al. 2018a). Magni et al. samples in 30% (v/v) hydrogen peroxide (H2O2). The
(2019) applied an saturated NaCl solution to separate digestion by H2O2 can destroy most organics present
the microplastics in the influent, effluent, and sludge in the sample (Stock et al. 2019). Li et al. (2018b)
samples from primary, secondary, and tertiary treat- extracted microplastics from dewatered sewage sludge
ments, and it was observed that the high-density using saturated NaCl solution followed by digestion
particles [PVC: 1.16–1.58 kg/L; polyoxymethylene with 30% H2O2 (as shown in Fig. 5) and the results
(POM): 1.41–1.61 kg/L] cannot be separated. showed that an average 78.27% of microplastics can
123
Table 4 Separation and digestion methods adopted for analyzing microplastics originating from wastewater streams
Source Separation Digestion Recovery References
(%)
Sludge, Spain NaCl – – Bayo et al. (2016)

Effluent, USA – 30% H2O2 with0.05 M FeSO4 as the 87 Dyachenko et al. (2017)
catalyst
Upstream and downstream, NaCl 30% H2O2 with0.05 M FeSO4 as the – Estahbanati and Fahrenfeld
USA catalyst (2016)
Effluent and sludge, Canada – 30% H2O2 – Gies et al. (2018)
Effluent, Turkey NaI 30% H2O2 with 0.05 M FeSO4 as the – Gündoğdu et al. (2018)
catalyst
Effluent and sludge, Finland – 30% H2O2 with 0.05 M FeSO4 as the – Lares et al. (2018)
catalyst
Effluent, South Korea ZnCl2 30% H2O2 with0.05 M FeSO4 as the Lee and Kim (2018)
catalyst
Sludge, China NaCl 30% H2O2 67–98 Li et al. (2018b)
Effluent ad sludge, Italy NaCl 15% H2O2 78–98 Magni et al. (2019)
Effluent, Denmark – 30% H2O2 with0.05 M FeSO4 as the 57–78 Simon et al. (2018)
catalyst
Effluent, UK – 30% H2O2 – Tagg et al. (2015)
Effluent, Australia NaI 30% H2O2 – Ziajahromi et al. (2017)
be recovered, as evidenced by Fourier-transform effluent samples and then heated at 70 °C for 30 min
infrared spectroscopy (FTIR) analysis. with constant stirring. An extra addition of 30% H2O2
The main drawback for the digestion by H2O2 is the was added when the digestion of organics was not
requirement of a large amount of H2O2; thus, it is less completed. Subsequently, the extract was recovered
efficient for treating a larger sample volume in the by vacuum filtration over a 0.8 lm membrane filter.
economic perspective. To solve this, Tagg et al. (2017) As confirmed by a dissecting stereomicroscope, WPO
studied the effectiveness of Fenton’s reagent [a mixture method led to a 87% recovery of the microplastics.
of H2O2 and ferrous ion (Fe2?)] on the isolation of While, due to the existence of cellulose fibers and fatty
microplastics from wastewater, and no significant alter- acids as two major interferents, a sequential WPO
nation in the microplastic properties was observed. To procedure was employed after a single cycle of
compare, Fenton’s reagent has advantage over H2O2 pre- digestion. Briefly, after a single WPO digestion, the
treatment: (1) time-efficient; and (2) the ability to deal extract was filtered through a 0.125 mm sieve and then
with large sample volumes. Gündoğdu et al. (2018) washed with hexane and distilled water. The solid
digested the secondary effluent by a mixture of 30% materials in the sieve was then digested again using a
H2O2 and 0.05 M Iron (Fe) (II) at 75 °C, and then NaI 30% H2O2–0.05 M FeSO4 mixture for 3–6 digestion
solution was added for density separation. Following this, cycles in order to completely remove cellulose and
the suspension underwent centrifugation for 5 min at other organic materials.
3500 rpm and then filter over a 55 lm filter, and the
collected matters were characterized by microscopy and 4.3 New approaches developed for extracting
l-Raman spectroscopy. microplastics
In another study, the digestion by wet peroxide
oxidation (WPO) for characterizing the microplastics Recently, Phuong et al. (2018) developed a new
in secondary effluent was evaluated by Dyachenko extraction method by centrifugation with ultrapure water
et al. (2017). Initially, 80 mL of 30% H2O2 and 40 mL for microplastics present in sediments without the use of
of 0.05 M Iron (II) sulfate (FeSO4) were added into the H2O2 as the digestion agent. It was reported that
123
Dewatered sewage sludge Stirring for 15 min Settling for 2 h
Repeat extraction
Saturated NaCl solution step for 3 times
Rinse with distilled water Filtration Top layer
Extracts
30% H2O2 solution
Incubate overnight
Distilled water
Filtration
Rinse with distilled water
Dry in a desiccator for 3 days
Fig. 5 A schematic diagram of the extraction procedure adopted for microplastics in the sewage sludge (Li et al. 2018b)
potassium hydroxide (KOH) was ineffective in the sieved sediment samples, followed by centrifugation and
digestion treatment since the precipitation still occurred filtration over a 12 lm pore-size filter. This procedure
even after centrifugation (Phuong et al. 2018). Besides, was validated by spiking the sediment samples with four
the use of 65% nitric acid (HNO3) as the digestion agent commercially available polymers including PE, PP,
resulted in a 66–100% recovery efficiency for PE and PVC, and polyethylene terephthalate (PET). However, to
polypropylene (PP). However, it has been reported that the best of our knowledge, no study so far has adopted
HNO3 shows negative impact on the microplastics, such this method to extract microplastics present in the
as: (1) destroy microplastics when the digestion temper- wastewater; therefore, future studies should be con-
ature above 60 °C; (2) damage the polymeric structure of ducted to evaluate the recovery efficiency of extraction
nylon; (3) discolor PE; and (4) react with the surface of by ultrapure water and centrifugation for microplastics
PVC and thus affects its surface morphology (Claessens from various wastewater systems.
et al. 2013; Li et al. 2018a).Subsequently, two different
separation methods including ultrapure water and 50%
potassium iodide (KI) were investigated before centrifu- 5 Identification and characterization
gation. In the case of KI solution, large amounts of of microplastics
materials were observed in the suspension and at the
surface of supernatant after centrifugation, resulting in 5.1 FTIR and Raman spectroscopy
large-sized microplastics being analyzed by l-FTIR and
thus a longer processing time is required. On the other FTIR and Raman spectroscopy are two commonly
hand, for the separation by ultrapure water, an amount of used methods for characterizing microplastics present
20 mL of ultrapure water was added to 25 g of 1 mm- in various environmental systems (Carr et al. 2016;
123
Dyachenko et al. 2017; Gies et al. 2018; Lares et al. operating conditions were as follows: injector tem-
2018). Two different working principles are applied: perature of 300 °C, split ratio of 5, and final temper-
(1) the change in the dipole moment of chemical bonds ature of 700 °C. Besides, it was found that Py–GC/MS
produces an infrared spectrum in the FTIR analysis; offered several advantages over Raman spectroscopy
and (2) Raman analysis offers a molecular fingerprint like the feasibility for identifying co-polymer without
spectrum according to the polarizabilities of chemical the use of chemometric method. Nevertheless, some
bonds (Strungaru et al. 2019). A range of FTIR types of polymers with polar subunits, like PEST and
technologies have been developed, among which polyether, can not be detected by Py–GC/MS because
attenuated total reflectance (ATR)-FTIR is suitable for of the formation of polar pyrolyzate(Challinor 1989).
characterizing irregular microplastics and l-FTIR is Additionally, this technique is only applicable for
applicable for small-sized microplastic samples certain selected types of polymers such as PE and PP
(around 20 lm) (Prata et al. 2019). Despite FTIR due to the limitation on the pyrolysis database (Li et al.
analysis is a non-destructive and reproducible tech- 2018a). Whereas, Py–GC/MS might be favorable for
nology, this approach is very time-consuming and a the analysis of microplastics due to the fact that PE and
trained operator is needed (Rocha-Santos and Duarte PP are two common polymeric type in the
2015). Moreover, Raman spectroscopy is an analytical microplastics.
approach that can only be applied for the detection of Other thermal degradation approaches have also
compounds with aromatic bonds, C–H, and C=C been employed for analyzing the characterization. For
bonds since the alteration of the polarizability of a instance, Dümichen et al. (2017) studied the polymeric
chemical bond is necessary for the analysis. This composition of microplastics originating from a
approach allows for characterizing the size of biogas plant by TED-GC/MS technology. This tech-
microplastics down to 1–2 lm and it is not constrained nology is a combination of thermal solid-phase
by the samples properties like shape and thickness (Li extraction and thermal desorption.
et al. 2018a; Strungaru et al. 2019). Raman technique In addition, the thermogravimetric analysis coupled
can analyze the sample containing organic or inor- with differential scanning calorimetry (TGA–DSC)
ganic fillers, pigments, and those cannot be detected has been used for analyzing the microplastics present
by FTIR spectroscopy (Imhof et al. 2016). Notwith- in the wastewater streams. Majewsky et al. (2016)
standing, the long processing time, polymer heating adopted TGA–DSC technique for determining the
and degradation, as well as fluorescence inference are amount of microplastics in two effluent samples from
the main drawbacks of Raman spectroscopy (Strun- a WWTP in Karlsruhe. The authors reported that the
garu et al. 2019). PE in the effluents represented 17–34% (81–257
mgPE/m3effluent) of the total extracted materials, while,
5.2 Thermal degradation approaches no PP was not detected in the effluents. Even though
TGA–DSC offers an alternative or complementary
To overcome the time-consuming problem of FTIR approach to the time-consuming FTIR analysis in the
and Raman spectroscopy, pyrolysis–gas chromatog- qualitative and quantitative measurements of
raphy coupled with mass spectrometry (Py–GC/MS) microplastics, only PE and PP can be identified owing
has been utilized for microplastics. During this to the overlapping transition temperature of the
analysis, the large-molecular weight compounds can different polymers. Besides, the size, number, color,
be thermally degraded into small-molecular weight and shape of microplastics can not be provided by
compounds under inert conditions (Fischer and TGA–DSC technique, as the breakage of microplastic
Scholz-bottcher 2017). Py–GC/MS technique is cap- samples can be observed during the analysis (Strun-
able of determining some polymeric compositions and garu et al. 2019).
organic plastic additives which cannot be easily
separated, dissolved, and extracted (Qiu et al. 2016). 5.3 Nile red staining
Hermabessiere et al. (2018) performed an optimiza-
tion study on the identification of microplastics in the The use of staining dye such as Nile red is a low-cost
bivalve, beach, and sea water surface using Py–GC/ method for the analysis of microplastics. Previous
MS and Raman spectroscopy. The optimized studies reported that the characterization of
123
microplastics using Nile red staining has showed a in the organics-rich wastewater. Mintenig et al. (2017)
similar accuracy when compared with FTIR and studied the microplastics in effluents via FPA-assisted
Raman spectroscopy (Shim et al. 2016; Maes et al. transmission l-FTIR, and this technique is allowable
2017; Catarino et al. 2018). Moreover, Nile red for the detection of small-sized microplastics
staining technique has the advantages of: (1) short (* 20 lm). For all effluent samples, the abundance
incubation time (10–30 min); (2) high recovery effi- of microplastics was found to be 10–9000 microplas-
ciency (up to 96.6%); and (3) with or without a tics/m3 and 0–50 microplastics/m3 for the microplas-
cleaning step by bleach when using vibrational tics with a size\ 500 lm and[ 500 lm, respectively.
spectroscopy (Prata et al. 2019). Catarino et al. In addition, PE was identified as the most dominant
(2018) identified the presence of microplastics in polymeric type in both size groups of microplastic
Mytilus edulis by staining with Nile red dye in samples. A similar method by FPA-assisted FTIR
methanol at 1 lg/mL. This method led to a 48% of imaging was adopted by Simon et al. (2018) where the
recovery efficiency of microplastics, which was com- abundance of microplastics present in the influent and
parable to that obtained from FTIR analysis (50%). effluent was determined. The authors stated that the
Shim et al. (2016) optimized the microplastics iden- FPA-based FTIR imaging is an effective method for
tification by Nile red staining, and it was observed that investigating the polymeric type in microplastics;
5 mg/L Nile red solution in hexane was effective for however, it can only provide an estimation of the
staining a variety of types of microplastics including amount of microplastic instead of providing an
PE, PP, PS, polycarbonate (PC), polyurethane (PU), absolute value.
poly(ethylene–vinyl acetate) (PEVA), polyamide In summary, it is very difficult to analyze the
(PA), and PEST, with the exception of PVC. However, microplastics in organic-rich wastewater. Current
to the best of our knowledge, no study so far has methods used for characterizing microplastics origi-
utilized Nile red dye to analyze the microplastics from nating from wastewater systems are incomparable
wastewater systems. Therefore, future studies are since the unit of the concentration of microplastics
necessary to explore the feasibility of Nile red staining adopted is not consistent. Moreover, the differences in
for the characterization of microplastics present in the the sampling sites and methods and the contamination
organic-rich samples like wastewater. However, its control render the comparison among analytical
major drawback is correlated to: (1) the formation of approaches more difficult. As a result, a standardized
weak signals for certain types of polymers like PET; analytical protocol for microplastics present in the
(2) the microfibers are reported to be very difficult to wastewater streams should be established (He et al.
stain by Nile red dye; and (3) a fluoresce microscopy is 2018).
needed (Tamminga et al. 2017).
5.4 FPA-based FTIR imaging 6 What happens to microplastics in WWTPs
Even though a wide range of analytical methods have 6.1 Treatments and removal efficiency
been applied for microplastics in marine organisms of microplastic in WWTPs
and sediments, no specific technique has been estab-
lished for the analysis of microplastics originating Typically, a wastewater treatment plant is capable of
from wastewater systems. To fill this gap, Tagg et al. operating primary, secondary, and tertiary treatment to
(2015) identified and characterized the microplastics remove contaminants prior to discharging the effluents
present in the wastewater via focal plane array (FPA)- into the surrounding environment. As suggested by
assisted reflectance micro-Fourier-transform imaging Carr et al. (2016), most microplastics can be removed
analysis combined with a pre-treatment using 30% by primary treatment (e.g., skimming and settling) and
H2O2. FPA is a detector that is very useful for fewer amounts of microplastics can be observed in the
identifying the small-sized microplastic beads on their tertiary effluent. A flow diagram describing the fate of
surface areas. The authors reported FPA-based l- microplastics in a WWTP is depicted in Fig. 6. Most
FTIR analysis was observed to be effective for the recent studies investigating the microplastics present
characterization of PE, PP, PVC, and PS microplastics in the sludge and effluent are summarized in Table 5.
123
Removal efficiency: 78-95%
Influent Screening
Removal efficiency: 20% Tertiary treatment
Sedimentation Aeration Clarification Chlorination/UV
Secondary treatment Removal efficiency: 95-99%
Primary sludge Waste activated sludge Effluent
Primary treatment
Sludge
Fig. 6 A flow diagram describing the transport of microplastics in a tertiary wastewater treatment plant (Note The removal efficiency
of each treatment is determined based on the amount of microplastics present in the influent) (Raju et al. 2018; Sun et al. 2019)
6.1.1 Effect of treatment process present in the sludge. The treatment by anaerobic
digestion led to a reduction in the abundance of
Previous studies have explored the effect of treatment microplastics, which might be attributed to the poly-
process on the removal efficiency of microplastics. mer degradation by microorganism within the anaer-
Lee and Kim (2018) compared three biological obic digestion system; however, this role needs to be
treatments namely, anaerobic-anoxic-aerobic, elucidated.
sequence batch reactor, and the Media processes on
the removal rate of microplastics. The authors reported 6.1.2 Removal efficiency
that the concentration of microplastics in the effluents
of anaerobic-anoxic-aerobic, sequence batch reactor, Gündoğdu et al. (2018), for example, studied the
and the Media processes was 0.44 particles/L, 0.14 microplastics concentration in the influent and sec-
particles/L, and 0.28 particles/L, respectively, and the ondary effluent from two municipal WWTPs in
removal efficiency for microplastics with a size Turkey. It was found that the influent and secondary
[ 106 lm was estimated to be in the range of 98–99% effluent contained 4,665,778 and 3333.3 microplas-
for all three treatments. No difference of removal tics/day, respectively, thus leading to a 91% of
efficiencies was found among the tested treatments. removal rate.
This might suggest that most microplastics were Gies et al. (2018) reported that an amount of
removed by grease and grit removal treatment and 1.76 ± 0.31 trillion microplastics/year is discharged
primary settling. Besides, a higher removal efficiency into the WWTP in Vancouver, Canada, among them
was obtained from smaller sized microplastics 1.28 ± 0.54 trillion microplastics/year is retained in
(106–300 lm) when compared with that obtained the primary sludge and 0.36 ± 0.22 trillion microplas-
from larger sized microplastics ([ 300 lm). This tics/year is detected in the secondary sludge. Based on
result might be attributed to the affinity of microplas- this, a high removal efficiency (99%) of microplastics
tics with a small particle size to the sticky media (e.g., can be achieved by the WWTP.
biofilm and floc). Kalčı́ková et al. (2017) studied the transport and
In another study, Mahon et al. (2017) examined the fate of PE microbeads in the WWTP was explored.
effects of three different wastewater treatment pro- The microbeads removal efficiency by secondary
cesses including anaerobic digestion, thermal drying, treatment was about 52%. Besides, it was observed
and lime stabilization on the amount of microplastics that the PE microbeads at small size classes were
123
Table 5 Recent studies on microplastic pollution detected in the effluent and sludge
Sources Analytical Main conclusions References
approaches
Effluent
FPA-based l- FPA-based FT-IR coupled with H2O2 pre-treatment was an effective approach for Tagg et al.
FTIR analyzing microplastics in wastewater (2015)
Microscopy Most microplastics removed by primary treatment (skimming and settling) Carr et al.
FTIR Tertiary effluent contributed less to the microplastic pollution (2016)
Some types of toothpaste formulation were significant sources of microplastics
FTIR Microplastic removal efficiency of primary and secondary treatment was 78.34% and Murphy et al.
20.1%, respectively (2016)
High amounts of microplastics can be observed in the sludge
FTIR Around 0.28, 0.48, and 1.54 microplastics/L can be found in the effluent after tertiary, Ziajahromi
secondary, and primary treatment, respectively et al. (2017)
Fibers were the dominant type of microplastics detected in the effluent
Microscopy All treatment provided a removal efficiency of 98% Lee and Kim
FTIR A high fraction of blue and black fibers can be observed in all effluent samples (2018)
FTIR PEST and PE were the most dominant polymer in the microplastics Talvitie et al.
Membrane bioreator resulted in the highest removal efficiency of microplastics (99%) (2017a)
The size of 20–100 lm and fibers were the most common size fraction and types of
microplastics, respectively
Microscopy PEST fibers and PE fragments were the most dominant type of microplastics Lares et al.
FTIR 98.3% of microplastics can be removed by conventional wastewater treatment (2018)
Raman Size: 0.5–1 mm
microscopy
Microscopy Fibers and fragments were the most common type of microplastics Gies et al.
FTIR No difference can be observed in the composition of microplastics between primary and (2018)
secondary effluent
A microplastics removal of 99% can be achieved
Microscopy PEST was the most predominant chemical composition of microplastics Gündoğdu
l-Raman The removal efficiency of microplastics was 73–79% et al. (2018)
microscopy Type: fibers (60%), films (20%), and fragments (20%)
Microscopy Chemical composition: PEST and PA Magni et al.
FTIR Type: lines (41%), films (38%), and fragments (21%) (2019)
Size fraction: 0.1–0.5 mm (52%), 0.01–0.1 mm (27%), 1–5 mm (14%), and 0.5–1 mm
(7%)
Sludge
Microscopy Type: films (51%), fragments (34%), and lines (15%) Magni et al.
FTIR Size fraction: 0.1–0.5 mm (54%), 0.01–0.1 mm (24%), 0.5–1 mm (12%), and 1–5 mm (2019)
(10%)
Chemical composition: acrylonitrile-butadiene (27%), PE (18%), and PEST (15%)
Microscopy Chemical composition: PP, nylon, PA, ethyl acrylate, and norbornene Bayo et al.
FTIR (2016)
DSC
Microscopy Abundance: 4196–15,385 microplastics/kgdry sludge Mahon et al.
FTIR Chemical composition: HDPE, PE, PEST, acrylic, PET, PP, and PA (2017)
SEM Type: fibers (78.5%), fragments (18.4%), films (1.9%), other unidentified particles
(0.6%), and spheres (0.3%)
123
Table 5 continued
Sources Analytical Main conclusions References
approaches
Microscopy Abundance: 22.7 ± 12.1 9 103 microplastics/kgdry sludge Li et al.

SEM Color: white (59.6%), black (17.6%), red (9.0%), orange (3.3%), green (2.3%), blue (2018b)
M-FTIR (1.7%), and others (6.5%)
Type: fibers (63%), shafts (15%), films (14%), flakes (7.3%), and spheres (1.3%)
Chemical composition: PO (fibers and shafts), PC (fibers), PE (films), PA (films), alkyd
resin (flakes), PS (spheres)
Microscopy Blue and black fibers and black fragments were the most dominant type microplastics Lee and Kim
FTIR (2018)
Microscopy Chemical composition: PEST, PA, PE, and various polymers (PE, PP, and PEST Lares et al.
FTIR fragments with similar kind of appearance) (2018)
Raman Type: fibers and fragments
microscopy
Microscopy Abundance: 14.9 ± 6.3 microplastics/kg dry primary sludge; 4.4 ± 2.9 microplastics/ Gies et al.
FTIR kg dry secondary sludge (2018)
Fibers was the most common type in both primary and secondary sludge
likely retained in the activated sludge, whereas larger clarification), which corresponds to a removal effi-
sized microbeads tended to partition into the effluent. ciency of 20.07% (based on the amount of microplas-
Most importantly, a high affinity of PE to the tics in the influent) before releasing into the receiving
negatively charged activated sludge flocks was found, water.
which suggests the potential of microplastics being
accumulated in the sediments and affects marine 6.1.3 The presence of microplastics in the effluent
organisms (Teuten et al. 2007). This could be due to
the electrostatic attraction between the positively Gündoğdu et al. (2018) found that the most commonly
charged surface of PE microbeads and negatively detected microplastic type in the effluent was fiber
charged activated sludge flocks. (60%) followed by film (20%) and fragment (20%). l-
Murphy et al. (2016) studied the fate and removal Raman spectroscopy analysis showed that the PE,
rate of microplastics during a secondary WWTP, and a PEST, PVC, acrylonitrile butadiene styrene, POM,
reduction of * 15.70 microplastics/L of influent to nylon-6, and PP were identified as the main polymeric
* 0.25 microplastics/L of effluent was achieved, compositions of microplastics in the effluent, among
corresponding to a removal efficiency of 98.41% for which PEST was the most frequently observed
microplastics. While, in the consideration of flow rate polymer. PEST is a preferable material used in the
of WWTP, an estimation of 23 billion microplastics textile industry owing to its strength and durability,
might be released from the final effluent annually. and thus substantial amounts of PEST microfibers are
Specifically, the number of microplastics detected in expected in the wastewater (Napper and Thompson
the grit and grease removal stage (second stage) was 2016). In a work by Carr et al. (2016), the most
* 8.7 microplastics/L, leading to the highest reduc- frequently identified microplastics in the WWTPs
tion efficiency (44.59%) for microplastics. Following were blue and irregular PE particles, which are
this, in the third stage by primary settling, around 3.4 commonly utilized in the whitening toothpaste for-
microplastics/L can be found and this results in a mulation. This suggests that some types of toothpaste
removal efficiency of 33.75% (based on the amount of formulations make contribution to the amount of
microplastics in the influent). Finally, the amount of microplastics detecting in the WWTPs.
microplastics was further reduced to 0.25 microplas- In general, due to the ineffective for conventional
tics/L by final treatment stage (aeration and treatments in removing small-sized microplastics
123
(\ 100 lm), further research must be carried out to slurry is normally generated from primary and
establish new treatment technologies with a focus on secondary wastewater treatment. Previous literature
the removal of microplastics with a size smaller than claimed that around 99% of microplastics remain in
100 lm. the sludge after multiple stages of wastewater treat-
ment processes, making agriculturally-applied sludge
6.2 Advanced treatment and removal efficiency (also known as biosolid) an important source of
of microplastics microplastic pollution to the environment (Mahon
et al. 2017). Many studies have reported the abun-
Despite the conventional wastewater treatments exhi- dance of microplastics in the sludge (Gies et al. 2018;
bit high efficiencies (* 99%) for removing Lares et al. 2018; Li et al. 2018b).
microplastics, substantial amounts of microplastic Li et al. (2018b) investigated the abundance and
pollutants can still be released into the aquatic characterization of microplastics in 79 different sludge
environment in the consideration of a large amount samples collected from 28 WWTPs across China, and
of effluent being discharged every day. To solve this, the results showed that the average concentration of
Lares et al. (2018) evaluated the removal efficiency of microplastics in the dried sludge was 22.7 9 103
microplastics by an advanced treatment (i.e., mem- microplastics/kgdried sludge. Microscopic analysis indi-
brane bioreactor), and this treatment led to a higher cated that fibers (63%) and white (59.6%) were found
removal efficiency (99.4%) than that obtained from to be the predominant type and color, respectively, of
conventional activated sludge process (98.3%). the microplastics in the dewatered sludge. As indi-
Talvitie et al. (2017a) investigated the removal cated by FTIR analysis, the main polymeric compo-
efficiency of microplastics from effluent using four sitions of sludge-based microplastics were low-
different advanced final-stage treatment technologies density plastics such as polyolefin (PO), acrylic fibers,
including membrane bioreactor, discfilter, rapid sand PE, PA, alkyd resin, and PS. Nevertheless, the high-
filtration, and dissolved air flotation. The authors density plastics like PVC (q = 1.16–1.58 g/mL) and
reported that the number of microplastics in the PET (q = 1.37–1.45 g/mL) were not detected since
primary effluent significantly reduced from 6.9 their higher densities could complicate the density
microplastics/L to 0.005 microplastics/L with the use separation by saturated NaCl solution (q = 1.2 g/mL)
of membrane bioreactor, which represents a 99.9% of (Hidalgo-Ruz et al. 2012).
microplastics removal efficiency. Similar to mem- In the work by Bayo et al. (2016), different sludge
brane bioreactor, the usage of rapid sand filter and samples were collected after primary treatment and
dissolved air flotation led to 97% and 95% efficiency, anaerobic digestion. The authors found that the ethyl
respectively, for removing microplastics from sec- acrylate (an important monomer for producing resins,
ondary effluent. To compare, the discfilter removed plastics, rubbers, or dental materials) was identified as
the microplastics in the secondary effluent from 0.5 to one of the main compounds in the sludge. It should be
2.0 microplastics/L to 0.003–0.3 microplastics/L, noted that ethyl acrylate as a toxic compound has
resulting in a 40–98.5% removal efficiency. More- demonstrated the feasibility for transferring the
over, the small sized microplastics (20–100 lm) were adsorbed metals (e.g., Pb, Cd, and Zn) into the food
identified to be dominant in three out of four chain (Browne et al. 2013).
investigated wastewater treatment plants, with the Mahon et al. (2017) examined the abundance and
exception for treatment by membrane bioreactor. properties of microplastics in the sludge from seven
Therefore, it is necessary to employ an advanced final WWTPs in Ireland, and the amount of microplastics
treatment to remove the microplastics with a size extracted from sludge was in the range of 4196–15,385
smaller than 100 lm. microplastics/kg of sludge (on a dry basis). Besides,
the majority of extracted microplastics were com-
6.3 Characterizations of microplastics in sludge posed of 75.8% of fibers and small amounts of
fragments (18.4%), films (1.9%), spheres (0.3%),
Throughout the settling process of wastewater treat- and other (0.9%). In addition, the main polymeric
ment, the majority of microplastics could be entrained components detected in the microplastic from sludge
and ended up in the sludge. Sludge as a semi-solid included high-density polyethylene (HDPE), PE, and
123
PA. As shown in Fig. 7a–c, the surface morphology of 7 Potential environmental contamination
microplastics originating from the treated sludge after by microplastics
thermal drying exhibited fracturing and blistering;
however, the microplastics, which were treated by As indicated by literature, considerable amounts of
lime stabilization, showed a more shredded and microplastics can still be released into the aquatic
weathered appearance (Fig. 7d–f). Additionally, environment after wastewater treatments (Raju et al.
Fig. 7g–i indicated that the surface texture of 2018). The feasibility of microplastics for absorbing
microplastics isolated from the treated sludge after harmful agents like pharmaceuticals has been evalu-
anaerobic digestion had a deep cleavage, which was ated. Prata et al. (2018) evaluated the influence of the
distinct from microplastics extracted from sludge after mixture of microplastics and pharmaceutical (pro-
thermal drying or lime stabilization. cainamide and doxycycline) on their toxicity for
Furthermore, Lares et al. (2018) stated that the microalgae (Tetraselmis chuii), and the results showed
effect of treatment approach on the polymeric com- the toxicity of individual pharmaceutical was
position of microplastics was insignificant. In general, increased in the presence of microplastics. This
PEST (79.1%) accounted for the most abundant in all phenomenon might be attributed to the interaction
microplastic samples, followed by PE (11.4%) and PA between microplastics and the cell wall of microalgae,
(3.7%). The type and size for the majority of thus facilitating the uptake and/or the toxic action of
microplastics was observed to be fibers and \ 1 mm, doxycycline/procainamide. In another study, the toxic
respectively. effects of florfenicol, microplastics, and their mixture
on the freshwater exotic invasive bivalve Corbicula
fluminea were studied by Guilhermino et al. (2018). It
Fig. 7 Surface morphology of microplastics isolated from various treated sewage sludge samples after thermal drying (a–c), lime
stabilization (d–f), and anaerobic digestion (g–i) (Mahon et al. 2017)
123
was found that both microplastics and florfenicol 8 Challenges and future perspectives
exhibited toxicity to C. fluminea; while a stronger
toxic effect was observed in the mixture of florfenicol As indicated by literature, microplastics could
and microplastics. Fonte et al. (2016) also observed undergo a series of degradation processes, such as
the toxicological interaction between microplastics thermal degradation, mechanical action, and biodegra-
and cefalexin to Pomatoschistus microps. Besides, it dation, thereby causing changes in their surface
was found that an increase in the temperature led to a morphology and polymeric composition (Cooper and
higher toxicity of cefalexin alone and in the mixture Corcoran 2010; Hidalgo-Ruz et al. 2012). Thus, a
with microplastics. database containing the properties of microplastics in
On the other hand, microplastics may act as carriers terms of chemical composition and surface morphol-
or transport vectors for POPs like polycyclic aromatic ogy when subjected to various degradation processes
hydrocarbons and (PAHs) polychlorinated biphenyls must be established in the future. Moreover, microor-
(PCBs) owing to their large specific surface areas ganism might readily colonize the surface of
(Wang et al. 2018a). Microplastics could float in the microplastics, which could lead to the formation of
microlayer of sea surface due to a lower density than biofilm and complicate the subsequent spectroscopic
water, in which hydrophobic contaminants such as analysis (Li et al. 2018a). Consequently, it could be
PCBs and 2,2-bis(p-chlorophenyl)-1,1-dichloroethene very difficult to differ the microplastics from natural
can be concentrated by 105–106 times (Mato et al. polymers (e.g., chitin, cellulose, and chitosan) when
2001). Chen et al. (2019) investigated the accumula- considering the small size of microplastics (\ 5 mm)
tion of PHAs and PCBs on the plastics, and the results (Li et al. 2018a). Besides, microorganism might be
showed that PS exhibited the highest concentrations of transported along with microplastics and thus could
organic pollutants (PAHs = 23,696.7 lg/kg; PCBs = introduce pathogens into the surrounding environment
234.6 lg/kg). This is possibly due to the fact that: (1) (Jiang 2017).
PS can act as a sink for some types of PAHs; and (2) PS To reduce the microfiber released from synthetic
is an amorphous polymer, whereas other plastics like clothing during domestic laundering, there are several
PP contain crystalline regions and therefore more significant directions for future research such as: (1)
energy is required to disrupt their polymeric structures conduct comparative studies on the varying types of
(Rochman et al. 2013). However, the role of washing machines; (2) evaluate the effects of wash
microplastics as vectors of absorbed pollutants is still duration and spinning speed on the microfiber
under debate. Beckingham and Ghosh (2017) carried released; (3) examine the influences of fabric design
out a comparative study on the bioavailability of PCBs and textile choice on the microfiber loss; and (4)
in microplastics, wood, biochar, and coal by measur- investigate the temporal dynamics of release through-
ing the solid-water distribution coefficient, gut fluid out the life time of a garment product (Napper and
solubilization, and bioaccumulation with Lumbriculus Thompson 2016).
variegatus. It was found that the bioavailability of In addition, the standardized and effective analyt-
PCBs in microplastics was significantly lower than ical techniques used for the identification and charac-
that from natural sediments. The authors concluded terization of microplastics in the wastewater systems
that the contribution of organic contaminants to the must be developed and verified by extensive amounts
aquatic environment from microplastics was smaller of research (Bayo et al. 2016). For example, the use of
than that from natural pathways. Bakir et al. (2016) different units (e.g., number/volume and mass/vol-
also reported that the ingestion of microplastics by ume) makes the direct comparison among the current
animals did not offer a route for transferring adsorbed studies impossible (Silva et al. 2018). Besides, there
organic pollutants from ocean to biota. are several challenges in the existing sampling tech-
When considering the widespread of microplastic niques for microplastics, including: (1) the highly-
pollution and their interactions with harmful agents, efficient and detailed sampling methods are still
future research is needed to thoroughly understand: (1) lacking; (2) the seasonal or inter-annual variants of
the synergistic toxic effects of widely used pharma- environmental parameters have not been considered in
ceuticals and microplastics; and (2) the role of the previous literature; and (3) most studies don’t
microplastics as vectors for POPs.
123
consider the short spatial and/or temporal (hours and 5. Even though the role of microplastics as vectors
meters) variations (Costa et al. 2018; Silva et al. 2018). for POPs is still undetermined (e.g., PAHs and
Furthermore, the underlying mechanism of accel- PCBs), microplastics have demonstrated the pos-
erated proliferation of microplastics throughout the sibilities for absorbing harmful agents like phar-
multiple stages of wastewater treatment processes maceuticals which can be identified in the
requires to be examined. For instance, the role of wastewater.
microorganism in the anaerobic digestion process
must be thoroughly understood as it might serve as a Acknowledgements The authors would like to acknowledge
promising remediation approach (Mahon et al. 2017). the funding from NSERC through the Discovery Grant awarded
to Dr. Amarjeet Bassi. In this article, copyright permission has
been obtained for the following figures: Figs. 1, 2, 3, 4 and 7
from their original publishers: Elsevier and ACS Publication
9 Conclusions respectively. The documents for the permission are available
upon request.
Microplastics as one of the serious environmental
problems have received a great deal of attention.
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Rev Environ Sci Biotechnol (2019) 18:207–230

Current research trends on microplastic pollution

Published online: 13 April 2019

applied during sampling period. Nevertheless, sam-

Surface filtration is an highly effective sampling 3.3 Contamination

Fig. 3 A stacked sampling

Sludge, Spain NaCl – – Bayo et al. (2016)

Dewatered sewage sludge Stirring for 15 min Settling for 2 h

Rinse with distilled water Filtration Top layer

30% H2O2 solution

Rinse with distilled water

Dry in a desiccator for 3 days

5.4 FPA-based FTIR imaging 6 What happens to microplastics in WWTPs

Removal efficiency: 78-95%

Removal efficiency: 20% Tertiary treatment

Sedimentation Aeration Clarification Chlorination/UV

Secondary treatment Removal efficiency: 95-99%

Primary sludge Waste activated sludge Effluent

Microscopy Abundance: 22.7 ± 12.1 9 103 microplastics/kgdry sludge Li et al.

11:812–821. https://doi.org/10.2495/SDP-V11-N5-812- mainland China. Water Res 122:53–61. https://doi.org/10.

Anal Chem 113:84–92. https://doi.org/10.1016/j.trac.2019. Netherlands. Environ Toxicol Chem 35:1627–1631.

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