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Journal of Hazardous Materials 367 (2019) 504–512

Contents lists available at ScienceDirect

Journal of Hazardous Materials


journal homepage: www.elsevier.com/locate/jhazmat

Review on the occurrence and fate of microplastics in Sewage Treatment T


Plants
Georgia Gatidoua, , Olga S. Arvanitib, Athanasios S. Stasinakisa

a
Department of Environment, University of the Aegean, 81100, Mytilene, Greece
b
Department of Food Technology, Ionian University, 28100, Argostoli, Greece

GRAPHICAL ABSTRACT

ARTICLE INFO ABSTRACT

Keywords: Microplastics are plastic fragments lower than 5 mm that are detected in the environment causing various effects
Microliter on organisms. Several research articles have recognized Sewage Treatment Plants as important sources of
Presence polyethylene and polypropylene beads, polyester, polyamide and other types of microplastics. For their de-
Analysis termination, techniques such as visual identification using microscope, Fourier-transform infrared and RAMAN
Wastewater
spectroscopy are used, while chemical oxidation, enzymatic maceration and density separation are applied as
Biosolids
pretreatment methods for the removal of the inorganic and organic content. Microplastics’ concentrations range
up to 3160 particles L−1, 125 particles L−1 and 170.9 × 103 particles Kg-1 TS dw in raw, treated wastewater and
sludge, respectively. Their removal during wastewater treatment ranges between 72% and 99.4%; the main
processes that contribute to their removal are primary and secondary treatment, while the effect of tertiary
treatment depends on the applied technology. Entrapment in suspended solids and accumulation to sludge are
the major mechanisms governing their fate. A standardized protocol for samples’ collection and pretreatment as
well as microplastics’ isolation and characterization is needed; future reseach should investigate the possible
chemical and physical changes of microplastics during treatment, and their role as carriers for the transfer of
emerging micropollutants.


Corresponding author.
E-mail address: ggatid@env.aegean.gr (G. Gatidou).

https://doi.org/10.1016/j.jhazmat.2018.12.081
Received 11 June 2018; Received in revised form 6 December 2018; Accepted 20 December 2018
Available online 29 December 2018
0304-3894/ © 2018 Elsevier B.V. All rights reserved.
G. Gatidou et al. Journal of Hazardous Materials 367 (2019) 504–512

1. Introduction point sources of microplastics [36]. This important review paper con-
tains information on the fate of microplastics in STPs, their interactions
Plastic pollution is a high-priority problem that has received in- with microcontaminants as well as their effects in aquatic organisms;
creasing attention during the last decade [1–3]. Plastic items can slowly however, it is based on papers published before 2016. According to
breakdown into smaller pieces and due to their lightweight nature, they Scopus database, ever since numerous research papers have been
are dispersed by ocean currents and wind to the coastal environment published on the field, providing much more and better quality in-
[1]. Microplastics are plastic fragments with size lower than 5 mm, formation on the occurrence and fate of microplastics in STPs.
separated into primary and secondary [4]. The primary microplastics Under this frame, this review article contains information for the
are intentionally manufactured to be of microscopic size as they are sampling and analytical procedures that are followed for the mon-
used in abrasive cosmetic products [5]; whereas secondary micro- itoring of microplastics in STPs, while the type and the concentrations
plastics are formed from the breakdown of plastics litter after exposure of microplastics, typically found in wastewater and sludge samples, as
to water, wind and sunlight [6,7]. Microplastics are also categorised well as their removal efficiencies and behavior during different treat-
according to their shape and colour. The main types that are detected in ment processes are also discussed. The current gaps in the literature are
the environment are fragments, pellets, fibres, films, granules, and highlighted and the future perspectives for research are indicated.
styrofoam [8]. The occurrence of microplastics has been mentioned
worldwide [9,10], while the effects from their accumulation on aquatic 2. Sampling and analysis of microplastics in sewage treatment
organisms have been reported in several studies and include reduction plants
of feeding activity, oxidative stress, genotoxicity, growth delay and
death [11–13]. Physical or chemical changes of microplastics, when Microplastics’ collection is usually performed by sieving [37,38] or
found in the environment, seem to affect their uptake and toxicity filtration [39,40] using sieves and filters with various mesh/pore sizes
[14,15]. Most of the experiments have been conducted with fish and, in to distinguish size categories of microplastics. The volume of either
many cases, concentrations higher than those commonly found in the grab [27,37] or composite samples [27,41] varies between some mil-
environment have been used [12,13]. Additionally, it is known that liliters [27,37,42,43] or liters for the influents [44–46] to several liters
microplastics accumulate and transfer toxic compounds to the en- [42,47] or even few m3 for the effluents [37,40,48] (Table 1). The
vironment that are either used during their production or are sorbed explanation for the wide range of sample volumes between raw and
onto the plastic media when the microplastics are in water [16,17]. treated wastewater is that influent normally has high content of organic
Several studies have shown that they contain different priority pollu- matter and as a result, filters’ or sieves’ clogging is possible to be caused
tants such as organochlorine pesticides, polycyclic aromatic hydro- if large volumes are collected. On the contrary, effluent has sig-
carbons, polychlorinated biphenyls, and polybrominated diphenyl nificantly lower content of organic material and therefore it is achiev-
ethers [18–22]. Due to the higher affinity of these contaminants for the able to filter large volumes. Additionally, treated wastewater is ex-
plastic media than water, accumulation up to one million times higher pected to contain fewer microplastics. Therefore, it is wise to sample
onto the plastic particle can be occurred [23]. In a recent work, it has and handle higher volumes [39] especially when larger particles are
also been reported that microbeads contained in biosolids could serve targeted to be identified [49]. For instance Talvetie et al. [27] measured
as vectors for heavy metals contamination when biosolids are applied to various categories of microplastics in the effluents using three different
the soil [24]. filters with pore sizes 20, 100 and 300 μL. According to the results, for
Based on the above and taking into account the durability of mi- the determination of larger microplastics (≥ 300 μm), that corre-
croplastics and their trend to be transferred within food webs [25,26], sponded to less than 5% of the total amount of particles, 10.5 to 13.5 L
their occurrence in the environment is a matter of global concern. of effluents were filtered. On the contrary, smaller microplastics
Under this point of view, the identification of the potential aquatic- (20–100 μm) which corresponded to almost 70% of the total micro-
based and land-based sources of microplastics remains a challenging plastics’ amount were determined after the filtration of only 2 L of
issue. Among the land base sources municipal sewage, stormwater and sample. But even when same types of effluents are collected, still are
riverine transport seem to be of high importance [27–29]. In a recent observed variations in the sample volumes between different articles.
study, Cheung and Fok [30] estimated that in Mainland China Talvitie et al. [42], Carr at al. [37], Michielssen et al. [38] and Zia-
306.9 tonnes of microbeads per year are emitted to the environment, jahromi et al. [44], when analyzed tertiary effluents, they collected
while 80% of them are derived from the effluents of Sewage Treatment sample volumes of 2 to 285 L, 1.89 × 105 to 2.23 × 105 L, 34 to 85 L
Plants (STPs). Other studies have also pointed out the contribution of and 200 L, respectively. This high discrepancy it is probably due to the
sewage on the amounts of polyester and acrylic fibers found in the lack of a standardized and generally accepted sampling and further
marine environment [31,32]. analytical procedure for microplastics’ study. Indeed, the nature of
Since 2009, several research articles have been published reporting these “pollutants” allows only partial validation of the analytical
the occurrence of microplastics in wastewater and sewage sludge methods because microplastics are found in many different materials,
samples. Specifically, a search at Scopus database using the keywords shapes and sizes [50]. Moreover, samples with regards to microplastics,
“microplastics” and “wastewater” indicates the existence of 74 pub- present high heterogenicity since, unlike to chemical compounds,
lications in scientific journals (Fig. S1). These publications contain in- cannot be dissolved. Thus, when a researcher is trying to validate a
formation on different disciplines such as concentration levels of mi- method, comes across with questions such as how much sample should
croplastics in wastewater, methods for the identification of be collected and what size, mass and type of material should be spiked
microplastics in wastewater and sludge, effects of microplastics con- in the sample during recovery experiments. As for the target micro-
tained in wastewater on organisms etc. This number is reduced to 57 plastics’ fractions it should be ideal if the complete range from 1 to
publications when the keywords “microplastics” and “wastewater 5000 μm could be analyzed as also reported by [50] in order to obtain a
treatment” are used. The receiving results are even less, only 12, when more comprehensive view of the contamination extent. Regarding the
the keyword “fate” is also added to the previous ones indicating that collected sample volume, there are no available recommendations in
scientists have quite recently started to study the role of different the literature. Definitely, its size is affected by the limit of detection
wastewater treatment processes on microplastics’ behavior. Regarding (LOD) of the analytical method. Although being crucial, only few stu-
the existence of review papers on the field, despite the fact that a sig- dies have up to now reported the determination of LOD during micro-
nificant number of review papers are available for the analysis, occur- plastics’ analysis [49,50]. Certainly, when dealing with such particles
rence, effects and fate of microplastics in the aquatic environment presenting high variety in size, material and shape, its calculation is a
[29,33–35], only one article has been published for the role of STPs as challenging topic. However, since its determination reinforces the

505
Table 1
In Information on the studied Sewage Treatment Plants, worldwide, applied water/sludge processes and identification methods.
Country Treatment type Population Average treated Sample size: Water sample Sludge Particle size Identification method Reference
G. Gatidou et al.

served sewage volume (L) / mass (g, wet weight-ww) processing Sample processing (μm)
(m3 day−1)

Finland Tertiary 800,000 NR Influent:0.3 Filtration device – 20-200 Visual observation & FT-IR [42]
Primary effluent: 1–20 spectroscopy
Secondary effluent: 1–20
Tertiary effluent: 2–285
France Primary & biological NR 240,000 0.05 Automatic sampler – 100-5000 Visual observation [43]
treatment
Scotland Secondary 650,000 NR Inffluent:30 Steel bucket and – > 65 Visual observation & FT-IR [45]
Primary effluent: 30 steel sieve spectroscopy
Secondary effluent: 50
U.S.A. Secondary, tertiary, NR 2,500,000 raw wastewater: 1–2 Sieving – 20-4750 Visual observation [38]
(3 STPs) anaerobic membrane (data given for preliminary
bioreactor one STP) effluent:
1–6
primary effluent: 10–20 secondary
effluent: 10–20 Tertiary effluent: 34–38
U.S.A Tertiary NR 1,060,000 Influent: 0.1 Sieving Digestion with 20-400 Visual observation & FT-IR [37]
(7 STPs) (data given for Tertiary effluent: 1.89*105-2.23*105 sodium hypochlorite spectroscopy
the largest STP) Sludge: ∼5 (NR)
U.S.A. Primary, secondary, tertiary 3,500- 6,490- 382,000 5.00 × 102-2.10 × 104 Filtration – 125-355 & Visual observation [40]
(17 STPs) (depending on the STP) 56,000,000 > 355
Sweden Mechanical, chemical & 12,000 NR Influent:2 Filtration Filtration > 300 Visual observation & FT-IR [39]
biological Effluent: 1000 spectroscopy
Sludge:25 g

506
Russia Mechanical treatment and NR ̴ 960,000 Influent: 0.1 Filtration device – 20-300 Visual observation [52]
purification Effluent: 8
Australia Tertiary NR NR 0.75 Filtration – NR Visual observation & FT-IR [31]
(2 STPs) spectroscopy
Germany Primary, secondary, tertiary 7.0 × 103- NR Effluent: 390-1000L Filtration pump Density separation > 500 & ATR-FT-IR spectroscopy & [48]
(12 STPs) (depending on the STP) 2.1 × 105 Sludge: 500 < 500 FPA- based transmission
micro-FT-IR
Netherlands (7 NR NR NR Filtration Density separation 10-5000 Visual observation & FT-IR [60]
STPs) spectroscopy
Australia Primary, secondary, tertiary ̴ 150,000 to 13,000-308,000 Primary effluent: 3-100 Filtration device – 25-500 Visual observation & FT-IR [44]
(3 STPs) (depending on the STP) 1,230,000 Secondary effluent: 27-150 spectroscopy
Tertiary:200
Finland Primary, secondary NR ̴ 10,000 Influent: 0.8-3 Primary effluent: 4-30 Sieving Drying at 45 °C for 250 & 5000 Visual observation & FT-IR / [46]
Sludge: 3-20 18h Raman spectroscopy
Finland Tertiary 800,000 Grab sample Filtration device Filtration > 300-20 Microscopy and FT-IR [27]
Influent: 0.1a,b,c
After pre-treatment: 50-333a, 7-10b, 0.5c
After AS: 200-333a, 20-30b, 0.5c
Effluents: 1000a, 100b, 2 c
24-h composite sample
Influent: 0.1a,b,c
After pre-treatment: 13.2-14.5 a, 8.5-
10.5b, 0.5c
After AS: 11-14.5La,b, 1c
Effluents: 10.5-13.5a,b, 2b
Denmark Biological treatment (one of Raw wastewater:1 Filtration – 10-500 Focal Plane Array (FPA)- [49]
(10 STPs) ten WWTR also applies sand Effluent: 4.1-81.5 based FT-IR
filtration)
(continued on next page)
Journal of Hazardous Materials 367 (2019) 504–512
G. Gatidou et al. Journal of Hazardous Materials 367 (2019) 504–512

Reference reliability of the results, it should be determined following the 3-Sigma


method like Simon et al. [50] did. As for sludge samples, both wet and

[47]
dry types are analyzed and the treated quantities are in the scale of mL
or grams, respectively [39,46].
In some studies, before microplastics isolation, samples are pre-
treated in order to remove the inorganic and organic content.
Microscopy and FT-IR
Identification method

Degradation of labile organic matter is performed using an oxidizing


agent (e.g. hydrogen peroxide) [37,40,44,46] or enzymatic maceration
[48], while inorganic compounds such as sand and rust can be removed
by density separation [48]. It is worth mentioning that samples pre-
treatment is not applied in all research papers of the field; there are
several studies where no pretreatment method has been followed but
the collected samples were just filtered and subjected to analysis for
microplastics identification and counting [27,38.41,45]. As there is still
Particle size

a lack of a unified standardized established method regarding samples’


collection and pretreatment as well as microplastics’ isolation and
(μm)

1-65

Note: “NR”: Not reported; “FT-IR”: Fourier transform infrared spectroscopy; a: filter mesh size = 300 μm, b: filter mesh size = 100 μm, c: filter mesh size = 20 μm.

characterization, comparison among different studies becomes very


difficult while the received results present high variation. Vollertsen
Sample processing

and Hansen [50] recognizing the gap in the literature regarding ana-
lytical methods for microplastics determination in wastewater, under-
line the importance for the establishment of a broad-spectrum metho-
Filtration
Sludge

dology.
To avoid contamination with microplastics during sampling and
samples’ preparation, special care should be taken on the types of
and secondary only)

clothing used (avoiding these which are made from synthetic fibers) as
Sieving (primary

well as on the cleaning of the equipment (petri dishes, containers, filter


Water sample

papers, forceps) and the surfaces in the lab [45]. However, despite the
processing

precautions are taken, contamination is not avoided [27,48,49] and


sometimes can reaches over 30% of the estimates microplastics [27].
Nevertheless, since background contamination affects the limit of de-
tection of the used method and also influences the sample size, it always
volume (L) / mass (g, wet weight-ww)

should be accounted. Several authors have reported the parallel ana-


Influent:1, primary effluent: 30,

lysis of field blanks in order to investigate possible contamination by


other sources and prevent the overestimation of their results
[27,47–49]. Moreover, if possible, glass or metal equipment should be
secondary effluent: 30

used instead of plastic as also recommended by Vollertsen and Hansen


Sludge: 5 g (ww)

[50].
Regarding the methods applied for the determination of micro-
Sample size:

plastics, these vary from visual identification using microscope


[38,40,43,52] to Fourier-transform infrared (FT-IR) [42,44,45] and
RAMAN spectroscopy [46]. Having in mind that almost up to 70% of
the small particles, which are characterized visually as microplastics,
Average treated

are usually not confirmed as plastics by FT-IR spectroscopy [52],


(m3 day−1)

spectroscopic techniques are strongly recommended against visual ob-


̴ 490,000

servation for the reliable determination of microplastics’ chemical


sewage

composition. The use of visual observations alone may lead to over-


estimation or underestimation of particles quantity due to the high bias
for distinguishing natural and synthetic materials [43]. For instance,
Mintenig et al. [48] reported that only 50% of the visually detected
Population

1,300,000

fibres were confirmed as being synthetic fibres in treated wastewater


served

samples. Therefore, it is crucial the visual observations to be followed


by spectroscopic analysis in order to secure the consistency of the re-
sults. It is worth mentioning that spectroscopic equipment is expensive
and requires highly trained staff to handle it. Moreover, it presents
uncertainties which are due to the fact that only a part of the sample is
scanned during analysis, while often there are differences between the
Treatment type

spectra from natural samples and reference spectra of pure materials


Secondary

[50]. Nevertheless, research regarding microplastics should be con-


ducted with these techniques because the verification of plastic parti-
cles is a matter of high importance.
Table 1 (continued)

3. Occurrence of microplastics’ in wastewater and sludge

Research conducted since 2009 has highlighted the crucial role of


Country

Canada

wastewater as potential pathway of different groups of microplastics


such as polyethylene and polypropylene beads, polyester, polyamide

507
G. Gatidou et al.

Table 2
Published data on the occurrence, removal and daily discharges of microplastics from Sewage Treatment Plants, worldwide.
Country Shape & type of detected microplastics* Number of microplastics Number of microplastics Number of Removal rate Daily discharges Reference
influent in final effluent microplastics in sludge (particles d−1)

Finland Synthetic particle and textile fibers 430 synthetic particles/L & 8.6 synthetic particle/L & – 98% Synthetic – [42]
180 textile fibers/L 4.9 textile fibers/L particle, 97% for
fibres
France Fibers 260-320 /L 14-50 particle/L – 83–95% – [43]
Scotland Flakes, fibers, film, bead, foam (alkyds, polystyrene-acrylic, polyester, 15.7 /L 0.25/L – 98.4% 6.5 × 107 [45]
polyurethane, acrylic, polyamide, polypropylene, polyethylene,
polyethylene terephthalate)
U.S.A. Fiber, fragment, microbead, nurdle, paint chip, other > 80- < 140 /L 0.5-5.9 / L – 95.6-99.4% 9–110d [38]
(3 STPs)
U.S.A Irregularly Shaped polyethylene 1 /L ∼0.0007 /L 103 /Kg (NR) 99.9% 0.93 × 106 [37]
(7 STPs)
U.S.A. Fragments, fibers, films, foam, pellets – 0.05/L – – 15 × 103 [40]
(17 STPs)
−3 3
Sweden Fibers, fragments, flakes 15.1 /L 8.25 × 10 /L 16.7 × 10 /Kg (dw) 99.9% – [39]
Russia Textile fibers, synthetic & black particles 467 textile fibers, 160 16 textile fibers, 7 – 96% – [52]
synthetic & 3160 black synthetic & 125 black
particles/L particles/L
Australia Fibers (polyester, acrylic, polyamide) – 1.0 /L – – – [31]
(2 STPs)

508
Germany polyethylene, polypropylene polyamide, polyvinyl chloride, polystyrene, – 0-0.05 /L (> 500) & 0.01- 103-2.4 × 104 /Kg – 9 × 107-4 × 109 [48]
(12 STPs) polyurethane, silicone and PUR-based coatings (“paint”), SAN, polyester, 9 /L (< 500) (dw) (annual)
polyethylene terephthalate, ethylene vinyl acetate, polyvinyl alcohol,
acrylonitrile butadiene styrene, polylactide and paint synthetic fibers
(polyamide, polypropylene, polyester)
Netherlands (7 Fibers, foils, spheres 68-910 /L 51-81 /L 510-760 /Kg (ww) 72% – [60]
STPs)
Australia polyvinyl chloride, polystyrene, polypropylene,polyethylene – 0.21-1.5 /L – – 1 × 107 [44]
(3 STPs) terephthalate, polyethylene, Nylon
3 7
Finland polyester, polyamide, polyethylene, various polymers 57.6 /L 1.0 /L 170.9 × 10 /Kg (dw) – 1.0 × 10 [46]
Finland Fibers (cotton, polyester, linen, viscose, wool, polyacryl), fragments, Grab sample* Grab sample** 186.7 ( ± 26.0)*103 > 99% 1.7 × 106 and [27]
flakes, films, spherical 380-636.7 0.7-14.2 (d.w.) 1.4 × 108
24-h composite sample** 24-h composite sample**
630-900 1.4-23.8
Denmark Acrylate, Styrene-Acrylonitrile copolymer, Vinyl-acetate-acrylic 7216 54 – 99.3% 3000e [49]
(10 STPs) copolymer, Polyethylene, Polypropylene, Polyethylene-Polypropylene
copolymer, Polyester, Polystyrene, Polyurethane, Polyvinyl chloride,
Ethylene-vinyl acetate, Polyamide, Poly(vinyl-acetate)
Canada Fibres, fragment, foam granule, sheet, pellet 31.1 ± 6.70 2.6 ± 1.4 after primary primary sludge: 97.1-99.1% 32-97 × 103 [47]
treatment, 14.9*103 ± 6.3
0.5 ± 0.2 after secondary secondary sludge:
treatment 4.4*103 ± 2.9

Note: “NR”: Not reported; “FT-IR”: Fourier transform infrared spectroscopy; a: filter mesh size = 300 μm, b: filter mesh size = 100 μm, c: filter mesh size = 20 μm; *: sampling during three different days; **: sampling
during three different days and after different treatment steps; d: value was given in kg L−1; e: value was given in Kg year−1.
Journal of Hazardous Materials 367 (2019) 504–512
G. Gatidou et al. Journal of Hazardous Materials 367 (2019) 504–512

and nylon fibres [31,43,44,47,53,54,55]. So far, some information is Kg-1 to 2.4 × 104 Kg-1 dw. Mahon et al. [63] estimated the concentra-
available for the amounts of microplastics contained in wastewater, tions of microplastics in sludge samples from different STPs in Ireland
while all the relevant studies have been conducted in North Europe, and ranged between 4.196 and 15.385 particles Kg-1 dw while in
USA and Australia. The detected amounts of microplastics varied be- Dutsch STPs, mean particle concentrations of 510 to 760 Kg− 1 wet
tween 1–3160 particles L−1 and 0.0007–125 particles L−1 for raw and weight of sludge have been determined [60].
treated wastewater, respectively (Table 2), depending on the size of the The abundance but also the morphology of microplastics seems to
STP and the used treatment processes. A comprehensive analysis of the be affected by the type of sludge treatment. So far, it has been observed
existing data can be found below. increased abundance of small fibers after sludge lime stabilization [67],
Leslie et al. [56] reported that microplastics’ concentrations in in- while morphological alterations of microplastics such as melting and
fluents and effluents of a Dutch STP were approximately 200 and 20 blistering have noticed after thermal drying of sludge [63]. Monitoring
items/L, respectively. Higher concentrations were found in the effluents of the concentrations and types of microplastics during different sludge
from a German STP (33 granules/L, 24 fibres/L and 24 fragments/L) treatment processes by Mahon et al. [63] showed that sludge alkaline
[57] and from three STPs in the Netherlands (55 microplastics/L) [58]. stabilization results to microplastics’ shearing, while anaerobic diges-
In a more comprehensive study, effluents samples were collected from tion resulted to lower amounts of microplastics in the produced sludge.
12 German STPs and analysed for microplastics [59]. According to the However, in this study, it was not clear if the decrease of microplastics’
results, microplastics smaller than 500 μm were detected in the ef- abundance was due to biodegradation or sampling errors. In a current
fluents with the most common particles to be items of whitish/trans- laboratory study investigating the biodegradability of polylactide fi-
parent color and irregular shape. As for the types of microplastics, the bers, Rom et al. [64] reported that activated sludge, operating at me-
most often found polymers were polyethylene, polyvinyl alcohol, sophilic and thermophilic conditions, was insufficient for the biode-
polystyrene, polyester, and polyamide. The number of microplastics gradation of this type of microplastic.
with size higher than 500 μm ranged up to 0.05 per L of treated was-
tewater. PE and polypropylene were the most frequently found poly- 4. Fate and removal of microplastics during wastewater treatment
mers, while most particles had partly foil-like shape. Similar types of
microplastics were also detected in effluents from a Finish STP by A STP normally comprises a primary, secondary and sometimes
Talvitie et al. [42]. Mason et al. [40] studied the concentrations and the tertiary treatment train to purify the receiving water using chemical,
type of microplastics in effluents originated from 17 US STPs. Ac- physical and biological treatment processes. Regarding the role of dif-
cording to their results, 0.05 ± 0.024 microparticles per L of treated ferent processes on microplastics’ removal, most of the studies agree
wastewater were determined on average, while the commonest type of that pretreatment processes remove microplastics from wastewater to a
particles were fragments and fibers. Significant inter- and intra-facility small or partial rate. On the other hand, a percentage of 72 to 98% of
variations were noticed both in the concentrations and the fractions of microplastics seem to be removed at primary treatment [27,37,45,60].
microparticles. Murphy et al. [45] determined the concentrations and Secondary treatment contributes to an extra 7 to 20% of removal
the types of microparticles in raw and treated wastewater originating [27,45], whereas microplastics’ elimination during tertiary treatment
from a Scottish STP. The most common types of polymers in STP’s inlet depends on the applied technology [27,38,41,48,44]. Several studies
were alkyds, polystyrene-acrylic and polyester; whereas polyester and reported that tertiary treatment does not guarantee the absence or re-
polyamide were mainly detected in treated wastewater. Finally, in a markable removal of microplastics. For instance, in a comprehensive
recent study, Leslie et al. [60] reported mean particle concentrations of study which took place in New York and where 34 STPs were examined,
68 to 910 L− 1 and 51 to 81 L− 1 in raw sewage and treated wastewater it was concluded that tertiary treatment processes such as membrane
from seven Dutch municipal STPs, respectively (particle sizes between microfiltration, continuous backwash upflow dual sand microfiltration
10 and 5000 μm). and rapid sand filters, did not assure lack of microbeads from the ef-
The concentrations of microplastics detected in treated wastewater fluents [65]. Additionally, Mason et al. [40] suggested that the use of
and the high volumes of effluents that daily end up to the aquatic en- granular tertiary filtration is not that effective and Carr et al. [37] did
vironment result in the transfer of great amounts of microplastics and a not observe a positive impact on microplastics elimination due to
considerable contamination (Table 2). Murphy et al. [45] calculated a gravity filters. On the contrary, Talvitie et al. [41], comparing different
daily discharge of 6.5 × 107 microplastics into the receiving water by a treatment processes, reported that the highest removal was achieved by
Scottish STP serving 650,000 inhabitants (average flowrate: the MBR (99.9%), followed by rapid sand filter (97%), dissolved air
260,954 m3 d−1), while Carr et al. [37] estimated a discharge of flotation (95%) and discfilter (40 to 98.5%). Michielssen et al. [38]
0.93 × 106 microplastics per day from a WWTP treating 1.06 × 106 m3 reported also that among the studied STPs, these with tertiary treat-
of wastewater d-1. Ziajahromi et al. [44] estimated that amounts as high ment and membrane bioreactor removed 97.2% and 99.4% of micro-
as 1 × 107 microplastics are discharged per day with the effluents of plastics, respectively. It is worth mentioning that the percentage of
reverse osmosis in an Australian STP serving 150,000 inhabitants. Si- microplastics’ removal in different processes is also affected by the type
milarly, Talvitie et al. [27] estimated high amounts of microplastics in of target microplastics.
the effluents of a Finnish STP treating 270,000 m3 wastewater per day. Information for the removal efficiency of microplastics in different
These amounts ranged between 1.7 × 106 and 1.4 × 108 particles d-1 STPs worlwide is given in Table 2, while the main results of selected
for different days of the week. papers are reported below. In general, total removal efficiencies of
Up to now, high microplastics’ concentrations in sludge have also microplastics in STPs range between 72–99.4% (Table 2). Specifically,
been found, varying between 103 and 170.9 × 103 microplastics Kg−1 Murphy et al. [45] observed microplastics’ removal during grit and
dw [37,39,48,61]. These results indicate the high potential of STPs in grease removal (44.6%), while an additional removal of 33.8% and
retaining microplastics from raw wastewater. Bayo et el. [62] analysed 20.1% was calculated during primary sedimentation and biological
sludge samples originating from the primary clarifier as well as after the treatment, respectively. Talvitie et al. [42] studied the removal of
anaerobic digestion and centrifugation and detected various types of textile fibers and synthetic particles in a Finnish STP and reported that
microplastics such as polypropylene, Nylon and transparent thermo- the textile fibres were mostly removed during primary sedimentation,
plastic polyamides. It is generally accepted that the detected amounts of while the contribution of this step on the removal of synthetic particles
microplastics in sludge are orders of magnitude higher than those find was limited. Most of these particles were removed during secondary
in raw and treated wastewaters. According to Mintenig et al. [48], sedimentation. Dris et al. [43] observed a removal of fibrous micro-
microplastics were detected in all analyzed sludge samples, collected plastics of up to 80% during primary treatment, while this percentage
from different STPs in Germany, and the amounts ranged from 1 × 103 increased to almost 95% after biological treatment. In a Russian STP the

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G. Gatidou et al. Journal of Hazardous Materials 367 (2019) 504–512

Fig. 1. Microplastics mass balance in a Finnish STP. Blue ar-


rows: wastewater; brown arrows: sludge; light brown arrow:
reject water from the dewatering process; AS: activated
sludge; BAF: biologically active filter; RAS: sludge recircula-
tion. Source: Talvitie et al. [27]. (For interpretation of the
references to colour in this figure legend, the reader is referred
to the web version of this article).

amount of microplastics was reduced about 96% after a secondary microplastics when physicochemical and biological treatment processes
treatment [51], while are applied. Based on the importance of polyester and polyethylene
Magnuson and Noren [39] reported a removal as high as 99.9%. microplastics, comprehensive studies regarding their fate and removal
Similarly, in a more recent study, Talvitie et al. [27] who investigated in STPs are also needed. Taking into account the reported effect of
the removal of microplastics in a full-scale STP also reported that 99% weathering, aggregation and differences in surface charges on micro-
removal was achieved after secondary treatment. It is worth mentioning plastics’ toxicity [14,15], further research is needed for their possible
that an important amount of microplastics which are removed at some chemical and physical changes during wastewater treatment. So far,
step of treatment is recycled back at the inlet of the STP. Analyses in there is also lack of data for the removal and the fate of microplastics in
sludge and reject water samples showed that from the 99% of the mi- constructed wetlands and other low cost systems applied in smaller
croplastics which were removed via primary and excess sludge, 20% settlements.
was recycled back at the inlet of STP via the reject water that came up The available information for the role of sludge treatment processes
after sludge treatment (Fig. 1) [27]. on microplastics’ removal is also limited and further data is needed
Regarding the mechanisms which are responsible for microplastics’ from full-scale STPs and lab-scale experiments. As in previous studies it
removal, so far there is limited information and almost all of them is has been reported that polymers can be microbially breakdown due to
derived from monitoring studies in full-scale STPs. During primary the activity of exoenzymes [68,69], the role of biodegradation during
treatment, a significant amount of microplastics is captured through anaerobic digestion should be further investigated. Additionally, as
skimming of floating solids [37,45], since lower density microplastics sludge reuse in soil is the predominant choice for most European
can float on wastewater [37]. Entrapment in suspended solids and ac- countries, accounting for more than 50% of the produced sludge in EU-
cumulation to the primary and secondary sludge is also another im- 27 [70], information is also needed for mobilization and transport of
portant mechanism explaining microplastics’ removal during waste- microplastics in sludge-amended soils and the possible ecological threat
water treatment [37,45]. In recent lab-scale experiments using a for the environment.
Sequencing Batch Reactor it was shown that 52% of microbeads were So far, several emerging contaminants such as surfactants, phar-
accumulated to activated sludge [66]. maceuticals, personal care products and perfluorinated compounds
have been detected in STPs [69–74]. Beside the existed knowledge on
the accumulation of priority pollutants to microplastics, no data is
5. Current gaps and future perspectives available for the role of microplastics as carriers of these compounds.

As great amounts of treated wastewater is discharged daily into the Appendix A. Supplementary data
aquatic environment worldwide, the role of STPs as land base source of
microplastics is of high importance. So far, a few data exists for the Supplementary material related to this article can be found, in the
amounts of microplastics found in wastewater, however a lack of data is online version, at doi:https://doi.org/10.1016/j.jhazmat.2018.12.081.
observed for the Mediterranean area, Asia and South America. The
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