Abundance and Characteristics of Microplastics in An Urban Wastewater

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Environmental Pollution 310 (2022) 119890

Contents lists available at ScienceDirect

Environmental Pollution
journal homepage: www.elsevier.com/locate/envpol

Abundance and characteristics of microplastics in an urban wastewater


treatment plant in Turkey☆
Gökhan Ekrem Üstün *, Kübra Bozdaş, Tuğba Can
Bursa Uludağ University, Faculty of Engineering, Department of Environmental Engineering, Bursa, 16059, Turkey

A R T I C L E I N F O A B S T R A C T

Keywords: Wastewater treatment plants (WWTPs) are considered one of the important sources of aquatic/terrestrial
Microplastics microplastic (MP) pollution. Therefore, the abundance and properties of MPs in the wastewater and sludge of an
Wastewater treatment plant urban WWTP in Bursa Turkey were investigated. The amount, properties, and removal of MPs were evaluated.
Sludge
The results showed that the average abundance of MPs was 135.3 ± 28.0 n/L in the influent and 8.5 ± 4.7 n/L in
Removal
Abundance
the effluent, with a 93.7% removal rate, MP was removed and transferred to the sludge. The daily MP amount
Characteristics released in the aquatic environment is calculated as 525 million MPs, and the annual amount is 1.9 × 1011 MPs.
The abundance of MPs in the sludge thickening and sludge filter cake is 17.9 ± 2.3 and 9.5 ± 2.3 n/g dry weight
(dw), respectively. The sludge disposal amount of WWTP is 81.5 tons/day and the approximate amount of MP
accumulated in the sludge per year is calculated as 2.8 × 1011 MPs. In wastewater and sludge samples, fragment
dominant shape, black main colour, and 500–1000 μm sizes are the most common size. The main MP types in
wastewater samples at the influent are polypropylene (PP, 36.8%), polyethylene (PE, 31.0%), polystyrene (PS,
11.8%), polyethylene terephthalate (PET, 8.0%), and polyamide (PA, 7.1%), at the effluent (PE, 33.0%), (PP,
52.5%), and (PS, 8.2%). In the sludge cake, the distribution is (PE, 40.8%), (PP, 27.6%), (PS, 18.7%) and (PET,
8.0%). The results of this study show that MPs are removed from wastewater with high efficiency by treatment
processes and a significant amount accumulates in the sludge. Therefore, it is suggested that to integrate
advanced treatment processes into urban WWTPs and use effective sludge disposal management practices to
reduce the amount of MP released into the environment with effluent and sludge.

1. Introduction absorb/adsorb pollutants (e.g. heavy metals, persistent organic pollut­


ants (POPs), toxic substances) from the surrounding environment with
The increase in the production and use of plastic materials and the their hard to degrade surfaces and high surface areas (Batel et al., 2018).
inadequate management of plastic waste cause the world to be polluted WWTPs are one of the most important sources for the release of MPs
with these wastes rapidly. About 6.3 billion Mt of plastic polymers was into aquatic/terrestrial environments (Ziajahromi et al., 2017). Despite
produced and discarded in 2015, of which only 9% were recycled, 12% around 90% MP removal from WWTPs, high volume treated wastewater
were incinerated, and the remaining 79% accumulated in landfills or discharge is a potential source of MP for aquatic environments (Bozdaş
terrestrial environments (Mendenhall, 2018). Plastic production is et al., 2020). It has been reported that MPs abundances in the influent of
projected to double over the next 20 years if current growth rates WWTPs in different parts of the world range from 0.28 n/L to 31,400 n/L
continue (Lebreton and Andrady, 2019). Microplastics (MPs) which are (Liu et al., 2021). The MP abundances in the effluent of WWTPs are in
generally defined as solid polymer residues smaller than 5 mm the range of 0–447 n/L and these large differences in MP abundances
(Thompson, 2015), attract attention with their potential negative effects could be related to the different sampling methods applied in the
on ecosystems. The high resistance to degradation, hydrophobic nature studies, the pretreatment, and the analysis of the samples (Sun et al.,
and lightness of MPs cause them to spread rapidly on a global scale with 2019). Most MPs removed from WWTPs accumulate in sludge (Li et al.,
storms, runoff, and winds and pose a risk of pollution (Piñon-Colin et al., 2018). The MP abundance in the treated sludge has been reported to
2020; Zaki et al., 2021; Zhou et al., 2021). In addition, MPs can easily range from 4400 n/kg to 240,000 n/kg depending on the treatment


This paper has been recommended for acceptance by Eddy Y. Zeng.
* Corresponding author.
E-mail address: gokhaneu@uludag.edu.tr (G.E. Üstün).

https://doi.org/10.1016/j.envpol.2022.119890
Received 9 May 2022; Received in revised form 29 July 2022; Accepted 31 July 2022
Available online 3 August 2022
0269-7491/© 2022 Elsevier Ltd. All rights reserved.
G.E. Üstün et al. Environmental Pollution 310 (2022) 119890

Fig. 1. WWTP flow chart and sampling points: inlet of raw wastewater (Influent, labeled as W1), outlet of the grit chamber (labeled as W2), outlet of the secondary
sedimentation tank (Effluent, labeled as W3), returned sludge (labeled as S1), outlet of sludge thickener (labeled as S2) and sludge filter cake (labeled as S3).

technologies (Liu et al., 2021). In addition, the use of sludge formed in taken as 24-h composite (equal volume, every hour) with Enderes
WWTP as fertilizer in agricultural lands plays an important role in the Houser automatic sampling devices. Autosamplers were programmed to
terrestrial input of MPs (Edo et al., 2020). There are few studies on the sample hourly composite samples (250 mL every 15 min) for a total
amount, removal, and environmental release of MPs in WWTPs in period of 1 day. Samples were taken from a depth of 50 cm and collected
Turkey and there is no effective policy for the management and disposal in 1 L PE sample containers (8.5 cm square bottom) and stored in a 4 ◦ C
of plastic waste. refrigerator until analysis. Grab samples were collected using a 10 L steel
Bursa is the 4th largest city in Turkey with its industrialization and bucket (Lares et al., 2018). According to Table 1, wastewater volumes at
population. In this study, the abundance, properties, and removal effi­ sampling points throughout the treatment units have been increased. At
ciency of MPs in wastewater and sludge samples taken from different each sampling point, the volume of sampling was dependent on the
treatment stages of a WWTP located in one of the anthropogenically ability to filter samples with high organic matter that rapidly clogs the
affected regions of Turkey were examined, and the amount of MP sieves and causes overflow (Ben-David et al., 2021). Also, due to the low
released into the environment was evaluated. concentrations and uneven distribution of MPs in treated wastewater,
recent efforts have used a more representative sampling approach by
2. Material and methods increasing the sampling volume (Talvitie et al., 2017).

2.1. Study location


2.3. Extraction of MP from wastewater
The WWTP where the study took place, is located at (40◦ 14′ 14.4′′ N
28 55′ 07.7′′ E) and in the drainage basin; urban areas, industrial facil­
◦ Wastewater samples were passed through a size of stainless steel
ities (textile, metal plating, laundry, casting, machinery manufacturing, sieves of 5 mm, 3 mm, 1 mm, 500 μm, and 300 μm at room temperature
auto subsidiary industry, chemical industry) and landfill leachate firstly. Some PE microbeads recommend keeping temperatures 60 ◦ C or
treatment plant. The design flow of the facility was 87,500 m3/day, and lower to minimize MP damage as they begin to melt during heating
the average current flow rate was 61,800 m3/day in the 4 months (be­ water when the temperature reaches 60 ◦ C (Munno et al., 2018).
tween August and November 2021) when the sampling was conducted. Therefore, the temperature was chosen as 60 ◦ C during the drying and
Approximately 90% of the wastewater coming to the plant is domestic oxidation phase of the samples. Freshly prepared 20 mL FeSO4 solution
and the remaining part originates from the above-mentioned areas. The (0.05 M) and 20 mL H2O2 solution (30%) were added to the beakers for
plant was designed according to the modified five-stage Bardenpho organic matter removal on dry samples and mixed vigorously (Hossain
process. The plant receives wastewater from over 650,000 inhabitants et al., 2021; Patchaiyappan et al., 2020). The beakers were incubated for
and applies treatment processes that include screening (coarse mesh size 5 min at room temperature. It was then heated to 60 ◦ C on a magnetic
of 150 mm, fine mesh size of 20 mm), grit removal, biological process, stirrer for 30 min 20 mL of H2O2 was added to beakers with visible solid
and sedimentation. Effluent is discharged to the Marmara Sea via Nilüfer particles and continued to add H2O2 until no solid particles were visible
Creek. The sludge coming from the sedimentation is first transferred to (Yang et al., 2019). The beakers were then covered with needle-punched
the sludge thickening unit and then to the sludge dewatering unit by aluminum foil to allow gas to escape (Koelmans et al., 2019). The bea­
dosing the cationic polymer. The average daily production of sludge kers were left to cool for 1–2 h at room temperature until no reaction
cakes is 81.5 tons/day, and the sludge cakes are sent to the Sludge was observed (Ziajahromi et al., 2021). The material from the oxidation
Incineration Plant to generate electricity. The flow chart of the facility step was transferred to a separatory funnel with distilled water and a 5 M
and the sampling points of the samples are shown in Fig. 1. NaCl solution (Masura et al., 2015). The saturated solution of NaCl (1.2
g/cm3) is preferred because it is environmentally friendly, inexpensive,
and easy to find. The low recovery rates of high-density MPs (such as
2.2. Sampling methodology PVC and PET) are the disadvantage of using NaCl. NaI (1.6 g/cm3) and
ZnCl2 (1.7 g/cm3) salts, which can be used for high-density MPs, have
The sampling points, sampling status, sample volumes, and sieve disadvantages such as being expensive and toxic to aquatic biota
sizes of the plant are shown in Table 1 of Supplementary Material. It is (Crichton et al., 2017). Natural fibers (cotton, wool, unknown cellulose)
recommended to take samples in dry weather so that rainy weather does (Barrows et al., 2018) were not included in the analysis. Samples were
not affect the samples (F. Liu et al., 2019). For this reason, samples were filtered using glass fiber filters with a pore diameter of 0.45 μm
collected on dry days. Wastewater samples (influent and effluent) were (Whatman GF/F) using vacuum filtration. The filters were placed in

2
G.E. Üstün et al. Environmental Pollution 310 (2022) 119890

Fig. 2. Number of MPs in wastewater and sludge samples.

glass petri dishes and left to dry for 24-h at room temperature. The filters database or standards was evaluated when a minimum of ≥0.7 simi­
were then visually examined under a stereo microscope. larity was obtained (Magni et al., 2019).

2.4. Extraction of MP from sludge 2.6. Quality control

S1 and S2 samples were placed in clean glass bottles (2 L) using a All glassware and equipment were rinsed with distilled water before
stainless steel container. The S3 sample was placed in 500 mL glass use to avoid potential contamination during sampling and laboratory
bottles with a volume of 250 g (wet weight) using a stainless steel processing. The dried glassware and equipment were then covered with
spatula. All sludge samples are covered with aluminum foil to prevent aluminum foil (Radityaningrum et al., 2021). In order not to affect the
possible contamination and stored in a 4 ◦ C refrigerator until analysis. test results of MPs that may be present in the environment and cause
All sludge samples dried at 60 ◦ C for 15–20 days in glass beaker (Jiang contamination; glass and metal equipment were preferred instead of
et al., 2020). After weighing the dry samples by 10 g, density separation plastic, 100% cotton lab coat was used, filtered samples were stored in
was performed with saturated NaCl solution. Especially in sludge sam­ closed glass petri dishes, all glass after the experiment, the items were
ples, it is preferred to separate the MP particles from the sludge by washed with tap water and then 2 times using distilled water (Bayo
density separation before purification (Gies et al., 2018; Magni et al., et al., 2021; Prata et al., 2019). Before the experiments, the bench was
2019). Sludge sample after drying was placed in a beaker, and a satu­ wiped 3 times with 70% ethanol and distilled water (Xu et al., 2021).
rated NaCl solution was added in a ratio of 1:2 (V/V) placed on 300 rpm
a stirrer for 1 h while stirring, and then immersed overnight using glass 2.7. Data analysis
separation funnel. This procedure has been repeated 3 times to prevent
possible MP losing. After the separation, the supernatant was filtered The average values and standard deviations of samples were calcu­
and digested according to the wastewater sample treatment method. lated, which was expressed as mean ± standard deviation (std). All the
Differently, since the organic content of the sludge samples is thought to data were initially tested for normality (Shapiro-Wilk Test) and homo­
be high, the purification process was carried out by adding H2O2 and geneity of variance (Levene’s Test). One-way analysis of variance
FeSO4 solution, 2 times as much as the wastewater samples. (ANOVA) was used to investigate the significance of differences in the
number of MPs between different stages in the treatment process. The
2.5. MP quantification and characterization post-hoc Tukey test was used to determine which groups differed
significantly from each other (p < 0.05). The tests were performed in
MPs were classified according to size (300–500 μm, 501–1000 μm, SPSS 26.0 software and the level of statistical significance was set at p <
1001–3000 μm and 3001–5000 μm); shape (fiber, film, fragment, and 0.05.
granular), and colour (white, black, transparent, red, blue, yellow/or­
ange, green, pink, and purple) were also recorded. Firstly, the mem­ 3. Results and discussion
brane filters were studied under a dissecting LEICA EZ4E
stereomicroscope (8-35x objective combined with a digital camera). The 3.1. The abundance of MPs in treatment stages
series of images obtained from the stereomicroscope was stacked and
the particle number, shape, colour, and size of the MPs were recorded The abundance of MPs at the WWTP influent is affected by several
with the help of LibreOffice Draw Imaging Software (version 4.2.7.2). factors, including the population of the watershed served by the WWTPs,
After visual inspection, the particles were rinsed with Milli-Q water to industrial facilities in the area, and the level of urban development (Raju
remove residual residue and a representative fraction (~10%) greater et al., 2020). The wastewater samples W1, W2, and W3 reflect the dis­
than >300 μm (Blair et al., 2019) was randomly taken to determine the tribution of MPs after treatment in various structures in the WWTP. The
polymer type (Raju et al., 2020). The measurements of all samples using abundance of MPs at these three points is 135.3 ± 28.0, 78.3 ± 38.6,
the ATR-FTIR spectroscopy (PerkinElmer) instrument in the range of and 8.5 ± 4.7 n/L, respectively (Fig. 2). The results showed that MP was
4000–400 cm− 1 were made with the attenuated total reflectance (ATR) removed from wastewater with a removal rate of 93.7% and transferred
technique, and the measurement parameters were 10 scans at a scan to the sludge. Wastewater data was homogeneously and normally
speed of 0.20 cm s− 1 with spectral resolution of 4 cm− 1. Spectra were distributed (p > 0.05). The MP abundance in the W3 significantly
compared between molecules in the system’s built-in database. The decreased compared to W1 (One-way ANOVA, p < 0.05). The Tukey test
PerkinElmer software (PerkinElmer Spectrum version 10.5.1) library showed that a significant difference between the W1 and W3. The
was used to determine the relevant polymer type for the spectra (Jung abundance of MPs reported in WWTP effluent varied between 0.13 and
et al., 2018; Raju et al., 2020). Positive match between samples and 129.13 n/L (Lv et al., 2019; Cunsolo et al., 2021). Due to the high MP

3
G.E. Üstün et al. Environmental Pollution 310 (2022) 119890

Fig. 4. The relative percentage (%) of the shapes of the MPs during treat­
ment processes.

Fig. 3. The relative percentage (%) of the sizes of the MPs during treat­
difficulties in the collection and analysis of small size MPs (e.g. <300
ment processes.
μm), it was stated that a significant portion (80.5%) of the studies in
aquatic environments were performed with larger size MPs (Conkle
removal efficiency in WWTPs, a significant amount of MP is retained in
et al., 2018). For this reason, MPs quantifications could be under­
the sewage sludge (Lofty et al., 2022). Removal rates of MPs in waste­
estimated (Carr et al., 2016).
water on a unit basis were calculated as 41.3% (W1–W2), 89.1%
(W2–W3). MPs with a higher density than water can be removed by
3.3. Shape of MPs
physical precipitation in the grit chamber (Sun et al., 2019; Yang et al.,
2019). In the secondary sedimentation tank, MPs are attached to the
The fragment and fiber occupied a significant proportion
suspended solids or wrapped in activated sludge in the wastewater and
(47.5–58.5% and 20.3–30.9%, respectively) among all of the WWTP
removed by settling (Bretas Alvim et al., 2020; Okeke et al., 2022).
units (Fig. 4), while granular and film occupied a relatively small pro­
The abundances of MPs in sludge samples of S1, S2, and S3 are 167
portion (10.3–18.4% and 4.6–10.0%, respectively). In the W1, the
± 27.2 × 102 n/kg, 179 ± 22.5 × 102 n/kg, and 95 ± 22.8 × 102 n/kg,
fractions of fragments, fibers, granular and films are 50.6%, 27.7%,
respectively (Fig. 2). Sludge data was homogeneously and normally
15.2%, and 6.5%, respectively. Proportions of fragments and granular
distributed (p > 0.05). The ANOVA showed no significant difference
decrease from 50.6% to 15.2% in the influent to 47.5% and 13.6% in the
between the abundance of sludge units (p < 0.05). While the solids
effluent, respectively.
concentration of the sludge increases in the sludge thickening tank, the
In contrast, the percentage of fibers and films increases from 27.7%
sludge volume is reduced. The abundance of MPs in the sludge thickener
to 6.5% in the influent to 30.9% and 8.1% in the effluent, respectively.
than in the sludge cake means that a significant amount of MP is
The most frequently observed MP shapes in wastewater samples were
returned to the treatment system via rejected water. It has been noted
fragment (58.5%) and fiber (27.7%), followed by granular (15.2%) and
that the dehydrated sludge contains 54% less MP than the previous
film (8.1%). The proportion of fibers increased from 27.7% at the
aerobically digested sludge (Alavian Petroody et al., 2021).
influent to 30.9% in the effluent, and it has been reported that due to the
small size and morphology of the fibers, they can release through the
3.2. Size of MPs treatment stages to the environment (Talvitie et al., 2017).
In sludge samples, the shape distribution was observed as fragment
The size distributions of MPs of wastewater and sludge samples (57.9%), fiber (26.4%), granular (18.4%) and film (11.1%). Fragments
collected in various parts of the WWTP are shown in Fig. 3. The are the dominant MP shape in both the water and sludge samples similar
500–1000 μm and 300–500 μm MP were the common size of MPs in all to data previously reported (Lv et al., 2019; Zhang et al., 2021). Frag­
wastewater samples, accounting for 46.2%–32.4% (W1), 53.7%–22.7% ments are usually related to anthropogenic activities and the decom­
(W2), 29.9%–45.3% (W3), respectively. Vardar et al. (2021) found that position of larger plastics (Vianello et al., 2013; Wei et al., 2020). Fibers
the dominant size range was 500–1000 μm in wastewater samples, and in wastewater often originate from the textile and tourism industries; the
1000–2000 μm and then 500–1000 μm in sludge samples. Larger MPs daily washing of clothes contributes to most of the fibers in WWTPs (Sun
(>3000 μm) decrease along wastewater treatment units (from 6.8% in et al., 2019). A garment made from synthetic materials can release more
W1 to 3.4% in W3) while increasing in sludge samples (from 3.4% in S1 than 1900 fibers per wash (Browne et al., 2011). As with the two species
to 4.5% in S3). Yang et al. (2021) note that large MPs decreased during (fragment and film) in all samples in this study, similar results were
purification. reported by Murphy et al. (2016), who found that MP species in
During WWTP units, large MP particles become smaller particles due wastewater (fragment 67.3% and film 18.5%). On the whole, the dis­
to wear and fragmentation (X. Liu et al., 2019) and therefore small MP tributions of MPs of different shapes among WWTP units are similar,
particles can be found in high proportion in WWTP effluent (Jiang et al., with no significant differences.
2020). Size distribution percentages of W1 and W2 samples are close to
each other since the MP removal is not at an effective level in the screen 3.4. Colour distribution of MPs
and grit chamber units. Smaller particle size MPs were detected in the
return sludge, sludge thickener and filter cake especially the 500–1000 Colour distribution in wastewater and sludge samples is shown in
μm and 300–500 μm MP, in which the proportion was 60.7%–20.2% Fig. 5. MPs in wastewater samples were black (35.3–45.6%), followed
(S1), 54.3%–27.1% (S2), 44.44%–26.48% (S3), respectively. Jiang et al. by transparent (19.5–27.1%), blue (9.7–13.9%), white (8.5–9.7%), and
(2020), have found that MPs of 500–1000 μm are common in waste­ red (5.5–7.6%) colour distribution. In sludge samples, most of the MPs
water and sludge samples in studies conducted and that the removal rate found were black (29.0–40.4%), followed by transparent (29.7–34.3%),
of small-sized MPs in wastewater is low. Nevertheless, due to the blue (9.5–12.2%), white (5.7–8.0%), and red (6.6–7.2%).

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G.E. Üstün et al. Environmental Pollution 310 (2022) 119890

Fig. 5. The colour distribution of MPs in WWTP units. (For interpretation of the references to colour in this figure legend, the reader is referred to the Web version of
this article.)

Fig. 6. Type characterization percentage of MPs in the WWTP. A) analysis transmittances of ATR-FTIR spectra of various MPs identified B) the percentage of MPs
influent (inner ring) and effluent (outer ring) wastewater samples. C) the percentage of MPs sludge thickener (inner ring) and sludge cake (outer ring) samples.

Other colours were detected below 5%. Black, transparent, white and 3.5. Type of MPs
blue colours are dominant in all samples. In many studies, black,
transparent, gray, and white colours dominate and these are similar to A total of 791 particles (365 in wastewater samples and 426 in sludge
data previously reported ones (Zhang et al., 2017; Li et al., 2018; Long samples) were detected in this study, and 325 particles (146 in waste­
et al., 2019). Vardar et al. (2021), found black and blue colours to be water samples and 179 in sludge samples) were confirmed to be plastic
dominant in wastewater and sludge samples. Yang et al. (2019) deter­ using ATR-FTIR. The results demonstrate that 41% of the suspected
mined that black (36.60%), transparent (33.84%), and blue (11.88%) particles were confirmed as MP. Particles smaller than 300 μm were not
colours predominate in China’s largest municipal WWTP effluent, sug­ analyzed by ATIR-FTIR. 7 types of MP were detected in the samples.
gesting that the colour of MPs came from a number of different sources. They were PE, PP, PS, PET, PA, Ethylene vinyl acetate (EVA) and Styrene
The colour distribution is similar to this study. The predominance of acrylonitrile (SAN). Most of the other micro particles are the remaining
black and transparent MPs could be related to the plastic bags, bottles, contains calcium stearate and glycerin, oleic acid, monooleate, cellulose
cling film, cups, and packaging bags that are used daily in our lives acetate, acrylic, lecithin, cellulose, wood chips, animal fur, silicone,
(Yang et al., 2021; Zhang et al., 2021). Coloured MP particles can latex, toothpaste residues, cosmetic raw materials, and silicates. The MP
contain harmful components such as heavy metals (Wang and Wang, types identified in WWTP and their distribution in treatment units are
2018), POPs, pathogens (Rochman et al., 2014), and it has been found shown in Fig. 6.
that organisms living in the aquatic environment consume more col­ According to Fig. 6 B, common types of MP observed in wastewater
oured plastic particles selectively (Oβmann et al., 2018; Su et al., 2020). samples were PP (36.8%), PE (31.0%), PS (11.8%), PET (8.0%), PA

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G.E. Üstün et al. Environmental Pollution 310 (2022) 119890

Table 1
Some newly reported MPs abundance, removal and release in wastewater treatment plants.
Country The Population Mesh size (μm) Treatment Influent Effluent Removal MPs Sludge Ref.
capacity of of served level concentration concentration (%) release concentration
WWTP (n/L) (n/L) (n/day) (n/kg or n/L)
(m3/day)

China 1.0 × 106 2.4 × 106 5000, 50 S/T 12.03 (±1.29) 0.59 (±0.22) >95 0.59 N/A Yang et al.
(±0.22) x (2019)
109
China N/A 3.5 × 106 355, 125, S 6.55 0.59 90.52 6.50 × N/A Long et al.
63,43 108 (2019)
5 6
Italy 4.0 × 10 1.2 × 10 5000,2000,63 S/T 2.5(±0.3) 0.4(±0.1) 84 1.6 × 106 RAS:113 (±57) Magni et al.
× 105 n/kg (2019)
China System A: N/A 500, 250, 125, S/T System A: 0.28 System A: 0.13 System A: System A: N/A Lv et al.
5.0 × 104 62.5,25 (±0.02) (±0.01) 53.6 6.5 × 106 (2019)
China 3.0 × 105 1.0 × 105 1700, 550,80 S/T 16 2.9 81.9 8.70 × DSU: 2.92 × 103 Ren et al.
108 n/kg (2020)
Spain 3.5 × 104 2.1 × 105 0.45 S 12.43 (±2.70) 1.23 (±0.15) 90.1 6.7 × 106 N/A Bayo et al.
(GGR) (2020)
5 6
China 6.0 × 10 3.1 × 10 80 S/T 126.0 (±14.0) 30.6 (±7.8) 75.7 N/A DSU:3.63 × 104 Jiang et al.
n/kg (2020)
SFC:4.63 × 104
n/kg
China WWTP A: N/A 149 S/T WWTP A: 23.3 WWTP A: 7.9 WWTP A: 9.1 × WWTP A (SFC): Tang et al.
7.0 × 104 S/T (±2.0) (±1.1) 66.1 1010 13.4 (±0.7) n/L (2020)
WWTP B: WWTP B: 80.5 WWTP B: 30.3 WWTP B: WWTP B (SFC):
3.0 × 105 (±6.3) (±3.0) 62.7 63.4 (±3.8) n/L
Spain 1.62 × 104 7.041 × 104 0.45 T 3.78 (±0.48) 1.38 (±0.48) 64.26 1.6 × 107 N/A Bayo et al.
(2021)
Turkey 4.0 × 105 2.0 × 106 2000,50,25 S 72.6 8.2 84.7–93.0 2.2934 × SFC: 3.2 × 104 Vardar et al.
106 n/kg (2021)
Finland 3.018 × 1.6 × 105 300,100,20 S/T 61 0.8 99 0.02 × ES: 142 n/L Salmi et al.
104 109 SFC: 9.37 × 103 (2021)
n/kg
Japan 2.0 × 105 N/A 20 T 19.16 5.15 95.6 N/A SFC: 5.8 × 104 Nakao et al.
n/kg (2021)
England 1.9 × 105 4.1 × 105 100,38 S 2102.16 129.13 93 2.45 × 1.97 × 106 n/kg Cunsolo
107 et al. (2021)
China N/A N/A 0.45 S/T 288.5 22.9 92.1 3.4 × 109 RAS: 1.012 Yang et al.
(±10.2) × 104 (2021)
n/kg
BPF: 1.234
(±5.7) × 104 n/
kg
Thailand DS:1.2 × 2.27 × 105 1000, 500,50 S/T 77 (±7.21) 10.67 (±3.51) 96.97 2.8 SS: 2.63 Tadsuwan
105 (±183) (±1.26) × 104 and Babel
RS:3.0 × × 108 n/kg (2022)
105
Turkey 6.18 × 104 6.5 × 105 5000,3000, S 135.3 (±28.0) 8.5 (±4.7) 93.7 5.25 × SFC: 9.55 × 103 This study
1000,500,300 108 n/kg

Note: N/A- Not Available, S:Secondary, T: Tertiary, DS: Dry seasons, RS: Rainy seasons, DSU: Dewatering sludge unit, SFC: Sludge filter cake, DIS: Digested sludge,
GGR: Grit and grease removal, RAS: Recycled activated sludge. ES: Excess sludge, BPF: Belt press filter, SS: Sewage sludge.

(7.1%) at influent; PE (33.0%), PP (52.5%), PS (8.2%), PA (4.1%) and the effluent of 12 WWTPs in Germany (Mintenig et al., 2017), and MPs
PET (2.2%) at the effluent. Other types of MPs such as SAN and EVA with larger than 500 μm were determined in 10 of them. When the species
little proportion could be observed in all samples. A decrease in the distribution and percentage of these MPs are analyzed, the dominant
number of polymer species and a change in the dominant polymer type species are PE (59%) and PP (16%), which is similar to the current study.
were detected in wastewater samples at the influent and effluent of the In addition, 121 WWTPs from 17 countries were examined and the most
WWTP. The most common polymer types PE, PP, PS, and PET were common MP types in wastewater were reported to be PE (22%), PS
found in all samples. The detection of 4 of the 5 most produced plastic (21%), and PP (13%) (Yaseen et al., 2022).
types on a global scale in all samples is compatible with the use of plastic In sludge samples (Fig. 6C) observed MP types are; PE (38.5%), PP
materials (Geyer et al., 2017). Similarly, PP and PE were determined as (30.6%), PS (17.2%), PET (6.1%) at sludge thickener while PE (40.8%),
the most common species in WWTP influent and effluent (Long et al., PP (27.6%), PS (18.7%) and PET (8.0%) distributions were observed at
2019; Magni et al., 2019). In a sewage treatment plant in China (Yang the sludge cake. PA, SAN, and EVA with little proportion could be
et al., 2021), the ratio of MP species in water samples was found to be PP determined in samples. According to Fig. 6C, there is no significant
(33%), PE (23%), and PS (18%), respectively, which is similar to this difference in the polymer composition of the sludge samples. The
study. Materials containing PE, PP, and PS species are widely used in polymer composition of MPs in sludge was similar to that of influent. PP
toothpaste, cosmetic products, water bottles, food packaging bags, and and PE were determined as dominant species in all samples. The sig­
clothing. The dominance of these species also indicates that most of the nificant difference between samples is that PP increases in wastewater
WWTP influent originates from domestic wastewater (Carr et al., 2016). samples and decreases in sludge samples. This can be explained by the
In a study examining rural domestic WWTPs, it was reported that PP, PE, fact that the density of PP is less than that of water (X. Liu et al., 2019;
PS and PET they were the most common types in the wastewater, as in Yang et al., 2021). MPs removal is related to its density, which its type
this study (Wei et al., 2020). MP type and size analysis were examined in can determine. MPs that are denser than wastewater (e.g. PET:

6
G.E. Üstün et al. Environmental Pollution 310 (2022) 119890

0.96–1.45 g/cm3) are easily removed from wastewater by physical the environment. However, there are many MPs released to aquatic/
precipitation; they accumulate in sludge. terrestrial environments with high treated wastewater flow rates and
treatment sludge applications in agricultural lands as bio-solid fertilizer.
3.6. Amount of MPs released into aquatic/terrestrial ecosystems MPs continue to be a problem for human and ecosystem health due to
the increasing use of plastics worldwide. Therefore, it is suggested that
Sources contributing MP to aquatic environments, wastewater to integrate advanced treatment processes into WWTPs and use effective
(municipal and industrial) effluents (Dris et al., 2015; Magni et al., sludge disposal management practices (e.g. incineration and pyrolysis)
2019), sludge/biosolids (Mintenig et al., 2017; Crossman et al., 2020), to reduce the amount of MP released into the aquatic/terrestrial
urban surface runoff (Galafassi et al., 2019) and atmospheric deposition ecosystems.
(Cai et al., 2017). A recent study found that in wet weather, drainage
system overflow (wet weather flow) contributes approximately six times Credit author statement
the annual contribution of MPs to the watershed than the contribution of
WWTPs (Chen et al., 2020). MPs and other anthropogenic particles have Gökhan Ekrem Üstün: Conceptualization, Supervision, Writing-
been measured in Lake Ontario surface waters and other water sources Reviewing and Editing. Kübra Bozdaş: Visualization, Validation,
(rainwater runoff, agricultural runoff, and wastewater effluent). The Writing – original draft preparation. Tuğba Can: Methodology, Data
anthropogenic particle concentrations in the lake samples were curation, Investigation, Writing – original draft preparation.
measured as 0.8 n/L, while the amount from the water sources was 15.4
n/L, 13.3 n/L, and 0.9 n/L from the rainwater, effluent, and agricultural Declaration of competing interest
runoff, respectively (Grbić et al., 2020). The removal of MPs at high
rates by WWTPs cannot prevent the release of significant amounts of MP The authors declare that they have no known competing financial
into aquatic environments due to the large values of treated wastewater interests or personal relationships that could have appeared to influence
flow rates. Considering the average flow rate of the WWTP (61,800 the work reported in this paper.
m3/day) and the average MP amount from the effluent of 8.45 n/L, an
average of 525 million MPs per day is released into aquatic environ­ Data availability
ments. The use of treated wastewater in the study area for irrigation and
its discharge into the sea at the basin outlet cause pollution of aqua­ No data was used for the research described in the article.
tic/terrestrial environments with MP. The WWTP effluent is released
into the Nilüfer Creek and used for irrigation throughout the basin. This Acknowledgments
stream is the influent to the Marmara Sea (Üstün, 2009). Studies on MP
removal in WWTPs in recent years are presented in Table 1. The MP This research was conducted with the financial support of the
removal efficiency of observed in this study is in the same order as other Research Fund of The Bursa Uludağ University (No:BAP FGA
urban WWTPs, ranging from 63.41% to 99.6%. Advanced treatment 2021–322). The authors would like to thank Bursa Water and Sewerage
processes can be integrated into the WWTP to reduce the amount of MP Administration (BUSKİ) for their help in collecting the wastewater and
released into the aquatic environment. In the Netherlands, MP removal sludge samples during the experimental runs and Dr. Ahmet Aygün, and
rates were reported to be 88% and 97% for WWTPs without and with Dr. Yunus Kaya for their help in ATR-FTIR analyses.
advanced treatment, respectively (Leslie et al., 2017).
The abundance of MPs in the sludge cake is 9.5 ± 2.3 n/g, the sludge Appendix A. Supplementary data
disposal amount of WWTP is 81.5 tons/day, and the amount of MPs
accumulated in the sludge per year is calculated as 2.8 × 1011 MPs. Supplementary data to this article can be found online at https://doi.
Disposal of the sludge in the incineration plant prevents MP release in org/10.1016/j.envpol.2022.119890.
terrestrial environments. When sludge is applied to agricultural lands as
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