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Journal of Water Process Engineering 55 (2023) 104200

Contents lists available at ScienceDirect

Journal of Water Process Engineering


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

Abundance, characteristics and seasonal variation of microplastics in a


domestic sewage treatment plant in Nanjing, China
Juan Huang *, Jing Tuo , Luming Wang , Jiaming Liu
Department of Municipal Engineering, School of Civil Engineering, Southeast University, Nanjing 211189, China

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

Keywords: Sewage treatment plants are a potential route of microplastics (MPs) into the environment, hence it's urgent to
Microplastics investigate MPs in wastewater and sludge through lengthy sampling campaigns. In this study, a sewage treatment
Sewage treatment plant plant in Nanjing, China was chosen, seasonal variation of MPs in influent was analyzed by collecting samples
Seasonal variation
during a 12-month sampling campaign (at monthly intervals over a one-year period). Abundance and charac­
Abundance
Characteristic
teristic of MPs from different treatment stages were also investigated. The results showed that there was a
seasonal variation in the amount of MPs in influent and the abundance of MPs was significantly greater in
summer than other seasons. The average MPs abundance was 41.0 items/L and 3.0 items/L in influent and
effluent, with a total 92.6 % removal rate. Overall, 125–355 μm were the main size in each treatment section,
with fibers dominant shape and transparent main color. Additionally, the primary polymer compositions of MPs
were polyethylene (PE) and polypropylene (PP) using micro-Roman spectroscopy. The daily MPs emission from
effluent and sludge was estimated to be 300 million and 1274 million items/d, demonstrating that the sewage
treatment plant is an important source of MPs into the environment despite the high removal rate of MPs.

1. Introduction [11,12]. MPs can be easily ingested by many aquatic organism due to
small size and therefore enzymatic activity restriction, organ clogging,
Microplastics (MPs), which are typically described as solid polymer endocrine disruption, oxidative stress and even mortality may be caused
remnants smaller than 5 mm, become one of the new environmental [13]. Additionally, MPs have the potential to be carriers of some pol­
research hotspots due to their potential harm to ecosystems [1]. The lutants like persistent organic pollutants (POPs), heavy metals, and toxic
average annual increase in worldwide plastic production from 1950 to substance [14], which will probably raise the risk of MPs to aquatic
2020 reached 1.5 million tons [2]. The wide use of plastic materials and creatures [15]. In recent years, it's reported that MPs can also enter the
the inadequate management of plastic waste have led to an incremental food chain through various aquatic organism and pose potential risks to
trend of MPs in the environment. The presence of MPs was reported in human health such as the damage for digestion, reproduction, respira­
almost all environmental worldwide according to previous in­ tory and metabolism [16,17].
vestigations, such as natural water bodies, sediments, sewage treatment Sewage treatment plants, which are designed to deal with waste­
plants, and aquatic organisms [3–6]. MPs spread quickly on a worldwide water in physical, chemical, and biological processes, are identified as a
scale with storms, runoff, and winds and constitute a risk of pollution potential source of MPs entering the environment [18]. Although the
due to their great resistance to degradation, hydrophobic nature, and removal rate of MPs in most sewage treatment plants is achieved at >90
light weight [7,8]. It has been reported that the MPs' abundance in %, many MPs still enter the environment through high volume discharge
surface water of semi-enclosed bays in South Korea was up to 2 items/L of treated sewage [19]. It has been estimated that over 9.1 × 1010 MPs
[9], and Yan et al. investigated 26 sampling points in the Pearl River and were discharged daily via domestic wastewater in China [13]. Murphy
analyzed that the average abundance of MPs ranged from 8.9 to 19.9 et al. reported that around 6.5× 107 MPs per day enter the receiving
items/L [10]. Moreover, MPs have been found in indoor dustfall samples aquatic systems from a wastewater treatment plant in Scotland [20].
from Chinese cities at mass concentrations of 1550–120,000 mg/kg, as Moreover, the majority of MPs are retained in sewage sludge in raw
well as in atmospheric dustfall from Paris, Farburg and Germany wastewater. It's estimated that over 80 % of MPs enter the sludge during

* Corresponding author.
E-mail address: 101010942@seu.edu.cn (J. Huang).

https://doi.org/10.1016/j.jwpe.2023.104200
Received 4 June 2023; Received in revised form 17 July 2023; Accepted 21 August 2023
Available online 1 September 2023
2214-7144/© 2023 Elsevier Ltd. All rights reserved.
J. Huang et al. Journal of Water Process Engineering 55 (2023) 104200

Fig. 1. Schematic diagram of main stages of the sewage treatment plant and sampling points: influent (W1), outlet of the grit chamber (W2), effluent (W3),
sludge (S).

wastewater treatment, which poses another potential risk [21]. Millions down to under 80 % before being carried outside for disposal.
or more MPs enter the terrestrial environment through the use of sludge
produced in sewage treatment plants as fertilizer in agricultural regions 2.2. Sampling method
[22]. Therefore, it's essential to investigate the occurrence and charac­
teristic of MPs in sewage treatment plants to fully comprehend the Wastewater samples and sludge samples were taken three times each
possible risk they pose to our environment. However, most researchers' month from October 2020 to September 2021 (April–May in Spring,
findings were based on samples collected within a short period time, June–September in Summer, October–November in Autumn, and
which may lead to inaccurate results. Long et al. studied influents and December–March in Winter) at various locations shown in Fig. 1. The
effluents from several sewage treatment plants in Xiamen within couple sampling time was concentrated between 10:00 and 11:00 am in a single
of days [23]. Ren et al. collected samples from different treatment stages day. Additionally, each sampling needed to be triplicate. Exact 10 L of
of a wastewater treatment plant in Zhengzhou during less than a week wastewater and 30 g of sludge were collected at sampling locations in a
[24]. Zhang et al. collected water samples for MPs studies from each stainless steel bucket. The collected samples were sealed, transferred to
stage of a sewage treatment plant in Guilin during a 3-day period [25]. the laboratory and stored at 4 ◦ C for further analysis.
Since wastewater is closely related to human activities, it has been re­
ported that the emerging contaminants (such as pharmaceuticals) con­
centration varies over time [26], thus the presence of anthropogenic 2.3. Extraction of microplastics
MPs in wastewater may also change with time. Meanwhile, Hajji et al.
reported that there was a significant seasonal variation in MPs abun­ The method for extracting MPs from collected samples was devel­
dance in the influent of sewage treatment plants and the difference may oped through the adaptation and modification of previously published
have large implication on their estimation of the monthly mass load and works [27,28]. In our study, the chosen stainless steel sieves sizes were
actual MPs emission [27]. The MPs abundance and characteristic in (5000 μm, 355 μm, 125 μm, 63 μm, and 38 μm). The sieves were rinsed
influent have an essential impact on the sources and loadings of MPs with deionized water for three times after sieving to ensure all residual
pollution. Therefore, it's essential to accurately analyze the fluctuation were transferred to a 500 mL beaker properly. The sieved samples were
of MPs occurrence in influent of sewage treatment plants for a better placed in 90 ◦ C drying oven for at least 24 h until totally dry [23,29].
understanding of MPs load. The amount of chemicals needed for the subsequent wet peroxide
Studies on the presence and characteristic of MPs in sewage treat­ oxidation (WPO) was then calculated from the weight of the dried
ment plants effluent have been largely reported. However, the seasonal samples [29]. Then, 20 to 50 mL of a 30 % hydrogen peroxide (H2O2)
variation of MPs in influent and the occurrence of MPs among each solution and an equal volume of a 5 mol/L ferrous sulfate (FeSO4) so­
treatment stage are limited with few studies. Hence, a long-term (12 lution were added, and the mixture was heated and stirred at 70 ◦ C for
months), systematic and comprehensive investigation at a typical 30 min to fully react and eliminate the organic debris from samples.
sewage treatment plant in Nanjing, China was carried out in this Samples were let to cool down and then ZnCl2 (97 g/100 mL) was
research to study the seasonal changes of MPs in influent, as well as the added to facilitate density separation. Subsequently, 5–10 mL of hy­
distribution characteristic of MPs in different treatment stages to further drochloric acid solution was added to induce the dissolution of ZnCl2.
clarify the variation among the processes in the sewage treatment plant, The solution was transferred to a partition funnel, left to separate for 24
which can provide theoretical support for process optimization of MPs h, and the supernatant was filtered using a vacuum extraction machine
removal in sewage treatment plants. (nitrocellulose membrane of 5 cm diameter and 0.45 μm pore size).
Finally, the filters were placed in a clean and dry petri dish and allowed
2. Materials and methods to dry naturally at room temperature, while being loosely covered with
aluminum foil to avoid contamination.
2.1. Study location
2.4. Examination and identification of microplastics
Nanjing is located in the east of China, downstream of the Yangtze
River, and is one of the important central cities in China. In this study, In this study, MPs were identified using a stereomicroscope
wastewater and sludge samples were collected from a sewage treatment (PXS6555T-B5) combined with a micro-Roman spectroscopy (LabRam
plant in Nanjing (located at 45◦ 48′N and 126◦ 42′E). The projected ser­ HR800). According to the classification criteria of morphological char­
vice area for the sewage treatment plant is around 80 km2, receiving acteristics of MPs established in previous studies, all samples of sus­
wastewater from over 200,000 inhabitants. The design flow was pected MPs were detected by vertical optical microscope, and the
100,000 m3/day and approximately 80 % of the wastewater coming to abundance, color, size and shape of MPs in each sample were recorded.
the plant is domestic. Screening+cyclonic sedimentation tank is used for The suspected MPs then were examined using a micro-Roman spec­
the primary treatment, and Anaerobic-Anoxic-Oxic (A2O)+MBR are troscopy, operating at laser wavelengths of 785 nm and 532 nm. High
used for the total secondary treatment. The sludge is dewatered by belt resolution spectra were recorded in 400–4000 cm− 1 to identify the MPs,
type thickening, and after dewatering, the water content is brought compared to the spectra in the database.

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J. Huang et al. Journal of Water Process Engineering 55 (2023) 104200

also found a remarkable seasonal fluctuation in MPs abundance [23,30].


There are various factors influencing the temporal distribution of MPs
abundance in influent of sewage treatment plants, such as the rainfall,
average temperature, population densities, and the area of afforested
land [31]. The possible explanation for the high levels of MPs in summer
may be higher personal care product consumption and laundry waste­
water production [32,33]. MPs like the microbeads can often be found in
cosmetics and personal care products and a single wash of clothing can
release up to megabytes of MPs per liter [34]. Other factors might
include a rise in population over the summer because Nanjing is a
popular tourist destination and attracts a lot of visitors during the
summer holiday period (about 2776 ten thousand tourists shown in SI
Table S2), as well as a potential increase in the consumption of plastic
products. Furthermore, increased solar irradiation, which facilitates
quicker water evaporation, could account for the increased concentra­
tion of MPs in wastewater during the hot period [35]. The second-
highest average concentration was found in autumn, possibly as a
result of intense rainstorm events during the rainiest time of year in our
region, which caused urban overflow of soil-retained MPs into the
sewage system [36].The lower MPs abundance in winter may reflect a
Fig. 2. Abundance of MPs in Spring (April–May), Summer (June–September),
higher contribution of weather conditions, MPs become stuck in ice or
Autumn (October–November), and Winter (December–March).
snow due to cold temperatures, making it difficult to enter sewage
treatment plants [37]. However, different results were reported by Ben-
2.5. Quality assurance and quality control
David et al., who found higher MPs abundance in winter [38]. It may be
caused by regional disparity or climatic contrast, as China is a sub­
At each sampling site, the sampler was cleaned three times using
tropical wet monsoon climate while Israel is etesian climate. Further­
distilled water before each sampling to avoid cross-contamination of
more, the methods utilized for sampling, the volume of water used, how
MPs. Throughout the experiment, sample contact time with air was
the water is taken, the variations in analytical techniques, and whether
reduced and the use of plastic devices was avoided. A control group was
the influent is domestic or industrial can all affect the discrepancy [39].
set up, performed with the same experimental methods and steps to
Fig. 2 also shows the MPs seasonal variation in different treatment
assess the possible MPs contamination from the surrounding environ­
stages. The number of MPs after primary treatment reached 19.6 ± 3
ment, and no external MPs pollution was found.
items/L in Spring, 21.9 ± 2.6 items/L in Summer, 20.4 ± 3.5 items/L in
Two spiking recovery tests were conducted to evaluate the depend­
Autumn, and 17.2 ± 1.8 items/L in Winter. The concentrations were
ability of extraction method used in this study. 400 polystyrene (PS)
further reduced after secondary treatment and the range of variation
particles with diameters of 100 μm and 74 μm were added to the control
was narrowed, varying between 2.3 and 3.5 items/L. The seasonal
group while using the same sieving, digesting, and density separation
variability was highly attenuated in the effluent, as the MPs total
method as mentioned above. The detected PS particle counts were 367
removal rates of the plant were about 93.0 %, 92.3 %, 93.0 % and 93.8 %
and 354, respectively, with spiking recoveries of 91.75 % and 90.5 %. It
in Spring, Summer, Autumn, and Winter shown in Table 1. The perfor­
suggests that sampling-related contamination was in control and would
mance of treatment stages is not significantly impacted by seasonal
not interfere with experiments.
changes, which indicates the plant has a buffering effect on seasonal
variations in the influent. And the removal rate of MPs in treatment
2.6. Data analysis stages usually depends on the characteristics of MPs, such as physical
and chemical features [37].
SPSS 26.0 software was used for all statistical analyses. Tukey's
comparison test was used to investigate the significance of differences in 3.1.2. Seasonal characteristic of MPs in influent
the number of MPs between different seasons and treatment stages, and It is necessary to characterize the physical properties of MPs in
the level used for statistical analysis was set at p < 0.05. influent as they can imply distinct inputs and sources and may also affect
the sewage treatment plants performance. Fig. 3 depicts influent MPs
3. Results and discussion size, shape, color and type in each season to accurately estimate char­
acteristic of MPs entering to the sewage treatment plant.
3.1. Seasonal variation of influent MPs In this study, the largest quantity was discovered in the size range of
125 to 355 μm in influent, which accounted for 38.0 % in Spring, 35.3 %
3.1.1. Seasonal variation of MPs abundance in Summer, 32.9 % in Autumn, and 34.2 % in Winter (Fig. 3a). The size
Fig. 2 shows the changes in MPs concentration between the different range between 63–125 μm and 38–63 μm formed the second largest
seasons. The mean abundance of MPs in influent was substantially proportion: 28.1 % and 21.7 % in Spring, 26.5 % and 24.2 % in Summer,
higher (p < 0.05) in summer (45.8 items/L) compared to spring and 29.2 % and 24.2 % in Autumn, 29.2 % and 24.8 % in Winter, respec­
winter (39.2 and 37.9 items/L respectively). Long et al. and Bayo et al. tively. In the same time, only a few particles larger than 355 μm were

Table 1
Total removal rate % (T) and MPs removal % (M) in treatment stages at different seasons.
Spring Summer Autumn Winter

T M T M T M T M

Primary treatment 49.9 % 49.9 % 52.3 % 52.3 % 49.8 % 49.8 % 54.6 % 54.6 %
Secondary treatment 93.0 % 86.2 % 92.3 % 84.0 % 93.0 % 86.3 % 93.8 % 86.6 %

The bold figures represent the sewage treatment plant's cumulative efficiency in removing MPs after both treatment stages.

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J. Huang et al. Journal of Water Process Engineering 55 (2023) 104200

Fig. 3. Seasonal Characteristic of MPs in influent: size (a), shape (b), color (c), type (d). Ring from inner to outer indicates Spring, Summer, Autumn, and Winter,
respectively.

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J. Huang et al. Journal of Water Process Engineering 55 (2023) 104200

Fig. 4. (a) MPs abundance in wastewater and sludge samples (W1–3 was collected from influent, primary effluent, and secondary effluent, respectively, S was
collected from sludge). (b) Correlation between MPs and TSS (Data from W1, W2 and W3).

found: 4.5–7.5 items/L in samples. The higher proportion of small MPs Fibers were the predominant type of MPs in every season, repre­
in influent may be caused by the fact that MPs with larger particle sizes senting over 43.8 % in all samples and fragment formed the second
gradually break down into smaller MPs during migration [40]. The re­ largest proportion, while film and granular formed the lowest (Fig. 3b).
sults imply that MPs entering the sewage treatment plant tend to be The prevalence of fibers may be related to the discharge of fiber particles
relatively small in each season. from textile products after washing [41]. According to recent estimates,

Fig. 5. The relative percentage (%) of MPs during treatment stages: size (a), shape (b), color (c), type (d).

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J. Huang et al. Journal of Water Process Engineering 55 (2023) 104200

Fig. 6. The removal rate (%) of MPs during treatment stages: size (a), shape (b), color (c), type (d).

about 18,000,000 synthetic fibers were discharged into the washing example, PE is widely used in packaging, personal care product and food
water when 6 kg of synthetic product was washed in a washing machine containers, and PP is often used in water bottles [48]. Other studies have
[42]. Additionally, MPs utilized in personal care items including facial also found PP, PE, PS, and PET were dominant in influent of a rural
cleansing gels, toothpaste, masks, and soaps are most likely the source of domestic sewage treatment plant [49].
the granular [43]. And films are usually come from packaging, including
those of ready-made goods and shopping bags [44]. 3.2. MPs abundance and related results in treatment stages
The percentage color distribution of MPs is shown in Fig. 3c.
Transparent and blue were the main colors, their proportions for Spring, The distribution of MPs in each treatment stage was reflected in
Summer, Autumn, and Winter were 32.9 % and 24.6 %, 34.4 % and 24.2 wastewater samples W1, W2, and W3. The number of MPs at these three
%, 38.9 % and 24.2 %, 34.5 % and 23.0 %, respectively. The next were points was 41.0 ± 8.3, 21.6 ± 5.1, and 3.0 ± 1.3 items/L, respectively
white and black, while green accounted for the least in each season. The (Fig. 4a). It was noticed that the abundance of MPs in sludge was 18.2 ±
results were caused by large amount of PE in influent in each season 9.3 items/g (Fig. 4a). A sizable proportion of MPs were remained in
(Fig. 3d) since primary PE was predominantly transparent in color. The sludge. The Tukey test revealed that there was a significant difference in
variety of colors showed the complexity of the sources of MPs. Plastic MPs abundance between W1 and W3 (p < 0.05), with a total MPs
bottles, bags, cups, packaging bags and cling film utilized on a daily removal rate of 92.6 %.
basis could be the source of transparent and black MPs. Furthermore, The number of MPs removed by different stages in wastewater
due to the leaching, oxidation, and aging of dyes brought on by treatment varied. MPs removed by primary treatment ranged from 40.0
weathering and ultraviolet exposure in aquatic environment, the orig­ % to 55.0 %, while secondary treatment can remove up to 86.0 % MPs.
inal brilliant color of MPs may turn black or transparent [45]. Dyed MPs Large and suspended particles can be effective intercepted by grid and
may include hazardous substances like heavy metals, pathogens, and grit chamber, and MPs tend to adhere to solid particles, which allows
persistent organic pollutants [46,47]. them to be retained by the primary treatment process [50]. The larger
MPs with the type of PE and PP were dominant in each season, fol­ removal rate in secondary treatment may be related to adequate contact
lowed by PET and PS (Fig. 3d). And the least proportion was observed in time between MPs and wastewater to help them sink to the bottom in the
PES type class: 0.5–0.8 items/L from Spring to Winter (Fig. 3d). The biochemical tank. According to Carr et al., longer contact time facili­
results can be closely related to domestic wastewater taking up mostly tated the formation of biofilm on the surface of MPs [32]. And biofilm
proportion of influent in the studied sewage treatment plant as most of can be used as a substance to change the surface characteristics or
the plastic derivatives identified are used in household products. For density of MPs, which was conducive to their settlement [51].

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J. Huang et al. Journal of Water Process Engineering 55 (2023) 104200

Meanwhile, sludge flocs or bacterial extracellular polymers can facilitate stage. Different shape showed different removal characteristics in pri­
the aggregation of plastic particles during the biochemical reaction, mary treatment. The removal effectiveness of granular and fragment
which in turn led to the deposition of MPs [52]. was limited in primary treatment, only accounting for 31.0 % and 36.2
However, the study of MPs pollution remains as academic research. %. However, primary stage had better removal rate on fiber and film (p
It is not currently become a regular pollution monitoring indicator like < 0.05), with removal rates of 55.3 % and 53.1 %, respectively (Fig. 6b).
COD, organic carbon and other pollutants. Previous studies have tried to It has also been demonstrated by other studies that primary treatment
find a correlation between TSS and MPs and hence TSS might be used as can effectively remove fibers [58]. The removal rate of all shape of MPs
an indicator of MPs [53]. In this study, a strong linear correlation be­ by secondary treatment was significant (p < 0.05), while the removal of
tween MPs and TSS (rPearson = 0.98, p < 0.01) has been found (Fig. 4b), fibers was relatively low (Fig. 6b). On the one hand, the surface of fiber
which give an indication of the possibility that MPs abundance could be is typically smooth, while the rough and irregular surfaces of fragment,
estimated by SS content. film, and granular make them simple to remove by settling with the solid
particles [23]. On the other hand, the irregular and complex surface is
3.3. Characteristics of MPs in treatment stages more likely to support microbes, which further accelerates its
degradation.
3.3.1. Size
The size distributions of MPs of wastewater and sludge samples taken 3.3.3. Color
in various stages of the sewage treatment plant are presented in Fig. 5a. Seven different colors including red, blue, yellow, transparent,
38–355 μm were the common size of MPs, while 355–5000 μm white, black and green were observed in this study (Fig. 5c). MPs of
accounted for the least proportion. This was similar to the study by transparent color were the most common in all samples, accounting for
Conley et al. on the size of MPs in different stages of sewage treatment 38.0 % (W1), 31.0 % (W2), 36.0 % (W3), and 24.9 % (S), respectively.
plants [54]. 38–63 μm (39.4 %) accounted for the dominant size range in And the next is blue, black and white. In many researches, transparent,
effluent (W3) as large MPs could become smaller due to abrasion and white, blue and black colors dominate [23]. Lares et al. also found
breakage and therefore small MPs can be observed in high concentration transparent colors predominate in effluent of China's largest sewage
in sewage treatment plants effluent [55]. In sludge samples, the size treatment plant [29]. Vardar et al. suggested transparent and blue colors
distribution was observed as 355–5000 μm (31.6 %), 125–355 μm (28.2 to be the dominant in wastewater and sludge [59]. The average removal
%), 63–125 μm (21.1 %) and 38–63 μm (19.1 %). Larger particle size rate of red and blue MPs in primary treatment stage was low, which was
was the dominant in sludge. The size of MPs in sludge was bigger than 27.5 % and 14.6 % respectively (Fig. 6c), but the average removal rates
that in wastewater, according to Sherri et al., smaller MPs might stay of other colors were >40.0 %, with green removal rate reaching 100 %.
afloat in the water column, whereas larger ones were more likely to sink It's possible that the blue and red colors in influent were mostly small
to the bottom [56]. fragments or granular. Secondary treatment is effective in removing all
The size disparity caused a significant variation in removal rate be­ colors MPs, especially for yellow colors MPs (93.8 %).
tween sewage treatment facilities. The primary treatment was more Colors can also reveal the presence of chemical additions and the
effective in removing large-sized MPs with removal rates of 63.6 ± 5.8 possible environmental risk. For example, azo colorants, which give
% and 55.2 ± 3.3 % for 355–5000 μm and 125–355 μm, respectively (p transparent plastics their vivid clear color, are soluble and rapidly
< 0.05), and lower for 63–125 μm and 38–63 μm with 25.5 ± 5.0 % and migrate [60]. And brightly colored plastics are often created using heavy
32.4 ± 3.7 %, respectively (p > 0.05) (Fig. 6a). 63–125 μm and 125–355 metals like chromium, cobalt, copper, selenium, cadmium and lead
μm MPs can be effectively removed by secondary treatment (p < 0.05), [61]. Furthermore, a variety of aquatic species could selectively
with removal rate of 91.9 ± 6.2 % and 92.9 ± 4.2 % (Fig. 6a). The consume MPs of different colors, according to earlier investigations. For
difference in removal rate of MPs between primary and secondary instance, in Tokyo Bay [62], the majority of MPs in the digestive tracts of
treatment may be due to the water inlet mode. In the grit chamber, the Japanese anchovies were white or transparent (71 %). And Planktivo­
inlet flow rate was relatively high, making it challenging to create an rous palm ruff juveniles prefer to catch black MPs over blue or yellow
effective flocculation and clarifying impact. While in secondary treat­ MPs according to the study conducted by Ory et al. [63]. Therefore, the
ment process, the low flow velocity was more conducive for suspending large amount of white, blue and black MPs in the sewage treatment plant
smaller MPs. And activated sludge had a better precipitation and may be a potential source of pollution to aquatic environment and raise
adsorption rate on MPs in wastewater at low flow rates. Thus, the sec­ the risk to aquatic creatures.
ondary treatment had the capacity to remove small and low-density MPs
that the primary treatment was unable to remove. The same results were 3.3.4. Type
also obtained by Ren et al., who found primary treatment had a higher Six types of MPs were identified in W1, W2, W3, and S as shown in
removal rate for large-sized MPs, and secondary treatment had a higher Fig. 5d. PE and PP were the most common in all samples, making up
removal rate for small-sized MPs [24]. 32.6 % and 28.2 % in W1, 36.0 % and 28.0 % in W2, 20.0 % and 26.0 %
in W3, 23.4 % and 22.6 % in S, respectively. PE (23.4 %), PP (22.6 %),
3.3.2. Shape PS (14.9 %), PET (16.7 %), PA (15.9 %), PES (2.6 %) were identified in
Four types of MPs (granular, film, fiber, fragment) were observed in sludge samples, which is similar to the composition of MPs in influent.
W1, W2, W3 and S (Fig. 5b). Fiber and fragment accounted for a sizeable Similarly, the most common species in sewage treatment plants influent
percentage (46–56 % and 31–38 %, respectively) in all wastewater and effluent were determined to be PP and PE [64]. Yang et al. studied
samples, while a relative small percentage (7–16 % and 4–7 %, the component in a sewage treatment plant in China, the study found
respectively) was taken up by film and granular. Proportions of fiber and that PP (33 %), PE (23 %), and PS (18 %) were dominant in water
fragment increased from 46 % and 31 % in influent to 56 % and 33 % in samples [65]. Additionally, 121 sewage treatment plants from 17
effluent, respectively. Fiber and fragment were also the dominant MPs different countries were analyzed, and it was discovered that PE (22 %),
shape in sludge samples (Fig. 5b). Previous studies also suggested the PS (21 %), and PP (13 %) were the most prevalent MP types in waste­
dominance of fiber and fragment in wastewater and sludge samples water [66]. The most popular types of polymer consumed in China are
[57]. The slender and long shape of fibers made it difficult to be removed PE, PP, and PS. As a result, the structure of plastic polymer consumption
by process. Furthermore it has been noted that fibers can be released in China may mirror the polymer type in sewage treatment plants.
throughout the treatment stages to the environment because of their The removal rate of PP and PE was limited in primary treatment,
small size and form [21]. only accounting for 39 % and 47 % (Fig. 6d). However, pretreatment
Fig. 6b shows the removal rate of each shape of MPs in different stage had better removal effect on PET, PA and PES, ranging from 50 %

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J. Huang et al. Journal of Water Process Engineering 55 (2023) 104200

Table 2
MPs abundance, removal, and release in sewage treatment plants.
Location Water Sludge Ref.

Influent Effluent Removal MPs released MPs released


(items/L) (items/L) (%) (million items/day) (million items/day)

India 1860.0 ± 265.0 148.0 ± 51.0 92.0 30,000 – [69]


Xian, China 288.5 22.9 92.1 3400 – [41]
Thailand 77.0 ± 7.2 2.3 ± 1.5 97.0 280 ± 183 – [70]
Ningbo, China 78.0 ± 2.9 6.0 ± 2.8 92.3 140–230 1300 [71]
Madrid, Spain 171.0 ± 42.0 12.8 ± 6.3 92.5 300 2191 [22]
Zhengzhou, China 16.0 2.9 81.9 870 315 [24]
Australia 92.0 0.2 99.8 1020 4100 [72]
Xiamen, China 13.7 1.7 87.4 650 – [23]
Nanjing, China 41.0 ± 8.3 3.0 ± 1.3 92.6 300 1274 This study

to 60 % (Fig. 6d). Roberto et al. reported that the removal effect of MPs treatment stages was discussed in a domestic sewage treatment plant in
was positively correlated to its density, which played an important role Nanjing, China. The 12-month sampling campaign revealed that MPs
in its rise and fall in environment [67]. The densities of PE, PP, PET, PA abundance in influent fluctuated with seasons and summer had a larger
and PES are 0.91–0.97, 0.91, 1.38, 1.15, and 1.37 g/cm3, respectively. number of MPs entering the sewage treatment plant. Additionally,
MP polymers denser than sewage are more easily removed by physical 125–355 μm accounted for a substantial part of size range in each
precipitation, whereas smaller or medium density polymers float in the treatment stage. Fiber was the major shape with transparent main color
middle and upper layers of wastewater and are difficult to remove with in wastewater and sludge samples. And PE and PP were the main
other solids [23]. The average removal rate of secondary treatment for composition of MPs. However, although there was 92.6 % reduction in
PA was relatively low (76 %), while for other components exceeded 80 MPs in the sewage treatment plant, about 300 million items MPs per day
%. Overall, the sewage treatment plant had a good interception and are still released to aquatic environment from treated wastewater and
removal effect on all components of MPs, with an average removal rate 1274 million items MPs are released to terrestrial habitats per day due to
of >85 %. treated sludge applications in agricultural lands as bio-solid fertilizer.
Therefore, it's suggested to pay attention to enhancing techniques in
3.4. The fate of MPs in the sewage treatment plant sewage treatment plants to lessen the MPs abundance discharged into
environment. For example, tertiary treatment may be used for further
The MPs balance analysis in treatment stages would help to under­ MPs reduction, and sludge disposal must be taken seriously to reduce
stand the fate of MPs. The detailed calculation of MPs count balance can MPs pollution in soil. In addition, sewage treatment plants should
be found in SI Text S1 and Table S1. It's observed that the removed MPs employ different treatment techniques due to the different MPs inputs
between W2 and W3 were 1417 million items/day, while the MPs in into wastewater over the month in order to efficiently eliminate con­
sludge were 1274 million items/day. The missing 10.1 % of the MPs taminants from wastewater.
count balance are expected to arise from MPs loss in the process of
sludge treatment, as MPs can either be biological degradation or broken CRediT authorship contribution statement
down to particles below the size detection limit [68]. Also, fluctuation of
daily flow and sludge disposal would lead to the discrepancies, as well as Juan Huang: Writing – review & editing, Funding acquisition,
the sampling and measuring uncertainties. Methodology, Project administration. Jing Tuo: Investigation, Data
The potential MPs release to environment can be calculated based on curation, Writing – original draft. Luming Wang: Investigation, Soft­
the count balance. About 300 million items MPs were released into ware, Methodology. Jiaming Liu: Methodology, Investigation.
environment per day based on average flow rate of the sewage treatment
plant. And the daily MPs emission in other sewage treatment plants was Declaration of competing interest
also as high as 300–30,000 million items as shown in Table 2. Patil et al.
stated that roughly 30,000 million items MPs were released into aquatic The authors declare that they have no known competing financial
environment per day on average at a treatment plant in India [69], interests or personal relationships that could have appeared to influence
which was around 100 times the emission of this study. Another study the work reported in this paper.
also reported that approximately 3400 million items MPs were dis­
charged to environment daily from a sewage treatment in Xian, China Data availability
[41]. Another potential route for the release of MPs to environment is
the use of sewage sludge on agricultural fields. Based on the count Data will be made available on request.
balance established in this study, a daily discharge of 1274 million items
MPs could be released to the terrestrial environment. The daily MPs Acknowledgements
emission from sludge phase in other sewage treatment plants was also
about 315–4100 million items based on the recent studies. Li et al. This work was supported by grants from the Jiangsu Provincial key
studied the total sludge production in China and estimated that the daily Research and Development Program (Grant No.BE2022831).
average amount of sludge-based MPs entering to environment can reach
to 427 billion items [31]. All of these results show that large amounts of Appendix A. Supplementary data
MPs were released from sewage treatment facilities to environment,
despite having a relatively high removal rate. Supplementary data to this article can be found online at https://doi.
org/10.1016/j.jwpe.2023.104200.
4. Conclusion

In this study, the seasonal variations of MPs in influent were


analyzed, and occurrence as well as characteristics of MPs in different

8
J. Huang et al. Journal of Water Process Engineering 55 (2023) 104200

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