A Review of The Removal of Microplastics in Global Wastewater Treatment

Environment International 146 (2021) 106277
Contents lists available at ScienceDirect
Environment International
journal homepage: www.elsevier.com/locate/envint
Review article
A review of the removal of microplastics in global wastewater treatment

plants: Characteristics and mechanisms
Weiyi Liu a, Jinlan Zhang a, Hang Liu a, Xiaonan Guo a, Xiyue Zhang a, Xiaolong Yao b,
Zhiguo Cao c, Tingting Zhang a, *
a
Department of Environmental Science and Engineering, Research Centre for Resource and Environment, Beijing University of Chemical Technology, Beijing 100029,
People’s Republic of China
b
Department of Environmental Science and Engineering, Beijing Technology and Business University, Beijing 100048, People’s Republic of China
c
School of Environment, Henan Normal University, Xinxiang 453007, People’s Republic of China
A R T I C L E I N F O A B S T R A C T
Handling Editor: Frederic Coulon Wastewater treatment plants (WWTPs) are considered to be the main sources of microplastic contaminants in the
aquatic environment, and an in-depth understanding of the behavior of microplastics among the critical treat
Keywords: ment technologies in WWTPs is urgently needed. In this paper, the characteristics and removal of microplastics in
Microplastics 38 WWTPs in 11 countries worldwide were reviewed. The abundance of microplastics in the influent, effluent,
Wastewater treatment technology
and sludge was compared. Then, based on existing data, the removal efficiency of microplastics in critical
Environmental toxicity
treatment technologies were compared by quantitative analysis. Particularly, detailed mechanisms of critical
Fate
Meta-analysis treatment technologies including primary settling treatment with flocculation, bioreactor system, advanced
oxidation and membrane filtration were discussed. Thereafter, the abundance load and ecological hazard of the
microplastics discharged from WWTPs into the aquatic and soil environments were summarized. The abundance
of microplastics in the influent ranged from 0.28 particles L− 1 to 3.14 × 104 particles L− 1, while that in the
effluent ranged from 0.01 particles L− 1 to 2.97 × 102 particles L− 1. The microplastic abundance in the sludge
within the range of 4.40 × 103–2.40 × 105 particles kg− 1. In addition, there are still 5.00 × 105–1.39 × 1010
microplastic particles discharged into the aquatic environment each day Moreover, among the critical treatment
technologies, the quantitative analysis revealed that filter-based treatment technologies exhibited the best
microplastics removal efficiency. Fibers and microplastics with large particle sizes (0.5–5 mm) were easily
separated by primary settling. Polyethene and small-particle size microplastics (<0.5 mm) were easily trapped by
bacteria in the activated sludge of bioreactor system. The negative impact of microplastics from wastewater
treatment plant was worthy of attention. Moreover, unknown transformation products of microplastics and their
corresponding toxicity need in-depth research.
1. Introduction area (Thompson et al., 2004). As a result, microplastics always cause

chronic toxicity due to their accumulation in organisms (Li et al., 2018).
Microplastics widely occur in the atmosphere (Abbasi et al., 2019), Wastewater treatment plants (WWTPs) are considered to be the main
soil (Guo et al., 2020), ocean (Wang et al., 2020b), freshwater (Han recipients of terrestrial microplastics before entering natural aquatic
et al., 2020) and even in the sediment of an Arctic freshwater lake systems (Sun et al., 2019), which convert primary microplastics into
(González-Pleiter et al., 2020). They can adsorb pollutants, such as secondary microplastics. The microplastics occurring in municipal
polycyclic aromatic hydrocarbons (Sørensen et al., 2020), heavy metals wastewater commonly originate from daily human life activities. For
(Foshtomi et al., 2019), polybrominated diphenyl ethers (Singla et al., example, polyester and polyamide components are commonly shed from
2020), pharmaceutical and personal care products (Liu et al., 2019a; Ma clothing during the laundry process (Napper and Thompson, 2016), and
et al., 2019c) from environmental media due to their small volume personal care products such as toothpaste, cleanser and shower gel enter
(particle debris size usually smaller than 5 mm) and high specific surface WWTPs resulting from our daily use (Magni et al., 2019). Moreover, the
* Corresponding author.
E-mail address: [email protected] (T. Zhang).
https://doi.org/10.1016/j.envint.2020.106277
Received 27 July 2020; Received in revised form 6 November 2020; Accepted 7 November 2020
Available online 20 November 2020
0160-4120/© 2020 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
W. Liu et al. Environment International 146 (2021) 106277
plastics in garbage are decomposed by microorganisms in the leachate 2. Methods

and then are discharged into WWTPs (Durenkamp et al., 2016). In
addition, the microplastics floating in the atmosphere, which have been 2.1. Data collection
emitted by plastics industries and vehicles, also converge in WWTPs via
atmospheric deposition (Liu et al., 2019c; Mintenig et al., 2017; Wright The publications were obtained by searching all databases in the
et al., 2020). It has been proven that untreated microplastics are China National Knowledge Infrastructure and Web of Science using
commonly discharged from WWTPs, enter water bodies, and eventually search terms such as microplastic, wastewater treatment plant, sewage
accumulate in the environment (Carr et al., 2016). Therefore, it is urgent treatment plant, and sludge. The search included all available publica
to study the performance of microplastic by different treatment tech tions until April 2020. The search results indicated that microplastic was
nologies in WWTPs and understand the mechanism of removing first defined in Science by Thompson in 2004 (Thompson et al., 2004).
microplastics to reduce the amount of microplastics entering the natural The first study on the occurrence and removal of microplastics in
aquatic system. However, few pieces of research have been found to WWTPs was published in 2015 by Talvitie et al. (2015). Relevant pub
summarize the microplastics removal mechanisms of the critical treat lications over the past three years (2018–2020) have been reviewed. The
ment technologies in the WWTPs. publications were individually assessed to eliminate irrelevant articles
According to previous studies on the microplastic treatment tech based on their abstracts, tables, and figures. Ultimately 23 highly rele
nologies in WWTPs, microplastics were not completely removed from vant papers covering microplastics in global WWTPs were considered
wastewater by these treatment technologies. For example, after the for meta-analysis. Data retention criteria in publications included: 1) the
preliminary, primary, secondary and tertiary treatment processes in a name of the corresponding treatment process and microplastic abun
WWTP in the UK, the overall abundance decreased by 6%, 68%, 92% dances of the influent and effluent; 2) polymer types, shapes and particle
and 96%, respectively (Blair et al., 2019). Mechanical, chemical, and sizes of microplastics and their abundances; 3) studies are independent
biological treatment processes removed approximately 99% of the of each other and there are no duplicate studies; and 4) basic informa
microplastics entering a WWTP (Ziajahromi et al., 2016). After treat tion of WWTPs (location, daily capacity, serving population, etc.).
ment, the removed microplastics were primarily transferred to the GetData Graph Digitizer (v.2.25) was used to extract the data of the
sludge phase (Ngo et al., 2019). microplastic abundances (the influent and effluent of treatment tech
Moreover, other noteworthy results, which are different from the nology) and removal efficiency presented in the graph.
results mentioned above, were obtained. For the same treatment process Due to the difficulty in measuring the mass of microplastics, the
of microplastics, the microplastics removal efficiencies differed among behavior from the perspective of the quantity abundance (particle L− 1)
various WWTPs. For example, aeration grit chambers, anaerobic-anoxic- was evaluated in this study. The microplastic abundance and removal
oxic (A2O) and advanced oxidation (UV and O3) processes were adopted efficiency were generally provided in the publications. Otherwise, non-
as microplastic treatment methods in a Beijing WWTP, and their detection was assigned a zero value (Yang et al., 2018). It was clear that
microplastics removal efficiencies were 58.84%, 54.47% and 71.67%, the inconsistent microplastic shape nomenclatures and size classes were
respectively (Yang et al., 2019). However, the microplastics removal discussed in the existing research publications. An ambiguous nomen
efficiencies for the same treatment processes in a Shanghai WWTP clature inhibits research progress, leading to confusion and miscom
decreased to 49.56%, 26.01%, and 0.78%, respectively (Jia et al., 2019). munication (Hartmann et al., 2019). For analysis convenience, the film
These results indicate that it is very challenging to understand the role of or sheet, pellet or spherical or bead and particle or granule were
a given treatment process in microplastics removal in a WWTP via a consistently renamed film, pellet and particle, respectively. The micro
single investigation. Moreover, the conventional study methods on plastic size classifications were 100 μm, 500 μm, 1 mm and 5 mm in
microplastics removal are mainly based on qualitative analysis rather previous studies (Wang et al., 2019). Thus, this study divided the size in
than quantitative analysis (Ngo et al., 2019). Therefore, it is necessary to the meta-analysis as smaller than 0.5 mm, 0.5–1 mm and 1–5 mm.
develop new methods to qualitatively assess the removal performance of
microplastics in WWTPs.
In recent years, as a statistical method for the quantitative analysis of 2.2. Quantitative meta-analysis
a series of independent features of the same object, meta-analysis has
been increasingly applied to analyze wastewater problems in a more Meta-analysis was performed in R-project for Statistical Computing
scientific manner (Erni-Cassola et al., 2019). For example, meta-analysis (version 3.6.2) using the meta package (Schwarzer, 2007). The micro
results indicated that photocatalysts generally attain the highest diaz plastic data obtained from each independent study was analyzed, and
inon elimination efficiency with an average efficiency of 79.2% (95% the microplastics removal of different treatment technologies was
confidence interval: 76.8%–81.5%) (Malakootian et al., 2020). Another compared. The risk ratio (RR) value was assigned as the effect size in a
meta-analysis study revealed that membrane bioreactor systems might single study. The calculation method of the RR value can be found
present the highest removal efficiency of organic trace contaminants in elsewhere (Schwarzer, 2007). An RR value lower than 1 indicated that
wastewater (Melvin and Leusch, 2016). To date, no qualitative assess microplastics could be removed, and lower the value is, the better the
ment of the removal of microplastics in WWTPs via meta-analysis has removal is. The effect size in the meta-analysis was a weighted average
been reported. It is believed that the meta-analysis approach can provide of each single study. A study with a higher weight value was supposed to
a better understanding of the characteristics of microplastics in WWTPs impose a greater influence on effect size. The weights were determined
and a more accurate estimate of microplastics removal in critical by the random effects model of meta-analysis, due to the high hetero
wastewater treatment technologies. geneity among the studies (McKenzie et al., 2016).
In this study, the critical microplastic treatment technologies in AI
global WWTPs are reviewed. Meta-analysis was first performed to RR = (1)
AE
identify the optimal microplastics removal technology. Thirty-eight
WWTPs in eleven countries worldwide were investigated in terms of where AI and AE denote the event probabilities for the experimental and
the occurrence, transfer, and removal mechanism of microplastics in control groups, respectively.
different critical treatment technologies. The discussion focused on the In this study, meta-analysis was used to investigate the removal ef
removal behavior of various microplastic shapes, polymer types, and ficiency of microplastics in the primary, secondary, and tertiary treat
particle sizes. In addition, the risks of microplastics to the aquatic and ment processes, and also to compare the removal efficiency between
soil environments were also evaluated. The results are instructive for a critical treatment technologies. Further, we also analyzed the removal
scientific understanding of the fate of microplastics in WWTPs. efficiency of different classifications of microplastics (shapes and
2
particle sizes) in these treatment processes.

I2
τ2 = W (4)
1 − I2
2.3. Heterogeneity and publication bias
df Σωi
W= ∑ (5)
The heterogeneity test aims to determine whether genuine differ (Σωi )2 − ωi 2
ences exist between study results (Higgins et al., 2002). The heteroge
neity can be expressed by I2, τ2, or the Cochran Q test (Higgins et al., where ωi is the weight of each study, θi is the effect value (RR) of each
2003; Langan et al., 2019). The I2 quantity, ranging from 0% to 100%, study, θ is the average of the effect value (RR), and df is the degree of
describes the degree of inconsistency among studies in a meta-analysis freedom (k-1).
sense. The larger the I2 quantity is, the larger the difference between Contour enhanced funnel plots were used to test for publication bias.
studies is. The heterogeneity variance parameter is denoted as τ2, which The funnel plots were performed in R-project using the meta package.
effectively reflects the heterogeneity among studies. The Cochran Q test These plots showed effect sizes and standard errors in each meta-
statistic is computed by summing the squared deviations of each study’s analysis. The effect sizes which were symmetrical and on the top of
estimate from the overall meta-analysis estimate, thereby weighting the funnel proved there was no bias (Egger et al., 1997).
each study’s contribution in the same manner as conducted in the meta-
analysis. The p-value is obtained by evaluating the chi-square distribu 3. Characteristics of the microplastics in WWTPs
tion with (k-1) degrees of freedom (df) (k: the number of studies). The
difference among studies is caused by random errors when the p-value is 3.1. Microplastics in wastewater
smaller than 0.05.
∑ Microplastics were frequently detected in the influent and effluent of
Q= ωi (θi − θ)2 (2) WWTPs. Table 1 lists the location, daily treatment capacity, serving
population, source of wastewater and main treatment technologies of
Q − df the WWTPs in this study. The microplastic abundances in the primary,
I2 = × 100% (3)
Q secondary, and tertiary treatment processes and effluent are
Table 1
Information of WWTPs in this study.
Location Capacity Population Treatment processes Source of wastewater Reference
(m3/day)
R1 Scotland, UK 166,422 1.8 × 105 Pri, Sec, Ter (Nitrification) Municipal Blair et al., 2019
R2 Cartagena, Spain 35,000 2.1 × 105 Pri, Sec Municipal and Industrial Bayo et al., 2020
R3 Madrid, Spain 28,400 – Sec (A2O) Municipal Edo et al., 2020
R4(W1) Hong Kong, China 93,000 – Pri, Sec Municipal Ruan et al., 2019
R4(W2) Hong Kong, China 2,400,000 – Pri, Ter (Chlorination) After primary treatment Ruan et al., 2019
R5(W1) Daegu, Korea 26,545 – Pri, Sec, Ter (Coagulation, O3) Municipal and Industrial Hidayaturrahman and Lee, 2019
R5(W2) Daegu, Korea 469,249 – Pri, Sec, Ter (Coagulation, DF) Municipal and Industrial Hidayaturrahman and Lee, 2019
R5(W3) Daegu, Korea 20,840 – Pri, Sec, Ter (Coagulation, RSF) Municipal and Industrial Hidayaturrahman and Lee, 2019
R6 Wuhan, China 20,000 – Pri, Sec (A2O), Ter (Chlorination) Industrial, Agricultural, Municipal Liu et al., 2019d
R7(W1) M-City, Korea – – Pri, Sec (A2O) Municipal Lee and Kim, 2018
R7(W2) Y-City, Korea – – Sec (SBR) Municipal Lee and Kim, 2018
R7(W3) S-City, Korea – – Pri, Sec Municipal Lee and Kim, 2018
R8 Mikkeli, Finland 10,000 – Pri Municipal Lares et al., 2018
R9(W1) Sydney, Australia 17,000 6.7 × 104 Sec Municipal Ziajahromi et al., 2017
R9(W2) Sydney, Australia 48,000 1.5 × 105 Sec Municipal Ziajahromi et al., 2017
R10(W1) Wuxi, China 50,000 – Pri, Sec (OD), Ter (UV) Municipal Lv et al., 2019
R10(W2) Wuxi, China 70,000 – Pri, Sec (A2O + MBR) Municipal Lv et al., 2019
R11(W1) Helsinki, Finland – – Ter (DF) Municipal Talvitie et al., 2017a
R11(W2) Turku, Finland – – Ter (RSF) Municipal Talvitie et al., 2017a
R11(W3) Hameenlinna, Finland – – Ter (DAF) Municipal Talvitie et al., 2017a
R11(W4) Mikkeli, Finland – – Ter (MBR) Municipal Talvitie et al., 2017a
R12 Scotland, UK 260,954 6.5 × 105 Pri, Sec Municipal Murphy et al., 2016
R13(W1) Shanghai, China – 3.5 × 106 Pri, Sec (A2O), Ter (UV) Municipal Jia et al., 2019
R13(W2) Shanghai, China – 2.9 × 106 Pri, Sec (A/O), Ter (UV) Municipal Jia et al., 2019
R14 Helsinki, Finland 270,000 8.0 × 105 Pri, Sec, Ter (BAF) Municipal Talvitie et al., 2017b
R15 Beijing, China 1,000,000 2.4 × 106 Pri, Sec (A2O), Ter (UF, UV, O3) Municipal Yang et al., 2019
R16 Vancouver, Canada 493,271 1.3 × 106 Pri, Sec Municipal Gies et al., 2018
R17 Helsinki, Finland – 8.0 × 105 Pri, Sec, Ter (BAF) Municipal Talvitie et al., 2015
R18 Northern, Italy 400,000 1.2 × 106 Pri, Sec, Ter (SAF) Combined sewers Magni et al., 2019
R19(W1) Detroit, USA 2,500,000 – Pri, Sec, Ter (Chlorination) Raw wastewater and stormwater Michielssen et al., 2016
R19(W2) Detroit, USA 1700 – Pri, Sec, Ter (Chlorination) Raw wastewater and stormwater Michielssen et al., 2016
R20 Paris, France 240,000 – Pri, Sec (Biofilter) Municipal and Industrial Dris et al., 2015
R21(W1) Xiamen, China 75,000 3.4 × 105 Pri, Sec Municipal and Industrial Wang et al., 2019
R21(W2) Xiamen, China 245,800 1.2 × 106 Pri, Sec Municipal and Industrial Wang et al., 2019
R22 Xiamen, China 257,936 1.0 × 106 Pri, Sec (Biofilter) Municipal and Industrial Long et al., 2019
R23(W1) Los Angeles, USA – – Ter (GF) – Carr et al., 2016
R23(W2) Los Angeles, USA – – Ter (Centrata thickening) – Carr et al., 2016
R24 Oldenburg, Germany 35,616 2.1 × 105 Ter (PF) Municipal and Industrial Mintenig et al., 2017
(1) Pri, Sec, Ter refer to primary treatment, secondary treatment and tertiary treatment
(2) A2O: anaerobic-anoxic-oxic; A/O: anoxic oxic; OD: oxidation ditch; DF: disc filter; RSF: rapid (gravity) sand filter; DAF: dissolved air flotation; BAF: biologically
active filter; GF: gravity filter; PF: post-filtration; SAF: sand filter; UF: ultra-filtration
3
summarized in Table S1. The microplastic abundances in the influent of the WWTPs.
the WWTPs ranged from 0.28 particles L− 1 to 3.14 × 104 particles L− 1
(mean value: 1.90 × 103 particles L− 1; median value: 57.60 particles 3.2.1. Shape
L− 1). The shape is an important classification factor of microplastics. The
The differences in the microplastic abundance could be related to a shape of microplastics affects their removal efficiency in WWTPs
variety of complex factors, such as the population served, wastewater (McCormick et al., 2014). Nine shapes of microplastics were detected in
sources (municipal or industrial), economy, and lifestyle. In the the influent and effluent of the WWTPs. The abundances of the different
municipal WWTPs, the microplastic abundance was lower, ranging from microplastic shapes observed in the WWTPs are summarized in Table 2.
0.28 particles L− 1 to 6.10 × 102 particles L− 1 (mean value: 1.27 × 102 Fibers, pellets, fragments, and films were the most widely detected
particles L− 1; median value: 31.10 particles L− 1). In the municipal and microplastics in wastewater, and their highest abundances were
industrial WWTPs, the microplastic abundances ranged from 1.60 par 91.32%, 70.38%, 65.43%, and 21.36%, respectively (Bayo et al., 2020;
ticles L− 1 to 3.14 × 104 particles L− 1 (mean value: 5.23 × 103 particles Hidayaturrahman and Lee, 2019; Lares et al., 2018).
L− 1; median value: 1.86 × 102 particles L− 1). However, few studies have The fiber, a filamentary microstructure, was the dominant micro
investigated the microplastic emissions directly from plastic processing plastic shape in the WWTPs. The microplastic fibers originated from
industrial WWTP. In terms of the serving population, the abundance of domestic washings. The increasing amount of washing and textile con
the influent microplastics was positively correlated with the serving sumption resulted in the more frequent detection of fibers (Cesa et al.,
population in most WWTPs (Mason et al., 2016). The microplastic 2017). During the textile production process, fibers are also produced in
abundance was also influenced by the sampling and detection methods. shearing and splicing processes, after which they enter wastewater
Limited wastewater sample volumes increased the uncertainty of the (Hidayaturrahman and Lee, 2019; Napper and Thompson, 2016). The
microplastic abundance and experimental errors. These problems microplastic fragments and pellets originated from cosmetics and per
enhanced the difficulties in the research on the microplastic fate in the sonal care products, such as toothpaste, masks, and soaps (Carr et al.,
WWTPs. 2016). The microplastic films originated from plastic packing bags
As indicated in Table S1, microplastics were detected in all treatment (Kazour et al., 2019). Moreover, other microplastic shapes, such as
processes in the WWTPs. The microplastic abundance gradually foams, particles, ellipses, lines, and flakes, were also detected in the
decreased from primary treatment to secondary treatment. The primary WWTPs.
treatment process based on physical mechanisms was considered the
first barrier to remove microplastics in WWTPs. Primary settling tank 3.2.2. Particle size
was the most commonly implemented primary treatment method. The Microplastics may end up in the food chain, and the size of micro
microplastic abundance after primary treatment processes ranged from plastics rather than their shape was a crucial factor influencing their
0.22 particles L− 1 to 1.26 × 104 particles L− 1 (mean value: 6.87 × 102 performance and transformation in the WWTPs (Lehtiniemi et al.,
particles L− 1; median value: 4.90 particles L− 1). Their abundance 2018). Therefore, it is important to highlight the particle size of
decreased by 4.06–98.96% (mean value: 56.75%; median value: microplastics.
54.88%), compared to the abundance of microplastics in the influent. The distribution of the microplastic particle sizes in the WWTPs is
After the primary treatment process, biological treatment (secondary shown in Fig. S1. The abundance of the microplastics smaller than 1 mm
treatment process) was the most critical technology in the WWTPs. In ranged 65.0–86.9% in the influent and 81.0–91.0% in the effluent. With
biological treatment, A2O was the most widely used technology in decreasing microplastic sizes, the primary microplastics were crushed
WWTPs. Meanwhile, the biofilter technology had a high biomass load (physical, chemical, and biological processes) into secondary micro
and a high volumetric reaction rates, which improved the pollutant plastics (Magni et al., 2019). The smaller microplastic particles were
removal efficiency and gradually became more popular in WWTPs (Liu more likely to be ingested by plankton, filter-feeding organisms, and
et al., 2020a; Rocher et al., 2012). The abundances after secondary fishes, which can cause a series of toxicological effects in these organ
treatment processes ranged from non-detection to 7.86 × 103 particles isms (Qiao et al., 2019). Therefore, the research of the particle size of
L− 1(mean value: 4.67 × 102 particles L− 1; median value: 6.90 particles microplastics, especially the smaller particle size (smaller than 1 mm)
L− 1), resulting in a decrease of abundance by 20.45–95.45% (mean can be of guiding significance for the subsequent study of biological
value: 66.63%; median value: 73.53%). toxicity and the environmental transformation of microplastics.
To further remove the contaminants, 61.76% of the WWTPs
employed tertiary treatment processes, such as advanced oxidation and 3.2.3. Polymer type
membrane filtration processes. After tertiary treatment processes, the The abundances of the different microplastic polymer types in the
microplastic abundance further decreased in most of the investigated influent and effluent are listed in Table 3. Twenty-nine kinds of poly
WWTPs (85.71%), while in others, the abundance increased. The mers were detected in the influent and effluent of the WWTPs. Poly
abundance of the microplastics in effluent ranged from non-detection to ethene (PE), polypropylene (PP), polyamide (PA), polyester (PES),
2.97 × 102 particles L− 1 (mean value: 19.26 particles L− 1; median value: polystyrene (PS) and polyethene terephthalate (PET) were the top six
0.40 particles L− 1). Compared with the influent, the microplastic most widely detected microplastics in the wastewater, and their highest
abundance decreased by 50.00–99.57% (mean value: 85.58%; median
value: 90.34%). As a result, at most 50.00% of the microplastics in the
WWTPs was still discharged through the effluent and entered the Table 2
The abundance of different shapes of microplastics in WWTPs.
receiving water systems. Hence, microplastic-targeted treatment pro
cesses are urgently needed. Shape Influent (particles L− 1) Effluent (particles L− 1) Detection times
3
Fiber 0.22–4.60 × 10 nd-35.00 12
3.2. Shape, particle size and polymer type distribution in the influent and Fragment 0.25–3.40 × 103 nd-80.00 11
effluent Film 0.06–1.30 × 103 nd-12.00 9
Pellet 0.01–2.21 × 104 nd-1.33 × 103 7
Foam nd-2.33 nd 4
Microplastics are a type of polymer mixture with various shapes and Particle nd-2.91 × 102 nd-10.00 3
sizes. Different shapes and sizes of microplastics possessed different Ellipse 0.36 nd 1
physicochemical and toxicity properties (Lehtiniemi et al., 2018). Line 0.12 0.12 1
Flake 0.92 nd 1
Therefore, this study emphasized the occurrence and removal of
microplastics with different shapes, particle sizes, and polymer types in Note: nd means non-detection.
4
Table 3 (Sun et al., 2019). Table 4 summarizes the microplastic abundance levels
The abundance of different polymer types of microplastics in WWTPs. in the sludge treated by different treatment technologies within the
Polymer Abbreviation Influent Effluent Detection range from 4.40 × 103 particles kg− 1 to 2.40 × 105 particles kg− 1. The
(particles (particles times microplastic abundance in the sludge from the primary treatment pro
L− 1) L− 1 ) cess was higher than that of the secondary treatment process. Gies et al.
Polyethene PE 0.03–1.05 0.00–0.67 9 (2018) estimated that 0.54–1.28 trillion microplastics occurred in pri
Polypropylene PP 0.02–1.42 0.00–0.22 8 mary sludge and 0.22–0.36 trillion microplastics occurred in secondary
Polyamide PA 0.06–0.71 0.00–0.06 6 sludge. In addition, Talvitie et al. (2017b) calculated that 20% of the
Polyester PES 0.22–6.31 0.07–1.33 6
Polystyrene PS 0.00–0.41 0.00–0.08 5
microplastics in the secondary sludge flowed back into the wastewater.
Polyethene PET 0.01–0.63 0.00–0.16 5 Sludge utilization has received much attention in recent years. The
terephthalate sludge from the WWTPs was mainly utilized for agricultural purposes in
Polyurethane PUR / PU 0.07–1.40 0.00–0.02 4 Norway (82%), Ireland (63%), the US (55%), China (45%) and Sweden
Polyvinyl chloride PVC 0.12–1.65 0.00 3
(36%), and it was incinerated in the Netherlands (99%), Korea (55%)
Polyvinyl acetate PVA 0.26–0.50 0.00–0.01 2
Alkyd – 0.13–4.51 0.00–0.02 2 and Canada (47%), while the sludge was applied as soil compost in
Ethylene- EVA 0.00–0.01 0.00 2 Finland (89%) and Scotland (40%) (Fig. 1) (Rolsky et al., 2020). Soil
vinylacetate contaminated with microplastics represents a great threat to crops and
Polyacrylates – 0.06–0.40 0.00–0.03 2 agricultural products. Corradini et al. (2019) reported that the average
Acrylic 1.30 0.03 1
microplastic abundance in agricultural soils originating from sludge
–
Polyvinyl ethylene PVE 0.09 0.00 1
Polyvinyl fluoride PVF 0.09 0.00 1 disposal was 3,500 particles kg− 1. Pyroplastics are a new type of
Styrene- SBS 0.02 0.00 1 pollutant derived from the informal or more organized burning of
butadiene- manufactured microplastics. After sludge incineration, pyroplastics
styrene
enter the environment and cause great threats (Turner et al., 2019). In
Styrene-ethylene- SEBS 0.06 0.00 1
butadiene- China, 35% of the sludge originating from WWTPs still enter landfills
Styrene (Fig. 1). Microplastics are further transferred into the soil and ground
Styrene SAN 0.01 0.00 1 water through the leachate (Chen et al., 2012; Rolsky et al., 2020). In
acrylonitrile general, soil contamination of microplastic is scarcely known and is thus
Polyvinyl alcohol PVAL 0.03 0.00 1
considered one of the pressing concerns related to microplastics.
Acrylamide – 0.09 0.00 1
Polyethene& PE&PP 0.09 0.01 1
Polypropylene 4. Removal of microplastics in the WWTPs
Paint – 0.01 0.00 1
Polystyrene acrylic PS acrylic 0.30 0.00 1
4.1. Comparison of the different treatment technologies for microplastics
Polyvinyl acrylate PV acrylate 0.09 0.00 1
Styrene- – 0.01 0.00 1 removal
vinyltoluene-
butylacrylate Previous studies reported the microplastics removal efficiency via
Polyterpene – 0.03 0.01 1 individual field sample collected from primary, secondary, and tertiary
Acrylonitrile- 0.80 0.01 1
treatment processes. However, these studies could not accurately
–
butadiene
Ehtylene-acrylate – 0.14 0.01 1 determine the optimal treatment process and mechanism of micro
Ehtylene- – 0.28 0.00 1 plastics removal. Therefore, this study compared the removal efficiency
propylene of different treatment technologies in global WWTPs via meta-analysis.
The different treatment technologies applied in the WWTPs included
primary treatment processes (primary settling treatment, grit and grease
abundances were 64.07%, 32.92%, 10.34%, 75.36%, 24.17%, and
treatment), secondary treatment processes (A2O, biofilters, and other
28.90%, respectively (Long et al., 2019; Mintenig et al., 2017; Talvitie
bioreactors) and tertiary treatment processes (UV, O3, chlorination,
et al., 2017a; Ziajahromi et al., 2017). The PE, PP, and PS microplastics
biologically active filters (BAFs), disc filters (DFs), and rapid sand filters
originated from plastic products, including food packaging bags, plastic
(RSFs)).
bottles, and plastic cutlery (Lares et al., 2018; Mintenig et al., 2017;
Fig. 2 shows the meta-analysis results for the different treatment
Talvitie et al., 2017b). The PA, PET, and PES microplastics mainly
technologies. The weighted average RR values of the primary, second
originated from textiles and synthetic clothing, which are the main
ary, and tertiary treatment processes were 0.40, 0.39, and 0.48,
sources of household microplastics (Hernandez et al., 2017; Sun et al.,
respectively (Fig. S2). The primary and secondary treatment processes
2019; Wei et al., 2019). Furthermore, the mechanical crushing of plastic
attained similar microplastics removal efficiencies. The tertiary treat
products, the tire, and textile industries and the rubber particles in road
ment process achieved limited removal efficiency. Especially, the
dust were also identified as potentially important sources of the PE, PP,
PS and PES microplastics (Hidayaturrahman and Lee, 2019; Nizzetto
et al., 2016; Talvitie et al., 2017a).
Table 4
In addition to the polymer types mentioned above, specific polymers
The abundance of microplastics in the sludge of different wastewater treatment
were also identified in the WWTPs. For example, alkyds, which are processes.
widely used in industrial coatings, exhibited the highest abundance in a
Treatment Process Abundance (Particles
Glasgow WWTP (28.67%) (Murphy et al., 2016). Therefore, research kg− 1)
priority should be assigned to specific polymer types in addition to
R6 Primary clarifier + A2O + Secondary clarifier 2.40 × 105
common polymers.
R7 Primary settling tank + A2O + Secondary 1.49 × 104
(a) settling tank
R7 SBR 9.65 × 103
3.3. Microplastics in the sludge (b)
R7 Primary settling tank + Secondary settling tank 1.32 × 104
Most of the microplastics removed from wastewater were retained in (c)
the sludge (Mahon et al., 2017). It was found that the microplastic R16 Primary settling 1.49 × 104
R16 Secondary clarifiers 4.40 × 103
abundance in the sludge was much higher than that in the wastewater
5
poor efficiency in microplastics removal. But a recent study showed that

69–79% of microplastics entering WWTPs are removed by screening and
grit treatment (Ziajahromi et al., 2021). Only light floating microplastics
could be removed during the grease skimming process (Sun et al., 2019).
Grit and grease process combined with primary settle treatment could
improve the efficiency of removing microplastics. Bioreactor (except
A2O and biofilter) attained a notable microplastics removal efficiency.
Sequence batch reactor process (SBR) was found to have removal 98%
microplastics (Lee and Kim, 2018). However, A2O technology was not
suitable for the removal of microplastics because of the sludge returned.
Jiang et al. (2020) indicated that the anoxic-oxic process (A/O) captured
about 16.9% of microplastics in wastewater. The removal efficiency of
the same treatment process is closely related to the characteristics of
wastewater and the types of microplastic polymers. Advanced oxidation
processes showed the medium removal efficiency of microplastics. It can
be seen that the removal efficiencies of microplastics in critical treat
ment technologies are quite different.
4.2. Influence of the microplastic shape, particle size and polymer type on
microplastics removal
Fig. 3 shows the meta-analysis results of microplastics removal for

four shapes by different treatment technologies which was calculated
Fig. 1. Proportions of sludge utilization type in 12 countries (the remaining
utilization types were described as ‘others’).
with the data summarized in Section 3.2.1. Among the four microplastic
shapes, fibers were the most widely detected microplastics in waste
water. Their weighted average RR values in the primary, secondary and
tertiary treatment processes were 0.31, 0.41, and 0.43, respectively
(Fig. S3). Primary treatment has superiority over secondary and tertiary
treatment for fiber microplastics removal. Fibers were easily trapped
during primary treatment due to flocculation and settling. After the
primary treatment process, most of the easily settled or skimmed par
ticles were removed, but the remainder might exhibit a neutral buoy
ancy (Sun et al., 2019). In contrast, fragments exhibited excellent
removal efficiency during the secondary treatment process. The
weighted average RR values of fragments were 0.41, 0.30, and 0.36,
respectively (Fig. S3). Fragments with a lamellar structure gradually
agglomerated and were ingested by the activated sludge (Jeong et al.,
2016). The weighted average RR values of the films in the primary,
secondary, and tertiary treatment processes were 0.35, 0.34, and 0.47,
respectively (Fig. S3). The microplastics removal efficiencies of the
primary and secondary treatment processes were higher than that of the
tertiary treatment processes. Pellets were easier to remove during the
tertiary treatment process. The weighted average RR values of the pel
lets in the primary, secondary and tertiary treatment processes were
0.63, 0.76, and 0.35, respectively (Fig. S3). Both filter-based and
Fig. 2. Meta-analysis results of microplastics removal by different treat
ment processes.
tertiary treatment processes exhibited a wide range of the 95% CIs

(0.22–1.06) because of the difference between the advanced oxidation
process and filter technology. Among them, the advanced oxidation
treatment process removed pollutants via chemical methods, while filter
technology removed pollutants through physical methods. The micro
plastics removal efficiency of the critical treatment technologies fol
lowed the sequence of biofilters, filters, primary settling, bioreactors
(except for A2O and biofilters), grit and grease removal with primary
settling, advanced oxidation, grit and grease removal, and A2O, with
weighted average RR values of 0.32, 0.33, 0.39, 0.41, 0.42, 0.56, 0.61
and 0.73, respectively (Fig. S2).
Therefore, filter-based technologies (biofilter, ultrafiltration (UF),
rapid sand filter (RSFs), etc.) achieved the best performance in removing
microplastics. Among them, RSF technology provides rapid and efficient
removal of microplastics (Talvitie et al., 2017a). But in this process, the
microplastics will be broken into smaller particles (Prata, 2018; Sol
et al., 2020). Primary settling treatment attained an excellent efficiency
Fig. 3. Meta-analysis results of microplastics removal with different shapes by
in removing microplastics, while grit and grease treatment exhibited a
different treatment processes.
6
advanced oxidation treatment processes could effectively intercept promising. The impact of different shapes, particle sizes, and polymer
pellets. Moreover, the tertiary treatment process also presented an types on microplastics removal in different treatment processes should
extremely high efficiency in removing microplastics with specific receive more attention. What’s more, the mechanisms of microplastics
properties and very small particle sizes. removal by the critical treatment technologies should also be studied in
Fig. 4 shows the meta-analysis results of microplastics removal for depth.
three particle sizes by the different treatment processes. During the
tertiary treatment process, the microplastics usually had a small particle 4.3. Mass of microplastics
size (smaller than 0.5 mm), which was more difficult to detect and
remove (Hidalgo-Ruz et al., 2012). In addition, in the advanced oxida The quantification of microplastics focused on determining the
tion processes, microplastics were continuously crushed, resulting in a number of particles, because the influence and behavior of microplastics
negative removal (Lv et al., 2019; Ruan et al., 2019). Therefore, the is closely related to the number of particles (Andrady, 2011). Because of
meta-analysis was only conducted on the primary and secondary treat the aging of the microplastics in the environment, the microplastics
ment processes. Microplastics with particle sizes smaller than 0.5 mm were broken into small particles. Therefore, using the mass of micro
were easily trapped during secondary treatment processes. The plastics to supplement the description of the occurrence of microplastics
weighted average RR values in the primary and secondary treatment could scientifically and accurately quantify the load of microplastics in
processes were 0.70 and 0.48, respectively (Fig. S4). Microplastics with the environment (Rocha-Santos and Duarte, 2015). Mass balance was
a particle size ranging from 0.5 mm to 1 mm were better removed during used as an intuitional way to explore the fate of microplastics in WWTPs.
primary treatment processes, as well as microplastics with a particle size From a mass point of view, the WWTP has shown excellent perfor
ranging from 1 mm to 5 mm. The weighted average RR values of the mance in the removal of microplastics. Simon et al. (2018) investigated
microplastics in the 0.5–1 mm size range were 0.31 and 0.74, respec the mass of microplastics in the influent and effluent of 10 WWTPs in
tively (Fig. S4). The weighted average RR values of the microplastics in Denmark for the first time. The mass of microplastics in the influent
the 1–5 mm size range were 0.06 and 0.53, respectively (Fig. S4). On the ranged from 61 μg L− 1 to 1189 μg L− 1 (mean value ± standard deviation:
one hand, the fibers and films had a large particle size and low density, 352 ± 324 μg L− 1; median value: 240 μg L− 1). The mass of microplastics
and they were easily removed by flotation and grease removal processes. in the effluent ranged from 0.5 μg L− 1 to 11.9 μg L− 1 (mean value ±
On the other hand, the pellets in personal care products had high den standard deviation: 4.4 ± 4.3 μg L− 1; median value: 3.7 μg L− 1). Through
sity, and they generally sank to the bottom of pools due to gravity the mass balance of the microplastics in the WWTP, it can be found that
(Lehtiniemi et al., 2018). only 0.22–6.23% of the microplastics will enter the natural aquatic
Common polymer analytical methods included gas chromatography system through the effluent. Furthermore, Lv et al. (2019) systematically
coupled to mass spectrometry (Dümichen et al., 2017), liquid chroma evaluated the mass of microplastics in the effluent of each critical
tography (Elert et al., 2017), Fourier transform infrared spectroscopy treatment process from two WWTPs in Wuxi, Jiangsu Province, China.
(Mintenig et al., 2017) and Raman spectroscopy (Lares et al., 2018). The mass of the microplastics in the influent of two WWTPs was 280 ±
However, it was still difficult to identify individual microplastic polymer 4.5 kg per day and 392 ± 4.5 kg per day, respectively. After the primary
type due to the limitation of these analytical methods (Hidalgo-Ruz treatment process (aerated grit chamber/ rotary grit chamber), the mass
et al., 2012). Thus, a meta-analysis for the different polymer types could of the microplastics was reduced to 271.6 ± 2.5 kg and 388 ± 2.5 kg per
not be conducted until now. PE, as the most frequently detected day, respectively. After the secondary treatment process (oxidation
microplastic polymer type in the WWTPs, was efficiently removed ditch/ anaerobic-anoxic-oxic), the mass of the microplastics was
during the secondary treatment process, which was also true for PS reduced to 225 ± 5.0 kg and 329 ± 3.5 kg per day, respectively. After the
polymer. The positively charged PE and PS microplastics had a high tertiary treatment process (UV disinfection/ Membrane tank), the mass
affinity for the negatively charged activated sludge mass (Bhattacharya of microplastics in the effluent was 8.4 kg and 1.96 kg per day,
et al., 2010). respectively. Mass of microplastics accumulated in excess sludge was
In a word, fibers and microplastics with large particle sizes (0.5–5 0.51 kg per day from oxidation ditch system and 0.033 kg per day from
mm) were easily separated by primary settling. Polyethene (PE) and anaerobic-anoxic-oxic-membrane tank system. It can be seen that only
small-particle size microplastics (smaller than 0.5 mm) were easily 3% or less of the microplastics in the wastewater treatment plant were
trapped in the activated sludge by bacteria. Therefore, choosing suitable discharged into the aquatic environment and 1% of the microplastics
treatment technologies for microplastics removal in WWTPs is quite were retained in the sludge produced by the biochemical treatment
process. The remaining 96% of the microplastics were degraded, skim
ming or retained by the membrane. Among them, membrane retention
occupied a larger proportion, which can be seen from the high removal
rate of the filter-based process.
4.4. Publication bias
Contour enhanced funnel plots of the microplastics removal by pri

mary, secondary, and tertiary treatment processes were presented in
Fig. S5. Contour enhanced funnel plots of the different shapes and par
ticle sizes microplastics removal by different treatment processes were
presented in Fig. S6 and Fig. S7, respectively. Collectively, although the
extractable studies are relatively few in some of the meta-analysis, no
evidence of publication bias was observed in the funnel plots.
4.5. Mechanisms of critical treatment technologies in microplastics

removal
4.5.1. Primary settling with flocculation

Fig. 4. Meta-analysis results of microplastics removal with different particle Fig. 5 showed the schematics of flocculation and primary settling
sizes by different treatment processes. technologies in microplastics removal. In the flocculation process, flocs
7
Fig. 5. The schematics of primary settling with flocculation technologies in microplastics removal (Lapointe et al., 2020).
Fig. 6. The schematics of the bioreactor system in microplastics removal. (A) Activated sludge process (Zhang et al., 2020); (B) MBR (Adapted from Li et al., 2020);
(C) Biofilter; (D) A2O (Liu et al., 2020b).
8
interacted with microplastics via hydrogen bonds, van der Waals forces, microplastics removal in the MBR system. What’s more, the removal of
or electrostatic forces (Duan and Gregory, 2003; Lapointe et al., 2020). microplastics could be related to the size of microplastics. The mem
Like-charged microplastic particles maintain stability due to the repul brane applied in the MBR system usually has a pore size of 0.1 μm. Thus,
sive inter-particle electrostatic forces. Flocculants possessing opposite the microplastics could be removed in the MBR system theoretically. (Li
charges with microplastics effectively reduced the repulsive potential et al., 2020).
between microplastic particles. It was possible for the Brownian motion The biofilter technology was applied as a deep treatment unit after
and mechanical agitation to become operative, leading to microplastics the bioreactor system. The microplastics entered the biofilter treatment
and flocs aggregation (Larue et al., 2003). unit have smaller particle size and lower density. These increased the
Both iron-based salts and aluminum-based salts are widely used difficulty in microplastics removal. But biofilter technology still
flocculants in wastewater treatment (Ma et al., 2019a). The flocculation demonstrated the highest removal performance of microplastics (Fig. 2).
of microplastics with iron was caused by the adsorption of iron hy Biofilter technology integrated physical and biological purification
droxide aggregates (Larue et al., 2003). Small aggregates with high processes (Fig. 6C), and biofilm filtration and adsorption were the main
positive charge were locally adsorbed on the microplastic surfaces at low mechanisms for microplastics removal. The microbe film growing on the
pH media. In this case, flocs neutralized microplastic charges and surface of the inert filter material was in contact with the microplastics
eliminated repulsion forces between microplastics. At neutral and basic and increased the contact area between microplastics and microorgan
pH media, the floc aggregates size increased, and aggregated form isms. Excess microbes and retained microplastics were easy to be
bridges between microplastics (Larue et al., 2003; Ma et al., 2019b). removed by backwashing in the ascendant water flow (Rocher et al.,
Microplastics interacted with aluminum-based flocculants via hydrogen 2012).
bonds. Cationic aluminum flocculant was also electrostatically attached Microplastics are regarded as carriers of the microbes, so the
to anionic carboxyl groups in the weathered microplastics. The presence occurrence of microplastics will influence the community and activity of
of new functional groups (such as hydroxyl group (OH), carboxyl group microbial. Li et al. (2020) found that with the addition of PVC, the mi
(COOH), and carbon-carbon double bond (C– – C)) on the weathered crobial community composition was reduced immediately and the
microplastic surface promoted interactions between the flocs and number of operational taxonomic units decreased from 1665 to 1533.
microplastics (Lapointe et al., 2020). Subsequently, the number of operational taxonomic units increased to
Subsequently, the primary settling technology mainly removed the 1735. The percentage of each bacterial in the bacterial community
settable parts in the suspended microplastics. Most of the non-sinkable slightly changed with the operation time. Therefore, the existence of
floating microplastics adhered to the flocs and precipitated together, microplastics PVC did not pose obvious operational taxonomic unit
others were skimmed as scum (Lee et al., 2012). These microplastics reduction and has an insignificant effect on the microbial community
were discharged as primary sludge (Murphy et al., 2016). Existing structure change. At the same time, it is gratifying that virgin micro
studies proposed the mechanisms for the removal of microplastics in plastics do not significantly affect the activities of ammonia oxidizing
flocculation technology and primary settling technology but lack of bacteria, nitrite oxidizing bacteria, and phosphorus accumulating or
identification of the degradation products of microplastics and their ganisms (Liu et al., 2019b). Therefore, the effect of microplastics on the
physiochemical properties. The toxicity of the substances generated performance of the bioreactor system should not be overemphasized.
after the flocculation and the impact of settling time on settling effi However, the toxicity of additives contained in the microplastic to
ciency of primary settling technology are less known. bacteria was unclear. Subsequent research should consider the impact of
microbe containing microplastics on conventional pollutant removal.
4.5.2. Bioreactor system Among them, the influence of microplastics on the function of microbe
Fig. 6 showed the schematics of the bioreactor system in micro after adsorption of conventional pollutants also needs in-depth study.
plastics removal. As shown in Fig. 6A, the bioreactor system removed
microplastics mainly through the ingestion of microbe and the forma 4.5.3. Advanced oxidation
tion of sludge aggregates. In particular, domesticated activated sludges Chlorination and UV-oxidation were the most popular advanced
were likely to promote the accumulation of microplastics in WWTPs. oxidation processes in WWTPs. Chlorine is a widely used as disinfection
Sludge containing microplastics was removed during the subsequent agent in WWTPs. Microplastics were not completely resistant to the
secondary settling process (Jeong et al., 2016). attack of chlorine (Kelkar et al., 2019). The chlorination process
A2O is the most widely used bioreactor system in WWTPs (Fig. 2). increased the microplastic abundance because of the cracking of
However, it had a relatively poor microplastics removal efficiency owing microplastics (Lv et al., 2019; Ruan et al., 2019). The schematic of
to the sludge return. Some of the microplastics (20%) transferred into microplastics degradation in chlorination was shown in Fig. 7A. Chlo
the sludge would flow back to the aqueous phase. Furthermore, the rine potentially broke the existing bonds and introduced new bonds. The
degradation of microplastics in A2O was quite slow. Previous studies new chemical structure of high-density polyethylene (HDPE) in chlori
reported several functional bacteria with microplastic degradation. The nation disinfection was C-C-C asymmetrical chain, C-C-C symmetrical
bacterial strain Rhodococcus degraded 6.4% of the PP polymer mass in chain, CH2 twist, and CH2 bend (Kelkar et al., 2019), identified that
40 days (Auta et al., 2018). And Ideonella sakaiensis complete degraded intense chlorination might result in a force of compression on the Raman
PET film microplastics in 6 weeks (Yoshida et al., 2016). However, the peaks. (Eichhorn et al., 2001). A new chlorine carbon bond (Cl-CH2-C-H)
existing hydraulic retention time (7–14 h) cannot achieve the effective was formed in chlorination. Carbon-chlorine bonds might increase
degradation of microplastics only by microorganisms in WWTPs. toxicity and hydrophobicity, which resulted in microplastics more easily
Therefore, the conventional activated sludge method is not ideal for adsorbing and accumulating harmful contaminants (Wang et al., 2018).
removing microplastics in WWTPs. Additionally, chlorine occurred on both the aliphatic and aromatic
Membrane bioreactor (MBR) technology has recently become a during PS degradation (Zebger et al., 2003). Raman shifting of the
popular treatment process in WWTPs. It presents an excellent perfor aliphatic C-H backbone towards a higher wavenumber (from 2901 cm− 1
mance in microplastics removal (removal efficiency 99.9%) (Talvitie to 2940 cm− 1) was observed. This shift signified the force of compres
et al., 2017a) due to a high mixed-liqueur suspended solids concentra sion on the backbone bond towards higher energy (Eichhorn et al.,
tion (range from 6000 mg L− 1 to 10000 mg L− 1) (Dvořák et al., 2013). As 2001). Chlorination also changed the physical and chemical properties
shown in Fig. 6B, MBR technology integrated membrane separation and of microplastics due to its strong oxidizing nature (El-Shahawi et al.,
traditional activated sludge method. Most the microplastics were 2010). However, PP was resistant to chlorination. Even at high dosage
retained in the biofilm carrier side of the MBR system. This indicated and long exposure time, the change of chemical bond was scarcely
that the adsorption effect was one of the major contributors to observed (Kelkar et al., 2019). Due to competitive reactions and chlorine
9
Fig. 7. The schematics of advanced oxidation technologies in microplastics removal. (A) Chlorination (Kelkar et al., 2019); (B) SEM images of the three types of
virgin and UV-oxidation microplastics (Cai et al., 2018); (C) UV-oxidation; (D) PVC UV-oxidation reaction (Shi and Zhang, 2006).
quenching, the coexistence of other pollutants, microorganisms and will be broken to reduce the relative molecular mass (Cai et al., 2018).
biofilms might alter the impact of microplastics structure in However, the intermediates and the toxicity of UV-oxidation micro
chlorination. plastics were less known. The impact of UV irradiation time and envi
The schematic of removal microplastics in UV-oxidation was shown ronmental differences on microplastic degradation requires in-depth
in Fig. 7C. The UV-oxidation occurred on the surface of the micro research. In addition, the influence of the salinity and dissolved organic
plastics, resulting in the change of their topography and chemical matter on the degradation of microplastics in WWTPs also needs to be
characteristics (Cooper and Corcoran, 2010). Virgin microplastics pre considered.
sent relatively homogeneous and compact textures. After UV-oxidation,
the surface of microplastics became relatively rough (Fig. 7B). Granular 4.5.4. Membrane filtration
oxidation/flakes, cracks/flakes, and flakes were common situations of Membranes with a uniform pore distribution have been widely
degradation for the PE, PP, and PS. However, microplastics with cracks applied during wastewater treatment. The schematic of removal
and flakes were easy to break, which produced smaller and even nano- microplastics in membrane filtration was shown in Fig. 8. Membrane
scale plastics (Cai et al., 2018). Cracks as an extension of fractures were filtration technologies intercepted microplastics in aqueous phase using
considered as stress concentrators and fracture loci. The formation of different forms of membrane filtration (Baker, 2012). Microplastic
flakes embrittlement occurs on the brittle surface areas or layer of the particle size was larger than the ultrafiltration membrane pore size
microplastics (Cooper, 2012). As shown in Fig. 7D, part of the peroxy (nano-scale). Thus, microplastics were completely rejected by the ul
free radicals was formed by the cleavage of C-C bonds and C-H bonds trafiltration membranes (Ma et al., 2019b). Microplastics filtration led to
under the condition of UV irradiation (Cai et al., 2018; Gewert et al., a final water flux decline of 38% (Enfrin et al., 2020). This result showed
2015; Wang et al., 2020a). What’s more, UV irradiation could initiate the existence of interactions between microplastics and the membrane
hydroxyl groups (OH) and chromophore groups (including several pores and surface. Microplastics were adsorbed within and onto the
unreacted monomers (C– – C), carbonyl groups (C–– O) and hydroperox pores, or onto the membrane surface at a high rate. With the increase of
ide groups (ROOH)) in the microplastic surfaces to form oxygen- exposure time, more and more microplastics were permeating across the
containing free radicals and initiate the chain reactions. (Fig. 7D) (Cai membrane. For some special membranes, such as polysulfone mem
et al., 2018; Singh and Sharma, 2008; Wang et al., 2020a; Zbyszewski branes, were relatively hydrophilic. Microplastics and polysulfone
and Corcoran, 2011). These peroxy free radicals produced by the UV membranes were negatively charged and hydrophobic. Thus, attractive
irradiation would undergo secondary reactions to form crosslinking polar forces were counterbalanced by the repulsive electrostatic forces
compounds (Fig. 7D). And the molecular chain with a carbonyl group induced by the membrane surface charge and microplastics (Enfrin
10
Fig. 8. The schematic of ultrafiltration technology in microplastics removal (Enfrin et al., 2020).
et al., 2020). capacity of WWTPs. These microplastics likely cause harm to aquatic
However, in order to ensure the long-term stable operation of the organisms (Ma et al., 2020). Developing countries and areas with inef
microfiltration and ultrafiltration membranes, fouling control must be fective wastewater treatment processes should pay more attention to the
strictly enforced (Kumar and Ismail, 2015). At the same time, intermo microplastics pollution of aquatic environments.
lecular repulsion of microplastics and the electrostatic interactions be The microplastics in sludge are eventually retained in the soil envi
tween microplastics and the membrane surface were the main ronment. Sludge is considered one of the most important sources of
mechanisms in microplastics removal by ultrafiltration technology. The microplastics in the soil environment (Bläsing and Amelung, 2018).
electrostatic interactions between microplastics and ultrafiltration 43,000–63,000 and 30,000–44,000 tons of microplastics yearly entered
membranes were detrimental for the performance infiltration (Enfrin European and North American agricultural soils, respectively (Nizzetto
et al., 2020). Meanwhile, membranes suffered from surface fouling due et al., 2016). The decomposition of these microplastics lasts up to 1,000
to the formation of a concentration polarization layer during water years (Tudor et al., 2019). Microplastics absorb toxic compounds and
transfer across the membrane (Enfrin et al., 2020). This concentration aggravate soil pollution (Li et al., 2019). The accumulation and trans
polarization induced the formation of the cake. It decreased the per portation of microplastics not only harms the growth of plants but also
formance of membrane filtration by adsorption and stacking of micro affects the functions and microbial communities in soil (Guo et al.,
plastics or solutes onto the surface of the membrane (Baker, 2012). 2020). The ecological toxicity effect and risk of compound pollution of
Therefore, efficient and stable cleaning procedures need further microplastics and other pollutants necessitates further study.
research to limit the influence of microplastics on membranes.
6. Conclusions and future perspectives
5. Environmental toxicity and risk of microplastics
A meta-analysis helps us to better understand the fate of micro
Microplastics enter aquatic and soil environments through waste plastics in WWTPs. The filter-based treatment process attained the
water and sludge discharge. They are emerging pollutants as well as highest microplastic removal efficiency. Fibers and microplastics with
carriers of heavy metals and organic contaminants. Microplastics large particle sizes (0.5–5 mm) were easily separated by primary
adsorbed heavy metals and polycyclic aromatic hydrocarbons could be settling. PE and small-particle size microplastics (<0.5 mm) were easily
ingested by benthic animals, leading to bioaccumulation in marine food trapped in the activated sludge and by bacteria in the WWTPs. The in
chains (Foshtomi et al., 2019). Microplastics disrupt the soil structure teractions and removal mechanisms between microplastics and critical
and microbe metabolism and thus affect the water holding capacity of treatment technologies were quite different. Conventional flocculation
the soil (Machado et al., 2018). Certain properties (such as the structure) interacted with microplastics via van der Waals forces, hydrogen bonds,
of land plants might improve the uptake of microplastics and other or electrostatic forces in flocculation technology. The bioreactor system
pollutants (He et al., 2018). removed microplastics mainly through the ingestion of microbe and the
The microplastics in the effluent from WWTPs ultimately converge in formation of sludge aggregates. Advanced oxidation process affected the
the aquatic environment (rivers and oceans). Primary microplastics are physical/chemical properties of microplastics, broke the existing bonds,
broken into secondary microplastics via physical, chemical, and bio and introduced new bonds. In membrane filtration technology, in
logical treatment processes (González-Pleiter et al., 2019). As a conse teractions between microplastics and the membrane pores and surface
quence, WWTPs are considered to be the main sources of secondary made the microplastics easily adsorbed onto the membrane surface.
microplastics in the aquatic and soil environments. According to one Some of the microplastics removed from the above technologies were
investigation from a WWTP in China, the mass of microplastics dis finally transferred into the sludge, the others released from the WWTPs
charged into the water is less than <10 kg per day (Section 4.3), but due posed environmental toxicity and risks.
to its low density and small volume, the number of microplastics frag In current studies of the microplastics in WWTPs, certain problems
ments is still high (Lv et al., 2019). As listed in Tables 1 and S1, the need to be resolved in future research. To better evaluate the fate of the
abundance of the microplastics in the effluent is 5.00 × 105–1.39 × 1010 microplastics in WWTPs or other environmental media, further research
particles on a daily basis (mean value: 7.20 × 109 particles; median should focus on the development of standardized sampling and analysis
value: 2.00 × 108 particles). In other words, billions of microplastic methods. Simultaneously, further research should prioritize the study of
particles are discharged into rivers every day due to the high daily specific microplastics, especially in industrial zones. The influencing
11
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Declaration of Competing Interest
Dümichen, E., Eisentraut, P., Bannick, C.G., Barthel, A.K., Senz, R., Braun, U., 2017. Fast
identification of microplastics in complex environmental samples by a thermal
The authors declare that they have no known competing financial degradation method. Chemosphere 174, 572–584. https://doi.org/10.1016/j.
chemosphere.2017.02.010.
interests or personal relationships that could have appeared to influence
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Environment International 146 (2021) 106277

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