Chemical Engineering Journal 410 (2021) 128381

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Chemical Engineering Journal

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

Occurrence and removal of microplastics in wastewater treatment plants

and drinking water purification facilities: A review
Yan Laam Cheng a, 1, Jong-Gook Kim b, 1, Hye-Bin Kim b, Jeong Hwan Choi b, Yiu Fai Tsang a, c, *,
Kitae Baek b, *
a
Department of Science and Environmental Studies, The Education University of Hong Kong, Tai Po, New Territories 999077, Hong Kong
b
Department of Environment & Energy and Soil Environment Research Center, Jeonbuk National University, Jeonju, Jeollabukdo 57896, Republic of Korea
c
State Key Laboratory of Marine Pollution, City University of Hong Kong, Tat Chee Avenue, Kowloon, Hong Kong, China

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

Keywords: Wastewater treatment plants (WWTPs) are important sources of microplastics (MPs), having a high daily
Microplastics discharge of MPs despite a relatively high removal efficiency of MPs. Recently, MPs have been detected in
Removal drinking water purification facilities (DWPFs), indicating a direct threat to humans. In this review, we summarize
Treatment processes
published papers on the occurrence and removal efficiency of MPs, focusing on the status of removal mechanisms
Treated effluent
through different unit operations and processes. For WWTPs, the mass concentrations of MPs in influent ranged
Drinking water
Microfibers from 61 to 5,600 µg/L, and 0.5–170 µg/L of MPs were found in treated effluent, representing an overall removal
efficiency of 93.8%–99.8%. Due to limited publications using mass as MP concentration, the comparison of MP
abundance among studies was based on the number concentration. MPs have been found in influents at levels of
1.01–31,400 items/L, and in treated effluents at 0.004–447 items/L, with a high variation of MP removal from
10.2% to 99.9%. Preliminary and primary treatments contribute to MP removal, while the efficiency of sec­
ondary and tertiary treatments is highly dependent on the applied techniques. Disinfection has a relatively high
potential to breakdown MPs into smaller sizes. For DWPFs, MPs in raw water ranged from 1 to 6,614 items/L,
and 1–930 items/L of MPs were found in treated water, representing an overall removal efficiency of 66.9%–
100% regardless of the treatment types. Yet, the understanding about the role of DWPFs on MP removal is
inadequate. Although many studies on WWTPs have been published, many issues have yet to be resolved, and
further research is warranted on standardization of analytical methods and the removal mechanisms behinds to
develop effective remediation of MPs in WWTPs and DWPFs.

1. Introduction
Plastic production has significantly increased to 288 million tonnes
annually over the last 60 years and is expected to reach 33 billion tons by
2050 [1]. The problems posed by plastic debris have raised global
concerns because of widespread distribution and the associated envi­
ronmental and ecological consequences [2–4]. MPs are a subject of
mainstream research and have received more attention than
macroplastics and mesoplastics. MPs are either plastic particles between
1 µm and 5 mm in diameter or fragmented macroplastics not exceeding
5 mm [5–7]. MPs can also be categorized by shape, color, and polymer
type. However, no standardized category for MP classification has been
established [8].
MPs are classified as either primary or secondary MPs [9]. Primary
MPs are intentionally manufactured in microscopic sizes for different
applications, whereas secondary MPs are the degradation of plastic

Abbreviations: A2O, Anaerobic-anoxic-aerobic; ASP, Activated sludge process; BPA, Bisphenol A; DBP, Dibutyl phthalate; dw, Dry weight; DWPFs, Drinking water
purification facilities; FTIR, Fourier-transform infrared spectroscopy; GAC, Granular activated carbon; HDPE, High-density polyethylene; MBR, Membrane biore­
actor; MPs, Microplastics; PA, Polyamide; PAM, Polyacrylamide; PE, Polyethylene; PES, Polyester; PET, Polyethylene terephthalate; PP, Polypropylene; PS, Poly­
styrene; PVC, Polyvinyl chloride; RO, Reverse osmosis; ROS, Reactive oxygen species; SBR, Sequencing batch reactor; UV, Ultraviolet; ww, Wet weight; WWTPs,
Wastewater treatment plants.
* Corresponding authors.
E-mail addresses: tsangyf@eduhk.hk (Y. Fai Tsang), kbaek@jbnu.ac.kr (K. Baek).
1
Co-first authors.

https://doi.org/10.1016/j.cej.2020.128381

Available online 4 January 2021

1385-8947/© 2021 Elsevier B.V. All rights reserved.
Y.L. Cheng et al.
waste by external forces or the breakdown of large particles [6,10].
Fig. 1 summarizes the pathways of MPs from their points of origin to
terrestrial and aquatic environments. Boucher and Friot reported that
the major land-based source of primary MPs in marine was road runoff
(66%), followed by treated effluent from WWTPs (25%). Fibers shed
from synthetic clothes and microbeads from personal care products are
discharged into domestic wastewater and then accumulate in aquatic
environments if treatment process do not remove MPs from the influent
[11,12]. Municipal wastewater typically contains MPs from domestic
activities (e.g., washing machines and body cleaning), agriculture, and
industry, all of which are a major source of MPs. Wastewater treatment
can effectively remove MPs, but the treated effluent still contains a
considerable amount of MPs, particularly the smallest MPs which are the
most difficult to detect and remove [13]. Massive use of plastic products
and poor disposal management has resulted in the ubiquitous presence
of MPs in aquatic environments. Plastic waste from landfills or unin­
tentional disposal is another source of MPs in aquatic environments.
Although plastics are durable, they are still susceptible to degradation
through mechanical degradation, including oxidation, photo­
degradation, hydrolysis, and biodegradation at the early stages and
fragmentation afterward [14]. MPs produced by abrasion of larger
plastic products can directly enter aquatic environments through surface
runoff and deposit or accumulate on roads and soil surfaces [15,16].
Tires and coating materials are examples of MPs that erode from the use
of plastic products. MPs can be ingested by an aquatic organism, float
from one aquatic system to another, or deposit and accumulate on the
seabed or riverbed [17]. MPs are also light and can enter the environ­
ment through atmospheric fallout. Dris et al. reported that daily atmo­
spheric fallout contributes between 2 and 355 items/m2 [18]. Wind
transfer is another possible pathway for transporting MPs from one
location to another [19,20]. However, the sources and release of MPs are
difficult to trace precisely, and no standardized protocol has been
established.
Concerns about health risks and ecotoxicological impacts associated
with MPs have been raised in recent decades [21]. MPs are an efficient
Fig. 1. Sources and pathways of MPs (modified from [5,14,15,18,20,84]).
2
Chemical Engineering Journal 410 (2021) 128381
adsorbent of persistent organic pollutants due to their high specific
surface area and strong hydrophobicity [10,22,23]. The adsorption
process occurs through pore-filling or hydrophobic partitioning in­
teractions in the interlayer structure of MPs [24,25]. Chemicals,
particularly hydrophobic organic chemicals, adsorbed onto the surface
can cause a synergistic toxic effect [26–28]. MPs can also adsorb heavy
metals from the surrounding environment [29,30]. The small size and
high stability of MPs correspond with a high potential to damage or­
ganisms. With the high affinity for toxic contaminants, such as organ­
ochlorine pesticides, polycyclic aromatic hydrocarbons, and
polychlorinated biphenyls, MPs can be fatal to human beings when
absorbed and inhaled [31–33]. Concentrations of adsorbed pollutants on
MPs can reach up to 1 million times that of ambient concentrations.
According to the Marine Strategy Frame Instruction Report, the MP-
pollutant association has toxic effects on organisms in the forms of
enzyme production, nutrient dilution, reduced growth rates, and
reproductive failure and death [34].
Quantitative data has been used to report the occurrences of MPs and
calculate the MP removal in WWTPs and DWPFs. For wastewater and
drinking water samples, the commonly reported unit of MP abundance
was items per liter, whereas a few reported as items per cubic meter. For
sludge samples, the commonly reported unit of MP abundance was items
per gram (dw), whereas a few reported as items per kilogram (dw) or
items per gram (ww). The quantification of MPs is directly affected by
the analytical methods, and most studies used visual identification
through different microscopies and spectroscopies (Tables S1-S3). These
methods provided valuable information in terms of size distribution,
shape composition, color composition, and composition of polymer
types [35]. Due to MP fragmentation, it has been suspected the over­
estimation of the MP presence in the samples [36]. The mass concen­
tration of MPs has been reported as a conserved base quantity which the
physical and chemical characteristics of MPs do not affect the quanti­
fication of MPs [36]. Among considered papers in this review, two
published papers reported mass concentration of MPs, which cannot
consider for comparison in this review.
Y.L. Cheng et al.
Recently, different reviews have been published to summarize the
occurrences and fates of MPs in WWTPs and DWPFs. For WWTPs, re­
views have extensively focused on the methodologies adopted in sample
collection, MP extraction, and MP analysis [37–39]. Meanwhile, most
review papers have covered the overall occurrence of MPs in influent
and treated effluent, in terms of MP abundance and MP characterization
(i.e., size, shape, and polymer type), and MP discharged to the receiving
environment [13,37–41]. Some reviews have reported the removal ef­
ficiency of MPs in different treatment levels or by conventional unit
operations and processes [39–42]. Besides, a few papers have consid­
ered the MP retention in sludge [39,41]. However, these reviews
considered the removal of MPs based on the change in MP abundance
without considering the changes in size distributions, shape composi­
tions, and compositions of polymer types. The physiochemical charac­
teristics of MPs might have influences on the removal of MPs by different
unit operations and processes, which should be considered when
examining the removal mechanisms. Due to the limited publications in
the occurrence of MPs in DWPFs, reviews have extensively focused on
the occurrence of MPs in freshwater system and drinking water [43–45].
The discussions about the removal of MPs by water treatment are limited
when the results in published papers were mainly the occurrence of MPs
in raw water and treated water in DWPFs [43–45]. Besides, the physi­
ochemical characteristics of MPs should consider for the removal effi­
ciency of MPs in DWPFs.
This review aims to examine the removal mechanisms of MPs be­
hinds the applied unit operations and processes in WWTPs and DWPFs.
For WWTPs, it is to explore the occurrence and removal efficiency of
MPs with respect to both wastewater and sludge in terms of size, shape,
and polymer type and to evaluate the MP removal performance of each
unit operation and process in different treatment levels. For DWPFs, it is
to assess the occurrence and removal efficiency of MPs in drinking water
from the perspectives of size, shape, and polymer type and to determine
the effectiveness of MP removal by each unit operation and process in
both physical and chemical treatments.
2. Methodology
Since 2009, several studies have conducted field investigations of
MPs in WWTPs. Recent studies have considered the removal efficiency
of MPs by each unit operation and process, while the early studies have
considered only the abundance of MPs in influent and treated effluent
and the overall removal efficiency of MPs. This review extensively fo­
cuses on SCI(E), which was published from 2014 to 2020. Thirty papers
on WWTPs, including fourteen on sludge treatment, and three papers on
DWPFs have been published. The keywords included “microplastics,”
“wastewater treatment plants,” “drinking water treatment plants,” and
combinations of the terms.
For the evaluation of the effectiveness and efficiency of the removal
performance, the major concern was the actual removal rate of MPs
reported in published papers. For WWTPs, thirteen published papers
were considered because they reported the MP abundance and the
changes in the characteristics of MPs in each unit operation and process.
For DWPFs, only one published paper was considered and compared
with the results from laboratory. Since the MP concentration was re­
ported based on the number concentration, the changes in size distri­
butions, shape compositions, and compositions of polymer types were
also considered to examine the removal efficiency in WWTPs and
DWPFs. Furthermore, with the available discussion from laboratory
results, the potential effects of MPs on the performance of unit opera­
tions and processes were considered to further examine the
effectiveness.
3
Chemical Engineering Journal 410 (2021) 128381
3. Occurrences and removal of MPs in treatment plants
3.1. Occurrence of MPs in WWTPs
3.1.1. Wastewater
Municipal wastewater is a major source of MPs in WWTPs [46,47]. A
significant amount of MPs is distributed in WWTPs because of washing
machines, tire wires, and human activities [11,48–50]. The composi­
tions of MP sources are also determined by the complexity of the
wastewater collection system and the design flow of the WWTP. The
presence of MPs was greatly affected by the treatment levels (pre­
liminary, primary, secondary, or tertiary treatment as shown in Table 1).
Table 2 summarizes the MP concentrations in influent and treated
effluent from WWTPs. Based on number concentration, MPs in the
influent ranged from 1.01 to 31,400 items/L, while 0.004–447 items/L
of MPs were found in treated effluent, contributing a high variation of
MP removal from 10.2% to 99.9%. The large variations were influenced
by MP characterization (i.e., size cut-off and analytical methods) and
unit operations and processes of WWTPs (Tables S1 and S4) [55,68].
Despite a relatively low MP concentration in treated effluents, the daily
discharge of MPs was still relatively high because of the high treatment
capacity of WWTPs [39,64]. The average of the total daily discharged
MPs was 1.6 × 109 items/L (estimate based on data in Table 2). The
estimate showed >1 × 1010 items/L of MPs being discharged from some
WWTPs, indicating that the total discharged MPs were affected by
characteristics of WWTPs.
Based on mass concentration, MPs in the influent ranged from 61 to
5,600 µg/L, while 0.5–170 µg/L of MPs were found in treated effluent,
representing an overall removal efficiency of 93.8%–99.8% (Table 2).
Recently, MP quantification based on number concentration has been
criticized for exaggerating MP abundance because this involves count­
ing the numbers of suspected particles [36]. For example, one polymer
type was PP (12%) based on number concentration, but they possessed
39% in mass concentration [36]. Furthermore, due to the polymer
density and size of MPs, 27%, 14%, and 10% of acrylates, PES, and PE in
number concentration contributed 12%, 8%, and 7% in mass concen­
tration, respectively [36]. The number concentration and mass con­
centration showed opposite results. Lv et al. found that MP
concentration based on number unit dynamically increased cross-
treatment systems due to the breakdown of larger MPs [56]. The over­
all removal efficiencies of MPs were 53.6% and 82.1% based on number
concentration, but these values varied when reported on a mass basis (i.
e., 97% and 99.5%) [56]. Therefore, determining particle number and
mass simultaneously is more reasonable. MP concentration based on
mass offers a more reliable and representative approach compared with
counting the numbers of suspected MPs [36,75]. Identification and
simultaneous application of criteria for mass and particle number are
Table 1
Unit operations and processes of wastewater treatment in typical WWTPs.
Treatment levels Unit operations and processes
Preliminary Grease chamber; grid (coarse grid and fine grid); grit chamber
treatment (aerated grit chamber and rotary grit chamber); grit lift; oil
chamber; screen (bar screen, coarse screen, fine screen, step
screen); sieve; skimming tank
Primary treatment Coagulation-flocculation; sedimentation
Secondary Anoxic selector; A2O process; ASP; biofilter; filter bed; media
treatment filter; oxidation ditch; sequence batch reactor process; trickling
filter
Tertiary treatment Biological active filter; decarbonation; disc filter; dissolved air
flotation; gravity sand filter; membrane filtration
(ultrafiltration, RO); maturation pond; MBR; nitrification
Disinfection Chlorination; sodium hypochlorite disinfection; ozonation; UV
disinfection
Notes: A2O process: Anaerobic-anoxic-aerobic process, ASP: Activated sludge
process, MBR: Membrane bioreactor, RO: Reverse osmosis, UV disinfection:
Ultraviolet disinfection
Y.L. Cheng et al. Chemical Engineering Journal 410 (2021) 128381

Table 2
Overall MP removal efficiency and daily MP discharge in the selected WWTPs.
Number Treatment type Unit operations and processes Country MP concentration MP concentration Removal Discharge References
of in influent in effluent efficiency (items/day)
WWTPs (items/L) (items/L) (%)

1 Secondary Grit and grease chamber, primary Spain 3.20 0.31 90.3 1.09 × 107 [51]
sedimentation, ASP
1 Secondary Screen, grit and oil chamber, France 290 32 88.1 8.40 × 109 [52]
primary sedimentation, biofilter
1 Secondary Bar screen, primary sedimentation, Canada 31.1 0.5 98.4 3.29 × 104 [53]
trickling filter, secondary
sedimentation, chlorination
1 Secondary Step screen, sieve, grit chamber, Finland 57.6 1 98.3 1.00 × 107 [54]
primary sedimentation, ASP,
disinfection*
Pilot-scale Step screen, sieve, grit chamber, 0.4 99.3 –
membrane primary sedimentation, ASP, MBR,
bioreactor disinfection*
1 Secondary Coarse grid, fine grid, aerated grit China 79.9 28.4 64.4 5.68 × 108 [55]
chamber, primary sedimentation,
A2O process, secondary
sedimentation, chlorination
1 Secondary Aerated grit chamber, oxidation China 0.28 (5,600 µg/L) 0.14 (170 µg/L) 50.0 (97.0) 6.5 × 106 [56]
(System A) ditch, secondary sedimentation, UV
disinfection
Secondary Rotary grit chambers, A2O process, 0.06 (30 µg/L) 78.6 (99.5) 3.5 × 106
(System B) MBR, UV disinfection
1 Secondary – Sweden 15.1 0.008 99.9 4.25 × 104 [57]
1 Secondary Coarse screen, fine screen, grit and Scotland 15.7 0.25 98.4 6.52 × 107 [58]
grease chamber, primary
sedimentation, ASP
1 Secondary Screen, primary sedimentation, United 147.0 3.7 97.5 3.1 × 108 [59]
ASP, Sodium hypochlorite States
disinfection
2 Screen, anoxic selectors, ASP, 126.0–147.0 17.3–17.6 86.0–88.2 2.0–3.3 ×
Sodium hypochlorite disinfection 108
1 Secondary Coarse screen, grit lift, fine screen, Korea 29.9 0.4 98.5 1.9 × 104 [60]
primary sedimentation, A2O
process, UV disinfection
1 Coarse screen, grit lift, fine screen, 16.5 0.1 99.1 7.9 × 104
primary sedimentation, SBR, filter
bed, UV disinfection
1 Coarse screen, grit lift, fine screen, 13.9 0.3 98.0 1.1 × 105
primary sedimentation, media filter,
secondary sedimentation, UV
disinfection
7 Secondary – The 68.0–910.0 39.0–65.3 10.2–95.7 – [61]
Netherlands
7
1 Tertiary Coarse screen, grit chamber, Scotland 1–13 1–3 96 2.2 × 10 [62]
primary sedimentation, ASP,
nitrification tank
1 Tertiary Screen, grit and grease chamber, Italy 2.5 0.4 84 1.6 × 108 [63]
ASP, sand filtration, disinfection*
1 Tertiary Bar screen, grit chamber, pre- Finland 610 13.5 97.8 – [64]
aeration, primary sedimentation,
ASP, biological filter
1 Tertiary Coarse screen, grit chamber, Finland 567.8 2.5 99.6 – [65]
primary sedimentation, ASP,
biological active filter
1 Tertiary Bar screen, grit chamber, pre- Finland – 0.03–0.3 – – [66]
aeration, primary sedimentation,
ASP, biological filter, disc filter***
1 Step screen, sieve, grit chamber, – 0.005 – –
primary sedimentation, ASP,
MBR***, disinfection*
1 Preliminary treatment****, primary – 0.1 – –
sedimentation, ASP, dissolved air
flotation
1 Coarse screen, grit chamber, fine – 0.02 – –
screen, primary sedimentation, ASP,
gravity sand filter, UV disinfection
1 Secondary Bar screen, grit chamber, primary United 133.0 5.9 95.6 – [67]
sedimentation, ASP, chlorination States
1 Tertiary Bar screen, grit chamber, primary 83.3 2.6 96.9 –
sedimentation, trickling filter,
secondary sedimentation, ASP,
granular sand filter, chlorination
(continued on next page)

4
Y.L. Cheng et al. Chemical Engineering Journal 410 (2021) 128381

Table 2 (continued )
Number Treatment type Unit operations and processes Country MP concentration MP concentration Removal Discharge References
of in influent in effluent efficiency (items/day)
WWTPs (items/L) (items/L) (%)

Pilot-scale Bar screen, grit chamber, anaerobic 0.53 99.4 –

anaerobic MBR, chlorination
membrane
bioreactor
1 Primary Screen, coagulation-flocculation, Hong Kong 1.01 0.4 60.4 7.32 × 108 [68]
sedimentation, chlorination
1 Secondary Screen, grit chamber, primary 2.06 0.27 86.9 2.24 × 107
sedimentation, ASP, UV disinfection
1 Primary Screen, grit chamber, sedimentation Australia – 0.48 – 4.60 × 108 [69]
1 Secondary Screen, grit chamber, primary – 0.48 – 8.16 × 108
sedimentation, ASP, UV disinfection
1 Tertiary Screen, primary sedimentation, – 0.21–0.28 – 1.00 × 107
biological treatment**, flocculation, –3.60 × 108
dechlorination, ultrafiltration,
membrane filtration (ultrafiltration,
reverse osmosis), decarbonation
1 Secondary Grit removal, centrate thickening United 1 8.8 × 10-4 99.9 9.30 × 105 [70]
system, ASP, chlorination States
-6
7 Tertiary Primary sedimentation, ASP, – 0–2.43 × 10 99.9 7.43–2.08
gravity filter, chlorination × 102
5 Secondary**** Biological treatment** Germany – 0.08–7.52 – 4.19 × 104 [71]
3 Secondary Skimming tank, primary, – – –1.24 × 107
sedimentation, biological
treatment**
1 Tertiary Skimming tank, primary, – –
sedimentation, biological
treatment**, filtration*****
1 Biological treatment**, maturation – –
pond
2 Skimming tank, primary, – –
sedimentation, biological
treatment**, maturation pond
9 Secondary – Denmark 2,223–18,285 19–447 94.9–99.8 – [36]
(61–1,189 µg/L) (0.5–11.9 µg/L) (93.8–99.8)
1 Tertiary – 8,149 19 99.8 –
11 – – China 79.3–342.7 3.6–13.6 89.2–97.1 2.72 × 107 [72]
–1.02 × 108
11 Secondary Coarse screen, primary United – 0.004–0.195 – 5.2 × 104 [73]
sedimentation, ASP, disinfection* States –1.2 × 107
1 Tertiary Coarse screen, primary – 0.009 – 1.0 × 105
sedimentation, ASP, granular
filtration (sand, anthracite coal),
disinfection*
1 Coarse screen, primary – 0.019 – 4.1 × 106
sedimentation, ASP, biological
aerated filter, disinfection*
1 Coarse screen, primary – 0.047 – 1.5 × 107
sedimentation, ASP, granular
filtration (gravel, sand, anthracite
coal), disinfection*
1 Coarse screen, primary – 0.064 – 2.0 × 106
sedimentation, ASP, granular
filtration (gravel, anthracite coal),
disinfection*
1 Coarse screen, primary – 0.092 – 4.1 × 106
sedimentation, ASP, granular
filtration (sand), disinfection*
1 Coarse screen, primary – 0.127 – 9.6 × 106
sedimentation, ASP, granular
filtration (dual media), disinfection
*
1 Tertiary Grit chamber, primary Korea 4,200 33 99.2 8.8 × 108 [74]
sedimentation, ASP, coagulation,
ozonation
1 Tertiary Grit chamber, primary 31,400 297 99.1 1.39 × 1011
sedimentation, ASP, coagulation,
membrane filter (10 µm)
1 Tertiary Grit chamber, primary 5,840 66 98.9 1.37 × 109
sedimentation, ASP, coagulation,
rapid sand filtration

Notes: The value in blanket is the removal rate based on mass concentration. A2O process: Anaerobic-anoxic-aerobic process, ASP: Activated sludge process, MBR:
Membrane bioreactor, RO: Reverse osmosis, UV disinfection: Ultraviolet disinfection
*
The author did not state the details of disinfection adopted in the selected WWTPs.
**
The author did not state the details of biological treatment adopted in the selected WWTPs.

5
Y.L. Cheng et al.
***
Pilot-scale system was adopted in the selected WWTPs.
****
No primary treatment was adopted before biological treatment.
*****
The author did not state the details of filtration adopted in the selected WWTPs.
required.
3.1.2. Sludge
Sludge is another pathway for MPs to enter terrestrial environments,
such as landfills and soil [10,76]. Sludge treatment consists of thick­
ening, stabilization, conditioning, and dewatering (Table 3). Table 4
summarizes the MP concentration in all phases of sewage sludge from
WWTPs. MPs were measured at 18.5–21.2 items/g (dw), 4.4–113 items/
g (dw), and 4.0–27.3 items/g (dw) in primary, secondary, and MBR
sludge, respectively. A high effectiveness of sedimentation corresponded
to a high MP concentration in raw sludge but low MP abundance in the
treated effluent. The MP concentrations in stabilization were 14.2–15.4
items/g (dw), 2.7–170.9 items/g (dw), and 10.0–14.1 items/g (dw) in
thermal dried sludge, digested sludge, and lime stabilized sludge. No
comprehensive study is available showing that the sludge treatment
process will cause either MP fragmentation or MP degradation. Instead,
all published reports considered the occurrence of MPs at different
stages of sludge. The MP concentration in dewatered sludge was much
higher than in raw sludge, at 9.7–186.7 items/g (dw). Mechanical
dewatering may make a high contribution to MP fragmentation,
resulting in a significant increase in MP concentration in dewatered
sludge.
3.2. Occurrence of MPs in DWPFs
As the list of items used for regular monitoring of water quality does
not typically include MPs, and the effects of MP contamination of
drinking water on humans is unknown. Few published studies have
conducted field investigations of MP concentrations in raw water and
treated water from DWPFs. Only one field investigation focused on MP
occurrence with respect to the unit operations and processes in DWPFs,
while a few laboratory studies have investigated the effectiveness of
coagulation and ultrafiltration on MP removal [79–81]. The presence of
MPs is greatly affected by the physical and chemical treatments in
DWPFs (Table 5). Table 6 summarizes MP abundance in raw and treated
water and the overall removal efficiency in different DWPFs. The MP
concentration in raw water varied from <1 to 6,614 items/L, and the
concentration in treated water varied from <1 to 930 items/L, repre­
senting an overall removal rate of 69.9%–100% [80,83]. Despite a
relatively high rate of MP removal in DWPFs, the relatively high con­
centration of MPs in treated water implies that the treatment methods
employed in DWPFs are less efficient than those employed in WWTPs.
MPs have a low mass and are easily transported and deposited on
either land or aquatic environments by wind and rain. Apart from
contamination from dense population centers or industrial activity, the
small MPs tend to be introduced through atmospheric fallout or the
fragmentation of plastic debris in catchment areas or freshwater sys­
tems. Approximately 3 to 10 tonne of pure polymer fibers are deposited
in every 2,500 km2 annually [18]. Atmospheric fallout and wind transfer
are considered major contributors to MP occurrence in raw water. No
treatment of stormwater is typically required before it is discharged to
Table 3
Unit operations and processes of sludge treatment in typical WWTPs.
Treatment Unit operations and processes
types
Thickening Dissolved air flotation; gravity belt filter; rotary drum;
sedimentation
Stabilization Anaerobic digestion; aerobic digestion; composting
Conditioning Chemical conditioning (ferric chloride, lime, aluminum sulphate,
organic polymer); thermal conditioning
Dewatering Belt filter press; centrifugation; drying beds; plate filter press
6
Chemical Engineering Journal 410 (2021) 128381
aquatic environments; and surface runoff is therefore believed to be
another major pathway. Eroded tires and fragmented road paint enter
freshwater bodies through runoff to roadside drainage [84]. Both
intentional and unintentional disposal of MP-containing products or
plastic debris contribute secondary MPs to freshwater bodies. Water,
wind, or UV radiation can break down plastic debris into secondary MPs
[14], making MP concentration in raw water a reliable indicator of the
intensity of MP pollution in water supply sources.
3.3. MP characteristics in WWTPs and DWPFs
3.3.1. Sizes
The term “microplastics” refers to particles of a wide range of sizes
up to a few microns in diameter. The classification of MPs is greatly
influenced by size because indiscriminate definitions affect the strate­
gies used in sampling (i.e., sieves employed in field studies) [13]. Filella
et al. argued that it is impossible to compare results among multiple
studies as neither clear criteria have been adopted to define the size of
MPs nor have standardized sampling and extraction protocols been
established [85]. Common mesh sizes of sieves range from 0.7 to 500
µm, while the detection limit of sizes generally range from 10 to 250 µm
(Tables S4-S6). The selection of sieves has an influence on MP removal
rates; for example, small MPs may be lost when a sieve with a large mesh
size is used [54]. Size is an influential factor affecting MP removal by
different unit operations and processes, which one large MP can be
fragmented to several small MPs and therefore a negative removal is
reported. The differences in size fractions and unit operations and pro­
cesses in WWTPs are associated with diverse removal performances
among studies, and standardization of size fractions is compulsory for
the future studies.
Most MPs fall in the size range of 10 to 5,000 µm (Fig. S1). As influent
passes through each treatment level, larger MPs gradually reduce
whereas smaller MPs gradually increase (Fig. S1). In general, the relative
abundance of MPs > 500 µm in influent is 35.5% and reduces to 33.1%,
28.7%, and 28.1% after preliminary, primary, and secondary treat­
ments, respectively, but tertiary effluent consists of 36.8% of MPs > 500
µm. Meanwhile, the relative abundance of MPs between 300 and 500 µm
in influent generally reduces from 30.7% to 2% after tertiary treatment.
MPs > 500 µm are either removed in different treatment levels or
fragmented into smaller MPs. MPs < 300 µm commonly occupy in each
treatment level at range from 43.5% to 55.7% (Fig. S1). Although
influent only consists of 44.8% of MPs between 20 and 100 µm, this size
range remains a high level above 70.0% after preliminary treatment.
This implies that MPs are more prone to be fragmented into smaller MPs,
instead of being removed.
Several studies showed different size distributions and removal ef­
ficiencies of MPs that passed though unit operations and processes
applied [54,55,63,65,69]. Lv et al. compared the preliminary effluent
from aerated grit chamber and rotary grit chamber, which the former
effectively removed all MPs between 250 and 500 µm from influent
[56]. MPs between 250 and 500 µm increased by 27.3% after rotary grit
removal, while MPs between 125 and 250 and MPs between 25 and 62.5
µm were observed in preliminary effluent at 5.3% and 75.8%, respec­
tively [56]. Since no MPs in influent fall in these size ranges, the vortex
water flow in rotary grit chamber contributes to MP fragmentation. The
addition of mechanical stirring in grit chamber might also contribute to
MP fragmentation [56]. Therefore, preliminary treatment is likely to
facilitate the initial fragmentation of MPs or enhance the frangibility of
MPs.
Primary effluent contains 81.0% and 64.0% of MPs between 20 and
250 µm and MPs between 100 and 500 µm, respectively (Fig. S1). Pri­
mary treatment influenced the size distribution of MPs mostly among
Y.L. Cheng et al. Chemical Engineering Journal 410 (2021) 128381

Table 5

References
Unit operations and processes of water treatment in typical DWPFs.
Treatment types Unit operations and processes

[53]

[54]

[55]
[56]

[57]
[58]
[60]

[61]

[77]
[63]
[65]
[70]
[71]
[78]
Physical Clarification; flotation; GAC filtration; membrane filtration;
treatment rapid sand filtration

14.9 (A2O process); 9.7 (SBR); 13.2

Chemical Coagulation-flocculation
MP concentration in dewatered

treatment
Disinfection Chlorination; ozonation; UV disinfection

Notes: GAC filtration: Granular activated carbon filtration, UV disinfection:

sludge (items/g) (dw)

Ultraviolet disinfection

other treatment levels, which can efficiently remove MPs > 300 µm and
(Media) MPs between 100 and 300 µm at 97.9% and 99.7%, respectively [65].
240.3

186.7
Liu et al. also reported the reduction in MPs > 1,000 µm, but the portion
16.7

22.7
113
<2

47
–

–
of MPs between 20 and 300 µm gradually increased [55]. MP frag­
mentation by mechanical erosion might contribute to the reduction of
large MPs [55]. Although larger MPs are more prone to settle in primary
sedimentation, the removal performance of primary treatment might
stabilization (items/g) (dw)
MP concentration in lime

require further investigation.

In general, the removal performance of secondary treatment relies on
the presence of secondary sedimentation. Bayo et al. showed that the
portion of MPs between 200 and 600 µm significantly reduced from 61%
in aeration tank to 38% in sedimentation tank [51]. Lv et al. also indi­
cated the portion of MPs between 62.5 and 125 µm substantially reduced
12.1

from 43.7% in oxidation ditch to 0% in secondary effluent [56]. The size

–

–
–

–
–
–

–
–
–
–
–

distribution in secondary sludge reflects the removal performance of

secondary treatment, which is efficient settlement of large MPs.
Generally, large MPs (>250 µm) dominate in secondary sludge (Fig. S2).
MP concentration in anaerobic

Magni et al. reported that three-fourths of MPs in secondary sludge were

>100 µm [63]. Lv et al. indicated that all MPs in secondary sludge were
digestion (items/g) (dw)

>500 µm [56]. Leslie et al. found that 50%–66% of MPs in secondary

Notes: A2O process: Anaerobic-anoxic-aerobic process, MBR: Membrane bioreactor, SBR: Sequencing batch reactor

sludge from three WWTPs were between 10 and 300 µm [61]. Lares et al.
found that 11% of MPs were smaller than 250 µm in secondary sludge
[54]. Small MPs might be entrapped by biological flocs or coated with
biofilm, which unintentionally settled to secondary sludge. However,
170.9

4.0
–

–
–

–
–
–

–
–
–
–
–

the removal mechanism of secondary treatment remains unclear.

The removal efficiency of tertiary treatment depends on the pore size
of filter. When the pore size of filter is smaller than MPs, MPs are less
MP concentration in thermal

prone to pass through unit operations and processes applied. Ziajahromi

et al. reported that RO completely removed MPs with a size of 25–100,
MP concentrations in sludge collected from various processes in the selected WWTPs.

190–500, and > 500 µm, and those 100–190 µm were reduced by 20.8%
drying(items/g) (dw)

after RO [69]. Lv et al. showed that the portion of MPs between 62.5 and
125 µm greatly reduced from 62.5% to 16.7% after MBR, which one-
fourth of MPs in MBR sludge were between 62.5 and 125 µm [56].
Lares et al. found that 15% of MPs were smaller than 250 µm in MBR
9.0

sludge [54]. Despite the insignificant difference in the proportions of

–

–
–

–
–
–

–
–
–
–
–

small MPs in MBR sludge, MBR is a direct removal method for small
MP concentration in raw sludge

MPs, depending on the pore size of membrane.

76.3 (ww) (secondary sludge)
23.0 (secondary sludge); 27.3

0.7 (ww) (secondary sludge)

0.72 (secondary sludge); 4.0

Large MPs (>1 mm) were commonly found in stabilized sludge

1 (ww) (secondary sludge)
14.9 (primary sludge); 4.4

regardless of the stabilization methods (i.e., anaerobic digestion, lime

stabilization, and thermal drying), while small MPs (<250 µm) were
(secondary sludge)

dominant in dewatered sludge (Fig. S2). Mahon et al. indicated that

(items/g) (dw)

(MBR sludge)

(MBR sludge)

97.7%, 99.2%, and 76.0% of MPs were >1 mm in thermal dried,

digested, and lime stabilized sludge, respectively [78]. Although Lares
et al. found only one-third of MPs in digested sludge were large MPs,
62% of MPs were between 250 and 1,000 µm [54]. These results imply
–

–
–
–

–
–

–
–

that sludge stabilization may not contribute to MP fragmentation as

small MPs are rarely identified in stabilized sludge. However, limitations
Number of

on detectable sizes may have contributed to reports of low occurrence of

WWTPs

small MPs (<300 µm). For dewatering, small MPs predominated in

28
1

1
1

1
1
3

1
1
1
6
7

dewatered sludge by 76.0%–89.1% [55,61]. Mechanical dewatering

equipment, such as belt filter presses, plate filter presses, and drying
Netherlands

United States

beds, has a high potential to facilitate MP fragmentation, which can

Germany
Scotland

cause a significant increase in the fraction of MPs < 300 µm. These might
Country

Sweden
Finland

Finland
Canada

Ireland
Table 4

China
China

China
Korea

require further investigation with respect to the fate of MPs during

Italy
The

7
Y.L. Cheng et al.
Table 6
Overall MP removal efficiency and daily MP discharge in the selected DWPFs.
Country Number of Unit operations and processes MP concentration in raw
DWPFs water (items/L)
China 1 Coagulation-flocculation, 6,614.0
clarification, sand filtration, GAC
filtration, ozonation
Czech 1 Coagulation-flocculation, sand 1,473.0
Republic filtration, chlorination
1 Coagulation-flocculation, 1,812.0
clarification, sand filtration, GAC
filtration
1 Coagulation-flocculation, flotation, 3,605.0
sand and GAC filtration
Germany 5 Aeration, filtration, filtration, <1.0
filtration
Notes: GAC filtration: Granular activated carbon filtration
sludge treatment.
In general, the smallest (<10 µm) MPs predominated by 79.9%–
90.0% in raw water while MPs>50 µm accounted for <10% in raw water
(Figs. S3a and S3b). Mintenig et al. found that all MPs in raw water were
between 50 and 150 µm (Fig. S3a) [83]. DWPFs can completely remove
large MPs, and no MPs > 50 µm were observed in treated water
[80,82,83]. Complete removal of small MPs was achieved when the
DWPFs only applied triple filtrations without coagulation-flocculation
[82]. In general, DWPFs achieved a relatively high removal efficiency
of 69.9%–81.9% for MPs < 10 µm, but this size still predominated in
treated water by 75%–99.9% (Figs. S3a and S3b) [80,82]. Among
physical treatment, GAC filtration is associated with superior perfor­
mance in removing small MPs compared with other techniques
(Fig. S3b). It can remove MPs < 10 µm and 10–50 µm at a rate of 56.4%–
61.0% and 50%–100%, respectively [80,82]. Although sand filtration is
a relatively ineffective method to remove MPs < 10 µm by 31.8%, it can
completely remove MPs > 50 µm [80]. After coagulation-flocculation,
dissolved air flotation generally had a better removal performance
than clarification, regardless the sizes of MPs [80,82]. Dissolved air
flotation can achieve complete removal of MPs > 50 µm and remove
MPs < 10 µm and 10–50 µm by 79.3% and 91.3%, respectively [82].
Clarification can achieve removal of MPs > 50 µm and 10–50 µm by
97.0% and 78%, respectively, but it was ineffective to remove MPs < 10
µm at a rate of 28.3%–47.5% [80]. This implies that it is difficult to settle
small MPs, even coagulant and flocculant are added to facilitate clari­
fication. Except for coagulation-flocculation, size of MPs is not a factor
affecting the removal performance of disinfection. Ozonation and
chlorination can remove MPs between 10 and 50 µm by 41% and 50%,
respectively [80]. Yet, ozonation increased MPs < 5 µm by 8.4%, while
chlorination increased MPs between 5 and 10 µm by 4.7% [80]. The
reduction in MPs > 10 µm might not be due to the removal by either
ozonation or chlorination, but both contribute to MP fragmentation.
3.3.2. Shapes
Shape is another characteristic to reflect the removal performance by
different unit operations and processes. The morphologies of MPs
include fiber, fragment, pellet, film, and foam. Other studies classified
MPs into lines, granules, sheets, and spheres [21,86–88]. Some consid­
ered flakes and chips as shapes of MPs [39,57,73]. The surface rough­
ness of MPs had effects on removal, which fibers and pellets were less
prone to capture by mechanical methods [8]. Fragments and granules
exhibit angular and twisted morphologies and curved surfaces that are
prone to be removed [89].
Fiber and fragment shapes generally occupy a large proportion of
MPs in influent at 61.7% and 47.8%, respectively (Fig. S4). Lv et al.
showed that the influent contained no fragment, but the preliminary
effluent from aerated grit chamber and rotary grit chamber contained
40.9% and 84.1% of fragment, respectively [56]. Although both used
different mechanisms to remove solids, the turbulence of water flow in
8
Chemical Engineering Journal 410 (2021) 128381
MP concentration in Removal Discharge References
treated water (items/L) efficiency (%) (items/day)
930.0 85.9 1.1 × 1014 [80]
443.0 69.9 1.4 × 1011 [82]
338.0 81.3 2.9 × 109
628.0 82.6 4.8 × 109
<1.0 100 – [83]
each unit design facilitate MP fragmentation by mechanical breakdown.
Influent contained 21.5 and 8.54 items/L of fibers and fragments,
respectively, which was reduced by 92.7% and 89.1% in fibers and
fragments, respectively, after primary treatment [53]. Fibers and frag­
ments reportedly accumulate in primary sludge to fractions of 65.1%
and 34.2%, respectively, while a few foams and pellets can be found in
primary sludge, at 0.5% and 0.2%, respectively [53]. Since primary
sedimentation removes MPs by gravity, the removal of particular shape
corresponds to the polymer type. Without chemical or biological pro­
cesses, the removal efficiency of primary sedimentation is solely
dependent on the density of MPs, which the polymer types of fiber are
usually high in density. Besides, fiber might be adhered on the surface of
suspended solids and unintentionally removed in primary treatment.
Chemically enhanced primary treatment can achieve the removal of fi­
bers and fragments by 88.9% and 47.7%, respectively [68]. Fibers might
be entrapped by flocs or adhered on flocs, which warrant further
investigation on the removal mechanism.
ASP removed 57.6% and 56.9% of fibers and fragments from primary
effluent [51,53,54,64,65,68,74]. Particularly, secondary sedimentation
contributed to the removal of 82.0% and 81.1% of fibers and fragments,
respectively [51]. Similar to primary treatment, the biological flocs
collide with all shapes of MPs, enhancing the accumulation rate of fibers
and pellets in secondary sludge. In secondary sludge, fiber is still the
predominant shape by 50%–100%, followed by fragments (5.7%–25%)
[53,54,56,61]. Neither foams nor pellets were identified in secondary
and MBR sludge [53,54,56,63]. These findings imply that secondary
sedimentation has a greater potential to settle fibers and pellets, while
primary sedimentation is more effective for settling fragments.
The removal efficiency of tertiary treatment depends on the unit
operations and process applied. Fibers and fragments were increased by
4.7% and 210.9%, respectively, after biological active filter, because
fragmentation occurred at the fiber-made filter [65]. Meanwhile, fiber is
more prone to longitudinally pass though rapid sand filtration [69].
Lares et al. found that MPs were composed of 88.3% fibers and 11.7%
fragments in MBR sludge, whereas Lv et al. found no MP fibers in MBR
sludge, which instead consisted of fragments (75%) and films (25%)
[54,56]. The variations in shape composition in MBR sludge shows that
MBRs may not be able to remove certain shapes, whereas the removal
efficiency of MBR is a function of size. Despite a relatively high removal
rate for fibers and fragments at different treatment levels, fibers and
fragments are still dominant in treated effluent at 26.9% and 32.5%,
respectively (Fig. S4), reinforcing the need for a better understanding of
removal mechanisms.
The composition of MP shapes is similar among different stages of
sludge, except for dewatered sludge (Fig. S5). Fiber is still the dominant
shape, appearing as 82.4%, 87.0%, and 62.1% of MPs in digested,
thermal dried, and lime stabilized sludge, respectively [54,78]. With the
exception of a relatively high proportion of fragments (37.0%) in lime
stabilized sludge, fragments represented 7.5% and 8.4% of MPs in
Y.L. Cheng et al.
digested and thermal dried sludge, respectively [54,78]. Meanwhile,
sludges stabilized by different methods contained<3.1% and 0.4% of
films and pellets, respectively [54,78]. The insignificant difference in
the shape compositions between raw and stabilized sludge implies that
sludge stabilization has no effect on removal of certain shapes or MP
fragmentation. Despite relatively high variation in fiber constituents
(15%–72.5%) in dewatered sludge, the fragment was the major shape in
dewatered sludge, appearing as 22.2%–75.8% of MPs, followed by film
(12.9%–14.0%) [55,57,60,90]. The proportion of pellets increased in
dewatered sludge, with Liu et al. and Li et al. reporting 17.1% and 1.3%
pellet content in dewatered sludge, respectively [55,90]. Mechanical
dewatering may therefore contribute to increases in fragment, film, and
pellet by MP fragmentation.
In general, DWPFs are more capable to remove pellets and frag­
ments, regardless the unit operations and processes applied (Fig. S6a).
DWPFs can effectively remove pellets and fragments at rate of 75.7%–
91.0% and 73.7%–85.5%, respectively, but the effectiveness on fiber
removal varied from 25.0% to 89.2% [80,82]. Fiber removal (25.0%)
was the worst when DWPFs adopted only coagulation-flocculation and
sand filtration (Fig. S6a) [82]. The unit operation and process adopted
after coagulation-flocculation is critical to determine MP removal, with
clarification tending to remove more fibers and pellets, and flotation
more capable of removing fragments [82]. Although clarification
removed 54.6% of fibers from raw water, the removal efficiency of
fragments and pellets was relatively low, at 36.3% and 29.8%, respec­
tively [80]. Since PET particles are mostly in the shape of fiber and PET
has 1.38 g/cm3 of density, fibers are more prone to be settled during
clarification. In addition, fibers might be entrapped to flocs or adhered
on the surface of flocs, which enhanced the removal of fibers during
clarification.
Among physical treatments, GAC filtration had better removal per­
formance than sand filtration, regardless the shapes of MPs (Fig. S6b)
[80]. It is simply because the efficiency of sand filtration is corresponded
to sizes of MPs, while the effectiveness of GAC filtration is related to the
polarity of MPs. Since the clarified water consisted of 5.4% of MPs > 10
µm, this limited the removal performance of sand filtration with the
efficiency no >40% regardless of shapes [80]. Besides, the porous spaces
between filter media allowed the penetration of small MPs, which the
treated water from sand filtration contained 52.6% and 29.5% of fibers
and fragments, respectively [80]. Meanwhile, PE and PP particles are
mostly in the shape of pellets and fragments, which are more prone to be
adsorbed during GAC filtration. This achieved removal of pellets and
fragments by 81.5% and 66.0%, respectively, which was the most
effective methods among other techniques [80]. Except from
coagulation-flocculation, shape of MPs is not a factor affecting the
removal performance of disinfection. Despite the insignificant removal
of pellets by 1.8%, ozonation increased fibers and fragments by 6.0%
and 7.9%, respectively [80]. Wang et al. explained that the shearing
force of the flow induced the breaking of MPs into fibers and fragments
[80]. Meanwhile, although chlorination reduced fibers and fragments by
4.4% and 12.5%, respectively, pellets were increased by 16.9% after
chlorination [80]. The increase in particular shape might be due to the
chemical degradation and fragmentation of the corresponding polymer
type.
3.3.3. Polymer types
The term polymer refers to the chemical structures and properties of
MPs, which are useful indicators of their fate and the pathways of MPs in
WWTPs [75]. The composition of polymer types corresponds to shape
composition. PES (60%–96.3%) and PA (3.1%–20%) particles are usu­
ally fibrous MPs, while PE (63.9%–78%), PP (20%–100%), and PS
(12%–80%) particles are commonly found in the shapes of fragments
and pellets [54,56,63]. The reduction of particular polymer type might
indicate the removal of the corresponding shape. Yet, the composition of
polymer types is rather difficult to compare, because studies have
adopted random sampling on identification and validation of suspected
9
Chemical Engineering Journal 410 (2021) 128381
MPs in samples. Gies et al. only verified part of the suspected MPs in
influent and primary effluent, and no information about polymer types
was provided for secondary effluent [53]. Complicating matters further
are misleading results from non-MPs. Other than MPs, non-plastics such
as glass and silica have been identified because of confusion arising from
similar colors and shapes [55]. Blair et al. reported that only 39% of
1,308 suspected particles were confirmed to be MPs [62]. Bayo et al.
found that MPs comprised 46.6% of suspected particles, with the bal­
ance composed of silicon dioxide, silicates, and cellulose [51]. Failure to
consider the suspected MPs particles at each treatment level can lead to
confusion regarding MP removal efficiency. Without standardized
criteria for MP characterization and identification, it is difficult to
determine which treatment methods have a greater potential to remove
low density of MPs.
More than 23 polymer types of MPs, including 11 co-polymers, have
been detected in wastewater to date (Tables S4) [51,58,63]. Except PVC,
PA, PE, PES, PET, PP, and PS are commonly detected in wastewater and
sludge samples. Generally, polymers of higher density are more common
in raw sludge, while polymers of lower density are more common in
treated effluent. Lares et al. reported that the portion of PES gradually
reduced from 90% to 49% between influent and secondary effluent,
while 95% of MPs were PES in secondary sludge [54]. Meanwhile, they
also found that the portion of PE gradually increased from 5% to 36%
between influent and secondary effluent, while only 5% of MPs were PE
in secondary sludge [54]. Although Magni et al. identified a relatively
high proportion of PE (18%) in secondary sludge, two-thirds of the MPs
in secondary sludge contained high-density polymers, including PES,
polyacrylates (1.05 g/cm3), polyetrafluorethylene (2.2 g/cm3), and
polyurethane (0.96–1.26 g/cm3) [63]. These results imply that polymer
type is a crucial factor affecting the retention of MPs in sludge or the
maintenance of MPs in wastewater.
Unlike MP fragmentation into small size or angular shape, polymer
type of MPs does not change to another type because of fragmentation.
This can be an indirect tool to indicate the potential fate of MPs in
different treatment level. Despite a relatively high retention of PES in
secondary sludge, secondary effluent still contained 23% of PES fibers
[63]. Simultaneously, fibers increased by 68.0% after secondary treat­
ment [63]. These imply that PES fibers might be fragmented during
treatment process; therefore, the composition of PES and fibers
increased in secondary effluent. Murphy et al. found that the composi­
tions of PA, PES, and PP gradually increased from influent to treated
effluent, but no information about the changes in shape composition was
provided [58]. The relationship between shape and polymer type of MPs
should be carefully considered in the future research on the fates of MPs
in wastewater treatment.
The proportions of polymer types in digested sludge are similar to
those of raw sludge. PES is the major polymer type in digested sludge at
86%, followed by PA (6%) and PE (4%) [54]. Due to limited results and a
lack of standardized criteria, it is difficult to determine whether diges­
tion can degrade polymers. Significant changes among different studies
were found in the proportions of polymer types in dewatered sludge. PE
and PP were the major polymer types in dewatered sludge, at 40% and
34%, respectively [55,58,71]. Meanwhile, Liu et al. and Mintenig et al.
identified 58% and 0%–20% of PA in dewatered sludge, respectively
[55,71]. A small amount of PES (16.7%) was identified in dewatered
sludge [58]. PS particles (7%) were identified in dewatered sludge, but
no PS was found in raw sludge or digested sludge [58,71]. Neither PVC
nor PET were identified in the dewatered sludge [55,58,71]. Sudden
changes in the compositions of polymer types many warrant further
investigations of the fate of MPs during sludge treatment.
Since coagulation-flocculation is a common unit operation and pro­
cess, the presence of PAM in treated water is significantly relevant to
water treatment. PAM is added as flocculant to facilitate the floc for­
mation, but no unit operation and process can completely remove PAM
from water [80,82]. GAC filtration is associated with superior perfor­
mance in removing PAM particles compared with other techniques [80].
Y.L. Cheng et al.
Besides, GAC filtration had the highest removal rates of PET, PE, and PP
particles compared with other techniques [80]. Unlike other physical
treatments, the removal mechanism of GAC filtration is depended on the
polarity of solids, in other words, the polymer type is a significant factor
affecting the removal efficiency of GAC filtration. Since PE and PP
particles are non-polar MPs, GAC filtration achieved 77.6% and 62.1%
of removal on these MPs [80]. Meanwhile, the efficiency of clarification
is also depended on the polymer types, which density of MPs is associ­
ated with the settlement. Clarification was responsible to settle 52.7% of
PET particles, which shared equal contribution with GAC filtration [80].
Although PE and PP particles have<1 g/cm3 of density, clarification
achieved 48.8% and 47.4% of removal, respectively [80]. This implies
that coagulation-flocculation plays a significant role in agglomeration of
MPs to flocs, which facilitate the removal of light-density MPs during
clarification.
Polymer type of MPs is also crucial to examine the effects of chemical
treatment on MPs. Undoubtedly, both ozonation and chlorination have
no effects on MP removal when the reduction of each polymer type is
<7% [80]. Additionally, these might induce chemical degradation and
thereby accelerate MP fragmentation. PET and PE particles increased
after ozonation by 10.2% and 5.4%, respectively, while chlorination
increased PP particles by 4.1% [80]. Yet, the effects of ozonation and
chlorination on MPs might require further investigation. Despite a
relatively high removal of PET particles by 44.3%, the effectiveness of
sand filtration is not corresponded to the polymer type of MPs. Since the
removal of fibers was slightly higher than the removal of other shapes,
the removal of PET particles was correspondingly higher than the
removal of other polymer types.
Fig. 2. Removal efficiency of MPs in different unit operations and processes in the selected WWTPs.
10
Chemical Engineering Journal 410 (2021) 128381
3.4. Removal of MPs in WWTPs
Preliminary, primary, secondary, and sometimes tertiary treatments
are used to purify wastewater with physical, chemical, and biological
treatments and to meet discharge standards for biochemical oxygen
demand and total suspended solids (Table 1). Drawing on data from 13
studies, the removal efficiency was evaluated, with influent MP quan­
tities varying from 1.01 to 31,400 items/L. The removal efficiency of
MPs by preliminary treatment reached 6.0%–58.6%. Primary treatment
contributed an extra 19.1%–99.0% to removal, whereas MP elimination
in secondary treatment varied from − 66.7% to 92.6% (Fig. 2). Mean­
while, the removal efficiency by tertiary treatment ranged from –72.7%
to 99.9% (Fig. 2). Unit operations and processes in each treatment level
and the characteristics of MPs contributed to different removal effi­
ciencies. This heterogeneous value can be attributed to diverse unit
operations and processes associated with different treatment levels
(Fig. 2). The removal efficiency differed according to treatment level.
3.4.1. Preliminary treatment
MP removal in preliminary treatment has received relatively little
attention, and few studies have considered the removal efficiency of MPs
by preliminary treatment [56,58,62,67]. Unit operations and processes
in preliminary treatment are not designed to remove MPs from influent,
but 6.0%–58.6% of MPs are unintentionally removed (Table S7). The
typical screen size is >6 mm; therefore, MPs may be removed when they
are attached to large debris or entrapped in large debris [67]. Yet, it is
still possible for direct removal of MPs if fine screen or microscreen are
employed in WWTPs.
In general, preliminary treatment achieved a relatively high removal
Y.L. Cheng et al.
of MPs. Michielssen et al. reported that the removal efficiencies of pre­
liminary treatment in two WWTPs were 58.6% and 35.1%, which both
WWTPs have adopted bar screen and grit chamber for preliminary
treatment [67]. Despite no detail information about the changes on size
distribution, size composition, and composition of polymer type, MPs
might be adhered on the surface of large debris or unintentionally
captured along with large debris during preliminary treatment. Murphy
et al. also found that screening and grit/grease removal contributed to a
removal rate of MPs at 44.6%, while grit and grease contained <2 and
7.9 items/g of MPs, respectively [58]. PE particles were substantially
removed at a rate of 85.2%, followed by PP particles (74.4%) and PA
particles (71.7%) [58]. Besides, abundant PE microbeads from a facial
cleanser were observed in the grease at a rate of 32.2% [58]. Although
the microscopic sizes of MPs are more prone to pass through preliminary
treatment, the light-density of MPs float on the surface and water and
are ready to be skimmed during grease removal [58]. The removal of
MPs by preliminary treatment is therefore unintentional results of
screening and grit/grease removal.
Considering the design of preliminary treatment, the performance of
MP removal in preliminary treatment varies. Blair et al. reported that the
removal efficiency was only 6% in preliminary treatment, but they did
not provide a detailed explanation [62]. Since the coarse screen of
selected WWTP has targeted to remove solids >12 mm, MPs are prone to
pass through screening. In the study of Murphy et al., the targeted sizes
of solids are >19 mm and 6 mm, which might be possible to remove
larger MPs. Furthermore, the removal performance of MPs by grit/
grease chamber depends on the designs of unit operation and process.
MP concentration in aerated grit chambers was reduced by 21.4%,
whereas that in a rotary grit chamber increased by 371.4% [56]. In the
aerated grit chamber, the addition of air causes a spiral water flow, and
both heavier grit and lighter organic particles are thrown out and settled
after hitting the side wall. The turbulence in water flow might facilitate
MP removal, when the light-density of MPs is pull in the turbulence and
entrapped with heavier solids. Rotary grit chamber creates vortex water
flow, which solids with a specific gravity of 2.4 to 2.65 are settled by
gravity. The vortex water flow might pull down light-density of MPs, the
friction force from mechanical stirring causes MP fragmentation. Rotary
grit chamber removed 35.3% of MPs > 0.5 mm, the dominant portion of
small MPs (25–62.5 µm) in the preliminary effluent implied a break­
down of MPs from mechanical stirring in the rotary grit chamber [56].
Preliminary treatment may therefore facilitate the initial fragmentation
of MPs in wastewater.
3.4.2. Primary treatment
Studies have generally considered the MP removal in primary
treatment combining with preliminary treatment, which achieved a
relatively high removal of MPs at a rate of 40.7%–97.9%
[53,55,64,65,74]. As shown in Fig. 2 and Table S7, 19.1%–99.0% of MPs
are removed in primary treatment, which is the major level to remove
MPs from wastewater. The common method adopted in primary treat­
ment is sedimentation. Circular and rectangular tanks are common de­
signs for sedimentation, which circular designs are associated with
superior sedimentation performance [91]. No study has examined MP
removal rate according to the designs of the sedimentation tank, but MPs
are prone to remove with suspended solids [92]. After primary treat­
ment, low density of MPs remains in the primary effluent and can be
released to the environment or secondary treatment, while settled MPs
are transferred to disposal or sludge treatment. Future research should
not only consider the MP removal in preliminary and primary treat­
ments separately, but also estimate the removal efficiency of each unit
operation and process in preliminary treatment.
Sedimentation in primary treatment is the major contributor of MP
removal along WWTPs, which achieves 19.1%–99.0% of removal
(Fig. S2). Michielssen et al. reported a relatively high MP removal by
sedimentation in two WWTPs (i.e., 61.6% and 82.1%) [67]. Blair et al.
also reported a high MP removal by sedimentation with a rate of 60%–
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Chemical Engineering Journal 410 (2021) 128381
76% [62]. Besides, Murphy et al. indicated a moderately high removal
efficiency of MPs by sedimentation (i.e., 60.9%) [58]. The absence of
PVC particles and a few PS particles (5.9%) were observed in primary
effluent, whereas it contained 14.7% of PE particles [58]. Since the
removal mechanism of sedimentation is the settlement of suspended
solids by gravity, high-density of MPs are settled by sedimentation,
while the light-density of MPs pass through sedimentation. This implies
polymer type is a major factor affecting the removal efficiency of sedi­
mentation. Both PES and PA particles have density higher than 1 g/cm3,
but abundant of PES fibers (29.4%) and PA fibers (14.7%) were observed
in primary effluent [58]. Additionally, Bayo et al. reported a poor
removal performance of MPs by sedimentation (i.e., 19.0%), which fi­
bers increased by 21.4% comparing with influent [51]. Even the density
of MPs is higher than that of wastewater, shape, especially fibrous MPs,
might be a significant factor when considering the removal performance
of sedimentation. Furthermore, Lares et al. reported an almost complete
removal of MPs by sedimentation with a rate of 99.0% [54]. Over 98% of
removal was found in each size range (i.e., 1–5 mm, 0.5–1 mm, 0.25–0.5
mm, and < 0.25 mm); thereby sizes of MPs did not affect the removal
efficiency by sedimentation [54]. To conclude, sedimentation is a sig­
nificant unit operation and process in removing MPs, which shape and
polymer type of MPs might influence the removal performance by
sedimentation.
Another method employed in primary treatment is coagulation-
flocculation, which is a chemically enhanced sedimentation [93,94].
This can achieve 50.0%–97.9% of MP removal (Fig. S2). The addition of
coagulants such as alum or ferric chloride and gentle stirring facilitate
floc formation, enhancing sedimentation by increasing particle sizes
[42]. Although Talvitie et al. considered the removal efficiency of
coagulation-flocculation combined with the preliminary treatment, the
removal efficiency of MPs varied from 50% to 97.9% [64,65]. Ruan et al.
found that the chemically enhanced primary sedimentation had MP
removal by 78.2%, whereas the traditional sedimentation only reached
41.7% [68]. Based on the changes in shape composition comparing with
influent, coagulation-flocculation can achieve the removal of fibers and
films by 93.2% and 86.3%, respectively, while the removal of fragment
varied from 32.4% to 96.4%. Fibers might be entrapped during floc
formation or adhered on the surface of flocs, which accidentally
removed by coagulation-flocculation. This requires further investigation
in laboratory to verify whether coagulation-flocculation achieve higher
removal of MPs in terms of shapes.
3.4.3. Secondary treatment
Secondary treatment is typically used to remove suspended or dis­
solved organic matter and nutrients through different biological unit
operations and processes. Sun et al. summarized that secondary treat­
ment achieved 0.2%–14%, while Gatudou et al. indicated secondary
treatment contributed to additional removal by 7%–20% [37,39].
However, the removal efficiency of MPs varied from –66.7% to 92.6% in
secondary treatment (Fig. 2 and Table S7). During biological treatment,
bacteria can attach to and form a biofilm layer on MP surfaces, causing
the bacteria-associated MPs to settle in a final sedimentation tank as
secondary sludge [51,95]. This suggests that MPs could be redistributed
from the liquid to solid phase. However, few studies have investigated
MP-microorganism interactions (such as biofilm formation, aggregation,
and inhibition) or the mechanisms behind MP removal by biological
treatment. MPs may leach additives to wastewater or adsorbed organic
pollutants and heavy metals from wastewater. This leachate may inhibit
or suspend the growth of microorganisms or the formation of biological
floc. However, the fates of MPs in biological treatment remains unclear.
ASP has a superior removal performance of MPs in secondary
treatment. The removal efficiency of MPs by ASP varied from –66.7% to
92.6% (Fig. 2). During ASP, MPs are entrapped in biological flocs and
then be separated from primary effluent [51,65,74]. Unlike primary
sedimentation, secondary sedimentation achieved an average of 71.3%
fiber removal [51,64,65,68,74]. The sedimentation after aeration allows
Y.L. Cheng et al.
the settlement of biological flocs, which suspended fibrous MPs might be
further entrapped by the moving down flocs or adhered on the surface of
biological flocs. Bayo et al. showed that the MP removal by aeration
achieved only 17.8%, whereas secondary sedimentation enhanced MP
removal by 85.4% [51]. This implies that sedimentation might be an
important unit operation and process in secondary treatment, which
allow an additional MP removal during settlement of biological flocs.
However, Lares et al. reported a negative removal of MPs by ASP at a
rate of –66.7% [54]. With the availability of sedimentation, secondary
treatment serves to remove the remaining MPs from primary effluent,
which the sizes of MPs are smaller, and the density of MPs are lighter.
Apart from ASP, a few studies have considered the removal efficiency
of MPs by other unit operations and processes in secondary treatment.
Oxidation ditch is a relatively effective unit operation and process to
remove MPs, which achieved 95.6% [56]. Most MPs, especially 92.3% of
fibers, were entrapped by activated sludge [56]. However, based on
mass concentration, the removal efficiency by oxidation ditch only
reached 16.5% [56]. In general, A2O process is less effective in removing
MPs with a variation from –21.2% to 28.1% (Fig. 2). To note, A2O
process achieved 15% of MP removal based on mass concentration [56].
The recirculated sludge in A2O process might contribute to the relatively
low MP removal by A2O process, which MPs were accumulated within
A2O process [56]. Both studies showed an increased in fibers from
22.1% to 257.1%, while MPs between 0.1 and 1 mm increased by
115.8% [55,56]. During A2O process, stirring in anaerobic and anoxic
tanks and aeration in aerobic tanks might enhance the friction force in
the water, which cause MP fragmentation. Yet, this requires further
investigation.
3.4.4. Tertiary treatment
Tertiary treatment is the final cleaning process to further improve the
quality of treated effluent before it is reused or discharged to the envi­
ronment [71]. Either advanced techniques (membrane filtration, MBR,
dissolved air flotation, and activated carbon adsorption) or conventional
techniques (sand filtration and disc filters) are employed, depending on
site-specific needs and opportunities to use the resulting effluent
(Table 1). Tertiary treatment provides an additional MP removal op­
portunity for WWTPs, with a removal efficiency from –72.7% to 96.3%
(Fig. 2). Filtration (MBR, gravity bed filter, sand filtration, and disc fil­
ters) is a common strategy used in tertiary treatment. MBR is the most
effective technique for MP removal when the pores of the membrane are
smaller than 0.1 µm [56]. Talvitie et al. found that MBR achieved nearly
complete (99.9%) removal of MPs, with the treated effluent containing
only 0.005 items/L of MPs [66]. Lv et al. investigated a parallel system
in secondary WWTPs, reporting that one of the systems that adopted
membrane filtration to replace traditional sedimentation achieved
80.5% MP removal in treated effluent (0.028 items/L of MPs) [56].
During MBR, MPs is directly captured by the membranes, which the
permeate contains a few amount of MPs. However, the presence of MPs
might induce frequent clogging in MBR, which require backwash to
clear the sludge cake layer. During backwash, MPs might accidentally
release and pass through tertiary treatment. Thus, the removal perfor­
mance of MBR varies, depending on the frequency of backwash and the
pore size of membrane.
Apart from MBR, the removal efficiency of rapid sand filtration and
disk filters varies among published reports. Since the porosity of filter
media is larger than MPs, MPs are more prone to pass though rapid sand
filtration. However, the removal efficiency of MPs by rapid sand filtra­
tion ranged from 55.6% to 95.0% (Fig. 2). During rapid sand filtration,
MPs are entrapped by filter media (i.e., sand grains) or adhered on the
surface of filter media [66]. Meanwhile, the removal efficiency of MPs
by disc filters varied from 40.0% to 98.5% (Fig. 2). The removal per­
formance by disc filters depends on the pore size of filters. Remarkably,
the MP removal by 10 µm sized disc filter (i.e., 40.0%–79.6%) was worse
than 20 µm sized disc filter (i.e., 98.5%) [66,74]. The presence of MPs
induced clogging in disc filters, requiring frequent backwash [74].
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Chemical Engineering Journal 410 (2021) 128381
During high-pressure backwash, some MPs can pass through the filter,
resulting in lower removal efficiency [74]. The removal efficiency of
MPs is highly dependent on the size of the filter pores, which MBR has
the best MP removal among the techniques of physical filtration. The
porosity of filter media in rapid sand filtration is much larger than in
other techniques, MPs are more prone to passing through this unit
operation and process.
In contrast, tertiary treatment does not guarantee superior perfor­
mance in MP removal compared with other treatment levels. Mason
et al. found no clear correlation between tertiary treatment and MP
removal after examining 17 different WWTPs in the United States [73].
The pore size of RO systems is the smallest among the membrane
techniques and should exhibit the best performance of MP removal.
However, Ziajahromi et al. found that RO was associated with an un­
expectedly low removal efficiency of 2.8% but provided no detailed
explanation [69]. Talvitie et al. reported that a biological active filter
was ineffective at removing MPs, contributing to a negative removal of
72.7% [65]. Furthermore, Carr et al. showed that MP removal perfor­
mance by gravity filtration in bench-scale research was superior to
practices in WWTPs, and no MPs were detected in bench-scale backwash
[70]. Tertiary treatment therefore contributes both positive and nega­
tive effects to MP removal.
3.4.5. Disinfection
Chlorination, ozonation, and UV radiation are disinfection methods
employed in WWTPs before discharging the treated effluent [42,96].
These disinfectants might degrade MPs or break them into smaller sizes,
and even nanoplastics, before they degrade in the environment. How­
ever, no study has focused on the fate of MPs before and after disin­
fection and our understanding of the effect of disinfection on MP
removal is limited.
Ozone is a strong oxidant that can be converted into radicals causing
degradation of polymers [97]. Ozonation can reportedly contribute to a
removal rate of MPs at 89.9%, and a decrease in MP concentrations to 33
items/L [74]. Meanwhile, ozonation can contribute to decomposition of
MPs, but no detail explanation was provided [98]. To the best of our
knowledge, ozonation can degrade MPs within a brief contact time, but
the fate of MPs before and after chlorination has not been yet investi­
gated in detail.
Due to large surface-to-volume ratios, MPs are more prone to re­
actions in chlorination. Michielssen et al. found that chlorination
contributed to a removal rate of MPs at 7%, but no explanation was
provided [67]. Liu et al. found that MP concentrations were reduced by
7.1% after chlorination, and the treated effluent contained 28.4 items/L
of MPs [81]. Kelkar et al. stated that PP, HDPE, and PS are resistant to
chlorination and their chemical and physical structure does not change
[99]. However, Ruan et al. reported that MP abundance increased by
81.8% after chlorination, because intense redox reactions contributed to
the breakdown of MPs [68]. Low density of MPs is prone to breakdown
during chlorination [68]. The fate of MPs during chlorination is uncer­
tain, but the chemical interactions between MPs and chlorination leads
to the formation of new bonds and structures and alters the adsorption
mechanisms between MPs and other organic pollutants.
The fate of MPs before and after UV disinfection has yet to be
investigated in detail [56,68]. Lv et al. reported that UV disinfection
contributes to a removal efficiency of 1%, breaking MPs into smaller
sizes by oxidation [56]. Photochemical reactions during UV disinfection
enhances the frangibility of MPs by reducing elasticity and absorbing
light [16]. In addition, Naik et al. reported that UV radiation can alter
the surface of HDPE, transforming smooth MPs into fibrous particles
[100]. Contrary to HDPE, PS and PP polymer types did not physically
degrade [100]. Due to rough surfaces and the presence of oxygen-
containing functional groups, UV irradiation accelerated the aging of
PS, and enhanced the adsorption capacity of MPs after aging [101]. The
effects of UV disinfection, especially on molecular structure, are influ­
enced by the polymer types of MPs.
Y.L. Cheng et al.
3.4.6. Factors affecting MP removal in WWTPs
Overall, the removal efficiency of MPs varies among different
treatment levels. First, the operating conditions of unit operations and
processes affect overall MP removal. For example, high MP concentra­
tions accelerate clogging in membrane techniques, which requires
frequent backflow and reduces removal efficiency of the membrane
techniques [74]. The same technique with different operating conditions
(e.g., hydraulic retention time, flow rate, and treatment capacity) can
alter MP removal. Lv et al. indicated that the variations of MP removal
between two preliminary systems were caused by different hydraulic
retention times [56]. Second, the characteristics of the influent deter­
mine the MP concentrations and characteristics of MPs in the influent
and affect the overall removal efficiency of MPs. Gündoğdu et al. re­
ported that influent is highly dependent on population, flow, seasonal
variations, and sources (i.e., domestic wastewater or industrial waste­
water) [46]. The presence of MPs in industrial influent was 1.8 times
greater than that from domestic influent [8]. Bayo et al. described a
relationship between seasonal variability and MP abundance [51]. MP
concentrations among seasons showed significant statistical differences,
with summer higher than other seasons [51]. In general, composition of
polymer type detected in a WWTP reflects daily life of the people the
plant serves [13,57,70,72]. Influent from urban WWTPs may contain
primarily PE, PP, PA, and PES, because of the use of personal care
products and toothpaste, and the washing of synthetic clothes
[58,69,70,73]. In contrast, industrial wastewater contains high amounts
of PA, PE, and PP [55,72]. Third, different unit operations and processes
contribute to different removal mechanisms of MPs among treatment
levels. Table 1 shows that various unit operations and processes are
employed in WWTPs, depending on site specifics. The removal mecha­
nism in preliminary treatment is mainly unintentional removal by
screening and grit/grease removal through entrapment between MPs
and solids or adherence to the surface of solids, whereas MP removal in
primary treatment (i.e., sedimentation) is determined by the polymer
type and shape. Secondary treatment (i.e., biological treatment)
removes MPs from wastewater by exploiting interactions between mi­
croorganisms and MPs (e.g., biofilm formation) and the presence of
secondary sedimentation. The effectiveness of tertiary treatment varies
among unit operations and processes being employed and cannot
guarantee significant MP removal. In particular, the effectiveness of
filtration depends on the pore sizes of the filter media and the frequency
of clogging. In general, different factors, including site-specific WWTPs
(design of treatment levels, treatment capacity, and flow rate), MP
characteristics (size, shape, and polymer type), and operating conditions
of unit operations and processes contribute to performance of MP
removal. Considerable research is needed on other parameters affecting
MP removal.
3.5. Sludge treatment
Despite the lack of comprehensive studies of the occurrence of MPs
from raw sludge to dewatered sludge, the existence of MPs in sludge is
acknowledged to pose a threat to the performance of anaerobic diges­
tion. The presence of MPs can affect anaerobic digestion in terms of
methane production, induction of ROS, and hydrogen production under
alkaline anaerobic fermentation [102,103]. With the presence of PVC
particles in anaerobic digestion, the microbial populations in metha­
nogens, hydrolytic microbes, and acidogens changed slightly, with
methane production eventually reduced to 75.8% in the presence of 60
PVC items/g [102]. However, the impacts of the presence of MPs may
depend on the type of MP polymer. With the presence of PE particles at
the same concentration levels as PVC MPs, a significant reduction in
methane production was found [104]. Leachate from MPs such as BPA
and DBP also inhibited performance in anaerobic digestion. A total of
3.6 µg/L of BPA was released when the concentration of PVC particles
was 60 items/g [102]. Although no clear explanation is available on the
effects of BPA leachate on methane production, a strong relationship has
13
Chemical Engineering Journal 410 (2021) 128381
been found: a high MP concentration corresponds to a high concentra­
tion of BPA, and less methane is produced [102]. Wei et al. reported
finding DBP leachate during alkaline anaerobic fermentation in the
presence of PET particles [103]. Almost 2.4 µg/L of DBP was released
when the concentration of PET particles was 60 items/g [103]. The
presence of MPs can also affect hydrogen production in alkaline
anaerobic fermentation. Wei et al. reported that a high level of PET in
anaerobic digestion limited the availability of protein, polysaccharides,
glutamate, glucose, and butyrate, which restrained hydrolysis, acido­
genesis, and acetogenesis, and therefore reduced hydrogen production
[102]. In the presence of PET, microbial populations in hydrogen pro­
ducers and hydrolytic microbes were limited, and the hydrogen yield
was limited to 70.7% [103].
3.6. Removal of MPs in DWPFs
Although DWPFs can achieve an overall MP removal rate of 69.9%–
100%, a substantial amount of MPs has been found in treated water
[80,82,83]. A DWPF employing coagulation-flocculation and sand
filtration achieved a removal efficiency of MPs at 69.9% [82]. Mean­
while, there was no significant difference in rates of MP removal when
DWPFs applied either clarification or flotation after coagulation-
flocculation. DWPF with clarification removed 81.3% of MPs while a
similar facility with flotation removed 82.6% [82]. To the best of our
knowledge, only Wang et al. investigated MP removal in each treatment
method used in DWPFs, and only Ma et al. investigated MP removal in
water through coagulation-flocculation and ultrafiltration in the labo­
ratory [79–81]. Wang et al. found the overall MP removal in advanced
DWPFs reached 82.1%–88.6% [80]. Despite multiple reports of signifi­
cant MP abundance in raw water, the removal efficiency of advanced
DWPFs is slightly higher than that of conventional WWTPs [82].
Generally, chemical treatment contributes between 40.5% and 54.5% of
MP removal, and physical treatment contributed another 29.0% to
60.9%, but disinfection resulted in MP fragmentation at a rate between
–9.3% and 6.8% (Fig. 3). Fig. 3 provides overall performances and
removal efficiencies of each treatment, based on data from Wang et al.
[80].
3.6.1. Physical treatment
Physical treatment is the major method adopted in DWPFs, which
achieves 29.0%–60.9% of removal (Fig. 3). To settle flocs from
coagulation-flocculation, conventional DWPFs employ clarification. MP
removal reached 40.5%–54.5% when coagulation-flocculation was
combined with clarification (Fig. 3). Complete settlement of MPs > 10
µm and a relatively high settlement of MPs between 5 and 10 µm
(44.9%–75.0%) were observed, especially fibrous MPs [80]. This
implied that coagulation-flocculation enhances the aggregation of larger
MPs with flocs, which increases the density and facilitates clarification
[80]. However, lab-scale research showed that clarification after
coagulation-flocculation had poor removal performance of PE particles
with the efficiency of 15%–40% [79,81]. The removal of MPs by clari­
fication is downward movement, and it highly depends on the aggre­
gation of MPs and flocs. If MPs are not adsorbed or trapped by flocs
during coagulation-flocculation, MPs are more prone to escape from
clarification. To note that, pristine MPs were used in laboratory exper­
iment, while MPs found in DWPFs were mostly weathered. This differ­
ence might affect the interactions among MPs, coagulant, and
flocculant, and thereby affecting the removal performance by
clarification.
Apart from clarification, advanced DWPFs use dissolved air flotation
to replace traditional settlement of flocs from coagulation-flocculation.
Although Pivokonsky et al. found no significant difference in overall
removal efficiency between clarification and flotation, the overall MP
removal was slightly higher (82.6%) in advanced DWPFs adopted
flotation [82]. Unlike clarification, dissolved air flotation is an upward
movement, when fine air bubbles facilitate the flotation of MPs. Even
Y.L. Cheng et al.
Fig. 3. Removal efficiency of MPs in different unit operations and processes in the selected DWPFs.
MPs are not adsorbed or trapped by flocs during coagulation-
flocculation, MPs might be removed by dissolved air flotation. MPs
are more prone to float on the surface and skimmed during dissolved air
flotation, because of the density of common polymer types (0.83–1.58 g/
cm3). Dissolved air flotation is believed to result in higher MP removal
efficiency when compared with clarification.
Membrane filtration has been proposed to employ after coagulation-
flocculation, and lab-scale research has shown complete MP removal by
ultrafiltration [79,81]. Similar to the membrane filtration in WWTPs,
the removal of MPs by ultrafiltration is the direct entrapment of MPs
without the limitation on shapes or polymer types. The only concern of
the removal performance is the sizes of MPs. If the sizes of MPs are larger
than the pore size of membrane, this technique can achieve complete
removal of MPs. Membranes with a pore size of 30 nm retained almost
all PE particles, regardless the types of coagulants being dosed and the
availability of coagulation-flocculation [79,81]. Yet, the dynamics
among cake layer formation, membrane fouling, the presence of MPs,
and the flocs were relatively complex, which affected the effectiveness
of membrane filtration on MP removal [79,81]. The presence of small
MPs and high dosage of coagulants induced frequent membrane fouling
and disrupted the uniformity of cake layer formed, so the specific
membrane flux reduced to 0.17 after operating for 300 s [79,81].
Meanwhile, the presence of large MPs enhanced the porosity of the cake
layer and even caused breakage of cake layer, which mitigated mem­
brane fouling [79,81]. Apart from the replacement of clarification after
coagulation-flocculation, membrane techniques can also be employed
for filtration to replace traditional techniques. It is believed to have a
higher MP removal efficiency compared with typical sand filtration. The
pore size of membrane is typically 0.1 nm to 1.0 µm, and a small pore
size corresponds to a high removal efficiency of MPs. However, mem­
brane filtration is not a cost-effective method due to frequent membrane
fouling and the high operating cost associated with high pressures.
In filtration, conventional DWPFs employ sand filtration to remove
additional particles before disinfection. DWPFs reportedly can achieve
complete removal on MP through the application of triple filtration
[83]. Low levels of MPs in raw water lead to low concentrations in
treated water, which do not reflect the removal efficiency of DWPFs on
MPs [83]. The presence of MPs in treated water is likely due to the
abrasion of DWPF pipes and tanks [83]. Wang et al. found that sand
filtration can remove 29.0%–44.4% of MPs, which was effective to
remove MPs > 10 µm [80]. Remarkably, it can remove 30.9%–49.3%
and 23.5%–50.9% of fibers and pellets, respectively [80]. Yet, this
technique is not a promising method for removing MPs from water [80].
The effectiveness of sand filtration depends on particle size, which the
typical effectiveness size is 0.45 to 0.70 mm in rapid sand filtration. The
potential removals of MPs by sand filtration are either entrapment be­
tween the filter media or adherence to the surface of filter media [80].
Apart from sand filtration, advanced DWPFs use GAC filtration to
replace traditional filtration of impurities in the water. Wang et al. re­
ported that it can remove 56.8%–60.9% of MPs, especially removing
73.7%–98.5% of MPs < 5 µm [80]. Besides, it had a relatively good
performance on removing pellets (76.8%–86.3%), followed by frag­
ments (60.3–69.1%) [80]. This might be corresponded to the high
removal of PE and PP particles at the rate of 72.9–86.2% and
59.4–66.8%, respectively [80]. GAC filtration depends on the polarity of
the solids through adsorption, which polymer type becomes the crucial
14
Chemical Engineering Journal 410 (2021) 128381
factor affecting the removal performance by GAC filtration. Non-polar
MPs are more prone to be adsorbed by granular activated carbon. The
adsorption of PE and PP particles favors the removal of pellets and
fragments by GAC filtration.
3.6.2. Chemical treatment
Coagulation-flocculation is the primary method of chemical treat­
ment in DWPFs. Coagulation is the process of destabilizing colloidal
particles with coagulants, while flocculation is the process of colliding
and aggregating destabilized particles into large flocs. Wang et al. found
that 40.5%–54.5% of MPs were removed by coagulation-flocculation
combined with clarification in DWPF, whereas lab-scale research
showed MP removal by coagulation-flocculation reached < 40%
[79–81]. Either alum-based coagulants or iron-based coagulants are
typically added during coagulation. A high dose of coagulant generally
corresponds to a high removal efficiency in solids. The MP removal ef­
ficiency of alum-based salts (<10%) was higher than that of iron-based
salts (<5%) for each diameter of PE particles (500 µm to 5 mm) when a
typical dose of coagulants in DWPFs (0.74 mM alum and 0.36 mM iron)
was added [81]. The effectiveness of coagulation-flocculation is also
based on the pH of water. Superior removal performance for PE particles
was found at a pH lower than 6.0, with alum-based salts forming smaller
flocs with larger specific surface areas. The iron-based coagulant
removed PE particles more effectively (>15%) at a pH below 8.0 [79].
The removal rate improved with the use of anionic PAM and high doses
of alum-based coagulants [79,81]. Increased settlement of PE particles
was observed when an interaction occurred between anion PAM and
alum-based floc, resulting in the capture of small PE particles. A similar
situation occurred when anion PAM was added to an iron-based coag­
ulant, with the removal efficiency approaching 91% [79]. This implies
that the addition of PAM in coagulation-flocculation facilitates removal
of MPs, particularly small MPs. Since the removal performance of
coagulation-flocculation is affected by the types of coagulant, pH of
water, and the availability of PAM while the operating conditions of
DWPFs are fixed, the removal mechanisms might depend on the inter­
action with MPs.
Regarding the impact of MP size on coagulation-flocculation, lab-
scale research has produced differing results. The highest removal effi­
ciency of small PE particles (500 µm) was only 8.3% and it gradually fell
to 2.7%, 1.7%, and 1.0% for MPs 0.5–1 mm, 1–2 mm, and 2–5 mm in
size, respectively [81]. The surface charge of MPs is reportedly a sig­
nificant factor affecting removal efficiency [79,81]. Lab-scale research
revealed that MPs purchased from a manufacturer tend to be clear. MPs
may be stable particles that rarely collide with coagulants, leading to a
low removal efficiency. In addition, pure MP-flocs cannot settle because
of their low density. However, MPs in DWPFs may adsorb a certain
amount of chemicals or heavy metals from the environment, producing a
slightly different surface charge than is associated with MPs in lab-scale
research, and a greater potential to form flocs with coagulants.
3.6.3. Disinfection
Disinfection has no contribution to MP removal, instead it might
induce MP fragmentation. Wang et al. showed that ozonation had a
negative removal of MP ranged from –9.3% to –0.3%, while the removal
efficiency of chlorination ranged from –0.7% to 6.8% [80]. Based on the
changes in polymer type, PET and PE particles were increased by 10.2%
Y.L. Cheng et al.
and 5.4% after ozonation, respectively, while only PP particles were
increased by 4.1% after chlorination [80]. Meanwhile, ozonation
induced the fragmentation on fibers and fragments, while chlorination
broke down pellet [80]. Wang et al. explained that MPs might encounter
great shearing force in ozonation, but it was more likely the destruction
of residual organic matter by ozonation to remove biofilm-coated MPs
[80]. The impacts of disinfection on the fates of MPs might require
further investigation.
4. Recommendations for future research
Physical treatment in WWTPs plays a major role in MP removal [58].
Despite a relatively high removal rate of MPs in WWTPs, a considerable
amount of MPs is released to the environment through the discharge of
treated effluent or sludge application. Our current understanding of the
correlation between WWTPs and MP removal is limited to field in­
vestigations, and the removal mechanisms are not yet clear. While the
presence of small MPs in treated effluent provides evidence of MP
fragmentation during treatment, the actual fate of MPs within unit op­
erations and processes has not been examined in the field. The removal
mechanisms of each unit operation and process (ASP, sedimentation,
grit removal, and MBR) are not supported by laboratory studies. Several
important factors, including the characteristics of populations (e.g., in­
come level, domestic activities, and living standards), characteristics of
influent (e.g., types of wastewater and combined stormwater), and the
operating conditions of unit operations and processes, have not been
consider. These factors may limit the effectiveness of management
strategies to eliminate discharges of MPs from WWTPs.
The diverse methodologies involved in designing sample collection
procedures, MP extraction, and MP analysis further undermine the
usefulness of comparisons among studies (Tables S1-S3). Future
research should consider several strategies. First, standardized protocols
for sampling and MP extraction should be established. Sampling
methods, consideration of the diurnal and temporal nature of waste­
water, and the representativeness of volume are major parameters that
determine MP occurrence rates in WWTPs [90]. Sampling details,
including location, weather, unit operations and processes, flow rate,
and types of influents, should be disclosed. Due to the high organic
content of wastewater and sludge, digestion is an unavoidable step in
MP extraction. Researchers have adopted various methods, including
oxidation and chemical degradation, to model digestion, but no com­
parisons have been made among the methods. A vast amount of infor­
mation is required to incorporate all parameters and statistical data
relevant to WWTPs and MPs. Reliable and rapid analytical techniques
should be developed to eliminate the subjective judgment inherent in
visual observation of samples [105]. FTIR and Raman spectroscopy are
commonly used for the chemical characterization of MPs [54]. Mass
concentration through FTIR and thermoanalytical techniques are a more
robust measures that are less affected by size [106,107]. These methods
are effective for chemical analysis, but novel validation methods should
be developed for rapid, reliable, and cost-effective analysis.
Both our understanding of removal mechanisms within WWTPs and
effective methods for MP removal are limited in the field [70]. Instead of
being removed, some MPs are separated or fragmented into smaller
pieces in WWTPs. Future research should consider a paradigm shift from
MP removal to separation, due to the inherent nature of biological and
chemical resistance of MPs. Ideally, MPs could be decomposed into the
carbon cycle and completely mineralized by biodegradation, photo­
degradation, thermo-oxidation, and hydrolysis. The possible fates of
MPs within WWTPs should include complete mineralization of MPs into
water and carbon dioxide and the transition of MPs to wastewater and
sludge. To conclude, future research is needed with respect to the sep­
aration of MPs in WWTP.
15
Chemical Engineering Journal 410 (2021) 128381
5. Conclusion
WWTPs and DWPFs have two opposing roles: major removal
equipment and important sources of MPs. This paper comprehensively
reviewed the occurrences and removal of MPs in WWTPs and DWPFs.
Standards and protocols for MPs in WWTPs are lacking. Size, polymer
type, sampling method, treatment process, and analysis differ by study,
making comparisons difficult. MP abundance in terms of mass should be
considered to replace the number unit. Mass units destroy other in­
fluences by thermo-analytical methods, thereby offering more accurate
MP quantification than number units.
For WWTPs, the mass concentrations of MPs in influent ranged from
61 to 5,600 µg/L, and 0.5–170 µg/L of MPs were found in treated
effluent, representing an overall removal efficiency of 93.8%–99.8%.
Since only two published papers reported the mass concentrations of
MPs, the comparison of MP abundance in this review was based on the
number concentration. The number concentration of MPs in influent and
treated effluents ranges from 1.01 to 31,400 items/L and 0.004 to 447
items/L, respectively. Fragments/fibers are the dominant shapes, and
PE/PA/PS is the major polymer type of MPs. The relatively low con­
centration of MPs in effluent remains a concern due to large daily dis­
charges. MPs were removed during preliminary, primary, secondary,
and tertiary treatments at efficiencies of 6.0%–58.6%, 19.1%–99.0%,
–66.7%–92.6%, and –72.7%–99.9%, respectively. Preliminary and pri­
mary treatments make a higher removal contribution than do secondary
and tertiary treatments. Girt/grease removal exhibits the highest
removal efficiency through mechanical and physical potential, but it
might facilitate the initial MP fragmentation. The effectiveness of ter­
tiary treatment is highly dependent on the applied unit process. Disin­
fection has the greatest potential to induce MP fragmentation or
chemical degradation of MPs. The concentration of MPs in dewatered
sludge was much higher than in raw sludge, at 9.7–186.7 items/g (dw).
Mechanical dewatering may contribute to MP fragmentation, resulting
in a significant increase in MP concentration in dewatered sludge.
During sludge treatment, no unit processes are available to remove MPs
from raw sludge. The presence of MPs in sludge can affect anaerobic
digestion in terms of methane production, induction of ROS, and
hydrogen production. Although the latest studies consider the perfor­
mance of MP removal in each unit operation and process, in-depth
discussions of the responsible removal mechanisms are rare. Instead of
MP removal, the fate of MPs is primarily the function of the separation
from liquid to solid in the treatment plant. Future research should
consider the possibly of mineralization and transition of MPs within
WWTPs.
For DWPFs, the concentration of MPs in raw water and treated water
of DWPFs ranges from 1 to 6,614 items/L and 1 to 930 items/L,
respectively. Fragment shapes are dominant, and PET is a major polymer
type. The removal efficiency of MPs varies from 69.9% to 100%
regardless of the types of treatment. A relatively high overall removal
rate of MPs is available in the literature, but the reported variance in MP
concentration in treated water indicates a human health risk.
Coagulation-flocculation may cut MP abundance in water by half, but
the removal performance depends on the operating conditions (e.g., pH,
coagulant, and the addition of PAM) and surface charge of MPs. Mem­
brane filtration is the preferred process to remove MPs from water,
followed by GAC filtration and dissolved air flotation. Disinfection
might contribute MP fragmentation by chemical degradation.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Y.L. Cheng et al. Chemical Engineering Journal 410 (2021) 128381

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