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Journal of Environmental Chemical Engineering 10 (2022) 107142

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Journal of Environmental Chemical Engineering


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

Microplastic abundance and removal via an ultrafiltration system coupled


to a conventional municipal wastewater treatment plant in Thailand
Katekanya Tadsuwan , Sandhya Babel *
School of Bio-chemical Engineering and Technology, Sirindhorn International Institute of Technology, Thammasat University, Pathum Thani 12121, Thailand

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

Editor: Despo Kassinos A wastewater treatment plant is one of the land-based sources of microplastics in freshwater environments. A
conventional wastewater treatment plant alone is not designed for microplastic removal. This study evaluates the
Keywords: abundance and microplastic removal efficiency of a conventional wastewater treatment plant and the load daily
Microplastics released to water environment. It also investigates the effect of coupling a pilot-scale ultrafiltration system.
Wastewater treatment plant
Samples were collected at each unit operation by grab sampling. Sludge samples were collected from return
Sludge
activated sludge after the final clarifier to find microplastic pollution levels that might contaminate agricultural
Tertiary treatment
Ultrafiltration soil. The results showed that on average, 77 ± 7.21 particles/L were found in the influent, and 10.67 ± 3.51
particles/L were discharged with the final effluent, resulting in 86.14% overall removal efficiency in a traditional
treatment system. When an ultrafiltration unit was taken into consideration, the number of microplastics in the
effluent reduced to 2.33 ± 1.53 particles/L, which increased the removal efficiency up to 96.97%. The abun­
dance of microplastic particles in sludge samples generated from the final clarifier was 2.63 ± 1.26 × 104
particles/kg (dry weight). The most dominant group was 0.05–0.5 mm, and fibers accounted for more than 60%
of total microplastics at every sampling point. The results from spectroscopic analysis showed that polyethylene
terephthalate (PET) was the major type of microplastics, followed by polyethylene (PE) and polypropylene (PP).
This study shows that advanced technology in tertiary treatment plants could substantially remove microplastic
pollution in wastewater. Moreover, the absence of primary sedimentation tank can also influence removal of
microplastics.

1. Introduction laundry processes [7] and also enter through personal care products
such as toothpastes, cleansers, and shower gels [8]. A study by Browne
Plastic is used widely because of its durability, low price, and light et al. [9] showed that MPs detected at the shoreline were the same type
weight. However, the material persists in the environment. The accu­ as MPs from WWTP effluent. Most conventional wastewater treatment
mulation of plastic waste has become a global challenge. One of the plants are not designed to eradicate these small-size plastics [10]. Some
issues arising from plastic waste that has raised attention worldwide is advanced treatment technologies including membrane bioreactor, rapid
microplastic (MP), which is commonly defined as a plastic particle in the sand filter, dissolved air filtration, disc-filter [11], reverse osmosis (RO)
range of 5 mm to 1 nanometer [1]. MPs manufactured for use as in­ [12], and post-filtration [13] have been suggested as an addition to help
dustrial scrubbers or as microbeads in cosmetic products are called remove MPs [11–13]. Different treatment technologies in WWTPs can
primary MPs, while those which are formed as a result of degradation of affect removal efficiency of MPs [14]. Characteristics of MPs such as size
larger plastics are called secondary MPs [1]. These minute-sized plastic and shape impact their removal rate [15]. It is also important to study
particles are known to be toxic to marine species [2] and pose threats to the performance of an individual WWTP because of the different design
human health through the food chain [3,4]. and wastewater characteristics.
Wastewater treatment plants (WWTP) are considered one of the Thailand is a top-ten plastic polluter to marine environment [16]. In
land-based sources of MPs [5]. WWTPs act as a receptor for MPs from 2020, 6300 tonnes of plastic waste was produced daily in Thailand [17].
industry, household waste, and landfill [6]. Most of the MPs present in The study on the abundance and MP removal efficiency in WWTPs re­
the wastewater treatment system originate from fiber shedding during quires attention because WWTP is the final barrier and a point source of

* Corresponding author.
E-mail address: sandhya@siit.tu.ac.th (S. Babel).

https://doi.org/10.1016/j.jece.2022.107142
Received 12 November 2021; Received in revised form 24 December 2021; Accepted 3 January 2022
Available online 5 January 2022
2213-3437/© 2022 Elsevier Ltd. All rights reserved.
K. Tadsuwan and S. Babel Journal of Environmental Chemical Engineering 10 (2022) 107142

MPs before they enter freshwater ecosystem. Some recent studies in further sorted using tweezers. MP samples on the 500 and 53 µm sieves
Thailand have focused on MP removal in conventional WWTPs [18,19]. were carefully washed out from the sieves using Deionized (DI) water.
However, there is no study so far that investigates the performance of Thereafter, the samples were categorized into 3 size fractions: 1–5 mm,
tertiary treatment in a WWTP in Thailand for MPs removal. A conven­ 0.5–1 mm, and 0.05–0.5 mm. Each size fraction of the MP samples was
tional WWTP with a pilot-scale of advance filtration technology was kept in laboratory bottles at 4 ◦ C prior to the analysis.
selected for the study. The objective of the ultrafiltration (UF) is to clean Sewage sludge (SS) after the final clarifier (Fig. 1) was collected from
the water further for reuse. It is demonstrated in this study whether the randomized points and homogenized in a glass bottle with a total weight
addition of UF can improve the efficiency of MP removal in a WWTP. of approximately 0.5 kg per bottle. Sludge samples were preserved in a
This study investigates the abundance, morphology, and types of refrigerator at 4 ºC.
MPs in a conventional WWTP coupled with a pilot-scale UF system in
Thailand. The removal efficiency of each unit operation was examined 2.3. Sample processing
to find the most effective removal step, and the overall removal effi­
ciencies of a traditional treatment plant and an additional tertiary 2.3.1. Liquid fraction
treatment have been compared. Daily discharge of MPs into water MP samples were transferred to beakers and kept in the oven at 60 ◦ C
bodies was also estimated based on the abundance and treatment ca­ for 24 h. Wet peroxide oxidation, adopted from [22], was used as
pacity of the WWTP. pre-treatment for the isolation of MPs from organic-rich wastewater
without affecting particle size, and enables MPs for spectroscopic
2. Materials and methods method [23]. The dry samples were treated with Fenton’s reagent pre­
pared by mixing 0.05 M Fe (II) solution with 30% hydrogen peroxide
2.1. Study site (H2O2) (Chem-Supply™) to remove organic materials attached to the
MP particles. Subsequently, 20 mL of Fe (II) solution and 20 mL H2O2
A conventional WWTP with an installation of an advance treatment were added to the dry samples and these samples were heated up to
unit was selected for the study. The WWTP serves an area of 20.7 km2 in 60 ◦ C (following Munno et al.) to accelerate the reaction and to prevent
four districts of Bangkok with a population of 227,660. The total length MP losses during digestion [24]. Further addition of H2O2 was done in
of the collection system’s pipeline is 49.4 km. The wastewater collection case there were still traces of organic matter [25]. The samples were left
system is a combined sewer. The treatment capacity of this WWTP is to cool down for 24 h and then filtered through a set of sieves to wash
120,000 m3/d and 300,000 m3/d in dry and rainy seasons, respectively. away the residue from Fenton’s reagent with DI water. The samples were
The treatment plant is a close underground system to prevent air and then transferred to a beaker and dried at 60 ◦ C.
noise pollution. This wastewater treatment plant includes primary Density separation was employed to separate MP particles from
treatment, secondary treatment, and a pilot-scale tertiary treatment fa­ sediment and other inorganic materials. In this study, a sodium iodide
cility. The treatment technology in tertiary treatment is UF (polyether (NaI) (99.0% KemAus) solution with a density of approximately 1.5 g/
sulfone (PES)/polyvinylpyrrolidone (PVP) blend membrane) with a pore cm3 was used due to its high recovery rate, cost-effectiveness, and
size of 0.1 µm. There are 2 sets of UF in this WWTP. Each set can treat up recyclability [26,27]. The NaI solution was added to the samples and
to 1000 m3 of wastewater daily. Treated wastewater after the final stirred continuously for 15 min. The samples were transferred to a cyl­
clarifier is discharged directly into the canal, while the effluent from UF inder and left for 24 h to let them settle down. Particles that floated on
is used for decorative purposes and cleaning within the building. the surface of the solution were extracted and categorized into three size
fractions by wet sieving: 1–5 mm, 0.5–1 mm, and 0.05–0.5 mm. MP
2.2. Sampling method samples were vacuum-filtered onto a gridded cellulose nitrate mem­
brane filter with a pore size of 0.45 µm (Whatman), placed on a petri
MP samples were collected by 1 L grab sampling (n = 3) using a dish, and covered with aluminum foil.
stainless-steel bucket at each unit operation, as illustrated in Fig. 1, and Fluorescent tagging using Nile Red (Biotium) (adapted from Tam­
transferred into glass bottles. On-site filtration was impractical for this minga et al. [28]) was used to quantify MPs smaller than 0.5 mm. Nile
WWTP. Grab sampling could result in three orders of magnitude of MPs red staining method can be used to discriminate synthetic polymers from
than other net-based methods [20,21]. Grab sampling is able to capture other inorganic particles [29]. Filter papers containing samples with size
smaller size range of MPs and higher amount of non-fibrous plastic [20]. fraction of 0.05 – 0.5 mm were stained with Nile Red in chloroform
Samples from the WWTP were filtered through a set of sieves in the (99.8% RCI labscan) (1 mg/mL). Samples were covered with aluminum
laboratory. Plastic pieces on the 5.0 mm sieve were kept separately and foil and left under the fume hood for 24 h. Stained filter papers were
classified as macro-plastics. Samples retained on 1 mm sieve were photographed under a fluorescence microscope (Delta Vision™ Elite cell

Fig. 1. Flow chart of the selected WWTP with sampling locations. S1 = influent after the coarse screen, S2 = after the grit chamber, S3 = after the aeration tanks,
S4 = final effluent after final clarifier, S5 = effluent after ultrafiltration, and SS = sewage sludge.

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K. Tadsuwan and S. Babel Journal of Environmental Chemical Engineering 10 (2022) 107142

Imaging System). and the size fractions were determine by two-sample t-tests. The value of
p < 0.05 was considered as significantly different.
2.3.2. Sludge samples
Sludge samples were collected from return activated sludge. Samples 3. Results and discussion
were first dried at 105 ◦ C until a constant weight was obtained and then
the total solid content was determined. Saturated Nal solution was 3.1. MP abundance in the WWTP
added to a beaker of the sewage sludge sample and continuously stirred
for 15 min. The top water layer was separated and washed with DI water MPs were grouped into three size fractions: 1–5 mm, 0.5–1 mm, and
to remove salt residue. Samples were dried at 60 ◦ C before pre-treatment 0.05–0.5 mm. Visual sorting under an optical microscope was used to
with Fenton’s reagent, similar to the samples in liquid fraction. After find the number of MPs (size fractions of 1–5 mm and 0.5–1 mm), which
cooling down for 24 h, the samples were filtered through a sieve set and were then combined with the number of MPs (0.05–0.5 mm) from a
the residue of Fenton’s reagent was washed off with DI water. The florescence microscope. An example of a dyed filter photographed under
retained samples on each sieve size were grouped into three size frac­ a fluorescence microscope is shown in Fig. 2. There were no plastic
tions: 1–5 mm, 0.5–1 mm, and 0.05–0.5 mm. Afterwards, these samples pieces larger than 5 mm found in this study. The most abundant size of
were vacuum filtered with a cellulose nitrate membrane filter. Nile red MPs in the treatment system were in the size range of 0.05–0.5 mm
tagging was also employed with the size fraction of 0.05–0.5 mm to (Fig. 3). Size 0.05–0.5 mm MPs were significantly more abundant than
identify the abundance of MPs. 1–5 mm and 0.05–0.5 mm (p < 0.05) sized MPs. The average number of
MPs entering the system was 77 ± 7.21 particles/L (S1), and a total of
2.4. MP quantification and characterization 10.67 ± 3.51 particles/L were discharged with the final effluent (S4)
(Table 1). MPs within the size fraction of 1–5 mm were successfully
Filter papers with size fractions of 1–5 mm and 0.5–1 mm were removed after the secondary treatment (Fig. 4). MPs were significantly
inspected under a light microscope (Olympus CX41) with magnifications removed by the grit chamber and fine screen (S2) (p < 0.05). The
of × 4 and × 10. Particles were counted and categorized into shapes: number of MPs removed by the grit chamber and fine screen (S2) was
fragment, fiber, film, and bead. Stained filter papers with a size fraction 25.55% (Table 1). The number of MPs increased to 40.70% in the
of 0.05–0.5 mm were observed through a fluorescence microscope aeration tank (S3) (Table 1). MPs were not completely eliminated from
(Delta Vision™ Elite cell Imaging System) with a magnification of × 4. the treatment system but they were retained in the sludge. Once the
The visible blue florescence spots were counted, and the morphologies sludge was recycled and returned to the aeration tanks, MPs were
were identified. resuspended in this stage. Thus, no removal of MPs was observed during
To obtain removal efficiency of the WWTP, the number of MPs in the this process. Most importantly, 81.91% of MPs were removed after the
influent and effluent were calculated using Eq. (1). final clarifier (S4) (Table 1). The removal of MPs at the final clarifier was
significant (p < 0.05). Furthermore, there was an extra 78.16% MP
influent ​ (MPs/L)-effluent (MPs/L)
% removal efficiency = × 100% reduction after the UF (S5). Therefore, the addition of UF aided in a
influent ​ (MPs/L) significant removal of MPs (p < 0.05).
(1) The overall removal efficiency was based on the number of MPs at
The polymer types of MPs were identified using spectroscopic the influent and effluent. Overall removal efficiency was calculated at
method. MP samples, sizes 1–5 mm and 0.5–1 mm, were picked out with 86.14% after the final clarifier, and 96.97% after the tertiary treatment.
tweezers individually and analyzed by Fourier-transform infrared As per the results, the installation of an UF unit could improve the
(FTIR) spectroscopy (Nicolet iS50, Thermo Scientific) in the attenuated overall efficiency of the WWTP. Despite of the small pore size of UF
total reflectance (ATR) mode with a diamond microtip. The resolution membrane (0.1 µm), 0.05–0.5 mm MPs was the only group detected in
for analysis was 4 cm-1, with 32 scans. Particles smaller than 0.5 mm the UF effluent. MP particles tend to escape the WWTP by occasional
were identified using micro-FTIR (Nicolet iN10, Thermo Scientific) with breakthroughs of filters [30], and are released into the environment. In
the resolution of 8 cm-1 and 64 scans. Ten spots on each filter paper were addition, smaller size particles correspond to greater adsorption of
selected for identification. Spectral fingerprints were compared to persistent organic pollutants due to higher specific surface area [31,32].
reference spectra library available in the OMNIC software to obtain However, membrane fouling can occur due to the formation of the
polymer types with a match factor of ≥ 0.70. cake layer, which is the main obstacle for the membrane filtration’s

2.5. Quality control

Mitigation measures to control airborne- and waterborne-


contamination were strictly followed during sampling and analysis.
Plastic containers and equipment were avoided, and only metal and
glassware were used. DI water was used to rinse all the equipment and
glassware before use in the experiment. The work bench was wiped with
70% ethanol. Most of the procedures were performed under a fume
hood. Blank samples (DI water) were used as control samples during the
experiment. Filter papers of blank samples were observed under a mi­
croscope. A range of 7–12 particles per L of DI water, mostly fibers, was
found on the blank filter papers. The number of similar MPs on blank
samples were subtracted from the study membrane filters as they are
considered background contamination.

2.6. Statistical analysis

Statistical analysis was performed using Minitab 20 software. The Fig. 2. MP particles photographed under a fluorescence microscope with
significant differences between the abundance at each sampling point 4 × magnification.

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K. Tadsuwan and S. Babel Journal of Environmental Chemical Engineering 10 (2022) 107142

100% action to prevent the accumulation of MPs in the ocean.


90% Due to the lack of primary sedimentation, MPs were largely removed
80%
after the secondary treatment. Thus, a final clarifier is the most impor­
tant unit for MP removal in this WWTP. A study by Liu et al. [33] re­
70%
ported that a primary settling tank exhibited excellent MP removal
60%
0.05 - 0.5 mm
efficiency. The combination of grit and grease removal and primary
50%
0.5 - 1 mm
sedimentation is the most crucial step for MP removal [36]. Fiber can be
40% 1 - 5 mm easily trapped with grit or gets attached to larger particles and settles
30% down during the primary treatment [37], while fragments can be
reduced further in secondary processes by entrapment in solid flocs and
20%
settlement in a final clarifier [38]. However, the entrapment of MPs on
10%
an unstable floc might result in redistribution and escape during the
0% clarification process [38].
S1 S2 S3 S4 S5 SS
Tertiary and advanced treatments are used to remove specific pol­
Fig. 3. Percentage distribution of the different size classes of MPs during the lutants that cannot be removed by conventional treatments [10]. Table 2
wastewater treatment steps. S1 = after inlet pumping, S2 = after the grit trap, provides MPs removal efficiencies of various tertiary treatment tech­
S3 = the aeration tank, S4 = effluent from the final clarifier, S5 = effluent from nologies. Most of the advanced technologies displayed high removal
ultrafiltration, and SS = sewage sludge. efficiency to above 90%. The overall removal efficiency of MP is this
study is in accordance with the study by Mintenig et al. [13]. With an
installation of UF unit, approximate 97% of MP removal is attained. The
Table 1 membrane bioreactor (MBR) exhibited the highest removal rate. MBR is
Number of MPs released from each sampling site per day, and removal also considered as the most cost-effective option for MP removal [39].
efficiencies.
The number of MPs in the influent and effluent can vary depending on
Sampling MPs/L million MPs/ % Removal Cumulative % the size of the smallest mesh. Regardless of the level of removal effi­
site day after each removal
ciency, considerable amounts of MP particles can still escape into the
location
environment because of the large volumes of wastewater being treated
S1 77( ± 7.21) 9240 ± 865 0 0 daily.
S2 57.33 6880 ± 970 25.55% 25.55%
( ± 8.08)
The abundance of MP particles in sludge samples generated from the
S3 96.67 11,600 ± 3611 – 25.55% final clarifier was 2.63 ± 1.26 × 104 particles/kg (dry weight). The
( ± 30.09) number of MPs in the sludge is in the range of the study by Li et al. in
S4 10.67 1280 ± 421 81.91% 86.14% China and Lassen et al. in Germany [42,43]. The largest group of MPs in
( ± 3.51)
the sewage sludge was of size fraction 0.05–0.5 mm, similar to MPs in
S5 2.33 280 ± 183 78.16% 96.97%
( ± 1.53) liquid fraction (Fig. 4). MPs removed during the settling stage in the
final clarifier were retained in the sludge. Sewage sludge from the final
clarifier is typically dewatered by the sludge dewatering system within
the WWTP and later transported to other sludge digestion facilities. Dry
140
sewage sludge is later used for agriculture. A study by Chen et al. [44]
120 found that agricultural soil was contaminated with fibers and
Microplastic particles/L

100 microbeads due to the use of sewage sludge as fertilizer. Synthetic fibers
S1
detected in sludge-applied soil retained the same characteristics even
80 S2
after many years of the application as they were in the sludge [45].
S3
60 Kumar et al. [46] reported some adverse effects of MPs in the soil
S4
40 environment that negatively impact flora and fauna and pose risks to
S5
human health when chemicals in MPs are transferred through the food
20
chain. MPs contaminating the soil can also be transported to water
0 bodies by surface runoff.
1-5 mm 0.5-1 mm 0.05-0.5 mm total
Other sludge treatment was assessed to investigate the abundance of
Fig. 4. Number of MP particles per L of wastewater from treatment steps. MP and their spread with land application. MPs were also found in the
S1 = after inlet pumping, S2 = after the grit trap, S3 = after the aeration tank, sludge after thermal drying and lime stabilization [47]. Smaller size
S4 = effluent from the final clarifier, S5 = effluent from ultrafiltration, and SS range of MPs were detected in a larger proportion in sludge after lime
= sewage sludge. stabilization due to shearing stress during treatment process [47].
Incineration was predicted to be a promising method for MP removal
performance [33]. Therefore, it is important to implement mitigation from the sludge. However, the bottom ash from the incinerator was
measures for membrane fouling from MPs such as frequent backwash. contaminated with MPs and was pointed out as a potential source for
The application of coatings onto commercial membrane materials pro­ MPs [48]. There is still a challenge to remove MP from the sludge,
vides high polarity and controlled surface chemistry which can reduce otherwise, these pollutants might end up in the environment.
membrane fouling [34].
The capacity of this WWTP was 120,000 m3/day in the dry season 3.2. MP characterization
during the sample collection. A total of 1280 ± 421 million particles
could be released daily from secondary effluent (S4) into the connected Fibers were found in both liquid fraction and sewage sludge (≥ 60%)
freshwater ecosystem (Table 1). Even when a full-scale UF unit is (Fig. 5). Fibers are the dominant group, as per several studies [15,40,
operated, 280 ± 183 million MPs per day can still be discharged to 49–51]. Even though large proportions of fibers were found in the
nearby canals regardless to higher removal efficiency (Table 1). It is effluent from secondary treatment (S4) and UF (S5), some of the fibers
reported that more than one million MP particles are discharged daily were removed by the final clarifier, and they were found in the sewage
from wastewater treatment plant in many countries (Australia, Canada, sludge (SS) (Fig. 5). Larger proportion of fibers were detected in S3
Scotland, Finland, and Italy) [35]. This high MP load requires urgent collected from aeration tanks than at S2 as a result of recycled sewage

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K. Tadsuwan and S. Babel Journal of Environmental Chemical Engineering 10 (2022) 107142

Table 2
Comparison of MP removal by tertiary treatment technologies.
Location Type of tertiary treatment Influent (MPs/L) Effluent (MPs/L) Overall removal efficiency Reference

Germany UF ND 0 (>500 µm) 97% [13]


1 × 104 (<500 µm)
a
Australia UF and reverse osmosis (RO) 2.2 0.28 after UF 0.21 after RO 90% [12]
China Denitrification 12.03 ± 1.29 0.59 ± 0.22 95.16 ± 1.57% [40]
UF
O3
UV
Finland Pilot-scale MBR 57.6 ± 12.4 0.4 ± 0.1 99.4% [41]
Finland MBR 6.9 0.005 99.99% [30]
Rapid sand filter 0.7 0.02 97%
Dissolved air floatation 2 0.1 95%
Disc-filter 0.5 – 2.0 0.03 – 0.3 40 – 98.5%
Italy Sand filter 2.5 ± 0.3 0.4 ± 0.1 84% [8]
Thailand Pilot-scale UF 77 ± 7.21 2.33 ± 1.53 96.97% This study

ND = no data
a
the number of MPs in the primary effluent was used for calculation.

100%
3%2%
90% 3%
6%
Percentage distribution of shapes

80% PE
3% 29% PET
70%
60% EDPM rubber
bead
10% PP
50% fragment
film PS
40%
fiber
4% Acrylic polymer
30%
PU
20%
PA
10%
Alkyd
0%
S1 S2 S3 S4 S5 SS
40%
Fig. 5. Percentage distribution of different shapes of MP samples, found at each
sampling point in the WWTP. S1 = after inlet pumping, S2 = after the grit trap, Fig. 6. Polymer type distribution of microplastics identified by FTIR and
S3 = aeration tank, S4 = effluent from the final clarifier, S5 = effluent from micro-FTIR.
ultrafiltration, and SS = sewage sludge.
suspected microfibers. An example of PET fibers is shown in Fig. 7. PET
sludge. Microplastic fibers, which were already trapped to flocs, were is a predominant group of polyesters (PES) used for fiber production
carried along with the sludge and redistributed in the aeration tanks. [53]. The study by Lares et al. reported that the majority of microplastic
The percentage of fibers is even higher in S4 because fibers could easily fibers found in the WWTP were identified as PES [41]. Murphy et al. also
escape with the overflow from weir during final clarification. Talvitie detected the largest proportion of PES in the final effluent from the
et al. [5] found insignificant removal of fibers during secondary treat­ WWTP [36]. Some of the fibers were identified as natural polymers such
ment, and fibers were mostly removed during primary sedimentation. as silk and cotton, some particles were organic debris such as chipboard,
Since the studied WWTP had no primary sedimentation tank, thus and film was identified as cellophane. The number of other natural
higher number of fibers were found in the effluent. In S5, although the materials was excluded from the total count. Talvitie et al. reported that
mesh size of the UF is very fine, fibers can still escape due to their small cotton was the dominant group among fibers detected in the WWTP.
size and morphology [30]. A small proportion of film and fragments Though natural polymers are considered as non-plastic materials, they
were also detected in the sludge (SS). Only 5.13% (2 items) of spherical can become anthropogenic pollutant when they are released to the
MPs (beads) were found in effluent from grit removal (S2). The reduced environment due to the manufacturing processes of natural polymers
number of microbeads from personal care products detected in this including dying or bleaching and the blending of chemical additives to
WWTP might be a result of a ban on plastic microbead usage in Thailand improve mechanical properties [54,55]. Natural fibers may absorb
from January 1, 2020 [52]. surrounding pollutants and act as a carrier to harmful substances which
MPs with a size fraction of 1–5 mm and 0.5–1 mm were analyzed can be released to the environment [56]. Michielssen et al. introduced a
with FTIR. The selected MP samples were large enough to be handled term called “small anthropogenic litter” which include plastic material
with tweezers. MPs in the size range of 0.05–0.5 mm were tested by FTIR and cellulosic products manufactured from natural material [57]. Both
connected with a microscope (micro-FTIR) and photographed. The synthetic and natural fibers can pose negative impact to the environ­
limitation of spectroscopic analysis was that all of 0.05–0.5 mm parti­ ment. WWTPs act as a final barrier to prevent these pollutants to the
cles, which is the largest proportion, could not be tested by micro-FTIR. water bodies.
Ten spots were selected as a representative of each filter paper. Only The proportion of synthetic textiles is about 60% of the global fiber
50% of all suspected particles were tested by both FTIR and micro-FTIR, production [58]. The three main polymer types used in textile industry
and 68 items were found to be synthetic polymers from every sampling are PET, acrylic (polyacrylonitrile; PAN), and nylon (polyamide; PA)
point. The results from both FTIR and micro-FTIR showed that there [59]. The types of microfibers found can be related to the synthetic
were 9 types of polymers found in the samples (Fig. 6). The most pre­ textile released during washing. Polyester shed the highest amount of
dominant polymer type was polyethylene terephthalate (PET) from fibers in one wash among all the types of fabric [60]. Up to 700,000

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K. Tadsuwan and S. Babel Journal of Environmental Chemical Engineering 10 (2022) 107142

A
100

80

% Transmittance
60

40

20

0
3400 2400 1400 400
Wavenumber (cm-1)

B
100

80
% Transmittance

60

40

20

0
3400 2400 1400 400
Wavenumber (cm-1)

Fig. 7. Example spectrum of MP samples (A) red fiber identified as polyethylene terephthalate (PET) (B) black fragment identified as isotactic polypropylene (PP).

fibers can be released per average wash load [7]. Microfibers are the contaminated in wastewater depends on the population the WWTPs
most dominant shapes detected along the shoreline and in open oceans serve. Regardless to high removal efficiency of the WWTP with UF unit,
[58]. WWTPs can be a potential land-based source of microfibers found the WWTP is considered as an important source of MPs to aquatic
along the coastline and in the ocean. Therefore, Carney Almroth et al. environment.
[60] have suggested solutions to reduce the number of fibers generated
through laundering including smarter textile production, additional 4. Conclusions
filters in household washing machines, and prewashing and vacuum
exhaustion during textile manufacture. Besides PET fibers, polyethylene The results of MP sampling from the selected WWTP show that MPs
(PE) is the second largest polymer in the WWTP. PE has been used in a were discharged with the final effluent from this conventional treatment
wide range of applications, especially in packaging. PE production ac­ system. Since this WWTP lacks a primary settling tank, the final clarifier
counts for 36% of the total plastic production and is the largest group assumes a major role for MP removal. The addition of a tertiary treat­
among non-fiber plastic products [61]. PE was found in the form of film ment using UF enhanced the overall removal efficiency of the plant.
and fragments in the studied samples. Carr et al. found some However, the operation of the UF unit is still on a pilot-scale.
irregular-shape PE derived from toothpaste [38]. High PE loads detected The actual number of MPs discharged with the final effluent was
in wastewater could be from both cosmetics and abrasion of household considerable from the conventional WWTP. The most dominant group in
products [13]. both liquid fraction and sewage sludge was of size fraction
The result of this study is in accordance with the study of Ziajahromi 0.05–0.5 mm, and more than 60% fibers were found at every sampling
et al. and Lares et al. where the most abundant group of MPs was point. The results from FTIR and micro-FTIR show that the most abun­
polyester fiber followed by PE [12,41]. Mintenig et al. found that PE dant group was PET in the form of fibers derived from the laundering
dominated all samples in WWTPs and most of the synthetic fibers were process. The retained MPs were found in the sewage sludge. Most of the
identified as PES [13]. PE and PES were also the most abundant MPs in sludge after digestion and air-drying is released into soil. Thus, MP
treated wastewater [62]. Sun et al. reviewed that there were 4 common pollutants can be transported to aquatic environments by surface runoff.
polymers found in the influent and effluent of WWTPs: PES, PE, PET, and It is still challenging to eliminate MPs retained in the sludge to prevent
polyamide PA, and other types were acrylate, alkyd, polypropylene further spread to the environment. Further study should focus on the
(PP), polystyrene (PS), Polyurethane (PU), PS acrylic, polyvinyl alcohol, treatment technology to remove MPs from the sludge.
and polylactide (PA) [63]. The differences of polymer types of MPs Ultrafiltration as a tertiary treatment can enhance MP removal in a

6
K. Tadsuwan and S. Babel Journal of Environmental Chemical Engineering 10 (2022) 107142

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