ORIGINAL RESEARCH

published: 05 April 2022

doi: 10.3389/frwa.2022.835451

Contamination and Removal

Efficiency of Microplastics and
Synthetic Fibres in a Conventional
Drinking Water Treatment Plant
Angel Negrete Velasco 1*, Stéphan Ramseier Gentile 2 , Stéphane Zimmermann 2 and
Serge Stoll 1*
1
Group of Environmental Physical Chemistry, Department F.-A. Forel for Environmental and Aquatic Science, University of
Geneva, Geneva, Switzerland, 2 SIG, Industrial Boards of Geneva, Geneva, Switzerland

Microplastics have been detected all around the globe in freshwaters which are
frequently used to produce drinking water. Therefore, the contamination of raw water with
microplastics that supplies drinking water treatment plants, and their removal efficiency
is raising more concern and interest. In the present study, we evaluated the microplastic
Edited by: contamination in a conventional drinking water treatment plant (Geneva, Switzerland)
Rafael Trevisan,
Federal University of Santa
and the contribution of coagulation on the efficiency of the filtration systems (sand
Catarina, Brazil and activated carbon filtrations) in the removal efficiency of microplastics (MPs) and
Reviewed by: synthetic fibres. This work was performed in a pilot station that replicates the main
Qiqing Chen, drinking water treatment process. Raw water and effluents of each filtering processes
East China Normal University, China
Scott Coffin, were analysed for the presence of MPs and synthetic fibres with sizes ≥ 63 µm using
California Water Resources Control infrared spectroscopy. The contamination of MPs in raw water and in drinking water
Board, United States
ranged from 19.5 to 143.5 MPs/m3 and from 0 to 8 MPs/m3 (in presence and absence
*Correspondence:
Angel Negrete Velasco
of coagulant), respectively. On the other hand, concentration of synthetic fibres ranged
[Link]@[Link] from 7.7 to 23.8 synthetic fibres/m3 in raw water and from 0 to 3 synthetic fibres/m3 in
Serge Stoll drinking water. Results show that on average 89% of microplastics and 81% of synthetic
[Link]@[Link]
fibres (≥63 µm) are retained in water treatment in absence of coagulant. Better final
Specialty section: removal efficiency of microplastics (97%) and synthetic fibres (96%) was observed in
This article was submitted to drinking water with coagulation treatment. The chemical composition of microplastics
Water and Human Health,
a section of the journal and synthetic fibres is found more heterogeneous in raw water than after sand filtration
Frontiers in Water and activated carbon filtration.
Received: 14 December 2021 Keywords: microplastics, synthetic fibres, conventional drinking water, coagulation, infrared spectroscopy
Accepted: 11 February 2022
Published: 05 April 2022

Citation: INTRODUCTION
Negrete Velasco A, Ramseier
Gentile S, Zimmermann S and Stoll S Owing to the relatively low production costs and more attractive physicochemical properties than
(2022) Contamination and Removal
other materials, the use of plastics has rapidly grown since the 1950’s. Plastics are used in many
Efficiency of Microplastics and
Synthetic Fibres in a Conventional
consumer products, like plastic bags, food packaging and dispensable utensils, among other single
Drinking Water Treatment Plant. use objects. Consequently, plastic production has increased over years, arriving to over 350 million
Front. Water 4:835451. tonnes in 2019 (Plastics Europa, 2019). Furthermore, plastics are resistant to degradation that will
doi: 10.3389/frwa.2022.835451 persist in the environment. These factors, and others, ultimately lead to the accumulation of plastics

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Negrete Velasco et al. Microplastics in Drinking Water

in the environments (da Costa et al., 2016). In 2015, it was Slovakia and Switzerland) presented lower mean concentrations
estimated that around 60% of plastics ever produced end up being (3.6 particles/L) than other regions in the world, such as in
in natural environments (Geyer et al., 2017). USA (6.24 particles/L) or India (9.24 particles/L). In contrast,
Plastics have been categorised depending on their sizes Mintenig et al. (2019) reported between 0 and 7 microplastics/m3
as macroplastics (>20 mm), mesoplastics (5–20 mm), and (with sizes > 20 µm) in raw water (from groundwater sources)
microplastics (1 µm−5 mm) (Barnes et al., 2009). Microplastics and in the resulting drinking water. Furthermore, the removal
can be further classified, depending on their origin, as primary efficiency of microplastics in drinking water treatment plants
(made of small sizes like pellets, sequins or microbeads which are has been reported in some studies. In 2017, Pivokonsky
mainly used in cosmetics or decorative products) or secondary et al. observed the lowest removal efficiency (around 70%) of
(as a result of the breakdown of bigger plastic materials). microplastics in a conventional drinking water treatment plant
Microplastics reach freshwater systems (Eerkes-Medrano et al., involving coagulation/ flocculation and sand filtration. It was
2015; Horton et al., 2017) regardless their sizes, shapes and found that 83% of microplastics were removed on average
chemical compositions and are found both at significant from raw water in two drinking water treatment plants in
concentrations in water columns and sediments (Colton et al., Czech Republic performing coagulation/flocculation, in presence
1974; Kühn et al., 2018). Some important rivers in Europe have of sedimentation or flotation, sand filtration and granular
been studied to assess the contamination of microplastics, for activated carbon filtration (Pivokonsky et al., 2018). Surprisingly,
instance, the Rhine (Klein et al., 2015; Mani et al., 2015), the they found microplastic concentration up to 650 microplastics
Seine (Dris et al., 2018), the Danube (Lechner et al., 2014), (>1 µm) per litre. The removal efficiency at every treatment
and the Rhône (Constant et al., 2020). The contamination in step (coagulation/flocculation, sedimentation, sand filtration,
lakes (Eriksen et al., 2013; Hu et al., 2020; Bertoldi et al., and activated carbon filtration) was also assessed in drinking
2021) have also been assessed in some parts of the world water treatment plants with raw water providing from the
and it has been shown that even remote environments do not Yangtze River (China; Wang et al., 2020) and Úhlava River
escape from this contamination (Allen et al., 2019; González- (Czech Republic; Pivokonský et al., 2020). Cumulative removal
Pleiter et al., 2020). In Switzerland, microplastic and fibre efficiencies >72% were achieved in both studies, however,
contamination of water and sediment of a remote alpine lake the concentrations of microplastics in drinking water ranged
(Lake Sassolo) was recently reported. Average concentration of between 930 and 151 microplastics/L. On the other hand, the
microplastics (≥125 µm) in the water column was found equal effects of coagulation-flocculation and filtration systems were
to 2.6 microplastics/L, whereas 33 microplastics/kg were detected studied in laboratory experiments (Ma et al., 2019; Lapointe et al.,
in the sediment (Negrete Velasco et al., 2020). Furthermore, 2020; Shahi et al., 2020; Skaf et al., 2020), utilising concentrations
Faure et al. carried out a study to evaluate the contamination (10–50 mg/L) of alum coagulant largely exceeding those typically
of the six biggest lakes in Switzerland (Faure et al., 2015; Faure used in conventional water treatment plant (0.3–0.5 mg Al3+ /L).
and De Alencastro, 2016). They found microplastics and textile Currently, to the best of our knowledge, no study has
fibres in the surface waters and beach sediments of Lake Geneva, been published about the impact of coagulation on sand
Lake Constance, Lake Maggiore, Lake Neuchatel, Lake Zurich, filtration and activated carbon filtration processes in realistic
and Lake Brienz. On average, 220,000 ± 160,000 and 33,000 conditions. Indeed, it is not possible to suppress or interfere
± 46,000 microplastics/km2 were found on the surface of Lake with the coagulation in a regular and operational drinking water
Geneva (Grand Lac and Petit Lac, respectively), we estimated to treatment plant. In the present study, we used a pilot scale
be around 0.2 microplastics/m3 based on the information given drinking water treatment plant (DWTP) which is the replica of
by the authors. Recently, another study carried out by Oceaneye the main DWTP of Geneva. This pilot scale reproduces all the
(2020) showed that the average contamination of microplastics processes and conditions which are used in the main station
(>300 µm) in Lake Geneva was of the same order of magnitude which supplies drinking water for 500,000 consumers. The goal
as in North Atlantic sea (53,817 particles/km2 ) and ocean average of this study is to evaluate microplastic and fibre contamination
value (32,000 particles/km2 ). In addition to the contamination and the contribution of coagulation to the overall efficiency of the
of microplastics in water resources, the occurrence of hazardous filtration systems (sand and activated carbon) in the removal of
elements (like Cd, Hg, and Pb) at elevated concentrations microplastics and synthetic fibres. Sample volumes were at least
adsorbed or incorporated on microplastics has been studied in equal to 1,000 L over a sample period of 23–30 h, hence obtaining
beaches of Lake Geneva (Filella and Turner, 2018). a representative sample in terms of volume [as recommended by
Since microplastics have been detected in freshwaters Koelmans et al. (2019) and Mintenig et al. (2019)] and time.
(Pivokonsky et al., 2018; Ferraz et al., 2020; Wang et al., Synthetic fibres were considered in the present study
2020) at significant concentrations, assessing the concentration as a specific type of microplastic. Indeed, in addition to
of microplastics in tap water has raised interest so as to their morphologies, potential difficulties in separation and
evaluate related hazard and risk (Kosuth et al., 2018; Shruti characterisation, they have also emerged as a relatively new area
et al., 2020; Kirstein et al., 2021). An investigation conducted of study such as the shedding of microfibers from synthetic
by Kosuth et al. (2018) recently shows the contamination of fabrics during conventional clothes washing (Hartline et al.,
81% of tap water with microplastic and synthetic fibres from 2016; De Falco et al., 2019) and fall out in indoor environments
14 countries sampled around the globe (Kosuth et al., 2018). (Zhang et al., 2020). Like many other types of microparticles,
Samples in the EU (England, France, Germany, Ireland, Italy, fibres have been found in natural compartments, fauna and

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urban areas (Remy et al., 2015; Dris et al., 2017; Gasperi et al., conducted in special laboratory rooms devoted to microplastics
2018; Collard et al., 2019). Moreover, textile fibres, regardless analyses. In particular, the working room was closed during
of their nature, could contain additives and dyes (including manipulations to avoid air currents. Floor was mopped with soap
nanoparticles), which are in some cases hazardous to wildlife and and filtered ultrapure water, and all work surfaces were wiped
humans (Darbra et al., 2012; Remy et al., 2015; Gita et al., 2019). down with ethanol prior to starting work. The use of plastic
materials was reduced as much as possible in the laboratory,
MATERIALS AND METHODS although they could not be avoided entirely. The only plastic
materials used were nitrile gloves and the washing bottle made
Sampling Site and Collection of Teflon FEP (Thermo Fischer Scientific, New York, USA).
The drinking water pilot station that was subjected to Despite the degree of quality of the ultrapure water (Milli Q water,
investigation uses raw water from Lake Geneva. This pilot Millipore, Schaffhausen, Switzerland, with R > 18 MΩ·cm),
station (Figure 1A) replicates the main drinking water treatment it was systematically filtered with a nitrate cellulose philtre
plant (DWTP) in Geneva, which is designed to produce (0.45 µm, Sartorius stedim biotech, Göttlingen, Germany) in
drinking water for 500,000 users. The treatment processes involve a glass filtration unit (VWR, Leuven, Belgium) to remove all
essentially raw water pre-treatment, sand filtration, activated microplastics and fibres that the plastic parts of the Milli Q water
carbon filtration and pH correction to achieve calco-carbonic instrument could release. This filtered ultrapure water was stored
equilibrium, as shown in (Figure 1B). Water from Lake Geneva in a glass drum for upcoming uses. All glassware and sieves were
is first chlorinated, 1 mm screen (strainer) filtered and pumped washed with soap, natural bristles brushes and rinsed with filtered
to supply the drinking water treatment plant and pilot station. ultrapure water. Only cotton clothing was always worn, even
The average flow of raw water entering the pilot station is 1 m3 /h. under the cotton lab coat. A lint roller was used to remove all
Polyaluminum chloride PAlCl, (Al(OH)m Cl(3−m) )n Gilufloc 83 fibres attached to the clothes and lab coat, in order to reduce
(BK Giulini GmbH, Germany) with 83% basicity and containing a possible intake of fibres into the samples. All materials were
23% Al2 O3 is used to promote coagulation at a concentration covered with aluminium foils when they were stored, transported
of 0.36 mg Al3+ /L. Then pre-treated water flows through a and during sampling.
conduct of 40 m to allow the coagulant to react (5 min reaction) Since laboratory working conditions are important to improve
before passing through a bilayer sand philtre of quartz sand the quality and comparability of results (Koelmans et al.,
(h = 80 cm depth) and pumice stone (h = 50 cm depth) at a 2019; Cowger et al., 2020; Schymanski et al., 2021), the
filtration speed of 5 m/h (rapid sand filtration). The water passes working environment was evaluated with one positive control
afterwards through an activated carbon philtre that has the same and one blank per sampling campaign. The positive control
dimension as the sand philtre and is made up of a mixture of was assessed with microplastic glitter particles (n = 50) of
Chemviron F300 (75%) and AquaCarb (25%). Both philtres have 430 µm (smallest dimension), bought in a recreative store,
a quartz gravel support layer of 35 cm. Sampling is performed mixed with 20 L filtered ultrapure water. Positive control and
via fountains (Supplementary Figure 1) providing water from blank samples were subjected to the same procedure as a
raw water, before (coagulation), after sand filtration and after regular sample.
activated carbon filtration.
The sampling campaigns were carried out in a first time
to evaluate the filtration systems (sand and activated carbon) Extraction of Microplastic Particles and
without coagulant, and in a second time in the presence of Fibres
coagulant. The physicochemical parameters (pH, turbidity, and The retained material in the steel sieves were transferred with
conductivity) were checked before sampling in order to ensure 100 mL filtered ultrapure water to 250 mL glass beakers to
that the sampling was conducted with stable conditions. Values proceed with a digestion of the organic matter. A volume of
are given in Supplementary Tables 1, 2. The flow rate of the 100 mL of an hydrogen peroxide (H2 O2 30% wt, REACTOLAB
sampling fountains was carefully measured in triplicate before SA, Servion, Switzerland) solution was added to the beakers and
and after the samplings. We aimed for representative samples left at 60◦ C. Hydrogen peroxide was chosen to digest natural
and considered volumes between 1,000 and 1,950 L of raw organic matter over other digestion techniques (with strong
water, before and after sand filtration and after activated carbon acids or bases) that could be more aggressive or less convenient
filtration (ACF) The samples were passed under gravity at the (Hanvey et al., 2017; Renner et al., 2018). This oxidant was
pilot station fountains through a set of four stainless steel sieves also used in the digestion of compost, sediments, wastewater
(ISO 3310-1) of 200 mm diameter with 500, 250, 125, and 63 µm and freshwater samples in other experiments conducted in our
mesh sizes. group, showing good results in degradation of organic matter
and not affecting visual identification. Therefore, this extraction
Contamination Mitigation protocol was based on Negrete Velasco et al. (2020), but adjusted
Special attention needs to be paid when working with drinking according to the type of sample and the objectives of this work.
water samples regarding contamination issues. In this work, After 5 days of digestion, the samples were filtered with a
several precautions were taken to reduce the contamination of 63 µm stainless steel mesh of 100 mm diameter. The recovered
the sample with microplastics and fibres in accordance with material from the 250 and 500 µm sieves was transferred to
the literature (Schymanski et al., 2021). All experiments were 0.45 µm nitrate cellulose philtres (0.45 µm, Sartorius stedim

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FIGURE 1 | Picture of the corresponding pilot station (1 m3 /h) that replicates the main DWTP in Geneva (A) and scheme of the drinking water treatment with marked
sampling sites (1/2/3) (B).

biotech, Göttlingen, Germany). The material retained on the Optic and Infrared Spectroscopy Analysis
63 and 125 µm sieves was transferred to aluminium oxide The whole surface of the cellulose nitrate philtres was first
(Al2 O3 ) philtres (AnodiscTM 47, 0.2 µm, GE Healthcare Life observed using an optical microscope (Olympus BX-40, Tokyo,
Sciences WhatmanTM , Buckinghamshire, United Kingdom) for Japan) to achieve a qualitative analysis. The microscope is
chemical identification of the microparticles with FT-IR. All equipped with a 2x, 4x, 10x optical lens for the collection of
philtres were stored immediately after filtration in clean glass images of the philtres surface. The microparticles and fibres were
Petri dishes. then transferred to the support of the spectrometer (Spectrum

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TABLE 1 | Examples of MPs (A–F) and synthetic fibres (G–L) pictures obtained with IR microscope (A–I) and optic microscope (H–L) found in raw water (left column),
after sand filtration (middle column), and after activated carbon filtration (right column).

Raw water Water after sand filtration Water after activated carbon filtration

Two FT-IR, Perkin Elmer, Beaconsfield, United Kingdom) to be microparticles were observed and in most cases tested by FT-
analysed by attenuated total reflectance (ATR). IR, excepted when mineral microparticles were suspected (no
Regarding the aluminium oxide philtres, they were placed transmittance signal). All data were collected with a resolution
in the moving stage of the FT-IR spectrometer coupled to an ≤8 cm−1 and ≥ 8 co-added scans in accordance with Schymanski
optical microscope (Spotlight 200i FT-IR microscopy system, et al. (2021). The obtained spectra with the Spectrum© software
PerkinElmer, Beaconsfield, United Kingdom), which is equipped (version 10.5.3, Perkin Elmer) were subjected to a library search
with a mercury cadmium telluride (MCT) detector with aperture using the ATR Perkin Elmer polymer library (with over 100
range between 10 and 100µm. Due to the time-consuming spectra). The entire overlap region (600 to 4,000 cm−1 ) was
analysis, no systematic observation of the entire surface of used for the ATR spectra, while a spectral range was defined
the Al2 O3 philtres was performed and only a quarter of between 1,250 and 4,000 cm−1 for FT-IR analysis because of
the surface was analysed following the model presented in the absorption properties of the Al2 O3 philtre. Indeed, the
Supplementary Figure 2. This model is a combination of use of the entire overlap region (600 to 4,000 cm−1 ) using
cake slice and random models (Schymanski et al., 2021). All Al2 O3 philtres decreases the degree of correlation in FT-IR

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analysis. Microparticles and fibres having spectra with a search synthetic fibres images obtained by microscopy are shown in
score higher than 75% of coincidence with a polymer in the Table 1. Average concentration of MPs in raw water was found
library were considered as microplastic or synthetic fibres. equal to 95 ± 49 MPs/m3 whereas the average concentration
Therefore, chemical identification with infrared spectroscopy of synthetic fibres was 15 ± 7.7 synthetic fibres/m3 . These
was mainly based on a threshold of 75% correlation rate. values were higher than those reported by Faure et al. (2015)
Special attention was paid with nylon (polyamide PA) during in the surface of Lake Geneva (around 0.2 MPs/m3 , with sizes
the interpretation of spectra, since the spectrum of nylon is >300 µm) but lower than those reported in raw waters of DWTP
quite similar to some proteins, and false positive is likely to in Yangtze River (China): around 600 MPs/L (Wang et al., 2020)
occur (Schymanski et al., 2021). and Úhlava River (Czech Republic): between 4 and 80 MPs/L
(Pivokonský et al., 2020) by considering only microplastics with a
Characterisation of Microparticles diameter >50 µm. This difference could be explained by the fact
In the present study, considered microparticles were comprised that different sizes were analysed, and that raw water is extracted
in sizes between 63 and 1,000 µm and divided in four classes from Lake Geneva at a depth of 30 m. Indeed, microplastic
of sizes (≥63 to <125 µm, ≥125 to <250 µm, ≥250 to concentrations has been found to be heterogeneous in the water
<500 µm, and ≥500 µm). The size of particles was defined column, with lower microplastic concentrations in intermediate
with the mesh and verified with the software measuring layers than near-surface or near-bottom layers (Zobkov et al.,
instruments (OLYMPUS cellSens Entry© and Spectrum IR© ) 2019).
of the respective microscopes. Regarding the size verification In the presence of coagulant, water after sand filtration
with FT-IR coupled to an optical microscope, the marker of contained less MPs and synthetic fibres than in raw water, with
the IR light was fixed with the lower and upper boundary (for values comprised between 0 and 11.4 MPs/m3 and from 0 to 1
example 63 × 125 µm) to ensure the correct class of size of the SF/m3 . Treated water after activated carbon filtration contained a
particle. Moreover, microparticle classification was based both lower number of MPs (Figures 2A, 3A), between 0 and 4 MPs/m3
on the nature of the microparticles and shape. On one hand, and synthetic fibres (Figures 2B, 3B) remained in values from 0
we considered MPs (fragments, films, pellets, beads, and foams), to 1 synthetic fibres/m3 . On the other hand, the concentration of
and on the other hand, mineral and organic microparticles that MPs in water treatment without coagulant ranged from 0 to 5.6
were also extracted from sample analysis. A distinction was MPs/m3 after sand filtration and the number of synthetic fibres
made for fibres, since they can be natural, semi synthetic or reached values up to 6.3 synthetic fibres/m3 . The content of MPs
synthetic and which constitute a specific type of microparticles. was slightly higher in water after activated carbon (0–8 MPs/m3 )
Therefore, microparticles were divided into four groups: non than after sand filtration, but the range of concentrations of
plastic microparticles, microplastics (MPs) (including fragments, synthetic fibres decreased (0–3 synthetic fibres/m3 ).
films, pellets, foam, and beads), non-synthetic fibres (natural and According to these results, we observed that there was a
semi-synthetic), and synthetic fibres. variability from one sampling campaign to another. Moreover,
MPs and synthetic fibres were observed in all treatment stages.
RESULTS AND DISCUSSION However, MP and SF concentrations in raw water were low, as
previously mentioned. On the other hand, our findings indicate
Monitoring Contamination that this pilot station, which replicates the main DWTP in
Positive control resulted in recovery rate of 96% of the Geneva, did not notably contribute to water contamination with
microplastic glitter particles (Supplementary Figure 3). This MPs and synthetic fibres. Much higher concentrations of MPs
value is similar to that reported by Enders et al. (2020) with and synthetic fibres were found in the drinking water treatment
PA microplastics of 450 µm. One blank of ultrapure water was plants related to Yangtze River (Wang et al., 2020) and Úhlava
analysed in parallel with each sampling campaign to assess the River (Pivokonský et al., 2020). Indeed, between 0 and 1,000
potential contamination during sample treatment. No MPs nor MPs and synthetic fibres/L of drinking water were determined,
synthetic fibres were detected in the blanks. However, between however, the sample volumes were significantly smaller (1–2 L).
32 and 80 non-synthetic fibres/L (mainly white) were found in In contrast, Mintenig et al. (2019) determined lower amounts
the blanks. Chemical nature of most of these fibres were not of MPs (0–7 MPs/m3 ) and synthetic fibres (3–43 fibres/m3 ) in
possible to identify due to the lack of reference materials in raw water and drinking water from the Oldenburg-East-Frisian
the libraries (home-made and ATR Perkin Elmer library). The water board in Germany (Mintenig et al., 2019). However, in this
values obtained in the blanks were, nevertheless, lower than case, the source of raw water was ground water (naturaly filtered
those obtained during the validation stage of the method (data through the soil), explaining why a significant lower number of
not presented). MPs and synthetic fibres was found, compared to the studies of
Pivokonski et al. and Wang et al. considering the Yangtze and
Abundance of Microplastic and Synthetic Uhlava rivers, respectively.
Fibres
Non plastic microparticles (organic and mineral) were not Microplastic and Synthetic Fibres Size
counted in this study and only the results of fibres identified as Distribution
synthetic were presented as a significant number of non-synthetic Microparticles were divided into four size classes: ≥63
fibres was found in the blank samples. MPs and synthetic fibres to <125 µm, ≥125 to <250 µm, ≥250 to 500 µm, and
were found in all samples of raw water, examples of MPs and ≥500 µm. MPs were found more abundant than synthetic

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FIGURE 2 | Concentration of MPs (A) and synthetic fibres (B) in raw water, after sand filtration and after activated carbon filtration in presence of coagulant of each
sampling and average with standard deviation.

fibres in all size classes. As show in Figures 4A, 5A, no changed to 74.5 and 92% with and without coagulation,
MPs were detected in sizes ≥250 µm in any sample. In respectively. In drinking water, the difference was more
raw water 77% of the MPs were found in the smallest pronounced in presence of coagulant (50%) and without
size class (63–125 µm). After sand filtration, this ratio coagulant (84%).

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FIGURE 3 | Concentration of MPs (A) and synthetic fibres (B) in raw water, after sand filtration and after activated carbon filtration in absence of coagulant of each
sampling and average with standard deviation.

Contrary to MPs, synthetic fibres were mostly identified in size In presence of coagulant (Figure 4B), synthetic fibres were
class ≥250 µm both in the presence and absence of coagulant found significantly removed after sand filtration. No synthetic
(Figures 4B, 5B). In the case of raw water, the percentage fibres were identified in drinking water in sizes <250 µm, but
of synthetic fibres in the smallest size class was around 55%. synthetic fibres ≥250 µm were still persistent although in low

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FIGURE 4 | Size distribution concentrations of MPs (A) and synthetic fibres (B) in presence of coagulant.

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FIGURE 5 | Size distribution concentrations of MPs (A) and synthetic fibres (B) in absence of coagulant.

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numbers. Without coagulant (Figure 5B), synthetic fibres were coagulant (Figures 6A, 7A). MPs like PES, PP, and PVA
mainly found (92%) in size classes <250 µm after sand filtration, were not detected after sand filtration in presence or not
however, size distribution was more heterogeneous after ACF, of coagulant. MPs made of PEVA prevailed over the entire
where only 42% of synthetic fibres were found in sizes <250 µm. water treatment with coagulant. In drinking water, MPs of
Microplastic concentrations reported here in raw water were PE and PEVA were identified whereas other types of plastic
higher than those reported in the surface of Lake Geneva by Faure were not detected. In contrast, MPs of PA, PE, PEVA,
et al. (2015) (around 0.2 MPs/m3 ) (Faure et al., 2015). However, and others were identified after ACF in water treatment
we did not observe microplastic higher than 250 µm, whereas without coagulant.
they only studied microparticles higher than 300 µm on surface Fibres (natural, semi-synthetic or synthetic) were easily
water of Lake Geneva. The absence of microplastics higher than recognised (visually) in the samples, but their chemical
250 µm could be explained by the distribution of microplastics composition was not successfully identified in most of cases
in the water column. Water quality (temperature and density because of their elongated shape and reduced thickness.
gradients) play in fact an important role in the transport and Important concentrations of fibres were found all along
retention of microplastics in water column (Zobkov et al., 2019). the drinking water treatment, even if several actions
In addition, microplastic characteristics (size, form density, were taken to prevent contamination. Some fibres such as
roughness, etc.) and biofouling have an impact in the fate of cotton, viscose and cellulose were observed and subsequently
microplastics in the water column. Dai et al. (2018) observed identified in the analysis by infrared spectroscopy. As shown
elevated proportions of microplastics smaller than 300 µm with Supplementary Figure 6, <10% of fibres were identified as
increasing water depth, indicating that a smaller microplastic was synthetics after infrared spectroscopy analysis, indicating
more likely to sink than a larger one (Dai et al., 2018). that natural and semi-synthetic fibres could represent a more
Our findings indicate that MPs and synthetic fibres significant contribution in numbers than synthetic fibres. The
concentrations globally increase with smaller sizes, which results of fibres concentration with and without coagulant are
is in agreement with comparable research dealing with MPs presented in Supplementary Figure 6.
in DWTPs. Indeed, similar research about MPs in DWTPs The heterogeneity of SF chemical composition was more
(Pivokonsky et al., 2018; Pivokonský et al., 2020; Novotna et al., important in raw water, as depicted in Figures 6B, 7B. Synthetic
2019; Johnson et al., 2020; Wang et al., 2020) observed that fibres made of PES were identified in all samples, such as
size distribution were displaced towards smaller sizes. However, polyethylene terephthalate (PET) and polybutylene terephthalate
higher numbers were determined in those studies which (PBT). In contrast, some synthetic fibres such as PA, PMMA,
also indicated that MPs <50 µm persisted in drinking water and PEVA were not detected after sand filtration. In presence
treatment. Therefore, we can also expect here higher number of coagulant, only PES fibres were identified after sand filtration
of MPs and synthetic fibres with sizes <63 µm. Nevertheless, and ACF (Figure 6B). In comparison, water treatment without
the analysis of smaller sizes (<63 µm) was out of scope in the coagulant was found to reduce the heterogeneity of SF chemical
present study. composition, but PES, PP, and others the type of synthetic fibres
prevailed over the entire water treatment (Figure 7B).
Qualitative Analysis At this point, we can conclude that water treatment did not
As mentioned in Section Abundance of Microplastic contribute to water contamination with MPs and synthetic fibres
and Synthetic Fibres, many microparticles, identified (≥63 µm). Some studies indicate that microplastics less than
as non-plastic by infrared spectroscopy, were observed 63 µm and nano-sized plastics are created from the abrasion of
in all samples. Among the most frequent non-plastic retained microplastics with the filtration masses during water
microparticles, we identified cellulose and proteins as treatment (Cai et al., 2018; Enfrin et al., 2019; Li et al., 2022).
products of digested organic matter. Cellulose microparticles This could be indeed a problem in drinking water treatment.
and fibres were excluded because this material was used However, other studies such as the one of Ramirez Arenas et al.
to philtre the ultrapure water (Milli-Q) as mentioned in (2022), which investigated the removal efficiency of polystyrene
the methodology section. Due to the contamination of nanoplastics (124 ± 38 nm) negatively charged in conventional
samples with nitrate cellulose, we chose not to consider the water treatment, indicated global removal efficiency equal to
corresponding microparticles. 99.4%. Thus, more near nanoscale microplastic and nanoplastic
Materials like Polyamide (PA), Polyethylene (PE), Polyester research is necessary, as well as more advanced methodologies
(PES), Polymethyl methacrylate (PMMA), polypropylene (PP), and instruments to expand the knowledge regarding these
polystyrene (PS), polyvinyl alcohol (PVA) and ethylene (vinyl important issues in drinking water.
acetate) copolymer (PEVA), and some other materials were Chemical heterogeneity from raw water to final drinking water
identified by infrared spectroscopy. Examples of infrared spectra was neither amplified nor stable in the purification process.
and corresponding pictures of MPs and synthetic fibres are given Indeed, chemical composition of MPs and synthetic fibres were
in the Supplementary Figures 4, 5. reduced to just a few materials in drinking water. The occurrence
Our findings indicate that the chemical composition of of the different chemical types of plastics (MPs and synthetic
MPs was found more heterogeneous in raw water than fibres) that we identified coincide with those reported by
in samples after sand filtration, as shown in Figures 6, 7. Pivokonsky et al. (2018), Pivokonský et al. (2020) and Wang et al.
Sand filtration removed most plastic types with or without (2020) such as PET, PE, PP, and PEVA. However, compared to our

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Negrete Velasco et al. Microplastics in Drinking Water

FIGURE 6 | Chemical composition of MPs (A) and synthetic fibres (B) in raw water, after sand filtration and after activated carbon filtration in presence of coagulant.

results, no significant difference in the chemical heterogeneity Determination of Microplastic and

of plastics occurred from raw water to drinking water in that Synthetic Fibres Removal Efficiencies
research. In other words, these studies dealing with microplastics In presence of coagulant, the total removal of MPs attained
in drinking water did not observe an important reduction of 97 ± 3%, which corresponds to a final concentration
plastic heterogeneity. equal to 2.6 MPs/m3 . However, as shown in Figure 8, a

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Negrete Velasco et al. Microplastics in Drinking Water

FIGURE 7 | Chemical composition of MPs (A) and synthetic fibres (B) in raw water, after sand filtration and after activated carbon filtration in absence of coagulant.

non-negligible number of MPs was already removed after ± 7% of synthetic fibres were removed after sand filtration,
sand filtration indicating its efficiency. The removal rate of corresponding to 0.3 synthetic fibres/m3 . Total removal
MPs after sand filtration with coagulant reached 92 ± 11%. efficiency of synthetic fibres was equal to 97 ± 7%, which
In comparison, synthetic fibres were removed with slightly indicated that no significant further removal was obtained
better efficiency than MPs after sand filtration. On average, 96 after ACF.

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Negrete Velasco et al. Microplastics in Drinking Water

FIGURE 8 | Average MPs and synthetic fibres cumulative removal efficiency with their respective standard deviations.

Removal efficiency of MPs in drinking water treatment They found a removal efficiency of microplastics (fibres and
without coagulant resulted in 95 ± 5% after sand filtration. fragments >50 µm) greater than 96% after sand filtration in
Cumulative removal efficiency of MPs decreased to 89 ± 13% Plzen drinking water treatment plant (Pivokonský et al., 2020).
after ACF, corresponding to an average of 4.3 MPs/m3 . In However, a lower removal efficiency was observed for MPs
contrast, the removal efficiency of synthetic fibres was 68 ± 36% >1 µm (around 80%).
after sand filtration. Total removal of synthetic fibres further Regarding the cumulative removal efficiency after ACF,
improved after ACF, reaching 81 ± 17%, which corresponds to Wang et al. (2020) obtained 100 % removal efficiency with
1.7 synthetic fibres/m3 , as depicted in Figure 8. MPs >50 µm. However, overall removal efficiency in drinking
Our results indicate that sand filtration itself retains a water was found equal to 86% considering MPs >1 µm which
significant number of MPs and synthetic fibres. Moreover, represented a concentration of 930 ± 71 MPs/L. In contrast,
coagulation (at least at the low dosage operated in the plant) Pivokonský et al. observed an enhancement in removal efficiency,
is not found here to play a key role in the removal of MPs, considering all range sizes studied (MPs >1 µm). Nonetheless,
as shown in Figure 2A. Indeed, removal efficiencies were found they did not found an improvement in removal efficiency of
very close compared to the absence of coagulation (Figure 3A). MPs (synthetic fibres included) with sizes >50 µm in Plzen
However, the concentration of MPs further decreased after ACF DWTP, arriving to around 94% cumulative removal efficiency
in the treatment with coagulant (Figures 2A, 3A). This could (Pivokonský et al., 2020). The overall removal efficiencies in four
indicate that the coagulation process improves the performance drinking water treatment plants studied by Pivokonsky et al.
of the filtration systems, even if the MPs were not completely (2018), Pivokonský et al. (2020) were >81% (Pivokonsky et al.,
removed from water or that a significant reduction was observed. 2018; Pivokonský et al., 2020). MPs and synthetic fibres >50 µm
Furthermore, our results indicate that the use of coagulant in were almost or completely removed in drinking water, with
drinking water treatment benefits removal of synthetic fibres, by values ranging from 0 to 2 fragment MPs/L and from 0 to 5
almost eliminating them from the water. synthetic fibres/L. The highest average removal efficiency (99.9%)
If comparison is now made with the literature, Wang et al. was reported in drinking water treatment in England and Wales
(2020) found no MPs (fibres, fragments nor spheres) >50 µm by Johnson et al. (2020) by considering MPs ≥25 µm (Johnson
after sand filtration in a drinking water treatment plant which et al., 2020). In addition, lower numbers of MPs (0–3 quantifiable
includes a flocculation/sedimentation process. They reported MPs/m3 ) were reported compared to other studies.
100% removal efficiency of MPs after sand filtration. However, Such a variability of the removal efficiency of MPs in this
they obtain a removal efficiency ranging between 58.9 and 70.5% study and in others must be related to raw water quality
of fibrous and non-fibrous MPs (1–50 µm). Compared to our and operational process conditions which can influence the
findings, similar values were reported by Pivokonský et al. (2020). DWTPs ability to eliminate or reduce microplastic from

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Negrete Velasco et al. Microplastics in Drinking Water

drinking water. We sampled under optimal conditions (i.e., Plastic contamination was limited; however, the concentration
1–2 days after and before backwashing of filtration masses). of MPs and synthetic fibres is expected to increase significantly
However, the filtration masses are not always steady and with smaller sizes. This is an important issue indicating
evolves over time, following processes of clogging, washing, that microplastics of small sizes (i.e., <63 µm) as well as
starting, and functioning. Further research is needed to assess nanoplastic contamination could be more significant and
the evolution of the filtration masses over time and their more investigation will be necessary to expand the knowledge
efficiency over different conditions, i.e., each operational cycle. regarding MPs and synthetic fibres in drinking water treatment
Furthermore, raw water quality also plays an important role under conventional conditions.
in the capability of DWTP in removing contaminants from
water. Water quality parameters, like turbidity, pH, temperature DATA AVAILABILITY STATEMENT
and conductivity also play an important role in comprehending
the removal efficiency of microplastics in DWTP, as shown The raw data supporting the conclusions of this article will be
by Sarkar et al. (2021). made available by the authors, without undue reservation.

CONCLUSION AUTHOR CONTRIBUTIONS

The contribution of coagulation to the efficiency of filtration All authors listed have made a substantial, direct, and intellectual
systems (sand and activated carbon) in the removal of MPs contribution to the work and approved it for publication.
and synthetic fibres was investigated in a conventional drinking
water plant. The content of MPs and synthetic fibres was limited FUNDING
in raw water (95 MPs/m3 and 15 synthetic fibres/m3 ), most
likely because the water is extracted from Lake Geneva at a This project was funded by Water Research Fund (FOWA) from
depth of 30 m. The results obtained in this study indicates that Société Suisse de l’Industrie du Gaz et des Eaux (SSIGE/SVGW
sand filtration removes a considerable amount of MPs (>79%), 026-19) and the Services Industriels de Genève (SIG 026-19).
regardless of the presence of coagulant. Therefore, coagulation
is not found to play an important role here in the elimination ACKNOWLEDGMENTS
of MPs. However, a significant effect was observed for synthetic
fibres after sand filtration since their removal efficiency was The authors acknowledge financial support received from
improved, from 69% in absence of coagulant to 96% in presence SSIGE/SVGW, SIG, and University of Geneva. We also
of coagulant. The concentration of MPs and synthetic fibres in acknowledge the technical support of all the people involved
treated water without coagulant was limited (4.3 MPs/m3 and in the use and maintenance of the pilot station and Delphine
1.7 synthetic fibres/m3 ) with removal efficiencies of MPs and Borboën for the positive controls data.
synthetic fibres equal to 89 and 81% respectively. Treated water
with coagulation, sand filtration and ACF was found to contain a SUPPLEMENTARY MATERIAL
negligible content of MPs (2.6 MPs/m3 ) and synthetic fibres (0.3
SF/m3 ) and removal efficiencies higher than 96%. Moreover, MPs The Supplementary Material for this article can be found
with sizes <250 µm were found prevalent in the drinking water online at: [Link]
treatment plant. 2022.835451/full#supplementary-material

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other clean water samples with micro-Raman and micro-infrared spectroscopy: Publisher’s Note: All claims expressed in this article are solely those of the authors
minimum requirements and best practice guidelines. Analyt. Bioanalyt. Chem. and do not necessarily represent those of their affiliated organizations, or those of
413, 5969–5994. doi: 10.1007/s00216-021-03498-y the publisher, the editors and the reviewers. Any product that may be evaluated in
Shahi, N. K., Maeng, M., Kim, D., and Dockko, S. (2020). Removal
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Metro station free drinking water fountain- a potential “microplastics is an open-access article distributed under the terms of the Creative Commons
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doi: 10.1016/[Link].2020.114227 is permitted, provided the original author(s) and the copyright owner(s) are credited
Skaf, D. W., Punzi, V. L., Rolle, J. T., and Kleinberg, K. A. (2020). Removal of and that the original publication in this journal is cited, in accordance with accepted
micron-sized microplastic particles from simulated drinking water via alum academic practice. No use, distribution or reproduction is permitted which does not
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