Journal of Water Process Engineering xxx (xxxx) xxx

Contents lists available at ScienceDirect

Journal of Water Process Engineering

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

Presence and fate of microplastics in the water sources: focus on the role of
wastewater and drinking water treatment plants
Margherita Barchiesi *, Agostina Chiavola, Camilla Di Marcantonio, Maria Rosaria Boni
DICEA, Department of Civil, Constructional and Environmental Engineering, Faculty of Civil and Industrial Engineering, University of Rome Sapienza, Via Eudossiana 18,
00184 Rome, Italy

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

Keywords: Microplastics are nowadays considered as ubiquitous pollutants since have been found widespread in all envi­
Drinking Water treatment plants ronmental compartments, particularly in the water sources. In the urban water cycle, the drinking water
Microplastics treatment plants and the wastewater treatment plants are the first and last barriers to microplastics pollution,
Wastewater treatment plants
respectively. The present work aims at presenting the information available on microplastic presence in the
Water
urban water cycle, reporting and linking what is known at the different stages. Focus is on the water sources and
on the role of the water treatment plants as source and control of microplastics pollution. Aspects evaluated are
microplastics abundance, characterization in terms of morphology, size and polymer composition, spatial and
temporal variations, factors influencing their distribution and abundance, effects of treatments on their removal.
Up to now there is no common framework for microplastics collection, sample pre-treatment, identification,
quantification and classification. Data comparison is hindered due to the various analytical protocols imple­
mented; hence the conclusions driven are mostly indicative or of very local significance. The available infor­
mation is not evenly distributed among the urban water cycle components. For the establishment of proper
microplastics pollution control strategies, the relative role of wastewater and drinking water treatment plants
needs to be better deepened in terms of both quantity and quality effects.
All these aspects are afforded in the present review which is based on the more recent data published by the
specialized literature.

1. Introduction canyons and arctic ice [4]. It can be assessed that all the environmental
compartments are contaminated: water [5,6], soil and sediments [4,7],
Plastic is a general term introduced to gather materials made of air [8,9], biota [10,11]. Usually MPs are considered every plastic frag­
synthetic polymers. Such various polymers are origin to materials that ment with main dimension lower than 5 mm; typically a lower boundary
vary widely in terms of physical and chemical characteristics. Hence the of 1 μm is used to mark out Nanoplastics (NPs) [2,3,12–14]. Indeed,
versatility of plastic and its subsequent widespread use: from clothes to there is no common definition among the EU countries or elsewhere. The
everyday life tools, from personal care products to transport means and European Chemical Agency (ECHA) hence proposed a “working defini­
many others. Plastic production rocketed over the years since the tion” based on the substance, state, morphology and dimensions [15,
beginning of its mass distribution. Drawback of this large diffusion is 16]. MPs are also grouped according to their origin into primary and
that 60 % of all the plastic produced has been discharged into landfills or secondary MPs: the former are those designed purposefully as such,
ended up in natural environments [1,2]. The high persistence results in a while the latter are the results of shattering and fragmentation of larger
worldwide spreading of plastic litter due to various transport processes. plastic debris, due to a combination of mechanical stress, UV radiation
Their spread is also favored by the fragmentation of plastic debris into and (micro)biological degradation [2,17].
smaller pieces, reaching the size of micro and nanometers [3]. There­ MPs cannot be defined positively harmless, since alterations to biota
fore, Microplastics (MPs) are nowadays considered as ubiquitous pol­ due to their exposure have been reported; however, the hazards related
lutants: indeed, they have been found not only in the surroundings of to MPs for humans have not been fully understood yet [18,19]. MPs will
urban environments, but also in secluded places such as submarine indeed be tackled in the new release of the EU drinking water directive

* Corresponding author.
E-mail address: [email protected] (M. Barchiesi).

https://doi.org/10.1016/j.jwpe.2020.101787
Received 8 July 2020; Received in revised form 26 September 2020; Accepted 3 November 2020
2214-7144/© 2020 Elsevier Ltd. All rights reserved.

Please cite this article as: Margherita Barchiesi, Journal of Water Process Engineering, https://doi.org/10.1016/j.jwpe.2020.101787
M. Barchiesi et al. Journal of Water Process Engineering xxx (xxxx) xxx

along with other emerging contaminants [20]. Furthermore, actions retention capability of wastewater treatment plants towards MPs, large
toward their reduction in the environment have also been suggested by loads are discharged to the environment every day by these facilities
the SAM (Scientific Advice Mechanism) Group of Chief Scientific Advi­ [24]. Besides, the application of treated sludge for agricultural purposes
sors to the European Commission [21]. Indeed, MPs are considered both turns them back into sources of MPs for the environment.
in the Marine Strategy Framework Directive (MSFD) and the EU Plastic MPs fate and transport in water environments are influenced by
Strategy [17] and nominated as pollutants of concern in the EU review many different factors, such as MPs density, shape and size, and also
of the Urban Waste Water Treatment Directive (UWWTD) [22]. relations with biota. All such factors interact with the characteristics of
Research on MPs rocketed in the last decade, beginning with studies on the hosting waterbody: water flow velocity, water depth, bottom
the marine environment but broadening soon to other environmental topography, seasonal variation of water flow, tidal cycle, storms, floods
compartments and to related toxicology. If some clarity on certain as­ and anthropogenic activity (e.g. dam release) [25].
pects have been achieved, such as their widespread presence, still the
dearth of certainties regarding their effects and behavior compels to a 3.1. Surface waters: rivers and lakes
massive effort in deepening the understanding of the topic. This review
work aims at presenting an overview of what is known of MPs in the Regarding freshwaters, a comprehensive summary of the data
urban water cycle, focusing on the role of water treatment plants in available until 2019 about MPs in freshwaters is found in Rios Mendoza
spreading and control of MPs. A first section is hence dedicated to the and Balcer [26]. Regardless of the un-homogeneity of the data, the au­
presence of MPs in the water sources, a second section to the fate of MPs thors drew the following main observations: in China there was the
in drinking water treatment plants and their presence in drinking water, highest concentration of MPs in the world, being also one of the bigger
a third section is focused on the presence and fate in wastewater treat­ plastic producer; urban areas tended to have higher concentration of
ment plants, a fourth section is dedicated to the studies that tried to MPs as compared to rural areas; stormwater retention ponds concen­
understand the link and role of wastewater treatment plants in modifi­ trated MPs [26]. Another rich source of data is the review by Schell et al.
cation and determination of microplastic pollution in water bodies. The [27] where the authors compared studies using homogeneous units of
last two sections aimed at connecting the information gathered to offer measurements: i.e. they transformed the units of MPs/surface into
an overview of MPs in the urban water cycle and the possible future MPs/volume, when it was possible. In conclusion it was assessed that
perspectives. MPs concentration in European freshwaters was in the interval
1–100 MP s/m3, with some noticeable exceptions. The highest values
2. Foreword on data comparison were reported in the Snake River in North America (5,405,000 MPs/m3)
and in Vietnam, while very high concentrations were found in Asia,
Data comparison is central and essential to researchers in order to specifically in China (as reported above). However, when including the
evaluate the results obtained, validate them, frame them within the MPs lowest size, the results did not differ significantly among the
related context, understand likenesses and differences in distributions, countries. The same authors highlighted that smaller particles were
trends and behaviors. often the most frequent ones; they also underlined how different sam­
Up to now though there is no common framework for MPs sampling, pling protocols and devices led to significantly different results.
sample pre-treatment, MPs identification, quantification and classifica­ Increasing MPs concentration were linked to urban areas. Fragments
tion. This greatly affects the chance of retrieving information by com­ and fibers from Polyethylene (PE) and Polypropylene (PP) were the MPs
parison of literature data. Indeed, there is not only a lack of coherence in most frequently found. The predominance of PE and PP, as of fibers and
the data collected on microplastic presence in the various media fragments, had been confirmed also by Li et al. [28]. “Temporal hot­
involved, but even among studies related to the same environmental spots” in MPs concentration might be linked to weather conditions:
compartment. storms and rainfall could increase the runoff and the sewage contribu­
The use of different methodologies for each step of the MPs analysis, tion, while floods could be related to the resuspension of sediments and
results in not comparable data: for instance, a too small sample volume hence of sedimented MPs [27]. The authors noticed how higher con­
might hamper its representativeness, difference in targeted size range as centration was generally found in riverbeds compared to river beach and
in the solution used for density separation leads to different MPs con­ shore sediments [27]. The role of the hydrological features of rivers for
centration and characteristics, all identification techniques have diverse the MPs sedimentation and the influence of winds, waves and beach
strengths and weaknesses. Moreover, there is neither a standardized size morphology on their deposition on lake shores was also reported by
classification nor a common morphological classification [23]. many studies [27].
Without precise information on the analytical protocols followed and Following, the recent updates published in 2020, obtained on Ebs­
the quality assessment conducted, the data showed are not even indic­ coHost search engine of the University of Rome La Sapienza (a sum up of
ative and possibly misleading. which is reported in the supplementary material), are summarized and
commented.
3. Microplastics evidences in water sources Based on these papers, fibers, followed by fragments, were confirmed
as the most common, as well as the smallest size fractions and PE and PP
MPs sources to water environments have been ascribed to many as most frequent polymers. However, there are also some studies who
different origins. Galafassi et al. [24] reported an estimation of MPs reported a prevalence of beads [29] or films [30,31]. Socio-economic
inputs to water systems based on data from scientific and grey literature features of the area under study are confirmed as relevant factors in
(i.e. non-conventional scientific publications, e.g. governmental reports, determining MPs pollution. Table 1, obtained from the same list of 2020
issues papers etc.). Sources considered were land-based and off-shore, studies, reports the factors mainly affecting MPs pollution. Particularly,
including wastewater treatment plants, tires and roadways, municipal the specific aspect and parameters are highlighted along a brief sum­
solid waste, primary MPs loss, blasting abrasive and paints [24]. The mary of the conclusions. Among these factors there are: hydrological
relevance of an effective waste management system was also underlined and morphological characteristics of the catchment, weather and
by Wong et al. [25]. According to Galafassi et al. [24], the higher climate related phenomena and socio-economic factors. Specifically, the
contribution to MPs pollution was linked to tires and fragmentation of MPs abundance is strongly related to the Gross Domestic Product (GDP)
either litter or fishery and aquaculture equipment [24]. The authors also of the area, as the presence and quantity of industries. On this account, it
underlined how wastewater treatment systems achieved an important is worth of notice the attempt by Zhang et al. [32] at defining the
reduction of land-based sources originated from factories, buildings and relation between MPs abundance and the type of industry (primary,
urbanized areas. However, it was highlighted that even with the high secondary, tertiary). These parameters are strictly followed by

2
M. Barchiesi et al. Journal of Water Process Engineering xxx (xxxx) xxx

Table 1 Table 1 (continued )

Factors influencing MPs abundance in the environment. Topic Ref. Parameter Main conclusions
Topic Ref. Parameter Main conclusions
with flow was indicated as
Statistically significant “inconsistent”
difference in MPs 19 Rainfall, flow Could not determine clear
concentration upstream and patterns between MPs
downstream WWTPs effluent abundance and river flow rate
1 Sampling device
with a manta trawl net, no or rainfall (sampling
statistically significant difficulties in flood
difference with a pumping conditions)
device sampler Spatial vs 20 Spatial variations (as in
MPs abundance and the fibre temporal geographical, demographical
content detected with a pump variations or WWTPs inputs) had higher
Analysis
sampling device was influence on MPs abundances
methodology 2 Sampling device
significantly higher compared than temporal variation (as in
to that recovered by plankton flow or wind conditions)
nets Higher MPs concentration was
21
Differences in MPs found at rivers mouth
Influence of
concentration between the Higher concentration in the
3 Sampling point hydrological
left, middle and right section inner and outer bends of the
features 22
of the stream river compared to the straight
MPs mainly distributed on the tracts
4 Sampling point surface compared to the other
Ref. 1 [40], 2 [32], 3 [41], 4 [36], 5 [33], 6 [42], 7 [32], 8 [40], 9 [43], 10 [44],
depth levels
Significant correlation of 11 [29], 12 [45], 13 [37], 14 [39], 15 [46], 16 [43], 17 [41], 18 [39], 19 [38],
parameters with MPs 20 [47], 21 [31,35,36], 22 [37].
GDP, population concentration, (positive
5
density, (land use) correlation though not
population density and land-use. The differentiation between rural and
significant with build-up land
use)
urban areas is though not well defined. Their relative influence on the
Significant correlation of MPs abundance is also related to the surroundings state in terms of
GDP, population
6
density
parameters with MPs pollution and catchment characteristics, of morphology and flow
concentration regime. Indeed, if urban areas are often characterized by higher MPs
Significant correlation of
pollution, the difference compared to the surroundings is not always
parameters with MPs
concentration, (correlation significant nor confirmed. Also, the hydraulic characteristics of the
Per capita GDP,
7 though not significant with water body and anthropic changes are put under the spotlight by some
primary industry
population density, basin authors: Huang et al. [33] observed a noticeable decrease in MPs
area, runoff and tertiary abundance in water downstream the river dam, while Dahms et al. [34]
industry)
MPs concentration
did not notice a difference in MPs abundance in water, while observed
8 industrialization significantly higher in higher MPs abundance in sediments and biota upstream. River mouths
industrial areas appears to be often a concentration spot for MPs, while the straight
Influence of socio- Packing industry as probable tracts seem to ease MPs flow along the river compared to inner and outer
9 industrialization
economical source of the MPs
bends [31,35–37]. Atmospheric deposition is also considered: Constant
features The predictors indicative of
urbanized areas (as et al. [38] evaluated the role of MPs atmospheric deposition as possibly
population density and urban significant; by contrast, Stanton et al. [39] considered such contribution
10 urbanization
percent) were among the being not important but argued that the low values recorded could be
highest in explaining MPs linked e.g. to the sampling height and other various environmental and
abundance variation
The predictors related to
meteorological factors. Regarding weather related phenomena, the in­
urban filters explained the 22 crease of MPs pollution due to rainfall might be linked to the contri­
11 urbanization % of the variation, while 15 % bution given by the urban drainage collecting MPs otherwise deposited
was linked to MPs possible on urban surfaces; the rain events of high intensity could easily clean
source
urban surfaces conveying a first peak followed by dilution. A higher
No significant correlation
12 urbanization among MPs abundance and concentration of MPs is expected during dry season due to the reduced
distance from the city centre effect of dilution with respect to the wet season. All these hypotheses
No significant difference in need confirmation and critical proof.
13 urbanization MPs abundance between Regarding specifically MPs sources to water bodies, it is interesting
urban and rural area
Urban areas were not always
the approach applied by Grbić et al. [44] to assess the relevance of
14 urbanization responsible of a significant stormwater and agricultural runoff. They found MPs in all streams, with
increase in MPs abundance noticeably a 22 % of tire and road wear particles in the urban runoff and
MPs concentration were nowhere else; they also noticed polymers related to agricultural activ­
15 seasonality always higher in dry season
ities in the agricultural runoff.
compared to wet season
MPs concentration were These reviews and studies show that space and time variations are
always higher in dry season important factors to assess the MPs pollution in surface waters. More­
Weather and 16 seasonality
climate
compared to wet season over, a careful evaluation of sampling points, methods and time has to
(limited) be always considered in MPs research.
influence
Positive correlation between
17 rainfall MPs abundance and rainfall
events
No seasonality in UK river MPs
3.2. Groundwaters
18 Seasonality, flow
abundance and the relation
Information on MPs in groundwaters are rather scant. The MPs found
in two Illinois karst aquifers were mostly fibers along with other

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M. Barchiesi et al. Journal of Water Process Engineering xxx (xxxx) xxx

pollutants, that suggested septic effluents as the source; however, the whole scale by a limited number of works. The results are reported in
authors underlined the need for further studies [48]. The characteristics Table 2 and discussed below, whereas the few bench-scale experiences
of the polymers found by Mintenig et al. [49] led the authors to the are summed up in Table 3.
conclusion that the MPs contamination was mostly due to abrasion The first study reported in Table 2 evaluated the treatment efficiency
during the drinking water supply chain or to airborne contamination of three different DWTPs. The change in the relative abundance of MPs
during the analysis [49]. Another evidence of MPs in groundwater is morphology suggested the possible presence of a relationship between
offered by Ganesan et al. [50] who found PET and Polyamide in the shape and removal [54]. The second study evaluated instead the pres­
groundwater of Tamil Nadu, India. The consideration of the multiple ence of MPs in various points of the drinking water supply chain,
possible paths for MPs into groundwaters, the transportation within and including the inlet and outlet of a plant treating groundwater. The
the relevance of those as water sources [51], is urging for a more microplastic presence was found to be very low; it was hypothesized that
extensive survey. its origin could be linked to atmospheric or supply chain contamination
[49].
4. Microplastics presence and fate in drinking water treatment The third study cited in the table is the first one, to the best knowl­
plants edge of the authors, to report the removal efficiency for MPs particles at
each step of the water treatment line of a DWTP [62]. MPs size distri­
Evidences of MPs in drinking water were first collected in 2017 by a bution, morphology and composition were also assessed at each step,
“not peer-reviewed” research work published later on with PLOSONE and possible relations between such characteristics and the removal
[52]. In 2018 other data appeared in scientific journals [53–56], efficiency was considered. No MPs >50 μm were found in the effluent
whereas the World Health Organization (WHO) commissioned a report and the relative percentage of the 1− 5 μm increased. Ozonation caused
on the presence and possible hazards of MPs in drinking water [19]. In an apparent slight increase in MPs abundances, due to the shear forces
the review on MPs in freshwaters and drinking water by Koelmans et al. exerted by the flow. The authors hypothesized also an increased effi­
[57] a first assessment of data quality was attempted. Other review ciency in identification due to the more effective organic matter diges­
works were then developed, as that published by Eerkes-Medrano et al. tion of the sample by the pre-treatment step, favored by the ozone
[58]. In the paper by Akhbarizadeh et al. [59] focus was on bottled oxidation occurred in the water treatment line. The GAC step removed
water, whereas Novotna et al. [60] and Shen et al. [61] addressed the partially the MPs from the ozonation effluent, though the mechanism
fate of MPs in the drinking water treatment plants. Evidences of MPs at responsible was unclear [62].
the end of the water supply chain are uncanny, though origin and cause Based on the reported data, it can be assessed that DWTPs contribute
of pollution are far to be fully cleared. Plastics in bottled water might to a significant reduction of MPs, also when treating surface waters
indeed significantly be linked to the packaging material and its wear; where the influent load is higher. Moreover, the CFS + SF + GAC layout
however, presence of MPs in glass bottled water suggests also different seems to able to remove above 80 % of influent MPs, according to the
origins of the pollution [59]. According to the studies until now pub­ data of the second DWTP of the first study (WT2) and the DWTP
lished, MPs found at the outlet of drinking water treatment plants vary considered in the third research (which included ozonation too) [54,49].
noticeably in concentration, from 0 [49] to 930 MPs/L [62] due to the Furthermore, it is confirmed the higher selective removal of fibers, [54,
different water sources, plant layout and analytical methods. The chance 62], possibly related to the plant layout [54]. In general, the most
of contamination by the water supply chain purification and conveying challenging size fraction seems to be the smallest, being the harder to
equipment is also suggested [49]. remove and therefore frequently found in the effluents (see Table 2). The
Drinking water treatment plants (DWTPs) are not designed specif­ interactions with other parameters, such as inflow water quality and
ically to treat MPs, though the removal of solids and colloids is a specific DWTPs process characteristics, are to be still further investigated. Hence
obligation to the obtainment of potable water. MPs belong indeed to the more studies are required to drive more conclusive deductions on all
“solids” category. Features relevant to understand the treatment effi­ these aspects.
ciency are the MPs size, morphology and polymer composition as their Regarding specifically the coagulation process, put under the spot­
surface characteristics. On this account, MPs are defined as hydrophobic light being one of the most used to obtain and enhance solid-liquid
[19], while polymers surface charge is reported in Novotna et al. [60]. separation, from the bench scale studies it seems that at the co­
The possible interactions with the various treatment processes employed agulants dose used at full scale, the removal efficiencies are low and
in the water treatment sector were analyzed by Enfrin et al. [3] and Shen anyhow size dependent. The optimization of the operative parameters is
et al. [61], although the experimental data available are few. To which hence still to be defined. The reported efficiency by CFS in a full scale
extent DWTPs are able to purify raw water from MPs has been studied at DWTP though was higher compared to that obtained at the bench scale

Table 2
Studies on the removal efficiency of DWTPs towards MPs.
Ref. P.Q.I Size Source Treatment layout IN OUT R%
target

1 WPO; SEM, FTIR, 1μm- water CF + SF (WT1) >10 μm only 1473 ± 34 (WT1) <10 μm 443 ± 10 70 (WT1)
RAMAN 5 mm reservoir CFS + SF and GAC (WT2) 10 % c.a 1812 ± 35 (WT2) prevails (WT1) 81 (WT2)
water CF + flot + SF and GAC Fragments 3605 ± 497 Fragment 338 ± 76 83 (WT3)
reservoir (WT3) PET + PP (WT3) PET + PP (WT2)
river MPs/L 628 ± 28
(WT3)
MPs/L
2 HCl+H2O2 + 3μm- groundwater Filtration + aeration 0− 7MP s/m3. All 50− 150 μm, PEST, PVC, PE, PA and epoxy resin n.a
(ZnCl2) 5 mm
FTIR
3 H2O2 + 0.2μm- river CFS + SF + ozonation + GAC 1− 5 μm, fibers 6614 ± 1132 1− 5 μm, 930 ± 72 82.1–88.6
SEM + RAMAN 5 mm PET, PE MPs/L fibers MPs/L
PET; PE

Ref. 1 [54], 2 [49], 3 [62] P.Q.I – pre-treatment, quantification and identification methods; IN = influent; OUT = effluent; R %=removal efficiency; CF coagu­
lation/flocculation; CFS coagulation/flocculation/sedimentation; GAC granular activated carbon; SF sand filtration; flot. floatation.

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M. Barchiesi et al. Journal of Water Process Engineering xxx (xxxx) xxx

Table 3 Table 3 (continued )

Bench scale studies on MPs removal in water treatment plants. Ref. Process Observations Main results Notes
Ref. Process Observations Main results Notes on methods
on methods
the particles
1 CFS, -High Al-based salts -Novotna et al. [60] lowering filtration
ultrafiltration dimension of performed observed how the efficiencies
particles used better, although need of coagulation 3 Disinfection HDPE and PP
-Only PE at dosage for removing by chlorine seemed to be quite
particles typically used in particles of the agents resistant to
evaluated water works the order of millimeters commonly used
(supposedly removal was is doubtful, being dosage while PS
fragments) only of 8 %. usually devoted to was an exception: it
-No fibers Increasing the the removal of shows indeed
included dose to 405 mg/ colloidal solids. detectable changes
L Al (15 mmol/ -Shen et al. [61] in structure even at
L), removal and Novotna et al. CT values as low as
efficiency of [60] observed how 75 and
about 37 % was the PAM added 150mg*min/L [66]
obtained. exceeded by far the
Ref 1 [63], 2 [64], 3 [66].
High removal maximum allowed
efficiency by WHO for
obtained by drinking water. [62]: this can be linked to the different size range evaluated by the
polyacrylamide -Novotna et al. [60] studies and also to the higher variety of MPs in raw water compared to
(PAM). underlined how the
Complete presence of much
the synthetic one used for the bench scale studies. Indeed, at full scale,
removal smaller MPs is the size-related removal is confirmed by a higher retainment of the
obtained by expected in DWTPs bigger particles; however, the shape mostly retained were fibers, not
ultrafiltration. compared to those included in the bench scale studies [62–64]. Concerning filtration on
used in the study
whatsoever matrix, much needs to be unveiled too: the interactions
(indeed confirmed
by the studies between MPs and the solids are still unclear as well as the effect of
previously reported operational parameters (e.g. flow velocity, backwash time). Anyway,
in Table 2), hence the removal efficiencies reported for CF + SF seems to be around 60− 70
the partial % [54,62]. Regarding membrane processes for drinking water treat­
usefulness of the
results obtained
ment, plenty is still to be uncovered, beginning with the behavior of
[60]. membrane towards different MPs morphology classes and sizes. A step
2 CFS, filtration Particles size -Removal <2 % - No significant forward in this direction can be considered the study by Enfrin et al. [65]
range for all size difference in specifically tackling the kinetic and mechanistic aspects of membrane
(<125 μm) classes with Al removal
fouling by MPs and NPs [65]. The chemical agents used in oxidation and
and amount, coagulant at full percentages among
polymers used scale DWTP the size classes with disinfection might have some effects on the particles but this aspect is
(PE, PS), dosage. Al coagulant also yet to be fully assessed [62,66].
coagulants -removal - PolyDADMAC:
dosage and increase with significant removal 5. Microplastics presence and fate in wastewater treatment
filtration PolyDADMAC increase. for the
parameters (max. of 13.6 %) 45–54 μm particles
plants
chosen to -Higher removal - Low removal
resemble as efficiency by efficiency obtained Wastewater treatment plants (WWTPs) receive sewage from the
much as filtration on are most probably pertinent area and treat it in order to abide by the discharge limit reg­
possible those anthracite (from linked to the
ulations. Contaminants targeted by wastewater directives are mainly
of a full scale 86.9 %–99.9 %) buoyant nature of
DWTP. Test -Effect of biofilm the plastic used for solids, organic matter, nutrients and pathogens. Wastewater treatment
performed on is significant on the trial plants are hence not designed to specifically remove MPs [67]. Sources
clean CFS removal of - Wide differences of MPs to wastewater treatment plants are directly linked to the flow
particles, microplastics among size classes origin: separate or combined sewage systems, domestic or industrial
afterwards (increase to 16.5 and not
one size class %), no proportional to the
wastewater, landfill leachate. Separate systems convey wastewater from
is chosen, and significant change of particles household appliances and commercial or industrial wastewater. For
processes variation for size for removal instance, MPs due to domestic discharge are mainly linked to the Per­
evaluated on filtration. efficiencies by sonal Care Products (PPCP) (as exfoliants, toothpaste) and fibers from
MPs colonized filtration
synthetic clothes washing [68], while MPs of industrial origin are
by biofilm - CFS removal on
-No fibers MPs with biofilm: mainly related to air blasting applications and water discharge by plastic
included change in particle items production factories [69,70]. MPs in landfills leachate are con­
size and density nected to the degradation processes that plastic items undergo in the
plus the production peculiar environmental conditions that establish in the landfill itself:
of Extracellular
Polymer Substance
causes of modification for the polymers are indeed the varying pH
(EPS), promote conditions, the formation of gases and aggressive compounds as the
aggregation and changes in mechanical stress [71]. Combined sewage systems deliver to
sinking rate. the WWTP the water from the urban runoff too, hence implying the
Besides,
presence of MPs linked to the embrittlement of larger plastic debris
microorganism’s
colonization might found on the urban ground, tires fragments due to friction with roads
result in surface [67] and MPs from atmospheric deposition [69]. Indeed, Sun
fragmentation of et al. [67] reported in their review evidences of increasing MPs con­
centration in influent linked to combined sewage collecting systems,

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M. Barchiesi et al. Journal of Water Process Engineering xxx (xxxx) xxx

probably due to the urban runoff gathered. Stormwater retention ponds Table 4
have been found as hotspots for MPs pollution, being moreover those Factors influencing influent characteristics.
related to industrial and commercial area more polluted than those Factors Ref. N◦ of plants/ Notes
linked to highway and residential areas [72]. research
An overview of the fate of MPs along the whole water treatment line period
was compiled by Carr et al. [73] where the findings from 8 WWTPs of Socio-economic 1 50 WWTPs/fall -MPs load strongly correlated with
Southern California were reviewed and compared to the other re­ months population served and influent
searches available at that time. Each step of the treatment was analyzed volumetric flow rate
-The relative contribution of indirect
in light of MPs characteristics and the possible removal processes were source remains unclear
pinpointed. Same approach was followed by Ngo et al. [69] in a very Socio-economic / 2 3 WWTPs/ -Location (urban or rural) and
comprehensive analysis of the literature on MPs in WWTPs, addressing weather- more than 1 treatment of industrial WW relevant
also the sources and pathways to the plants. In Sun et al. [67], it was related year for the explanation of the dynamics
and relative MPs concentration,
instead deeply analyzed the MPs analytical protocols (updated later on
characteristics and per-capita load.
by Bretas-Alvim et al. [74]) as well as the characteristics of MPs in -Significant correlation with rainfall
wastewaters and their fate in WWTPs. Sludge was explicitly targeted by found only for a WWTPs located in a
Lusher et al. [75] and Rolsky et al. [76]. Among the latest reviews of rural area hence runoff relevant for
peculiar interest is the one compiled by Schell et al. [27] on freshwater less densely populated areas
- Satisfactory linear relationship for
and terrestrial ecosystems: here a specific section on WWTPs was also MPs abundance and the number of
included, presenting one of the most up to date gathering of information plastic-related manufacturers in the
7 WWTPs/3
on this topic. Another complete summary of the data is found in the 3 area studied.
days
article by Birch et al. [77]. -No indication of correlation
between MPs concentration and
population density
5.1. Influent to WWTPs -Average influent concentration was
not statistically different between
Data on the MPs concentration in the influent to the WWTPs vary the WWTPs.
Socio-economic - Fibers per-capita load of one of
highly among the literature researches: to the best knowledge of the
them was significantly higher
author, the highest value recorded until now is 10,044MPs/L related to a 3 WWTPs/1 compared to the others: this was
10 μm finest mesh [78], while the lowest value is 1.5MPs/L related to a 4
year explained by the more diverse
26 μm finest mesh [79]. Lower values were reported by Carr et al. [80] sewages received by the plant,
and Mason et al. [81] but without a chemical identification [80,81]. including residential, commercial,
and industrial (the other two treated
Such a variability might be linked to external factors such as the char­
mostly residential and commercial
acteristics of the served area, weather, season, type of sewage collecting sewages)
system and plant treatment capacity; however, it might also have origin 2 WWTPs/ 1 -Influence of industries on
5
from the applied measurement protocol. Therefore, understanding the week concentration and characteristics
influence of the external factors is possible only for those researches that - Statistically significant differences
in influent MP concentration:
analyzed more WWTPs, where results of different plants can be 1 WWTP/more summer MP concentration in
considered comparable aside of the applied analytical protocols. The 6
than 1 year influent was indeed higher
information on the influence of socio-economic factors and - (Noticeably they didn’t find time
weather-related factors on the influent to WWTPs as the observation of related pattern for the effluent)
1 WWTP/6
time-related patterns are summed up in Table 4. 7 - No significant seasonal patterns
month
The presence of industrial wastewater can influence the character­ 3 WWTPs/
- No apparent trend for influent MP
istics of the inflow to a WWTP, especially in terms of polymers abun­ 8 more than 1
concentration
dance, morphology and variety [70,84]. The specific contribution of Time related
year
industrial effluents to the WWTPs in terms of MPs could hence be - Inflow in-season variability
patterns 3 WWTPs/1
9 comparable to the all-year degree of
considered of importance, although not yet defined precisely in its year
variability
quantity nor quality [88]. Therefore, it is relevant to define the char­ -Daily variability observed: not
acteristics of the industrial contribution to MPs inflow to WWTPs, for a 1 WWTP/1.5 statistically significant increase in
10
better choice of the remediation strategies. Regarding possible daily or year mean MPs concentration was found
between morning and afternoon
seasonal variation, the information available do not allow for some
- Reported variation between
clarity and more studies are required for a better understanding of the morning and afternoon but
1 WWTP/
issue. 11 remarked how the absence of
1 year c.a
Another important aspect to consider is the potential link with other replicates could demote the power of
pollutants. For instance, a strong linear relationship between MPs and the observation.

suspended solids was indicated by Long et al. [70], whereas Bayo et al. Ref. 1 [82], 2 [79], 3 [70], 4 [83], 5 [84], 6 [85], 7 [86], 8 [79], 9 [83], 10 [85],
[85] noticed an inverse relationship [85]. Bayo et al. [85] found also 11 [87].
significant inverse relations between high COD influent and PS and PET
abundance. Moreover, in the same paper it is reported an inverse rela­ size range, with highest percentage within 1.5− 38μm: often overlooked
tion between influent MPs and nutrients in the outflow, justified by the lower size classes could indeed contain more MPs. Finally, Simon et al.
possible adsorption of nutrients on the MPs surfaces [85]. [78] found that the influent concentration of MPs to 10 WWTPs was not
Regarding raw wastewater characteristics, Ngo et al. [69] noticed normally distributed in terms of particle numbers nor of mass; however,
fibers and fragments as the main fractions in WWTPs influent (average they did not deepen the understanding of the differences among the
of 56.7 % and 34.4 %, respectively), while the most common polymers WWTPs.
were PE and PP (ranging 11–42 % and 3–32 %, respectively), PET (up to Conclusively, influent load of MPs to WWTPs and their characteris­
42.26 %), PES (79.1 %) and PA (61.2 %) [69]. Regarding MPs size, Sun tics seem to be possibly influenced by various factors: source of MPs
et al. [67] reported how often the fraction >500 μm was the most pre­ (industrial, domestic…), population served, sewage collecting system,
sent. Raju et al. [89] found instead increasing frequency with decreasing

6
M. Barchiesi et al. Journal of Water Process Engineering xxx (xxxx) xxx

rainfall and seasonality. It is still to be understood which of these and PS were the most abundant in sludge compared to other low-density
characteristics have the higher effect and the relative contribution in polymers, confirming the role of density during separation by sedi­
different contexts. Regarding time related patterns, although some data mentation. The different removals reported by the various papers can be
are reported, definite conclusions cannot be drawn (Table 4). related to the various secondary treatments and operational conditions
applied in the plants, and the different size and types of MPs.
5.2. Fate of MPs in WWTPs According to Ngo et al. [69] the Membrane Biological Reactor (MBR)
is the best technology for MPs-containing wastewater treatment,
According to the review by Ngo et al. [69], fibers are the most reaching consistently removal efficiency higher than 99.5 %. The au­
difficult items to be removed, whereas PE and PP, most abundant in the thors underlined anyway the need of research on fouling and liquid
influent, are almost absent in the effluent, because being removed by distribution after a period of operation [69].
skimming due to their low density. By contrast, according to Fahrenfeld Indeed, Bayo et al. [86] noticed how, in a WWTP in Spain during
et al. [90], fibers and films are the best removed items. This disagree­ eighteen months of observations, MBR process showed higher removal
ment is probably linked to the different characteristics in terms of the efficiency than CAS + RSF (79.01 % vs 75.49 % respectively) though the
plant layout and analytical protocols used in the studies reviewed. The difference was not statistically significant. The removal percentages
overall MPs removal efficiency found in the literature ranges from about reported by this work were not as high as could be expected, but
60 % to 99.9 %. Among the factors influencing the removal efficiency, coherent with Raju et al. [89] who examined a wider MPs size range
the plant layout and the technology are of sure relevance [69]. The [89]. Bayo et al. [86] found also statistically significant differences in
analytical protocols used for the evaluation of MPs may also play a role: MPs particles removal as compared to fibers for the conventional acti­
as already explained in the previous sections, different analytical pro­ vated sludge plus rapid sand filtration (CAS + RSF) and the Membrane
tocols lead to different fractions of MPs extracted from the samples. Biological Reactor (MBR) [86]. The authors confirmed moreover the
Therefore, the calculated removal efficiencies are possibly different not different removal of polymers: indeed, of the 14 polymers detected in
only for MPs overall abundance, but also for the different classes used for the influent, only melamine (MUF) was found in the effluent from the
their characterization (e.g. removal of fibers, fragments). MBR. whereas LDPE, nylon and polyvinyl were detected in the effluent
Regarding pre- and primary treatments, the reported removal effi­ from RSF.
ciency by Ngo et al. [69] varied from 40.7 % up to 91.7 %: this was not Tertiary treatments removal efficiency was well summarized by Sun
only related to the presence or absence of an aerated grit chambers but et al. [67]: membrane processes are considered a reliable solution to
also to the influent characteristics in terms of polymer types [69]. The MPs pollution whereas filtration systems (e.g. disc filters, rapid sand
authors also argued how fibers were the less removed items at these filtration, others) are not as dependable. Rapid sand filtration (RSF)
steps [69]. Sun et al. [67] also reported based on their literature analysis showed significant inconsistences in the removal rate of MPs according
a removal range of 35–59 % in pre-treatments and 50− 98 % after pri­ to Ngo et al. [69] too. Sun et al. [67] added that biological aerated filters
mary treatments, linking these values to the MPs density too, with the (BAF) and maturation ponds did not significantly change the MPs
lighter being removed by skimming and the heavier by settling. They amount in the effluents [67].
added that the pre-treatments had the largest impact in MPs relative size Finally, Park et al. [82] found that plants supplied with advanced
distribution, being able to remove those of larger size. Noticeably it is phosphorous removal processes showed significantly higher removal
here argued how fibers were more effectively removed by pretreatments efficiencies [82].
than fragments, noticing a decrease in the relative abundance of fibers Regarding effluent characteristics, Freeman et al. [93] reported how
after the pretreatments [67]. polyester microfibers and polyethylene microparticles are the most
Regarding secondary treatments, considering “activated sludge and found in WWTPs effluents, whereas according to Sun et al. [67] MPs of
sedimentation”, Ngo et al. [69] reported removal efficiencies in the the smallest size fractions are most common. For some authors, the
range 28.1–66.7 % related to different configurations (aerobic tank, lowest size classes have indeed the higher frequency [89,91,92]; how­
succession of anaerobic, anoxic and aerobic). According to the authors, a ever, other authors do not confirm this finding [79].
longer retention time boosts the growth of biofilms on MPs, resulting in Regarding effluents time related patterns, Bayo et al. [85] found no
increased weight and flocs entrapment and therefore a better removal. significant difference among seasons. Weather related events appear to
The authors underlined anyway the need of further research on the topic have significant relevance in some cases, as indicated by Mintenig et al.
[69]. In some studies, MPs overall removal obtained by secondary [49] where noticeably higher concentration was found in the effluent in
treatments was higher than 90 % [82,85,91,92]. a time frame including a strong rain event. This finding was already
Sun et al. [67] reported a further decrease in the secondary treat­ underlined by Wolff et al. [94], who indicated as responsible the higher
ments of 0.2–14 % compared to the primary treatments. and confirmed flow velocity and hence poorer settleability of the particles. Long et al.
the unknown interactions between flocculants, microbes and MPs, as [70] found also a strong relationship between effluent MPs concentra­
well as the relevance of retention time and nutrients. Moreover, frag­ tion and the operating load of the WWTPs.
ments appeared to be removed more than fibers: the authors noticed Conclusively, fibers appear to be the less retained by the WWTPs and
indeed an increase in relative abundance of fibers after secondary the most abundant in the effluent along with the fragments. The effects
treatments, followed by a decrease in higher size MPs classes, even if of WWTPs on the size distribution and polymers variety has not been
with some exceptions [67]. Lower removal of fibers by secondary completely cleared yet. Regarding plant layout, pre- and primary
treatments was indeed confirmed also by recent papers [85,89]. Park treatments have a significant role in MPs removal; the effect of the
et al. [82] found a higher relative abundance of fibers in the effluent as secondary and tertiary treatments depends upon the technology chosen,
compared to the influent. However, this could be linked to the different although a significant removal is often obtained by the secondary
sampling devices used for the two streams: compared to the influent treatments. The relevance of operational parameters has to be deepened:
(grab sampling), filtration time of the effluent on site is longer due to the based on the available data, it seems that the lower the hydraulic
higher volume to sample, hence the fibers have a higher chance of retention time of the whole plant, the lower the MPs removal. About
slipping through the sieves [82]. In Bayo et al. [85], a statistically sig­ tertiary processes, membranes are more efficient and reliable than
nificant removal of MPs larger fractions by the main WWTPs processes is filtration in retaining MPs. Concerning temporal related patterns, there
observed, decreasing the mean size of MPs along the treatment line until are recorded evidences, but no definitive conclusion can be driven: more
the biological reactor (water treatments included grease and grit comparable information is needed for the evaluation of such variations.
removal, primary clarifier and biological reactor). The mean size
increased a little in the effluent [85]. Raju et al. [89] noticed how PET

7
M. Barchiesi et al. Journal of Water Process Engineering xxx (xxxx) xxx

5.3. Presence and fate of MPs in sludge (with points given on the probability level of source belonging), and a
ninth class as “others” for unidentifiable plastic objects. They also
MPs presence in the sludge is a direct consequence of MPs removal defined a “diversity index” to quantify the variety of MPs sources. These
from the water treatment line. Those MPs removed by preliminary two tools were conceived to help in individuating management strate­
treatments are disposed without further treatments and are likely to end gies based on the variety of the MPs sources hypothesized. This
up in landfills or incinerated. Instead, MPs embedded within sludges, approach was indeed used by Liu et al. [40] to understand and describe
follow these in the sludge treatment line. If MPs concentration in sewage MPs pollution sources and distribution in the Haihe river [40]. This
sludge has been verified in different points of the treatment line by classification still leaves some decision to the operator and it is therefore
several studies, the effect of sludge treatments on MPs is yet to be fully prone to human errors, even if strongly limited by the rules imposed by
cleared. Lusher et al. [75] provided a comprehensive table with studies the method. Therefore, more automated systems should be developed.
carried out until 2019, considering different WWTP layouts for the water The topic of MPs sources individuation and quantification has also
and sludge treatment line, and also MPs concentration and main char­ already been addressed in literature. Indeed the review by Fahrenfeld
acteristics [75]. Studying the available literature, Lusher et al. [75] et al. [90] deals with the issue of source tracking in freshwater envi­
observed how the inhomogeneous analytical protocols applied did not ronments and identifies three methods to this purpose: (1) linking par­
allow for a proper comparison among studies. However, general ticles characteristics to sources, (2) source sampling and mass balance to
agreements among studies can be found on some aspects: concentrations establish inputs, (3) considering particle surface contaminants to
are higher when smaller fractions are included in the analysis, alteration implicate potential sources. Cowger et al. [23] specifically focused on
in shape and size might indicate an influence of sludge treatment pro­ WWTPs as MPs sources, categorized instead MPs water pollution evi­
cesses [75]. The studies evaluating MPs in different steps of the sludge dences from WWTPs in anecdotal evidence, taxonomic evidence and
treatment line are hardly found. Lares et al. [13] took samples from evidences based on MPs correlation between the effluents and the water
activated sludge and digested sludge, while Talvitie et al. [95] sampled body. The correlation was evaluated based on proximity and quantity of
excess and dried sludge: both did not clarified about the possible effects WWTPs discharge. Of the 23 studies they reviewed, 11 had the aim of
of the different sludge treatments. Edo et al. [92] sampled sludge from establishing the role of WWTPs as MPs source, only 6 sampled WWTPs
the anaerobic digester and the commercialized pellets at the end of the effluent too and only 5 did not establish the wastewater effluent to be a
sludge treatment line and noted how processing the sludge at 300 ◦ C did significant contributor.
not alter significantly the MPs particles. Xu et al. [96] studied the sludge Mass balance would theoretically offer the most reliable results, but
profile in a WWTP in China over three months and detected an increase various issues must be considered: e.g. mass distribution along a whole
in MPs content in the sludge probably linked to the rainfall conveying section is necessary though not always easily achievable; sampling of
urban runoff to the plant. Regarding MPs characteristics, Edo et al. [92] different matrices would be appropriate to establish sources and sinks
noted that MPs in sludge were on average smaller than those in waste­ (water, sediments and in some cases even biota) [23]; the lowest size
waters and that the relative abundance of fibers was higher than in classes appear to be the most common, especially in freshwaters, but
wastewaters. Potential fragmentation as well as melting and blistering their contribution to the whole mass evaluation could be expected to be
have been reported, linked to high pH and mechanical mixing in lime less relevant [47]. Anyway, to the best knowledge of the authors, no
stabilization and to heat drying [75]. Another aspect to give attention to researches have applied this method yet.
is the role of rejected water, reported to release about 20 % of MPs back Studies on MPs are including more often information on both
to the water treatment line where it is recirculated [75]. morphology and chemical characterization. To understand how this
Information on the effect of the sludge treatment line on MPs is information is used to evaluate WWTPs as source of MPs, two cases are
clearly scant and not directly comparable when considering the different here considered: first, where only up-stream and down-stream sections
sampling and analytical procedures. It is clear how treated sludge could to a WWTP are analysed, and the second one where also the WWTP
represent another source of MPs to the environment: there are indeed effluent is considered.
studies that demonstrated how the application of sludge in agriculture Indeed, as reported by Fahrenfeld et al. [90], and as could be
and sludge-based fertilizers caused MPs accumulation in soil [97–99]. concluded by the previous section of this review, the MPs fingerprint of a
WWTP effluent in terms of MPs characteristics is not necessarily fore­
5.4. Linking the sources to the receivers: the WWTPs case seen [90].
Aspect of interest should be the definition of what is “upstream” and
It has been assessed that WWTPs can be considered a source of MPs “downstream” sampling, in terms of distance from the WWTP, water­
to the environment; however, their specific role in water sources MPs body characteristics and WWTP effluent plume. This aspect is also not
pollution still requires a better understanding. Besides, it is of utmost always clearly reported.
interest the identification of potential removal and reduction of the MPs Studies where upstream and downstream sections to WWTPs were
pollution achievable through WWTPs. purposefully targeted, but WWTPs effluent was not analysed, are re­
MPs source apportionment has hence become a fundamental task to ported in Table 5 (ref. 1–9), as the source apportionment strategy.
be solved, but how to realize it based on the field results is still a matter Mostly, source apportionment followed morphology and difference in
of debate. A strategy could be the study of MPs morphology. Helm [100] concentration. Limits on morphology-based attribution have been
suggested the definition of a common taxonomy classification for MPs; already discussed in this section. When evaluating MPs concentration
however, still in 2019 Cowger et al. [23] reported 19 different terms for difference between upstream and downstream a WWTP, the dilution
MPs morphology, used differently by various studies in often over­ properties of the waterbody has to be considered; hence, a high load of
lapping subsets [23,100]. Moreover, the allotment of sources based on MPs from a WWTP can be unseen due to missing change in concentra­
mere taxonomy has been challenged: as an example, fibers, one of the tion. Also, if the MPs concentration in WWTP effluent and the waterbody
most found items in WWTPs effluents, could have origin in wastewater is similar, a variation in concentration between up-stream and down-
effluents, but also in atmospheric fallout or in fishing nets decay [8,101]. stream section is not recorded although the relative contribution of
Microbeads also could have origin e.g. in personal care products or air the WWTP to the MPs pollution of the water body could be relevant.
blasting products [69]. Polymers characterization might add some in­ Often indeed, as shown in Table 5, the difference is not significant, but
formation: the plastic objects marketed need indeed different polymer the WWTPs are still confirmed as source of MPs to the receiving water
properties according to their use [102]. An attempt in classification was body. On the contrary, a significant difference could be linked of course
realized by Wang et al. [101] considering morphology, size and chem­ to the higher MPs concentration in the WWTP effluent (if other sources
ical characterization. Eight classes were defined with possible sources could be excluded or deemed not relevant); however, the scenarios, also

8
M. Barchiesi et al. Journal of Water Process Engineering xxx (xxxx) xxx

Table 5
Studies reporting up-stream and down-stream concentration to WWTPs (ref. 1-9), up-stream, down-stream concentration to WWTPs and effluent characterization (ref.
10-17).
Ref. Country Water Matrix analysed WWTP capacity Streamflow Results and WWTP as source attribution methods
body

1 CA river water, sediment n.a n.a Significant increase of MPs abundance downstream only in one
over ten WWTPs evaluated
No evaluation of apportionment if not based on concentration, (but
environmental predictors based on MPs concentration and
morphology)
2 CHINA river water n.a 26.4*10^9 m3/y Different results with different sampling devices, but in
conclusion WWTPs deemed as one of the main discharge sources
of MPs in the river
Evaluation of apportionment based on concentration, (sources on MPs
morphology and chemical characterization)
3 UK river water 10− 900*10^3 P.E n.a MPs generally increased downstream WWTPs, no variation of MPs
types hence
Evaluation of apportionment based on concentration and morphology
4 GER river water (Teltow Canal discharge) / (WWTP effluent) = Significant increase of MPs concentration for one over three
[0.65− 2.6] during the sampling days WWTPs considered. No spatial or temporal variation for MPs
shape and size, hence
Evaluation of apportionment based on concentration and morphology
5 CA river water, biota 200*10^3 P.E (24.1–77.4*10^3 n.a Higher concentration upstream the WWTP
mc/d during sampling days) Evaluation of apportionment based on concentration and morphology
6 USA river water n.a n.a WWTP had no effect on MPs concentration or type
Evaluation of apportionment based on concentration and morphology
7 USA river WWTP, water WWTPs effluent was 0− 98 % of (5− 185mc/s) No correlation between MPs types and WWTPs, role of WWTPs as
streamflow source remains unclear
Evaluation of apportionment based on concentration and morphology
8 USA river water Contrib. of effluent to flow (%) [13.17− 110.82] MPs concentration higher downstream of 7 out of nine WWTPs
(two significantly higher)
Evaluation of apportionment based on concentration and morphology
and bacterial communities
9 USA river water 8.69 – 18.9*10^3 mc/d n.a Significant increase of MPs downstream of some WWTPs as
function of size class and morphology (I and II MPs)
Evaluation of apportionment based on concentration and morphology
(size class, I and II MPs)
10 NL River WWTP, M 0.041− 3.4 mc/s Meuse 350 mc/s Confirmation of WWTPs as source
river surface water D 0.53− 9.7 mc/s av No general increase between up and down stream WWTPs
Dommel 3.1 mc/ Higher concentration attributed to diffuse sources or other
s av riverine dynamics and processes
No evaluation of apportionment, if not based on concentration
11 CA Creeks, WWTP, water n.a n.a Confirmation of WWTPs as “dominant” source
lake Evaluation of apportionment based on concentration and MP
characterization
12 ES Lagoons WWTP, sediments 207685− 929962 m3/y authorized discharge Confirmation of WWTPs as source
Higher MPs concentration in artificially recharged lagoons
Evaluation of apportionment based on concentration and MP
morphology and spectra
13 USA River WWTP, water, n.a n.a Confirmation of WWTPs as source
sediment, air No significant increase up and downstream WWTP
Study focused on microfibers
Other sources or reservoirs of synthetic microfibers suggested
No evaluation of apportionment, if not based on concentration
14 CHINA River WWTP, water 0.55− 1.2*10^6 mc/d n.a Confirmation of WWTPs as source
sediment No significant relation between MPs pollution in urban river and
the geographical location of the WWTPs
No evaluation of apportionment, if not based on concentration
15 CA River Water, sediments n.a n.a Confirmation of WWTPs as source
MPs concentration significantly higher downstream WWTPs than
upstream
No evaluation of apportionment, if not based on concentration
16 FR River WWTP, water, atm n.a n.a Confirmation of WWTPs as source
fallout MPs. A subsequent study deepened these aspects but focused only
on the fibers class.
No evaluation of apportionment, if not based on concentration
17 NL River, sea WWTP Water, 385− 30000 m3/h n.a Confirmation of WWTPs as source
sediments, biota Dry weather flow No evidence of dilution for effluent MPs, hence the presence of
many diffuse sources of MPs is suggested
No evaluation of apportionment, if not based on concentration

Ref. 1 [29], 2 [40], 3 [103], 4 [104], 5 [105], 6 [106], 7 [107], 8 [108], 9 [109], 10 [47], 11 [44], 12 [30], 13 [110], 14 [111], 15 [112], 16 [113], 17 [114] n.a not
available.

9
M. Barchiesi et al. Journal of Water Process Engineering xxx (xxxx) xxx

from an environmental management point of view, are different ac­ interventions. Elements added to the systems are mainly the water
cording to the relative flow of the effluent. From a local point of view, supply chain and the water sanitation systems, including stormwater
this is of paramount importance to establish where to direct the efforts in management. In this review, the information on MPs in the main sec­
reducing MPs pollutions and their possible outcome. Moreover, if the tions of the urban water cycle have been examined and, in this section,
concentration of MPs in the water body is always reported, that is not the the main conclusions are summed up for a complete overview.
same for WWTPs volume discharge and river flow, which instead is Regarding the water supply chain, MPs have been extensively found in
needed for a proper evaluation of relative contribution to MPs pollution. surface waters and have been fully characterized in terms of size, colour,
MPs concentration is indeed the key parameter for toxicology and risk shape and chemical constituents. However, the determination of sour­
analysis, but it is not enough for the beginning of MPs pollution control ces, their relative contribution and the influence of the socio-economic
strategy. factors and hydrological features of the catchments, remain a local in­
Gaining the information on WWTPs effluent characterization in formation due to the absence of analytical protocol standardization,
terms of MPs seems not to suffice to a proper source apportionment and lacking anyhow in quantification and certainty. Groundwater sources
relative role evaluation either. Indeed, as shown in the records 10–17 of have been instead less explored, though the few information available
Table 5, main apportionment strategy is still based on concentration confirm their pollution due to also MPs. The water supply chain is
difference. The analysis of the WWTP effluent is indeed mostly used only supposed to be responsible of MPs contamination to a certain extent, but
to confirm the MPs source and not to establish more definite certainties more tests are needed to generalize such an assessment. Drinking water
on relative contribution. treatment plants remove MPs with different results depending on plant
Moreover, another relevant aspect linked to WWTPs role in MPs layout and water sources, though the evidences are once again too scant
pollution is the possible change not only in MPs concentration but also in to generalize. The influence of operational parameters on the removal
MPs characteristics distribution. Size, shapes, colour and chemical efficiency of the various units is still mostly unknown. Presence of MPs
composition are indeed all factors influencing the biota uptake [115, in drinking water and beverages have been extensively demonstrated,
116]. though the effects of their ingestion by humans are still to be under­
Indeed, some studies noticed even statistically significant changes in stood. Used water ending up in the wastewater collecting systems are
distribution between upstream and downstream sections to WWTPs enriched in MPs by households and industries; moreover, stormwaters
[108,109]. Moreover, Grbić et al. [44] using nMDS (non-metric multi­ have been proved to be contaminated by secondary MPs of various
dimensional scaling) plots found non-existent grouping based on genera, such as from tires wear. Influent to wastewater treatments are
chemical classification, while for categories and colour/categories the indeed confirmed to be heavily polluted by MPs, while time related
lake surface MPs pollution grouped first with agricultural runoff and patterns and MPs distribution characteristics need more research.
next with stormwater runoff. Instead, Baldwin et al. [107] observed that Wastewater treatment plants have been extensively studied in regard to
no plastic types were correlated with the WWTPs effluent contribution MPs, but still not enough information have been gathered on the influ­
to the streamflow. Hylton and Ghezzi [106] noticed no effects of WWTPs ence of operational parameters, processes influencing MPs removal and
on particle types (or abundance) and Lin et al. [111] did not observed distribution, effect of the treatment on MPs fragmentation; this scarce
influence of WWTPs geographical location on MPs pollution. knowledge is still due to the ever-present lack of method standardiza­
Worth mentioning is also the study by Uurasjärvi et al. [117] where tion. MPs have been recorded also in WWTPs effluents and sludge and
proximity, taxonomy and chemical characterization were investigated are hence spread into the environment through sludge application in
in a northern European lake. They found the highest amount of MPs agriculture, water reuse for irrigation and water discharge in the
close to the effluent of a WWTP and with the typical characteristics of receiving waterbody, hence possibly back to a water source. Moreover,
synthetic clothes release [117]. Colours and chemical composition were also the atmospheric compartment has been checked positively for MPs
considered determinant to attribute the origin of fibers to fishing nets pollution, becoming another source due to deposition and fallout.
and ropes by Migwi et al. [35] in lake Naivasha. A mention is also to be Considering the whole cycle, MPs can be therefore considered
given to studies like the one by Zhang et al. [32] where the WWTPs ubiquitous. The MPs presence in the water cycle cannot be defined as
effluent was thoughtfully characterized; however, there was no analysis “closed”. New MPs are indeed steadily introduced and formed in the
of upstream sections and hence the data were used only for an evalua­ system. The continuous feed by human activities, specifically by urban
tion of daily discharges as a confirmation of WWTPs as source. areas and industries is indeed confirmed, even if its relative contribution
In conclusions, WWTPs are undoubtfully a source of MPs to fresh­ to an already polluted environment is not easily accounted. Fragmen­
waters systems, their relevance though is highly locally dependent. MPs tation is also another source of MPs generation within the cycle,
concentration is the key parameter for the related environmental risk occurring both in natural environments and anthropic, e.g. in the water
assessment, and hence rightfully the factor mostly studied; however, to treatment plants. Atmospheric deposition is now considered a signifi­
evaluate the better management solutions to the MPs pollution, the role cant reality and it is possible the resuspension of MPs from dry surfaces
of WWTPs in terms of relative loads has to be deepen more. It cannot or even from the water surface by wave breaking and bursting bubbles
also be overseen the possible changes in MPs distribution in the water­ [9]. Besides, it is likely the MPs sinking with sediments or circling within
body, linked to the WWTPs effluent discharge, considering the relevance the water bodies. Sediments are also possibly resuspended in rivers due
of factors such as shape, size and colour in biota uptake. to flow regime changes, but ultimately MPs will end up trapped on the
bottom floor elsewhere or fragmented in the tiniest pieces. Indeed, for
6. MPs in the urban water cycle example, deep sea sediments might be considered as a sink for MPs
[119], but according to MPs characteristics and from what seen so far,
The hydrological water cycle is defined as “a conceptual model the same might stand for both river beds and lakes bottom. It is also
describing the storage and circulation of water between the biosphere, at­ confirmed the accumulation of MPs in soils treated with WWTPs sludge,
mosphere, lithosphere and the hydrosphere” [118]. Storage compartments with eventually a further transportation elsewhere by runoff. MPs
are the atmosphere, oceans, lakes, rivers, streams, soils, glaciers, pollution is pervasive, always introduced and generated within the
snowfields and groundwater aquifers. Processes leading to circulation cycle, with effects on each compartment due to transport processes, both
are: evapotranspiration, condensation, precipitation, infiltration, natural or modified by the anthropic manufactures (e.g. those present in
percolation, snowmelt and runoff, also called the “water cycle compo­ urban areas, water supply chain, wastewater collecting systems and
nents” [118]. All the components and storage compartments are present water treatment plants included): it is clear how, to be properly
in the urban water cycle but modified in their relative effect by urban­ addressed, it needs to be considered in its whole and not as a phenom­
ization; complexity is added to the hydrological cycle by anthropogenic enon restricted to separated sections. To do so, coherent description of

10
M. Barchiesi et al. Journal of Water Process Engineering xxx (xxxx) xxx

MPs among the different compartments is needed. An interesting start­ interests or personal relationships that could have appeared to influence
ing point in such a direction could be the approach designed by Kooi the work reported in this paper.
et al. [120] where MPs are described by a 3D continuous probability
distribution, with size, density and shape as dimensions. Description of Appendix A. Supplementary data
MPs by continuous values while depicting simultaneously the three
main attributes (shape, size, density) allows indeed the representation of Supplementary material related to this article can be found, in the
the true complexity of the objects [120]. Moreover, the definition of online version, at doi:https://doi.org/10.1016/j.jwpe.2020.101787.
shapes based on the Corey shape factor reduces the uncertainties in
classifications [120]. Furthermore, this approach, by exploiting the
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