Chemical Engineering Journal 414 (2021) 128692

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Chemical Engineering Journal

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Engineered technologies for the separation and degradation of

microplastics in water: A review
Oscar M. Rodríguez-Narvaez a, Ashantha Goonetilleke b, Leonidas Perez c, d, Erick R. Bandala e, *
a
Departamento de Química, DCNE, Universidad de Guanajuato, Cerro de la Venada s/n, Pueblito de Rocha, Guanajuato C.P. 36040, Mexico
b
Queensland University of Technology (QUT), Brisbane, Australia
c
Plataforma Solar de Almeria, Spain
d
CIESOL, Joint Research Centre University of Almeria-CIEMAT, 04120 Almeria, Spain
e
Division of Hydrologic Sciences. Desert Research Institute. 755 E. Flamingo Road, Las Vegas, Nevada 89119-7363, USA

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

Keywords: In recent years, the presence of the group of contaminants, termed as microplastics (MPs) has been recognized as
Engineered MPs degradation significant water pollutants with considerable potential for exerting adverse impacts on human health and
Engineered MPs separation wildlife. Natural attenuation has practically no effect while conventional treatment processes are not capable of
Water treatment
entirely removing MPs which are reported to accumulate in the environment, in organisms in the aquatic food
web and, potentially reaching humans. This in-depth review critically evaluates the state-of-the-art engineered
technologies suitable for the separation and degradation of microplastics in water with potential for real-scale
application. The outcomes of the review confirmed that very limited number of studies are reported in this
field, the majority from recent years and have focused on using phase-changing processes, including coagulation-
flocculation, flotation, and membrane processes. A few other studies have reported the use of chemical or bio­
logical digestion, and even fewer, engineered removal using biodegradation, wet oxidation, and advanced
oxidation processes. This paper focuses on the type of MPs being removed, the process conditions and the
outcomes reported in research literature. The emerging trends in the field are also highlighted as well as the
identification of current knowledge gaps and future research directions along with perceptive comments and
recommendations related to the application of available technologies for water treatment.

1. Introduction
Microplastics (MPs) are plastic fragments smaller than 5 mm in any
dimension without a specific lower limit [1] which are reported being
accumulated throughout all ecosystems, including in pristine environ­
ments such as Antarctica, remote mountain-tops, and the deep ocean
floor supposedly free from human impact [2]. After the first acknowl­
edgement in early 2000′ s, MPs presence in the environment have raised
ever increasing concerns because of the little known impacts these
particles may have on living organisms, ecosystems [3] and because of
the magnitude of the problem, as approx. 1.5 million tonnes of MPs are
estimated to be released into aquatic environments every year [1].
The identified primary sources of MPs are commercial products such
as face cleansers, drilling fluids, 3D printing products, pharmaceutical
vectors, and industrial abrasives, which contain particles referred to as
primary MPs. Primary MPs are defined as MPs manufactured to a
microsize [4]. The other significant source of MPs is from the degrada­
tion of larger plastic debris by mechanical, chemical, or biological
processes, generating secondary MPs [5]. Both, primary and secondary
MPs have been reported as persistent, potentially toxic pollutants
entering marine and freshwater environments with significant potential
to become a global ecological and environmental hazard [6-10]. The
toxic properties of microplastics is due to the fact that various chemical
compounds are either added as additives to achieve desirable properties
during manufacture or adsorbed from the surrounding environment.
Additionally, MPs have been reported capable of adsorbing organic
contaminants from water (e.g., emerging contaminants) and their
transport to different ecosystems. Consequently, subjected to physical
and chemical processes such as desorption and aging, the adsorbed
organic contaminants can be released back into the environment, pro­
moting the presence of unexpected complex mixtures of organic con­
taminants even in sites otherwise considered as pristine [11,12].

* Corresponding author.
E-mail address: erick.bandala@dri.edu (E.R. Bandala).

https://doi.org/10.1016/j.cej.2021.128692
Received 12 May 2020; Received in revised form 11 January 2021; Accepted 21 January 2021
Available online 27 January 2021
1385-8947/© 2021 Elsevier B.V. All rights reserved.
O.M. Rodríguez-Narvaez et al. Chemical Engineering Journal 414 (2021) 128692

Further, their hydrophobic surfaces act as habitat for microbial coloni­ Table 1
zation [13]. Unfortunately, very little is known about the engineered MPs sources in water environments.
separation, and/or the application of degradation technologies for the MP type Source Receiving Reference Main findings
removal of this highly ubiquitous contaminant [14-22]. matrix
The primary aim of this review was to critically evaluate the state-of- Primary Sewage Freshwater [23] Over 112 million MP
the-art in relation to currently available engineered separation, and effluent particles (60–70 µm
degradation technologies being used in practical applications or labo­ cosmetic microbeads)
ratory methods with the potential for successful full-scale application, were estimated to be
released daily into
particularly in freshwater, as well as to identify current knowledge gaps the receiving water
and to provide recommendations for further research. bodies
Secondary Sewage Freshwater [24] MPs were measured
2. Main sources of MPs in aquatic ecosystems effluent before and after the
release of effluent
from six wastewater
The majority of scientific studies on the presence of MPs in aquatic treatment plants.
ecosystems are primarily in relation to marine environments. This re­ Other sources were
view has specifically focused on freshwater ecosystems because of the also found to be
involved
increasing interest in the separation and degradation of MPs, in order to
Secondary Sewage Freshwater [25] MPs (53–105 µm size
mitigate the undesirable consequences to human health. Table 1 lists effluent range) were found
recent studies on the main sources of MPs in freshwater. As evident, ranging from 0.79 to
wastewater effluent is the major source of MPs to water environments 1.56 mg L− 1
[23-25], followed by agricultural runoff [26,27], and other non-point Secondary Agricultural Freshwater [26] MPs in the range of
runoff 320–480 items m− 3
sources [28,29] as illustrated in Fig. 1. Wastewater is particularly con­
were found in lake
cerning because of its potential to not only contribute secondary MPs, water
but also primary MPs commonly generated from synthetic textiles and Secondary Agricultural Freshwater [27] MPs ranging from 34
cosmetic products [23,30-33]. runoff to 10 particles < 0.5
mm L− 1 were found
The primary source of discharge of MPs into freshwater is via
in water
wastewater treatment plant (WWTP) effluent [35]. Despite the fact that Secondary Urban runoff Freshwater [29] 36 sites in 29
the removal rate of MPs in a conventional wastewater treatment plant is Japanese rivers were
reported to be in the range of 73% to 79%, the treated effluent on tested for MPs. MPs
average carries as much as 220,000–1.5 million MP particles per day were found in 31 of
the 36 sites,
[35]. Application of simple mass balance to the wastewater treatment
correlated with
process suggest a significant amount of MPs remaining in the waste­ urbanization and
water or being transferred to sludge during WWTP operations as illus­ population density
trated in Fig. 2. Secondary Food waste Freshwater [48] The use of MP
There is limited information available on the influence of anthro­ surveys as surrogate
for MP analysis
pogenic activities or population characteristics on the type and load of discouraged
MPs present in wastewater effluent and/or waste sludge. Studies have Secondary Urban runoff Freshwater [49] MPs concentration
reported a wide variety of shapes, sizes, and chemical characteristics of was higher in
MPs, which is influenced by their source, and how these characteristics freshwater (1.8–2.4
items L− 1) compared
will affect their mobility in the environment and exert potential adverse
to coastal water (0.9
impacts on human and ecosystem health [37-40]. Therefore, it is chal­ items L− 1)
lenging to standardize MP particles found in aquatic environments and Secondary Sewage Freshwater [50] Increase in MPs was
is a significant limitation in current research in this area. Some recent effluent found upstream/
studies suggest a possible correlation between the spatial and temporal downstream of
sewage effluent
distribution of MPs and specific population dynamics [41]. However, release
the potential consequences arising from the presence of MPs in storm­ Secondary Household/ Freshwater [51] Land use did not
water [42,43], compost [37,40], or mobility in soils after successive industrial influence MPs
sludge application remains mostly unknown [44]. This lack of in-depth wastewater concentration in
water
knowledge is a significant constraint for the formulation of effective
Secondary Sewage Freshwater [52] 0.57 MPs particles/L
management strategies for the mitigation of MP pollution. Hence, this effluent were found in river
can be considered as an important knowledge gap which merits further water
investigation. Recent studies also suggests that correlations exist be­ Primary Synthetic Wastewater [30] Synthetic textiles
tween the spatial and temporal distribution of MPs and factors such as textiles microfibers ranged
from 175 to 560
population density, total investment in fixed assets, and the extent of microfibers g− 1 found
forested land [41]. Nevertheless, multiple limitations (e.g., small sam­ Primary Synthetic Wastewater [31,32] 6 million fibers
pling volumes, presence of potential bias in extraction and quantifica­ textiles released from 5 kg
tion methods) are cited by researchers calling for further investigations wash of polyester
fabric
before robust conclusions can be derived about the correlation between
Secondary Synthetic Wastewater [33] Correlation between
the spatial and temporal distribution of MPs and the above noted factors. textiles detergent addition
It is clear that further systematic studies regarding the spatial and and fibers released
temporal distribution of MPs and the role of wastewater treatment Secondary Sewage Wastewater [35] Raw wastewater:
process parameters on MPs concentration are needed. This requires effluent 1–6.5 million MPs/
day; effluent: 220 K-
controlled experiments where some variables can be maintained un­ 1.5 million MPs per
changed in order to observe the influence of potential key parameters, day
making this an important research opportunity. (continued on next page)
Studying the role of WWTP operations on the distribution of MPs in

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O.M. Rodríguez-Narvaez et al. Chemical Engineering Journal 414 (2021) 128692

Table 1 (continued ) removal. This is in agreement with other studies where the effectiveness
MP type Source Receiving Reference Main findings of the WWTP in the removal of MPs could be correlated with the
matrix chemical composition of the particles. For example, Talvite et al. [47]
Secondary Sewage Wastewater [46] MPs > 500 µm were
reported that, in general, polyethylene (PE) and polypropylene (PP)
effluent found, no microbeads microbeads are removed more easily compared to polystyrene (PS) and
Primary Synthetic Wastewater [53] Polyester MPs (<7K polyester (PES) microfibers, which have been noted as among the most
textiles fibers m− 2 L− 1) found difficult MPs to remove, which could be attributed to their relatively
to be higher than
lower exposed area, and higher mobility compared to microbeads. These
other fabrics
Primary Synthetic Wastewater [54,55] Cotton and rayon authors [47] tested the efficacy for the removal of MPs of different
textiles microfibers degrade, wastewater treatment processes, including disc filters, rapid sand filters,
polyester persisted dissolved air flotation, and membrane bioreactors. It was found that the
Secondary Urban debris Stormwater [56] 10–2000 µM MPs shape of the MPs exerts a significant influence in terms of removal ef­
ranging from 490 to
22,894 items m− 3
ficiency depending on the wastewater treatment process. For example,
found in stormwater microfibers pass through the final-stage treatment relatively more easily
ponds compared to microbeads because of the relatively small size and
morphology [47].
The nature of the MPs has also been suggested to play a significant
wastewater effluent and/or sludge is another robust approach to assess
role in the removal efficiency, with primary MPs being more effectively
the transport and fate of these particles in freshwater ecosystems.
removed compared to secondary MPs, because the former is usually
Depending on the quality of the raw wastewater, different treatment
shaped as microbeads while the latter is most likely to be textile fibers or
processes are employed to produce effluent suitable for compliance with
other debris. Despite these encouraging results, relatively little infor­
the applicable local, regional, or national regulations. Past researchers
mation is available on the efficiency of wastewater treatment (conven­
have suggested that the concentration and diversity in the types of MPs
tional and advanced) in the removal of MPs and its correlation with the
in wastewater effluent after treatment can be correlated with the water
specific characteristics of the MP particles (morphotype and nature of its
treatment processes employed [45]. This in turn, could be correlated
polymeric origin), the volume of wastewater treated, and variations in
with the presence of these particles in the influent into the treatment
the MPs load. This is another important knowledge gap which merits
plant [46]. Lv et al. [46] found significant differences among different
significant attention because it will contribute to advancing research
wastewater treatment processes in relation to the efficacy of MPs

Fig. 1. Main sources of microplastics in freshwater (modified from [34]).

3
O.M. Rodríguez-Narvaez et al.
Fig. 2. Estimated MP particle flow in a typical wastewater treatment plant (modified from [36]).
with a focus on identifying simple, but effective ways to design waste­
water treatment processes to further enhance the removal of MPs within
a treatment plant and, consequently, prevent further distribution into
aquatic ecosystems.
3. Engineered MPs separation processes
Once released into a freshwater resource used for potable con­
sumption, MPs possess characteristics that cause major problems in
drinking water treatment processes. For example, Enfrin et al. [57] re­
ported significant fouling of ultrafiltration membranes due to pore
blockage by MPs in the size range between 13 to 690 nm after 48 h of
operation at 1 bar pressure. The researchers also found a permeate water
flux reduction up to 38% and over 25% of the MPs initially present in the
feed were absorbed to the membrane surface within 48 h of filtration. In
another study, Li et al. [58] applied feed water with polyvinylchloride
(PVC) particles (10 particles L-1) into a membrane bioreactor to simu­
late polluted surface water. They found MBR was effective in treating
organic matter and ammonia with removal rates of over 80% and 95%,
respectively. The removal performance, however, was immediately
inhibited when the PVC MPs was added to the membrane bioreactor.
The application of membrane treatment was also tested for the
separation of MPs in landfill leachate [59] with researchers reporting a
significant reduction of MPs loading. Differences in the distribution of
polymeric materials at different sampling locations and the presence of
membrane-related polymer in membrane treated effluent was also
observed suggesting the generation and release of MPs particles from the
system. Similar results have been also confirmed by Ding et al. [60] for
drinking water treatment plants using membrane filtration. These re­
searchers found that chemical cleaning can cause aging and breakage of
organic membranes, and MPs may be released in long-running drinking
water treatment plants. Nevertheless, MPs are not the only reason for
severe fouling of membrane processes, but other water constituents can
also play a significant role. For example, Li et al. [61] studied ultrafil­
tration (UF) membrane fouling by MPs and found that particles of
average size 1 µm caused the most severe fouling among the investigated
sizes, but they also identified a synergistic effect between MPs and other
compounds in raw water. Consequently, the need for more in-depth
analysis of the efficacy of membrane processes for the removal of MPs,
4
Chemical Engineering Journal 414 (2021) 128692
their limitations, challenges posed, and the effects caused by other water
quality parameters remains to be investigated. The current limited un­
derstanding provides another interesting knowledge gap worth
exploration.
Freshwater input into drinking water treatment facilities are sus­
pected as a potential exposure source to humans. However, only a very
limited number of studies have investigated this phenomenon [62].
Among the limited studies available, researchers have identified the
presence of MPs as small as 20 µm and investigated the effectiveness of
conventional water treatment processes (e.g., coagulation, flocculation,
clarification, and filtration) in their removal. Mintenig et al. [62] found
a significant decrease in MPs numbers in the treated water compared to
raw water. However, no information has been provided on the treatment
process/es responsible for the removal, nor the relationship between the
type/s of MPs and their removal in the water treatment process. In
another study, Li et al. [63] found significant membrane bioreactor
fouling when polyvinylchloride (PVC) particles where added to the raw
water. The researchers found that the membrane bioreactor (MBR) to be
highly efficient for organic matter and ammonia removal (85% and
95%, respectively) in raw water. However, when MPs were added to the
raw water at concentration as low as 10 particles L− 1, organic matter
and ammonia removal was immediately inhibited, indicating that MPs
contamination led to irreversible membrane fouling.
3.1. Coagulation-flocculation/flotation
Separating MPs from liquid matrices is the initial approach that past
researchers have adopted [64,65]. However, this can be a complex
process because of the wide range of feedstock, possessing a diversity of
chemical and physical characteristics [4,66,67]. A number of MP sepa­
ration methods have been developed over the years, including filtration,
sieving, filtration using activated carbon, among others [3,53,68,69].
Some of these methods (e.g., filtration and sieving) are mostly used as
pre-treatment for MPs quantification [35,48,52,70]. However, despite
their potential, very few studies have been reported on their use as
engineered processes for MPs separation [47].
Most commonly used engineered separation methods for MPs
include coagulation-flocculation/flotation (C-F/F). The C-F/F process is
based on solid/liquid heterogeneous separation, which largely depends
O.M. Rodríguez-Narvaez et al. Chemical Engineering Journal 414 (2021) 128692

on fluid and solid density [71,72]. Table 2 shows the different C-F/F and
related separation methods used for the removal of MPs in freshwater
with potential for full scale application [73-75]. Among these, density
separation has been used in the past at laboratory scale, but without any
approaches for scale-up reported in research literature. Probably, this
could be due to the high treatment cost associated with the need for
electrolyte addition [76]. Application of scaled-up density separation
methods without electrolyte addition has also been reported in research
literature, but only when a coagulation-flocculation process is used as
pretreatment (Table 2). As evident in Table 2, chemical and
electrochemically-based coagulation-flocculation processes used for
MPs removal have shown significant removal efficiency [77,78]. How­
ever, it is important to note that density separation may not always be
effective as the density of MPs can vary with time due to microbial
growth on the surface. Consequently, the effectiveness of various elec­
trolytes can be questionable [79].
In chemical coagulation-flocculation, several coagulant types has
been widely reported for the removal of organic and inorganic con­
taminants commonly present in water [80,81]. However, only FeCl3,
AlCl3 and a few polymers have been reported for MPs removal, along
with a wide range of doses to achieve high removal efficiencies
[15,77,82,83]. Considering the variety of coagulant products available
in the market for full scale application, this lack of knowledge on their
efficacy in relation to the removal of MPs in freshwater represents a
significant knowledge gap.
The potential use of plant-based coagulants such as gums and ex­
tracts is another important avenue for investigation for possible appli­
cation for scale-up of the coagulation-flocculation approach. However, it
is not possible to locate studies on the application of widely known
plant-based coagulants such as Nimali warnasakera seeds, Moringa olei­
fera seeds, or cactus gum, for MPs removal as evident in Table 2. This is
despite their reported high efficiency for the removal of organic and
inorganic contaminant in water [84-87].
Table 2 shows that only one single study has reported on the use of
electrocoagulation (EC) for MPs separation [78]. The use of EC has
proven to be highly efficient in the removal of different contaminants
even in highly complex wastewater matrices [89]. However, in the
application for the separation of MPs in water, a significant amount of
knowledge is not available. For example, aluminum and iron electrodes
have been commonly used and their effect on the EC process is well
known [89]. However, there is no clear understanding of how electrode
materials can influence MPs separation. The lack of research on the
mechanisms involved in the C-F/F processes for MPs separation in water
is another significant knowledge gap which needs to be bridged. An
improved understanding would enable optimizing the separation pro­
cess in order to achieve enhanced outcomes. Further, no systematic
information on the physical and/or chemical characterization of the
sludge/foam produced after the C-F/F processes based on the applica­
tion of advanced analytical instrumentation such as X-ray powder
diffraction and FTIR are available in research literature. The availability
of such information would enable an enhanced understanding of the
changes in the characteristics of the MPs removed, such as their inter­
action with ions released from the electrodes, and the potential changes
to their mobility as a result. Additionally, mass balance information is
not available in relation to the final fate of MPs subsequent to the C-F/F
process to understand whether MPs are trapped in the floc produced and
dragged down to the sludge layer or form part of the foam layer at the
top of the reactor. This knowledge would be invaluable for optimizing
the removal process to achieve enhanced outcomes.
3.2. Biological and chemical digestion
Separation of MPs in water has also been performed using two pri­
mary methods, namely, biological and chemical digestion. Some studies
have promoted biological digestion (BD) as a highly efficient method for
MPs separation. However, most studies in this area have not presented a
systematic approach and/or included information about process effi­
ciency in relation to the separation of different types of MPs. Commonly,
results in relation to the overall MPs separation is provided [16,90-95].
A detailed understanding of the separation of individual species of MPs
is important as the inherent toxicity varies with the different types and
chemical composition, and in turn, the assessment of risk associated
with the presence of MPs in water. Several significant knowledge gaps
can be identified in relation to the use of BD methods for MPs separation.
For example, the application of BD has been primarily demonstrated for
MPs separation at laboratory scale with density separation using a ma­
trix with high electrolyte concentration. This means that there is a need
for a secondary process for MPs degradation [96-98].
Table 3 lists studies where systematic research had been undertaken
to develop digestion methods for MPs separation. Scherer et al. [94]
reported the use of different invertebrates (such as Daphnia magna,
Chironomus riparius, Physella acuta, Gammarus pulex and Lumbriculus
variegatus) for MPs separation. The researchers found that the optimal
separation was achieved by Daphnia magna (DP) when the MP particle
size is (i.e., <10 µm) small, while the other invertebrates preferred
larger particle sizes of MPs (i.e., >90 µm). Nevertheless, despite the fact
that the above noted study tested the effect of different abiotic and biotic
factors (e.g., temperature, presence of natural particles) on the separa­
tion process, no information was included about the potential for
scaling-up. This is identified as a significant knowledge gap because of
the innovation arising from the use of invertebrates for MPs ingestion.
The most frequently reported chemical digestion (CD) process is wet

Table 2
MPs separation by coagulation-flocculation/flotation.
Treatment MP type Matrix Removal, MPs characteristics Process highlights Reference
%

Electrocoagulation Polyethylene (PE) Synthetic 90–99 MP dia.:10 mm; [PE] 0.1 Filter pore size 0.33 µm; EC coupled with Al electrodes; [78]
wastewater g L− 1 [NaCl] 2–10 g L− 1; pH 3–10; J 11–23 A m− 2; 60 min;
settling 16 h
Coagulation PE Deionized 0–60 MP dia.: <0.5 mm–>5 Filter pore 100 kDa; 0.15 MPa; [NaCl] 10 mM; pH 6–8; [15]
water (DI) mm; [PE] 0.33 g L− 1 [FeCl3⋅H2O] 0–5 mM; [AlCl3⋅H2O] 0–15 mM;1 min @ 300
rpm; 14 min @ 100 rpm; settling time 30 min
Coagulation PE DI 0–90 MP dia.: <0.5 mm–>5 Filter size 100 kDa; 0.15 MPa; pH: 6–8;[FeCl3⋅H2O] 0–5 [77]
mm; [PE] 0.33 g L− 1 mM; 1 min @ 300 rpm; 14 min @ 100 rpm; 30 min settling
Coagulation PE Raw water 90–100 [PE]: 5 mg L− 1 Alum concentration 5–10 mg L− 1 [88]
Density separation PE,PS, polyvinyl Wastewater 6.7–87 Particle size range Wastewater dried at 60◦ C; KHCO3 150 mL; Settling over [73]
chloride (PVC) 0.65–6.7 mm night
Density separation Polystyrene (PS) DI 20–100 Particle size range [ZnCl2] 5.64 M; settling time 48 h [74]
0.05–100 µm; [PS]
50–500 mg L− 1
Density separation PE, PS, Riverbank 30–100 [MPs] 367.7 g L− 1 [NaCl]@ saturation; shake time 1 min; settling time 24 h; [75]
polypropylene (PP) filter diameter 11 µm; dry at room temperature

5
O.M. Rodríguez-Narvaez et al. Chemical Engineering Journal 414 (2021) 128692

Table 3 3.3. Other MP separation methods

MPs separation by biological and chemical digestion.
Digestion Digester MP type Removal, Process Reference Table 4 lists other non-conventional treatment methods investigated
process % highlights for MPs separation in water. Among these, magnetic removal appears to
type be a highly attractive approach based on the addition of iron-based
Biological Range of PS 1–100 PS size [94] magnetic nanoparticles to the water sample, which will trap the MPs
microbial 1–90 µM; and then the mixed particles can be separated using a magnetic field
strains [PE] [105]. However, as noted by Grbic et al. [105], the use of magnetic
3–3000
particles
nanoparticles may not be useful in the case of some MP types. Chemical
mL− 1; 60 and physical properties of the MPs play a significant role in the ability to
min; attach magnetic nanoparticles. The separation capacity of the method
ingestion depends significantly on the linkage between the magnetic nano­
rate rage
particles and MPs. Grbic et al. [105] also hypothesized that the viscous
8–6180
particles coating of the magnetic nanoparticle surface could attach these nano­
h− 1 particles to MPs and enable subsequent recovery from water. However,
Chemical Wet PE,PS, PVC 50–100 [H2O2] [73] no experimental evidence was included in the study supporting this
peroxide 30% (v/ hypothesis.
oxidation v); 30
min; 75◦
Unfortunately, very limited knowledge is available on the applica­
C; particle tion of magnetic separation of MPs. This constitutes a significant
size range knowledge gap which merits further investigation. For example, using
0.65–6.7 other metallic nanoparticles (e.g., silver and copper) or bimetallic
mm
nanoparticles (e.g., cobalt- and copper-ferrites) which can attach to the
Chemical Alkaline PE, PS, PVC 6.7–100 [KOH] [73]
digestion 10%(v/ MPs instead of iron nanoparticles may allow some improvement in the
v); efficiency of the process and enhance its applicability at full scale.
sample/ However, the use of metallic nanoparticles may represent a potential
KOH ratio constraint if human and/or ecosystem health risks are present in the
1:10; 48
context of the release of the nanoparticles to the environment. There­
h; 40 ◦ C;
particle fore, as part of the investigation of nanotechnology applications, ethical
size range and social implications and public acceptance as well as risk minimi­
0.65–6.7 zation also needs to be taken into consideration along with the search for
mm
effective methodologies [106].
Chemical Fe2+/ PE,PS,PP, 47–96 PE size [104]
H2O2 polyethylene range Electrostatic separation, which entails the separation of particles by
terephthalate 0.85–0.5 mass using a low energy charged beam, is another non-conventional
(PET) mm; PET MPs separation technology which takes advantage of electromagnetic
size range properties. In this case, water containing MPs pass through different
0.32–0.4
electrostatic fields and are attracted to different containers depending
mm; pH 3;
[H2O2] on the surface characteristics [107]. Electrostatic separation technology
30% (v/ has been shown to apply not only to separate MPs in different matrices
v); [Fe2+] (e.g., solid or liquid), but also being able to separate MPs by type, which
0.07 M
is important for particle degradation. However, relatively very limited
information is available on the key aspects of this process. For example,
oxidation (Table 3), where organic matter is degraded at high temper­ the specific electrostatic field required for the removal of different MPs
ature and pressure in the presence of an oxidant [99-101]. All of these types has not been conclusively identified. It is clear that extensive
studies have used low oxidant concentration (i.e., <30% v/v), as well as research is required on the application of electrostatic separation of MPs
acidic- and/or basic-solution to avoid MPs degradation or modification in water, including the identification of advantages and limitations as
as the CD process was considered as a pre-treatment in experimental well as the feasibility for full scale application.
studies for the quantification of MPs in environmental samples. How­ Pressurized fluid extraction (PFE), which refers to the extraction of
ever, hydrothermal processes such as wet oxidation have been found to water in the presence of dissolved contaminants using a solvent at high
be highly effective for the dissolution of organic solids and the break­ temperature and pressure, is a technology which has been investigated
down of dissolved organics, with noteworthy potential for full scale in depth [108-110]. Fuller and Gautam [111] reported on the applica­
application in sewage sludge degradation [102]. Avoiding MPs degra­ tion of PFE for MPs separation (see Table 4), suggesting that this tech­
dation or modification should not be a restriction on the application of nology can be effective for MPs removal. Nevertheless, the application of
CD processes in field applications. Having a single treatment process PFE technology for MPs separation has barely been reported in research
which can separate and destroy MPs would prove to be an attractive literature. In this regard, several knowledge gaps can be identified
technology. Unfortunately, it was not possible to locate any studies on including the need to explain how the polarity of the carrier phase will
the application of CD or related processes for MPs separation and affect MPs separation efficiency. This is because, same as noted for
degradation. This lack of information about the potential of wet oxida­ magnetic separation technologies, different MP types possess different
tion not just for full scale separation of MPs, but also for their degra­ surface characteristics. Therefore, using only one carrier polarity may
dation in water or sludge is also identified as a key knowledge gap. This imply that some MPs will not be separated. However, this may also have
merits further exploration as a cost-effective, non-selective treatment its advantages as MPs can be separated selectively, where the most toxic
technology possessing significant potential in the removal of pollutants species can be targeted. Further, temperature and pressure within the
either at high or low concentrations [103]. Chemical digestion would be PFE system are significant variables potentially affecting the process
preferable to BD because it is rapid, and processes such as wet oxidation performance because, depending on the conditions tested, temperature
or other similar methods using high oxidant concentration, tempera­ and pressure may trigger physical and/or chemical modification of the
tures and/or pressure could be a feasible approach to destroy MPs. MP particles. This in turn, can affect the mechanisms involved in MPs
attraction to the PFE bed. Exploring PFE process for MPs separation is

6
O.M. Rodríguez-Narvaez et al.
Table 4
MPs separation using other technologies.
Separation technology MP type Matrix
Magnetic PE,PET,PS, PVC Benthic
organisms
Electrostatic PET,PP,PS,PVC Different
Pressurized fluid PS, high density Wastewater
extraction (PFE) polyethylene (HDPE)
another potential research area which merits further investigation.
4. Engineered technologies for MPs degradation
Very limited number of studies on engineered MPs degradation
technologies are available in research literature (Fig. 3). Based on the
results presented in Table 5, it is evident that a significant knowledge
gap is the lack of robust comparison of the outcomes presented in the
small number of studies reported. In most of these studies, changes in the
physical and/or chemical characteristics using advanced instrumenta­
tion such as XRD, SEM and FTIR have not been reported. The analysis of
any changes to the MPs surface could be used as evidence of the process
effect on the different MPs species investigated [5,112-114]. However,
this methodological approach involves significant challenges because
the observed physical and/or chemical changes can occur not only due
to the application of the degradation process, but also due to the variable
MPs characteristics depending their polymeric origin. A robust approach
for comparison can be the indirect estimation of MPs degradation which
could be obtained by measuring the amount being released into solution.
For example, the analysis of the chemical oxygen demand (COD) and/or
total organic carbon (TOC) concentration in solution can reflect the
Fig. 3. Engineered degradation technologies of microplastics.
Chemical Engineering Journal 414 (2021) 128692
Removal, Process highlights Reference
%
49–90 Synthetic freshwater; particle size range 0.2–1 mm; [Fe] 10 mg L− 1; 200 [105]
mL; [MPs] = 5–10 pieces L− 1
90 –100 10 pieces of each MPs; MP diameter 63–5000 µm;3 times pass; drum [107]
speed 66.5 rpm; electrode voltage 20 kV; 2 h
84–100 MPs size range 50 µm–1 mm; [MPs] 10–20 mg; 40 g of glass beds; [111]
60–200◦ C; 1,500 psi
release of MPs to the reaction mixture, which in turn can be compared
independently of the MPs type tested. Indirect analysis has been used by
past researchers, but only to estimate the generation of by-products after
MPs decomposition [115,116]. Its potential to quantify MPs decompo­
sition pathway is worthy of further investigation.
Photodegradation has been reported as the dominant environmental
process for the degradation of most plastics which occurs from exposure
to the combined ultraviolet (UV) and infrared fraction of solar radiation
[125]. Exposure to solar radiation will generate degradation and/or
modification of plastics (e.g., tensile strength reduction, C–H bonds
rupture, roughness increase and cracks and pores generation) mainly
through photo-oxidation processes [126]. However, the solar tempering
of plastics can also result in the transformation of some chemical com­
pounds used in the manufacture which could well lead to more toxic
compounds being released into the water [127]. Photo-oxidative
degradation of polymers (e.g., PE, PP, and nylon) exposed to the envi­
ronment usually begins with solar UV-A radiation (λ = 315–400 nm)
generating a photodegradation process where some chemical or physical
changes are achieved in the polymeric structure of the plastics
[126,128]. On the plastic surface, this deterioration can be observed by
pitting formation, crazing or cracking, discoloration, erosion, or
7
O.M. Rodríguez-Narvaez et al. Chemical Engineering Journal 414 (2021) 128692

Table 5
Engineered MPs degradation processes without radiation.
Degradation MP type Main results Process highlights Reference
process

Biodegradation PE 14.7% MPs weight loss; 22.8% particle diameter decrease 60 days;[MPs] 1% (w/v); Bacillus sp., Paenibacillus sp. [112]
Biodegradation PET 0.88–1.5% crystallinity increase; 0.2 –0.3 optical density [PET] 1 g L− 1; 48 h; pH 7, 12; [(NH4)6Mo7SO4⋅7H2O] 0.2 µg [116]
increase; 47– 78% diameter decrease; terephthalic acid L− 1;[H3BO3] 0.5 µg L− 1
production and degradation
Wet oxidation PSPE 0.30–0.75 carbonyl index increase; 0.20–0.25O/C ratio increase [K2S2O8]100 mM; [MPs] 25 g L− 1; 70 ◦ C; 30 days; pH 7 [114]
Fenton reaction PSPE 0.05–0.15 carbonyl index increase;0.10–0.15O/C ratio increase [H2O2] 9.9 mM;[Fe2+] 3 mM; [MPs] 25 g L− 1; 70 ◦ C; 30 days;
pH 4
Fenton reaction PE,PE, PVC No changes in functional groups observed by FTIR [FeSO4⋅7H2O] 3.33–10 mg mL− 1; pH 5; 1 mL of 30% H2O2; [5]
[MPs] 7 g L− 1
Electro-Fenton PVC 80% dechlorination Oxygen flow 40 mL min-1; TiO2/Graphite cathode; applied [117]
process potential − 0.7 V vs Ag/AgCl
UV irradiation LDPE 12.2– 68% tensile strength decrease; C–H bonds break; waviness 15 W; 1.8 mW cm− 2; λ 280–320 nm; 30–90 days; Lamp [118]
and roughness increase; cracks and pores generation; decreased distance 15 cm; [NaCl] 0.6, 0.017 M; 30 ◦ C
%C
UV radiation Different OH and C = O groups generation; cracks and flakes generation Simulated sunlight radiation; UV340 lamp; 30–90 days; lamp [113]
distance 30 cm;15 plastic pellets/petri dish;
Photocatalysis LDPE 0.71–1.49 carbonyl index increase; 0.51–1.35 vinyl index Platinum/Zinc oxide nanorods; 50 W; 175 h; Lamp distance [119]
increase 10 cm
Photocatalysis HDPE 6% mass loss N-TiO2; 27 W; λ 400–800 nm; 20 h; Lamp distance 12 cm; [120]
[HDPE] 2 g L− 1
Photocatalysis HDPE – 75% mass loss C, N-TiO2; 27 W; λ 400–800 nm; 50 h; Lamp distance 25 cm; [121]
[C,N-TiO2] 4 g L− 1;[HDPE] 4 g L− 1; pH 3–11; Temp. 0, 20 and
40 ◦ C
Photocatalysis PE 6% mass loss Hydroxy-rich ultrathin BiOCl; 250 W; λ 420 nm; 5 h; [BiOCl-X] [122]
1 g L− 1;[PE] 1 g L− 1
Photocatalysis HDPELDPE 4.65 and 1.8% mass loss of HDPE and LDPE, respectively N-TiO2; 50 h; Lamp distance 21.5 cm; [PE] 4 g L− 1; pH 3 [123]
Photocatalysis PP 65% volume reduction ZnO nanorods; 120 W; 60 mW cm− 2;Lamp distance 20 cm; [124]
456 h; flow 300 mL min− 1;[PP] 104 particles L− 1
Mg@NCNTs/PMS Different 5–50% weight loss; morphology modifications; functional pH 3, 7, 11;[MPs] 5–12 g L− 1;[PMS] 6.5 mM;[Mg@NCNTs] [115]
groups modification; by-products generation 0.1–0.3 g L− 1;
25-160◦ C; 8 h

embrittlement [113,118].
Table 5 lists selected studies reporting on the use of UV radiation (λ
= 280 − 320 nm) for MPs degradation. In these studies, significantly
long periods of UV irradiation were used to generate measurable
chemical and/or physical changes in MPs [113,118]. Further research is
needed to better understand the viability of the process, primarily
considering the feasibility of using long time periods of UV irradiation.
For example, there is no information available on the use of MPs
photooxidation where UV radiation is combined with high temperature
and/or pressure. It is possible that under appropriate temperature and
pressure conditions, MPs may become more vulnerable for attack by free
radicals (e.g., hydroxyl radical) and a faster MPs decomposition process
being achieved. Also, when UV-C radiation (λ = 255–280 nm) is used,
the higher energy involved would be expected to improve free radical
generation and MPs degradation, as it has been reported for the removal
of organic contaminants using UV-C radiation from synthetic and nat­
ural water samples [129,130]. An important research avenue worth
exploration is using UV radiation coupled with oxidants (e.g., hydrogen
peroxide, and persulfate) for MPs degradation. The UV/oxidant couple
has previously been reported with high efficiency for the degradation of
several organic contaminants in the aqueous phase [129,131]. For
example, when hydrogen peroxide (H2O2) is decomposed by UV radia­
tion, hydroxyl radicals (•OH) are produced which may be able to
accelerate MPs degradation. Also, if a higher power source is used for the
process (e.g., UV-C), UV radiation will be expected to not only decom­
pose MPs and H2O2, but also generate in-situ, a higher amount of hy­
droxyl radicals and improve MPs degradation [132,133]. However, to
the best of our knowledge, there no studies available on the application
of UV/H2O2 for MPs degradation, highlighting an important research
avenue worthy of further investigation.
As shown in Table 5, UV irradiation was not found to be an efficient
treatment process for MPs degradation. However, significantly better
results have been obtained using photocatalysis resulting in achieving
higher MPs mass loss compared to experiments without photocatalyst
[119-123]. Despite the encouraging results, only a limited number of
photocatalyst have been investigated for MPs degradation from the wide
variety reported in literature which have been used for other applica­
tions (e.g., carbon-based materials and metal oxides). This lack of in­
formation on the efficacy of photocatalyst materials on MPs degradation
processes is identified as an interesting future research avenue for
exploration.
Evaluating the data given in Table 5, it can be noted that different
quantification methods have been used in the different studies cited to
determine MPs degradation efficiency. This makes it challenging to
compare the efficiency of the different photocatalysts tested and to
understand their effect on MPs degradation. The creation of standard­
ized quantification methods to determinate MPs degradation efficiency
is another significant knowledge gap worth exploration in addition to
the investigation of the degradation mechanisms of MPs in the presence
of photocatalysts.
Engineered biodegradation of MPs have been tested [112,116],
where only slight modifications to the MPs structure (i.e., 28% particle
diameter reduction) were found after 60 days using wild bacterial
strains (i.e., Bacillus sp., and Paenibacillus sp.) [112]. However, when
engineered bacterial strains were used (i.e., Comamonas testosterone),
MPs physical and chemical modifications were achieved within 48 h
(Table 5) [116]. Despite the fact that bacteria modification showed
improved MPs degradation, there is a significant potential drawback in
view of the risk associated with the potential accidental release of bac­
teria into the environment. This may pose a significant threat to the
ecosystem because genetically modified organisms (GMOs) may inter-
breed with other strains (i.e., wild types or native species) or compat­
ible relatives [134]. Also, natural organism tolerance abilities may be
enhanced, which will alter the ecological relationship and behavior of
native species. GMOs can have a faster growth rate enabling a
competitive advantage over native organisms and becoming invasive
species, spreading into habitats and generating ecological and economic
damage.

8
O.M. Rodríguez-Narvaez et al.
GMOs are commonly developed to survive under extreme environ­
mental conditions, making elimination from the environment difficult
[135,136]. The use of biological digestion for MPs decomposition using
GMOs has a number of significant knowledge gaps. For example, using
GMOs or algae to complement conventional biological treatment (e.g.,
active sludge or bio-discs) for MPs decomposition is a very compelling
approach meriting further exploration because the resulting technology
can be suitable for full scale application. However, developing biological
treatment using GMOs must include identification of potential human
and ecosystem health risks that could arise from exposure to GMOs.
Alternately, it could entail developing a technology capable of pre­
venting the release of GMOs into the environment.
Studies have reported on the use of Fenton and Fenton-like reactions
for MPs decomposition as listed in Table 5. As shown, the Fenton reac­
tion has been found to be able to achieve only limited chemical or
physical changes in the MP particles (e.g., increased carbonyl index, O/C
ratio) when a low hydrogen peroxide (H2O2) concentration was used (e.
g., 10 mM) [5,114]. In some other studies, no changes in the FTIR ab­
sorption spectrum were noted for experiments performed at high pH.
This is attributed to the low solubility of iron at the reaction conditions
tested [5]. When wet oxidation using persulfate was tested for MPs
degradation [114], physical and chemical modifications of MPs were
observed after 30 days when 100 mM of persulfate was used.
Despite the encouraging results reported in research literature,
several drawbacks can be identified. For example, the required amount
of time reported for the modification of MPs (30 days) is significantly
long and probably impractical for full scale application. Additionally,
relatively little is known on the success of the application of these
treatments for MPs decomposition. This can be considered as a signifi­
cant knowledge gap which merits further investigations. For example,
testing the performance of different oxidants, in addition to persulfate
(e.g., peroxymonosulfate, percarbonate, or hydrogen peroxide) at
different pH, temperature and concentrations may lead to the identifi­
cation of new processes that may prove successful in the decomposition
of MPs in a cost-effective way.
Fenton-like processes have been reported achieving significant
physical and chemical modification of MPs (e.g., 50% weight loss) after
8 h of treatment [115]. The combination of peroxymonosulfate (PMS)
and manganese-modified carbon nanotubes (Mn@CNTs) at high tem­
perature (>100 ◦ C) and acidic conditions (pH = 3) have been reported to
have achieved significant MPs weight loss [115]. However, despite the
encouraging results, there are also significant knowledge gaps. For
example, no information is available on the influence of the primary
variables tested for MPs degradation (e.g., PMS concentration,
Mn@CNTs load). MPs could also be degraded using other advanced
oxidation processes (e.g., the Co/PMS reaction), which has been re­
ported to be highly effective in the degradation of organic contaminants
[131,137]. As reported by Kang et al. [115], compounds with different
carbon structures (e.g., low chain polymeric compounds) are likely to be
released into the water after the melting of MPs and could be degraded
using sequentially coupled secondary treatment.
Other Fenton-like reaction which can be effective for MPs degrada­
tion is the electro-Fenton process. Miao et al. [117] reported that the
electro-Fenton process using a TiO2/graphite cathode was highly effi­
cient for polyvinylchloride (PVC) MPs degradation. These researchers
found that H2O2 production improved when a TiO2/graphite cathode
was used, generating a relatively higher amount of hydroxyl radicals
when compared with the conventional Fenton reaction. Under these
conditions, 80% dechlorination was observed in relation to PVC MPs.
Hydrothermal carbonization (HTC), on the other hand, is a ther­
mochemical treatment producing solid carbon-rich materials (hydro­
char) [138]. The HTC process can be operated at low reaction conditions
when compared with combustion, pyrolysis, and gasification [139].
During HTC process, materials are upgraded in hot compressed water
inducing hydrolysis, aromatization, dehydration, recondensation, and
decarboxylation reactions, giving rise to the formation of high value
9
Chemical Engineering Journal 414 (2021) 128692
added products [140]. The quality of the hydrochar produced depends
on the composition of process liquor, as product formation and overall
reaction can be highly influenced by process water quality. Both,
hydrochar and liquid phase depends heavily on the feedstock used, re­
sidual moisture, quality of feed water and HTC reaction temperature and
reaction time.
There are several studies where HTC of several materials (especially
biomass) were investigated. However, the lack of detailed knowledge on
HTC of MPs remains a pending research task. In a previous study, Ini­
guez et al. [141] explored the hydrothermal carbonization (HTC) of a
mixture of 87 plastic materials to examine the characteristics of the final
products obtained and to test the feasibility of converting marine plastic
debris to fuel. They found that the increase in temperature of the HTC
process reduced the content of inorganic anions and increased the net
calorific value of the resulting hydrochar. The final products from HTC
are solid hydrochar, which can be used for several applications such as
fuel, catalyst, carbon sequestration and adsorbents [142-144]. Despite
the interesting outcomes from Fenton-like and HTC processes as po­
tential approaches for the degradation of MPs, only a limited number of
examples of their application are currently available in research litera­
ture, suggesting this lack of information is a significant gap of knowl­
edge worth exploration.
5. Conclusions
As highlighted in the review, in recent years significant research has
been undertaken for the development of engineered technologies for the
separation and degradation of microplastics in freshwater. However,
significant knowledge gaps still exist, pointing to the ongoing challenges
to ensure water safety. The key findings of this review are:
• Wastewater effluent is a significant contributor of MPs in freshwater.
Unfortunately, a significant lack of knowledge remains in relation to
the influence of anthropogenic activities and population density on
the type and load of MPs present in wastewater effluent and waste­
water sludge.
• There is also a significant knowledge gap of in relation to the efficacy
of wastewater treatment on the removal of MPs and correlation with
the specific characteristics of the MP particles, volume of treated
wastewater, and variations in the MPs load.
• A significant amount of separation methods have been investigated,
mainly as pre-treatment for MPs quantification at laboratory scale.
Very few full scale or laboratory scale methods with potential for
scaling up have been reported.
• Coagulation-flocculation/Flotation processes have been investigated
for the separation of MPs in freshwater. However, relatively only a
small number of coagulants and flocculants have been studied. The
need for testing other commercially available products, including
plant-based coagulants, as well as non-conventional coagulation
processes (i.e., electrocoagulation) reported in research literature as
being cost-effective for water treatment remains to be investigated
in-depth.
• Chemical and biological digestion have been tested in the past for
effective separation of MPs. However, the lack of a systematic
approach and/or in-depth information on the process efficiency have
been noted, along with complete absence of information on the use of
chemical digestion-related processes (i.e., wet oxidation) not only as
a pre-treatment measure for the quantification of MPs, but also as a
way to degrade MPs.
• Very few studies have reported on effective engineered MPs degra­
dation technologies, and even fewer are reported suitable for scaling
up.
• Photodegradation is reported as having encouraging potential for
MPs degradation. However, this entails significantly long process
periods which may pose a noteworthy drawback for full scale
O.M. Rodríguez-Narvaez et al.
application. Furthermore, additional research is needed for devel­
oping a better understanding of the feasibility of the process.
• Engineered biodegradation is another alternative identified in
research literature for degradation of MPs, but was found most
suitable when engineered bacterial strains are used. However, sig­
nificant ethical considerations are required for full scale application.
• The use of advanced oxidation processes and/or nanomaterials is
another option with significant potential for scaling-up applications.
However, more information is needed in order to estimate the actual
feasibility of these processes in the field, including testing of a
broader range of oxidants and the concerns in relation to the release
of nanomaterials into the environment.
• The modification of MPs by thermal processes such as pyrolysis and
hydrothermal carbonization is identified as having significant po­
tential because MPs are carbon-based materials and can be used as
feedstock for the production of other carbon-based materials (e.g.,
biochar, hydrochar) with potential for environmental applications.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgments
This work was partially supported by Nevada Water Resources
Research Institute (Grant No G16AP00069). O.M. Rodriguez-Narvaez
grateful thank CONACyT and Universidad Autonoma de Nayarit for a
graduate fellowship.
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