1-s2.0-S0013935124003207-main
1-s2.0-S0013935124003207-main
1-s2.0-S0013935124003207-main
Environmental Research
journal homepage: www.elsevier.com/locate/envres
Review article
A R T I C L E I N F O A B S T R A C T
Keywords: Microplastics (Mps) have emerged as a pervasive environmental concern, with their presence detected not only
Microplastics in freshwater ecosystems but also in drinking and bottled water sources. While extensive research has centered
Coagulation precipitation on understanding the origins, migration patterns, detection techniques, and ecotoxicological impacts of these
Electrocoagulation
contaminants, there remains a notable research gap about the strategies for Mps removal. This study reviews
Advanced oxidation
Wastewater
existing literature on chemical approaches for mitigating microplastic contamination within wastewater systems,
focusing on coagulation precipitation, electrocoagulation, and advanced oxidation methods. Each approach is
systematically explored, encompassing their respective mechanisms and operational dynamics. Furthermore, the
comparative analysis of these three techniques elucidates their strengths and limitations in the context of MPs
removal. By shedding light on the intricate mechanisms underlying these removal methods, this review con
tributes to the theoretical foundation of microplastic elimination from wastewater and identifies future research
trajectories and potential challenges.
1. Introduction production to wear of plastic from household usage (Wei et al., 2023).
Key contributors include raw plastic manufacturing (Oliveira et al.,
The escalating utilization of plastic products across various in 2023), clothing washing (Zhou et al., 2023), and textile industry (Van
dustries, such as take-out services, express delivery, and beauty prod Tran et al., 2023), with nylon discharging numerous fibers during
ucts, has correspondingly heightened plastic consumption. However, the clothing synthesis or laundering (Zhuang and Wang, 2023). The release
aftermath of plastic usage, characterized by disposal methods like of microbeads from personal care products, like facial cleansers, sham
landfilling, random discarding, and incineration, has ushered in a con poos, and toothpaste, further aggravates the introduction of Mps into
cerning era of plastic-induced environmental contamination (Rouillon wastewater (Bostan et al., 2023). While primary wastewater treatment
et al., 2016; Miao et al., 2023; Trusler et al., 2023; Li et al., 2020). The removes larger particles, secondary treatment inadequately addresses
protracted exposure of everyday plastics to weathering, sunlight, and Mps due to the absence of dedicated removal processes (Sheriff et al.,
wear culminates in the breakdown of these materials into smaller frag 2023). This deficiency has led researchers to posit that wastewater
ments (Martina and Trini Castelli, 2023). Plastics smaller than 5 mm are treatment plants constitute a significant source of environmental
classified as microplastics (Mps). This includes primary Mps from microplastic pollution (Liao et al., 2023). Given Mps’ resistance to
household and personal care products and secondary Mps from degra natural degradation, their accumulation persists within ecosystems,
dation or breakage of primary plastics (Zhao et al., 2023; Basaran et al., posing environmental risks (Bai et al., 2023). The impact of Mps on plant
2023). Detectable Mps in wastewater include polyester (PES), poly and animal life is increasingly evident, resulting in altered catalase ac
ethylene (PE), polyamide (PA), polyethylene terephthalate (PET), tivities, oxidative stress responses, immune modulation, and reproduc
polypropylene (PP), polystyrene (PS), and polyurethane (PU) (Hasan tive hindrance (Chang et al., 2023; Stapleton et al., 2023). Humans,
and Jho, 2023; Ivy et al., 2023). positioned at the apex of the food chain, inadvertently ingest and inhale
MPs pollution stems from diverse sectors spanning industrial Mps, exposing themselves to toxic substances like phthalates and
* Corresponding author.
E-mail address: yanww5@mail.sysu.edu.cn (W. Yan).
https://doi.org/10.1016/j.envres.2024.118416
Received 14 November 2023; Received in revised form 23 December 2023; Accepted 2 February 2024
Available online 3 February 2024
0013-9351/© 2024 Elsevier Inc. All rights reserved.
B. Cui et al. Environmental Research 249 (2024) 118416
polybrominated diphenyl ethers, with implications for inflammation particle size and density.
and cell function (Haque and Fan, 2023; Ng and Todd, 2023). Coagulation is the predominant technique employed in numerous
To mitigate the ecological ramifications of Mps, considerable sewage treatment facilities for mitigating microplastic pollution. This
research is directed toward their removal from wastewater. Existing process involves the utilization of coagulants, such as iron salts and
approaches include electrocoagulation, membrane separation, activated aluminum salts. In a study by Ma et al., in 2019 (Ma et al., 2019a),
sludge, coagulation precipitation, photocatalytic degradation, and FeCl3⋅6H2O was employed as a coagulant to address the removal of PE
biodegradation through green algae (Xu et al., 2022; Egea-Corbacho from sewage (see Table 1 for details). Their findings highlighted a
et al., 2023; Martín-García et al., 2022; Tang, 2023; Zhou et al., 2021; noteworthy correlation: an increase in coagulant concentration corre
Ariza-Tarazona et al., 2020; Wu et al., 2022; Cui et al., 2023; Hou et al., sponded to a decrease in the efficacy of PE removal. This outcome can be
2022). These strategies span physical, biological, and chemical realms. attributed to the distinctive particle sizes of PE and the flocculant.
However, physical methods primarily relocate Mps to sludge, exacer Specifically, PE particles exhibit a millimeter-scale size, while the
bating sludge treatment demands. The efficacy of biological methods average dimensions of flocculant particles are in the nanometer range.
hinges on intricate environmental controls, and their applicability re This size incongruity diminishes the flocculant’s capacity to effectively
mains limited. Both physical adsorption and biological approaches capture and adsorb PE particles.
exhibit constraints, prompting a thorough examination of alternative Furthermore, the zeta potential of PE particles exhibited a negative
methods. This review, therefore, assesses recent chemical approaches value at pH levels exceeding 4. This property implies that lower pH
employed for Mps removal, providing insights into the comparative values within the aquatic environment facilitate the removal of PE
strengths and limitations of distinct methods. particles. However, altering coagulant dosages and the pH of the water
environment proves impractical for the real-world elimination of PE
2. Removal of mps particles. To address this challenge, the research team introduced
polyacrylamide (PAM) into the system. PAM operates as an adsorption
2.1. Coagulation and agglomeration processes bridge, effectively resolving the issues associated with coagulant dosing
and pH adjustments. The incorporation of anionic PAM results in an
The coagulation method constitutes a fundamental approach for increased flocculant density. Remarkably, the flocculant acquires a
microplastic (Mps) removal, operating on two primary mechanisms: positive charge in a water environment with a pH of 7. This positive
adsorption electric neutralization and sediment trapping, as depicted in charge enhances the efficacy of PE removal. Consequently, introducing
Fig. 1. These mechanisms necessitate distinct considerations: the former anionic PAM emerges as a strategic approach to enhance the removal of
revolves around Mps charge properties, while the latter factors in Mps PE particles within the coagulation process.
Fig. 1. The mechanism of removing Mps by coagulation and agglomeration processes. (a) Reproduced with permission from Duan et al. (Duan et al., 2022) copyright
2022, Elsevier; (b) Reproduced with permission from Zhou et al. (Zhou et al., 2021) copyright 2021, Elsevier.
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B. Cui et al. Environmental Research 249 (2024) 118416
Table 1
Summary of the literature on the removal of microplastics by coagulation and agglomeration processes.
MPs Mps Mps Removal method Types of coagulants Experimental details Removal Ref.
size,μm concentration efficiency
PE – – coagulation and agglomeration FeCl3⋅6H2O [FeCl3⋅6H2O] = 112 mg/L(2 mmol/L); 61.19% ± Ma et al.
processes pH = 8; [PAM]: cationic 3.67% (2019a)
PE – – coagulation and agglomeration AlCl3⋅6H2O [AlCl3⋅6H2O] = 405 mg/L(15 mmol/ 36.27% ± Ma et al.
processes PAM L); pH = 7; [PAM] = 15 mg/L 1.06% (2019b)
PS 1 μm 182 × 106 MP/ coagulation and agglomeration ferric chloride [ferric chloride] = 0.37 mmol/L; pH = 99.4% Rajala et al.
L processes 7.3; (2020)
PS 1 μm 182 × 106 MP/ coagulation and agglomeration polyaluminum chloride [polyaluminum chloride] = 0.16 98.2% Rajala et al.
L processes mmol/L; pH = 7.3 (2020)
PS <500 μm 0.05g/cm3 coagulation and agglomeration PAC [PS]0 = 500 mg/L; [PAC]0 = 60 mg/L; 77.83% Zhou et al.
processes pH = 6.90 (2021)
PE <500 μm 0.91g/cm3 coagulation and PAC [PE]0 = 500 mg/L; [PAC]0 = 90 mg/L; 29.70% Zhou et al.
7gglomeration8processes pH = 6.91 (2021)
PE 10–30 0.91g/cm3 coagulation and agglomeration Alum and cationic [PC]0 = 500 mg/L; [alum]0 = 20 mg/L; 92.7% Shahi et al.
μm processes polyamine-coated pH = 7 ± 0.2 (2020)
In addition, extensive investigations have been conducted for the Furthermore, the overall removal rate of polyester surpassed that of PE
removal characteristics of PS and PE, along with the underlying mech and PS. This discrepancy is attributed to the favorable shape of polyester
anisms involving the application of polyaluminum chloride (PAC) and strips, which facilitates the bridging effect, coupled with the presence of
FeCl3 coagulants, respectively (Zhou et al., 2021). Notably, the absence C=O on the ester group, promoting coagulant hydrolysate adhesion.
of coagulants resulted in a PE removal rate of 3.19% and a PS removal To enhance the coagulation efficacy, He et al. (2022) introduced
rate of 50.78%. Upon introducing coagulants to the experimental sys anionic polyacrylamide (APAM) as a coagulant aid alongside poly
tem, the removal efficiency of both microplastics exhibited a positive aluminum chloride (PAC) for PE removal. Their experimentation un
correlation with the increment in coagulant concentration. This trend veiled a nuanced relationship between PAC concentration and PE
continued until an optimal point was reached, beyond which the removal rate. This relationship exhibited three discernible stages: the
microplastics’ removal rates stabilized. Specifically, the most effective enhancement stage, the nearly complete removal stage, and the stabi
removal rates achieved were 29.70% for PE and 77.83% for PS. The lization stage. Notably, the optimal content for PAC was determined to
investigation further encompassed an analysis of the coagulation be 25 mg/L, while APAM demonstrated its efficacy within the range of 5
mechanism, delving into three distinct facets: charge neutralization, mg/L to 7 mg/L. This multifaceted exploration underscores the dynamic
adsorption, and coagulant hydrolysis. The findings elucidated that both interplay of coagulants and their aids in microplastic removal.
charge neutralization and adsorption processes were actively involved Of significance, the charge attributes of Mps are subject to alteration
in the coagulation mechanism. However, the contribution of coagulant with shifts in the water environment’s pH. Consequently, pH adjust
hydrolysates to the overall coagulation effectiveness exceeded that of ments within the water environment become essential when employing
the coagulant hydrolysis process. This nuanced insight into the mecha the adsorption electric neutralization mechanism for Mps removal.
nism sheds light on the consistent superiority of PAC over FeCl3 in terms However, this strategy encounters practical limitations in real-world
of coagulation efficiency. This disparity can be attributed to the water treatment scenarios. Conversely, Mps exhibit diverse particle
enhanced role of coagulant hydrolysates in PAC-mediated coagulation. sizes, and their removal rates vary correspondingly. Notably, for PE Mps,
Within the drinking water and wastewater treatment facilities, a smaller particle sizes correlate with more efficient removal. The removal
pivotal consideration emerges regarding the utilization of alum, which dynamics for PS Mps differ; PS Mps with sizes exceeding 500 μm man
should be carefully managed within a limit of 20 mg/L as advocated by ifest notably higher removal rates compared to those with sizes below
Gokulanathan et al., in 2021 (Gokulanathan et al., 2021). This recom 500 μm, as elucidated by Miranda Zoppas et al., in 2023 (Miranda
mendation underscores the need for thoughtful discernment when opt Zoppas et al., 2023). Intriguingly, PS possesses a density exceeding that
ing for and applying coagulants in practical treatment scenarios. of water, suggesting smaller PS particles might be prone to precipitation
Notably, Shahi et al. (2020) noted that when alum was employed formation. However, counterintuitively, the opposite could be true. This
singularly to remove PE, the most effective removal rate (70.7%) was might be attributed to smaller PS particles’ challenge in overcoming the
achieved at an alum dosage of 30 mg/L. To address this challenge, the water’s surface tension, which could hinder their effective precipitation
researchers introduced cationic polyamine-coated (PC) within a system formation. In essence, the coagulation method for Mps removal rests on
utilizing 20 mg/L of alum. This innovation resulted in a remarkable a delicate interplay between these mechanisms and the distinct char
26.8% increase in the removal efficiency of PE. Additionally, their in acteristics of different Mps, emphasizing the need for a detailed under
vestigations unveiled that the coagulation mechanism primarily standing when devising strategies for effective environmental
encompassed charge neutralization at lower coagulant concentrations, remediation.
transitioning to sedimentation network predominance at higher coagu
lant levels. As described above, primary Mps are transformed into sec
2.2. Electrocoagulation technique
ondary Mps under external factors such as natural weathering, exposure
to sunlight, and rain erosion. Consequently, the study’s scope should
Electrocoagulation serves as an integrated sewage treatment
encompass the removal of both primary and secondary MPs. In this
approach, amalgamating flocculation, flotation, and electrochemical
context, Lapointe et al. (2020) conducted a comparative analysis of raw
reactions. The fundamental unit of this technology is an electrolytic cell,
and weathered Mps removal rates while introducing coagulants (PAM).
wherein immersed anodes and cathodes are linked by an external direct
The coagulant concentration required for 1 NTU was employed (alum:
current (DC) power source. The application of external current prompts
2.73 mg Al/L; PAM: 0.3 g/L). Their findings revealed that the removal
the electrolysis of metal anodes, leading to the generation of metal
rate of raw Mps (PE: 82%, PS: 84%) was eclipsed by weathered Mps (PE:
cations. These cations subsequently undergo hydrolysis to yield hy
99%, PS: 99%). The transformation brought about by weathering led to
droxide ions in the aqueous medium. The combination of various hy
alterations in Mps surface roughness and functional groups, conse
droxide ions results in the formation of micro-flocculants. Under the
quently enhancing the affinity between Mps and coagulants.
joint influence of charge neutralization and grid interception, suspended
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pollutants coalesce into sinking flocculants. Additionally, the cathode between particle size and specific surface area enhances suspended
produces an insoluble gas, which elevates lighter flocs to the water matter entrapment.
surface, constituting the basis for contaminant removal via Similarly, Elkhatib et al. (2021) engaged in an experiment targeting
electrocoagulation. the removal of polyester flash particles from sewage via electro
In recent years, the application of electrocoagulation for removing coagulation. They identified optimal conditions by optimizing current
MPs pollutants from wastewater has gained traction. Distinguishing it density, MP concentration, pH, and electrolysis time. Subsequently, they
self from traditional methods, electrocoagulation operates within an applied these conditions to real sewage simulation by introducing
electric field environment, eliminating the need for additional co equivalent amounts of microplastics into chlorinated sewage within a
agulants. In this process, metal cations detach from the electrode, treatment plant. This endeavor yielded a microplastic removal rate of
forming micro-flocculants within the water (Fig. 2). These micro- 96.5% in the actual sewage scenario, slightly lower than the laboratory’s
flocculants then amalgamate with suspended particles, precipitating 98.5%. This discrepancy might arise due to competing suspended par
through collision, thus affecting pollutant removal from the water. An ticles in actual sewage, contending for hydroxide. Electrocoagulation
insightful study by Shen and colleagues (Shen et al., 2022) investigated electrode selection commonly favors iron or aluminum electrodes as
distinct MPs removal rates using various electrodes in electro anodes and alternative metal electrodes as cathodes. Departing from this
coagulation. The research encompassed plastic fibers (cellulose acetate practice, Hu et al. (2023) explored the removal of polyamide (PA) from
(CA) and polypropylene (PP)) sourced from discarded cigarette butts wastewater utilizing four electrode combinations: Fe–Al, Fe–Fe, Al–Fe,
and medical masks alongside granular microplastics (PE and poly and Al–Al. Remarkably, PA removal rates were 90.92%, 88.38%,
methylmethacrylate (PMMA)). An aluminum or iron electrode served as 86.94%, and 83.74%, respectively. Among these configurations, Fe–Al
the anode, while a copper electrode acted as the cathode. Optimization exhibited the most promising outcomes. The efficacy of Fe–Al arises
of multiple parameters was carried out within the reaction system, from the co-generation of iron and aluminum flocs within the electro
yielding high removal rates at pH 7.2: PE (93.2%), PMMA (91.7%), CA lytic cell. The iron floc boasts superior density and settleability, while
(98.2%), and PP (98.4%). Notably, the study highlighted that the the aluminum floc exhibits heightened adsorption capabilities. This
aluminum electrode outperformed the iron electrode, attributed to the multifaceted investigation underscores the potential of electro
smaller average particle size of aluminum flocculants (174.6 ± 24.3 μm) coagulation as a robust strategy for tackling microplastic contamination
compared to iron flocculants (243.8 ± 36.4 μm). The inverse correlation in wastewater environments.
Zooming in on the details, the anode typically employs iron or
aluminum electrodes. In the case of aluminum electrodes, anode elec
trolysis yields Al3+ ions that assume two distinct roles. Firstly, Al3+
rapidly associates with water molecules to form Al(H2O)3+ 6 ions. Sub
sequent hydrolysis of Al(H2O)3+ 6 leads to the release of H+ ions,
engendering a range of mononuclear hydroxides (Al(H2O)3OH2+, Al
(H2O)4OH2+, Al(H2O)5OH2+, and so forth) (Liu et al., 2023a). Secondly,
through hydration, Al3+ interacts with OH− to engender entities like Al
(OH)+ 2 and Al(OH)3. Notably, the hydroxyl groups within the formed
hydroxyl aluminum ions are unsaturated, facilitating their polymeriza
tion with additional Al3+ ions to construct hydroxyl bridges
(Liwarska-Bizukojć and Olejnik, 2020).
Consequently, mononuclear aluminum complexes progressively
polymerize, culminating in a polymer network and the eventual for
mation of micro-flocculants. This structural aspect of aluminum flocs
has been corroborated by studies that employed scanning electron mi
croscopy (SEM) (Zhang et al., 2019). When ferroelectric electrodes are
employed, the underlying principle aligns closely with aluminum elec
trodes, albeit culminating in the precipitation of γ-FeOOH. During these
reactions, researchers introduce anionic surfactants. This addition is
strategic, as micro-flocculants from the positive electrode carry a posi
tive charge. Surfactants amplify their removal rate by augmenting the
negative charge on microplastic surfaces. Moreover, surfactants expe
dite the cathode’s hydrogen evolution reaction, forming a more intense
bubble. Overall, electrocoagulation operates through a multifaceted
interplay of electrochemical reactions, hydrolysis, and charge in
teractions, with the composition of electrodes and the introduction of
surfactants serving as pivotal components in optimizing microplastic
removal efficacy.
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etc.) in the sp2 orbital of atoms can increase the production of active generation. Therefore, a crucial aspect of photocatalytic microplastic
sites and improve catalytic activity. In addition, carbon nanotubes, degradation is maintaining an optimal hydration state. Natural sunlight
graphene, and other materials with rich pore structures and controllable is comprised of ultraviolet, visible light, and infrared regions. Research
physical and chemical properties have also been favored by researchers. indicates that the photodegradation of microplastics in these regions
Therefore, Kang et al. (2019) first prepared carbonamide nanoparticles forms a progressive relationship. In this continuum, ultraviolet light
and then fixed carbonization onto N-doped carbon nanotubes through instigates direct photodegradation, while visible light raises tempera
pyrolysis to form Mn@NCNTs activated PMS to remove Mps in water. ture based on the same mechanism. Infrared light accelerates thermal
According to the experimental results, Mn@NCNTs calcined at 800 ◦ C oxidation. Verma et al. (2017) proposed expanding the nano-polymer’s
have good catalytic performance, and the best PE removal rate is 54% at absorption spectrum to enhance photodegradation, transitioning from
160 ◦ C. the ultraviolet to visible regions to optimize sunlight utilization. Their
study compared the catalytic efficiency of TiO2-rGO nanomaterials and
2.3.2. Photocatalytic degradation TiO2 nanomaterials, demonstrating that the former yielded greater
As a promising low-temperature treatment technology, photo polypropylene (PP) degradation under identical conditions. This
catalytic degradation capitalizes on catalyst-induced oxidation when improvement stemmed from the redshift of the catalyst’s absorption
illuminated by light energy. This process generates potent oxidizing spectrum due to rGO’s addition. The resulting Ti–O–C bond facilitated
active free radicals, which subsequently react with pollutants, leading to visible light absorption, and rGO acted as an efficient electron acceptor
pollutant removal (Table 2). Titanium dioxide (TiO2), an oxide semi due to its two-dimensional π-linkages, hindering electron-hole pair for
conductor, is renowned for its remarkable oxidation and photostability mation while promoting active species generation.
properties. However, TiO2’s catalytic activity is confined to the ultra Saifuddin et al. (2022) introduced the concept of an optimal removal
violet (UV) wavelength range below 385 nm, necessitating modifica rate. Specifically, they discovered that 1 mg of zinc oxide nanorods
tions to enhance its performance under solar energy. Researchers have could degrade 0.758 mg of PP microplastics. Using a TiO2@NC-MOF
ingeniously harnessed multi-walled carbon nanotubes (MWCNTs) to catalyst, they achieved 0.843 mg of PP degradation per 1 mg of
amplify TiO2’s photocatalytic performance (Kim et al., 2006). The ho TiO2@NC-MOF under ample UV irradiation. Notably, UV irradiation of
mogeneous structure of MWCNTs facilitates optimal catalyst dispersion, TiO2 surfaces yields electrons and holes. However, these unmodified
and their substantial electron storage capacity rapidly excites electrons surface electrons and holes tend to recombine, hindering active free
under light energy, forming recombination of electron-hole pairs. This radical generation. TiO2 requires support on a carrier facilitating rapid
generates more active free radicals, ultimately enhancing the catalyst’s electron transfer to address this. Transition metal borides’
efficiency. An et al. (2014) improved the photocatalytic process of TiO2 electron-filling properties have proved beneficial. He et al. (2023)
by preparing water-soluble MWCNTs via an acid steam method. Using loaded TiO2 onto FeB to degrade polystyrene (PS). By altering the cat
the sol-gel technique, these water-soluble MWCNTs were then employed alyst’s size, they manipulated the absorption spectrum region, thereby
with TiO2 to create a nanocomposite photocatalyst for polyethylene (PE) enhancing catalytic efficiency. FeB augmented light absorption, accel
degradation. This innovative approach resulted in a composite photo erated electron migration, and facilitated photoelectron-proton combi
catalyst with an absorption band spanning the entire UV-VIS region, nations to produce hydrogen fuel. In addition to TiO2, zinc oxide (ZnO)
significantly augmenting light absorption capacity. The weight of the has gained attraction as a photocatalytic material due to its
TiO2-MWCNTs (20 wt%)-PE sample was reduced by 35% after 180 h single-crystal wurtzite structure, promoting electron mobility and
under UV irradiation. enhanced light absorption (Sun et al., 2023). The controllable defect
Employing mussel protein as a nitrogen source and a pore-forming structure of ZnO amplifies active free radical production (Zheng et al.,
agent in conjunction with TiO2, Ariza-Tarazona et al. (2019) fash 2022). Recognizing that actual water systems maintain dynamic equi
ioned a nitrogen-doped TiO2 (N–TiO2) catalyst for the photocatalytic librium, Uheida et al. (2021) coated ZnO nanoparticles onto glass fibers
degradation of high-density PE. Significantly, the degradation kinetics to form a photocatalyst capable of removing PE in a flowing state,
coefficient in the water phase was three times that of the solid-phase closely mimicking sewage and water treatment scenarios. Their inno
experiment, attributed to the variance in water molecule content near vative approach successfully decomposed PE by analyzing the carbonyl
the catalyst—a pivotal factor influencing highly active species index and structural changes from long to short chains and
Table 2
Summary of the literature on the removal of microplastics by photocatalytic degradation.
Mps catalyst Supporting material Light Experimental details Removal Ref.
efficiency
LDPE Titania nanotubes 10 wt% of trinitrotoluene UV (primary wavelength [Light intensity] = 2.54 mW/cm2; 41% Ali et al. (2016)
of 315 nm) [time] = 45d;
LDPE Titania nanotubes – visible light (wavelength [Light intensity] = 6.76 mW/cm2; 48% Ali et al. (2016)
range of 400–700 nm) [time] = 45d
LDPE biosynthesized palladium LDPE@Pd nanocomposite solar light [Light intensity] = 9:00 a.m. to 5:00 49% Olajire and
nanoparticles (Pd NPs) film (1 wt% of Pd NPs) p.m. on every sunny day; [time] = Mohammed (2019)
30d
PS BiOCl PS/BiOCl composite film (3 500 W Halogen [Light intensity] = 9:00 a.m. to 5:00 48% Sarwan et al. (2020)
wt% of BiOCl) luminaire lamp p.m. on every sunny day; [time] =
90h
LDPE TiO2@amylose/polyiodide/ xenon lamp [Light intensity] = 100 W/cm2; 11.47% Zhao et al. (2021)
hydroxyethyl cellulose [time] = 72h;
PS Triton X-100 based TiO2 TiO2 nanoparticle films UV irradiation [Light intensity] = 365 nm; [time] 98.40% Nabi et al. (2020)
fabricated with Triton X-100 = 12h;
PP ZnO NRs ZnO NRs immobilized onto tungsten-halogen lamp [Light intensity] = 0.6 SUN (60 65% Uheida et al. (2021)
glass fibers substrates mW/cm2); [time] = 456h
HDPE N–TiO2 semiconductors fluorescent lamp [Light intensity] = 27W; [time] = 6.4% (Ariza-Tarazona
20h et al., 2019)
HDPE C, N–TiO2 semiconductor LED lamp [Light intensity] = 50W; [time] = 70% (Ariza-Tarazona
50h et al., 2020)
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TiO2 + hv → e- + h+ (1)
H2 O + h+ → H+ + OH• (2)
O2 + e− →O•−2 (3)
2HOO• → H2 O2 + O2 (5)
2.3.3. Electro-Fenton-like
Kiendrebeogo et al. (2021) conducted a study investigating the
impact of electrode oxidation on the elimination of polystyrene micro
spheres. They specifically explored the effectiveness of three anode
electrodes—boron-doped diamond (BDD), mixed metal oxide (MMO),
and iridium oxide (IrO2)—in conjunction with a titanium cathode.
Among these, BDD exhibited the most favorable outcomes, primarily
attributed to its considerably higher OH⋅- formation rate during the re
action process (4 and 7.4 times that of IrO2 and MMO, respectively).
Parameters such as anode area, electrolyte material and concentration,
current density, and reaction time were systematically optimized. Under
optimal conditions, a high removal rate of 89 ± 9% was achieved for 26
μm polystyrene microspheres. A comprehensive understanding of the
reaction mechanism was also presented. Initially, water molecules on
the anode’s surface relinquish electrons to generate OH⋅-. Additionally,
the presence of Na2SO4 triggers the production of SO4⋅- in the reaction
system, leading to the formation of active free radicals. These radicals
subsequently target C–H bonds within polystyrene, facilitating the cre
ation of C–O bonds. This sequence ultimately dismantles polymer chains
and facilitates the decomposition into smaller molecular entities.
Evidently, the high current intensity required for the above
mentioned study (108.4 mA/cm2) poses a notable challenge. Moreover,
due to microplastics’ hydrophobic nature and insolubility in water, their
Fig. 3. The mechanism of removing Mps by Photocatalytic degradation. (a)
removal efficiency through BDD anodizing technology hinges on their
Reproduced with permission from Liu et al. (Liu et al., 2023b), copyright 2023,
transfer rate from the aqueous solution to the electrode rod. Recognizing Elsevier; (b) Reproduced with permission from Cao et al. (Cao et al., 2022),
this, Lu et al. (2022) introduced surfactants, specifically Sodium Dodecyl copyright 2022, Elsevier; (c) Reproduced with permission from Zhong et al.
Sulfate (SDS), into the reaction system to enhance microplastic removal. (Zhong et al., 2024), copyright 2024, Elsevier; (d) Reproduced with permission
SDS offers dual benefits: first, it equilibrates interfacial tension and from Jiang et al. (Jiang et al., 2021), copyright 2021, Elsevier.
promotes homogenization; second, SDS generates supplementary active
free radicals through anodization, thereby boosting microplastic depicted in Fig. 4(b). In this context, Miao et al. (2020) proposed an
removal rates. They devised an SDS addition strategy involving its electrocatalytic method employing TiO2/C as a cathode for PVC
introduction (500 mg/L) during each half-life, except the last cycle, degradation. Notably, their results indicated a 56% removal rate and a
during electrolysis. Following 72 h of reaction, the presence of SDS 75% dechlorination rate after 6 h of electrolysis at − 0.7V and AgAgCl at
enhanced polystyrene (PS) removal rates by 1.35–2.29 times compared 100 ◦ C (Fig. 4(a)). This study sheds light on the intricacies of PVC
to the system without SDS. Polyvinyl chloride (PVC) degradation di removal, highlighting the challenges posed by its unique structure and
verges from PS or polyethylene (PE), as it necessitates breaking both the chlorine content.
long chain and eliminating chlorine. Electrochemical reduction ap
proaches to dechlorination include direct electrochemical reduction and
indirect electrocatalytic hydrogenation dichlorination, the latter
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B. Cui et al. Environmental Research 249 (2024) 118416
Fig. 4. The mechanism of removing Mps by Electro-Fenton-like. (a) Reproduced with permission from Miao et al. (Miao et al., 2020), copyright 2020, Elsevier; (b)
Reproduced with permission from Lu et al. (Lu et al., 2022), copyright 2022, Elsevier.
3. Comparison of methods current efficiency, and raise energy consumption. (2) Electrolyte Se
lection: Electrocoagulation necessitates continuous current flow,
When employing the coagulation method to address MPs, intro underscoring the need for electrolytes with high conductivity. (3) Water
ducing coagulants such as iron or aluminum salts is crucial, facilitating Impurities: Because metal electrodes are typically used in electro
the formation of larger flocs in wastewater. These flocs, in turn, effec coagulation, not all dissolved metal ions actively participate in the
tively remove MPs through mechanisms like charge neutralization, process. Some metal ions remain in the solution, necessitating subse
adsorption bridging (The bridging mechanism of adsorption means that quent removal. The photocatalytic degradation of microplastics offers
microorganisms can combine with solid suspended matter to form promise, yet several challenges persist within the entire system: (1)
bridge connection through ionic bond and hydrogen bond.), and capture Measurement limitations: Current measurements of MPs removal rates
rolling (Flocculant added to the water, will create a large flocculent. The in photocatalytic sewage degradation rely on the weight loss method.
constant movement of these flocculents in the water will sweep the This approach, however, primarily accounts for the adsorption of
surrounding small particles together, causing them to condense into microplastics onto the catalyst, failing to represent the actual dispersion
larger particles.). of MPs within sewage. (2) Catalyst After-Use Impact: Post-treatment, the
Researchers have established a direct correlation between the surface of the photocatalyst contains a combination of degraded MPs,
removal efficacy and microplastics’ surface charge, particle size, coag intermediate degradation products, existing inorganic organic matter
ulant dosage, and type. Furthermore, the pH level of the aqueous solu from sewage, and more. It remains uncertain whether this composition
tion significantly impacts the process, with optimal results observed in might inadvertently contribute to secondary environmental pollution.
acidic and neutral conditions. However, this constraint often limits the (3) Light Source dependency: Photocatalysts rely on an external light
method’s applicability in real-world water treatment scenarios. source for activation, with natural sunlight providing only a fraction of
In the electroflocculation process, MPs are eliminated via charge the required energy. The need for catalyst modification to enhance light
adsorption and capture within the flocs. This technique boasts several absorption adds to the economic costs associated with this method.
advantages, including reduced sludge production, simplified equipment,
and low energy consumption. Nonetheless, certain considerations war 4. Outlook
rant attention: (1) Anode Replacement: A pivotal factor influencing
electrocoagulation technology is anode passivation. Forming anode The removal of microplastics is still in the laboratory stage and has
passivation films can impede anode dissolution, elevate additional not been used in actual water plants. The following issues must be
7
B. Cui et al. Environmental Research 249 (2024) 118416
considered when choosing the method of removing microplastics and Ariza-Tarazona, M.C., Villarreal-Chiu, J.F., Barbieri, V., Siligardi, C., Cedillo-González, E.
I., 2019. New strategy for microplastic degradation: green photocatalysis using a
improving its practicality.
protein-based porous N-TiO2 semiconductor. Ceram. Int. 45, 9618–9624.
Ariza-Tarazona, M.C., Villarreal-Chiu, J.F., Hernández-López, J.M., Rivera De la Rosa, J.,
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sumption, so it is recommended to improve the reactor or process Alfaifi, M.Y., Elbehairi, S.E.I., Pandiaraj, S., 2023. Toxicity assessment of
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CRediT authorship contribution statement He, J., Zhang, Y., Ni, F., Tian, D., Zhang, Y., Long, L., He, Y., Chen, C., Zou, J., 2022.
Understanding and characteristics of coagulation removal of composite pollution of
microplastic and norfloxacin during water treatment. Sci. Total Environ. 831,
Baihui Cui: Investigation, Writing – original draft. Hongwei Rong: 154826.
Supervision. Tingting Tian: Writing – review & editing. Dabin Guo: Hou, H., Wang, S., Ji, B., Zhang, Y., Pi, K., Shi, Y., 2022. Adaptation responses of
Writing – review & editing. Luchun Duan: Writing – review & editing. microalgal-bacterial granular sludge to polystyrene microplastic particles in
municipal wastewater. Environ. Sci. Pollut. Control Ser. 29 (40), 59965–59973.
François Nkinahamira: Conceptualization. Pamphile Ndagijimana:
Hu, Y., Zhou, L., Zhu, J., Gao, J., 2023. Efficient removal of polyamide particles from
Conceptualization. Wangwang Yan: Project administration, Writing – wastewater by electrocoagulation. J. Water Proc. Eng. 51, 103417.
review & editing. Ravi Naidu: Methodology. Ivy, N., Bhattacharya, S., Dey, S., Gupta, K., Dey, A., Sharma, P., 2023. Effects of
microplastics and arsenic on plants: interactions, toxicity and environmental
implications. Chemosphere 338, 139542.
Jiang, R., Lu, G., Yan, Z., Liu, J., Wu, D., Wang, Y., 2021. Microplastic degradation by
Declaration of competing interest hydroxy-rich bismuth oxychloride. J. Hazard Mater. 405, 124247.
Kang, J., Zhou, L., Duan, X., Sun, H., Ao, Z., Wang, S., 2019. Degradation of cosmetic
The authors declare that they have no known competing financial microplastics via functionalized carbon. Nanosprings. Matter 1, 745–758.
Kiendrebeogo, M., Karimi Estahbanati, M.R., Khosravanipour Mostafazadeh, A.,
interests or personal relationships that could have appeared to influence Drogui, P., Tyagi, R.D., 2021. Treatment of microplastics in water by anodic
the work reported in this paper. oxidation: a case study for polystyrene. Environ. Pollut. 269, 116168.
Kim, S.H., Kwak, S.-Y., Suzuki, T., 2006. Photocatalytic degradation of flexible PVC/TiO2
nanohybrid as an eco-friendly alternative to the current waste landfill and dioxin-
Data availability emitting incineration of post-use PVC. Polymer 47, 3005–3016.
Lapointe, M., Farner, J.M., Hernandez, L.M., Tufenkji, N., 2020. Understanding and
Data will be made available on request. improving microplastic removal during water treatment: impact of coagulation and
flocculation. Environ. Sci. Technol. 54, 8719–8727.
Li, S., Wang, P., Zhang, C., Zhou, X., Yin, Z., Hu, T., Zhu, L., 2020. Influence of
Acknowledgments polystyrene microplastics on the growth, photosynthetic efficiency and aggregation
of freshwater microalgae Chlamydomonas reinhardtii. Sci. Total Environ. 714,
136767.
The authors acknowledge the National Natural Science Foundation Liao, Y-l, Tang, Q-x, Yang, J-y, 2023. Microplastic characteristics and microplastic-heavy
of China (52170071) and the Natural Science Foundation of Guangdong metal synergistic contamination in agricultural soil under different cultivation
Province (2022A1515011909). modes in Chengdu, China. J. Hazard Mater. 459, 132270.
Liu, F., Zhang, C., Li, H., Offiong, N.-A.O., Bi, Y., Zhou, R., Ren, H., 2023a. A systematic
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