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The Impact of Aging on the Physicochemical Properties, Environmental Processes and Toxic Effects of Microplastics

Yulong Wang , Yue Li , Fengbang Wang , Maoyong Song

Progress in Chemistry ›› 2025, Vol. 37 ›› Issue (1) : 46 -58.

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Progress in Chemistry ›› 2025, Vol. 37 ›› Issue (1) : 46-58 DOI: 10.7536/PC240707
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The Impact of Aging on the Physicochemical Properties, Environmental Processes and Toxic Effects of Microplastics
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Abstract

Microplastic pollution has become a major environmental issue of global concern. Microplastics can undergo aging under various environmental conditions. The aging process will change the physical and chemical properties of microplastics, thereby leading to changes in their environmental behaviors and toxicities. Therefore, exploring the aging process and mechanism of microplastics is of significance for understanding the environmental processes and health risks of microplastics. This article focuses on the aging process of microplastics in the environment and reviews it from the aspects of aging pathways, influencing factors, interactions with pollutants, release of chemical substances, and changes in toxicities. It also looks forward to the existing challenges and future research directions in the current studies on microplastic aging.

Contents

1 Introduction

2 Pathways of microplastics aging

2.1 Physical aging of microplastics

2.2 Chemical aging of microplastics

2.3 Biological aging of microplastics

2.4 Artificial aging of microplastics

3 The factors influencing microplastics aging

3.1 The impact of physical and chemical properties on microplastics aging

3.2 The impact of environmental conditions on microplastics aging

4 The impact of aging on microplastics

4.1 The impact of aging on the physical and chemical properties of microplastics

4.2 The impact of aging on the interaction between microplastics and pollutants

4.3 The impact of aging on the release of chemicals from microplastics

4.4 The impact of aging on the toxicities of microplastics

5 Conclusions and perspectives

Graphical abstract

Keywords

microplastics / aging / influencing factors / pollutants loading / additives leaching / toxic effects

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Yulong Wang, Yue Li, Fengbang Wang, Maoyong Song. The Impact of Aging on the Physicochemical Properties, Environmental Processes and Toxic Effects of Microplastics. Progress in Chemistry, 2025, 37(1): 46-58 DOI:10.7536/PC240707

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1 Introduction

Plastics are widely used in various fields such as agriculture, industry, construction, and people's daily lives. In 2019, the global annual production of plastics reached 460 million tons and shows a trend of increasing year by year. The Organization for Economic Co-operation and Development (OECD) predicts that by 2060, the annual production of plastic products worldwide will reach 1.2 billion tons[1]. However, due to issues related to production, use, and management, a large amount of plastic products end up in the environment, becoming "white pollution." Data indicates that only 9% of plastic waste is recycled, 19% is incinerated, nearly 50% goes into landfills, and the remaining 22% is discarded and scattered in the environment[1]. It is estimated that by 2050, about 120 billion tons of plastic waste will exist in landfills or the natural environment[2].
Plastic in the environment, under certain conditions (such as pulling, squeezing, friction, ultraviolet radiation, and biological factors), can break down into smaller fragments and particles. Scientists refer to these plastic fragments or particles that are less than 5 mm in size as microplastics. Microplastics can further generate even smaller particles; those with a size less than 1 µm are typically called nanoplastics[3-4]. Microplastics are ubiquitous in the environment, and their presence has been detected in soil, water bodies, the atmosphere, and living organisms[5-6]. At the second United Nations Environment Assembly in 2015, microplastic pollution was listed as the second major scientific issue in the field of environmental and ecological research, making it a significant global environmental problem on par with global climate change and ozone depletion. Studies have shown that humans and other organisms can be exposed to microplastics through food, drinking water, and respiration, leading to potential toxic effects, including immunotoxicity, genotoxicity, developmental toxicity, neurotoxicity, and oxidative stress[7-8], and may increase the risk of non-communicable diseases in humans[9].
Microplastics in the environment can undergo aging under the influence of mechanical forces, light, high temperatures, and microorganisms[10]. Aging alters the physicochemical properties of microplastics, including particle size, shape, surface groups, and elemental composition. For a long time, plastics were considered to be an inert material. Aging makes the properties of microplastics more active, not only affecting their migration and transformation processes in the environment but also influencing their interactions with other substances in the environment (such as heavy metals and other pollutants)[11]. In addition, aging can lead to the leaching of additives and intermediates from microplastics, increasing their toxic effects and ecological risks[12-13].
There are many types of microplastics, which can be categorized based on the type of plastic into polyvinyl chloride (PVC), polypropylene (PP), polyester (PET), polyamide (PA), polyurethane (PU), polyethylene (PE), and polystyrene (PS), among others. Therefore, the aging processes and influencing factors for different types of microplastics vary. This paper reviews recent research on the aging of microplastics to gain a deeper understanding of the processes and characteristics of microplastic aging, particularly the impact of aging on their physicochemical properties and toxicity.

2 Aging Methods Of Microplastics

The aging process of microplastics in the environment can be divided into physical aging, chemical aging, and biological aging (Figure 1).

2.1 Physical Aging Of Microplastics

Microplastics in the environment can break down into smaller particles under the influence of various forces, and when the size of the broken-down microplastics reaches the nanoscale, they form nanoplastics[14]. These forces include shear and tensile forces generated by waves and turbulence, frictional forces from rocks and soil, and collision forces between particles[15]. After sampling and analyzing microplastics on beaches, it was found that collisions cause microplastic particles to become nearly round. This physical aging process is also an important factor in the formation of surface textures on microplastics[16]. Physical aging is a major fragmentation pathway for microplastics in marine environments, and the resulting small plastic particles are more likely to reach open waters[17]. Physical aging also widely occurs in daily human life, with fabrics, food packaging, protective equipment, and care products generating large amounts of microplastics through this process[18⇓⇓-21]. When microplastics enter wastewater treatment plants, they can further fragment under mechanical stress. Research has found that a four-blade mechanical impeller can break down microplastics of about 200 μm into nanoplastic particles of about 100 nm in size at an energy density of 100 kJ∙L-1[22].

2.2 Chemical Aging Of Microplastics

Ultraviolet light, high temperatures, and reactive oxygen species (ROS) can cause chemical aging of microplastics.
Photo-aging is an important pathway for the chemical aging of microplastics, especially since ultraviolet radiation has a particularly significant effect on the aging of microplastics[23]. As shown in equations 1 to 7, chemical bonds in the carbon chains of microplastics can absorb light energy to produce free radicals. These free radicals react with oxygen to further generate peroxyl radicals, leading to chain scission or cross-linking, and ultimately forming more inert products[23-24].
Initiator → R i ⋅
R i ⋅ + O 2 → R i OO ⋅
R i OO ⋅ +RH → R i OOH+R ⋅
R ⋅ + O 2 → ROO ⋅
ROO ⋅ +RH → ROOH+R ⋅
R ⋅ +R ⋅ → R − R
R ⋅ +ROO ⋅ → ROOR
for microplastics in seawater, UV aging inhibits the vertical migration of hydrophobic microplastics such as PE and polytetrafluoroethylene (PTFE), but promotes the vertical migration of hydrophilic microplastics such as polymethyl methacrylate (PMMA)[25], thus leading to different long-term behaviors of microplastics with varying wettability in aquatic environments.
Thermal aging is another important pathway for the chemical aging of microplastics. Similar to the principle of photoaging, high temperatures cause the chemical bonds between microplastic molecular chains to dissociate, leading to the generation of free radicals as polymer chains break and initiating oxidation (Equations 8-15)[23,26].
( R ) n − R → ( R ) n − R ⋅
( R ) n − R ⋅ → ( R ) n − 1 − R ⋅ + R
R ⋅ + R ⋅ → R − R
R ⋅ + R O ⋅ → R O R
R ⋅ + R O O ⋅ → R O O R ⋅
R O ⋅ + R O ⋅ → R O O R
R O ⋅ + R O O ⋅ → R O R + O 2
R O O ⋅ + R O O ⋅ → R O O R + O 2
some studies have applied thermal treatment (at higher temperatures) to alleviate microplastic pollution in sludge[27]. The results of Sun et al.[28] showed that when the temperature reached 500 °C, the microplastic content in the sludge decreased from 550.8 to 960.9 particles·g-1 to 1.4 to 2.3 particles·g-1, and no plastic particles with a size between 10 and 50 μm were detected.
ROS is considered a key factor in the chemical aging of microplastics. ROS can initiate chain reactions by extracting H atoms or electrons from polymer chains, leading to the fragmentation of the polymer chains (Equations 16~19)[26,29].
R H → R ⋅
R ⋅ + O 2 → R O O ⋅
R O O ⋅ + R H → R O O H + R ⋅
R O O H → R O ⋅ + H O ⋅
research has found that under the influence of ROS, rainwater facilities containing different types of plastics can release a large number of microplastic particles, and there is a positive correlation between aging time and the amount of microplastics released[30]. Under ultraviolet light conditions, dissolved organic matter (DOM) can promote electron transfer to produce ROS, thereby accelerating the aging of microplastics[31].
Advanced oxidation processes (AOPs) have played a crucial role in the degradation of microplastics due to the generation of a large amount of reactive species (e.g., •OH). These reactive species can break down microplastics into small molecular intermediates and even further degrade them into CO2 and H2O[32]. Fenton oxidation is a common AOP[33]. Duan and Wang et al.[34] used a hydrothermal coupling Fenton system to decompose ultra-high molecular PE, achieving a weight loss rate of 95.9% for PE after 16 hours and a mineralization rate of 75.6% after 12 hours, with a significant amount of •OH generated during the process (Equations 20-21)[33].
F e 2 + + H 2 O 2 → F e 3 + + H O ⋅ + O H −
F e 3 + + H 2 O 2 → F e 2 + + H O O ⋅ + H +
in addition to Fenton oxidation, photocatalysis has also received significant attention in the field of plastic degradation. In photocatalysis, semiconductors absorb energy from a light source and get excited, generating ROS such as •OH and •O2- (produced from H2O), which can cause microplastics to undergo reactions such as cleavage and cross-linking, ultimately degrading them into CO2 (Equations 22-28)[35-36].
Photocatalyst + h υ → h V B + + e C B −
O 2 + e C B − → ⋅ O 2 −
⋅ O 2 − + H 2 O → H O O ⋅ + O H −
2 H O O ⋅ → O 2 + H 2 O 2
H 2 O 2 + h υ → 2 H O ⋅
h V B + + H 2 O → H O ⋅ + H +
R H + H O ⋅ + ⋅ O 2 − → C O 2 + H 2 O + O t h e r   p r o d u c t s
electrocatalysis, as another AOP technology, accelerates the transfer of charges at the interface between the electrode and the electrolyte by applying an electric field on the electrode surface, thereby promoting the degradation of microplastics[37]. Additionally, the combination of multiple technologies can produce more effective results. In photocatalysis, the easy formation of CO2, nanoplastics, and organic complexes leads to lower selectivity of products[38], while the efficiency of electrocatalysis is limited by the hydrophobic surface of plastics[39]. By combining photocatalytic and electrocatalytic technologies (i.e., using light energy to drive electrocatalytic reactions in photoelectrocatalysis), high-efficiency, high-selectivity, and sustainable degradation of microplastics can be achieved[37,39]. Espinoza-Montero et al.[40] achieved a high degradation efficiency of 89.91% ± 0.08% for high-density polyethylene (HDPE) microplastics in water using a TiO2-modified boron-doped diamond photoanode with a current density of 6.89 mA∙cm-2 over 10 hours.

2.3 Biological Aging Of Microplastics

Bacteria, fungi, algae, and other microorganisms are widely present in nature. Microplastics not only provide a habitat for the colonization and growth of microorganisms[41-42], but also offer a carbon source for microbial growth[43-44]. The biodegradation of microplastics can roughly be divided into processes such as colonization, depolymerization, assimilation, and mineralization[45]. Microorganisms can attach to the surface of microplastics for growth and reproduction[46], and release extracellular enzymes for the depolymerization of microplastics, generating low-molecular-weight oligomers, dimers, or even monomers[47]. Through assimilation and mineralization, microorganisms metabolize these low-molecular-weight polymers into substances such as CO2 and H2O[48⇓-50]. The biodegradation of microplastics provides an approach to remediate microplastic pollution. Compared with other microorganisms, fungi have stronger adsorption, colonization, survival capabilities, and the ability to secrete various degrading enzymes, making them more effective in the degradation of microplastics[51]. However, the biodegradation of microplastics may be a long and slow process. For example, the microbial degradation of PE requires 100-200 years in humic lake water, 300-4000 years in clear lake water, and 2000-20,000 years in artificial freshwater[52]. Moreover, the biodegradation process of microplastics might also produce a large amount of smaller micro/nano plastics. Research by Shao et al.[53] showed that marine bacteria Alcanivorax xenomutans and Halomonas titanicae generate a significant amount of micro/nanoplastics while degrading PS microplastics, potentially exacerbating the pollution of micro/nanoplastics in the ocean.
Some insects and zooplankton can also participate in the biodegradation of microplastics. After the action of Chironomus sancticaroli larvae, the average particle size of PS microplastics can decrease from 24.5 μm to 16.4 μm. This reduction may be due to the combined effects of digestive enzymes within the larvae, symbiotic bacteria, and the friction between PS microspheres and sand in the digestive tract[54]. Additionally, similar cases have been observed in mealworms[55] and earthworms[56]. Some zooplankton, such as Antarctic krill (Euphausia superba)[57] and rotifers[58], can convert microplastics into nanoplastics. It is noteworthy that biodegraded micro- and nanoplastics, due to the biofilm on their surfaces, exhibit unique physicochemical properties, which may lead to increased potential health hazards and ecological risks[59].
Currently, biodegradable plastics are becoming green alternatives to traditional plastics. Biodegradable plastics refer to plastics that can be converted into CO2, H2O, CH4, and biomass through the action of enzymes and microorganisms, including polyhydroxyalkanoates (PHA), polylactic acid (PLA), and polybutylene adipate terephthalate (PBAT)[60]. Compared with traditional microplastics, biodegradable plastics may degrade more easily into micro- and nanoplastics in the environment and release additives, and these microplastics have more oxygen-containing functional groups on their surfaces, allowing them to better carry pollutants[61]. In terms of microbial colonization, the biomass loaded on the surface of non-degradable plastics is lower than that on degradable plastics, but the bacteria and fungi loaded are more diverse[62].

2.4 Artificial Aging Of Microplastics

The natural aging of microplastics is a complex and dynamic process, with multiple aging effects often occurring simultaneously under most environmental conditions, influenced by a myriad of intricate factors such as time, climate, and geographical location[63]. In addition to these difficult-to-control factors, the experimental cycle for natural aging is quite long[64]. Therefore, researchers investigate the impact of specific factors on the aging of microplastics through artificial simulation conditions in the laboratory.
Common artificial aging techniques include light exposure and chemical oxidation[63]. Compared to natural aging, which can take decades or even centuries, artificial aging can cause significant changes in microplastics within just a few days or months, greatly accelerating the aging process[65]. In the study by Freitag et al.[66], the laboratory radiation intensity was 5.2 times that of the average irradiation intensity in Central Europe. Therefore, the laboratory aging times of 200, 400, and 600 hours corresponded to natural aging times of 43, 86, and 130 days, respectively. Although laboratory simulations cannot fully replicate the natural aging behavior of microplastics, they can be used to assess and predict the cycles and processes of microplastic aging[64]. By coupling various conditions, the gap between artificial simulations and natural conditions can be minimized. For example, Briffa et al.[67] constructed a test chamber to simulate the real aging environment of the Mediterranean coast by adjusting parameters such as UV irradiation, aeration, and temperature.

3 Factors Affecting The Aging Of Microplastics

The aging process of microplastics is influenced by a combination of various factors, mainly including the physical and chemical properties of the microplastics themselves and environmental conditions (Figure 2).

3.1 The Impact Of Physicochemical Properties Of Microplastics On Aging

The physical properties of microplastics include particle size, crystallinity, and color. Compared to larger-sized microplastics, smaller-sized microplastics are more easily oxidized due to their larger specific surface area. The study by Gu[68] shows that the rate of photo-aging of PVC increases with decreasing particle size. However, the research by Paik and Kar[69] indicates that small-sized PE nanoplastics are more difficult to age due to their higher crystallinity and lower entropy.
The crystallinity of microplastics reflects the proportion of their crystalline regions, which can be classified into crystalline phase, semi-crystalline phase, and amorphous phase[70]. A certain degree of crystallinity makes microplastics more robust, but excessively high crystallinity reduces their elasticity and increases brittleness[71], making them more prone to fragmenting into smaller particles during natural wear and tear[72].
The color of microplastics also affects their aging. Pigments with longer wavelengths, such as red or yellow, can absorb higher-energy short-wavelength light, while pigments with shorter wavelengths, such as blue, absorb lower-energy long-wavelength light. The longer the wavelength of the plastic color, the stronger the light absorption, the lower the ultraviolet transmittance, and the slower the photo-aging rate. Therefore, fragments of red plastic are usually larger than those of blue plastic[73]. Additionally, color may also influence the colonization of microorganisms on microplastics. For example, biofilms colonizing blue microplastics have a higher functional diversity compared to those colonizing transparent or yellow microplastics[74], and this varying degree of colonization further affects the biological aging of microplastics.
Compared to microplastics with main chains composed of O atoms, N atoms, and other atoms, microplastics with C atoms as the main chain are more difficult to age[75-76]. For example, the backbone chain of PE is composed of non-hydrolyzable C—C single bonds, making it difficult to be photodegraded due to the lack of chromophores in the UV-visible spectrum[77], and can persist for a long time in the natural environment. Microplastics with different molecular compositions have different wettability, and it is difficult for microorganisms to form biofilms on highly hydrophobic microplastic surfaces, thereby inhibiting their degradation[78]. Additives released during the aging process of microplastics may promote their degradation to some extent. The research results of Rivaton and Sleiman et al.[79] showed that PS films containing brominated flame retardants (BFRs) have a higher photo-aging rate than pure PS films, and the addition of BFRs also altered the degradation mechanism of PS, producing 14 types of brominated photoproducts.

3.2 The Impact Of Environmental Conditions On The Aging Of Microplastics

Environmental conditions can significantly affect the aging of microplastics (as shown in Table 1). The intensity and wavelength of light have a significant impact on the aging of microplastics. Research has found that microplastics with similar sources in beach sediments exhibit different degrees of aging due to exposure to different intensities of light[80]. When PVC is exposed to ultraviolet light of different wavelengths, the photo-aging efficiency of PVC under UVC irradiation is higher than under UVA and UVB conditions, and the intensity of ROS and leaching toxicity produced under UVC irradiation is the highest[81].
Oxygen is involved in the generation of ROS during the aging process of microplastics, effectively promoting the aging of microplastics[82]. In the photo-aging process of PVC, the concentration of Cl- released under aerobic conditions is greater than that released under anaerobic conditions[68]. Zhou et al.[83] believe that, under alternating anaerobic-aerobic conditions, the degree of aging of PS in sediments is greater than under static aerobic or static anaerobic conditions, due to the production of more ROS in the sediments under anaerobic-aerobic conditions. In the biological aging of microplastics, oxygen, as an electron acceptor for microbial enzymes, can influence microbial metabolism[84-85]; under anaerobic conditions, the addition of reductants can promote the rapid aging of microplastics[86].
Temperature can affect the aging rate of microplastics by influencing the kinetic processes of their molecular chain reactions[87], and under certain temperature conditions, it can also influence the release of additives and other substances[88]. In the per-sulfate and hydrothermal co-treatment of sludge, an increase in temperature led to the melting deformation of PP microplastics, as well as changes in roughness and crystallinity, thereby exacerbating the aging of PP[89]. Additionally, temperature can affect the biological aging of microplastics by influencing enzyme activity and microbial community structure. The results of a study by Zhou et al.[90] showed that the degradation efficiency of PS in super-thermophilic composting (70 ℃) was 7.3%, which is 6.6 times higher than that under traditional thermophilic composting conditions (40 ℃). This is because high temperatures enhance the oxidative capabilities of microorganisms such as Thermus, Bacillus, and Geobacillus.
The aging of microplastics in the environment is also influenced by other environmental factors. Compared to low salinity, high salinity more significantly promotes the photo-aging of PS microplastics in solutions containing humic acid (HA)[91]. Halide ions such as Cl- and Br- can significantly affect the photo-aging process of microplastics[92-93], but the impact of inorganic ions on the aging of microplastics is more complex, as they may participate in radical reactions during the photo-aging process of microplastics[94]. Environmental pH can influence the aging process of microplastics by interfering with microbial activity; a slightly alkaline soil environment may be conducive to microbial growth, thereby promoting the aging of PE[95]. Lower pH can promote the weakening of polymer bonds in PE that has been soaked in seawater, leading to distortion, dissolution, and peeling[96]. When microplastics are subjected to photo-aging in simulated seawater, a decrease in pH accelerates the aging of microplastics, though the extent of this effect varies depending on the type of polymer[97]. Organic substances in the environment, such as hyaluronic acid and vitamin C, can promote the generation of ·OH, thereby accelerating the photo-aging of PS microplastics and nanoplastics[98]. HA and fulvic acid (FA) can inhibit the aging of microplastics by scavenging ROS[99] or by blocking UV light from reaching the surface of the microplastics[82]. However, some studies have shown that low molecular weight FA (FA < 1 kDa) can promote the photo-aging of PS microplastics due to its strong redox capacity and electron donor ability[100]. Some pesticides, such as paraquat, can accelerate the aging of PE by generating superoxide[101]. The presence of other substances in the environment, such as pyrite[102], kaolinite, and montmorillonite[103-104], can also promote the aging of microplastics.

4 The Impact Of Aging On Microplastics

4.1 Aging-Induced Changes In The Physicochemical Properties Of Microplastics

Aging can significantly alter the size, morphology, and surface characteristics of microplastics. When PS is aged under O3 conditions, its average particle size can be reduced to half of what it was before aging[105]. After 60 days of photo-aging, low-density polyethylene (LDPE) and PP develop mud-like and parallel cracks on their surfaces, and PP fragments are observed between the cracks on the PP surface[106]. Under simulated beach conditions, the synergistic effect of ultraviolet light and sand abrasion can lead to the dissociation of C—C and C—H bonds in the main chain of microplastics, further causing the microplastics to become brittle and crack[107]. Aging also affects the color of microplastics; during UV aging, PS changes from white to yellow[108]. After UV aging, styrene-butadiene-rubber microplastics (mSBR) change from a smooth surface to a rough one, and their color shifts from nearly white to yellow, with the color becoming deeper as the aging time increases[109]. The reason for the color change in microplastics before and after aging may be due to the transformation of thermal stabilizers (such as phenolic antioxidants) into yellow quinone organic compounds[110], or it could be related to the competition between changes in the length of polyene chains and photobleaching[111].
Aging can alter the elemental composition and surface functional groups of microplastics. After PVC is aged by H2O2, the content of Cl increases, while the contents of Ca and O decrease[112]. After PP is irradiated by ultraviolet light, the mass percentage of O increases from 2.80% to 20.95%[113]. In terms of functional groups, aging can produce oxygen-containing functional groups such as hydroxyl, carbonyl, and aldehyde on the surface of microplastics. The increase in these oxygen-containing functional groups enhances the hydrophilicity of microplastics[114]. After PS is exposed to ultraviolet light, the oxygen-containing functional groups on its surface increase[115]. Under ultraviolet light, the C—H bonds on the surface of mSBR dissociate and form electron vacancies, which are then further oxidized into hydroxyl and carbonyl groups[109]. The changes in functional groups of microplastics vary with different aging pathways. After PE undergoes photo-aging and thermal aging, the concentrations of oxidation products (such as ketones, carboxylic acids, and esters) differ. This is because, during photo-aging, the Norrish reaction leads to the conversion of ketones into new unsaturated groups; whereas, in thermal aging, the lack of the Norrish reaction results in the accumulation of ketones[116]. Additionally, thermal aging does not necessarily cause significant changes in the structure of microplastics. Esterhuizen et al.[117] conducted thermal aging of polycarbonate (PC) at 70 ℃ for up to 160 days, but no significant changes were observed in the structure of the microplastics.

4.2 The Impact Of Aging On The Pollutant Load Capacity Of Microplastics

Microplastics can act as carriers for various pollutants in the environment, involving interactions such as hydrophobic effects, electrostatic interactions, hydrogen bonds, van der Waals forces, and π-π interactions[118]. Studies have found that the concentration of chemical pollutants on the surface of microplastics is six times that in the surrounding water[119]. The aging process alters the physicochemical properties of the microplastic surface, thereby affecting its ability to carry pollutants.
The adsorption of heavy metals by microplastics mainly includes physical adsorption, coordination, electrostatic attraction, hydrophobic interactions, and cation-π bond interactions[120-121]. After aging, the specific surface area of microplastics increases, it is easier to form a negative surface charge, and the hydrophilicity increases. These changes in conditions may be beneficial for the adsorption of heavy metals. The average saturated adsorption capacities of Cr(VI) by photo-aged PA, PS, and PE increased from 730.69, 146.11, and 75.61 μg∙g-1 to 736.31, 318.75, and 136.78 μg∙g-1, respectively, which is mainly attributed to the enhancement of electrostatic interactions after aging[122]. Fenton or H2O2 aging can significantly enhance the adsorption capacity of PS for Cd2+, mainly because more Cd2+ adsorption sites are exposed on the surface of aged PS. Research by Lin and Lan et al.[123] showed that O3 aging increased the hydrophilicity and negative charge on the surface of microplastics, thereby increasing their adsorption capacity for Hg(II) by 4 to 20 times compared to unaged microplastics. Tan et al.[124] studied the adsorption of Pb(II) by naturally aged microplastics in the Xiangjiang River. The results showed that the organic film on the surface of the aged microplastics played an important role in the adsorption of Pb(II). These organic films, rich in oxygen-containing functional groups such as carboxyl and hydroxyl, could adsorb Pb(II) through electrostatic forces. Breider et al.[125] compared the adsorption of Cu by PS aged with O3, a solar simulator, and lake water. Although the oxidation degree of PS aged in the lake was the lowest, its adsorption capacity for Cu was the highest. This might be due to the precipitation of elements such as Si, Al, Mg, and Fe from the lake onto the PS surface, forming metal oxides conducive to Cu adsorption.
Microplastics can interact with organic substances through hydrophobic interactions, surface coordination, van der Waals forces, hydrogen bonds, and π-π interactions, among which hydrophobic interactions play a dominant role[121]. Generally, the oxygen-containing groups formed on the surface of microplastics after aging are not conducive to their adsorption of hydrophobic organic pollutants. The study by Junck et al.[126] showed that aged PE has reduced hydrophobicity and forms negative charge sites on its surface, thus decreasing its adsorption capacity for the hydrophobic herbicide terbuthylazine. Li et al.[127] compared the adsorption of levofloxacin (LEV) by three types of microplastics: PE, PS, and PA. They found that PA had the strongest adsorption capacity for LEV, which was attributed to the polar-polar interactions between PA and LEV, as well as the hydrogen bonds formed between the amide groups of PA and the carbonyl groups of LEV. Photo-aging significantly enhanced the adsorption of LEV by the three types of microplastics, especially PS, where the adsorption enhancement was the most significant after aging. This is because the wrinkles and cracks produced on the surface of PS after aging provided a large number of adsorption sites for LEV and enhanced the π-π interactions between the benzene rings in PS and LEV. Liu et al.[128] studied the adsorption of tetracycline hydrochloride (TC-HCl) and cefalexin (CFX) by PE microplastics cultured in lake water. The adsorption rate of the two antibiotics by PE was related to surface diffusion, intraparticle diffusion, and film diffusion processes. The biofilm present on the surface of the lake-aged PE increased the specific surface area, produced C=O groups, and reduced the surface Zeta potential, thereby enhancing the adsorption of antibiotics by the microplastics. Kang et al.[129] exposed PP to air and sunlight for aging. Compared to unaged PP, the aged PP exhibited stronger adsorption capacity for nonylphenol due to its larger specific surface area, more oxygen-containing functional groups and adsorption sites, and stronger hydrogen bonding.

4.3 The Impact Of Aging On The Release Of Chemicals From Microplastics

Additives are chemicals that are intentionally added during the plastic production process to improve the quality and performance of plastic products, in order to resist the impact of O3, microorganisms, radiation, and humidity on plastic products[130]. Commonly used additives include phthalates (PAEs), bisphenol A (BPA), metals, and other compounds. During the aging process of microplastics, various additives are released into the environment or enter organisms as their polymer chains break down (Figure 3[131]).
Most research on the release of heavy metals from microplastics has focused on materials such as PET, PVC, PP, PE, and PS, with PVC releasing a higher amount of heavy metals (with higher concentrations of Ca, Cu, Zn, and Sb)[132]. During the H2O2 chemical aging process of PVC, the release of various metals including Cr, Ni, Pb, Cu, Zn, Cd, and Mn increases with the rise in H2O2 concentration[112]. Qu et al.[133] conducted studies on the release of Cd2+ from PP containing cadmium pigments. Under dark conditions, PP particles ranging from 2.00 to 3.50 mm hardly released any Cd2+, while particles smaller than 0.15 mm released a small amount of Cd2+; under simulated sunlight, PP particles smaller than 0.15 mm released a large amount of Cd2+, which originated from the photodissolution of pigments due to the reaction between photo-generated holes and the pigment lattice. Liu et al.[134] investigated the aging process of microplastics under simulated ultraviolet light, natural light, and in natural water bodies. Under simulated ultraviolet light, the zinc concentration in microplastics decreased with increasing aging time, showing a greater tendency to leach heavy metals. However, the zinc concentration in microplastics aged under natural light and in natural water showed significant fluctuations, attributed to the simultaneous release of heavy metals during the aging process influenced by light, water, and microorganisms, and the adsorption effect of biofilms formed on the surface of the microplastics.
The aging process of microplastics is often accompanied by the release of organic pollutants. When waste cathode ray tube plastic casings are placed in a solution containing humic substances, the concentration of polybrominated diphenyl ethers (PBDEs) in the plastic leachate ranges from 14 to 200 μg∙L-1(even though PBDEs have relatively hydrophobic physicochemical properties)[135]. During the advanced oxidation process of PS microplastics with UV light and sodium percarbonate, 15 oxidation intermediates, including styrene, acetophenone, benzaldehyde, and acetic acid, were detected[136]. Lin et al.[137]studied the chlorination aging process of PS and PE, finding that these microplastics release organic substances with the potential to form disinfection by-products. The release of organics during the aging of PS is more significant, possibly due to the lower chlorine resistance of PS, which leads to the fragmentation of microplastic particles during chlorination, promoting the release of organics. Another reason may be the difference in additives in PS and PE, as the lack of antioxidants in microplastics can accelerate the release of organics[138]. Some microplastics contain large amounts of organophosphate esters (OPEs), and Xiao et al.[139]believe that more than 60% of OPEs (and even 98% of highly hydrophobic OPEs) remain in the polymer and are slowly released over a long period. Hong et al.[140]conducted experiments on the aging of expanded polystyrene (EPS) in dark/light chambers and in seawater floating on the surface of a bay in Korea, comparing the leaching of hexabromocyclododecanes (HBCDDs). After 7 days of exposure, 37% of HBCDDs leached from EPS in the dark chamber, while 49% leached from EPS in the light chamber. During the seawater aging process, under the influence of multiple factors such as ultraviolet light, temperature, microorganisms, and wave action, 61% of HBCDDs leached from the EPS.
Currently, research on the release of chemicals from microplastics during biological aging is still limited, especially regarding the role of the ecological corona on the surface of microplastics. For example, the biofilm on the surface of microplastics can potentially act as a barrier affecting the leaching of additives, or it may utilize plastic as a carbon source, thereby accelerating the biodegradation of microplastics and increasing the release of chemicals[141]. Furthermore, the leaching of additives can further influence the interactions between microplastics and environmental microorganisms, making the process of chemical release from microplastics even more complex.

4.4 The Impact Of Aging On The Toxic Effects Of Microplastics

Research has shown that microplastics can trigger a variety of toxic effects, including metabolic disorders, inflammation, oxidative stress, and cell apoptosis[142-143]. After aging, the physicochemical properties of microplastics change, leading to alterations in their toxic effects. The toxic effects caused by aged microplastics can be categorized into: the inherent toxic effects of the microplastics themselves, the combined toxic effects from carrying other environmental pollutants, and the toxic effects of additives and intermediates released during the aging process (Figure 4).
The size of microplastics plays a critical role in their biological uptake. For example, 1 μm is a common size for microplastics to be captured by the gastric filters of crustaceans[144], while microplastics ranging from 11 to 700 μm are more likely to be ingested by amphipods[145]. Research by Vroom et al.[146] showed that after natural seawater aging, PS microplastics were ingested by marine plankton at a higher rate and proportion compared to unaged PS. This may be due to the formation of a biofilm on the surface of aged PS (which might contain substances similar to those found in the organisms consumed by plankton), thereby increasing the likelihood of ingestion. The aging of microplastics also affects their transport, accumulation, and metabolic processes within organisms. For instance, the particle size of microplastics to some extent determines their biodistribution characteristics in various organs; it is generally believed that smaller plastic particles are more easily transported to multiple organs and can penetrate cells more readily[147]. Zou et al.[148] subjected PA microplastics to photo-aging in water solutions containing HA and FA, and the results indicated that the aged PA exacerbated toxicity to zebrafish primarily through changes in its physicochemical properties rather than through leachates. Unaged PA was mainly distributed in the intestines of zebrafish, whereas aged PA could be detected in the intestines, pancreas, and liver, possibly because the smaller nanoplastics formed after aging could more easily pass through the intestinal membranes. Additionally, the aged PA not only led to reduced body length and weight, structural and functional damage to the intestines, increased ROS levels, and enhanced oxidative stress in zebrafish, but also downregulated genes related to triglyceride resynthesis and transport (such as cd36, dgat1a, and dgat2), thereby disrupting lipid metabolism. Moreover, changes in the functional groups on the surface of microplastics can also affect their toxic effects. Aging of PS resulted in significant nuclear shrinkage, disruption of F-actin structures, increased basal glycolysis rates, and decreased monolayer barrier integrity in A549 lung cells[149], which may be related to the increased content of C—O bonds and carboxyl groups on the surface of UV-aged PS microplastics. Wang et al.[150] studied the toxic effects of aged PS, PS-NH2, PS-COOH, and PMMA on Isochrysis galbana. After aging, PS had a greater detrimental effect on I. galbana (such as increased oxidative stress, inhibited growth, and altered energy metabolism), while PS-NH2 and PS-COOH exhibited lower toxicity due to the loss of functional groups. In contrast, PMMA showed strong resistance to aging due to its inherent structure and the high concentration of plasticizers it contains.
Aged microplastics can carry more environmental pollutants, thereby producing a combined toxicity to organisms. Wang et al.[151]'s research shows that aged PE can cause internal wear and mechanical damage to the digestive tract of the cladoceran Moina monogolica, and the Cd carried by PE may be released in the organism's digestive tract, producing a higher toxic effect through intracellular molecular targets. This composite exposure not only affects the reproduction of the organism but also causes malnutrition (such as reduced protein, carbohydrate, and lipid content) or even death in offspring. Similarly, the complex of aged PE carrying Ag has a stronger toxic effect on duckweed (Lemna minor) and water fleas (Daphnia magna) than aged PE alone, primarily due to the release of Ag from the complex (especially in acidic media) rather than PE itself[152]. It is noteworthy that this combined exposure does not necessarily produce a synergistic toxic effect. For example, photo-aged PET and Pb2+ can both inhibit the growth and reproduction of Chlorella pyrenoidosa when exposed individually (causing physical and chemical stress, respectively). When they coexist without adsorption, they can inhibit the growth of Chlorella pyrenoidosa cells and damage their cell membranes and antioxidant systems. However, after PET adsorbs Pb2+, the chemical stress on Chlorella pyrenoidosa decreases (although physical stress still exists) due to the reduction in the concentration and activity of Pb2+ in water[153]. Aged microplastics can also produce toxicity to organisms in combination with organic pollutants. Zong and Song et al.[154] studied the combined toxicity of aged PS and ciprofloxacin (CIP) on Escherichia coli. The study found that aging increased the adsorption rate and amount of CIP by PS. The toxic effects of the combined exposure of CIP and aged PS include downregulation of ABC transporter expression, leading to cell membrane damage, affecting amino acid and lipid metabolism, thus impacting cell growth, cell membrane integrity, and cellular antioxidant stress capacity, trapping gyrase molecules during and after the double-stranded DNA cleavage stage, blocking DNA replication, and downregulating osmY, osmB, and osmC genes, causing osmotic imbalance. However, the inhibition rate of CIP on Escherichia coli was reduced due to the adsorption of CIP on aged PS during combined exposure. Yu and Yang et al.[155] investigated the toxic effects of hydrothermally aged PLA in sludge and its adsorbed volatile organic compounds on mouse macrophages. Interestingly, compared to unaged PLA, the PLA composites treated at 120 ℃ and 130 ℃ increased cell viability (by 21.99% and 27.31%, respectively), possibly because cells can use the organic matter on the surface of aged PLA as a carbon source; however, the PLA composites treated at 140 ℃ decreased cell viability (by 16.07%), possibly due to the release of toxic substances from the PLA composites at high temperatures, causing cytotoxicity.
The aging process of microplastics can lead to the release of additives and intermediates, which may pose certain ecological risks. When thermoplastic polyurethane (TPU) microplastics undergo ultraviolet aging and chlorination, the LC50 (half-lethal concentration) of the released organics on human hepatocellular carcinoma cells (HepG2) is only about 10% of that of the original TPU, indicating a significant increase in cytotoxicity[156]. Peng et al.[157] exposed Chlorella vulgaris to seawater leachates from photo-aged PE and PVC. By comparing the gene function, cell growth, and oxidative stress of the microalgae, they found that the toxicity to the microalgae was in the order of PVC leachate > PE > PE leachate > PVC. The PVC leachate had the strongest toxic effect on the microalgae, possibly due to the release of more substances (including Zn, farnesol isomer a, 2,6-di-tert-butyl-4-methylphenol, and methyl acetate ricinoleate, etc.) from aged PVC. Exposure to the leachates reduced the cell density, cell dry weight, and chlorophyll a content of the microalgae but enhanced their secretion of extracellular polymers and the oxidative stress kinase system. At the transcriptome level, PE and PVC leachates exerted toxicity on the microalgal cells by disrupting the ribosomal biogenesis process and affecting the interaction between the microalgae and pathogens, respectively. It is noteworthy that a longer aging process might also reduce the toxic effects of microplastics. For example, unaged PC and short-term aged PC could have adverse effects on the growth and chlorophyll concentration of cress (Lepidium sativum), but as the aging time increased, the toxicity of PC to cress decreased. This may be due to the potential reduction in the release of microplastic additives with increasing aging time[117].

5 Conclusion and Prospects

Aging is an inevitable environmental process for microplastics. The changes in physical and chemical properties brought about by the aging process can affect the environmental behavior and toxic effects of microplastics, increasing the uncertainty of their environmental fate and health risks. Although a large number of studies have been conducted on the aging process of microplastics and some important progress has been made, there are still many challenges in both research methods and theoretical understanding.
(1) The alteration of the physicochemical properties of microplastics is a key factor leading to changes in their environmental behavior and toxic effects. During the aging process, multiple physicochemical properties of microplastics change simultaneously. Therefore, clarifying the structure-activity relationship between different physicochemical properties of microplastics and their biological processes and toxic effects is crucial for revealing the key biological processes and induced toxic effects of microplastics under complex environmental conditions.
(2) Although there are currently various methods to characterize the physicochemical properties of microplastics after aging, most of these methods can only perform qualitative analysis and cannot conduct quantitative analysis. Therefore, how to accurately measure and characterize the physicochemical properties of microplastics before and after aging, such as the number of surface functional groups, is key to elucidating the "true" dose-effect relationship between microplastic exposure and toxic effects.
(3) In real environments, chemical substances such as heavy metals and persistent organic pollutants, as well as microorganisms, can interact with microplastics. These interactions not only affect the aging of microplastics but also influence their environmental behavior and toxicity, further increasing the complexity of the process. Therefore, research based on real environments will help to improve our understanding of the aging process, environmental behavior, and health risks of microplastics.

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Funding

National Natural Science Foundation of China(22241604)

National Natural Science Foundation of China(22125606)

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