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Abbreviation (ISO4): Prog Chem      Editor in chief: Jincai ZHAO

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Progress in Chemistry >

2025 , Vol. 37 >Issue 1: 46 - 58

DOI: https://doi.org/10.7536/PC240707

Microplastics Special Issue

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

  • Yulong Wang 1, 2 ,
  • Yue Li 1, 2 ,
  • Fengbang Wang 1, 2 ,
  • Maoyong Song , 1, 2, *
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  • 1 Key Laboratory of Environmental Nanotechnology and Health Effects, Research Center for Eco- Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
  • 2 University of Chinese Academy of Sciences, Beijing 100049, China
*e-mail:

Received date: 2024-07-10

  Revised date: 2024-11-12

  Online published: 2024-11-12

Supported by

National Natural Science Foundation of China(22241604)

National Natural Science Foundation of China(22125606)

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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

Key words： microplastics; aging; influencing factors; pollutants loading; additives leaching; toxic effects

Cite this article

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

1 introduction

Plastics are widely used in agriculture, industry, construction and people's daily life. In 2019, the global annual output of plastics has reached 460million tons, showing an increasing trend year by year. The organization for economic cooperation and development predicts that the global annual output of plastic products will reach 1.2 billion tons in 2060[1]However, due to the problems of production, use and management, a large number of plastic products enter the environment and become "white pollution". Data show that only 9% of plastic waste is recycled, 19% of plastic waste is incinerated, nearly 50% of plastic waste enters the landfill, and the remaining 22% of plastic waste is discarded and scattered in the environment[1]It is estimated that by 2050, about 12billion tons of plastic waste will exist in landfills or the natural environment[2]。
Under certain conditions (pull, extrusion, friction, UV irradiation, biology, etc.), plastics in the environment will break into smaller fragments and particles. Scientists call these plastic fragments or particles smaller than 5 mm micro plastics. Microplastics can also further produce smaller particles. Plastic particles smaller than 1 µ m are usually called nanoplastics[3-4]Micro plastics are ubiquitous in the environment. People have found the existence of micro plastics in soil, water, atmosphere and organisms[5-6]At the second United Nations Environment Conference in 2015, microplastics pollution was listed as the second largest scientific issue in the field of environmental and ecological science research, which made it a major global environmental issue alongside global climate change and ozone depletion. Studies have shown that people or other organisms can ingest microplastics through food, drinking water, breathing and other exposure routes and produce potential toxic effects, including immunotoxicity, genetic toxicity, developmental toxicity, neurotoxicity and oxidative stress[7-8]And may increase the risk of non communicable diseases[9]。
Microplastics in the environment can age under the action of mechanical force, light, high temperature and microorganisms[10]Aging will change the physical and chemical properties of microplastics, including particle size, shape, surface groups and element composition. For a long time, plastic has been regarded as an inert substance. Aging will make the properties of microplastics become active, which will not only affect their migration and transformation process in the environment, but also affect their interaction with other substances in the environment (such as heavy metals and other pollutants)[11]In addition, aging will also lead to the leaching of additives and intermediates in microplastics, increasing their toxic effects and ecological risks[12-13]。
There are many kinds of micro plastics, which can be divided into polyvinyl chloride (PVC), polypropylene (PP), polyester fiber (PET), polyamide (PA), polyurethane (PU), polyethylene (PE) and polystyrene (PS) according to the types of plastics. Therefore, different kinds of microplastics have different aging processes and influencing factors. This paper reviews the research work on the aging of microplastics in recent years, in order to understand the aging process and characteristics of microplastics, especially the effect of aging on its physical and chemical properties and toxic effects.

2 Microplastics aging mode

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

Fig. 1 Physical, chemical and biological aging of microplastics

2.1 Physical aging of microplastics

The micro plastics in the environment can be broken into smaller particles under the action of various forces. When the size of the micro plastics is in the nanometer scale, nano plastics are formed[14]These forces include shear force and tensile force generated by waves and turbulence, friction force generated by rocks and soil, and collision force between particles[15]After sampling and analyzing the micro plastics on the beach, it is found that the collision makes the micro plastic particles become nearly circular, and this physical aging process is also an important factor for the generation of micro plastic surface texture[16]Physical aging is the main fragmentation pathway of microplastics in the marine environment, and the small-size plastic particles produced are easier to reach the open water[17]Physical aging also occurs widely in human daily life. Cloth, food packaging, protective equipment and nursing products can produce a large number of micro plastics through the physical aging process[18⇓⇓-21]When the micro plastic enters the sewage treatment plant, it can be further broken under the action of mechanical stress. It is found that when the energy density is 100 kJ · L-1The four blade mechanical impeller can decompose the micro plastic of about 200 μ m into nano plastic particles with a particle size of about 100 nm[22]。

2.2 Chemical aging of microplastics

UV, high temperature and reactive oxygen species (ROS) can cause chemical aging of micro plastics.
Photoaging is an important way of chemical aging of microplastics, especially the aging effect of ultraviolet radiation on microplastics is particularly obvious[23]As shown in equations 1-7, the chemical bonds in the carbon chain of the micro plastic can absorb light energy to produce free radicals, which react with oxygen to further generate peroxy free radicals, leading to chain fracture or cross-linking, and finally produce 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 the micro plastics in seawater, UV aging inhibited the vertical migration of hydrophobic micro plastics PE and polytetrafluoroethylene (PTFE), but promoted the vertical migration of hydrophilic micro plastics polymethylmethacrylate (PMMA)[25]Therefore, the long-term behavior of microplastics with different wettability in water environment is different.
Thermal aging is another important way of chemical aging of microplastics. Similar to the principle of photoaging, high temperature makes the chemical bonds between the molecular chains of micro plastics dissociate, and with the breaking of the polymer chain, free radicals are generated and oxidation begins (formula 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
Heat treatment (higher temperature) has been used to alleviate micro plastic pollution in sludge[27]. sun et al[28]The results showed that when the temperature reached 500 ℃, the content of microplastics in sludge increased from 550.8 to 960.9 particles · G-1Reduced to 1.4~2.3 particles ・ G-1And no plastic particles with particle size between 10~50 μ m were detected.
ROS is considered to be the key factor in the chemical aging of microplastics. ROS can extract H atoms or electrons from the polymer chain and trigger chain reaction, which will lead to fragmentation of the polymer chain (formula 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 ⋅
The study found that under the effect of ROS, rainwater facilities containing different types of plastics can release a large number of microplastics particles, and the aging time is positively correlated with the release of microplastics[30]Under UV light, dissolved organic matter (DOM) can promote electron transfer and produce ROS, which can accelerate the aging of microplastics[31]。
Advanced oxidation technologies (AOPs) play a key role in the degradation of microplastics due to the production of a large number of active substances (such as • oh). These active substances can decompose micro plastics into small molecular intermediates, and even further degrade into co2And H2O[32]Fenton oxidation is a common AOP[33]Duan and Wang et al[34]The ultra-high polymer PE was decomposed by Hydrothermal Coupling Fenton system. The weight loss rate of PE reached 95.9% in 16 h and the mineralization rate reached 75.6% in 12 h. a large amount of • oh was produced in the process (equation 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 attracted much attention in the field of plastic degradation. In photocatalysis, semiconductors absorb energy from light sources and are excited to produce • oh and • o2-ISO ROS (by H2These ROS can make the micro plastic undergo fracture, cross-linking and other reactions, and finally degrade it to Co2(equation 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
As another AOP technology, electrocatalysis accelerates the transfer of charge at the interface between electrode and electrolyte by applying an electric field on the electrode surface, thus promoting the degradation of microplastics[37]In addition, the combination of multiple technologies can produce more effective results. CO is easily formed in photocatalysis2The selectivity of the product is low due to the complex of nano plastics and organic compounds[38]The electrocatalytic efficiency is limited to the hydrophobic surface of the plastic[39]Through the combination of photocatalysis and electrocatalysis Technology (i.e. photocatalysis technology using light energy to drive electrocatalysis reaction), high efficiency, high selectivity and sustainable degradation of micro plastics can be obtained[37,39]Espinoza- Montero et al[40]Through photocatalysis technology, TiO2The results show that the modified boron doped diamond photoanode can reach 6.89 Ma · cm in 10 h-2The high degradation efficiency of high density polyethylene (HDPE) microplastics in water was 89.91% ± 0.08% at the current density of 0.

2.3 Biological aging of microplastics

Bacteria, fungi, algae and other microorganisms exist widely in nature. Microplastics not only provide a place for microorganisms to colonize and grow[41-42]It can also provide a carbon source for microbial growth[43-44]The biological aging of microplastics can be roughly divided into colonization, depolymerization, assimilation, mineralization and other processes[45]Microorganisms can adhere to the surface of micro plastics to grow and reproduce[46]And release extracellular enzymes for depolymerization of microplastics to produce low molecular weight oligomers, dimers and even monomers[47]Microorganisms metabolize these low molecular polymers into co through assimilation and mineralization2、H2O and other substances[48⇓-50]The biological aging of microplastics provides ideas for the remediation of microplastics pollution. Compared with other microorganisms, fungi have stronger adsorption, colonization, survival ability and the ability to secrete a variety of degrading enzymes, so they have better performance in the degradation of micro plastics[51]However, the biodegradation of microplastics may be a long-term and slow process. For example, microbial degradation of PE requires 100-200 yr in humus lake water, 300-4000 yr in clean lake water, and 2000-20000 yr in artificial fresh water[52]However, the biological aging process of micro plastics may also produce a large number of micro/nano plastics with smaller particle size. Shao et al[53]The research shows that marine bacteriaAlcanivorax xenomutansandHalomonas titanicaeWhile degrading PS microplastics, it will decompose and produce a large number of micro/nano plastics, which may aggravate the pollution of micro/nano plastics in the ocean.
Some insects and zooplankton can also participate in the biological aging of microplastics. AfterChironomus sancticaroliThe average particle size of PS microplastics can be reduced from 24.5 μ m to 16.4 μ m after the action of larvae, which may be caused by the joint action of digestive enzymes and symbiotic bacteria in the larvae and the friction between PS microspheres and sand in the digestive tract[54]In addition, in Tenebrio molitor[55]And earthworms[56]There are similar cases in vivo. Some zooplankton, such as Antarctic krill（Euphausia superba）[57]Rotifers[58]It can convert micro plastics into nano plastics. It is worth noting that the particles of bio aged micro nano plastics have special physical and chemical properties due to the biological crown carried on its surface, which may lead to stronger potential health hazards and ecological risks[59]。
At present, biodegradable plastics are becoming a green substitute for traditional plastics. Biodegradable plastics can be converted into CO by enzymes and microorganisms2、H2O、CH4And biomass plastics, including polyhydroxyfatty acid esters (PHA), polylactic acid (PLA) and polybutylene adipate terephthalate (PBAT), etc[60]Compared with traditional micro plastics, biodegradable plastics may be easier to degrade into micro nano plastics and release additives in the environment, and the surface of these micro plastics contains more oxygen-containing functional groups and can better load pollutants[61]In terms of microbial colonization, the biomass loaded on the surface of non degradable plastics is lower than that of degradable plastics, but the bacteria and fungi loaded on the surface are more diverse[62]。

2.4 Artificial aging of microplastics

The natural aging of microplastics is a complex and dynamic process. Under most environmental conditions, a variety of aging effects will occur at the same time, and are affected by complex factors such as time, climate and geographical location[63]In addition to these factors that are difficult to control, the experimental cycle of natural aging is long[64]Therefore, researchers explore the influence of specific factors on the aging of microplastics through the artificial simulation conditions in the laboratory.
Common artificial aging technologies include illumination, chemical oxidation, etc[63]Compared with natural aging for decades or even hundreds of years, artificial aging will make significant changes in microplastics in a few days or months, greatly accelerating the aging process[65]At Freitag et al[66]In the study, the radiation intensity in the laboratory is 5.2 times of the average radiation intensity in Central Europe, so the natural aging time corresponding to the aging time of 200, 400 and 600 hours in the laboratory is 43, 86 and 130 days respectively. Although laboratory simulation can not fully reflect the natural aging behavior of microplastics, it can be used to evaluate and predict the cycle and process of microplastics[64]Through the coupling of various conditions, the gap between artificial simulation and natural conditions can be made up as much as possible. For example, Briffa et al[67]A test chamber was built 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 affected by many factors, mainly including the physical and chemical properties of microplastics and environmental conditions（Figure 2）。
Figure 2 The aging of microplastics is affected by its physical and chemical properties and environmental factors

Fig. 2 The aging of microplastics is influenced by their physical and chemical properties and environmental factors

3.1 Effect of physical and chemical properties of microplastics on Aging

The physical properties of microplastics include particle size, crystallinity and color. Compared with large-size microplastics, small-size microplastics are easier to be oxidized because of their larger specific surface area. Gu et al[68]The results showed that the smaller the particle size, the higher the photoaging rate of PVC. But Paik and Kar[69]The results show that the aging process of PE nano plastics with small size is more difficult due to its high crystallinity and low entropy.
The crystallinity of microplastics reflects the proportion of its crystalline region. According to the arrangement of molecular chains of microplastics, it can be divided into crystalline phase, semi crystalline phase and amorphous phase[70]A certain degree of crystallinity will make the microplastics more tough, but too high crystallinity will reduce the elasticity and increase the brittleness of the microplastics[71]This makes it easier to break into small particles in the process of natural wear[72]。
The color of microplastics will also affect its aging. Red or yellow pigments with longer wavelengths can absorb short wavelength light with higher energy, while blue pigments with shorter wavelengths can absorb long wavelength light with lower energy. The longer the color wavelength of the plastic, the stronger the absorbance, the lower the ultraviolet transmittance and the lower the light aging rate. Therefore, the fragments of red plastic are usually larger than those of blue plastic[73]In addition, color may also affect the colonization of microorganisms on microplastics. For example, biofilms colonized in blue microplastics have higher functional diversity than biofilms colonized in transparent or yellow microplastics[74]However, the different degree of colonization will further affect the biological aging of microplastics.
Compared with the micro plastics with O, N and other atoms as the main chain, the micro plastics with C atoms as the main chain are more difficult to be aged[75-76]For example, the skeleton chain of PE is composed of C-C single bond which is not easy to hydrolyze, and it is difficult to be degraded by photooxidation due to the lack of chromophores in the UV-Vis spectrum[77]It can exist for a long time in the natural environment. Microplastics with different molecular composition have different wettability, so it is difficult for microorganisms to form biofilms on the surface of highly hydrophobic microplastics, which can inhibit the degradation of microplastics[78]The additives released during the aging process of microplastics may promote the degradation of microplastics. Rivaton and Sleiman et al[79]The results show that PS films containing brominated flame retardants (BFRs) have a higher photoaging rate than pure PS films, and the addition of BFRs also changes the degradation mechanism of PS, resulting in 14 kinds of brominated photoproducts.

3.2 Effect of environmental conditions on the aging of microplastics

Environmental conditions can have a significant impact on the aging of microplastics (e.gTable 1As shown in). The effect of light intensity and wavelength on the aging of microplastics is very significant. It is found that there are microplastics from similar sources in beach sediments, but they have different aging degrees due to different intensities of light[80]When PVC was exposed to different wavelengths of ultraviolet light, the photoaging efficiency of PVC irradiated by UVC was greater than that under UVA and UVB, and the ROS intensity and leaching toxicity produced by UVC irradiation were the largest[81]。
Table 1 Influence of environmental factors on the aging of microplastics

Table 1 The effects of environmental factors on the aging of microplastics

Microplastics Aging pathway Factor Effect Ref
PVC Light Wave length UVC > UVA and UVB 81
PS Sediment O2 Alternating anoxic-oxic conditions > static oxic and static anoxic conditions 83
PET Dark and anoxic conditions Reducing agents Reducing agents: （+） a 86
PP Activated persulfate and hydrothermal treatment Temperature High temperature: （+） 89
PS Compost Temperature High temperature: （+） 90
PS Light HA HA: （+） 91
PS Light and HA Salinity Hight salinity: （+） 91
PS Light Ions NO3-，Cl-，and Br-: （+）;
HCO3-: （/） b		 92
PBAT Light Ions NO3-: （+）
Cl- and Br-: （-） c		 93
PP Light Ions Cl-: （-） 94
PE Soil burial pH High pH: （+） 95
PE Seawater aquarium Temperature and pH High temperature: （+）;
Low pH: （+）		 96
PP and EVA d Light pH Low pH: （+） 97
EPS e Light pH Low pH: （/） 97
PS Light Organic matter Hyaluronic acid and vitamin C: （+） 98
PP Light Organic matter HA and FA: （-） 99
PS Light Organic matter FA<1kDa: （+） 100
PE f Light Organic matter Paraquat and Mancozeb: （+）;
Chlorpyrifos and Sulfur: （/）		 101
PS Light Organic matter Pyrite: （+） 102
PET Light Soil component Clay，iron oxides，MnO2，SiO2，and Al2O3: （+）;
Organic carbon: （-）		 103
PVC and PET Light Organic matter Kaolinite and montmorillonite: （+） 104
Note: a（+）: Promotion; b（/）: No significant effect; c（-）: Inhibition; dEVA: ethylene-vinyl acetate; eEPS: expanded polystyrene; f: PE film
Oxygen participates in the formation of ROS in the aging process of microplastics, which can effectively promote the aging of microplastics[82]CL released under aerobic conditions during photoaging of PVC-The concentration is higher than the CL released under anoxic conditions-concentration[68]. Zhou et al[83]It is considered that the aging degree of PS in sediments under anoxic aerobic alternation is greater than that under static aerobic and static anoxic conditions, which is due to the generation of more ROS in sediments under anoxic aerobic conditions. In the biological aging of microplastics, oxygen, as the electron acceptor of microbial enzymes, can affect the metabolism of microorganisms[84-85]Under anoxic condition, the addition of reductant can promote the rapid aging of microplastics[86]。
Temperature can affect the aging rate of microplastics by affecting the molecular chain reaction kinetics process[87]And affect the release of additives and other substances at a certain temperature[88]In the process of sludge persulfate and hydrothermal CO treatment, the temperature rise led to the melting deformation, roughness and crystallinity changes of PP microplastics, which aggravated the aging of PP[89]In addition, temperature can affect the biological aging of microplastics by affecting enzyme activity and microbial community structure. Zhou et al[90]The results showed that the degradation efficiency of PS in the super thermophilic compost (70 ℃) was 7.3%, which was 6.6 times higher than that in the traditional thermophilic compost (40 ℃). The reason was that the degradation efficiency of PS in the super thermophilic compost (70 ℃) was higher than that in the traditional thermophilic compost (40 ℃)Thermus、BacillusandGeobacillusAnd other microorganisms.
The aging of microplastics in the environment is also affected by other environmental factors. Compared with low salinity, high salinity can promote the photoaging of PS microplastics in solutions containing humic acid (HA)[91]。Cl-And br-Isohalide ions can significantly affect the photoaging process of microplastics[92-93]However, the influence of inorganic ions on the aging of microplastics is complex, which may participate in the free radical reaction in the photoaging process of microplastics[94]The environmental pH can affect the aging process of microplastics by interfering with the activity of microorganisms, and the slightly alkaline soil may be conducive to the growth of microorganisms, thus promoting the aging of PE[95]The lower pH can promote the weakening of the PE polymer bond soaked in seawater, and then make it twist, melt and peel off[96]When the microplastics in simulated seawater are photoaged, the decrease of pH will promote the aging of microplastics, but the aging effect varies with the type of polymer[97]Organic substances in the environment, such as hyaluronic acid and vitamin C, can promote the production of · Oh, which in turn promotes the photoaging of PS micro plastics and nano plastics[98]Ha and fulvic acid (FA) can be removed by removing ROS[99]Or prevent ultraviolet light from reaching the micro plastic surface[82]And inhibit the aging of microplastics. However, studies have also shown that low molecular weight fa (FA<1 kDa) can promote the photoaging of PS microplastics due to its strong redox ability and electron donor ability[100]Some pesticides, such as paraquat, can accelerate the aging of PE by generating superoxide[101]Other substances in the environment, such as pyrite[102], kaolin and montmorillonite[103-104]The existence of minerals can promote the aging of microplastics.

4 Effect of aging on microplastics

4.1 Changes of physical and chemical properties of microplastics during aging

Aging can significantly change the size, morphology and surface characteristics of microplastics. When PS is at o3After aging, the average particle size can be reduced to half of that before aging[105]After 60 days of light aging, slurry cracks and parallel cracks appeared on the surface of low density polyethylene (LDPE) and PP, and PP fragments were observed between the surface cracks of PP[106]Under the condition of simulating beach environment, the synergistic effect of ultraviolet light and sand abrasion will lead to the dissociation of C-C and C-H bonds on the main chain of the microplastics, which will further lead to the embrittlement of the microplastics and the generation of cracks[107]Aging will also affect the color of microplastics. PS will change from white to yellow during UV aging[108]After UV aging, the smooth surface of styrene butadiene rubber microplastics (MSBR) becomes rough, and its color changes from near white to yellow. The longer the aging time, the darker the color[109]The color change of microplastics before and after aging may be due to the change of heat stabilizers (such as phenolic antioxidants) into yellow substances such as quinone organics[110]It may also be related to the change of polyene chain length and the competition between photobleaching[111]。
Aging will change the composition of micro plastic elements and surface functional groups. PVC via H2O2After aging, the content of CL increased, while the content of Ca and O decreased[112]The mass percentage of O in PP irradiated by UV lamp increased from 2.80% to 20.95%[113]In terms of functional groups, aging can generate oxygen-containing functional groups such as hydroxyl, carbonyl and aldehyde groups on the surface of micro plastics, and the increase of these oxygen-containing functional groups will enhance the hydrophilicity of micro plastics[114]The surface oxygen-containing functional groups of PS increased after UV irradiation[115]Under UV irradiation, the C-H bond on the surface of MSBR was dissociated and formed electron vacancies, and then further oxidized to hydroxyl and carbonyl groups[109]The changes of functional groups of microplastics in different aging pathways are different. The concentrations of oxidation products (ketones, carboxylic acids and esters) formed by PE after photoaging and thermal aging are different, which is due to the Norrish reaction during photoaging, which leads to the conversion of ketones into new unsaturated groups; In thermal aging, the lack of Norrish reaction leads to the accumulation of ketones[116]In addition, thermal aging does not necessarily significantly affect the structure of microplastics. Esterhuizen et al[117]Polycarbonate (PC) was thermally aged at 70 ℃ for 160 days, but the structure of the microplastics did not change significantly.

4.2 Effect of aging on pollutant loading capacity of microplastics

Microplastics can be used as carriers of various pollutants in the environment, and the interactions involved include hydrophobic interaction, electrostatic interaction, hydrogen bond, van der Waals force and π - π interaction[118]The study found that the concentration of chemical pollutants on the surface of micro plastic was six times that in the surrounding water[119]The aging process changes the physical and chemical properties of the surface of microplastics, and then affects its ability to load pollutants.
The adsorption of heavy metals by microplastics mainly includes physical adsorption, coordination, electrostatic attraction, hydrophobic interaction, cation - π bond interaction, etc[120-121]After aging, the specific surface area of the microplastics increases, the surface negative charge is easy to form, and the hydrophilicity is increased. The changes of these conditions may be conducive to the adsorption of heavy metals. The average saturated adsorption of Cr (Ⅵ) by PA, PS and PE after photoaging increased from 730.69, 146.11 and 75.61 μ g · g, respectively-1Increased to 736.31, 318.75 and 136.78 μ g · G-1This is mainly due to the enhancement of electrostatic interaction after aging[122]. Fenton or H2O2Aging can significantly enhance the effect of PS on CD2+The main reason is that more CD is exposed on the aged PS surface2+Adsorption sites. Lin and LAN et al[123]Our research shows that, O3Aging increases the hydrophilicity and negative charge on the surface of the microplastics, so the adsorption capacity of the microplastics for Hg (Ⅱ) is 4~20 times higher than that of the non aged microplastics. Tan et al[124]The adsorption of Pb (Ⅱ) by naturally aged microplastics in Xiangjiang River was studied. The results showed that the organic films on the surface of aging microplastics played an important role in the adsorption of Pb (Ⅱ). These organic films were rich in oxygen-containing functional groups such as carboxyl and hydroxyl groups, and could adsorb Pb (Ⅱ) by electrostatic force. Breider et al[125]Compared o3Adsorption of Cu by PS, solar simulator and lake aging. The oxidation degree of aged PS in lakes is the lowest, but its adsorption capacity for Cu is the highest. This may be because the elements such as Si, Al, Mg and Fe in lakes precipitate on the surface of PS and form metal oxides conducive to the adsorption of Cu.
Microplastics can interact with organics through hydrophobic interaction, surface coordination, van der Waals force, hydrogen bond and π - π interaction, in which hydrophobic interaction is dominant[121]Generally speaking, the oxygen-containing groups formed on the surface of the aged microplastics are not conducive to their adsorption of hydrophobic organic pollutants. Junck et al[126]The results showed that the hydrophobicity of aged PE decreased and negative charge sites were formed on the surface, which reduced the adsorption capacity of hydrophobic herbicide terbutazine. Li et al[127]The adsorption of levofloxacin hydrochloride (Lev) on PE, PS and PA microplastics was compared. It was found that PA had the strongest adsorption capacity for LEV, which was due to the polar polar interaction between PA and LEV and the hydrogen bond formed between the amide group of PA and the carbonyl group of LEV. Light aging significantly enhanced the adsorption of Lev on the three microplastics, especially PS after aging. This is because the wrinkles and cracks on the surface of PS after aging provide a large number of Lev adsorption sites, and enhance the π - π interaction between benzene ring and LEV in PS. Liu et al[128]The adsorption of tetracycline hydrochloride (TC HCl) and cephalexin (CFX) on PE microplastics cultured in lake water was studied. The adsorption rate of PE to the two antibiotics is related to the surface diffusion, particle diffusion and membrane diffusion processes. There are many biofilms on the surface of aged PE in lake water. These biofilms enhance the adsorption of antibiotics by increasing the specific surface area, producing C=O groups and reducing the surface zeta potential. Kang et al[129]PP was exposed to air and aged in sunlight. Compared with non aged PP, aged PP showed stronger adsorption capacity for nonylphenol due to its larger specific surface area, more oxygen-containing functional groups and adsorption sites, and stronger hydrogen bonding effect.

4.3 Effect of aging on chemical release from microplastics

Additives are artificially added chemicals in the process of plastic production. Their purpose is to improve the quality and performance of plastic products to resist o3Effects of, microorganism, radiation and humidity on plastic products[130]Common additives include phthalate esters (PAEs), bisphenol A (BPA), metals and other compounds. During the aging process of microplastics, various additives will be released into the environment or enter the organism with the disconnection of its polymerization chain（Figure 3）[131]。
Figure 3 During the aging process of microplastics, additives and other chemicals will be released and threaten human health through the food chain

Fig. 3 Microplastics will release additives and other chemicals during the aging，and then threaten human health through the food chain

The research on the release of heavy metals from microplastics is mostly focused on pet, PVC, PP, PE and PS, among which PVC releases more heavy metals (the concentrations of Ca, Cu, Zn and Sb are higher)[132]. at h of PVC2O2During chemical aging, the release of Cr, Ni, Pb, Cu, Zn, CD, Mn and other metals increased with the increase of H2O2Increase with the increase of concentration[112]. Qu et al[133]For the determination of Cd in PP containing CD pigment2+Studies were carried out on the release of. Under dark conditions, 2.00~3.50 mm PP hardly released CD2+PP with particle size<0.15 mm released a small amount of CD2+Under simulated sunlight conditions, PP with particle size<0.15 mm released a large amount of CD2+, these CD2+The photodissociation of pigment is caused by the reaction between photogenerated holes and pigment lattice. Liu et al[134]The aging process of microplastics in simulated ultraviolet light, natural light and natural water was studied. Under simulated ultraviolet light, the concentration of Zn in the microplastics decreased with the increase of aging time, and tended to leach heavy metals. However, the concentration of Zn in the microplastics aged in natural light and natural water showed significant fluctuations, which was due to the fact that the microplastics released heavy metals under the aging effect of light, water and microorganisms, and the biofilm formed on the surface had a certain adsorption effect on heavy metals.
The aging process of microplastics is often accompanied by the release of organic pollutants. When the plastic shell of the waste cathode ray tube was placed in a solution containing humus, the concentration of polybrominated diphenyl ethers (PBDEs) in the plastic leachate ranged from 14 to 200 μ g · L-1(although PBDEs have relatively hydrophobic physicochemical properties)[135]Fifteen oxidation intermediates, such as styrene, acetophenone, benzaldehyde and acetic acid, were detected during the advanced oxidation of PS microplastics by UV/sodium percarbonate[136]. Lin et al[137]The chlorine aging process of PS and PE was studied. It was found that the organic substances released from these microplastics had the potential to form disinfection by-products. The release of organics during PS aging is more significant, which may be due to the fragmentation of microplastics particles during chlorination due to the lower chlorine resistance of PS. Another reason may be that the additives in PS and PE are different, because the lack of antioxidants in micro plastics will accelerate the release of organics[138]Some micro plastics contain a lot of organic phosphate esters (opes), Xiao, etc[139]It is believed that>60% of opes (even 98% of extremely hydrophobic opes) will remain in the polymer and slowly release over a long period of time. Hong et al[140]The aging experiments of expanded polystyrene (EPS) in dark/light room and seawater floating on the sea surface were carried out in the Gulf of Korea, and the leaching of hexabromocyclododecane (hbccds) was compared. After 7 days of exposure, 37% of hbccds were leached from EPS in dark cabins, while 49% of hbcdds were leached from EPS in light cabins. In the process of sea water aging, 61% of hbcdds were leached from EPS under the influence of ultraviolet light, temperature, microorganisms, wave turbulence and other factors.
At present, the research on the chemical release of microplastics in the process of biological aging is still limited, especially the role of the surface ecological crown of microplastics. For example, the biofilm on the surface of microplastics may not only act as a barrier to affect the leaching of additives, but also use plastics as a carbon source to increase the release of chemicals by accelerating the biodegradation of microplastics[141]In addition, the leaching of additives can further affect the interaction between microplastics and environmental microorganisms, resulting in more complex release process of chemical substances in microplastics.

4.4 Effect of aging on toxicity of microplastics

Studies have shown that microplastics can cause metabolic disorders, inflammation, oxidative stress, apoptosis and other toxic effects[142-143]After aging, the physical and chemical properties of microplastics changed, which led to the change of its toxic effect. The toxic effects of aging microplastics can be divided into: the toxic effects of microplastics themselves, the compound toxic effects caused by loading other environmental pollutants, and the toxic effects of additives and intermediates released by aging（Figure 4）。
Figure 4 During the aging process of microplastics, the microplastics themselves, the environmental pollutants loaded by the microplastics, and the released additives and intermediates will produce different biological toxicity

Fig. 4 During the aging process of microplastics, microplastics themselves，environmental pollutants loaded on microplastics, and released additives and intermediates can produce different biotoxicities

The size of microplastics plays a key role in biological uptake. For example, 1 μ m is a common size of microplastics intercepted by crustacean stomach filters[144]The microplastics of 11-700 μ m may be easily ingested by amphipods[145]. vroom et al[146]The results of the study showed that after natural seawater aging, the proportion and rate of uptake of PS microplastics by marine plankton were higher than those of non aged PS, which may be due to the formation of biofilms on the surface of aged PS (there may be similar substances in the organisms eaten by plankton), thus increasing the possibility of microplastics uptake. The aging of microplastics will also affect its transport, storage and metabolism in organisms. For example, the particle size of microplastics determines its biological distribution characteristics in various organs to a certain extent. It is generally believed that smaller plastic particles are easier to transport to more organs and penetrate into cells[147]. Zou et al[148]The PA microplastics were treated by photoaging in aqueous solution containing HA and FA. The results showed that the toxic effect of aged PA on zebrafish was aggravated mainly through its physical and chemical properties rather than the mechanism of extract. The non aged PA was mainly distributed in the intestines of zebrafish, while the aged PA could be detected in the intestines, pancreas and liver, which might be due to the fact that the smaller size of nano plastics formed after aging was easier to penetrate the intestinal membrane of organisms. In addition, aging PA not only led to the reduction of body length and weight, the damage of intestinal structure and function, the increase of ROS level in intestinal tract and the enhancement of oxidative stress, but also down regulated the genes related to triglyceride biosynthesis and transport（cd36、dgat1aanddgat2So as to interfere with lipid metabolism. In addition, the changes of functional groups on the surface of microplastics can also affect their toxic effects. Aging PS resulted in the significant reduction of A549 lung cell nucleus, the destruction of F-actin structure, the increase of basal glycolysis rate and the decrease of monolayer barrier integrity[149]This effect may be related to the increase of C-O bond and carboxyl content on the surface of PS microplastics after UV aging. Wang et al[150]The aging PS PS-NH2、 Effects of ps-cooh and PMMA on Isochrysis galbana（Isochrysis galbana）Toxic effects. After aging, PS caused great harm to Isochrysis galbana (such as increasing oxidative stress, inhibiting growth and changing energy metabolism), PS-NH2And ps-cooh are less toxic to organisms due to the loss of functional groups, while PMMA has strong aging resistance due to its own structure and the high concentration of plasticizer contained in it.
Aged microplastics can carry more environmental pollutants, and then produce joint toxicity to organisms. Wang et al[151]The results showed that PE after aging could lead to Cladocera organismsMoina monogolicaThe internal abrasion and mechanical damage of the digestive tract, and the CD carried by PE may be released in the biological digestive tract, resulting in higher toxic effects through molecular targets in cells. This combined exposure not only affects the reproduction of organisms, but also causes malnutrition (such as the reduction of protein, carbohydrate and lipid contents) and even death of offspring. Similarly, the aging PE loaded with Ag complex had a significant effect on duckweed（Lemna minor）And Daphnia（Daphnia magna）The toxic effect of aging PE is stronger than that of aging PE alone. The toxic effect is mainly due to the release of Ag in the complex (especially in acid medium) rather than PE itself[152]It is worth noting that this combined exposure sometimes does not necessarily produce synergistic toxic effects. For example, photoaged pet and Pb2+Chlorella can be inhibited when exposed alone（Chlorella pyrenoidosa）Growth and reproduction of (causing physical stress and chemical stress respectively). When they coexist but are not adsorbed, they can inhibit the growth of Chlorella cells and damage their cell membrane and antioxidant system. However, when pet adsorbed PB2+After that, due to Pb in water2+The concentration and activity of Chlorella vulgaris decreased, and its chemical stress on Chlorella vulgaris decreased (but there was still physical stress)[153]Aging microplastics can also combine with organic pollutants to produce toxicity to organisms. Zong and song et al[154]The effects of aging PS and ciprofloxacin (CIP) on Escherichia coli were studied（Escherichia coli）Combined toxicity. It was found that aging increased the adsorption rate and amount of CIP on PS. The toxic effects of combined exposure of CIP and aging PS include down regulating the expression of ABC transporter and causing cell membrane damage, affecting amino acid metabolism and lipid metabolism and affecting cell growth, cell membrane integrity and cell antioxidant stress ability, capturing rotating enzyme molecules during and after double stranded DNA cleavage and blocking DNA replication, and down regulatingosmY、osmB、osmCGene to make osmotic pressure imbalance, etc. However, when CIP and aging PS were exposed together, the inhibition rate of CIP on E. coli was reduced due to the adsorption of CIP on aging PS. Yu and Yang et al[155]The toxic effects of PLA and its adsorbed volatile organic compounds on mouse macrophages were studied. Interestingly, compared with the non aged PLA, the PLA complex treated at 120 ℃ and 130 ℃ increased the cell viability (by 21.99% and 27.31%, respectively), which may be because the cells can use the organic matter on the surface of the aged PLA as a carbon source; However, the PLA complex treated at 140 ℃ decreased the cell viability (by 16.07%), which may be due to the release of toxic substances in the PLA complex caused by high temperature.
The aging process of microplastics will lead to the release of additives and intermediates, which may bring certain ecological risks. After UV aging and chlorination of polyurethane (TPU) microplastics, the half lethal concentration (LC50) of organic substances released from TPU microplastics on human liver cancer cells (HepG2) was only about 10% of the original TPU, indicating a significant increase in cytotoxicity[156]. Peng et al[157]Microalgae（Chlorella vulgaris）By comparing the gene function, cell growth and oxidative stress of microalgae exposed to photoaging PE and PVC seawater extract, it was found that the toxicity to microalgae was PVC extract>PE>PE extract>PVC. The toxic effect of PVC extract on microalgae is the strongest, which may be due to the release of more substances (including Zn, farnesol isomer a, 2,6-di-tert-butyl-4-methylphenol, acetyl castor oil methyl ester, etc.) from aged PVC. The cell density, dry weight and chlorophyll of microalgae were decreased after exposure to the extractaBut it can enhance the secretion of extracellular polymer and oxidative stress kinase system. At the transcriptome level, PE and PVC extracts were toxic to microalgae cells by interfering with the ribosome biosynthesis of microalgae and affecting the interaction between microalgae and pathogens, respectively. It is worth noting that a longer aging process may also reduce the toxic effects of microplastics. For example, non aged PC and short-term aged PC can（Lepidium sativum）However, the toxicity of PC to Oenanthe javanica decreased with the increase of aging time, which may be due to the reduction of potential release of micro plastic additives during aging with the increase of aging time[117]。

5 Conclusion and Prospect

Aging is a necessary environmental process for micro plastics. The changes of physical and chemical properties brought by aging process will affect the environmental behavior and toxic effects of microplastics, and increase the uncertainty of their environmental fate and health risks. Although a large number of studies have been carried out on the aging process of microplastics and some important progress has been made, there are still many challenges in both research methods and theoretical cognition.
(1) The change of physical and chemical properties of micro plastic materials is the key to the change of its environmental behavior and toxic effect. During the aging process, many physical and chemical properties of microplastics will change at the same time. Therefore, clarifying the structure-activity relationship between different physical and chemical properties of microplastics and their biological processes and toxic effects is the key to reveal the key biological processes and induced toxic effects of microplastics under complex environmental conditions.
(2) Although there are many methods to characterize the physical and chemical properties of microplastics after aging, most of the methods can only be used for qualitative analysis rather than quantitative analysis. Therefore, how to accurately measure and characterize the physical and chemical properties of microplastics before and after aging, such as the number of surface functional groups, is the key to clarify the "real" dose effect relationship between microplastics exposure and toxic effects.
(3) In the real environment, chemical substances such as heavy metals, persistent organic pollutants and microorganisms can interact with microplastics, affecting the aging of microplastics and its environmental behavior and toxic effects, which further increases the complexity of the process. Therefore, the research based on real environment will help to improve the cognition of microplastics aging process, environmental behavior and health risks.

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