Skip to main content
Log in

Analysis and identification of degradation products in gas, particle, and liquid phases of polypropylene and polyethyleneterephthalate microplastics aging through non-thermal plasma simulation

  • Research Article
  • Published:
Environmental Science and Pollution Research Aims and scope Submit manuscript

Abstract

Plastic aging can cause alterations in the physical and chemical characteristics of plastics, as well as their behavior in the environment. Due to the extremely slow natural aging process, laboratory simulated aging methods have to be used. In this study, non-thermal plasma (NTP) was adopted to investigate the aging process of polypropylene (PP) and polyethylene terephthalate (PET) microplastics. Various analytical instruments, including proton transfer reaction mass spectrometry and single-particle aerosol mass spectrometry, were employed to examine and identify the organic constituents of the gas, liquid, and particle phase degradation products, as well as to monitor the degradation process. The results showed that after 90 min of aging, both PP and PET surfaces showed yellowing, and the carbonyl index of PP increased while that of PET decreased, with an increase in crystallinity. The organic components of reaction products, such as ketones, esters, acids, and alcohols, increased with longer aging times. Gas products mainly contain aromatic hydrocarbons, while particles from aged PET contain compounds with benzene rings and metal elements. Liquid products from aged PP show a significant presence of branched alkanes. Based on this analysis, degradation mechanisms of PP and PET by NTP were proposed. This investigation represents the initial systematically exploration of the release of organic substances during the degradation of microplastics mediated by NTP. It provides significant insights into the detrimental organic compounds emitted during this process, thereby offering valuable information for understanding the environmental and human health implications of natural microplastic degradation. Furthermore, it addressed the requirements for increased attention to the potential environmental risks associated with these harmful components.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8

Similar content being viewed by others

Data availability

Data will be made available on request.

References

  • American journal of industrial medicineWu X, Chen X, Jiang R, You J, Ouyang G (2022) New insights into the photo-degraded polystyrene microplastic: effect on the release of volatile organic compounds. J Hazard Mater 431: 128523. https://doi.org/10.1016/j.jhazmat.2022.128523

  • Andrady AL, Lavender Law K, Donohue J, Koongolla B (2022) Accelerated degradation of low-density polyethylene in air and in sea water. Sci Total Environ 811:151368. https://doi.org/10.1016/j.scitotenv.2021.151368

    Article  CAS  Google Scholar 

  • Ansari M, Moussavi G, Ehrampoosh MH, Giannakis S (2023) A systematic review of non-thermal plasma (NTP) technologies for synthetic organic pollutants (SOPs) removal from water: recent advances in energy yield aspects as their key limiting factor. J Water Process Eng 51:103371. https://doi.org/10.1016/j.jwpe.2022.103371

    Article  Google Scholar 

  • Bandow N, Will V, Wachtendorf V, Simon F-G (2017) Contaminant release from aged microplastic. Environ Chem 14:394–405. https://doi.org/10.1071/en17064

    Article  CAS  Google Scholar 

  • Cao Y, Lin H, Zhang K, Xu S, Yan M, Leung KMY, Lam PKS (2022) Microplastics: a major source of phthalate esters in aquatic environments. J Hazard Mater 432:128731. https://doi.org/10.1016/j.jhazmat.2022.128731

    Article  CAS  Google Scholar 

  • Castelvetro V, Corti A, Biale G, Ceccarini A, Degano I, La Nasa J, Lomonaco T, Manariti A, Manco E, Modugno F (2021) New methodologies for the detection, identification, and quantification of microplastics and their environmental degradation by-products. Environ Sci Pollut R, 1–17. https://doi.org/10.1007/s11356-021-12466-z

  • Deng Y, Zhu K, Sun Y, Xie L, Jiang W, Jiang Y, Guo X, Jia H (2023) Aging kinetics and mechanisms of polystyrene microplastic in water under sunlight irradiation: effects of inorganic cations. Gondwana Res. https://doi.org/10.1016/j.gr.2023.11.011

    Article  Google Scholar 

  • Ding L, Yu X, Guo X, Zhang Y, Ouyang Z, Liu P, Zhang C, Wang T, Jia H, Zhu L (2022) The photodegradation processes and mechanisms of polyvinyl chloride and polyethylene terephthalate microplastic in aquatic environments: Important role of clay minerals. Water Res 208:117879. https://doi.org/10.1016/j.watres.2021.117879

    Article  CAS  Google Scholar 

  • Duan J, Bolan N, Li Y, Ding S, Atugoda T, Vithanage M, Sarkar B, Tsang DCW, Kirkham MB (2021) Weathering of microplastics and interaction with other coexisting constituents in terrestrial and aquatic environments. Water Res 196:117011. https://doi.org/10.1016/j.watres.2021.117011

    Article  CAS  Google Scholar 

  • Enfrin M, Lee J, Gibert Y, Basheer F, Kong L, Dumee LF (2020) Release of hazardous nanoplastic contaminants due to microplastics fragmentation under shear stress forces. J Hazard Mater 384:121393. https://doi.org/10.1016/j.jhazmat.2019.121393

    Article  CAS  Google Scholar 

  • Fotopoulou KN, Karapanagioti HK (2017) Degradation of various plastics in the environment. Hazardous Chemicals Associated with Plastics in the Marine Environment, pp. 71–92

  • Gan Q, Cui J, Jin B (2023) Environmental microplastics: classification, sources, fates, and effects on plants. Chemosphere 313:137559. https://doi.org/10.1016/j.chemosphere.2022.137559

    Article  CAS  Google Scholar 

  • Gaonkar AA, Murudkar VV, Deshpande VD (2020) Comparison of crystallization kinetics of polyethylene terephthalate (PET) and reorganized PET. Thermochim Acta 683:178472

    Article  CAS  Google Scholar 

  • Gewert B, Plassmann M, Sandblom O, MacLeod M (2018) Identification of Chain scission products released to water by plastic exposed to ultraviolet light. Environ Sci Tech Let 5:272–276. https://doi.org/10.1021/acs.estlett.8b00119

    Article  CAS  Google Scholar 

  • Gigault J, Pedrono B, Maxit B, Ter Halle A (2016) Marine plastic litter: the unanalyzed nano-fraction. Environ Sci-Nano 3:346–350. https://doi.org/10.1039/c6en00008h

    Article  CAS  Google Scholar 

  • Guo T, Li X, Jianquan P, Zhen X, Dong J (2018) On-line quantification and human health risk assessment of organic by-products from the removal of toluene in air using non-thermal plasma. Chemosphere, 139–146

  • Hadiuzzaman M, Salehi M, Fujiwara T (2022) Plastic litter fate and contaminant transport within the urban environment, photodegradation, fragmentation, and heavy metal uptake from storm runoff. Environ Res 212:113183. https://doi.org/10.1016/j.envres.2022.113183

    Article  CAS  Google Scholar 

  • He W, Liu S, Zhang W, Yi K, Zhang C, Pang H, Huang D, Huang J, Li X (2023) Recent advances on microplastic aging: Identification, mechanism, influence factors, and additives release. Sci Total Environ, 164035

  • Hidayaturrahman H, Lee TG (2019) A study on characteristics of microplastic in wastewater of South Korea: Identification, quantification, and fate of microplastics during treatment process. Mar Pollut Bull 146:696–702

    Article  CAS  Google Scholar 

  • Huang P, Zhang Y, Hussain N, Lan T, Chen G, Tang X, Deng O, Yan C, Li Y, Luo L (2023) A bibliometric analysis of global research hotspots and progress on microplastics in soil‒plant systems. Environ Pollut, 122890. https://doi.org/10.1016/j.envpol.2023.122890

  • Jiang Z, Huang L, Fan Y, Zhou S, Zou X (2022) Contrasting effects of microplastic aging upon the adsorption of sulfonamides and its mechanism. Chem Eng J 430. https://doi.org/10.1016/j.cej.2021.132939

  • Khaled A, Rivaton A, Richard C, Jaber F, Sleiman M (2018) Phototransformation of plastic containing brominated flame retardants: enhanced fragmentation and release of photoproducts to water and air. Environ Sci Technol 52:11123–11131. https://doi.org/10.1021/acs.est.8b03172

    Article  CAS  Google Scholar 

  • Klages CP, Grishin A (2008) Plasma amination of low-density polyethylene by DBD afterglows at atmospheric pressure. Plasma Process Polym 5:368–376

    Article  CAS  Google Scholar 

  • La Nasa J, Lomonaco T, Manco E, Ceccarini A, Fuoco R, Corti A, Modugno F, Castelvetro V, Degano I (2021) Plastic breeze: Volatile organic compounds (VOCs) emitted by degrading macro- and microplastics analyzed by selected ion flow-tube mass spectrometry. Chemosphere 270:128612. https://doi.org/10.1016/j.chemosphere.2020.128612

    Article  CAS  Google Scholar 

  • La Nasa J, Mattonai M, Modugno F, Degano I, Ribechini E (2019) Comics’ VOC-abulary: study of the ageing of comic books in archival bags through VOCs profiling. Polym Degrad Stabil 161:39–49

    Article  Google Scholar 

  • Lee CO, Chae B, Kim SB, Jung YM, Lee SW (2012) Two-dimensional correlation analysis study of the photo-degradation of poly (ethylene terephthalate) film. Vib Spectrosc 60:142–145

    Article  CAS  Google Scholar 

  • Lee YK, Romera-Castillo C, Hong S, Hur J (2020) Characteristics of microplastic polymer-derived dissolved organic matter and its potential as a disinfection byproduct precursor. Water Res 175. https://doi.org/10.1016/j.watres.2020.115678

  • Lin Z, Jin T, Zou T, Xu L, Xi B, Xu D, He J, Xiong L, Tang C, Peng J, Zhou Y, Fei J (2022) Current progress on plastic/microplastic degradation: fact influences and mechanism. Environ Pollut 304:119159. https://doi.org/10.1016/j.envpol.2022.119159

    Article  CAS  Google Scholar 

  • Liu J, Huang Y, Zhao G, Jia B, Shang Y, Cheng P (2023a) Online study of the plasma-accelerated aging process and toxicity of polyethylene terephthalate. J Hazard Mater, 131870. https://doi.org/10.1016/j.jhazmat.2023.131870

  • Liu P, Zhan X, Wu X, Li J, Wang H, Gao S (2020) Effect of weathering on environmental behavior of microplastics: properties, sorption and potential risks. Chemosphere 242:125193. https://doi.org/10.1016/j.chemosphere.2019.125193

    Article  CAS  Google Scholar 

  • Liu S, Chen H, Ding Y, Zhou X, Ding Y, Liu S, Ke Z (2023b) Thermal aging of polystyrene microplastics within mussels (Mytilus coruscus) under boiling and drying processing. J Hazard Mater, 133282

  • Liu X, Yang R (2020) Conversion among photo-oxidative products of polypropylene in solid, liquid and gaseous states

  • Lomonaco T, Manco E, Corti A, La Nasa J, Ghimenti S, Biagini D, Di Francesco F, Modugno F, Ceccarini A, Fuoco R, Castelvetro V (2020) Release of harmful volatile organic compounds (VOCs) from photo-degraded plastic debris: a neglected source of environmental pollution. J Hazard Mater 394:122596. https://doi.org/10.1016/j.jhazmat.2020.122596

    Article  CAS  Google Scholar 

  • Luo H, Zhao Y, Li Y, Xiang Y, He D, Pan X (2020) Aging of microplastics affects their surface properties, thermal decomposition, additives leaching and interactions in simulated fluids. Sci Total Environ 714:136862. https://doi.org/10.1016/j.scitotenv.2020.136862

    Article  CAS  Google Scholar 

  • Ma J, Zhang Y, Zhang D, Niu X, Lin Z (2022) Insights into the molecular interaction between poly(vinylpyrrolidone)-iodine disinfection system and polypropylene microplastics in aquatic environment. Chem Eng J 430. https://doi.org/10.1016/j.cej.2021.132276

  • Meng J, Xu B, Liu F, Li W, Sy N, Zhou X, Yan B (2021) Effects of chemical and natural ageing on the release of potentially toxic metal additives in commercial PVC microplastics. Chemosphere 283. https://doi.org/10.1016/j.chemosphere.2021.131274

  • Miranda MN, Sampaio MJ, Tavares PB, Silva AMT, Pereira MFR (2021) Aging assessment of microplastics (LDPE, PET and uPVC) under urban environment stressors. Sci Total Environ 796:148914. https://doi.org/10.1016/j.scitotenv.2021.148914

    Article  CAS  Google Scholar 

  • Morent R, De Geyter N, Leys C, Gengembre L, Payen E (2007) Study of the ageing behaviour of polymer films treated with a dielectric barrier discharge in air, helium and argon at medium pressure. Surf Coat Tech 201:7847–7854

    Article  CAS  Google Scholar 

  • Panda P, Mahanta RK, Mohanty S, Paikaray R, Das SP (2021) Abatement of gas-phase VOCs via dielectric barrier discharge plasmas. Environ Sci Pollut R 28:28666–28679

    Article  CAS  Google Scholar 

  • Schrank I, Trotter B, Dummert J, Scholz-Böttcher BM, Löder MG, Laforsch C (2019) Effects of microplastic particles and leaching additive on the life history and morphology of Daphnia magna. Environ Pollut 255:113233

    Article  CAS  Google Scholar 

  • Shaw D, West A, Bredin J, Wagenaars E (2016) Mechanisms behind surface modification of polypropylene film using an atmospheric-pressure plasma jet. Plasma Sources Sci T 25:065018

    Article  Google Scholar 

  • Tao B, Wang G, Yin Z, Pu X, Jiang Y, Zhang L, Cheng J, Li Y, Zhang J (2020) Determination of the contents of antioxidants and their degradation products in sodium chloride injection for blood transfusion. J Anal Methods Chem 2020:1–12

    Article  CAS  Google Scholar 

  • Turner A, Filella M (2021) Hazardous metal additives in plastics and their environmental impacts. Environ Int 156:106622

    Article  CAS  Google Scholar 

  • Vera P, Canellas E, Nerín C (2018) Identification of non volatile migrant compounds and NIAS in polypropylene films used as food packaging characterized by UPLC-MS/QTOF. Talanta 188:750–762

    Article  CAS  Google Scholar 

  • Wang H, Zhu J, He Y, Wang J, Zeng N, Zhan X (2023a) Photoaging process and mechanism of four commonly commercial microplastics. J Hazard Mater 451:131151

    Article  CAS  Google Scholar 

  • Wang K, Wang K, Liang S, Guo C, Wang W, Wang J (2023b) Accelerated aging of polyvinyl chloride microplastics by UV irradiation: aging characteristics, filtrate analysis, and adsorption behavior. Environ Technol Innov 32:103405

    Article  CAS  Google Scholar 

  • Wang L, Zhang J, Huang W, He Y (2023c) Laboratory simulated aging methods, mechanisms and characteristic changes of microplastics: a review. Chemosphere, 137744. https://doi.org/10.1016/j.chemosphere.2023.137744

  • Wang Q, Chen M, Min Y, Shi P (2024) Aging of polystyrene microplastics by UV/Sodium percarbonate oxidation: organic release, mechanism, and disinfection by-product formation. J Hazard Mater 464:132934

    Article  CAS  Google Scholar 

  • Wang W, Themelis NJ, Sun K, Bourtsalas AC, Huang Q, Zhang Y, Wu Z (2019) Current influence of China’s ban on plastic waste imports. Waste Dispos Sustain Energy 1:67–78

    Article  Google Scholar 

  • Wu X, Liu P, Shi H, Wang H, Huang H, Shi Y, Gao S (2021a) Photo aging and fragmentation of polypropylene food packaging materials in artificial seawater. Water Res 188:116456. https://doi.org/10.1016/j.watres.2020.116456

    Article  CAS  Google Scholar 

  • Wu X, Liu P, Wang H, Huang H, Shi Y, Yang C, Gao S (2021b) Photo aging of polypropylene microplastics in estuary water and coastal seawater: Important role of chlorine ion. Water Res 202:117396. https://doi.org/10.1016/j.watres.2021.117396

    Article  CAS  Google Scholar 

  • Xi B, Wang B, Chen M, Lee X, Zhang X, Wang S, Yu Z, Wu P (2022) Environmental behaviors and degradation methods of microplastics in different environmental media. Chemosphere, 134354

  • Xiao L, Zheng Z, Irgum K, Andersson PL (2020) Studies of emission processes of polymer additives into water using quartz crystal microbalance—a case study on organophosphate esters. Environ Sci Technol 54:4876–4885

    Article  CAS  Google Scholar 

  • Xu S, Zhou P, Li H, Juhasz A, Cui X (2021) Leaching and in vivo bioavailability of antimony in PET bottled beverages. Environ Sci Technol 55:15227–15235

    Article  CAS  Google Scholar 

  • Yan Q, Ji J, Chen Y, Zhao G, Jia B, Xu L, Cheng P (2024) By-product reduction for the non-thermal plasma removal of toluene using an α-MnO2/Cordierite honeycomb monolithic catalyst in a honeycomb structure. Appl Catal B 343:123530. https://doi.org/10.1016/j.apcatb.2023.123530

    Article  CAS  Google Scholar 

  • Yu H, Hu W, He J, Ye Z (2019) Decomposition efficiency and aerosol by-products of toluene, ethyl acetate and acetone using dielectric barrier discharge technique. Chemosphere 237:124439

    Article  CAS  Google Scholar 

  • Zha F, Shang M, Ouyang Z, Guo X (2022) The aging behaviors and release of microplastics: a review. Gondwana Res 108:60–71. https://doi.org/10.1016/j.gr.2021.10.025

    Article  CAS  Google Scholar 

  • Zhang Y-T, Wei W, Huang Q-S, Wang C, Wang Y, Ni B-J (2020) Insights into the microbial response of anaerobic granular sludge during long-term exposure to polyethylene terephthalate microplastics. Water Res 179:115898

    Article  CAS  Google Scholar 

  • Zhao M, Zhang T, Yang X, Liu X, Zhu D, Chen W (2021) Sulfide induces physical damages and chemical transformation of microplastics via radical oxidation and sulfide addition. Water Res 197:117100. https://doi.org/10.1016/j.watres.2021.117100

    Article  CAS  Google Scholar 

  • Zhao X, Wang R, Zhang J, Lu S, Guo Z, Hu Z, Wang T, Dai P, Wu H (2023) Exploring simultaneous elimination of dimethyl phthalate and nitrogen by a novel constructed wetlands coupled with dielectric barrier discharge plasma. Chem Eng J 452:139666

    Article  CAS  Google Scholar 

  • Zhou L, Wang R, Liu Y, Zhang Y, Zhou J, Qu G, Tang S, Wang T (2022a) Plasma-induced conversion of polystyrene nanoplastics in water: Intermediates release, toxicity, and disinfection byproducts formation. Chem Eng J 433:134543. https://doi.org/10.1016/j.cej.2022.134543

    Article  CAS  Google Scholar 

  • Zhou L, Wang T, Qu G, Jia H, Zhu L (2020) Probing the aging processes and mechanisms of microplastic under simulated multiple actions generated by discharge plasma. J Hazard Mater 398:122956. https://doi.org/10.1016/j.jhazmat.2020.122956

    Article  CAS  Google Scholar 

  • Zhou Z, Sun Y, Wang Y, Yu F, Ma J (2022b) Adsorption behavior of Cu(II) and Cr(VI) on aged microplastics in antibiotics-heavy metals coexisting system. Chemosphere 291:132794. https://doi.org/10.1016/j.chemosphere.2021.132794

    Article  CAS  Google Scholar 

  • Zhu K, Jia H, Jiang W, Sun Y, Zhang C, Liu Z, Wang T, Guo X, Zhu L (2021) The first observation of the formation of persistent aminoxyl radicals and reactive nitrogen species on photoirradiated nitrogen-containing microplastics. Environ Sci Technol 56:779–789

    Article  Google Scholar 

  • Zurier HS, Goddard JM (2021) Biodegradation of microplastics in food and agriculture. Curr Opin Food Sci 37:37–44

    Article  CAS  Google Scholar 

Download references

Funding

The authors gratefully acknowledge financial support from the National Natural Science Foundation of China (No. 42277217 and 41877374).

Author information

Authors and Affiliations

Authors

Contributions

All authors contributed to the study conception and design. Investigation and writing—original draft preparation were performed by Zhaofeng Cai. Resources and data curation were performed by Jixing Liu. Visualization and software were performed by Gaosheng Zhao. Methodology was performed by Bing Jia. Supervision, validation, and formal analysis were performed by Yu Shang. Conceptualization writing—reviewing and editing, conceptualization, and funding acquisition were performed by Ping Cheng.

Corresponding author

Correspondence to Ping Cheng.

Ethics declarations

Ethical approval

This article does not involve any research related to humans or animals.

Consent to participate and publish

The authors agree to participate in and publish this manuscript.

Competing interests

The authors declare no competing interests.

Additional information

Responsible Editor: Thomas D. Bucheli

Publisher's note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary Information

Below is the link to the electronic supplementary material.

Supplementary file1 (DOCX 1060 kb)

Rights and permissions

Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Cai, Z., Liu, J., Zhao, G. et al. Analysis and identification of degradation products in gas, particle, and liquid phases of polypropylene and polyethyleneterephthalate microplastics aging through non-thermal plasma simulation. Environ Sci Pollut Res 31, 22847–22857 (2024). https://doi.org/10.1007/s11356-024-32586-6

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-024-32586-6

Keywords

Navigation