Abstract
Traditional stereomicroscopy (SM) is limited for the identification of microplastics of less than 500 µm in wastewater treatment plants (WWTPs). Accordingly, novel methods for the accurate quantification of these microplastics are needed. In this study, we investigated the polymer type, morphology, size distribution, and abundance of microplastics in each unit of three selected WWTPs by SM and a fluorescence-based protocol (FR) combined with FTIR. Using the FR method, most microplastics detected in the three WWTPs were 50–200 µm in size. Polyethylene, polypropylene, and polyamide were the main polymer types, and the distributions of fibers, films, and debris were determined. Despite highly similar microplastic removal rates (78.6‒95.2% (SM) and 77.4‒94.2% (FR)) in the WWTPs by the two methods, the microplastic abundances obtained by FR (405‒6987 items/L) were approximately 2 orders of magnitude higher than the corresponding results by SM (1‒21 items/L). In addition, a considerable number of small-sized microplastics (< 500 µm) were detected in the effluents (405‒947 items/L) using FR. These results clearly reveal that microplastics in WWTPs have been seriously underestimated in most previous studies based on SM. Further research should focus on the environmental risks of small-sized microplastics from WWTPs.
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References
Akhbarizadeh R, Dobaradaran S, Nabipour I, Tajbakhsh S, Darabi AH, Spitz J (2020a) Abundance, composition, and potential intake of microplastics in canned fish. Mar Pollut Bull 160:111633. https://doi.org/10.1016/j.marpolbul.2020a.111633
Akhbarizadeh R, Dobaradaran S, Schmidt TC, Nabipour I, Spitz J (2020b) Worldwide bottled water occurrence of emerging contaminants: a review of the recent scientific literature. J Hazard Mater 392:122271. https://doi.org/10.1016/j.jhazmat.2020b.122271
Akhbarizadeh R, Dobaradaran S, AmoueiTorkmahalleh M, Saeedi R, Aibaghi R, FarajiGhasemi F (2021) Suspended fine particulate matter (PM2.5), microplastics (MPs), and polycyclic aromatic hydrocarbons (PAHs) in air: their possible relationships and health implications. Environ Res 192:110339. https://doi.org/10.1016/j.envres.2020.110339
Ali I, Ding T, Peng C, Naz I, Sun H, Li J, Liu J (2021) Micro- and nanoplastics in wastewater treatment plants: occurrence, removal, fate, impacts and remediation technologies – a critical review. Chem Eng J 423:130205. https://doi.org/10.1016/j.cej.2021.130205
Amato-Lourenço LF, Carvalho-Oliveira R, Júnior GR, dos Santos Galvão L, Ando RA, Mauad T (2021) Presence of airborne microplastics in human lung tissue. J Hazard Mater 416:126124. https://doi.org/10.1016/j.jhazmat.2021.126124
Araujo CF, Nolasco MM, Ribeiro AMP, Ribeiro-Claro PJA (2018) Identification of microplastics using Raman spectroscopy: latest developments and future prospects. Water Res 142:426–440. https://doi.org/10.1016/j.watres.2018.05.060
Becucci M, Mancini M, Campo R, Paris E (2022) Microplastics in the Florence wastewater treatment plant studied by a continuous sampling method and Raman spectroscopy: a preliminary investigation. Sci Total Environ 808:152025. https://doi.org/10.1016/j.scitotenv.2021.152025
Bilgin M, Yurtsever M, Karadagli F (2020) Microplastic removal by aerated grit chambers versus settling tanks of a municipal wastewater treatment plant. J Water Process Eng 38:101604. https://doi.org/10.1016/j.jwpe.2020.101604
Bretas Alvim C, Mendoza-Roca JA, Bes-Piá A (2020) Wastewater treatment plant as microplastics release source – quantification and identification techniques. J Environ Manage 255:109739. https://doi.org/10.1016/j.jenvman.2019.109739
Carr SA, Liu J, Tesoro AG (2016) Transport and fate of microplastic particles in wastewater treatment plants. Water Res 91:174–182. https://doi.org/10.1016/j.watres.2016.01.002
Caruso G (2019) Microplastics as vectors of contaminants. Mar Pollut Bull 146:921–924. https://doi.org/10.1016/j.marpolbul.2019.07.052
De Falco F, Gullo MP, Gentile G, Di Pace E, Cocca M, Gelabert L, Brouta-Agnésa M, Rovira A, Escudero R, Villalba R, Mossotti R, Montarsolo A, Gavignano S, Tonin C, Avella M (2018) Evaluation of microplastic release caused by textile washing processes of synthetic fabrics. Environ Pollut 236:916–925. https://doi.org/10.1016/j.envpol.2017.10.057
Ding L, Mao R, fan, Guo, X., Yang, X., Zhang, Q., Yang, C., (2019) Microplastics in surface waters and sediments of the Wei River, in the northwest of China. Sci Total Environ 667:427–434. https://doi.org/10.1016/j.scitotenv.2019.02.332
Dobaradaran S, Schmidt TC, Nabipour I, Khajeahmadi N, Tajbakhsh S, Saeedi R, JavadMohammadi M, Keshtkar M, Khorsand M, FarajiGhasemi F (2018) Characterization of plastic debris and association of metals with microplastics in coastline sediment along the Persian Gulf. Waste Manag 78:649–658. https://doi.org/10.1016/j.wasman.2018.06.037
Duis K, Coors A (2016) Microplastics in the aquatic and terrestrial environment: sources (with a specific focus on personal care products), fate and effects. Environ Sci Eur 28:1–25. https://doi.org/10.1186/s12302-015-0069-y
Edo C, González-Pleiter M, Leganés F, Fernández-Piñas F, Rosal R (2020) Fate of microplastics in wastewater treatment plants and their environmental dispersion with effluent and sludge. Environ Pollut 259:113837. https://doi.org/10.1016/j.envpol.2019.113837
Erni-Cassola G, Gibson MI, Thompson RC, Christie-Oleza JA (2017) Lost, but found with Nile red: a novel method for detecting and quantifying small microplastics (1 mm to 20 μm) in environmental samples. Environ Sci Technol 51:13641–13648. https://doi.org/10.1021/acs.est.7b04512
Estahbanati S, Fahrenfeld NL (2016) Influence of wastewater treatment plant discharges on microplastic concentrations in surface water. Chemosphere 162:277–284. https://doi.org/10.1016/j.chemosphere.2016.07.083
Fan X, Gan R, Liu J, Xie Y, Xu D, Xiang Y, Su J, Teng Z, Hou J (2021) Adsorption and desorption behaviors of antibiotics by tire wear particles and polyethylene microplastics with or without aging processes. Sci Total Environ 771:145451. https://doi.org/10.1016/j.scitotenv.2021.145451
Funck M, Al-Azzawi MMS, Yildirim A, Knoop O, Schmidt TC, Drewes JE, Tuerk J (2021) Release of microplastic particles to the aquatic environment via wastewater treatment plants: the impact of sand filters as tertiary treatment. Chem Eng J 426:130933. https://doi.org/10.1016/j.cej.2021.130933
Gao X, Hassan I, Peng Y, Huo S, Ling L (2021) Behaviors and influencing factors of the heavy metals adsorption onto microplastics: a review. J Clean Prod 319:128777. https://doi.org/10.1016/j.jclepro.2021.128777
Gies EA, LeNoble JL, Noël M, Etemadifar A, Bishay F, Hall ER, Ross PS (2018) Retention of microplastics in a major secondary wastewater treatment plant in Vancouver. Canada Mar Pollut Bull 133:553–561. https://doi.org/10.1016/j.marpolbul.2018.06.006
Gillibert R, Balakrishnan G, Deshoules Q, Tardivel M, Magazzù A, Donato MG, Maragò OM, Lamy De La Chapelle M, Colas F, Lagarde F, Gucciardi PG (2019) Raman tweezers for small microplastics and nanoplastics identification in seawater. Environ Sci Technol 53:9003–9013. https://doi.org/10.1021/acs.est.9b03105
Hajiouni S, Mohammadi A, Ramavandi B, Arfaeinia H, De-la-Torre GE, Tekle-Röttering A, Dobaradaran S (2022) Occurrence of microplastics and phthalate esters in urban runoff: a focus on the Persian Gulf coastline. Sci Total Environ 806:150559. https://doi.org/10.1016/j.scitotenv.2021.150559
Hengstmann E, Fischer EK (2019) Nile red staining in microplastic analysis — proposal for a reliable and fast identification approach for large microplastics. Env Monit Assess 191:612. https://doi.org/10.1007/s10661-019-7786-4
Horton AA, Cross RK, Read DS, Jürgens MD, Ball HL, Svendsen C, Vollertsen J, Johnson AC (2021) Semi-automated analysis of microplastics in complex wastewater samples. Environ Pollut 268:115841. https://doi.org/10.1016/j.envpol.2020.115841
Huang W, Song B, Liang J, Niu Q, Zeng G, Shen M, Deng J, Luo Y, Wen X, Zhang Y (2021) Microplastics and associated contaminants in the aquatic environment: a review on their ecotoxicological effects, trophic transfer, and potential impacts to human health. J Hazard Mater 405:124187. https://doi.org/10.1016/j.jhazmat.2020.124187
Hüffer T, Weniger AK, Hofmann T (2018) Sorption of organic compounds by aged polystyrene microplastic particles. Environ Pollut 236:218–225. https://doi.org/10.1016/j.envpol.2018.01.022
Kankanige D, Babel S (2021) Contamination by ≥6.5 μm-sized microplastics and their removability in a conventional water treatment plant (WTP) in Thailand. J Water Process Eng 40:101765. https://doi.org/10.1016/j.jwpe.2020.101765
Kashfi FS, Ramavandi B, Arfaeinia H, Mohammadi A, Saeedi R, De-la-Torre GE, Dobaradaran S (2022) Occurrence and exposure assessment of microplastics in indoor dusts of buildings with different applications in Bushehr and Shiraz cities Iran. Sci Total Environ 829:154651. https://doi.org/10.1016/j.scitotenv.2022.154651
Kazour M, Terki S, Rabhi K, Jemaa S, Khalaf G, Amara R (2019) Sources of microplastics pollution in the marine environment: importance of wastewater treatment plant and coastal landfill. Mar Pollut Bull 146:608–618. https://doi.org/10.1016/j.marpolbul.2019.06.066
Lares M, Ncibi MC, Sillanpää M, Sillanpää M (2018) Occurrence, identification and removal of microplastic particles and fibers in conventional activated sludge process and advanced MBR technology. Water Res 133:236–246. https://doi.org/10.1016/j.watres.2018.01.049
Lee H, Kim Y (2018) Treatment characteristics of microplastics at biological sewage treatment facilities in Korea. Mar Pollut Bull 137:1–8. https://doi.org/10.1016/j.marpolbul.2018.09.050
Leslie HA, Brandsma SH, van Velzen MJM, Vethaak AD (2017) Microplastics en route: field measurements in the Dutch river delta and Amsterdam canals, wastewater treatment plants, North Sea sediments and biota. Environ Int 101:133–142. https://doi.org/10.1016/j.envint.2017.01.018
Li X, Li M, Mei Q, Niu S, Wang X, Xu H, Dong B, Dai X, Zhou JL (2021) Aging microplastics in wastewater pipeline networks and treatment processes: physicochemical characteristics and Cd adsorption. Sci Total Environ 797:148940. https://doi.org/10.1016/j.scitotenv.2021.148940
Liu X, Yuan W, Di M, Li Z, Wang J (2019) Transfer and fate of microplastics during the conventional activated sludge process in one wastewater treatment plant of China. Chem Eng J 362:176–182. https://doi.org/10.1016/j.cej.2019.01.033
Liu W, Zhang J, Liu H, Guo X, Zhang X, Yao X, Cao Z, Zhang T (2021) A review of the removal of microplastics in global wastewater treatment plants: characteristics and mechanisms. Environ Int 146:106277. https://doi.org/10.1016/j.envint.2020.106277
Liu S, Shang E, Liu J, Wang Y, Bolan N, Kirkham MB, Li Y (2022) What have we known so far for fluorescence staining and quantification of microplastics: a tutorial review. Front Environ Sci Eng 16:1–14. https://doi.org/10.1007/s11783-021-1442-2
Long Z, Pan Z, Wang W, Ren J, Yu X, Lin L, Lin H, Chen H, Jin X (2019) Microplastic abundance, characteristics, and removal in wastewater treatment plants in a coastal city of China. Water Res 155:255–265. https://doi.org/10.1016/j.watres.2019.02.028
Lv L, Qu J, Yu Z, Chen D, Zhou C, Hong P, Sun S, Li C (2019) A simple method for detecting and quantifying microplastics utilizing fluorescent dyes - Safranine T, fluorescein isophosphate, Nile red based on thermal expansion and contraction property. Environ Pollut 255:113283. https://doi.org/10.1016/j.envpol.2019.113283
Mao R, Lang M, Yu X, Wu R, Yang X, Guo X (2020) Aging mechanism of microplastics with UV irradiation and its effects on the adsorption of heavy metals. J Hazard Mater 393:122515. https://doi.org/10.1016/j.jhazmat.2020.122515
Mason SA, Garneau D, Sutton R, Chu Y, Ehmann K, Barnes J, Fink P, Papazissimos D, Rogers DL (2016) Microplastic pollution is widely detected in US municipal wastewater treatment plant effluent. Environ Pollut 218:1045–1054. https://doi.org/10.1016/j.envpol.2016.08.056
Mishra AK, Singh J, Mishra PP (2021) Microplastics in polar regions: an early warning to the world’s pristine ecosystem. Sci Total Environ 784:147149. https://doi.org/10.1016/j.scitotenv.2021.147149
Mohammadi A, Malakootian M, Dobaradaran S, Hashemi M, Jaafarzadeh N (2022) Occurrence, seasonal distribution, and ecological risk assessment of microplastics and phthalate esters in leachates of a landfill site located near the marine environment: Bushehr Port, Iran as a case. Sci Total Environ 842:156838. https://doi.org/10.1016/j.scitotenv.2022.156838
Murphy F, Ewins C, Carbonnier F, Quinn B (2016) Wastewater treatment works (WwTW) as a source of microplastics in the aquatic environment. Environ Sci Technol 50:5800–5808. https://doi.org/10.1021/acs.est.5b05416
Napper IE, Thompson RC (2016) Release of synthetic microplastic plastic fibres from domestic washing machines: effects of fabric type and washing conditions. Mar Pollut Bull 112:39–45. https://doi.org/10.1016/j.marpolbul.2016.09.025
Nguyen NB, Kim MK, Le QT, Ngo DN, Zoh KD, Joo SW (2021) Spectroscopic analysis of microplastic contaminants in an urban wastewater treatment plant from Seoul. South Korea Chemosphere 263:127812. https://doi.org/10.1016/j.chemosphere.2020.127812
Peng G, Zhu B, Yang D, Su L, Shi H, Li D (2017) Microplastics in sediments of the Changjiang Estuary. China Environ Pollut 225:283–290. https://doi.org/10.1016/j.envpol.2016.12.064
Prata JC, Sequeira IF, Monteiro SS, Silva ALP, da Costa JP, Dias-Pereira P, Fernandes AJS, da Costa FM, Duarte AC, Rocha-Santos T (2021) Preparation of biological samples for microplastic identification by Nile red. Sci Total Environ 783:147065. https://doi.org/10.1016/j.scitotenv.2021.147065
R Core Team (2018) R: a language and environment for statistical computing. R Foundation for Statistical Computing, Vienna, Austria.
Raju S, Carbery M, Kuttykattil A, Senthirajah K, Lundmark A, Rogers Z, SCB S, Evans G, Palanisami T (2020) Improved methodology to determine the fate and transport of microplastics in a secondary wastewater treatment plant. Water Res 173:115549. https://doi.org/10.1016/j.watres.2020.115549
Ren Z, Gui X, Xu X, Zhao L, Qiu H, Cao X (2021) Microplastics in the soil-groundwater environment: aging, migration, and co-transport of contaminants – a critical review. J Hazard Mater 419:126455. https://doi.org/10.1016/j.jhazmat.2021.126455
Schmidt C, Kumar R, Yang S, Büttner O (2020) Microplastic particle emission from wastewater treatment plant effluents into river networks in Germany: loads, spatial patterns of concentrations and potential toxicity. Sci Total Environ 737:139544. https://doi.org/10.1016/j.scitotenv.2020.139544
Shim WJ, Song YK, Hong SH, Jang M (2016) Identification and quantification of microplastics using Nile red staining. Mar Pollut Bull 113:469–476. https://doi.org/10.1016/j.marpolbul.2016.10.049
Shruti VC, Pérez-Guevara F, Roy PD, Kutralam-Muniasamy G (2022) Analyzing microplastics with Nile red: emerging trends, challenges, and prospects. J Hazard Mater 423:127171. https://doi.org/10.1016/j.jhazmat.2021.127171
Song YK, Hong SH, Jang M, Han GM, Jung SW, Shim WJ (2017) Combined effects of UV exposure duration and mechanical abrasion on microplastic fragmentation by polymer type. Environ Sci Technol 51:4368–4376. https://doi.org/10.1021/acs.est.6b06155
Summers S, Henry T, Gutierrez T (2018) Agglomeration of nano- and microplastic particles in seawater by autochthonous and de novo-produced sources of exopolymeric substances. Mar Pollut Bull 130:258–267. https://doi.org/10.1016/j.marpolbul.2018.03.039
Takdastan A, Niari MH, Babaei A, Dobaradaran S, Jorfi S, Ahmadi M (2021) Occurrence and distribution of microplastic particles and the concentration of di 2-ethyl hexyl phthalate (DEHP) in microplastics and wastewater in the wastewater treatment plant. J Environ Manage 280:111851. https://doi.org/10.1016/j.jenvman.2020.111851
Tang N, Liu X, Xing W (2020) Microplastics in wastewater treatment plants of Wuhan, Central China: abundance, removal, and potential source in household wastewater. Sci Total Environ 745:141026. https://doi.org/10.1016/j.scitotenv.2020.141026
Tong H, Jiang Q, Hu X, Zhong X (2020) Occurrence and identification of microplastics in tap water from China. Chemosphere 252:126493. https://doi.org/10.1016/j.chemosphere.2020.126493
Tong H, Jiang Q, Zhong X, Hu X (2021) Rhodamine B dye staining for visualizing microplastics in laboratory-based studies. Environ Sci Pollut Res 28:4209–4215. https://doi.org/10.1007/s11356-020-10801-4
Vardar S, Onay TT, Demirel B, Kideys AE (2021) Evaluation of microplastics removal efficiency at a wastewater treatment plant discharging to the Sea of Marmara. Environ Pollut 289:117862. https://doi.org/10.1016/j.envpol.2021.117862
Wang Z, Zhang Y, Kang S, Yang L, Shi H, Tripathee L, Gao T (2021) Research progresses of microplastic pollution in freshwater systems. Sci Total Environ 795:148888. https://doi.org/10.1016/j.scitotenv.2021.148888
Way C, Hudson MD, Williams ID, Langley GJ (2022) Evidence of underestimation in microplastic research: a meta-analysis of recovery rate studies. Sci Total Environ 805:150227. https://doi.org/10.1016/j.scitotenv.2021.150227
Wright SL, Kelly FJ (2017) Plastic and human health: a micro issue? Environ Sci Technol 51:6634–6647. https://doi.org/10.1021/acs.est.7b00423
Xia F, Yao Q, Zhang J, Wang D (2021) Effects of seasonal variation and resuspension on microplastics in river sediments. Environ Pollut 286:117403. https://doi.org/10.1016/j.envpol.2021.117403
Xia F, Liu H, Zhang J, Wang D (2022) Migration characteristics of microplastics based on source-sink investigation in a typical urban wetland. Water Res 213:118154. https://doi.org/10.1016/j.watres.2022.118154
Xiong X, Zhang K, Chen X, Shi H, Luo Z, Wu C (2018) Sources and distribution of microplastics in China’s largest inland lake – Qinghai Lake. Environ Pollut 235:899–906. https://doi.org/10.1016/j.envpol.2017.12.081
Xu X, Zhang L, Jian Y, Xue Y, Gao Y, Peng M, Jiang S, Zhang Q (2021a) Influence of wastewater treatment process on pollution characteristics and fate of microplastics. Mar Pollut Bull 169:112448. https://doi.org/10.1016/j.marpolbul.2021.112448
Xu Z, Bai X, Ye Z (2021b) Removal and generation of microplastics in wastewater treatment plants: a review. J Clean Prod 291:125982. https://doi.org/10.1016/j.jclepro.2021.125982
Yang T, Luo J, Nowack B (2021) Characterization of nanoplastics, fibrils, and microplastics released during washing and abrasion of polyester textiles. Environ Sci Technol 55:15873–15881. https://doi.org/10.1021/acs.est.1c04826
Zhang Q, Xu EG, Li J, Chen Q, Ma L, Zeng EY, Shi H (2020) A review of microplastics in table salt, drinking water, and air: direct human exposure. Environ Sci Technol 54:3740–3751. https://doi.org/10.1021/acs.est.9b04535
Zhang Y, Li Y, Su F, Peng L, Liu D (2022) The life cycle of micro-nano plastics in domestic sewage. Sci Total Environ 802:149658. https://doi.org/10.1016/j.scitotenv.2021.149658
Ziajahromi S, Neale PA, Rintoul L, Leusch FDL (2017) Wastewater treatment plants as a pathway for microplastics: development of a new approach to sample wastewater-based microplastics. Water Res 112:93–99. https://doi.org/10.1016/j.watres.2017.01.042
Ziajahromi S, Neale PA, Telles Silveira I, Chua A, Leusch FDL (2021) An audit of microplastic abundance throughout three Australian wastewater treatment plants. Chemosphere 263:128294. https://doi.org/10.1016/j.chemosphere.2020.128294
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This work was supported by the National Natural Science Foundation of China (Grant Nos. 51638006 and 51868011), the Department of Science and Technology of Guangxi (Grant No. 2018GXNSFGA281001), and the Special Fund for Guangxi Distinguished Experts.
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Jia-jing Pan: investigation and writing of original draft. Hong-tao Liu: Conceptualization and writing which included review and editing. Fei-yang Xia: Investigation and formal analysis. Jun Zhang: Conceptualization, writing which included review and editing, and supervision. Dun-qiu Wang: writing, which included review, and resources.
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Pan, J., Liu, H., Xia, F. et al. Occurrence and fate of microplastics from wastewater treatment plants assessed by a fluorescence-based protocol. Environ Sci Pollut Res 30, 28690–28703 (2023). https://doi.org/10.1007/s11356-022-24196-x
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DOI: https://doi.org/10.1007/s11356-022-24196-x