aState Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, School of Resources and Environmental Engineering, East China University of Science and Technology, Shanghai 200237, China
bState Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China
cShanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China
dPerkinElmer, Inc., Shanghai 201203, China
eMaihai Environmental Protection Technology Co., Ltd., Suzhou, Jiangsu 215000, China
fDepartment of Environmental Chemistry, Institute of Environmental Assessment and Water Research, Spanish Council for Scientific Research (IDAEA-CSIC), Barcelona 08034, Spain
Municipal solid waste (MSW) is an important destination for abandoned plastics. During the waste disposal process, large plastic debris is broken down into microplastics (MPs) and released into the leachate. However, current research only focuses on landfill leachates, and the occurrence of MPs in other leachates has not been studied. Therefore, herein, the abundance and characteristics of MPs in three types of leachates, namely, landfill leachate, residual waste leachate, and household food waste leachate, were studied, all leachates were collected from the largest waste disposal center in China. The results showed that the average MP abundances in the different types of leachates ranged from (129 ± 54) to (1288 ± 184) MP particles per liter (particles·L−1) and the household food waste leachate exhibited the highest MP abundance (p < 0.05). Polyethylene (PE) and fragments were the dominant polymer type and shape in MPs, respectively. The characteristic polymer types of MPs in individual leachates were different. Furthermore, the conditional fragmentation model indicated that the landfilling process considerably affected the size distribution of MPs in leachates, leading to a higher percentage (> 80%) of small MPs (20-100 μm) in landfill leachates compared to other leachates. To the best of our knowledge, this is the first study discussing the sources of MPs in different leachates, which is important for MP pollution control during MSW disposal.
Microplastics (MPs), as emerging contaminants, are attracting increasing attention because of their widespread occurrence and potential risk to the environment [1], [2]. MPs are “plastic particles with dimensions smaller than 5 mm,” and they were first detected in the marine ecosystem [3], [4]. Recently, they have also been detected in freshwater bodies [5], wastewater treatment plants (WWTPs) [6], soil [7], and even human placenta [8], [9]. Poor solid waste management activities (either nonmanagement or mismanagement), such as littering and dumping, are one of the major pathways plastic waste is released into the environment [10]. Geyer et al. [11] estimated that approximately 12 000 million tonnes of plastic waste will be discarded in landfills or the natural environment by 2050 if current production and waste management trends continues. The landfill leachate generated during solid waste disposal is a major source of MP pollution [12], [13], [14]. MPs in the leachate can easily transfer to other environmental media because their fluidity in leachates is higher than that in solid waste, and high abundances of MPs have been detected in rivers and groundwater around landfills [15], [16], [17]. Nurhasanah et al. [16] reported that downstream surface water has a threefold higher MP abundance than upstream surface water with inputs from landfill leachate drains. Additionally, MPs in leachates are vectors of other contaminants, such as heavy metals, pharmaceutical and personal care products, and antibiotic resistance genes [18], [19], [20], and exacerbate the adverse effects of leachate discharge on the surrounding environment.
Studies on the characteristics of MP contamination in landfill leachates have been conducted in some countries, including China [12], [21], [22], [23], [24], Indonesia [16], [25], and Thailand [26]. Different studies have reported different abundances of MPs in landfill leachates, ranging from < 1 to 291 MP particles per liter (particles·L−1) [12], [16], [21], [22], [23], [24], [25], [26], [27], [28], [29], [30], [31]. The use of different analytical methods is one of the reasons for the discrepancy in results in addition to the differences in the sample properties. For samples from the same site, studies targeting small-sized MPs (20 μm) have reported significantly higher MP abundances than those on large-sized MPs (> 50 μm) [21], [22]. Unfortunately, in most studies, the minimum particle size of MPs was still larger than 50 μm because of the complexity of leachate samples [13], [14], [32], [33], [34]. Another limitation in previous related studies was that the particles on filters were usually randomly selected as subsamples for identification (subsampling strategy), which may have led to considerable errors because of the inhomogeneous distribution of particles on filters and extrapolation from a small number of MP particles in the subsample [35], [36], [37]. Furthermore, previous studies were mainly based on only one sampling campaign, probably resulting in an over- or under-estimation of MP abundance. To comprehensively understand the pollution characteristics of MPs in leachates, multiple sampling campaigns and full identification of MPs with a broader size range are crucial.
Additionally, to date, the relevant information on MPs in leachates has only focused on landfill leachates [13], [33], [38]. However, landfills are not the sole disposal strategy for municipal solid wastes (MSWs). Many countries, including China, have been promoting waste sorting, and MSWs are categorized as hazardous waste, recyclable waste, household food waste, and residual waste. The sorted MSWs are treated and disposed in different ways. For example, residual waste is usually incinerated and food waste is used for resource utilization. Therefore, there are many types of other leachates than landfill leachates, such as raw incineration leachate and food waste leachate, which are generated from the stacking of fresh MSWs and food waste, respectively [39], [40], [41]. The lack of information on the presence of MPs in these leachates makes it difficult to estimate the MPs load in the raw influent of leachate treatment systems in the case of the new MSW disposal strategy and the subsequent MP amount removed during treatment. Furthermore, leachates generated after waste sorting allow a targeted analysis of their potential sources, which may provide references for further optimization of waste management. Therefore, a comprehensive study on MPs in different types of leachates is urgently required.
Herein, MPs with a size of 20-5000 μm in different types of leachates from the largest waste disposal center in China, which is located in Shanghai, the first city to enforce waste sorting in China, were studied. This study aimed to ➀ determine the occurrence and characteristics of MPs in three types of leachates (i.e., landfill leachate, residual waste leachate, and household food waste leachate) using optimized analytical methods and ➁ discuss the potential sources of MPs in different leachates. To the best of our knowledge, this is the first study on MP contamination in different types of leachates and may help future MP pollution control in MSW disposal.
2. Materials and Methods
2.1. Sampling and characterization
Leachate samples were collected from a waste disposal center in Shanghai, China. The waste disposal center, which has the highest disposal capacity in China, receives about 14 500 t·d−1 of MSWs and treats 4800 m3·d−1 of leachates. Three types of leachates were collected. Landfill leachates L1 and L2 were generated from MSW landfills of different landfill ages, which are approximately 16 and eight years, respectively. Details of the landfills are provided in Table S1 in Appendix A. MSW in Shanghai has not been directly landfilled after the implementation of waste sorting in 2019. Residual waste is incinerated. The fresh leachate generated before incineration was collected and named leachate L3. Household food waste is sent to the renewable energy utilization center. The leachate generated from the stacking of household food waste undergoes an anaerobic treatment and is delivered to a leachate treatment plant, together with other types of leachates. The leachate produced during the anaerobic fermentation was collected and named leachate L4. Disposal methods for MSWs before and after waste sorting and sampling points for leachates are shown in Fig. 1.
Duplicate samples of leachates (L1-L4, 250 mL) were collected during April, July, and December 2021. The sampling volume was 250 mL because it was more convenient to deliver the samples and results obtained with sample volumes of 250 mL or 1 L showed no significant difference in MP abundance (Kruskal-Wallis test, p > 0.05; Fig. S1 in Appendix A). Samples were collected in brown glass bottles, covered with aluminum foils to avoid contamination from plastic lids, and immediately transported to the laboratory for the following analysis.
2.2. Extraction of MPs
Samples were filtered using two stacked stainless-steel sieves (diameter = 5 cm) with descending mesh sizes of 150 and 20 μm. All solids collected on the 150 and 20 μm sieves were carefully rinsed into different beakers using 250 and 1000 mL of Milli-Q water, respectively (Fig. S2 in Appendix A). The volume of rinse water was determined using recovery experiments (Supplementary Text S1 in Appendix A). Approximately 35 and 15 mL of H2O2 (30%, v/v) were added to 250 mL and 1 L beakers, respectively, to remove natural organic matter, and the digestion process lasted at least two days until bubbling stopped. Then, the digested samples were filtered using a dual filter system, as described in the study by Xu et al. [21]. Particles in the samples were retained using a customized stainless-steel filter. The stainless-steel filters were placed in folded aluminum foils and dried at room temperature (∼25 °C).
2.3. Identification of MPs
All particles on the stainless-steel filter were examined using a Fourier transform infrared (FTIR) microscope (Spotlight 200i; PerkinElmer, USA), which was operated in the transmission mode. The spectrum was obtained as an average of 16 scans in the wavenumber range of 4000-650 cm-1 with a resolution of 4 cm-1.
Results were compared with the standard spectra from the data library (i.e., Polymers, Hummel, Poly1, Polyadd1, Polyatr, Rubber, and Fibers) to identify the polymer type. The results with matching degrees higher or equal to 70% were considered positive and credible. Results with matching degrees between 60% and 70% were manually examined and interpreted based on the proximity of their absorption frequencies to the chemical bonds in known polymers. Particles with matching degrees less than 60% were rejected [42].
MPs that passed the matching degree check were grouped based on their shapes, which were categorized as fragments (pieces of irregular, thick plastic), flocs (spherical or spongy textured particles), flakes (thin plastic sheets), films (translucent flimsy plastic), and fibers (fibrous or straight plastic). MPs were also categorized into four groups according to their colors, namely, translucent, light, dark, and characteristic (blue or red) because the imaging function of the FTIR microscope had a relatively low color resolution.
2.4. Quality assurance and quality control
Recovery experiments were performed to assess the reliability of the methods. First, the effect of rinse water volume (i.e., 250, 500, and 1000 mL) on the extraction of MPs was studied. The results are shown in Supplementary Text S1 and Table S2 in Appendix A, and chosen conditions showed high MP recoveries during the rinsing of 150 μm (250 mL: 98.2% ± 0.3%) and 20 μm (1000 mL: 97.2% ± 0.5%) sieves, respectively. Second, the recovery of MPs during the entire pretreatment process was studied using a modified method from the study by Xu et al. [21]. Polyethylene (PE) MPs (1 g·cm−3, blue; Cospheric, USA) equivalent to the environmental abundance (200-300 particles·L−1) were spiked in leachate samples. The number of spiked MPs was selected according to the previous reported results on MPs in landfill leachate (Table S3 in Appendix A). The leachate samples were first filtered using glass fiber filters (GF/F; Whatman, UK) to exclude the influence of MPs originally present in the samples. The sizes of standard MPs were 27-45, 53-106, and 125-1000 μm, and the corresponding proportions added to leachates were approximately 35% (27-45 μm), 25% (53-106 μm), and 40% (125-1000 μm), respectively, which were similar to the size distribution of MPs found in other studies on leachates [24]. The recovery of spiked MPs was (75.7% ± 1.5%) in leachate samples (the number of replicates was 3).
All apparatus (e.g., sampling bottles, stainless-steel sieves, beakers, and customized stainless-steel filters) used was cleaned once with ethanol and three times with Milli-Q water before use. Cotton lab coats and nitrile gloves were worn during the entire analytical procedure, and beakers were covered with aluminum foils during the digestion process to avoid contamination of MPs in the atmosphere. Field and laboratory blanks were analyzed using the same procedure described above. No MP was identified in all blank samples. This, along with the recovery results, indicates that the analytical protocol adopted in this study is valid.
2.5. Data analysis
All figures were plotted using OriginPro 2023 (OriginLab, USA), and statistical analysis was performed using SPSS 26.0 software (IBM, USA). The differences in MP abundances between different leachates were compared using the Kruskal-Wallis test, and the differences in types, sizes, shapes, and colors were determined using one-way analysis of variance followed by Tukey’s test (homogeneous variances) or Tamhan’s T2 test (heterogeneous variances). The level of significance was set at α = 0.05.
The condition fragmentation model was used to understand the stability and particle size distribution of MPs in different leachates. The simplified expression of this model is shown in Eq. (1) [43].
$ F(x)=1-\mathrm{e}^{-\lambda x^{\alpha}}$
where x is the size of MPs, F(x) is the cumulative distribution function (CDF) of the MP size, and λ and α are coefficients that describe the relative location and shape of the CDF and represent the extent of fragmentation and the stability of MPs, respectively (Supplementary Text S2 and Fig. S3 in Appendix A). A higher λ value indicates the presence of smaller MPs and a higher degree of fragmentation in the sample. If α > 1, the probability of being broken down into smaller MPs would be suppressed for MPs, whereas α < 1 indicated that MPs would suffer from progressive downsizing.
3. Results and Discussion
3.1. Abundance of MPs in different leachates
MP abundances in different leachates had no significant difference among different sampling campaigns (Kruskal-Wallis test, p > 0.05). Fig. 2 shows the average abundance of MPs in different leachates for all sampling events. The average abundances ranged one order of magnitude from (129 ± 54) (L2) to (1288 ± 184) particles·L−1 (L4). MP abundances detected in leachates in this study were higher than those identified in other studies on other potential MP sources, such as domestic, industrial agricultural, and livestock wastewater [44], [45], [46], [47]. For example, Wang et al. [44] studied the occurrence of MPs with sizes higher or equal to 16 μm in nine WWTPs in China and found that MP abundances in most WWTPs ranged from 18 to 45 particles·L−1. MP abundances obtained in this study were higher than or comparable to those reported in previous literature on landfill leachates (0.06-291 particles·L−1) [12], [16], [21], [22], [23], [24], [25], [26], [27], [28], [29], [30], [31]. These comparisons further indicated that leachates are an important contributor of MPs in the environment.
Leachates from landfills of different ages exhibited similar levels of MP contamination. The MP abundances in landfill leachates from the shorter (L2) and longer (L1) landfill ages were (129 ± 54) and (138 ± 67) particles·L−1, respectively. This finding contradicted a previous study [22]. Su et al. [22] investigated the occurrence of MPs in leachates from landfills of different ages and reported that landfill leachate with the longest landfill age had a significantly lower MP abundance than the shorter landfill ages. In their study, the minimum particle size detected was limited to 70 μm, which is much larger than the lower size limit of MPs (20 μm) in this study. This discrepancy in results may be because large plastics tend to break into small pieces (< 100 μm) with time and limitations in the analytical method can cause oversight of MP abundance, especially tiny plastics in landfill leachates from longer landfill ages. Because the detection size range was expanded in this study, a more comprehensive understanding of MP abundance in the leachates could be obtained.
Household food waste leachate (L4) exhibited the highest MP abundance of (1288 ± 184) particles·L−1, which was approximately seven and ten times higher than those of residual waste leachate (L3) and landfill leachates (L1 and L2), respectively. Because L4 was collected after anaerobic treatment, and the anaerobic treatment process can remove a considerable amount of MPs [48], [49], it is reasonable to propose that more MPs are present in the leachate directly collected from household food waste. The extensive sources of MPs in food are responsible for the high abundance of MPs in L4. MP contamination has been confirmed in rice, fruits, and vegetables [50], [51]. Disposable plastic containers also cause MP contamination in food [52], [53]. The MP abundance was the highest in household food waste, indicating the high MP pollution levels in food, and more attention should be paid to food safety to reduce the potential risk of MPs to human health.
3.2. Polymer type of MPs in different leachates
Fig. 3 shows that 34 polymer types were identified in the collected samples. PE and polypropylene (PP) were the most frequently present polymer types, detected in all leachate samples, with average proportions of 32% and 24%, respectively. By contrast, 11 polymer types, such as polycarbonate (PC), poly(styrene- acrylonitrile-butadiene) (ABS), and polyacrylamide (PAM), were found in only one type of leachate.
The total number of polymer types detected in landfill leachates (10 and 16 in L1 and L2, respectively) was lower than that in fresh leachates (29 and 21 in L3 and L4, respectively). As the landfill ages, some plastics degrade and cannot be found in landfill leachates. For example, rayon was detected in fresh leachates L3 and L4 but not in landfill leachates L1 and L2 because it has low crystallinity and orientation, can be used as a readily available source of carbon by microorganisms [54], [55], [56], and degrades by approximately 62% after 243 days of biodegradation [57].
Different leachates had significantly different characteristic polymer types. High density polyethylene (HDPE) is widely used in toys, milk bottles, and houseware [58]. However, surprisingly, HDPE was not detected in L4 and accounted for less than 1% in L3. By contrary, the proportions of HDPE in landfill leachates (L1 and L2) were high (∼10%). This may be because in landfill leachates, HDPE mainly originated from the geomembrane used in the landfill in addition to that from disposed MSWs. In the investigated landfills, HDPE geomembranes were used as anti-seepage and covering materials. They may break and release MPs during the long-term landfill process, resulting in HDPE contamination in the landfill leachate. Sun et al. [59] reported that mechanical damage and waste settlement during the construction and operation of a landfill led to the cracking of the geomembrane. Their results indicated that the HDPE geomembrane reached its service life after eight years of operation at landfill sites, and the material would have serious aging and defects. By contrast, HDPE was not detected in the leachate generated by an informal landfill (without geomembranes application) [30]. This result also supported the hypothesis that the broken HDPE geomembrane is one important source of MPs in the investigated sanitary landfill leachates.
The composition of MPs in L4 was different from those of the other three leachates. PE, polyamide or nylon (PA), and polyethylene polypropylene copolymer (PE/PP) were the main polymer types in L4, with average proportions of 21%, 13%, and 12%, respectively. The proportion of PA in L4 was approximately two times higher than that in L3 and significantly higher than that in L1 and L2. As discussed in Section 3.1, MPs in L4 reflected the pollution of MPs in food. Although the studies on MP contamination in food are limited, studies have reported that there was a high abundance of PA in mussels and fish [60], [61], [62], [63]. Broken nylon cages and cables used in the aquaculture are the potential sources of PA in these aquaculture animals [64]. Zhang et al. [65] also reported PE-PP (∼65%) and PE (∼30%) were the main types of MPs in crayfish. The predominance of PE, PA, and PE-PP in L4 showed that aquatic products may be one of the major sources of MPs in food in the studied region, in line with the dietary habits of people in Shanghai. Understanding the polymer type can help more accurately identify the source of MPs and provide references for future MP pollution control.
3.3. Morphology characteristics of MPs in different leachates
Fig. 4(a) shows the size distributions of MPs in different leachates. MPs with sizes of 20-100 μm in L1 and L2 accounted for 87% and 83%, respectively. Fewer small MPs (20-100 μm) were found in fresh leachates L3 (67%) and L4 (49%) compared to those in landfill leachates. According to the conditional fragmentation model (Fig. S4 in Appendix A and Table 1), landfill leachates, especially the one with a relatively long landfill age (L1), have higher λ values compared to L3 and L4, indicating higher degrees of MP fragmentation in landfill leachates. These results indicated that landfilling process had a significant impact on the size distribution of MPs and verified the hypothesis that large plastics were broken during the long-term landfill process, releasing a large number of small MPs in landfill leachate. Additionally, the α values obtained from the conditional fragmentation model are less than 1 for both L3 and L4. This indicated that MPs in L3 and L4 still suffered from progressive downsizing, and would continue to fragment into smaller MPs. Therefore, abundance of MPs in L3 and L4 may further increase during the subsequent leachate treatment processes.
Fig. 4(b) compares the shapes of MPs in different leachates, and the typical shapes of MPs are shown in Fig. S5 in Appendix A. Previous studies reported conflicting results about the shape of MPs in landfill leachates. He et al. [12] reported the predominance of fragments and flakes in landfill leachates, the proportions of which were 59% and 23%, respectively. Sun et al. [24] also found that more than 50% of the MPs in landfill leachates were fragments. However, in other studies [22], [23], fiber MPs had the highest contents in landfill leachates. For example, Su et al. [22] reported that fiber MPs accounted for about 60% of the total MPs in the leachate. Herein, fragments were the main shape of MPs in leachates (accounting for 51%-67% of MPs), whereas there was a smaller fraction of fiber MPs, ranging from 4% to 14%. Fiber is usually the most common shape in sewage, accounting for more than 85% of MPs detected in some studies [66], [67], and mainly originates from laundry and fiber manufacturing [6], [66], [67]. Fibers also fragment into smaller particles, which are identified as fragments. Therefore, the proportion of fragments increases with a decrease in the MP size [43]. The predominance of fragments rather than fibers in this study was consistent with the large proportion of small MPs and indicated that the origin of MPs in leachates was different from those in sewage.
Most MPs were light or dark colored (Fig. 4(c)). The proportion of translucent MPs in L1 was much higher than those in L2 (short landfill age) and L3 (without landfilled), probably because plastic aging occurred during the landfill process [24].
4. Conclusions
This study investigated the occurrence and characteristics of MPs in three types of leachates (landfill leachate, residual waste leachate, and household food waste leachate) collected from the largest waste disposal center in China. The abundances of MPs ranged from (129 ± 54) to (1288 ± 184) particles·L−1, and the household food waste leachate had the significantly highest MP abundance. A total of 34 different polymer types were identified, and large contributions of PE (32%) and PP (24%) were observed in all leachate samples. Different disposal strategies affect the characteristic of MPs in individual leachates. Landfilling process considerably affected the size distribution of MPs in leachates, leading to a higher percentage (> 80%) of small MPs (20-100 μm) in landfill leachates compared to other leachates. The shifting of waste disposal from landfilling to other disposal strategies may change MP contamination characteristics in leachates need to be treated.
Acknowledgments
This work was partly supported by the National Key Research and Development Program of China (2023YFC3711600), the National Natural Science Foundation of China (22076045 and 22376066), the Shanghai Talent Development Funding, and the Shanghai Youth Talent Support Program.
Compliance with ethics guidelines
Lei Zhang, Wentao Zhao, Liang Zhang, Zhenxiao Cai, Ruiqi Yan, Xia Yu, Damià Barceló, and Qian Sui declare that they have no conflict of interest or financial conflicts to disclose.
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