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Article history: A growing body of research has recently revealed that airborne microplastics could be an important source of
Received 7 January 2019 microplastic pollution in marine environments. However, the origins and spatial distributions of suspended at-
Received in revised form 11 March 2019 mospheric microplastics (SAMPs) are poorly understood. Further, SAMPs abundances have only been observed
Accepted 8 April 2019
using passive sampling devices that could lead to underestimates of abundances. To address these knowledge-
Available online 9 April 2019
gaps, the current study investigated the potential source and spatial distribution of SAMPs in Shanghai during
Editor: James Chapman May 2018 using an active suspended particulate sampler. SAMPs abundances from filtered air ranged from 0
to 4.18 n/m3 (items per cubic meter of air). Microfibers comprised 67% of all SAMPs, followed by fragments
Keywords: and granules comprising 30% and 3% of SAMPs, respectively. μ-FT-IR analysis revealed that the SAMPs consisted
Atmosphere of polyethylene terephthalate (PET), polyethylene (PE), polyester (PES), polyacrylonitrile (PAN), poly(N-methyl
Suspended atmospheric microplastics acrylamide) (PAA), rayon (RY), ethylene vinyl acetate (EVA), epoxy resin (EP), and alkyd resin (ALK). Synthetic
Distribution compounds comprised 54% of the observed particles, of which PET, PE, PES, PAN, PAA, and RY comprised 91% of
Composition the microplastics. Our preliminary evaluation indicated that textile clothes are likely major source of the airborne
microplastics. Modeling estimated that approximately 120.7 kg of SAMPs are annually transported through
Shanghai air. Moreover, an estimation of the ecological risk from SAMPs indicated that a minor ecological conse-
quence was present, necessitating further evaluation of SAMPs pollution. In addition, modeling estimated that
approximately 21 particles of microplastics are inhaled daily by people in Shanghai from outdoor environments.
Given the prevalence of airborne microfibers, it is critically urgent to reevaluate procedures for sampling,
transporting, and processing microplastic field samples. Future investigations should seek to develop more rigor-
ous and conclusive methods to evaluate these types of samples.
© 2019 Published by Elsevier B.V.
⁎ Corresponding author.
E-mail address: daojili@sklec.ecnu.edu.cn (D. Li).
https://doi.org/10.1016/j.scitotenv.2019.04.110
0048-9697/© 2019 Published by Elsevier B.V.
K. Liu et al. / Science of the Total Environment 675 (2019) 462–471 463
Fig. 1. Geographic visualization of sampling sites. a: Sampling stations (LK, YN, PJ, and NH); b: Photograph of LK station; c: Vertical distribution of sampling sites at the LK station (LK-1, LK-
2, and LK-3)-.
about 40–50 m downwind when sampling and after the instrumenta- (along its longest dimension) of microplastics were measured using
tion were initiated. the Image J software program (version 1.51j8) after importing high res-
olution photographs. Principal Component Analysis was performed to
2.4. Ecological risk assessment model explore the relationship between the SAMPs abundance and weather
variables of each during sampling period. The linear method from the
There is no current systematic and standardized model for assessing unconstrained model was chosen for evaluating the potential correla-
potential ecological risk that is completely suitable for microplastic pol- tion. Relative distance of stations in the bi-plot indicates the similarity
lution. Consequently, we developed a preliminary assessment method of samples composition.
in an attempt to better understand the potential ecological risks from
microplastics. The assessment of potential ecological risks (Hakanson, 3. Results and discussion
1980) has recently been applied towards pollution in sediments or
water column, and also to aerosol contamination. A modified version 3.1. Distribution of atmospheric microplastics
of the assessment model for potential ecological risks was calculated
as follows: Microplastics were detected in all but one sample analyzed here, in-
dicating a ubiquitous prevalence of SAMPs in atmospheric environ-
X
n
ments of Shanghai. SAMP abundances ranged from 0 to 4.18 n/m3,
RI ¼ Ei ð1Þ
i¼1
with a mean concentration of 1.42 ± 1.42 n/m3 (mean ± standard de-
viation) (Fig. 2). Compared to air sampled in Paris (Dris et al., 2017)
Ci exhibiting a median SAMPs level of 0.9 n/m3, a similar, but slightly
Ei ¼ T i ð2Þ
C0 higher contamination level (0.93 n/m3) was observed in Shanghai.
The concentrations of SAMPs are likely related to anthropogenic activi-
where RI and Ei correspond to the potential ecological risk and potential ties, population densities, and industrialization levels. Previous studies
ecological hazardous single indices, respectively. Ti, which was the have observed that domestic washing of clothes could produce consid-
heavy metal toxicity coefficient in the original model, was replaced by erable microplastic contamination (Browne et al., 2010; De Falco et al.,
the chemical toxicity coefficient for polymers, as described by Lithner 2018). Shanghai has a population of 24.18 million people that is nearly
et al. (2011). The ratio of Ci and C0 corresponds to the quotient of ob- twice that of Paris, which could lead to the generation of more domestic
served AMP polymer concentrations versus those of the background. microplastics. However, urban hygiene is carefully considered in Shang-
An ideal C0 value would be that from an air sample for total suspended hai. In particular, a number of air cleaning activities are conducted in
particulates prior to the rapid development of the synthetic fiber econ- Shanghai under the supervision of the Shanghai Municipal Environ-
omy. However, due to the lack of such data, the outdoor SAMPs abun- mental Protection Bureau (Shanghai Municipal Environmental
dance (0.9 n/m3) in Paris was chosen as the background value (Dris
et al., 2017). It is important to note that the exact data values were Table 1
not the focus of this study, but were rather used only to provide prelim- Pollution criteria of potential ecological risk by microplastics.
inary discussion for further assessment. The criteria levels for the poten-
Ecological risk RIa Ecological risk assessment Eib
tial ecological risk index are shown in Table 1.
assessment by single factor
Fig. 2. Horizontal (a) and vertical distribution (b) of suspended atmospheric microplastic abundances in Shanghai. In Fig. 2-a, distance away from the coastline of each station was
measured by the projection on the line connected LK and NH station.
Protection Bureau, 2018) and in accordance with the “Notice on further those of Zhao et al., 2015, which observed similar SAMP patterns in es-
establishment and re-inspection of the dust pollution control area”. For tuary environments. Specifically, microplastics were heterogeneously
example, daily street cleaning activities are conducted including dust distributed in the surface waters of the Jiaojiang, Oujiang, and Minjiang
sweeping and washing with water. These activities could possibly pro- estuaries. Moreover, microplastics exhibited high standard variations of
mote the settlement and reduction certain amount of contaminant 10.6%–119.8% and 12.1%–88.6% in the Jiaojiang and Minjiang estuaries,
SAMPs. respectively. In Fig. 3, approximated positive correlation is found
SAMPs abundances varied considerably among sampling sites (coef- when the angle between loading arrows of the environmental variables
ficients of variation: 33%–123%) (Fig. 2). These results are consistent is acute and negative when it is obtuse. Wind direction also appeared to
with those obtained from sediments and surface waters (Law and strongly correlate to the distributions of SAMPs in estuaries (Pearson's
Thompson, 2014), wherein the low density and buoyant characteristics correlation, R = 0.78, P = 0.01). Microplastics are easily distributed by
of microplastics likely contribute to their presence in those environ- winds, due to their low densities and small sizes. Other analyses have
ments. The highest abundance was observed at the YN station (mean: similarly documented that the spatial distribution of microplastics can
4.18 n/m3; Fig. 2-a). The smallest concentration (0 n/m3) was observed be significantly influenced by winds and greater abundances are ob-
near the sea side of Shanghai, which is potentially due to the dilution of served at downwind sites (Browne et al., 2010). In addition, relatively
SAMPs via ocean air and few human activities. However, there were high humidity levels contribute to the deposition of dust and SAMPs.
some cotton fiber identified on the filter and it was excluded to count. Here, a negative relationship was observed between relative humidity
The likely highest contributor to the horizontal distribution of SAMPs and the density of SAMPs (Pearson's correlation, R = -0.84, P = 0.03).
observed here is the degree of influence from anthropogenic activities. Intriguingly, significant linear correlations were not observed between
SAMPs abundances tended to decrease horizontally as distance to the SAMP abundances and the average population density (Pearson's corre-
coastline decreased (Fig. 1-a). The highest concentrations were ob- lation, R = 0.66, P = 0.44), road dust particulate (Pearson's correlation,
served at 1.7 m above the ground, with decreasing concentrations R = 0.16, P = 0.95), or PM 2.5 (Pearson's correlation, R = 0.77, P =
with increasing altitude. SAMPs were even observed 80 m above the 0.29). These results could possibly be attributed to the complex land-
ground (Fig. 1-b). However, no significant differences in concentrations scape of the Shanghai study area and the density of buildings.
were observed among samples from different altitudes (Kruskal-Wallis
test, p = 0.875 N 0.05), which could possibly result from admixture by 3.2. Morphological characteristics of observed microplastics
wind. The highest sampling station was still within the troposphere,
where the mixing effects of airflow convection are obvious. Thus, Typical microplastics observed here are shown in Fig. 4. Fibrous
these processes could lead to the homogenous vertical distribution of microplastics including fiber and fiber fragments were primarily ob-
atmospheric microplastics. Another potential source of SAMPs could served, which is consistent with observations from the Huangpu river
be the incomplete incineration of garbage in the study area. In addition, (Peng et al., 2018) and the Tehran metropolis (Dehghani et al., 2017).
SAMPs particles could be possibly attributed to the incomplete combus- Foam and film microplastics were not observed, which is similar to
tion of large plastic debris via chimneys. other studies (Cai et al., 2017). Surprisingly, fragments and granules
Principle component analysis (PCA) was used to determine the rela- were also observed in our study. As indicated above, fibrous
tionships between SAMPs abundances and environmental factors at the microplastics comprised 67% of the total particles, followed by frag-
sampling sites (Fig. 3). 84% of the total data variance could be explained ments and granules comprising 30% and 3%, respectively.
by factors 1 and 2 that explained 58% and 26% of all variance, respec- Fewer fragments and granules were observed 80 m above the
tively. Factor 1 contains loadings of the environmental variables dew ground, and the size distribution of SAMPs varied with altitude (Fig. 5-
point, psychro wet bulb temperature and heat stress index (0.34, 0.34 b). Microplastics observed here ranged in size from 23.07 to 9555 μm,
and 0.34, respectively). Factor 2 presents variables of relative humidity with a mean of 582.2 μm (Fig. 5-b). Microplastics smaller than 1 mm
(0.50), barometric pressure (0.33) and wind speed (0.23). Increasing comprised 87% of all synthetic items observed. The largest sized parti-
distance between sites was reflected in highly different SAMPs charac- cles were observed at 1.7 m above the ground, where overall sizes
teristics among all samples, with the exception of samples LK-2 and ranged from 23.07 to 9955 μm (average of 597.5 μm). Sizes ranged at
LK-3. These results reflect the heterogeneous distribution of SAMPs in the middle altitude (33 m above ground) from 25.07 to 504.6 μm with
the Shanghai study area. Further, these results are consistent with an average of 176.2 μm. At the highest altitude sampling point, particle
466 K. Liu et al. / Science of the Total Environment 675 (2019) 462–471
Fig. 3. Relationship between SAMPs abundances and environmental parameters from sampling sites. Circles and loading arrows in the biplot represent sampling stations and
environmental variables projection.
sizes ranged from 47.70 to 2230 μm with an average of 830 μm. The microplastics, with 25% and 28% of the total SAMPs, respectively. Al-
microplastics were variously colored including black, blue, red, trans- though the microfibers appeared similar in shape, we surprisingly
parent, brown, green, yellow, and grey particles (Fig. 4-c). Blue and found that the shape of these particles differed at the transversal sur-
black particles comprised the majority of the SAMPs, with 37% and face. A total of 29% of the microfibers were round and about 14–19 μm
33% of the total, respectively, and these colors were observed at every in size, while others were flat and exhibited sizes of 10–37 μm along
sampling site. Blue and black microfibers comprised most of the the longest dimension.
Fig. 4. Photographs of typically observed microplastics. a-c: fibers; d-e: fragments; f: a granule.
K. Liu et al. / Science of the Total Environment 675 (2019) 462–471 467
Fig. 5. Morphological and chemical composition of observed suspended atmospheric microplastics in Shanghai. a: Shape; b: Size; c: Color; d: Polymer; ground, aerial, and upper altitude
sampling heights (1.7, 33 m, and 80 m, respectively). PET: polyethylene terephthalate, PE: polyethylene, PES: polyester, PAN: polyacrylonitrile, PAA: poly(N-methyl acrylamide), RY:
rayon, EVA: ethylene vinyl acetate, EP: epoxy resin; ALK: alkyd resin.
3.3. Chemical composition of microplastics the source of microplastics primarily deriving from urban wastewater
discharge. In particular, partial similarity in microplastic polymer com-
Spectrum analysis indicated that the SAMPs were composed of poly- position between SAMPs and microplastics in sediment and water col-
ethylene terephthalate (PET), polyethylene (PE), polyester (PES), poly- umns strongly implied the presence of an intimate connection
acrylonitrile (PAN), poly(N-methyl acrylamide) (PAA), rayon (RY), between the two. Unlike SAMP deposition in Dongguan (Cai et al.,
ethylene vinyl acetate (EVA), epoxy resin (EP) and alkyd resin (ALK). 2017), PP and PS representing film and foam particles, respectively,
PES and RY were observed in air samples (Fig. 6), which is consistent were not observed here, which could possibly be related to the density
with an investigation of a freshwater river of Shanghai (Peng et al., and physical features of microplastics. PET, PE, and PES comprised
2018), wherein the SAMPs in the waters were likely derived from atmo- nearly half (49%) of the SAMPs observed here, followed by PAN and
spheric deposition and wind. Nevertheless, previous research has impli- PAA with 12% and 9%, respectively. In contrast, RY, EVA, EP, and ALK
cated the presence of hydraulic-driven patterns of microplastics, with polymers were relatively infrequently observed and accounted for 15%
468 K. Liu et al. / Science of the Total Environment 675 (2019) 462–471
of the total SAMPs. Fiber shaped SAMPs were identified as PET, PAN, 3.4. Risk assessment
PAA, RY, and PES, comprising 50%, 17%, 17%, and 2% of the totals, respec-
tively. An additional 46% of the suspected microplastics were identified Microplastics can be ingested by many organisms because of their
as cellulose (cotton and silk materials) and were thus not included in small sizes, and numerous investigations have demonstrated the bio-
the data presented here. However, these airborne microfibers still availability of microplastics in environments. For example,
pose a threat to human health, if inhaled. Consequently, these materials microplastics have been found in zooplankton (Desforges et al., 2015;
are worth reconsidering and evaluating in future studies. Sun et al., 2018), the digestive systems of bivalves (Li et al., 2018) and
A relatively high percentage of synthetic SAMPs are likely closely fish (Lusher et al., 2013), and even in mammals (Eriksson and Burton,
connected to the increasing production of synthetic fiber. A total of 2003; Zhao et al., 2016). Consequently, increasing environmental accu-
65.2 million metric tons of synthetic fiber was produced globally in mulation of microplastics poses significant threats to all organisms, in-
2014. Of this total, Asian production reached 52.5 million metric tons, cluding humans. Indeed, up to 1.1 × 104 pieces of microplastics are
rendering this area the highest producer of synthetic fibers. In addition, estimated to be eaten by European shellfish consumers every year
the production of cellulose and polyester reached 5.0 and 49.2 million (Van Cauwenberghe and Janssen, 2014).
metric tons between 1994 and 2014, respectively (American fiber man- In the present study, we preliminarily estimated the total level of
ufacturers association, 2014). Similarly, Asian production comprised the SAMPs in Shanghai and evaluated the potential health risk to urban res-
substantial majority of polyester production, totaling 82% of global pro- idents in the city. The total weight of atmospheric suspended
duction. Textiles made with synthetic fibers generally feature high resil- microplastics in Shanghai was calculated based on the following equa-
ience and resistance to abrasion. In addition, these materials exhibit tions:
finer touches and feels compared to natural fibers like cotton and silk.
Consequently, the manufacturers of textiles and furniture incorporate Total weight of SAMPs ¼ W g þ W m þ W h ð3Þ
these synthetic fibers into their products. Indeed, some blankets and
clothes available on the market are completely made of just one or X
80
two types of synthetic fibers (PET and PA). Likewise, PAN fibers are W α ¼ A ρβ S γ h ð4Þ
manmade wools that are characterized as soft feels, being easy to dye, i¼1:7
Table 2
Total weight of SAMPs identified in Shanghai.
Height Air volume (m3) Polymer type Density (g/cm3)a Volume of single SAMP (cm3) Total weight (kg)
Ground 8.76 × 109 CE 1.35 2.15 × 10−7 (Fiber); 1.25 × 10−8 (Fragment) 6.46
PET 1.45
PE 0.96
PES 1.38
PAN 1.18
RY 1.5
EVA 0.98
Aerial 1.61 × 1011 CE 1.35 1.57 × 10−7 (Fiber); 1.67 × 10−8 (Fragment) 1.45
PET 1.45
PAN 1.18
Upper 2.42 × 1011 CE 1.35 2.4 × 10−7 (Fiber); 2.15
PE 0.96 5.70 × 10−8 (Fragment)
PAA 1.3
EP 0.98
a
International Plastics Handbook (Osswald, 2006); PET: polyethylene terephthalate, PE: polyethylene, PES: polyester, PAN: polyacrylonitrile, PAA: poly(N-methyl acrylamide), RY:
rayon, EVA: ethylene vinyl acetate, EP: epoxy resin; ALK: alkyd resin.
where Wg, Wm, and Wh refer to the total weight of SAMPs in the air col- The prevalence of SAMPs could have possible negative influences on
umn at a specific altitude (1.7 m, 33 m, and 80 m above the ground, re- human health. Previous studies have indicated that workers in a textile
spectively), A and ρβ represent the average abundance of SAMPs and the factory suffered from dyspnea and were diagnosed with airway and in-
density of SAMPs (g/cm3) for different polymer types, respectively. Sγ terstitial inflammatory responses that were caused by plastic fibers and
(m2) and h (m) correspond to the area of the sample areas and the particles (Prata, 2018). Assuming that 10–20 m3 of air is consumed per
height of the air column, respectively. Sγ, S shanghai, and S land occupation day by an adult (Exposure factors handbook, 2011), our modeling esti-
refer to the area without residence occupation, the total area of Shang- mated that about 21 pieces of microplastics are inhaled daily by Shang-
hai, and the area occupied by buildings, with each given in m2 (Shanghai hai residents near the ground (using an average air volume of 15 m3).
Statistical Yearbook, 2017). Increasing production of synthetic materials would likely lead to expo-
Due to the high percentage (97%) of microplastics exhibiting fiber nential increases in SAMPs in the future and increased threats to human
and fragment types, the total level of SAMPs could be inferred to be health. However, it should also be noted that the relatively low abun-
the sum of SAMPs in Shanghai. The average mass of SAMPs at a specific dances of SAMPs in the environment are not enough to cause severe in-
height was also calculated. To calculate volumes from fibers and frag- flammatory responses. Moreover, fewer SAMPs could actually reach
ments, fibrous microplastics were regarded as cylinders, while frag- lungs after filtration and remediation by respiratory systems. Neverthe-
ments were considered as rectangles with the longest and shortest less, the potential risk from SAMPs necessitates additional inclusive and
sides as the sides of the rectangle and using an average thickness of 3 detailed scientific methods for their evaluation. In additional studies,
μm. The weight of SAMPs in Shanghai was thusly estimated to be microplastic sizes should also be considered when assessing risks, as
10.06 kg (Table 2). A considerable level of SAMPs was found near the many reports have indicated that small microplastics are more easily
ground, at almost three times that of the middle and higher altitudes. ingested by organisms (Jeong et al., 2016).
This disparity in abundances is likely related to denser anthropogenic
activities near the ground. 4. Conclusions
In addition to the transfer of microplastics through food chains,
microplastics can be translocated to humans through the air. Owing to The prevalence of airborne microplastics in a mega city (Shanghai)
their small size and buoyant characteristics, these SAMPs could then was evaluated in this study and the spatial distribution of SAMPs within
possibly be inhaled by humans, thereby endangering human health. Shanghai was investigated. Higher levels of SAMPs pollution were ob-
Previous studies have indicated that workers in a synthetic textile fac- served at the YN station and near the ground when compared to levels
tory are more likely to contract pneumonia or lesions due to fiber inha- at higher altitudes. The buoyant characteristics of SAMPs and their
lation (Prata, 2018). In addition, these SAMPs could also potentially transport by wind could be one critical source for marine microplastic
transport microorganisms (Jiang et al., 2018), representing an addi- pollution. A detailed comparison of SAMPs observed here, as compared
tional danger to exposed organisms once it enters the host respiratory to other studies, is provided in Table 4. Several commonalties in mor-
system. Recent studies have incorporated several methods to inclu- phological features and chemical compositions were observed among
sively evaluate the ecological risk from microplastics (Peng et al., these studies, suggesting that marine microplastics may ultimately de-
2018; Xu et al., 2018). However, most assessment models have been rive from terrestrial environments via atmospheric deposition.
based on pollutants in sediments or water columns, and are thus not ap-
propriate to evaluate the risk of atmospheric microplastics. A preliminary Table 3
risk assessment of SAMPs was conducted here that was based on the po- Potential ecological risk evaluation for SAMPs in the study area.
tential ecological risk index and incorporated abundances and polymer Sample Municipal Polymer type RIa Risk
types. Regional ecological evaluation via the potential ecological risk sites district level
model indicated that only a minor threat was expected for all sampling LK-1 Putuo CE, PET, RY 1.29 Minor
areas (Table 3). The RI ranged from 0.36 to 4.03 overall, while a higher LK-2 CE, PET, PAN 1.93 Minor
risk index was observed at the YN station, and the lowest ecological risk LK-3 CE, PE, PAA, EP 1.82 Minor
index was observed at the NH station closer to the sea, where anthropo- YN Changning CE, PET, PE, PES, PAN, RY 6.54 Minor
PJ Minhang CE, PET, PE, PES, PAN, EVA, ALK 2.29 Minor
genic activities were scarce. Less ecological risk was observed at the NH Pudong new CE, PET, PAN 0.23 Minor
higher altitudes relative to the near ground samples. However, it should area
be noted that the ecological risk index may represent an underestimate a
Potential ecological hazardous single indices; PET: polyethylene terephthalate, PE:
due to the lack of polymer toxicity coefficients for cellulose, rayon, and polyethylene, PES: polyester, PAN: polyacrylonitrile, PAA: poly(N-methyl acrylamide), RY:
alkyd resin, and their consequent exclusion from these analyses. rayon, EVA: ethylene vinyl acetate, EP: epoxy resin; ALK: alkyd resin.
470 K. Liu et al. / Science of the Total Environment 675 (2019) 462–471
Table 4
Characteristics of observed microplastic in the similar and adjacent area studies.
Paris (urban) Atmosphere Fiber 50–3250 N/A RY, PA, PE; PP Dris et al.,
2017
Paris Atmosphere Fiber 50–600 N/A RY, PET, PA Dris et al.,
2016
Dongguan Atmosphere Fiber, foam, film, – Blue, black, red yellow, pink, white RY, PE, PP, PS Cai et al.,
fragment 2017
Yantai Atmosphere Fiber, foam, film, 50–1000 Black, red, white, transparent PET, PE, PVC, PS Zhou et al.,
fragment 2017
Shanghai Atmosphere Fiber, fragment, 23.07–9554.88 Blue, black, red, transparent, brown, green, PET, PE, PES, PAN, PAA, RY, EVA, Present study
granule yellow, grey EP, ALK
Yangtze Sediment Fiber, fragment, pellet 46.8–4968.7 Transparent, blue, black, yellow, red, white RY, PES, AC, PET, PE-PP, PS Peng et al.,
estuary 2017
Yangtze Water Fiber, fragment, film 70–5000 Blue, black, transparent, pink, grey PE, PP, PVC, ABS, PS, PC, ASA, PUR, Xu et al., 2018
estuary SAN
PET: polyethylene terephthalate, PE: polyethylene, PES: polyester, PAN: polyacrylonitrile, PAA: poly(N-methyl acrylamide), RY: rayon, EVA: ethylene vinyl acetate, EP: epoxy resin; ALK:
alkyd resin.
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Microplastic size-dependent toxicity, oxidative stress induction, and p-JNK and p-
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