1 s2.0 S0048969722019647 Main
1 s2.0 S0048969722019647 Main
1 s2.0 S0048969722019647 Main
H I G H L I G H T S G R A P H I C A L A B S T R A C T
A R T I C L E I N F O A B S T R A C T
Editor: Philip K. Hopke Electronic waste (WEEE; from TV screens to electric toothbrushes) is one of the fastest growing waste streams in the
world. Prior to recycling, e-waste components (metals, wood, glass, etc.) are processed by shredding, grinding and
Keywords: chainsaw cutting. These activities generate fine and ultrafine particle emissions, containing metals as well as organics
Ultrafine particles (e.g., flame retardants), which have high potential for human health impacts as well as for environmental release. In
E-waste
this work, release of fine and ultrafine particles, and their exposure impacts, was assessed in an e-waste recycling fa-
Electronic waste
WEEE
cility under real-world operating conditions. Parameters monitored were black carbon, particle mass concentrations,
Human health ultrafine particles, and aerosol morphology and chemical composition. Potential health impacts were assessed in
Nanoparticles terms of cytotoxicity (cell viability) and oxidative stress (ROS) on <2 μm particles collected in liquid suspension. En-
Risk assessment vironmental release of WEEE aerosols was evidenced by the higher particle concentrations monitored outside the fa-
Toxicity cility when compared to the urban background (43 vs.11 μgPM2.5/m3, respectively, or 2.4 vs. 0.2 μgCa/m3). Inside
Heavy metals the facility, concentrations were higher in the top than on the ground floor (PM2.5 = 147 vs. 78 μg/m3, N = 15.4
Flame retardants ∗ 104 vs. 8.7 ∗ 104/cm3, BC = 12.4 vs. 7.2 μg/m3). Ventilation was a key driver of human exposure, in combination
Plasticisers
with particle emissions. Key chemical tracers were Ca (from plastic fillers) and Fe (from wiring and other metal com-
ponents). Y, Zr, Cd, Pb, P and Bi were markers of cathode TV recycling, and Li and Cr of grinding activities. While aero-
sols did not evidence cytotoxic effects, ROS generation was detected in 4 out of the 12 samples collected, associated to
the ultrafine fraction. We conclude on the need for studies on aerosol emissions from WEEE facilities, especially in
Europe, due to their demonstrable environmental and human health impacts and the rapidly growing generation of
this type of waste.
⁎ Corresponding author at: Institute of Environmental Assessment and Water Research (IDAEA-CSIC), C/ Jordi Girona 18, 08034 Barcelona, Spain.
E-mail address: [email protected] (M. López).
http://dx.doi.org/10.1016/j.scitotenv.2022.154871
Received 2 December 2021; Received in revised form 1 March 2022; Accepted 23 March 2022
Available online 29 March 2022
M. López et al. Science of the Total Environment 833 (2022) 154871
2.1. Particle emission and exposure scenarios - Miniature diffusion size classifier DiscMini (TESTO AG), reporting par-
ticle number concentrations and mean particle diameter between 10
As stated above, the purpose of this work was to generate data on dust and 700 nm, with a 1 min time resolution.
emissions and potential impacts on human exposure. It was not designed - Light-scattering laser photometer DustTrak TM DRX (TSI Model 8533),
as an occupational health assessment, and as a result it does not follow for total and size-segregated particle mass concentrations in the range
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M. López et al. Science of the Total Environment 833 (2022) 154871
250–3200 nm with 1 min time resolution. in a humidified incubator, and, before performing the assays, cells were
- Optical particle size (OPS, TSI Model 3330) for total and size-segregated allowed to reach 80% confluence in 75 cm2 culture flasks (Corning, NY,
particle mass concentrations in the range 0.3–10 μm across 16 channels USA) containing culture medium DMEM (Sigma, Steinheim, Germany) sup-
with 1 min time resolution. plemented with 10% fetal bovine serum (Sigma, Steinheim, Germany), 50
- MicroAeth® AE51 Black Carbon aerosol monitor, monitoring black car- U/mL of penicillin and 50 μg/mL streptomycin (Gibco, Paisley, Scotland,
bon (BC) concentrations with a 1 min time resolution. UK). Two different assays were performed on the aerosol samples collected:
- Cell viability assay: 5 ∗ 104 cells were plated in 96-well plates and incu-
2.3. Sample collection bated 24 h before exposure to 100 μL of sampling medium or fresh me-
dium (control cells) for 24 h. Alamar Blue (AB, Thermo Scientific™) and
Aerosol samples were collected on different substrates for the following 5-carboxyfluorescein diacetate acetoxymethyl ester (CFDA-
offline determinations: AMMolecular Probes, Invitrogen, Spain) where the dyes used to esti-
- Particle chemical composition: during the work shifts in each floor, mate metabolic activity and membrane impairment, respectively. The
PM10 (particle size matter of 10 μm) and PM2.5 (particle size matter fluorescence of dyes was read at the excitation/emission pairs of 530/
of 2.5 μm) samples were collected on quartz microfiber filters (37 mm 590 (AB) and 485/530 nm (CFDA-AM), in a Tecan Infinite M Plex
PTFE filters) using Personal Environmental Impactors (PEM, SKC®). plate reader (Männedorf, Switzerland). The percentage of viable cells
In addition, three particle size fractions (>2.5 μm, 2.5–0.25 μm, <0.25 was calculated by dividing the relative fluorescent units (RFUs) of ex-
μm) were collected, the coarser stages on polycarbonate 25 mm filters posed cells by RFUs of control cells, multiplied by 100.
and the last stage on Teflon 37 mm PTFE filters, using Personal Cascade - ROS generation was estimated by the oxidation 2′,7′-dichlorofluorescin
Impactors (PCIS, SKC®) connected to portable SKC Leland pumps (9 L/ (H2DCF-DA) (Sigma, Steinheim, Germany), which is deacetylated by
min). The inorganic particle chemical composition was determined by membrane esterases and then oxidized by intracellular ROS, becoming
ICP-MS and ICP-AES after an acid digestion procedure of the samples fluorescent (LeBel et al., 1992). Briefly, 5 ∗ 104 cells were seeded in 96-
(Querol et al., 2001). Halogenated flame retardants (HFRs) and organo- well plates and allowed to attach for 24 h. The culture medium was
phosphate esters (OPEs) were also analysed, reported in Balasch et al., replaced by 20 μM H2DCF-DA diluted in DPBS (1:10) supplemented
2022 with 10 mM glucose (DPBS-Glu) and the plate incubated for 30 min at
- Particle toxicity: twelve 30-minute samples were collected using an SKC 37 °C, 5% CO2. Cells were washed with PBS and exposed to sampling
BioSampler® connected to a sonic-flow BioLite+ pump (12.5 L/min) medium, fresh medium (control) or 5 μM 3-morpholinosydnonimine
(López et al., 2021). Particles <2 μm were collected in liquid suspension (SIN-1; positive control). The emitted fluorescence of DCF was
in Dulbecco's Modified Eagle's Medium (DMEM; Sigma, Steinheim, measured at ex/em pairs of 485/528 nm, after 15, 30, 60 and
Germany). The suspensions were stored at 2 °C after sample collection. 120 min of exposure to sampling medium. Generation of ROS was
Sampling time must be short (30 min) to minimise evaporation and expressed as fold induction (RFUs of exposed cells divided by RFUs in
avoid potential fungal growth in the medium. This, however, limits control cells).
the comparability between the toxicity results and the mean chemical
composition (sampled over 6 or 8 h shifts), as will be discussed below. 3. Results and discussion
- Particle morphology: particles were collected on Transmission Electron
Microscopy (TEM) grids (Quantifolil® Au grids with 1 μm diameter 3.1. Exposure metrics and concentrations
holes - 4 μm separation of 200 mesh) placed in sampling cassettes
(SKC INC., USA, inlet diameter 1/8 in. filter diameter 25 mm) following The results on particle concentrations from the online instruments are
the sampling setup described by Tsai et al., 2008 and Ribalta et al., summarised in Table 1 and shown in Fig. 1 as density plots. As discussed
2019. The cassettes were connected to an SKC Leland pump (3 L/ in the Materials and methods section, measurements were carried out
min). Samples were collected during the afternoon shift (14:00 h to under real-world operating conditions, representative of the facility's
22:00 h in the top floor and 14:00 to 20:00 h on the ground floor). usual activities. The concentrations of all of the parameters were higher
The gravimetric analysis was performed according to the European di- in the top floor (Table 1), probably resulting from the lower ventilation in
rective EN1234-1. It included pre-sampling and post-sampling weighing this area of the plant. As described above, there were no open windows
of each filter (including blanks). The pre-weighing and post-weighing connecting the top floor with outdoor air. Furthermore, the meteorological
were carried out following the same procedure: conditioning temperature conditions during the second campaign favoured particle scavenging out-
20 °C and relative humidity 50%. Each sample was weighed three times doors and therefore reduced potential infiltration of ambient aerosols
(24-hour interval in between) and the average value was recorded. The fil- (Chen et al., 2020), as it rained during 2 out of 4 days of the second
ters were weighed using a microbalance (Mettler-Toledo, model: XP105 week. Mean daily fine particle concentrations (PM2.5) were relatively
with electrostatic charge detection, Switzerland). higher in the top floor (147 μg/m3) than on the ground floor worker area
(78 μg/m3), while the background concentrations were relatively similar
2.4. Cell viability and generation of reactive oxygen species (37–43 μg/m3). The indoor/outdoor (I/O) ratio for PM2.5 was higher for
the top (3.4) than for the ground floor (2.1), which would indicate the influ-
The oxidative potential (OP) of fine particles describes their ability to ence of higher PM2.5 emissions and/or lower ventilation in the top floor. It
generate oxidative and inflammatory effects in bronchial cells is not possible with the available data to discern which factor was dominant
(Daellenbach et al., 2020; Imai et al., 2008; Kelly, 2003; Pietrogrande in the top floor, whether the higher emission or the lower ventilation. Con-
et al., 2021; Sisani et al., 2022). The oxidative stress generated by exposure versely, for the rest of the parameters monitored (PM10, N, BC), I/O ratios
to aerosols can be estimated using acellular and cellular methods (Sisani were very similar for both floors (2.6–2.7, 3.9–4.0 and 4.4–4.9, respec-
et al., 2022). typical acellular methods are based on dithiothreitol (DTT) tively). On the ground floor, where natural ventilation was significant
consumption or antioxidant depletion assays (using ascorbic acid, AA, or given that the gates were fully open at all times, the high I/O ratios (ranging
glutathione, GSH), while cellular tests are considered more representative between 2.1 for PM2.5 to 4.4 for BC) confirm the impact of the WEEE
of the actual processes and interactions taking place during cell exposure recycling activities on air pollutant concentrations and, subsequently, on
to aerosols. In cellular tests, exposure may be simulated through submerged personal exposure. Thus, natural ventilation alone does not seem sufficient
cell cultures or by air-liquid interaction (ALI) (Bessa et al., 2020a; Bessa to maintain low levels of exposure to pollutants in the facility.
et al., 2020b). In this work, the human alveolar cell line A549 was used The density plots in Fig. 1 were used to understand the concentrations
to assess the toxicity of the samples. It was maintained at 37 °C, 5% CO2, as well as the potential variety of emission sources impacting particle
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M. López et al. Science of the Total Environment 833 (2022) 154871
Table 1
Maximum, minimum, mean and standard deviation (SD) of the different parameters (black carbon (BC), number concentration (N), diameter (dP), mass concentration
(PM2.5 and PM10)) sampled in both campaign (October and November) in both scenarios (worker areas: top and ground floor) and back ground (BG).
BC (μg/m3) N(/cm3) Dp (nm) PM2.5 (μg/m3) PM10 (μg/m3)
Max Min Mean SD Max Min Mean SD Max Min Mean SD Max Min Mean SD Max Min Mean SD
October 2020 Top floor 35,105 2911 12,357 4060 586,084 34,958 153,652 73,442 51 25 37 6 1769 49 147 116 4804 90 357 317
BG 29,165 13 2518 2664 622,254 2455 39,197 62,554 89 10 43 22 290 17 43 28 1770 703 131 139
November Ground 24,268 1903 7156 4105 316,202 20,496 86,547 46,124 48 20 32 5 901 33 78 83 2280 63 172 210
2020 floor
BG 6981 37 1623 1320 216,426 3620 21,757 27,926 76 15 46 14 182 22 37 22 872 18 65 100
concentrations. BC concentrations, for example, were higher on average on may suggest the impact of a single, relatively uniform emission source.
the top than on the ground floor (12.4 vs. 7.2 μg/m3), but the density pro- The most plausible interpretation is that the main source of BC was diesel
files were highly similar on both floors with unimodal distribution, which engines, both from the forklifts operating on the ground floor and from
Fig. 1. Density plots of the different worker areas (Top floor and ground floor) of both campaigns (October and November), BC: Black Carbon (μg/m3); N: Number
concentration (/cm3); Dp: Diameter (nm); PM2.5 (μg/m3); PM10 (μg/m3).
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M. López et al. Science of the Total Environment 833 (2022) 154871
the trucks delivering the WEEE, which due to the effect of natural thermal (shredding, milling), and burning (possibly, uncontrolled) to recover valu-
convection and air exchange between both floors, caused them to concen- able materials. Most of the studies have been performed in China, followed
trate on the top floor. Aside from this, a certain influence of monitoring ar- by Ghana and India, with studies in European facilities being rather scarce
tefacts caused by iron interference (Derimian et al., 2008) could not be (Buiarelli et al., 2019; Julander et al., 2014; Papaoikonomou et al., 2018),
discarded. as discussed above.
Particle number (N) concentrations, on the other hand, showed differ- PM mass concentrations in different size ranges are the most frequently
ent density profiles on both floors and the highest differences in concentra- reported parameter, with TSP (total suspended particles) ranging between
tions between floors. The top floor data showed higher concentrations on 124 and 5066 μg/m3, PM10 between 173 and 1674 μg/m3, and PM2.5 be-
average than the ground floor (15.4 ∗ 104/m3 vs. 8.7 ∗ 104/cm3), as was ob- tween 11 and 2774 μg/m3 (Table 2) worldwide. Concentrations reported in
served with BC, but with a wider distribution, which suggests a greater va- European facilities were, unexpectedly, at the middle/upper end of the
riety of sources. These were probably due to the emissions generated during range. This could be due to the fact that recycling activities in Asian and
mechanical cutting of the TV screen frames (metallic). On the ground floor, African countries are frequently performed in open spaces and with scarce
concentrations were lower and less variable (narrower density plot), sug- monitoring, under non-existent or very poor regulatory frameworks and
gesting a single source with relatively constant emissions (probably, trucks protocols. Conversely, European facilities are enclosed (indoors) and mon-
and diesel forklifts, as in the case of BC). In terms of particle diameter, mean itored under EU regulations. A similar pattern is observed for flame retar-
Dp was very similar on both floors (32–37 nm; characteristic of diesel soot dant levels, which are higher in Europe and other HICs compared to
particles; Tritscher et al., 2011), also with a mostly unimodal distribution, LMICs (Ding et al., 2018; Nguyen et al., 2019; Tao Wang et al., 2018). In
with only a small secondary peak in the top floor probably linked to the in- any case, concentrations are largely variable and dependent on the type
cidental formation of new particles (Salmatonidis et al., 2018; Viana et al., of activity, proximity to the source and ventilation conditions, with me-
2017), due to the emissions of volatile compounds from the mechanical cut- chanical activities mainly affecting coarse particles while fine particles
ting saw. are more influenced by combustion processes (Table 2). In our study,
Finally, PM10 and PM2.5 showed bimodal density distributions, sug- hourly PM2.5 concentrations recorded in the working area and during
gesting the influence from at least two different sources with different con- working hours were in the range 17–404 μg/m3, showing high variability,
centrations, or a single source with two different emission profiles. The and with a mean value (147 μg/m3) in the range of those more commonly
variety of activities taking place in the recycling plant supports this inter- reported in literature. To the authors' knowledge, little is known about the
pretation. behavior of quasi-ultrafine and ultrafine particles in these environments,
In order to understand the magnitude of the concentrations of the differ- with only one study in Italy reporting on PM0.1 mass concentrations,
ent metrics monitored in the exposure scenarios, the results were compared which ranged between 6.6 and 25.9 μg/m3 (Buiarelli et al., 2019). Another
in terms of PM2.5 and N with representative urban background (UBG) con- study reported particle number (N) concentrations in US, recording mean
centrations (monitored in Barcelona city, Palau Reial EU-reference station) concentrations of 25 ∗ 104/cm3, associated with shredding activities
(Fig. 2). The concentrations inside the plant (in the worker areas, WA) were (Ceballos et al., 2020). N concentrations in our study were slightly lower,
always higher than in the outdoor air at the WEEE recycling facility (back- with mean hourly concentrations during work shifts in the range 2.2 ∗
ground, BG). As expected, the concentrations in BG were, in turn, higher 104–15.4 ∗ 104/cm3 (Table 1) while reaching 5-min maximum concentra-
than in UBG due to the influence of fugitive emissions from the process tions recurrently >20 ∗ 104/cm3. As a result, it may be concluded that the
and emissions from the forklifts and the trucks offloading the WEEE. This concentrations recorded at the WEEE recycling facility under study are
confirmed that the different activities in this e-waste recycling plant, con- comparable, even if slightly lower, than those reported for other
sidered representative of EU standards, generated distinct particle emis- European studies in terms of particle mass (PM2.5, PM10) and number con-
sions with potential to impact ambient air quality at local scale as well as centrations.
human health. In terms of indoor air, particle concentrations monitored
(maximum 8-hour PM4 recorded = 1485.92 μg/m3) did not exceed current 3.2. Chemical fingerprint of WEEE emissions
limit values (3 mg/m3 as time-weighted average).
In addition, a literature review was carried out to identify studies The PM < 0.25, PM0.25–2.5 and PM > 2.5 samples collected on the top
reporting air quality assessments at WEEE recycling facilities, as a basis and ground floors were analysed in terms of major and trace inorganic spe-
for establishing a comparative scenario to analyses the results obtained in cies. For the sake of simplicity and comparability with concentrations at a
this study. Detailed information can be found in Table 2. The review ac- nearby urban environment, values reported in the main text will corre-
counts for studies published between 2006 and 2020 in peer-reviewed spond to the PM2.5 fraction. Organic and elemental carbon (OC and EC)
journals, based on research databases Scopus and ScienceDirect. The search were also determined on a limited number of samples (two 24 h-PM10 sam-
terms included “air quality”, “e-waste”, “PM” and “heavy metals”. Activi- ples on the top floor and two on the ground floor) due to the low availability
ties assessed mainly comprised dismantling, mechanical workshops of samples collected on quartz microfiber filters. In both floors, the key
Fig. 2. Number concentrations and PM2.5 box plots comparing the different measurement areas in both campaigns (October and November).
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M. López et al. Science of the Total Environment 833 (2022) 154871
Table 2
Literature review of other studies on WEEE recycling plants.
Study Country Activities Pollutant Concentration Comments regarding heavy metals
(Kim et al., 2015) US (1) A chain-shredder, (2) a hammermill, and PM2.5–10 174–612 μg/m3 Compared to coarse PM measurements from a
(3) a cathode tube disassembly line used solely PM0.1–2.5 49–596 μg/m3 regional near-roadway, Pb and Ni were
to disassemble and recover components from enriched 170 and 20 times, respectively
monitors and televisions
(Gangwar et al., 2019) India E-waste burning PM10 243.310 ± 22.729 μg/m3 Emission from open air burning resulted in
high exposure of Pb, Cr, Ni, Cu and Zn to the
residents of the area
(Zheng et al., 2016) China Open burning and other e-waste recycling PM2.5 11–160 μg/m3 Higher values of Pb and Cd compared to the
operations (not specified) reference site
(Bungadaeng et al., 2019) Thailand Open burning processes. Compiling and PM2.5–10 441 ± 496 μg/m3
sweeping PM2.5 2774 ± 4713 μg/m3
(Fang et al., 2013) China Mechanical workshops PM10 326.3–394.5 μg/m3 Pb and Cu were the most enriched metal in
PM2.5 252.6–290.8 μg/m3 the PM2.5 and PM10 samples, respectively
Ceballos et al., 2020 US Shredding N > 10 nm 250 #/cm3
PM2.5 171 μg/m3
Bi et al., 2010 China Printed Circuit Boards (PCB) recycling TSP 1129–1688 μg/m3 Cd, Pb, Zn, Cu, Sb and Ni mainly caused by
workshop the burning of PCBs. High OC (381.9–562.6)
and EC (26.3–42.4 μg/m3) concentrations
(Deng et al., 2006) China Open burning and other e-waste recycling TSP 124 ± 44.1 μg/m3 Cr and Zn were the most enriched metals in
operations (not specified) PM2.5 62.12 ± 20.5 μg/m3 TSP and PM2.5, followed by Cu, Pb, Mn and
As. All metals exhibited a predominant
occurrence in the fine particulate fraction
(Xue et al., 2012) China PCB recycling workshop TSP 282.6 μg/m3 TSP and PM10 enriched by Cr, Cu, Cd, Pb
PM10 202.0 μg/m3
(Kwarteng et al., 2020) Ghana Open burning and other e-waste recycling PM10 214 μg/m3
operations (not specified) PM2.5 88 μg/m3
Papaoikonomou et al., 2018 Greece Dismantling and temporary storage PM10 382.4 ± 104.8 μg/m3 As and Pb concentrations in the indoor
samples were 140 and 40 times, respectively,
higher than those measured in the ambient air
of nearby city. CRT (cathode ray tubes)
processing release Sr, Pb, Cd and As
Buiarelli et al., 2019 Italy Dismantling activities PM0.1 17.6 (6.6–25.9) μg/m3
PM0.1–2.5 477.7 (147.1–704.6) μg/m3
PM2.5 495.2 (153.7–730.5) μg/m3
PM10 1674.4 (599.6–3077.9) μg/m3
TSP 5066.8 (2309.7–9682.0) μg/m3
Ding et al., 2018 China Not specified (rural e-waste recycling area PM2.5 182 ± 62.0 μg/m3
covering an area of about 330 km2)
Nti et al., 2020 Ghana Collecting, dismantling and open air burning of PM2.5 61.18–70.69 μg/m3
electrical cables to recover copper PM10 173.49–214.43 μg/m3
Julander et al., 2014 Sweden Indoor work (i.e., tasks involving handling of V, Sb, In, Pb and Hg showed significant
goods, for example, sorting of incoming and out- correlations between air and blood/urine.
going goods, truck driving, cleaning, supervision Significantly higher levels of Cr, Co, Pb, In
of work), outdoor work (e.g., mainly inspection and Hg was found in recycling workers.
tasks and transportation of goods), and office Rare metals such as In and Sb must be
work (i.e., computer work with no time in the monitored in these settings.
production buildings)
Wang et al., 2009 China Dismantling and recovery processes Cd, Cu and Pb were likely found to be
originated from e-waste related activities
Kuntawee et al., 2020 Thailand Not specified House dust and airborne levels of Cr, Hg, Ni,
and Pb were higher in the homes and
environment of subjects involved in e-waste
activities
(Wittsiepe et al., 2017) Ghana Not specified Significantly high median concentrations of
Pb, Cd, Cr and Ni
(Ngoc Ha et al., 2009) India Dismantling, extraction of valuable metals Concentrations of Cr, Mn, Co, Cu, In, Sn, Sb,
Tl, Pb and Bi in air from the e-waste recycling
facility were relatively higher than in city
(Ceballos et al., 2017) US Electronic dismantling, automated CRT cutting, Overexposure to Pb and Cd
electronics shredding, batteries sorting
tracers of e-waste (Julander et al., 2014; Kuntawee et al., 2020; range in the top floor and 3–6.4 μg/m3 range in the ground floor) and Fe
Papaoikonomou et al., 2018) and industrial activities (e.g., diesel combus- (4.5–10.3 μg/m3 range in the top floor and 1.9–5.4 μg/m3 range in the
tion, dust re-suspension, (Gulia et al., 2019)) were detected. Tables 3 and ground floor). Ca is a known mineral filler of plastics (Thenepalli et al.,
4 show the mean concentrations of trace and major elements, respectively. 2015), indicating the contribution of this material to PMx in the whole facil-
The presence of key tracers was corroborated with TEM images (Fig. 3). ity. Another sign of the impact of plastics handling is probably the high
As observed for the online parameters described above, element con- daily OC concentrations recorded, in the range 28–84 μg/m3. Similarly,
centrations in the top floor were higher than in the ground floor (Tables 3 EC concentrations were relatively high (between 5 and 19 μg/m3), proba-
and 4 and Figs. 4 and 5). This was linked to the poor ventilation in the bly linked to the diesel-powered forklifts operating in the facility, as well
top floor and the more favourable weather conditions during the week as from the trucks delivering the waste at the gate of the facility. In spite
when sampling was carried out on the ground floor Ca (7.0–15.6 μg/m3 of expected sources of carbonaceous aerosols at the different sampling
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Table 3
Maximum and minimum levels in PM2.5 of trace elements (ng/m3) in both campaigns in the worker area (WA) and in the back ground (BG) and mean annual levels of trace
elements in Palau Reial cabin that corresponds the levels in PM2.5 of the urban back ground (UBG).
ppb Top floor (October 2020) Ground floor (November 2020) PM2.5 trace elements average
2020 in Palau Reial station
(ng/m3) WA BG WA BG
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M. López et al. Science of the Total Environment 833 (2022) 154871
Fig. 3. Particles collected on TEM grids in the top floor (top) and in the ground floor (bottom).
the ground floor. For selected tracer metals, estimated inhaled doses were also in line with the available information on material composition in dif-
17 and 4 ngTi/kg body weight, 0.3 and 0.1 ngCd/kg, 34.8 and 4.7 ngPb/ ferent types of electrical and electronic equipment (Ghimire and Ariya,
kg, and 0.4 and 0.03 ngBi/kg, on the top and ground floors respectively. 2020), with releases from cathode ray tubes as one of the best-
The high concentrations described here emphasize that the main con- characterized sources (Ceballos et al., 2020; Lecler et al., 2015;
cern regarding e-waste handling is related to the toxicity of many of their Papaoikonomou et al., 2018), being mainly traced by Pb, Sr, Cd, Y and
components. This is why studies investigating on the concentrations of air- As, all of them were found in very high concentrations in this study
borne polychlorinated biphenyls (PCBs), brominated flame retardants (Table 4 and Fig. 5). The literature also reports that high exposures to
(BFRs) and heavy metals, together with their health implications, have heavy metals have even been detected at workers' homes, and also in sam-
sharply increased in recent years (Kim et al., 2019; Nti et al., 2020; Poole ples of blood, urine and hair (Julander et al., 2014; Kuntawee et al., 2020;
and Basu, 2017;Balasch et al., 2022) Focusing on heavy metals, the pres- Wang et al., 2009). On the other hand, organic and elemental carbon (OC,
ence of high concentrations of Pb, Ni, Zn, Sb, Ti, Cr, Cu, Hg, Cd, Mn, As EC) concentrations from WEEE facilities have been rarely reported in liter-
and Co in air has been frequently reported in literature (Table 2), with ature and mainly associated with uncontrolled burning activities, finding
values exceeding those recorded at near urban environments by factors elevated concentrations, up to 382–563 μg/m3 of OC and 26–42 μg/m3 of
higher than 100. This agrees with factors obtained in this study for the dif- EC (Bi et al., 2010; Ding et al., 2018), higher than those recorded in this
ferent species analysed, ranging between 5 and 3000 for PM2.5, when com- study.
paring working areas with the urban background. Results in this study are
3.3. Inhalation exposure impacts
Fig. 4. Concentrations of major elements (μg/m3) recorded at the different sampling Fig. 5. Concentrations of trace elements (ng/m3) recorded at the different sampling
sites (top floor, ground floor and BG) in comparison with the range of values at sites (top floor, ground floor and BG) in comparison with the range of values at
Palau Reial urban background (UBG). Note that values in the x axis correspond to Palau Reial urban background (UBG). Note that values in the x axis correspond to
a logarithmic scale. a logarithmic scale.
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M. López et al. Science of the Total Environment 833 (2022) 154871
Fig. 6. Percentage of cell viability measured with Alamar Blue and CFDA-AM in A549 cells exposed to samples collected with Biosampler in both campaigns during 30 min.
Results are expressed as percentage of control cells as mean ± SD of at least three different assays.
liquid suspension. Fig. 6 shows the cell viability of filtered samples (0.2 (ground and top floor, respectively; sampled in November 2020). Com-
μm). The results were similar for filtered (<0.2 μm) and unfiltered (<2 pared to other studies, this response in the range of that observed for
μm) samples. None of the samples evidenced significant cytotoxicity bisphenol A, nonylphenol, and octylphenol in placenta cells (Pérez-
using AB and CFDA; cell viability was always >80%.. The only sample Albaladejo et al., 2017). Lower response (1.5-fold) was detected for samples
close to the 80% threshold was sample #7, collected from the ground 9, 10 and 11. Samples 3, 4, 5, 6 and 8 (unfiltered) showed a response below
floor. Overall, these results did not evidence any strong cytotoxic potential control levels, suggesting an interference of the particles with the biological
for the samples analysed, but longer exposure times in more physiologically system. Results evidence an apparent absence of pattern in terms of ROS
relevant models (He et al., 2021) might help to better characterize the toxic generation by samples collected from the top and ground floors, which
potential of these samples in future experiments. limits the interpretation of the potential sources impacting aerosol reac-
Therefore, to understand the reactivity of the aerosols sampled when in tivity. Thus, it was concluded that the variability of the WEEE entering
contact with human lung cells, the samples were tested for oxidative stress the plant is probably the source of this heterogeneity in the particle re-
generation. Clear differences were observed between ROS generation in the activity assay. Different types of e-waste were processed each day in
unfiltered (Fig. 7) and filtered (Fig. 8) samples. This assay measures fluores- the facility (from gaming machines to fridges, televisions or toys),
cence at different times (15, 30, 60 and 120) to detect the generation of re- which meant that the type and intensity of the activities also varied
active oxygen species (ROS). In the case of the filtered samples from day to day. A larger number of samples, from a more repetitive pro-
(i.e., samples containing only ultrafine particles, <0.2 μm) a significant in- cess, would be necessary to understand the source of aerosol reactivity
duction of ROS was observed after only 15 min of exposure ROS generation and to correlate it with others parameters such as size-resolved particle
The response obtained for the filtered samples (Fig. 8) was higher than for chemical composition.
the unfiltered ones, confirming the larger hazard potential of ultrafine aero- In sum, it may be concluded that, even though exposure to ultrafine,
sols in comparison to fine particles (Oberdorster, 2000). fine and coarse aerosols from the different floors in the facility did not evi-
The samples with induced the highest levels of ROS (3-fold) generation dence cytotoxic effects, ROS generation was statistically significant for 4
were 1, 2 (both from the top floor; sampled in October 2020), 7 and 12 out of the 12 samples collected, especially for ultrafine particles.
Fig. 7. ROS production in A549 cells after 15, 30, 60 and 120 min exposure to Fig. 8. ROS production in A549 cells after 15, 30, 60 and 120 min exposure to
samples collected with Biosampler in both campaigns during 30 min. Values are samples, filtered at <0.2 μm, collected with Biosampler in both campaigns during
expressed as fold induction as mean ± SD of at least six replicates in three 30 min. Values are expressed as fold induction as mean ± SD of at least six
different plates assayed. Dotted line represents ROS production in control cells. replicates in three different plates assayed. Dotted line represents ROS production
*Statistically significant differences from control. in control cells. *Statistically significant differences from control.
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