Environment International 94 (2016) 69–75

Contents lists available at ScienceDirect

Environment International

journal homepage: www.elsevier.com/locate/envint

Influence of pollution control on lead inhalation bioaccessibility in PM2.5:

A case study of 2014 Youth Olympic Games in Nanjing
Shi-Wei Li a, Hong-Bo Li a, Jun Luo a, Hui-Ming Li a, Xin Qian a, Miao-Miao Liu a, Jun Bi a,
Xin-Yi Cui a,⁎, Lena Q. Ma a,b,⁎⁎
a
State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210046, People's Republic of China
b
Soil and Water Science Department, University of Florida, Gainesville, FL 32611, United States

a r t i c l e i n f o a b s t r a c t

Article history: Pollution controls were implemented to improve the air quality for the 2014 Youth Olympic Games (YOG) in
Received 31 March 2016 Nanjing. To investigate the influence of pollution control on Pb inhalation bioaccessibility in PM2.5, samples
Received in revised form 10 May 2016 were collected before, during, and after YOG. The objectives were to identify Pb sources in PM2.5 using stable iso-
Accepted 10 May 2016
tope fingerprinting technique and compare Pb inhalation bioaccessibility in PM2.5 using two simulated lung
Available online 19 May 2016
fluids. While artificial lysosomal fluid (ALF) simulates interstitial fluid at pH 7.4, Gamble's solution simulates
Keywords:
fluid in alveolar macrophages at pH 4.5. The Pb concentration in PM2.5 samples during YOG (88.2 ng m−3) was
Pb 44–48% lower than that in non-YOG samples. Based on stable Pb isotope ratios, Pb in YOG samples was mainly
Inhalation bioaccessibility from coal combustion while Pb in non-YOG samples was from coal combustion and smelting activities. While
PM2.5 Pb bioaccessibility in YOG samples was lower than those in non-YOG samples (59–79% vs. 55–87%) by ALF, it
Stable isotope was higher than those in non-YOG samples (11–29% vs. 5.3–21%) based on Gamble's solution, attributing to
Gamble's solution the lower pH and organic acids in ALF. Different Pb bioaccessibility in PM2.5 between samples resulted from
Coal combustion changes in Pb species due to pollution control. PbSO4 was the main Pb species in PM2.5 from coal combustion,
which was less soluble in ALF than PbO from smelting activities, but more soluble in Gamble's solution. This
study showed it is important to consider Pb bioaccessibility during pollution control as source control not only
reduced Pb contamination in PM2.5 but also influenced Pb bioaccessibility.
Published by Elsevier Ltd.

1. Introduction 2014). Accurate assessment of Pb exposure via PM2.5 inhalation there-

Due to its rapid industrialization, China has been experiencing se-
vere haze events, with PM2.5 as a main contributor (Guo et al., 2014;
Huang et al., 2014). An increasing body of evidences has shown the cor-
relation between exposure to PM2.5 and many diseases including lung
cancer (Cakmak et al., 2014; Richmond-Bryant et al., 2014). Lead (Pb)
is one of the most enriched metals in PM2.5 and has attracted much at-
tention during the past few decades (Sun et al., 2006). Numerous stud-
ies have investigated Pb levels in PM2.5, and significant correlation
between PM2.5 Pb levels and blood Pb levels in children has been ob-
served (Liang et al., 2010; Richmond-Bryant et al., 2014). These results
suggest that PM2.5 inhalation is an important Pb exposure pathway for
humans. It is therefore imperative to assess human health risks through
Pb exposure in PM2.5 via inhalation pathway.
Evidence shows that not all Pb in airborne particles can be absorbed
into the systemic circulation (Boisa et al., 2014; Wiseman and Zereini,
⁎ Corresponding author.
⁎⁎ Correspondence to: L.Q. Ma, State Key Laboratory of Pollution Control and Resource
Reuse, School of the Environment, Nanjing University, Nanjing 210046, People's Republic
of China.
E-mail addresses: lizzycui@nju.edu.cn (X.-Y. Cui), lqma@ufl.edu (L.Q. Ma).
fore requires the measurement of its bioavailability. Although in vivo as-
says using animals are more accurate to measure Pb inhalation
bioavailability, they are still in the development phase. Consequently,
in vitro assays using simulated lung fluid have been developed as they
are simple and practical to use. There are two common artificial lung
fluids, i.e., Gamble's solution and artificial lysosomal fluid (ALF), which
simulate two different processes after PM2.5 particles are inhaled into
lungs. They have been used to measure metal bioaccessibility in PM2.5.
For example, inhalation bioaccessibility of platinum group elements in
PM of Germany was measured using the two methods (Zereini et al.,
2012). Similarly, Wiseman and Zereini (2014) reported Pb bioaccessibi-
lity in PM2.5 at 84% (77–91%) by ALF and 4.0% (1.0–9.0%) by Gamble's
solution. However, compared to the large number of studies investigat-
ing Pb levels in PM2.5, there remains a knowledge gap regarding Pb in-
halation bioaccessibility in PM2.5.
It is well known that Pb speciation in soil is a main factor influencing
its Pb bioaccessibility (Rasmussen et al., 2011; Smith et al., 2011). Differ-
ent sources including industrial emission, vehicle exhaust, coal combus-
tion and suspended soil particles contribute to Pb in PM2.5
(Charlesworth et al., 2011; Cheng and Hu, 2010). For example, PM2.5
from smelting activities are more enriched with PbO due to Pb vapor

http://dx.doi.org/10.1016/j.envint.2016.05.010
0160-4120/Published by Elsevier Ltd.
70 S.-W. Li et al. / Environment International 94 (2016) 69–75
oxidization in the air (Batonneau et al., 2004) whereas more PbSO4 is
accumulated in PM2.5 from coal combustion due to the sulfate enrich-
ment in coal (Shah et al., 2009). Therefore, it can be expected that Pb in-
halation bioaccessibility in PM2.5 from different sources may vary
greatly. The influence of Pb sources on its oral bioaccessibility in soils
has been extensively studied (Bannon et al., 2009; Smith et al., 2011;
Cao et al., 2003; Hardison Jr. et al., 2004). However, the influence of Pb
source on its inhalation bioaccessibility in PM2.5 has not been well eluci-
dated. This knowledge gap is mainly due to the difficulty to identify the
Pb sources in PM2.5 by conventional approaches including chemical
mass balance, positive matrix factorization models and enrichment fac-
tor (Liang et al., 2016). In recent years, fingerprinting based on stable Pb
isotope ratios has been successfully used to determine Pb sources in var-
ious environmental media including airborne PM (Widory et al., 2010).
Here we hypothesized that the influence of contamination sources on
Pb bioaccessibility in PM2.5 can be effectively examined by coupling
the stable Pb isotope ratio technique with simulated lung fluid
extraction.
Nanjing is a mega city in eastern China with an area of 6587 km2 and
population of 8.2 million. It hosted the 2nd Summer Youth Olympic
Games (YOG) during August 16th–28th, 2014. Considering the poor
air quality in Nanjing, the local government implemented pollution con-
trols during the YOG. Approximately 2630 construction sites were
closed, and heavy-industry factories such as iron and steel industries
and petrochemical enterprises were required to reduce manufacturing
by 20%. Vehicles with high emissions such as trucks, engineered vehi-
cles, and vehicle van transporting hazardous materials were banned in
the city. In addition, 22 nearby cities were asked to cooperate with Nan-
jing to close industries with high pollution emission during the YOG
(Ding et al., 2015; Pan et al., 2015). Significant improvement in air qual-
ity was expected with the pollution control, so were the changes in Pb
contamination source in airborne PM during the YOG.
Therefore, the pollution control during the YOG provided us a
unique opportunity to study the influences of Pb sources on its bioacces-
sibility in PM2.5. To this end, PM2.5 samples were collected before, dur-
ing, and after the YOG in Nanjing. The overall objective of this study
was to investigate the influence of pollution control on Pb inhalation
bioaccessibility in PM2.5 by 1) identifying Pb sources using the stable
isotope ratio fingerprinting technique, and 2) measuring Pb inhalation
bioaccessibility using two in vitro methods (ALF and Gamble's solution).
The results from this study should provide us useful information for pol-
icy decision regarding pollution control and risk assessment for inhala-
tion exposure to air-born Pb.
2. Materials and methods
2.1. Sampling of PM2.5
Particulate matter (PM2.5) sample was collected for ~ 12 h using a
high volume air sampler (Model TE6070, Tisch Environmental Inc.) at
a flow rate of 1.13 m3 min−1 with quartz microfiber filters (Whatman,
203 mm × 254 mm). The sampling device was placed on the building
roof (~30 m height) of the School of the Environment of Nanjing Uni-
versity on Xianlin campus. The campus is located in northeastern Nan-
jing, ~ 20 and 5 km away from industrial zone and Qixia lead–zinc
mines.
A total of 32 PM2.5 samples were collected before (10 samples, June
1st–July 31st), during (9 samples, August 1st–August 31st), and after
(13 samples, September 1st–October 20th) YOG in 2014. Since the
local government started source controls in early August, August sam-
ples were considered as the YOG period. Before sampling, quartz micro-
fiber filters were heated at 500 °C for 5 h in a muffle furnace, and
equilibrated in a desiccator for 48 h before being weighed using an an-
alytical balance (Denver SI-234). After sampling, quartz microfiber fil-
ters were equilibrated in a desiccator before being weighed for PM2.5
mass. The PM2.5 mass was determined as the difference between the
filter weights before and after sampling. The filters were encased in tin-
foil and sealed in plastic bags and stored at −20 °C until analysis.
2.2. Total Pb concentration in PM2.5
Quantification of Pb in PM2.5 was performed by digesting quartz mi-
crofiber filters using ultra-pure concentrated HNO3 and 30% H2O2 ac-
cording to USEPA Method 3050B with slight modifications. Briefly, 1/
16 of quartz microfiber filters were cut into pieces of b2 mm2 using
acid-cleaned ceramic knife. The filters were digested with 10 mL con-
centrated HNO3 (1:1) by immersing quartz filters in concentrated
HNO3 so all PM2.5 particles were in contact with HNO3. Since PM2.5
and filter were digested together, the digestion process should measure
all the Pb on the filters. The digestion was conducted on a HotBlock di-
gestion system (Environmental Express, USA) at 105 °C for 5 h, and then
10 mL concentrated HNO3 was added. After concentrated HNO3 was
evaporated to near dryness and cooled down, 1–2 mL 30% H2O2 was
added. The digestion was continued to reach ~ 1 mL solution, which
was diluted to 50 mL with Milli-Q water, and filtered through 0.22 μm
filter before analysis. Concentrations of Pb in the solution were deter-
mined by inductively coupled plasma mass spectrometer (ICP-MS,
NexIONTM300X, Perkin Elmer, USA) with detection limit of
0.008 μg L−1. Standard Reference Material (SRM) D056–540 was per-
formed for QA/QC during digestion process. The Pb recovery was of
99.4 ± 5.78%, which is within the ± 10% recommended by USEPA
(2013).
2.3. Stable isotope ratios in PM2.5
Lead stable isotope ratios of 207/206Pb and 208/206Pb in digestion solu-
tion were determined using ICP-MS. Instrument parameters were set as
190 sweeps/reading, 1 reading/replicate, and 10 replicates/sample solu-
tion. Dwell time of 40 ms was set for 204Pb and 25 ms for 206Pb, 207Pb,
and 208Pb. Prior to analysis, Pb concentration in solution was diluted
to ~15 μg L−1 using 0.1 M high-purity HNO3. Standard reference mate-
rial (SRM) NIST 981 with concentration of 15 μg L− 1 was measured
every 5 samples to obtain ratio correction factors to compensate for
mass discrimination. The analytical precision for samples was generally
b0.5% for 207/206Pb and 208/206Pb. Measured 204/206Pb (0.0590 ± 0.0001),
207/206
Pb (0.9149 ± 0.0024), and 208/206Pb (2.1688 ± 0.0029) in the
SRM NIST 981 (n = 10) were in good agreement with the certified
values of 0.0590, 0.9146, and 2.1681.
2.4. Pb bioaccessibility in PM2.5
Two artificial lung fluids including artificial lysosomal fluid (ALF)
and Gamble's solution were employed to measure Pb inhalation bioac-
cessibility in PM2.5 (Boisa et al., 2014; Colombo et al., 2008; Zereini et
al., 2012). Detailed compositions of the lung fluids can be found in sup-
port information as Table S1. The extraction procedure was performed
according to Zereini et al. (2012). Briefly, 1/16 of quartz microfiber fil-
ters (b2 mm2) were placed in 50 mL high density polyethylene tubes
containing 30 mL of fluid. Based on the PM2.5 mass, the solid and solu-
tion ratio was 1:2400 to 1:14,000, which was in the range of 1:500 to
1:50,000 suggested by Julien et al. (2011). The tubes were put in an in-
cubator at 37 °C in dark. Samples were shaken for 10 min every 4 h on a
shaker at 50 rpm. Once inhaled into lungs, part of PM2.5 can be quickly
dissolved in the interstitial fluid, but 10–15% of the initially deposited
PM2.5 can be present in lungs after 1 day and their clearance in human
bronchial tree may last for several weeks (Hofmann and Asgharian,
2003; Lippmann et al., 1980). So the PM2.5 particles deposited in lung
are subject to both short and long retention with most studies using
1 day as the short term (Julien et al., 2011). For the long term, time var-
iations of 4–30 days were reported (Boisa et al., 2014; Zereini et al.,
2012). In our preliminary test, some fungi appeared in lung fluid after
15-day extraction. To avoid the analysis uncertainty caused by fungi,
 S.-W. Li et al. / Environment International 94 (2016) 69–75 71

15-day was selected as the long term, with 1 day as the short to assess
bioaccessible Pb in PM2.5. For 1 day extraction, pH was measured
every 4 h with no significant pH fluctuation being found. For the
15 day extraction, pH was checked every day and adjusted using nitric
acid and sodium hydroxide. At the end of 1- and 15-days, tubes were
centrifuged at 4000 rpm for 10 min with supernatants filtered through
0.22 μm polypropylene membrane filters. Concentrated HNO3 at 1% was
added into the supernatants for sample preservation. Solutions were
stored at 4 °C until analysis using ICP–MS.
2.5. Statistical analyses
All experiments were run with two replicates. One-way analysis of
variance (ANOVA) based on least-significant difference (LSD) was ap-
plied using SPSS 10.0 for windows to determine the significant differ-
ences in Pb concentrations, Pb bioaccessibility and stable Pb isotope
ratios in PM2.5 collected before, during, and after the YOG. All graphs
were created using Origin 9.0.
3. Results and discussion
3.1. Changes in PM2.5 and Pb concentrations before, during, and after the
YOG
Based on PM2.5 concentrations, our data suggested that source con-
trols by local government during the YOG were effective in improving
the air quality in Nanjing. The PM2.5 concentrations were 83–267, 41–
105, and 39–179 μg m−3 in samples collected before, during, and after
YOG (Fig. 1A). The average PM2.5 concentration during the YOG period
(61.4 μg m− 3, n = 9) was 64% and 47% lower than those before
(172 μg m−3, n = 10) and after the YOG (117 μg m− 3, n = 13). The
PM2.5 levels were also lower than the average PM2.5 concentration of
106 μg m−3 in August 2012 of Nanjing (Shen et al., 2014), indicating
the effectiveness of the source control at reducing PM2.5 levels in
Nanjing. The mean PM2.5 concentration during YOG period was compa-
rable to 64.7 μg m−3 during the 2008 Olympic in Beijing (Wang et al.,
2009) and 77.0 μg m− 3 during the 2010 Asian Games in Guangzhou
(Tao et al., 2015). Moreover, the average PM2.5 concentration after the
YOG was 32% lower than those before the YOG, which was partially ex-
plained by the changes in meteorology. Meteorological parameters dur-
ing sampling days, including temperature, relative humidity, visibility
and wind speed, were obtained from www.wunderground.com (Fig.
S1). The wind speed was negatively correlated with PM2.5 concentra-
tions while the relative humidity was positively correlated with PM2.5
concentration (p b 0.05) (Marcazzan et al., 2001). Based on the meteo-
rology parameters, the average wind speed before-YOG was 1.72 m s−1,
which was lower than 1.97 m s−1 after-YOG. Similarly, the average rel-
ative humidity before-YOG was 88%, which was higher than that after-
YOG (75%). The meteorological differences (i.e., higher wind speed and
lower relative humidity) may partially explain the lower PM2.5 levels in
samples after-YOG than before-YOG.
For samples collected before, during, and after the YOG, the Pb con-
centrations in PM2.5 based on air volume were 42.1–122, 36.9–77.9, and
40.5–233 ng m−3, (averaging 88.2, 49.1, and 95.3 ng m−3) (Fig. 1B). The
average Pb concentration in YOG samples was 44–48% lower than non-
YOG samples and was comparable to that during 2008 Beijing Olympic
Games (48.9 ng m−3) (Schleicher et al., 2012). However, though lower
Pb concentrations were observed, they were still higher than those in
cities from Europe and USA during normal days. For example, the aver-
age Pb concentrations in PM2.5 were 25 ng m−3 for 20 U.S. cities during
2003–2005 (USEPA, 2007) and 5.5–13 ng m−3 for European cities in-
cluding Athens, Helsinki, and Frankfurt (Pakkanen et al., 2001;
Remoundaki et al., 2013; Wiseman and Zereini, 2014).
At present, there is no standard for Pb concentrations in PM2.5. How-
ever, there are limits for total suspended particulates (TSP, b 100 μm) in
the air, which are 500 ng m−3 and 150 ng m−3 by China's Ambient Air
Quality Standard (CAAQS) and US National Ambient Air Quality Stan-
dard (NASQS), while standard for Pb in PM10 is 500 ng m−3 based on

Fig. 1. PM2.5 concentration (A) and Pb concentration (B) based on air volume before, during, and after the Youth Olympic Games (YOG) in Nanjing and Pb bioaccessibility (%) in PM2.5
collected before, during, and after YOG period using artificial lysosomal fluid (ALF) (C) and Gamble's solution (Gam) (D) after 1 day and 15 days extraction. Boxes represent 25th to
75th percentile, solid lines and squares in boxes are the median and mean values, error bars represent 1st to 99th percentiles, crossing symbols represent the minimum and maximum
values. Means marked with different letters indicate significant difference (p b 0.05). Dash line in Fig. A presents Chinese National PM2.5 standard, grade II 75 μg m−3 and dot line
presents USEPA standard, grade II 35 μg m−3.
72 S.-W. Li et al. / Environment International 94 (2016) 69–75

European directive of 2008/50/EC. To make a comparison between Pb
concentrations in PM2.5 and these standards, we estimated the Pb
mass in PM2.5, TSP and PM10. Based on previous studies on air quality
monitoring in Nanjing from 2010 to 2012, the mean mass ratios of
PM2.5 to PM10 and PM2.5 to TSP were 0.73 and 0.5 (Hu et al., 2012;
Shen et al., 2014). In addition, it was assumed that Pb concentrations
(mg kg−1) in PM10 and TSP were equal to that in PM2.5 even though
Pb is more enriched in fine particles (Hu et al., 2013). Lead concentra-
tions in TSP and PM10 in Nanjing were estimated by dividing Pb concen-
tration in PM2.5 with mass ratios of PM2.5 to PM10 and PM2.5 to TSP. The
estimated average Pb concentrations in PM10 and TSP in YOG samples
were 67.3 (50.5–107) and 98.2 (73.8–156) ng m−3, while they were
at 126 (57–188) and 184 (83–274) ng m−3 in non-YOG samples. For
the less stringent limits set by CAAQS (500 ng m−3 in TSP) and Europe-
an directive of 2008/50/EC (500 ng m−3 in PM10), Pb concentrations in
all samples complied with the values. However, Pb concentrations in
11% of YOG samples exceeded the NASQS limit (150 ng m−3) and 41%
did in non-YOG samples.
3.2. Changes in Pb sources in PM2.5 before, during, and after the YOG
In addition to Pb concentrations in PM2.5 based on air volume, the
mean Pb concentrations were also calculated based on PM2.5 particle
mass, which were 514, 850, and 764 mg kg−1 in samples collected be-
fore, during, and after YOG (Table 1). The relatively lower Pb mass con-
centration in non-YOG PM2.5 samples may attribute to the effect of
secondary organic aerosol (Huang et al., 2014). There are two main
sources of PM2.5, i.e., primary emitted particles (directly emitted to the
atmosphere, like dust from smelting or coal combustion) and secondary
organic aerosol (formed through gas-to-particle conversion in light-in-
duced chemical reaction based on air composition) (Hinds, 1999;
Huang et al., 2014). It was reported that the particles from secondary or-
ganic aerosol constituted 51–77% of PM2.5 during haze days (Huang et
al., 2014). Since haze events frequently occurred during the non-YOG
period, the relatively larger proportion of secondary organic aerosol in
PM2.5 may dilute Pb mass concentration in non-YOG PM2.5 samples.
On the other hand, it was possible that Pb in PM2.5 collected during dif-
ferent periods have different originations. For example, Pb concentra-
tion was 1788 mg kg− 1 in coal combustion dust, 6140 mg kg−1 in
metallurgic dust, and 238 mg kg− 1 in unleaded gasoline (Tan et al.,
2006). Given the different Pb concentrations between non-YOG and
YOG PM2.5 samples, it was expected that Pb sources in PM2.5 were dif-
ferent for non-YOG and YOG periods.
To further track the changes of Pb sources before, during, and after
YOG, stable Pb isotope ratios in PM2.5 samples were measured (Table 1
and Fig. 2). Significant differences in the stable isotope ratios
(207Pb/206Pb and 208Pb/206Pb) between YOG and non-YOG samples
were observed (p b 0.05). Stable Pb isotope ratios in PM2.5 were clearly
distinct from soils around Qixia Pb–Zn minerals (Fig. 2), so their contri-
bution was excluded. Stable Pb isotope ratios in most of the non-YOG
samples were between those of coal combustion ash and metallurgic
dust (Fig. 2), suggesting that both sources contributed to Pb in these
samples. This finding is consistent with Hu et al. (2014) who showed
that coal emissions and smelting activities were two important sources
for Pb in PM2.5 from urban sites of Nanjing. For YOG PM2.5 samples, the
isotopic ratios (207/206Pb and 208/206Pb) were elevated, being mainly o-
verlapped with those of coal combustion with several points overlap-
ping with unleaded gasoline (Fig. 2). During the YOG period, many
smelters in Nanjing were shut down, and it was not surprising that its
contribution to air Pb pollution was reduced in YOG samples (Ding et
al., 2015). However, coal combustion power plants were still in opera-
tion during the YOG to supply electricity to the city. Therefore, Pb in
YOG samples may come from coal combustion and unleaded gasoline
(Fig. 2). However, Pb concentration in YOG PM2.5 was 850 mg kg−1,
which was much higher than that for unleaded gasoline dust
(238 mg kg−1) (Tan et al., 2006). Therefore, unleaded gasoline did not
make much contribution to Pb in YOG PM2.5 samples even though
some data points overlapped with the isotopic ratios of unleaded gaso-
line dust. Overall, we found that Pb pollution sources changed from coal
combustion and smelting (non-YOG) to coal combustion (during YOG).
Therefore, PM2.5 samples during the YOG and non-YOG provided us a
unique opportunity to study the effects of Pb sources on Pb inhalation
bioaccessibility in PM2.5.
3.3. Pb bioaccessibility in PM2.5 by in vitro assays
Two in vitro assays, artificial lysosomal fluid (ALF) at pH = 4.5 and
Gamble's solution at pH = 7.4 were used to measure Pb bioaccessibility
in PM2.5 (Fig. 1C, D). In addition, two extraction durations (1 and
15 days) were used to simulate the short and long term retention of
PM2.5 particles after being inhaled into lungs.
ALF mainly simulates Pb inhalation bioaccessibility in macrophages.
After 1 day extraction, Pb bioaccessibility in YOG PM2.5 samples (61 ±
4.3%, n = 9) was significantly lower than those in before (66 ± 6.4%,
n = 10) and after YOG samples (78 ± 4.6%, n = 13). The data indicated

Table 1
Descriptive statistics of Pb concentrations (based on PM2.5 mass and air volume) and sta-
ble isotope ratios in PM2.5 collected before, during, and after Youth Olympic Games (YOG)
in Nanjing.

Pb (ng m−3) Pb (mg kg−1) 207

Pb/206Pb 208
Pb/206Pb

Before YOG (n = 10)

Min 42.2 410 0.8522 2.0896
Max 122 606 0.8588 2.1113
Median 90.8 523 0.8549 2.0948
Mean 88.2 514 0.8547 2.0969
SD 29 65 0.0020 0.0067

During YOG (n = 9)
Min 36.9 530 0.8520 2.0875
Max 77.9 1332 0.8663 2.1243
Median 45.7 835 0.858 2.1076
Mean 49.1 850 0.8593 2.1092
SD 13.5 249 0.0048 0.0122

After YOG (n = 13)

Min 40.5 445 0.8498 2.0821
Fig. 2. Ratios of 208Pb/206Pb vs. 207Pb/206Pb in PM2.5 collected before, during, and after
Max 233 1046 0.8576 2.0975
Youth Olympic Games (YOG) in Nanjing. Ranges or individual isotope ratios of different
Median 87.7 751 0.8539 2.0887
anthropogenic Pb sources, including coal, leaded and unleaded gasoline (Chen et al.,
Mean 95.3 764 0.8535 2.0896
2005), metallurgy dust (Tan et al., 2006), and lead growth curve (Cumming and
SD 51.3 169 0.0026 0.0050
Richards, 1975) and soil around lead-zinc mines.
 S.-W. Li et al. / Environment International 94 (2016) 69–75
that not only the total Pb concentrations in YOG PM2.5 (49.1 ng m−3)
were lower than those before and after YOG samples (88.2 and
95.3 ng m−3; Fig. 1B), so were the bioaccessible Pb based on ALF. The
bioaccessible Pb in this study (66–78%) were lower than the 84% report-
ed by Wiseman and Zereini (2014). This may be due to the heterogenic
compositions of airborne PM. After 15 day extraction, the mean Pb bio-
accessibility was significantly (p b 0.05) reduced to 60 ± 3.6% in sam-
ples collected before YOG, while those collected during and after YOG
slightly reduced to 59 ± 3.3 and 77 ± 4.5% with no statistical difference
(p = 0.21–0.50). This was consistent with previous study that average
Pb bioaccessibility was reduced from 84 to 60% as extraction duration
extended from 1 to 30 days (Wiseman and Zereini, 2014). The slight re-
duction in Pb bioaccessibility may be attributed to resorption of mobi-
lized Pb onto particle surfaces (Zereini et al., 2012).
Gamble's solution differs from ALF as it measures Pb bioaccessibility
after PM2.5 enters interstitial fluid in the lungs. Based on Gamble's solu-
tion, the average Pb bioaccessibility in PM2.5 after 1 day extraction were
10, 20, and 11% before, during, and after YOG, with Pb bioaccessibility in
YOG samples being significantly higher. After 15 day extraction, the
values decreased sharply to 5.0, 0.08, and 6.0% (Fig.1D). Besides the re-
sorption process (Wiseman and Zereini, 2014; Zereini et al., 2012), the
reduction of Pb bioaccessibility in Gamble's solution may be attributed
to the formation of insoluble Pb mineral, limiting Pb dissolution during
the extraction. For example, Pb bioaccessibility in mining waste tailings
and dusts was measured by Gamble's solution after 630 h, insoluble lead
phosphate minerals was observed after 24 h through SEM, which is
formed on the surface of dust, effectively limiting Pb dissolution
(Wragg and Klinck, 2007). Where Pb bioaccessibility in ALF was notably
higher than those in Gamble's solution, which was mostly attributed to
their pH difference, i.e., 4.5 vs. 7.4, as Pb is less soluble at higher pH (Li et
al., 2014). Wiseman et al. also found that Pb bioaccessibility in PM2.5 was
notably higher in ALF (84%) than that in Gamble's solution (4.0%) after
1 day extraction (Wiseman and Zereini, 2014). In gastrointestinal
fluid, the same phenomenon was also observed. For example, Pb bioac-
cessibility decreased from 46–99 to 22–60% when the extraction pH in-
creased from 1.5 to 2.5 in house dust samples (Li et al., 2014). Besides
pH, the difference in chemical components in the two lung fluids may
also influence Pb bioaccessibility. For example, based on Gamble's solu-
tion and water extract of four reference materials at same pH, the ex-
tractable Pb was significantly higher in Gamble's solution than that in
water (Julien et al., 2011). ALF and Gamble's solution have different
chemical compositions (Table S1), with ALF having more organic
acids. Organic acids have been reported to promote Pb dissolution
from Pb minerals in dust samples (Debela et al., 2010; Li et al., 2014),
which can partially explain the higher Pb bioaccessibility by ALF than
Gamble's solution.
Currently, there is no standard method to measure Pb inhalation bio-
accessibility in PM2.5. Due to its lack of organic components that are
present in human respiratory tract, Gamble's solution has been modi-
fied by adding organic acids, proteins, and surfactants (Boisa et al.,
2014; Gray et al., 2010; Stebounova et al., 2011). These additional com-
ponents were expected to increase Pb dissolution kinetics and hence Pb
bioaccessibility. To test this hypothesis, we added organic acids (ascor-
bic acid and uric acid), protein (mucin), and surfactant (dipalmitoyl
phosphatidyl choline-DPPC) to Gamble's solution (Table S1). The mod-
ified Gamble's solution was based on Boisa et al. (2014) and detailed
compositions can be found in Table S1. The method was used to extract
PM2.5 samples before, during, and after YOG (i.e., #1, 13, and 27) for
1 day. The Pb bioaccessibility was 23–43%, which was much higher
than 5.3–11% in Gamble's solution (Fig. 3).
To test the effect of individual component, we removed organic
acids, mucin, or DPPC from modified Gamble's solution and extracted
samples #1, 13, and 27 again. The Pb bioaccessibility was decreased to
1–9, 0.2–28, and 5.6–18%, indicating that these components contributed
to the increased Pb bioaccessibility in PM2.5 (Fig. 3). For example, surfac-
tant DPPC is a phospholipid secreted by type 2 cells and located in
73
Fig. 3. Comparison of Pb bioaccessibility extracted by Gamble's solution, IBM (inhalation
bioaccessibility method), and IBM without organic acids, DPPC, or mucin.
alveoli of lungs. Previous studies suggested that DPPC in lung fluid in-
creased the wettability of PM2.5 to reduce aggregation of PM2.5 and im-
proved the contact between PM2.5 and artificial lung fluid (Julien et al.,
2011). However, without in vivo data, we cannot determine which
method better simulated human lungs. These in vitro methods are de-
veloped to simulate the physiological environment in human lung
fluids. Therefore, the extractable Pb should be more realistic than total
Pb concentrations. In addition, these methods are favorable than in
vivo tests due to their cost saving and easy operation (Colombo et al.,
2008; Wiseman, 2015; Zereini et al., 2012).
Different Pb bioaccessibility in PM2.5 samples collected before, dur-
ing, and after YOG may be explained by the changes in Pb contamina-
tion sources due to pollution control. Stable isotope ratios illustrated
that Pb in YOG samples was mainly from coal combustion ash, while
Pb in non-YOG samples was from both smelting activities and coal com-
bustion (Fig. 2). We tried to identify Pb speciation in PM2.5 samples
using X-ray absorption spectroscopy (Fig. S2), but the result was unsuc-
cessful due to the interference from the complicated matrix in PM2.5.
However, based on Pb isotope ratio and X-ray absorption spectroscopy,
Tan et al. (2006) reported that Pb in PM10 samples from coal combus-
tion, and iron and steel smelters in Shanghai were mainly present as
PbSO4, PbO, and PbCl2. Based on scanning Raman microspectrometry
and X-ray photoelectron spectroscopy, Pb in smelter dust was mainly
present as PbSO4, PbSO4·PbO, PbSO4·4PbO, and PbO (Batonneau et al.,
2004), and based on X-ray absorption spectroscopy, PbSO4 was the
main Pb species in coal fly ash (Shah et al., 2009). Based on these litera-
tures, we expected higher portion of PbO in non-YOG samples and higher
portion of PbSO4 in YOG samples. It is reported that PbSO4 has lower
solubility than PbSO4·PbO and PbSO4·4PbO at pH = 4.5 in ALF, but the
opposite is observed at pH = 7.4 in Gamble's solution (Sommers and
Lindsay, 1979). While Na2Ac and NaHCO3 are present in Gamble's
solution, they are absent in ALF (Table S1). The HCO− 3 buffers Gamble's
solution to slightly alkaline pH (pH= 7.4), making PbSO4 more soluble
in alkaline solution than PbO in the presence of Ac2−. To test this hypoth-
esis, we measured Pb bioaccessibility of PbSO4 and PbO using ALF and
Gamble's solutions. Based on ALF, the bioaccessible Pb concentrations
were 324 ± 43.2 and 537 ± 27.1 mg L−1 for PbSO4 and PbO, and in
Gamble's solution they were 364 ± 10.0 and 85.6 ± 6.27 μg L−1. The
results confirmed that PbSO4 had lower bioaccessibility than PbO in ALF,
but the opposite was observed in Gamble's solution (data not shown).
4. Environmental implications
Due to poor air quality in China, Chinese government has imple-
mented various pollution control measures during YOG. Thus total con-
centrations of PM particles and PM-born Pb are expected to decrease
accordingly. However, little attention has been focused on the associat-
ed changes in Pb bioaccessibility in PM particles, which is important for
74 S.-W. Li et al. / Environment International 94 (2016) 69–75
assessing the health risks associated with inhalation of PM particles. Our
data showed that, due to the source control during YOG, Pb in PM2.5 had
lower bioaccessibility in alveolar macrophages (simulated by ALF), but
higher Pb bioaccessibility in interstitial lung (simulated by Gamble's so-
lution) in YOG samples than non-YOG samples. This highlights the im-
portance of not only reducing total Pb load in airborne PM, but also
bioaccessible Pb, which may directly impact human health.
Compared with Pb oral bioaccessibility using simulated gastrointesti-
nal solutions, studies on Pb inhalation bioaccessibility using simulated
lung fluid are rather limited. Gamble's solution was the only in vitro
method to measure Pb inhalation bioaccessibility until the development
of ALF (Beeston et al., 2010; Wiseman and Zereini, 2014). Several studies
showed that significantly higher amount of Pb in PM2.5 was extracted by
ALF than Gamble's solution. It is easier for smaller particles like PM2.5 to be
respired into distal lung part and phagocytized by macrophages, which is
simulated by ALF. Therefore, given the higher release of Pb in ALF and the
potential of PM2.5 to be phagocytized, the Pb bioaccessibility in PM2.5 may
be underestimated if only using Gamble's solution. Furthermore, alveolar
macrophages, once exposed to hazardous elements (such as Pb in PM2.5),
can be activated to produce large amount of reactive oxygen species,
which are closely related with pulmonary and systemic inflammation
(Huang et al., 2009). Consequently, it is expected that Pb bioaccessibility
in ALF (representing the cellular fluid in alveolar macrophages) can pro-
vide valuable information for toxicology studies of PM2.5.
As mentioned above, there is no standard in vitro method to measure
Pb inhalation bioaccessibility in PM2.5, and it is essential to validate in
vitro method with animal-based in vivo tests. However, there are chal-
lenges to conduct in vivo tests to measure Pb inhalation bioavailability.
First, after being inhaled, air particles can be deposited in nasal, laryngeal,
bronchial airways, and alveolar region with various clearance rates. Their
clearance rates depend on particle size and breathing cycle of animals.
The particles in nasal, laryngeal, and bronchial may be cleared relatively
quickly, but in alveolar region they may last several weeks, even several
years (Hofmann and Asgharian, 2003; Lippmann et al., 1980). It is there-
fore difficult to decide the reasonable exposure duration for in vivo tests.
In addition, PM2.5 is often collected on filters, which is difficult to re-
move. We tried to remove the particles from filters by sonication and
freeze drying, and then exposed them to mice. We found that ~60% of
the Pb on filters was lost after dissolving in water during sonication. In
addition, the aggregation state of PM2.5 particles changed during freeze
drying, which induced inaccuracy for in vivo exposure. We also tried to
expose mice with PbO and PbSO4 to see if we can obtain similar trend as
in vitro data. Briefly, 100 mg of PbO or PbSO4 (b 100 μm) were dispersed
into 50 mL saline solution, and exposed by oropharyngeal aspiration to
mice (Gavett et al., 2003), which were first fasted for 1 day (Li et al.,
2016). After 1 day, the Pb concentrations were measured in mice liver
and kidney. Unlike the in vitro result, there was no significant difference
for PbO and PbSO4 bioavailability (6.9 ± 3.7 vs. 7.9 ± 4.2 μg kg−1 in
liver, and 19 ± 12 vs. 9.6 ± 6.7 μg kg−1 in kidney) (Fig. 4). The unsuc-
cessful data may be resulted from the uncertainty of biological biomark-
er, exposure duration, or individual difference among mice. At present,
exposure chamber may be a promising tool for in vivo inhalation bio-
availability measurement. However, studies using an exposure chamber
are at the development phase as no in vivo data have been reported.
Nevertheless, these in vitro methods were developed to simulate the
physiological condition in human lung fluid, and bioaccessible Pb may
be more realistic than total Pb concentration for risk assessment. As
such, even though they may be less accurate than in vivo data, in vitro
Pb bioaccessibility measurement in PM2.5 is an important step in the
right direction to accurately assess the risk of PM2.5 to human health.
Acknowledgements
This work was supported in part by Jiangsu Provincial Natural Science
Foundation of China (no. BK20130558), Jiangsu Provincial Innovation
Team Program, and Jiangsu Provincial Double Innovation Program.
Fig. 4. Lead concentrations in the livers and kidney of mouse after two days of
oropharyngeal aspiration of ~50 mg of PbO or PbSO4 minerals.
References
Bannon, D.I., Drexler, J.W., Fent, G.M., Casteel, S.W., Hunter, P.J., Brattin, W.J., Major, M.A.,
2009. Evaluation of small arms range soils for metal contamination and lead bioavail-
ability. Environ. Sci. Technol. 43, 9071–9076.
Batonneau, Y., Bremard, C., Gengembre, L., Laureyns, J., Le Maguer, A., Le Maguer, D.,
Perdrix, E., Sobanska, S., 2004. Speciation of PM10 sources of airborne nonferrous
metals within the 3-km zone of lead/zinc smelters. Environ. Sci. Technol. 38,
5281–5289.
Beeston, M.P., van Elteren, J.T., Šelih, V.S., Fairhurst, R., 2010. Characterization of artificially
generated PbS aerosols and their use within a respiratory bioaccessibility test. Analyst
135, 351–357.
Boisa, N., Elom, N., Dean, J.R., Deary, M.E., Bird, G., Entwistle, J.A., 2014. Development and
application of an inhalation bioaccessibility method (IBM) for lead in the PM10 size
fraction of soil. Environ. Int. 70, 132–142.
Cakmak, S., Dales, R., Kauri, L.M., Mahmud, M., Van Ryswyk, K., Vanos, J., Liu, L.,
Kumarathasan, P., Thomson, E., Vincent, R., 2014. Metal composition of fine particu-
late air pollution and acute changes in cardiorespiratory physiology. Environ. Pollut.
189, 208–214.
Charlesworth, S., De Miguel, E., Ordóñez, A., 2011. A review of the distribution of particu-
late trace elements in urban terrestrial environments and its application to consider-
ations of risk. Environ. Geochem. Health 33, 103–123.
Chen, J., Tan, M., Li, Y., Zhang, Y., Lu, W., Tong, Y., Zhang, G., Li, Y., 2005. A lead isotope re-
cord of Shanghai atmospheric lead emissions in total suspended particles during the
period of phasing out of leaded gasoline. Atmos. Environ. 39, 1245–1253.
Cheng, H., Hu, Y., 2010. Lead (Pb) isotopic fingerprinting and its applications in lead pol-
lution studies in China: a review. Environ. Pollut. 158, 1134–1146.
Cao, X., Ma, L.Q., Chen, M., Hardison, D.W., Harris, W.G., 2003. Weathering of lead bullets
and their environmental effects at outdoor shooting ranges. J. Environ. Qual. 32,
526–534.
Colombo, C., Monhemius, A.J., Plant, J.A., 2008. Platinum, palladium and rhodium release
from vehicle exhaust catalysts and road dust exposed to simulated lung fluids.
Ecotoxicol. Environ. Saf. 71, 722–730.
Cumming, G., Richards, J., 1975. Ore lead isotope ratios in a continuously changing earth.
Earth Planet. Sci. Lett. 28, 155–171.
Debela, F., Arocena, J.M., Thring, R.W., Whitcombe, T., 2010. Organic acid-induced release
of lead from pyromorphite and its relevance to reclamation of Pb-contaminated soils.
Chemosphere 80, 450–456.
Ding, J., van der A, R.J., Mijling, B., Levelt, P.F., Hao, N., 2015. NOx emission estimates dur-
ing the 2014 Youth Olympic Games in Nanjing. Atmos. Chem. Phys. Discuss. 15,
6337–6372.
Gavett, S.H., Haykal-Coates, N., Highfill, J.W., Ledbetter, A.D., Chen, L.C., Cohen, M.D.,
Harkema, J.R., Wagner, J.G., Costa, D.L., 2003. World Trade Center fine particulate mat-
ter causes respiratory tract hyperresponsiveness in mice. Environ. Health Perspect.
111, 981.
Gray, J.E., Plumlee, G.S., Morman, S.A., Higueras, P.L., Crock, J.G., Lowers, H.A., Witten, M.L.,
2010. In vitro studies evaluating leaching of mercury from mine waste calcine using
simulated human body fluids. Environ. Sci. Technol. 44, 4782–4788.
Guo, S., Hu, M., Zamora, M.L., Peng, J., Shang, D., Zheng, J., Du, Z., Wu, Z., Shao, M., Zeng, L.,
Molina, M.J., Zhang, R., 2014. Elucidating severe urban haze formation in China. Proc.
Natl. Acad. Sci. 111, 17373–17378.
Hardison Jr, D.W., Ma, L.Q., Luongo, T., Harris, W.G., 2004. Lead contamination in shooting
range soils from abrasion of lead bullets and subsequent weathering. Sci. Total Envi-
ron. 328, 175–183.
Hinds, W.C., 1999. Aerosol Technology: Properties. Behavior, and Measurement of Air-
borne Particles (2nd).
Hofmann, W., Asgharian, B., 2003. The effect of lung structure on mucociliary clearance
and particle retention in human and rat lungs. Toxicol. Sci. 73, 448–456.
 S.-W. Li et al. / Environment International 94 (2016) 69–75
Hu, X., Zhang, Y., Ding, Z., Wang, T., Lian, H., Sun, Y., Wu, J., 2012. Bioaccessibility and
health risk of arsenic and heavy metals (Cd, Co, Cr, Cu, Ni, Pb, Zn and Mn) in TSP
and PM2.5 in Nanjing, China. Atmos. Environ. 57, 146–152.
Hu, X., Ding, Z., Zhang, Y., Sun, Y., Wu, J., Chen, Y., Lian, H., 2013. Size distribution and
source apportionment of airborne metallic elements in Nanjing, China. Aerosol Air
Qual. Res. 13, 1796–1806.
Hu, X., Sun, Y., Ding, Z., Zhang, Y., Wu, J., Lian, H., Wang, T., 2014. Lead contamination and
transfer in urban environmental compartments analyzed by lead levels and isotopic
compositions. Environ. Pollut. 187, 42–48.
Huang, Y.C.T., Zhuowei, L., Carter, J.D., Soukup, J.M., Schwartz, D.A., Yang, I.V., 2009. Fine
ambient particles induce oxidative stress and metal binding genes in human alveolar
macrophages. Am. J. Respir. Cell Mol. Biol. 41, 544–552.
Huang, R.-J., Zhang, Y., Bozzetti, C., Ho, K.-F., Cao, J.-J., Han, Y., Daellenbach, K.R., Slowik,
J.G., Platt, S.M., Canonaco, F., Zotter, P., Wolf, R., Pieber, S.M., Bruns, E.A., Crippa, M.,
Ciarelli, G., Piazzalunga, A., Schwikowski, M., Abbaszade, G., Schnelle-Kreis, J.,
Zimmermann, R., An, Z., Szidat, S., Baltensperger, U., Haddad, I.E., Prevot, A.S.H.,
2014. High secondary aerosol contribution to particulate pollution during haze
events in China. Nature 514, 218–222.
Julien, C., Esperanza, P., Bruno, M., Alleman, L.Y., 2011. Development of an in vitro method
to estimate lung bioaccessibility of metals from atmospheric particles. J. Environ.
Monit. 13, 621–630.
Li, H.B., Cui, X.Y., Li, K., Li, J., Juhasz, A.L., Ma, L.Q., 2014. Assessment of in vitro lead bioac-
cessibility in house dust and its relationship to in vivo lead relative bioavailability. En-
viron. Sci. Technol. 48, 8548–8555.
Li, J., Li, C., Sun, H.-J., Juhasz, A.L., Luo, J., Li, H.-B., Ma, L.Q., 2016. Arsenic relative bioavail-
ability in contaminated soils: comparison of animal models, dosing schemes, and bi-
ological end points. Environ. Sci. Technol. 50, 453–461.
Liang, C.-S., Duan, F.-K., He, K.-B., Ma, Y.-L., 2016. Review on recent progress in observa-
tions, source identifications and countermeasures of PM2.5. Environ. Int. 86,
150–170.
Liang, F., Zhang, G., Tan, M., Yan, C., Li, X., Li, Y., Li, Y., Zhang, Y., Shan, Z., 2010. Lead in
children's blood is mainly caused by coal-fired ash after phasing out of leaded gaso-
line in Shanghai. Environ. Sci. Technol. 44, 4760–4765.
Lippmann, M., Yeates, D., Albert, R., 1980. Deposition, retention, and clearance of inhaled
particles. Br. J. Ind. Med. 37, 337–362.
Marcazzan, G.M., Vaccaro, S., Valli, G., Vecchi, R., 2001. Characterisation of PM10 and PM2.5
particulate matter in the ambient air of Milan (Italy). Atmos. Environ. 35, 4639–4650.
Pakkanen, T.A., Loukkola, K., Korhonen, C.H., Aurela, M., Mäkelä, T., Hillamo, R.E., Aarnio,
P., Koskentalo, T., Kousa, A., Maenhaut, W., 2001. Sources and chemical composition
of atmospheric fine and coarse particles in the Helsinki area. Atmos. Environ. 35,
5381–5391.
Pan, L., Tang, H., Liu, X., 2015. Review and revelation of air quality assurance work during
the Nanjing Youth Olympic Games. Environ. Monit. Forewarning 7, 1–3.
Rasmussen, P.E., Beauchemin, S., Chénier, M., Levesque, C., MacLean, L.C., Marro, L., Jones-
Otazo, H., Petrovic, S., McDonald, L.T., Gardner, H.D., 2011. Canadian house dust
study: lead bioaccessibility and speciation. Environ. Sci. Technol. 45, 4959–4965.
Remoundaki, E., Kassomenos, P., Mantas, E., Mihalopoulos, N., Tsezos, M., 2013. Composi-
tion and mass closure of PM2.5 in urban environment (Athens, Greece). Aerosol Air
Qual. Res. 13, 72–82.
75
Richmond-Bryant, J., Meng, Q., Davis, A., Cohen, J., Lu, S.-E., Svendsgaard, D., Brown, J.S.,
Tuttle, L., Hubbard, H., Rice, J., 2014. The influence of declining air lead levels on
blood lead–air lead slope factors in children. Environ. Health Perspect.
Schleicher, N., Norra, S., Chen, Y., Chai, F., Wang, S., 2012. Efficiency of mitigation mea-
sures to reduce particulate air pollution—a case study during the Olympic Summer
Games 2008 in Beijing, China. Sci. Total Environ. 427–428, 146–158.
Shah, P., Strezov, V., Nelson, P.F., 2009. X-ray absorption near edge structure spectrometry
study of nickel and lead speciation in coals and coal combustion products. Energy
Fuel 23, 1518–1525.
Shen, G.F., Yuan, S.Y., Xie, Y.N., Xia, S.J., Li, L., Yao, Y.K., Qiao, Y.Z., Zhang, J., Zhao, Q.Y., Ding,
A.J., 2014. Ambient levels and temporal variations of PM2.5 and PM10 at a residential
site in the mega-city, Nanjing, in the western Yangtze River Delta, China. J. Environ.
Sci. Health A 49, 171–178.
Smith, E., Kempson, I.M., Juhasz, A.L., Weber, J., Rofe, A., Gancarz, D., Naidu, R., McLaren,
R.G., Grafe, M., 2011. In vivo-in vitro and XANES spectroscopy assessments of lead
bioavailability in contaminated periurban soils. Environ. Sci. Technol. 45, 6145–6152.
Sommers, L., Lindsay, W., 1979. Effect of pH and redox on predicted heavy metal-chelate
equilibria in soils. Soil Sci. Soc. Am. J. 43, 39–47.
Stebounova, L.V., Adamcakova-Dodd, A., Kim, J.S., Park, H., O'Shaughnessy, P.T., Grassian,
V.H., Thorne, P.S., 2011. Nanosilver induces minimal lung toxicity or inflammation
in a subacute murine inhalation model. Part. Fibre Toxicol. 8, 5.
Sun, Y., Zhuang, G., Zhang, W., Wang, Y., Zhuang, Y., 2006. Characteristics and sources of
lead pollution after phasing out leaded gasoline in Beijing. Atmos. Environ. 40,
2973–2985.
Tan, M., Zhang, G., Li, X., Zhang, Y., Yue, W., Chen, J., Wang, Y., Li, A., Li, Y., Zhang, Y., 2006.
Comprehensive study of lead pollution in Shanghai by multiple techniques. Anal.
Chem. 78, 8044–8050.
Tao, J., Zhang, L., Zhang, Z., Huang, R., Wu, Y., Zhang, R., Cao, J., Zhang, Y., 2015. Control of
PM2.5 in Guangzhou during the 16th Asian Games period: implication for hazy
weather prevention. Sci. Total Environ. 508, 57–66.
USEPA, 2007. Review of the National Ambient Air Quality Standards for Lead (EPA-452/R-
07-013).
USEPA, 2013. Test Methods for Evaluating Solid Wastes SW-846 EPA Method 6020 B: In-
organic Elements by ICP-MS. USEPA, Washington, DC.
Wang, W., Primbs, T., Tao, S., Simonich, S.L.M., 2009. Atmospheric particulate matter pol-
lution during the 2008 Beijing Olympics. Environ. Sci. Technol. 43, 5314–5320.
Widory, D., Liu, X., Dong, S., 2010. Isotopes as tracers of sources of lead and strontium in
aerosols (TSP & PM2.5) in Beijing. Atmos. Environ. 44, 3679–3687.
Wiseman, C.L.S., 2015. Analytical methods for assessing metal bioaccessibility in airborne
particulate matter: a scoping review. Anal. Chim. Acta 877, 9–18.
Wiseman, C.L., Zereini, F., 2014. Characterizing metal (loid) solubility in airborne PM10,
PM2.5 and PM1 in Frankfurt, Germany using simulated lung fluids. Atmos. Environ.
89, 282–289.
Wragg, J., Klinck, B., 2007. The bioaccessibility of lead from Welsh mine waste using a re-
spiratory uptake test. J. Environ. Sci. Health A 42, 1223–1231.
Zereini, F., Wiseman, C.L., Püttmann, W., 2012. In vitro investigations of platinum, palladi-
um, and rhodium mobility in urban airborne particulate matter (PM10, PM2.5, and
PM1) using simulated lung fluids. Environ. Sci. Technol. 46, 10326–10333.