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Characterization of metal aerosols in PM10 from urban, industrial, and Asian

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Article in Environmental Monitoring and Assessment · January 2009

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Environ Monit Assess (2010) 160:289–300
DOI 10.1007/s10661-008-0695-6
Characterization of metal aerosols in PM10 from urban,
industrial, and Asian Dust sources
Kihong Park · Hung Duy Dam
Received: 2 August 2008 / Accepted: 20 November 2008 / Published online: 23 December 2008
© Springer Science + Business Media B.V. 2008
Abstract Metallic elements (As, Be, Ca, Cd,
Co, Cr, Fe, K, Mn, Ni, Pb, Sb, Se, and Zn)
in PM10 aerosols were determined at urban
and industrial sites, which are affected by traffic
and residential sources, metallurgical activity, and
petrochemical and steel works. The effect of the
long-range transported Asian Dust on the metal
content of aerosols was also examined. At the
urban sampling site, concentrations of As, Cd,
Pb, Se, and Zn were assigned to road traffic and
combustion sources, Ca and Fe to soil dust sources
from long-range transported Asian Dusts, and Cr
and Ni to metallurgical sources transported from
the nearby industrial complex, based on Principal
Component Analysis (PCA). Enhanced Cr and Ni
concentrations at the metallurgical industrial site
suggest that local emissions from metal-assembly
facilities and manufacture of alloys contributed
to elevated levels of those metals. We also ob-
served that petrochemical activities contributed to
increased levels of Sb and Zn. When Asian Dust
events occurred, Ca, Fe, K, and Zn concentrations
dramatically increased compared to values with-
out the Asian Dust. Two different types of Asian
K. Park (B) · H. D. Dam
Research Center for Biomolecular Nanotechnology,
Department of Environmental Science
and Engineering, Gwangju Institute of Science
and Technology, Gwangju, South Korea
e-mail: kpark@gist.ac.kr
Dust events were observed. For the Asian Dust
event 1 (4/1/2007), the Fe and K concentrations
were much higher by a factor of 2–3 than those for
the Asian Dust event 2 (3/2/2008), while As, Mn,
and Zn concentrations were significantly higher
on the Asian Dust event 2. Backward trajectory
analysis showed that for the Asian Dust event 2,
the air mass had passed over the heavily indus-
trialized zones in China during long-range trans-
port to the current sampling site, suggesting that
the As, Mn, and Zn may have originated from
industrial sources.
Keywords Metal · Aerosol · Asian Dust · PM10
Introduction
Particulate matter (PM) with an aerodynamic
diameter less than 10 μm (PM10) in the am-
bient atmosphere affect earth’s radiation bud-
get (Intergovernmental Panel on Climate Change
2007), cloud formation, visibility impairment
(NRC 1993), and human health (Peters et al.
1997; Oberdörster 2000). Although metal-bearing
aerosols constitute a small fraction of the PM
mass, the exceeding concentration and/or long-
term exposure to metals could cause severe toxic
effects on human health. Thus, measurement of
metal concentration levels in inhalable particles is
290
important in determining their potential impacts
on human health (Allen et al. 2001).
Metal-bearing aerosols in the ambient at-
mosphere are produced by various anthropogenic
and natural sources. Combustion of fossil fuels
and wood, exhaust emission from vehicles, indus-
trial activities, energy production, construction,
and waste incineration are known to be anthro-
pogenic sources, while volcanic activity, wind-
eroded soil dusts (e.g., Asian Dust), forest fires,
and sea salt spray may contribute to natural metal-
bearing aerosols (Nriagu 1979; Allen et al. 2001;
Bilos et al. 2001; Wang et al. 2005). It was reported
that industrial metallurgic processes led to the
increased concentrations of As, Cd, Cu, Ni, and
Zn metals (Bilos et al. 2001; Wang et al. 2005).
Ni and Zn can also be produced by vehicle ex-
hausts and fuel oil combustion (Allen et al. 2001;
Espinosa et al. 2001; Mugica et al. 2002; Lopez
et al. 2005; Wang et al. 2005). Fe and Mn can be
emitted from steel industrial processes and from
Earth’s crust (Mugica et al. 2002; Lopez et al.
2005; Wang et al. 2005). K was reported to be
produced by biomass burning (Gatari et al. 2005;
Wang et al. 2005). Nonferrous metal smelters and
coal-burning can contribute to the increase of As
concentration level in ambient aerosols (Gatari
et al. 2005; Senlin et al. 2007). Thus, those previ-
ous studies suggested that various anthropogenic
sources contributed to metal-baring aerosols, and
characteristics and concentration levels of met-
als varied with spatial and temporal factors
(Kim 2004).
In order to identify emission sources for metals
in atmospheric aerosols and to better understand
their transport and deposition, it is necessary to
characterize metal emissions from specific local
sources and long-range transported metals. Thus,
the goal of this study is to determine metal emis-
sions from Asian Dusts, traffic and residential
source, metallurgical industry, and petrochemical
and steel manufacturing industry. To do this, 14
metals (As, Be, Ca, Cd, Co, Cr, Fe, K, Mn, Ni,
Pb, Sb, Se, and Zn) in PM10 were determined
at three sites [an urban Gwangju (Korea) site
characterized by traffic and residential sources, an
industrial complex site near Hanam (Korea) that
mainly consists of metallurgical activity, and a site
near Yeosu (Korea) that is affected by petrochem-
Environ Monit Assess (2010) 160:289–300
ical and steel works]. The effect of the long-range
transported Asian Dust on metal content and
the long-term variation of metal concentration
were examined at the Gwangju site. Backward
trajectory analysis, Principal Component Analysis
(PCA), and Enrichment Factor (EF) calculations
for metal concentrations were carried out to de-
termine the relationship among metals and to in-
vestigate their sources.
Experimental
Locations of sampling sites are shown in Fig. 1.
The urban Gwangju site is located ∼7.6 km north
of the downtown Gwangju city hall and is influ-
enced by traffic from a nearby highway (∼1.5 km
away from the site), residential heating from res-
idential/commercial areas (∼0.6 km away from
the site), and biomass burning from agricultural
areas (∼0.8 km away from the site). The Hanam
sampling site is located in the middle of Hanam
industrial complex which consists of 60% metal-
lurgical activities, 18% chemical production, and
23% other activities. The Hanam site is located
∼4.2 km southwest from the Gwangju sampling
site. The coastal Yeosu sampling site is located
near the south sea of Korea and is affected by the
largest petrochemical industrial complex and steel
works in Korea. The Yeous site is located ∼90 km
southeast from the Gwangju site.
PM10 samples were collected during the sam-
pling periods of April 2, 2007–April 27, 2007,
August 2, 2007–August 20, 2007, November 20,
2007–December 3, 2007, and January 16, 2008–
February 2, 2008 at the Gwangju site, April
3, 2007–April 27, 2007 at the Hanam site, and
January 16, 2008–February 2, 2008 at the Yeosu
site. Teflon filters with 37 mm diameter and
2 μm pore size (Teflo, Gelman Laboratory, USA)
with particle collection efficiency of 99.7% for
0.3 μm-sized particles were used for collecting PM
samples through a PM10 inlet (Baron and Willeke
2001; Balasubramanian and Qian 2004). Volumet-
ric flow rates were checked before and after the
sampling period (∼24 h) and did not significantly
deviate from the initial value. The filters were
weighed before and after the sampling using a
Environ Monit Assess (2010) 160:289–300 291

Agricultural areas
Gwangju
sampling site
Hanam industrial
Residential/
complex
Hanam commercial areas
sampling site Highway

Downtown

Japan
China
Korea

Hwangge um
industrial
complex Steel works

Yulchon
industrial
complex
Yeosu Industrial
complex Yeosu
sampling site

South sea
Residential/
commercial areas

Fig. 1 Location of sampling sites (Gwangju, Hanam, and Yeosu) with local sources examined in this study

microbalance (MC-5, Sartorius, USA) with 1 μg
sensitivity to obtain the net mass of collected
particles. The filters were equilibrated in the des-
iccators with stabilized temperature (22–23◦ C)
and relative humidity (30–40%) for at least 24 h
before and after the actual weighing. We fol-
lowed the analytical procedure for determina-
tion of trace metals on filters as set forth by
the Standard Operating Procedure in the EPA
Work Assignment (EPA 2005). The filters were
extracted with 20 ml 4% concentrated nitric acid
in Teflon centrifuge tubes by sonication for 3 h
setting in a heated 69◦ C water bath. After cool-
ing to room temperature for 30 min, the extracts
were diluted with deionized water to obtain 50 ml
final sample solutions and then stored in refrig-
erator before analysis. Samples were filtered by
Whatman 541 filter paper prior to inductively
coupled plasma-mass spectrometry (ICP-MS) and
atomic absorption spectroscopy (AAS) analysis.
Quantitative metal analysis was carried out by
external calibration standards at concentration
levels close to those of the samples during the
ICP-MS and AAS analysis. A drift correction
was done by running a set of external calibration
standards before and after the ICP-MS and AAS
analyses of the samples. The reagent and filter
blanks were also analyzed using the same proce-
dure as above.
To track sources of long-range transported
metals, air mass backward trajectories were cal-
culated using the HYSPLIT model developed by
National Oceanic and Atmospheric Administra-
tion (NOAA; Draxler and Rolph 2003). A 3-day
292 Environ Monit Assess (2010) 160:289–300

backward trajectory ending at the Gwangju site
at the height of 500 m AGL (above ground level)
was used in this study.
Results and discussion
Daily variation of PM10 mass concentration dur-
ing the four different sampling periods at the
Gwangju sampling site is shown in Fig. 2. Asian
dusts transported from China, which occasionally
occur in spring season over the Korean penin-
sula (Choi et al. 2001; Kim et al. 2002; Senlin
et al. 2007), were observed on April 1, 2007 and
March 2, 2008, having PM10 mass concentrations
of 723.6 and 326.5 ug/m3 , respectively, which are
much higher than the annual average of PM10
(47.6 ug/m3 ). As shown, the PM10 is the highest
in spring, while it is the lowest in summer. Long-
range transported particles (e.g., Asian Dust) and
fugitive dust occurred more often in spring sub-
stantially contributed to the increased PM10. A
previous study showed that the number of ultra-
fine particles (<100 nm) substantially increased in
summer in this area due to a strong photochemical
activity (Park et al. 2008). Our data suggest that
even when ultrafine particles exist in large number
in summer, their contribution to PM10 mass is not
substantial.
Average metal concentrations (As, Be, Ca, Cd,
Cr, Fe, K, Mn, Ni, Pb, Sb, Se, and Zn) in PM10
during the whole sampling period at Gwangju site
excluding Asian Dust events are shown in Fig. 3.
The most abundant elements in the PM10 are Ca
(1398 ng/m3 ), K (777 ng/m3 ), Fe (687 ng/m3 ), and
Zn (176 ng/m3 ) followed by Pb, Mn, Sb, Cr, and

Gwangju Korea air quality guideline

800

700
Asian dust event 1
PM10 mass concentration (µg/m3)

600

500

400
Asian dust event 2

300

200

100

0
4/1/2007
4/3/2007
4/4/2007
4/5/2007
4/6/2007
4/10/2007
4/11/2007
4/12/2007
4/13/2007
4/17/2007
4/18/2007
4/19/2007
4/20/2007
4/24/2007
4/25/2007
4/26/2007
4/27/2007
8/2/2007
8/5/2007
8/8/2007
8/12/2007
8/17/2007
8/20/2007
11/20/2007
11/21/2007
11/22/2007
11/23/2007
11/27/2007
11/29/2007
11/30/2007
12/1/2007
12/2/2007
12/3/2007
1/16/2008
1/17/2008
1/18/2008
1/19/2008
1/20/2008
1/21/2008
1/24/2008
1/25/2008
1/26/2008
1/31/2008
2/1/2008
2/2/2008
3/2/2008

Date

Fig. 2 PM10 concentrations at the urban Gwangju site by date, during the four sampling periods (April 2, 2007–April 27,
2007, August 2, 2007–August 20, 2007, November, 20, 2007–December 3, 2007, and January 16, 2008–February, 2, 2008)
Environ Monit Assess (2010) 160:289–300 293

Fig. 3 Average metal

concentrations in PM10 at
the urban Gwangju site
excluding Asian Dust
events

Ni in 7–62 ng/m3 . Concentrations of Be, Cd, Co,
and Se are below 5 ng/m3 . Average metal concen-
trations at Gwangju, Hanam, and Yeosu sampling
sites are summarized in Table 1 with guideline
values for specific metals. The As concentration
level at Hanam and Yeosu exceeded the PM10
annual average guideline (6 ng/m3 ; WHO 2000;
UK 2007), and the Cr and Ni at Hanam exceeded
the PM10 annual average guideline (20 ng/m3 ;
UK 2007). More comparison among sites will be
discussed later.
To investigate the effect of the Asian dusts on
metals, we compared metal concentrations (As,
Ca, Fe, K, Mn, and Zn) at Gwangju site with
and without the Asian Dust as shown in Fig. 4.
It shows that when the Asian dusts occurred,
Ca, Fe, K, and Zn concentrations dramatically
increased compared to average values without the

Table 1 Average metal Measured metal concentration (ng/m3 ) Guideline metal concentration (ng/m3 )
concentration in
Gwangju, Hanam, and Gwangju Hanam Yeosu Guideline based on Reference
Yeosu with guidelines for annual average (ng/m3 ) source
specific metals As 5.5 8.9 10.0 6 WHOa , UKb
Be 0.1 – 0.1 – –
Ca 1,398.1 4,530.9 2,791.4 – –
Cd 1.5 2.0 0.5 5 UKb
a WHO (World Health Co 0.5 1.2 0.6 5 ATSDRc
Organization) Air quality Cr 9.5 51.2 12.5 20 ATSDRc
guidelines for Europe Fe 687.2 2,118.0 958.8 – –
(WHO 2000) K 777.0 2,588.5 2,809.6 – –
b UK (United Kingdom)
Mn 31.7 44.1 16.0 150 WHOa
Air Quality standards Ni 7.3 32.8 5.5 20 UKb
(UK 2007) Pb 61.5 146.0 146.8 500 WHOa
c ATSDR (Agency for
Sb 11.1 14.1 34.1 – –
Toxic Substances and
Se 4.7 9.7 2.3 – –
Disease Registry)
(ATSDR 2007) Zn 176.0 484.7 544.0 – –
294
Fig. 4 Comparison of
metal (Ca, Fe, K, Mn, and
Zn) concentrations in
PM10 at Gwangju site on
Asian Dust events (April
2, 2007 and March 2,
2008) and average values
on non-Asian Dust events
Asian Dust. We also found that two Asian Dust
events (i.e., event 1 on April 1, 2007 and event
2 on March 2, 2008) differ in terms of specific
metal concentrations. On the Asian Dust event
1 (April 1, 2007), the Fe and K concentrations
were much higher by a factor of 2–3 than those
on the Asian Dust event 2 (March 2, 2008), while
As, Mn, and Zn concentrations significantly in-
creased on the Asian Dust event 2. To investi-
gate the reason for this, we used the HYSPLIT
model and examined the two air mass backward
trajectories for the time periods when the above
Asian Dust events occurred, each time starting at
the Gwangju site at an altitude of 500 m. For the
Asian Dust event 1, the air mass directly arrived
at our sampling site from the Gobi desert with-
out passing over the heavily industrialized zones
in China as shown in Fig. 5a, while when the
Asian Dust event 2 occurred, as shown in Fig. 5b,
the air mass originated from the Ordos desert
and passed over heavily industrialized zones in
China before arriving at our sampling site. Thus,
increased levels of As and Zn on the Asian Dust
event 2 might be related to mixing of dusts and
anthropogenic metals originated from the indus-
trialized zones in China during their long-range
transport.
Environ Monit Assess (2010) 160:289–300
Figure 6 compares Cr, Fe, Ni, Pb, and Zn
concentrations measured at the Hanam industrial
complex site and at the urban Gwangju site, which
had the highest difference between any two sites.
The higher Cr, Ni, Pb, and Zn concentrations at
the Hanam site compared to those at the Gwangju
site suggest that local emissions from the indus-
trial complex at Hanam contributed to elevated
levels of those metals. The Hanam industrial com-
plex includes many kinds of metal-assembly fa-
cilities, manufacture of alloys, and combustion
of fuels. When the correlation coefficient among
metals at the Hanam site was calculated, Cr and
Ni had a high correlation coefficient of 0.93, sug-
gesting that Cr and Ni have a similar source. We
also compared metal concentrations measured at
the Yeosu site with those at the Gwangju site
as shown in Fig. 7. Ca, K, Pb, Sb, and Zn con-
centrations are significantly higher at Yeosu than
Gwangju by a factor of 1.3–3.1. The site located
in Yeosu is close to one of the most concentrated
industrial areas in Korea including Yeosu petro-
chemical complex, Yulchon industrial complex,
and Gwangyang steel as shown in Fig. 1. The
petrochemical activities might contribute to the
increased levels of Sb and Zn (ATSDR 2007). Our
data suggest that specific metals were significantly
Environ Monit Assess (2010) 160:289–300 295

(a) (b)
Fig. 5 Air mass backward trajectories ending at the Gwangju site at an altitude of 500 m using the HYSPLIT model on
a Asian Dust event 1 (Arpil 1, 2007) and b Asian Dust event 2 (March 2, 2008)

Fig. 6 Comparison of
metal concentrations
(Cr, Fe, Ni, Pb, and Zn)
at Hanam industrial site
and urban Gwangju site;
these metals had the
highest difference in
concentration between
the two sites
296 Environ Monit Assess (2010) 160:289–300

Fig. 7 Comparison of
metal concentrations
(Ca, K, Pb, Sb, and Zn)
at Yeosu industrial site
and urban Gwangju site;
these metals had the
highest difference in
concentration between
the two sites

enhanced at Hanam (Cr, Ni, Pb, Zn) and Yeosu
(K, Sb, Zn) sites mainly due to local industrial
activities in those areas.
Enrichment factors (EFs) of metals (i.e., rel-
ative to the earth’s crustal abundances), can be
used to evaluate the effects of anthropogenic and
natural sources on the metal content of aerosols
(Bilos et al. 2001; Balasubramanian and Qian
2004; Lopez et al. 2005; Wang et al. 2005; Kim
and Jo 2006). The EF for each metal (X) can be

Fig. 8 Average
enrichment factors (EF)
for metals in PM10 at
Gwangju site with
Asian Dust (AD) and
non-Asian Dust
(non-AD) events, Hanam
site, and Yeosu site
Environ Monit Assess (2010) 160:289–300
Fig. 9 Principal
Component Analysis
(PCA) for PM10 metals
at Gwangju site
calculated as given by EF = [X/Fe]PM /[X/Fe]crust
where the Fe was used as a reference crustal
metal. The earth’s crustal mean abundances of
each element given by Taylor (1964) were used to
calculate the EF. The EF should be much higher
than unity if the source of metal comes from an an-
thropogenic origin. Since there is a variation in the
297
crustal abundance of metals from site to site, the
EF should be higher than 10 to be considered
as anthropogenic origin (Bilos et al. 2001; Choi
et al. 2001; Balasubramanian and Qian 2004).
Figure 8 shows the average EFs for metals in
PM10 at Gwangju site with Asian Dust (AD)
and non-Asian Dust (non-AD) events, Hanam
298 Environ Monit Assess (2010) 160:289–300

site, and Yeosu site. The EF for metals during

the Asian Dust event was found to be much
lower than others, confirming that a natural source
(i.e., soil dusts) significantly contributed to those
metals. At other sites, As, Cd, Pb, Sb, Se, and
Zn have higher EF (>100) than others, suggesting
that noncrustal sources contributed a substantial
fraction of these elements to the aerosol particles.
Especially, the EFs of Sb and Zn at the Yeosu site,
and Cr and Ni at the Hanam site are much higher
than values at other sites, which are consistent
with results from comparison of metals among
sites discussed in the previous section.
We also conducted principal component analy-
sis (PCA) which can be used to identify patterns
of correlations among metals by reducing a large
data set into a small number of principal com-
ponents (PCs; Berg et al. 1995; Pina et al. 2000;
Allen et al. 2001; Choi et al. 2001; Hien et al.
2001; Lopez et al. 2005; Kim and Jo 2006; John
et al. 2007). We used a statistical software (SPSS
V.15) with Varimax (orthogonal) rotation to de-
termine principal components having an eigen-
value larger than 1. With the PCA method, we
are able to infer whether metals come from a
similar source or not. At the Gwangju site, As,
Cd, Pb, Se, and Zn have high values in principal
component 1 (PC1), Ca and Fe have high values
in PC2, and Cr and Ni have high values in PC3
as shown in Fig. 9. The PC1 may be attributed
to road traffic and combustion sources, the PC2
to soil dust sources from long-range transported
Asian Dusts, and the PC3 to metallurgical sources
transported from Hanam industrial complex. Data
suggest that the Gwangju site is usually affected
by multiple sources including traffic from nearby
highways, residential heating, and the Hanam in-
dustrial complex. We also observed that with the Fig. 10 Cr and Ni concentrations in relation with wind
southwestern wind, which typically passed over direction at Gwangju site during the sampling period
the Hanam industrial complex in reaching the
Gwangju site, concentrations of Cr and Ni in-
creased as shown in Fig. 10. The PCA analysis
for metals at the Hanam and Yeous sites is also into PC2, and Cr, Fe, and Sb into PC3. Different
summarized in Table 2. At these sites, Ca and kinds of manufacture of alloys, metal-assembly
Fe were not grouped into a similar source (i.e., facilities, and combustion of fuels at Hanam site
Asian Dust source). This occurred because no might group metals into those distinct PCs. At the
Asian Dust event happened during the sampling Yeosu site, we identified two components as Ca,
period at both sites. At the Hanam site, K, Mn, Cd, Fe, K, Ni, Pb, and Zn for PC1, and As and Cr
and Pb were grouped into PC1, Ca, Cd, Se, and Zn for PC2.
Environ Monit Assess (2010) 160:289–300 299

Table 2 Principal Component Analysis (PCA) for PM10 metals at (a) Gwangju, (b) Hanam, and (c) Yeosu sampling sites
(only values exceeding 0.6 are shown for clarity)
Principal component As Ca Cd Co Cr Fe K Mn Ni Pb Sb Se Zn Variance
Gwangju
PC1 0.73 0.94 0.71 0.64 0.64 43.24
PC2 0.84 0.84 0.85 17.55
PC3 0.92 0.93 14.33
Hanam
PC1 0.82 0.89 0.84 38.52
PC2 0.67 0.68 0.84 0.73 20.73
PC3 0.67 0.93 0.70 13.19
Yeosu
PC1 0.99 0.98 0.97 0.98 0.99 0.95 0.82 78.01
PC2 0.90 0.99 21.98

Conclusions For that event, the backward trajectory analysis

In order to identify emission sources for metals
in atmospheric aerosols and to better understand
their transport and deposition, we characterized
metal emissions from specific local sources and
long-range transported metals. Comparison of the
metal content (As, Be, Ca, Cd, Co, Cr, Fe, K,
Mn, Ni, Pb, Sb, Se, and Zn) in PM10 aerosols
was conducted for three sites (Gwangju, Hanam,
and Yeosu in Korea) that are affected by differ-
ent local sources. Data showed that at the ur-
ban Gwangju site the levels of As, Cd, Pb, Se,
and Zn in PM10 can be attributed to road traffic
and combustion sources, Ca and Fe to soil dust
sources from long-range transported Asian Dusts,
and Cr and Ni to metallurgical sources from the
Hanam industrial complex. Higher Cr and Ni con-
centrations at the Hanam site than those at the
Gwangju site suggest that local emissions from
metal-assembly facilities and manufacture of al-
loys contributed to elevated levels of those metals.
At the Yeosu site, data showed that petrochemical
activities contributed to the increased levels of
Sb and Zn. The effect of long-range transported
Asian Dust on the metal content was also exam-
ined. When Asian Dust events occurred at the
Gwangju site, Ca, Fe, K, and Zn concentrations
significantly increased compared to ones without
the Asian Dust. Two different types of Asian
Dust events were observed during the sampling
period. For the Asian Dust event 2 that occurred
on March 2, 2008, As, Mn, and Zn concentra-
tions in the PM10 were significantly enhanced.
showed that the air mass passed over heavily in-
dustrialized zones in China during the long-range
transport, before arriving at the Gwangju site, sug-
gesting that natural dust-originated metals were
mixed with those originating from the industrial
sources.
Acknowledgements The research is supported by
Korea Research Foundation Grant (KRF-2007-331-
D00222) and Korea Science and Engineering Foundation
(KOSEF; no. R01-2007-000-10391-0).
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