J Atmos Chem (2011) 68:281–298

DOI 10.1007/s10874-012-9225-6

Long-term measurements of atmospheric PM2.5

and its chemical composition in rural Korea

Young-Ji Han & Seong-Rak Kim & Jin-Hee Jung

Received: 14 December 2011 / Accepted: 3 April 2012 /

Published online: 21 April 2012
# Springer Science+Business Media B.V. 2012

Abstract Long-term measurements of ambient particulate matter less than 2.5 μm in

diameter (PM2.5) and its chemical compositions were performed at a rural site in Korea
from December 2005 to August 2009. The average PM2.5 concentration was 31 μg m−3 for
the whole sampling period, and showed a slightly downward annual trend. The major
components of PM2.5 were organic carbon, SO42−, NO3−, and NH4+, which accounted for
55 % of total PM2.5 mass on average. For the top 10 % of PM2.5 samples, anionic
constituents and trace elements clearly increased while carbonaceous constituents and
NH4+ remained relatively constant. Both Asian dust and fog events clearly increased PM2.5
concentrations, but affected its chemical composition differently. While trace elements signif-
icantly increased during Asian dust events, NO3−, NH4+ and Cl were dramatically enhanced
during fog events due to the formation of saturated or supersaturated salt solution. The back-
trajectory based model, PSCF (Potential Source Contribution Function) identified the major
industrial areas in Eastern China as the possible source areas for the high PM2.5 concentrations
at the sampling site. Using factor analysis, soil, combustion processes, non-metal manufacture,
and secondary PM2.5 sources accounted for 77 % of the total explained variance.

Keywords PM2.5 . Chemical composition . Asian dust . Fog . Factor analysis . PSCF

1 Introduction

Fine particles, defined as particles less than 2.5 μm in diameter (PM2.5), have been of great
interest in many countries due to their significant adverse effects on human health and
visibility. They frequently act as cloud condensation nuclei (CCN) that can disturb the heat
balance of Earth, causing climate change (IPCC 2006). The size of PM2.5 generally follows

Y.-J. Han (*) : S.-R. Kim

Department of Environmental Science, College of Natural Science, Kangwon National University,
192-1 Hyoja-2-dong, Chuncheon, Kangwon-do, South Korea 200-701
e-mail: youngji@kangwon.ac.kr

J.-H. Jung
Division of Strategic Assessment, Integrated Environmental Research Group,
Korea Environment Institute, 290 Jinheungno, Eunpyeog-gu, Seoul, South Korea 122-706
282 J Atmos Chem (2011) 68:281–298

four modes—ultrafine (less than 0.01 μm), Aitken (0.01∼0.1 μm), accumulation
(0.1∼1.0 μm), and coarse (larger than 1.0 μm). The accumulation mode usually accounts
for significant fraction of the PM2.5 mass, and is formed from the coagulation of particles in
nuclei mode and from condensation of vapors onto existing particles, causing them to grow
to this size range (Seinfeld and Pandis 2006). On the other hand, the coarse particles are
mainly produced by mechanical processes from both natural and anthropogenic sources.
PM2.5 is a complex of primary aerosols emitted from both natural sources (such as
windborne dust, sea spray, and volcanoes) and anthropogenic sources (such as fuel com-
bustion, industrial processes, non-industrial sources, and transportation) and secondary
aerosols formed in the atmosphere by gas-to-particle conversion processes. Once particles
are emitted into the air, they change in chemical composition, mass, and size. In ambient air,
the major constituents of PM2.5 include ionic compounds (SO42−, NO3−, NH4+), elemental
carbon, metal compounds, a large variety of organic compounds, and other trace elements.
According to the literatures not only particle size and surface area but also chemical
composition determine the health risks, and particles from combustion sources, particularly
engine exhaust particles, are associated with greater health risks than those from natural
sources (Forsberg et al. 2005; Hong et al. 2010). Therefore, identification of the chemical
composition and potential sources of PM2.5 is critical to establishing appropriate reduction
strategies. The atmospheric lifetime of PM2.5 varies from a few days to a few weeks, meaning
that long-range transport can occur before deposition.
In Korea, PM2.5 concentration in ambient air has increased or been relatively consistent
(Kim et al. 2007; Han et al. 2008; Kim et al. 2011) despite many efforts (including industrial
transfer and fuel conversion) to improve air quality, while the concentrations of other typical
pollutants such as sulfur dioxide and carbon monoxide have steadily decreased over the past
few decades (Ministry of Environment, http://stat.me.go.kr/nesis). The long-range transport
of aerosols originating from China has been assumed to be an important cause of the
consistent PM2.5 concentrations in Korea (Kim et al. 2007; Han et al. 2008; Jeong et al.
2011). With industry developing at a rapid rate in China, air pollution has certainly become a
serious problem in the country and its neighbors, including Korea and Japan. Yet, another
important cause of transboundary pollution is the Asian dust storm (ADS), which often occurs
during the spring. ADS events originating from the Chinese or Mongolian desert areas
significantly enhance ambient aerosol concentrations in Korea, and are associated with adverse
health effects (Chen et al. 2004; Hong et al. 2010).
Due to the significant effect of PM2.5 on human health and air quality, most developed
countries have established strategies and policies to reduce PM2.5 concentrations. However,
Korea only regulates emissions of PM10 as fine particles, and air quality standards for PM2.5
have not been set. Therefore, studies reporting long-term monitoring data for PM2.5 are
lacking, and most of previous studies have focused on urban and industrial areas (Kim et al.
2007; Lee et al. 2008; Park et al. 2008; Nguyen and Lee 2010). However, the possible
sources that affect atmospheric PM2.5 concentration probably differ between urban and rural
areas and, consequently, the physical and chemical characteristics of PM2.5 in rural areas
may also differ from those in urban and industrial areas.
In this study, we collected PM2.5 samples and analyzed their chemical constituents including
ionic, carbonaceous, and other trace metal compounds in a rural area (Chuncheon) in Korea for
approximately 4 years from 2005 to 2009. Together with the overall characteristics of PM2.5, we
identified “high concentration events” when daily PM2.5 concentration reached the top 10 %,
and thoroughly examined their characteristics. In addition, the major sources that affected PM2.5
concentration at the sampling site were identified using back-trajectory based model (PSCF)
and factor analysis.
J Atmos Chem (2011) 68:281–298 283

2 Material and methods

2.1 Sampling site

The concentrations of PM2.5 and its chemical constituents were measured in a rural area
(Chuncheon) in Korea from December 2005 to August 2009. Chuncheon is a relatively
small town surrounded by mountains which limit the transport of locally emitted air
pollutants. The population of the city is 256,455, which is approximately 0.5 % of the
national population. There are no large industries in Chuncheon, and according to the
National Emissions Inventory of Korea, PM10 emissions were 391,263 t in 2007, represent-
ing only 0.4 % of the national total for PM10 emissions (Ministry of Environment, 2008).
However, it is located approximately 100 km northeast of urban (Seoul) and 150 km
northeast of industrial (Incheon) areas; therefore, air pollutants emitted in these areas can
be transported to Chuncheon when there is a westerly wind (Fig. 1). The sampling site was
the roof of the four-storey Kangwon National University Natural Sciences building. All
samples were collected every third day for 24 h.

2.2 Sampling and analysis

Sampling for PM2.5 followed the procedures outlined in the US EPA Compendium Method
IO-4.2 (U.S. EPA 1999). For PM2.5 mass monitoring, 37-mm Teflon filter (Pall Life Sciences,
Teflo) was placed in a clean Teflon filter pack (TFP) (URG) after Cyclone (URG) at a flow

Fig. 1 The sampling location (Chuncheon) with adjacent urban (Seoul) and industrial (Incheon) areas. Stars
indicate the major industrial areas of China
284 J Atmos Chem (2011) 68:281–298

rate of 16.7 Lmin−1. Teflon filters were stored in controlled conditions of temperature and
relative humidity for at least 24 h before and after sampling, and then weighed at least twice
using an analytical balance (Sartorius CP225D, readability 0 10−5 g). The filters were then
stored in a freezer before analysis for trace elements. To collect ionic compounds of PM2.5, a
three-stage TFP (47 mm) was used at a flow rate of 10 Lmin−1 after ionic gases (SO2, HNO3,
HNO2, and NH3) were first removed by denuders to prevent sampling artifacts. Denuders
were coated with a mixture of 50 mL ethanol, 1 g Na2CO3, 1 g of glycerol and 50 mL of
deionized water for acidic gases, and with a mixture of 100 mL of ethanol, 1 g of citric acid,
and 1 g of glycerol for basic gases. All ionic components of PM2.5 were first collected on a
Zeflour filter (Pall Life Sciences, Zeflour), and HNO3 and NH3 volatilized from the Zeflour
filter were collected on nylon (Pall Life Sciences, Nylarsorb) and paper (Whatman Interna-
tional Ltd) filters, respectively. Nylon filters were cleaned with ethanol and deionized water
before sampling. Paper filters were soaked in the solution mixed with 1 % citric acid (in
methanol), followed by drying on a clean bench before sampling. To collect carbonaceous
compounds of PM2.5, a prebaked (at 450 °C for 12 h) 47-mm quartz filter (Whatman
International Ltd.) was used at a flow rate of 16.7 Lmin−1 using an FH95 instrument
(Andersen).
After sampling, the filters for ionic compounds were soaked in 20 mL deionized water and
extracted by ultrasonication for 4 h at 60 °C, followed by filtration through 0.2-μm PTFE
syringe filters (Millipore). Thereafter, the samples were analyzed by ion chromatography
(Dionex, DX-120). Elemental and organic carbons were analyzed using the NIOSH (National
Institute of Occupational Safety and Health) method 5040 (Birch and Cary 1996) (Sunset Lab)
at Clarkson University, USA. Trace metals were analyzed by energy disperse X-ray fluores-
cence (XRF; Spectro X-Lab Pro) at Clarkson University. The details of the XRF procedure are
described in Sunder Raman et al. (2008). Also, the uncertainty of analytical XRF result can be
found in Rousseau (2001).
All apparatuses were cleaned with Alconox and deionized water before sampling and
analysis. The quartz filter was baked at 450 °C in a furnace for 12 h, and stored in a freezer
before use. All Zeflour and nylon filters used in this study were cleaned using deionized
water and ultrasonication before sampling. Field blank samples were collected after every
sixth sample for all PM2.5 constituents, and the collected samples were corrected by field
blanks. Average field blank values were 2.3, 1.2, and 0.6 μg m−3 for SO42−, NO3−, and
NH4+, respectively, contributing less than 30 % of the original sample values. The method
detection limit (MDL) was calculated as three times the standard deviation of field blanks,
and was 3.4, 2.6, and 1.6 μg m−3 for SO42−, NO3−, and NH4+, respectively. For organic
carbon (OC) and elemental carbon (EC), the average field blank values were 0.00 and
0.01 μg m−3, respectively, which contributed less than 1 % of sample values. MDL for OC
and EC was calculated as 0.04 and 0.08 μg m−3, respectively. The relative percent difference
(RPD) between duplicate analyses for SO4− (n011 sets), NO3− (n011), NH4+ (n010), OC
(n010), and EC (n010) were 4.0 % (0.3∼8.7 %), 1.8 % (0.4∼7.4 %), 2.0 (0.7∼5.0 %), 5.1
(0.4∼10.8 %), and 3.7 % (0.4∼13.4 %), respectively.
Average field blank, instrument detection limits (IDL), and RPD values for trace
elements are shown in Table 1. The IDL was calculated as three times the standard
deviation of lab blanks. MDL was substituted as IDL for trace elements. Concentrations
less than the IDL and the MDL were substituted with 0.5 × IDL and 0.5 × MDL for
trace elements and all other elements, respectively. The blank concentrations were
significant for all of the XRF elements, and all the elemental concentration in the
following sections were blank corrected. The quantification details are described by Sunder
Raman (2006).
J Atmos Chem (2011) 68:281–298 285

Table 1 Summarized QA/QC

results for trace elements Trace F.B. (ng m−3) % of original IDL (ng m−3) % RPD
Elements sample values

Na 0 0 31.1 11.9
Mg 11.5 12.6 31.1 27.0
Al 123.7 27.8 107.3 2.7
Si 39.9 5.9 35.9 3.5
Cl 15.3 2.5 6.2 8.1
K 0 0 1.6 7.3
Ca 315.5 40.1 31.9 2.5
Ti 6.4 15.8 4.3 5.1
V 1.5 33.3 0.6 14.7
Cr 21.2 52.7 4.0 7.2
Mn 4.2 23.1 0.6 6.1
Fe 289.1 41.5 198.1 4.3
Ni 26.1 37.3 17.0 5.0
Cu 244.0 54.5 52.0 8.1
Zn 44.3 37.1 34.4 3.4
As 0.0 0 0.6 5.8
Pb 14.1 27.1 11.6 7.3

2.3 Model description

The 5-day backward trajectories were calculated using the NOAA HYSPLIT 4.7 model with
Global Data Assimilation System (GDAS) meteorological data and a vertical mixing model.
The meteorological data fields were linearly interpolated into a terrain-following coordinate
system. The GDAS archive has three-hourly, global, one-degree latitude/longitude datasets
for pressure surfaces. In this study, the trajectories were calculated every 6 h for all 24 h
averaged samples using an arrival height of 500 m.
The Potential Source Contribution Function (PSCF) model uses chemical data
measured at the receptor site and associated back trajectories originating from the
receptor site to locate the source areas. The PSCF model was originally developed by
Ashbaugh et al. (1985) and Malm et al. (1986) and has been used extensively since
(Polissar et al. 2001; Hoh and Hites 2004; Han et al. 2007). The PSCF model counts
each trajectory segment endpoint that terminates within a given grid cell. The prob-
ability of an event at the receptor site is related to the number of endpoints in that
cell relative to the total number of endpoints for all of the sample dates. If N is the
total number of trajectory segment endpoints over the study period and if n segment
trajectory endpoints fall into the ijth cell, then the probability of this event (P[Aij]) is
calculated by nij/N. If mij is the number of segment endpoints in the same ijth cell
when the concentrations are higher than a criterion value, then the probability of this
high concentration event Bij is given by P[Bij]0mij/N. The PSCF value for the ijth cell
is then defined as a conditional probability PSCF(i,j)0P[Bij]/P[Aij]. Cells containing
emission sources are identified as having high conditional probabilities. This study
used a grid-cell size of 1°×1° and the criterion value was set to the arithmetic mean
concentration.
 286 J Atmos Chem (2011) 68:281–298

3 Results and discussion

3.1 Long-term trend of PM2.5 and its chemical compositions

3.1.1 PM2.5 mass concentration

The average PM2.5 concentration was 31 μg m−3 for the whole sampling period, which was
more than twice as high as the US National Ambient Air Quality Standard (NAAQS) of
15 μg m−3 (Fig. 2). Also, about 37 % of the entire PM2.5 samples exceeded the 24-h US
NAAQS of 35 μg m−3, showing the serious PM2.5 pollution at this sampling site. The
average concentrations were 37.0, 36.6, 34.3, and 29.6 μg m−3 for 2006, 2007, 2008, and
2009, respectively. The downward annual trend of PM2.5 was not statistically significant
(ANOVA, p-value > 0.05); however, the monthly mean concentrations were significantly
higher in 2006 and in 2007 than in 2008 and in 2009 at a significance level of 0.05 (paired t-test).
A few possible reasons may explain the decreasing annual trend of PM2.5.
The ADS was found to be a major cause of enhanced PM2.5 and PM10 concentrations in
Korea in previous studies (Lee et al. 2004; Kim et al. 2007; Han et al. 2008). The number of
samples collected during ADS occurrence (which are reported in real time region by region
by the Korean Meteorological Administration reports) generally decreased from 2006 to
2009 at this site (12, 13, 6, and 7 in 2006, 2007, 2008, and 2009, respectively), which
possibly contributed to the downward trend of PM2.5 concentrations. However, the average
annual PM2.5 concentrations, excluding ADS events, still decreased from 2006 to 2009 in
this study; therefore, ADS was not considered to be the primary reason for the decrease in
PM2.5. Precipitation can also reduce PM2.5 concentration; however, when rainy days were

250

Asian dust N = 313

24h US NAAQS (35 µgm-3) Mean = 31 µgm-3

200
PM2.5 concentrations (µg m-3)

150

100

50

0
05-12-01 06-06-01 06-12-01 07-06-01 07-12-01 08-06-01 08-12-01 09-06-01 09-12-01

Fig. 2 Daily PM2.5 concentrations from 2005 to 2009. Samples collected during ADS events are presented as
hollow circles
J Atmos Chem (2011) 68:281–298 287

excluded, PM2.5 concentrations still significantly decreased year after year. In Korea, the
special law for “Improving Air Quality in Metropolitan Area (IAQMA)” became effective in
2002 through the implementation of various measures to reduce PM10 emissions.
Since the sampling site was located approximately 100∼150 km northeast of the metro-
politan area (Fig. 1), air pollutants emitted in these areas could be transported to the
sampling site when there was a westerly wind, and the IAQMA law could possibly affect
the downward trend of annual PM2.5 concentration at the sampling site. In fact, according to
the National Emissions Inventory, PM10 emission rates in metropolitan areas have decreased
from 2003 to the present, whereas those where the sampling site was located (Chuncheon)
have even increased.
To identify the effect of PM2.5 emitted in metropolitan areas, the wind direction was
analyzed during the sampling period. As shown in Fig. 3, PM2.5 concentrations were
distinctly enhanced by westerly winds (42.6 μg m−3) in comparison with southerly
(24.4 μg m−3) and easterly winds (13.9 μg m−3). For both PM2.5 concentrations and
frequency of wind direction, westerly and northerly winds were more predominant than
easterly and southerly winds (Fig. 3). The metropolitan (Seoul) and industrial area (Incheon)
in Korea and in eastern China (including Shenyang, Beijing, and Shanghai) are also located
west of the sampling site (Fig. 1); therefore, the PM2.5 emitted in these industrial areas can
be transported to the sampling site, which would result in enhanced PM2.5 concentrations
with westerly winds.
The seasonal variation in PM2.5 was distinct (p<0.01, ANOVA), showing high concen-
trations in the winter and low concentrations in the summer (Table 2), which has also been
found in other cities in Korea (Lee et al. 2001; Kang et al. 2004a, b; Han et al. 2008). Higher
concentrations in the winter might be due to large-scale mechanisms such as differences in
meteorological conditions between winter and summer—for example, reduced mixing
heights, greater removal by wet deposition during the summer months, and predominantly
southerly winds during the summer months (Jung and Han 2008). This could explain the

100 80
Concentration
Frequency

80
60
Frequency of wind direction
PM2.5 Concentration (µg/m-3)

60

40

40

20
20

0 0
<=0.5m/s West NW North SW South NE SE East

Fig. 3 PM2.5 concentrations classified by wind direction

288 J Atmos Chem (2011) 68:281–298

Table 2 Concentrations of PM2.5 and its chemical constituents. Units of ionic and carbonaceous compounds
and ∑trace metals are μg m−3 while trace metals are shown in ng m−3

Spring Summer Fall Winter Total

PM2.5 (μg m−3) 41.1±28.8 22.6±18.0 30.2±21.7 44.0±23.6 31.0±23.3

SO42− 5.5±5.6 6.1±7.1 6.4±6.8 4.9±3.8 5.5±5.5
NO3− 4.4±3.3 1.6±1.1 3.1±2.2 4.5±4.2 3.8±3.4
NH4+ 4.6±4.0 3.5±2.8 3.0±2.4 4.4±5.5 4.0±4.3
OC 5.8±2.6 4.7±1.8 4.8±3.3 7.0±3.2 5.6±3.2
EC 1.7±0.8 1.4±0.6 2.2±1.4 2.5±1.3 1.9±1.1
∑Trace metals 5.3±3.4 1.5±0.8 2.4±1.2 4.2±1.5 3.6±2.5
Na (ng m−3) 330±244 153±176 87±193 128±201 200±302
Mg 144±91 30±21 42±24 61±38 80±114
Al 635±640 98±80 130±69 214±94 322±631
Si 1,381±1,386 159±150 283±178 490±222 693±1,483
Cl 442±301 56±70 541±422 1,661±1,137 635±875
K 577±371 160±215 401±286 536±247 437±460
Ca 627±290 340±165 366±173 446±138 471±281
Ti 61±60 14±7 17±8 25±9 34±60
V 4±2 3±1 2±1 4±1 3±2
Cr 21±9 18±8 16±6 19±6 19±4
Mn 18±19 7±5 12±9 15±11 14±12
Fe 675±535 194±94 261±119 325±95 408±585
Ni 14±6 12±5 13±6 14±5 14±3
Cu 220±100 202±89 178±73 199±68 204±40
Zn 83±50 48±33 77±44 89±44 75±48
As 9±5 3±3 8±5 14±6 7±6
Pb 40±22 17±12 38±22 56±23 38±26

large number of days in winter and spring when the daily PM2.5 exceeded the US NAAQS,
whereas PM2.5 concentration rarely exceeded the NAAQS in the summer (Fig. 2).
The major components of PM2.5 were OC, SO42−, NH4+, and NO3− in this study, and
accounted for 61 % (1∼108 %) of PM2.5 mass on average. The contribution of ionic constituents
was 50 % (8∼103 %) in the summer and 31 % (1∼73 %) in the winter. In contrast, both the
concentration and contribution of trace elements was lowest in the summer.
The PM2.5 concentration measured in this study was compared with the values identified
in previous studies performed in other cities of Korea and China (Table 3), and was found to
be significantly higher than the concentration in Gosan, the Korean national background site,
although it was generally lower than the values obtained in metropolitan and urban areas in
Korea. In contrast, the PM2.5 concentrations measured in metropolitan areas of China were
approximately three to five times higher than the PM2.5 concentration identified in this study.

3.1.2 Ionic constituents

The major ionic constituents of PM2.5 were SO42−, NO3−, and NH4+, which contributed
approximately 43 % (1∼103 %) to the total mass of PM2.5 on average (Table 2). The most
abundant species was SO42−, followed by NH4+, NO3−, and NO2−, showing a similar order
J Atmos Chem (2011) 68:281–298 289

Table 3 Comparison of PM2.5 concentration with other studies in Korea and China

Location Sampling period PM2.5 (μg m−3) Site description Reference

Gosan, Korea 2006 22.7 Background Kim et al. (2011)

2007 18.9
Seoul, Korea 2003–2005 43.0 Metropolitan Kim et al. (2007)
Iksan, Korea 2004 34.0 Rural/Residential Kang et al. (2011)
Suwon, Korea 2007–2008 46.1 Urban Lee et al. (2009a, b)
Beijing, China 2000 101.2 Metropolitan/Industrial Zheng et al. (2005)
Shanghai, China 2003–2005 94.6 Metropolitan/Industrial Wang et al. (2006)
Jinan, China 2006–2007 148.7 Urban Yang et al. (2012)
Chuncheon, Korea 2006–2009 31.0 Rural, residential This study

to the concentrations found in Gosan, the national background site (Choi and Kim 2004). In
most urban sites in Korea, it has been shown that NO3 −was significantly higher than NH4+
(Kim et al. 2007; Han et al. 2008). Urban areas have a high population density as well as a
massive traffic volume, which emits large quantities of nitrogen oxides; therefore, NO3 −formed
by nitrogen oxides is abundant in comparison with rural areas such as Chuncheon. The average
ratio of SO42−/NO3 −was 2.44±4.59 in this study, which was higher than the 0.65 found in
Seoul (urban) (Park and Kim 2005) and lower than the 3.2 found in Gosan (national back-
ground site) (Moon et al. 2005).
Ionic constituents also showed seasonal variation, but this differed for each constituent. SO42−
concentrations generally increased in the summer and decreased in the winter (Table 2);
however, there was no distinct statistical difference between two seasons (independent T-test,
p-value00.595). On the other hand, the concentrations of NO3− and NH4+ were statistically
higher in the winter than in the summer at a significance level of 0.05 (p-value00.047) and 0.1
(p-value00.087), respectively. A large portion of SO42− and NO3− in PM2.5 was identified as
secondary aerosols in many studies (Kang et al. 2004a, b). Secondary SO42 −is formed through
photochemical reactions, which often result in high concentrations in the summer (Wittig et al.
2004). However, much of the NO3− is a result of temperature-dependent atmospheric conversion
of nitrogen oxides and ammonia, which causes high concentrations in the winter (Chow et
al. 1994; Seinfeld and Pandis 2006). The volatilized fractions collected in back-up filters as
HNO3 and NH3 were 37 % and 43 % in the summer and 11 % and 7 % in the winter,
respectively. This suggests that the dissociation of NH4NO3 is significantly dependent on
temperature.

3.1.3 Carbonaceous components

Carbonaceous materials in PM2.5 are often classified as OC and EC which are operationally
defined. The concentration of OC was approximately threefold higher than that of EC on
average in this study (Table 2). Neither OC nor EC showed significant seasonal variation;
however, they generally increased in winter. EC originates from combustion processes while
OC can be either released directly from natural and/or anthropogenic sources (primary OC;
POC), or produced from gas-to-particle conversion in the atmosphere (secondary OC; SOC)
(Pandis et al. 1992; Turpin and Huntizicker 1995).
The OC/EC ratio is often used as an indicator of the origin of OC; ratios that exceed 2.0
indicate the presence of SOC (Turpin and Huntizicker 1995; Lee and Kang 2001). In this study
290 J Atmos Chem (2011) 68:281–298

there was a statistically significant correlation between OC and EC concentrations, indicating

that combustion sources emitting both EC and OC affected their concentrations in this area.
Average OC/EC was highest in the summer (3.9) and lowest in the fall (2.3), suggesting that a
large portion of OC could be assumed to be SOC. To identify the contribution of SOC to total
OC, the approach proposed by Turpin and Huntizicker (1995) was used as equation 1.

SOC ¼ OCtot  ECðOC=ECÞmin ð1Þ

where (OC/EC)min represents the OC/EC ratio from primary combustion sources and indicates
the minimum OC/EC ratio observed during the sampling period. In this study, the average value
of 1.28 for the lowest 5 % of the OC/EC ratio was used as (OC/EC)min. The fractions of SOC
contributing to OC were 60, 63, 35, and 52 % for spring, summer, fall and winter, respectively.
The high SOC fraction in spring and summer was explained by high photochemical activity;
however, the relatively high contribution of SOC in winter could not be justified by photo-
chemical reactions. Particle-to-gas partitioning is the product of a partitioning constant and the
total particulate mass concentration. At low temperatures, the partitioning constant is likely to
increase; as a result, semi-volatile organic compounds (SVOC) are adsorbed onto and/or
absorbed into particulate matter (Seinfeld and Pandis 2006). Also, as the PM2.5 mass concen-
tration increases in winter, more of the SVOC would be in the particulate phase because of the
greater surface and volume of particulate matter available. To examine the temperature depen-
dency of the gas-particle conversion of SVOC, the relationship of SOC concentration
and SOC/OC ratio with atmospheric temperature was identified. As shown in Fig. 4,
the SOC/OC ratio (0.41∼0.85 when T>25 °C) appeared to be greater at high temperatures, as
expected, due to active photochemical oxidation in the summer, but was also high at low
temperatures (0.24∼0.75 when T<0 °C), indicating that the partitioning of SVOC onto and/or
into particles was enhanced.

0.7 8
SOC/OC ratio
SOC concentration

0.6 6
SOC concentrations (µg m-3)
Ratio of SOC/OC

0.5 4

0.4 2

0.3 0
<0 0<T<10 10<T<15 15<T<20 20<T<25 T >25

Fig. 4 SOC concentrations and SOC/OC ratio by atmospheric temperature

J Atmos Chem (2011) 68:281–298 291

3.1.4 Trace elements

Seasonal average concentrations of total trace elements in PM2.5 were 5.3, 1.5, 2.4, and
4.2 μg m−3 for spring, summer, fall, and winter, respectively, showing a similar seasonal
trend to that of PM2.5 mass concentrations. Typical soil constituents such as Si, Al, Fe,
Ca, and Ti were predominant among trace elements at this rural site (Table 2), especially
in spring, and contributed approximately 61 % (35∼82 %) to the total mass of trace
elements primarily due to ADS events (n07). ADS has been identified as a major
incident which enhances atmospheric PM2.5 concentrations in many studies (Lee et al.
2004; Kim et al. 2007; Han et al. 2008). In this study the concentrations of crustal
elements, including Si, Al, Ti, Fe, K, and Mg, were more than twice as high during ADS
as those during non-ADS; however, even anthropogenic elements, including Zn, V, and
Cr, were also enhanced during ADS (Fig. 5). This result indicates that anthropogenic
particles produced in industrial areas of China were probably mixed in with the extremely
high concentration of fine particles that originated from deserts when a northwesterly
wind was observed in spring and winter.
Most of the elements showed distinct seasonal variation, with high concentrations in spring
and winter due to the predominantly westerly winds; however, some elements, including Cr,
Cu, Zn, and Ni, showed generally consistent concentrations over the seasons (Table 2). In
Chuncheon, the biggest PM10 source type is asphalt concrete production, which contribute
196.6 t of the total 439.8 t from anthropogenic sources (point, area, and mobile sources)
(Ministry of Environment, 2008). A variety of nonferrous slags which consist of Pb, Cu, Ni,
and Zn slags can be used as aggregate in hot mix asphalt (Federal Highway Administration
1998), suggesting these elements are possibly more impacted by local sources than other
elements. In this study, especially Cu and Ni showed relatively insignificant seasonal tendencies
while other metals were significantly affected by large-scale wind direction (Table 2).

6
Ratio of ADS / normal event

0
Al Si Ti Fe Mg Mn Ca K Na V Cr Zn Ni Cu As Pb Se Br Cl

Fig. 5 Change in concentrations of trace elements during ADS events

292 J Atmos Chem (2011) 68:281–298

The portion of sea-salt aerosol can often be determined by the ratio of Cl/Na. While the
typical Cl/Na ratio in ocean water is 1.17 (Finlayson-Pitts and Pitts 2000), the ratio was 3.17 in
this study, indicating that a significant portion of the measured Cl concentration was emitted
from anthropogenic sources such as open burning.

3.2 Enhanced concentration event

To identify the characteristics of high concentration events, the top 10 % of PM2.5 samples
were categorized. Average PM2.5 mass concentration increased approximately 2.8-fold
during high concentration events (84.2 μg m−3) compared with non-high concentration
events (29.6 μg m−3). OC, EC and NH4+ remained fairly constant, while anionic constitu-
ents, including SO42 −and NO3−, and trace elements increased by more than 1.5-fold during
high concentration events.
Previous studies showed that meteorological conditions significantly affect ambient aerosol
concentrations (Glavas et al. 2008; Han et al. 2008; Jung and Han 2008). In this study, the
westerly wind has already been shown to effectively enhance PM2.5 concentrations (Fig. 3). In
addition to wind direction, certain meteorological events including ADS (N07), fog (N022),
and precipitation (N012) can play significant roles in determining PM2.5 concentrations. In this
study, these three meteorological groups were classified and compared with normal conditions.
PM2.5 showed the highest average concentration during ADS (56.1 μg m−3), followed by fog
(43.7 μg m−3) and normal conditions (33.3 μg m−3), and the lowest average PM2.5 concentra-
tion (14.2 μg m−3) appeared during precipitation events (p<0.05; Tukey’s honestly significant
difference test) (Fig. 6). During ADS events, both trace elements and unidentified components
dramatically increased. Among trace elements, the typical crustal elements, such as Al, Si, and
Ti, were enhanced more than fourfold during ADS (Fig. 5). Other crustal elements, including
Ta, P, and Ag, that were not analyzed in this study were also liable to increase during ADS,
resulting in the increasing contributions of residue in Fig. 6.

60 100
OC
EC
SO42-
50 NO3
-
80
NH4+
Mass concentrations (µg m-3)

Trace
Residue
40
Contribution (%)

60

30

40
20

20
10

0 0
ADE Fog Rain Normal ADE Fog

Fig. 6 Mass concentrations and contributions of PM2.5 components under various meteorological conditions
J Atmos Chem (2011) 68:281–298 293

During fog events, the total PM2.5 mass was lower than that during ADS; however, the
concentrations of carbonaceous compounds and ionic constituents were much higher, while trace
elements and residue significantly decreased in comparison with ADS periods. When fog occurs,
relative humidity (RH) is likely to exceed the deliquescence relative humidity (DRH) of common
inorganic salts, and, as a result, the particle spontaneously absorbs water to form a saturated or
supersaturated salt solution. This deliquescence transition is accompanied by a significant
increase in the mass of the particle. Even when fog disappears and RH decreases during the
daytime, the salt solution generally crystallizes and the aerosol mass remains enhanced (Junge
1952; Richardson and Spann 1984; Cohen et al. 1987). In this study, NO3 −and NH4+ were
specifically enhanced during fog events compared with SO42 −and NO2−. Because salts such as
NH4HSO4 and NaHSO4 have low DRH at ambient temperatures, they can exist as aqueous
solutions even under the relatively low RH. However, inorganic salts that have a high DRH,
such as KCl, NaCl, NH4Cl, and NaNO3, are liable to increase when fog occurs, causing the
increased concentrations of NO3 −and NH4+ seen during fog events in this study. An approx-
imate threefold higher concentration of Cl was found during fog events than during ADS,
although most of the trace elements showed an opposite trend; this indicated that water content
in the aerosol was liable to absorb Cl-containing salts during fog events. However, slightly
lower wind velocity (0.8 ms−1) was observed during fog events than during non-fog events
(1.1 ms−1), which also possibly caused the high PM2.5 concentrations due to weak vertical and
horizontal mixing.
To identify the detailed wind pattern for high concentration events, the 120-h backward
trajectories were calculated for the top 10 % and the bottom 10 % of PM2.5 concentrations after
excluding ADS and precipitation events (Fig. 7). For top 10 % samples, a large number of the back
trajectories originated from the industrialized areas of China, including Beijing and Shanghai, as
well as the metropolitan areas of Korea. However, none of the trajectories incorporating low PM2.5
concentrations passed through the industrial area of China, although some went through the
Korean metropolitan areas. This result interestingly supports the hypothesis that regional sources
located in China were significant factors in increasing the PM2.5 concentrations in Chuncheon.
The PSCF (the back trajectory based model) was also used to identify the possible source
areas. It should be noted that sources located outside of the regions through which the
trajectories passed were not identified. To reduce the uncertainty in a grid cell with a small
number of endpoints, an arbitrary weight function W(nij) was applied when the number of end

Fig. 7 Five-day backward trajectories for high PM2.5 (top 10 %: left panel) and low PM2.5 (bottom 10 %:
right panel) samples
294 J Atmos Chem (2011) 68:281–298

points in a particular cell was less than three times the average number of end points for all cells
(Polissar et al. 2001). A detailed description of the arbitrary weight function can be found in
Han et al. (2005, 2007). Using the PSCF, the main industrial areas in eastern China (Beijing,
Shenyang, Jinan, and Shanghai) were identified as possible source areas likely to be responsible
for the enhanced PM 2.5 concentrations at the sampling site (Fig. 8). East China is currently
undergoing the most rapid industrialization in the world, and there has been a significant
increase in PM emissions as a result (Wang et al. 2011).

3.3 Factor analysis

Varimax rotated factor analysis was used to categorize the major source types that enhanced
PM2.5 concentrations in Chuncheon. Missing values were replaced with 1/3 of the MDL in this
study. In total, four factors accounted for 77 % of the explained variance (Table 4). Crustal
elements, including Mg, Al, Si, Ca, Ti, Mn, and Fe, belong to the same group, indicating a soil-
related source which explained approximately 33 % of the variance (Table 4). The second factor
showed high values for carbonaceous compounds, Cl, K, and Pb, which was possibly explained
by combustion processes, including transportation. The third factor was identified as non-
ferrous manufacture, since Cr, Ni, and Cu belonged to the same group, while secondary PM2.5
was classified as the fourth factor due to the high values for SO42−, NO3−, and NH4+. The soil-
related factor contributed most to the measured PM2.5 concentration, and the combustion
processes, the non-ferrous manufacture, and secondary PM2.5 contributed approximately
18 %, 14 % and 11 %, respectively.
The source contribution to PM2.5 in this study was compared with that identified in
previous studies performed in various cities in Korea. The other studies in Table 5 estimated

Fig. 8 Probable source areas affecting the PM2.5 concentration at the sampling site using PSCF modeling
J Atmos Chem (2011) 68:281–298 295

Table 4 Rotated factor analysis

of PM2.5 constituents Factor 1 Factor 2 Factor 3 Factor 4

OC .060 .581 .137 .381

EC −.003 .845 −.063 .233
SO42− .048 .085 −.287 .691
NO3− .043 .349 .075 .542
NH4+ −.031 .226 .156 .643
Na .516 −.091 .373 .482
Mg .911 .000 .217 .178
Al .969 −.014 .041 −.033
Si .973 .081 .084 −.007
Cl −.073 .826 .088 −.064
K .646 .564 .005 .331
Ca .757 .080 .392 .058
Ti .964 .060 .110 .030
V .358 .273 .527 .511
Cr .271 −.009 .906 .090
Mn .719 .518 .017 .115
Fe .958 .139 .139 .072
Ni .133 .420 .709 .032
Cu .085 −.037 .912 −.055
Zn .446 .641 .126 .468
Pb .307 .809 .102 .328
Eigen value 6.87 3.86 2.98 2.39
Variance % 32.72 18.40 14.20 11.36

the source contribution using positive matrix factorization (PMF), whereas this study used
factor analysis. Soil-related sources were estimated to be the main source type in Suwon
(urban site), Gosan (background site), and Chuncheon (the rural site used in this study).
However, soil-related sources were generally minor in Seoul (metropolitan) and Gwangyang

Table 5 Comparison of source contributions (%) of PM2.5 in this study with those identified in previous
studies

Soil-related Secondary Biomass Industry Motor Combustion

aerosol burning related vehicle

Seoula 1.0 37.5 16.4 12.2 13.3

Suwonb 32.8 26.2 11.0 7.2 11.1
Gwangyangc 7.9 10.3 2.9 16.9 19.3 29.0
Gosand 12.4 13.0 4.2 8.1 9.1
Chuncheone 33.0 11.0 14.1 18.0
a
Moon et al. (2011)
b
Lee et al. (2009b)
c
Huh and Yi (2004)
d
Moon et al. (2006)
e
This study
296 J Atmos Chem (2011) 68:281–298

(industrial area). Motor vehicles were included in “combustion” sources in Chuncheon in this
study, but were classified separately in the data from other cities obtained using PMF. In Gosan,
secondary aerosols were not identified, but were important in all other cities. Undetermined
sources contributed approximately 37 % of the total PM2.5 in Gosan according to Moon et al.
(2006), some of which may actually have been attributable to secondary aerosols. It should be
noted that in the other studies, the receptor model was used for the aerosol measurements with a
relatively short sampling period (less than 1 year), which may have caused greater uncertainty
in the results. Further, it is difficult to find receptor modeling studies of PM2.5 in Korea, and thus
the PM10 and PM12 concentrations were used to model Suwon and Gosan, respectively.

4 Conclusions

In this study, a total of 308 daily PM2.5 samples were collected at a rural site in Korea; the
average concentration was 31 μg m−3. The major components of PM2.5 were OC, SO42−,
NO3− and NH4+. High SO42− was found in the summer due to active photochemical
reactions, while NO3− was high in the winter due to the active atmospheric conversion of
nitrogen oxides and ammonia into NH4NO3(s) at low temperatures. A large portion of OC
was determined as SOC in this study. The high SOC to OC ratio was observed at both high
(>20 °C) and low (<0 °C) atmospheric temperatures.
The concentration of PM2.5 showed a downward annual trend; however, it still significantly
exceeded the annual US NAAQS of 15 μg m−3. One possible reason for this high PM2.5
concentration was emissions from regional and continental sources located in metropolitan areas
of Korea and industrial areas of China, which are situated west of the sampling site. For this
reason, when the prevailing winds were westerly, PM2.5 concentration was clearly enhanced.
Also, PSCF identified the industrial areas in eastern China as the possible source areas for the
enhanced PM2.5 concentration at the sampling site. In addition to wind direction, other meteo-
rological conditions significantly affected PM2.5 concentrations in this study. Both ADS and fog
events clearly increased PM2.5 concentrations, but affected the chemical composition differently.
During ADS, the typical crustal elements, such as Al, Si, and Ti, dramatically increased; while
carbonaceous and ionic compounds were highly enhanced during fog events. When fog occurs,
saturated inorganic salts which generally have a high DRH, such as KCl, NaCl, NH4Cl and
NaNO3, are liable to be formed, which increases the PM2.5 concentration. As a result, NO3−,
NH4+, and Cl were specifically enhanced during fog events in this study. The lowest average
PM2.5 concentration was observed during precipitation, due to the scavenging effect.
Factor analysis was performed to categorize the major source types that enhance PM2.5
concentrations, and four factors including soil, combustion processes, non-metal manufacture,
and a secondary PM2.5 mechanism were identified.

Acknowledgements This work was supported by the Korea Research Foundation Grant funded by the
Korean Government (MOEHRD, Basic Research Promotion Fund) (KRF-2008-331-D00278), and by Basic
Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry
of Education, Science and Technology (2009-0072989).

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