Aerosol and Air Quality Research, 15: 2305–2319, 2015

Copyright © Taiwan Association for Aerosol Research

ISSN: 1680-8584 print / 2071-1409 online
doi: 10.4209/aaqr.2015.04.0271 

Ultrafine Particles and PM2.5 at Three Urban Air Monitoring Stations in Northern
Taiwan from 2011 to 2013

Guan-Yu Lin1, Guo-Rui Lee1, Sih-Fan Lin1, Yi-Hung Hung1, Shih-Wei Li2, Guo-Jei Wu2,
Huajun Ye3, Wei Huang3, Chuen-Jinn Tsai1*
1
Institute of Environmental Engineering, National Chiao Tung University, Hsinchu, 300, Taiwan
2
Environmental Analysis Laboratory, Environmental Protection Administration, Jongli, 320, Taiwan
3
Focused Photonics (Hangzhou), Inc., Hangzhou, 310052, China

ABSTRACT

In this study, long term measurements of PM2.5 and ultrafine particles (UFPs) for daily average mass concentration at
Zhongshan (ZS), Sinjhuang (SJ), and Jhudong (JD) urban air monitoring stations were conducted from 2011 spring to
2013 autumn. The results showed that daily average UFPs mass concentrations in spring (average at 3 stations: 1.58 ± 0.74
µg m–3) and summer (average at 3 stations: 1.59 ± 0.53 µg m–3) were higher than those in autumn (average at 3 stations:
1.02 ± 0.28 µg m–3) and winter (average at 3 stations: 1.04 ± 0.48 µg m–3) due to the impacts by heavy traffic emission and
new particle formation event. The effective density (ρeff) and dynamic shape factor (χ) for ultrafine particles (UFPs) were
found to be 0.68 ± 0.16 g cm–3 and 2.06 ± 0.19, respectively, suggesting that the particle morphology was irregular shape.
Based on the calculated ρeff and χ, the average number and surface area concentration ratio of UFPs to those of PM2.5 at
these monitoring stations was determined to be 89.0 ± 5.5% and 42.1 ± 12.8%, respectively, suggesting that UFPs
contribute significantly to the health-relevant PM2.5 aerosol fraction in these stations.

Keywords: PM2.5; Nanoparticle measurement; Ultrafine particles; Effective density.

INTRODUCTION In the past, numerous studies used the Fast Mobility

Ultrafine particles (UFPs), defined as particles with the
diameter dp less than 0.1 µm (or called PM0.1), are drawing
public concerns because they are cleared less quickly and
completely from the lung than larger PMs under chronic or
repeated exposure and may translocate across the lung
epithelium into the circulatory system, leading to potential
adverse effect on the cardiovascular system and other
organs (HEI, 2013). The adverse effect could be attributed
to their number and surface area concentrations, and
concentration of bounded toxic air pollutants on them
(Chen et al., 2010a; Leitte et al., 2011; Hata et al., 2013).
Among all PM fractions, nanoparticles were found to
cause the major health risk because of low clearance and
rate and high deposition efficiency in the respiratory system
(Gorbunov et al., 2013). In order to understand the major
sources and evolution of UFPs to facilitate the prediction
of air quality and develop mitigation strategies, it is very
important to conduct long term measurements of UFPs.
*
Corresponding author.
Tel./Fax: +886-3-5731880
E-mail address: cjtsai@mail.nctu.edu.tw
Particle Sizer (FMPS) (Westerdahl et al., 2009; Sabaliauskas
et al., 2012; Betha et al., 2014; Kim et al., 2015) or the
Scanning Mobility Particle Sizer (SMPS) coupled with the
condensation particle counter (CPC) (Chen et al., 2010a;
Breitner et al., 2011; Jayaratne et al., 2011; Wang et al.,
2011; Xu et al., 2011; Gao et al., 2012; Young et al., 2012;
Cheung et al., 2013; Young et al., 2013; Cheng et al., 2014)
to investigate the number concentrations of UFPs. Most of
the researches have shown that both local rush hour traffic
emission and new particle formation (NPF) play key roles
in the diurnal variation of UFPs concentrations, in which
two concentration peaks in the morning and evening could
be attributed to traffic emission, while one peak in the
afternoon is due to NPF (Young et al., 2012; Cheung et al.,
2013; Young et al., 2013; Betha et al., 2014; Nikolova et
al., 2014).
In addition to pollutant sources, meteorological factors
including wind speed, wind direction, precipitation, relative
humidity, and temperature all have effects on seasonal and
long-term variation of UFPs concentrations (Morawska et
al., 2008; Wang et al., 2011; Young et al., 2012; Cheng et
al., 2014). However, the seasonal variation and long-term
measurements of UFPs number concentrations in Taiwan
were limited only the hourly average and diurnal patterns
of UFPs number concentration in central and northern
2306 Lin et al., Aerosol and Air Quality Research, 15: 2305–2319, 2015
Taiwan were reported (Young et al., 2012; Cheng et al.,
2014).
There are many previous long-term PM2.5 studies. For
example, Yu et al. (2013) conducted a long term PM2.5
study for a full year from January 1 to December 31, 2010
and indentified seven source types by PMF analysis, which
included secondary sulphur (26.5%), vehicle exhaust (17.1%),
fossil fuel combustion (16%), road dust (12.7%), soil dust
(10.4%), biomass burning (11.2%), and metal processing
(6.0%). Contributions of different sources varied by different
seasons with the combustion source types, including biomass
burning and fossil fuel combustion, being significantly higher
in the fall and winter compared to those in the spring and
summer. Huang et al. (2014) found that the increased mass
concentrations on high PM days were mainly caused by air
pollutant transport from the outside-Hong Kong regions, in
a full year study from March 2011 to February 2012 at
HKUST AQRS (Air Quality Research Supersite). The major
PM2.5 components (crustal materials, organic matter, soot,
ammonium sulfate, ammonium nitrate, and non-crustal trace
elements) accounted for 90% of the measured mass with
sulfate being the most abundant (32.0%), followed by organic
matter (23.5%) and ammonium (11.8%). PMF analysis
revealed that secondary sulfate formation process (annual
average of 31%), biomass burning (23%), and secondary
nitrate formation process (13%) were the three dominant
contributing sources to the observed PM2.5 throughout the
sampling year.
Regional dust transport has been shown to influence
local PM2.5 concentrations. Remoundaki et al. (2013)
found that the concentrations of crustal elements abrupt
increased during Saharan dust transport events in December
2010 in Athens, Greece. The sum of all measured chemical
components accounted for about 75% of PM2.5 concentrations
in which SIA (secondary inorganic aerosols) and
carbonaceous material (OM + EC) contributed almost equally
for about 30% in the PM2.5 mass, and while the dust
contribution was significant, which could be up to 23% of
PM2.5 mass during dust transport events, it was only about
5% in absence of such events. In Asia, Asian dust storm
(ADS) not only increase the coarse particle concentrations,
but also bring the fine and ultrafine particles to Taiwan
(Liang et al., 2013). Liang et al. (2013) applied the PCA
model to identify the potential source categories by measuring
ambient 10–500 nm particle number concentrations, size
distributions and composition data in Taipei, Taiwan and
found that three factors estimated during an ADS were
vehicular emissions (52%), dust storm (24%), and primarily
gasoline vehicles (12%), while during non-dust periods,
the three factors were vehicular emissions, secondary sulfate
and nitrate (40%), combustion processes and traffic-related
emissions (29%), and road dust (25%).
Long-term measurements for daily average fine particles
(PM2.5) and UFPs mass and number concentration in
northern Taiwan are still lacking. Therefore in this study,
PM2.5 and UFPs at urban air monitoring stations in northern
Taiwan from May 2011 to May 2013 were investigated. In
order to characterize the effective density (ρeff), dynamic
shape factor (χ), and number concentration of UFPs, a
 
MOUDI and a SMPS were further deployed at ZS station in
May 2014 to measure the mass and number distributions
simultaneously for atmospheric aerosols with 5.6 ≤ dp ≤
209.1 nm. The mass concentrations of UPFs were then
converted to number concentrations to investigate the ratio
of UFPs/PM2.5 in different metrics by using the calculated
ρeff and χ at ZS station for 3 stations. The sources and long-
term trends of UFPs number concentrations were finally
discussed.
METHODS
Sampling Sites and Experimental Methods
The mass concentration measurements for PM2.5 and
UFPs were conducted at the Zhongshan (ZS) air monitoring
station in Taipei City, the Sinjhuang (SJ) air monitoring
station in New Taipei City, the Judong (JD) air monitoring
station in Hsinchu County, which are shown in Figs. 1(a),
1(b), and 1(c) respectively. In addition to traffic emissions
as major air pollution sources, dust storm with air pollutants
from mainland China transported by the north-eastern
monsoon and biomass burning from Southeastern Asia
also impact on the air quality at these stations. The samples
at the ZS station were collected at the rooftop of a 4-floor
building located on the campus of Xin-Xing Junior High
School (25°03'41"N, 121°31'36"E) in Taipei (population:
2.70 million as of Dec. 2014), which is 30 m S of Minquan
E. Rd, 100 m W of Xinsheng Highway, 1.5 km S of No. 1
National Freeway, 2 km SW of Taipei International Airport,
and 2 km N of Taipei Main Station.
The SJ station is located at the rooftop of a four-floor
building in Fu-Jen Catholic University (25°02'16"N, 121°
25'59" E) (Fig. 1(b)) in New Taipei city (population: 3.97
million as of Dec. 20154). The traffic emission sources
mainly come from Zhongzheng Rd., Zhongshan Rd., and
No. 1 National Freeway, which is 600 m N, 300 m S, and
1.5 km S from SJ station, respectively. The SJ station is
also influenced by industrial emission from the New Taipei
Industrial Park (3.5 km SW), Taishan Industrial Park (3.5
km S), Gong'er Industrial Park (6 km SE). The JD station
is located at the rooftop of a four-floor building in Tatung
primary school in Zudong (24°44'32"N, 121°05'31"E)
(Fig. 1(c)), which is a relatively small town (population:
about 96000 as of Dec. 2014) surrounded by mountains.
The main sources of particulate matters could come from
the No. 3 National Freeway and the local No. 68 expressway
which are 6000 m NW and 200 m SW, respectively, away
from the JD station.
PM2.5 and UFPs mass concentration measurements were
conducted from May 3 2011 to Oct. 31 2013. Each sample
was collected for 24 hours and the number of samples was
55, 55 and 62 at ZS, SJ and ZD stations, respectively. The
total number of samples taken range from 8-24 per season
per station. The sampling strategy of this study is to use a
MOUDI to determine UFP mass concentrations and mass
distributions, a Dichotomous sampler to determine PM2.5
concentrations, and chemical analysis is to determine
chemical compositions of UFP and PM2.5. To characterize
the effective density and dynamic shape factor of UFPs
 Lin et al., Aerosol and Air Quality Research, 15: 2305–2319, 2015  2307

(a)

(b)

(c)
Fig. 1. (a) Zhongshan (ZS) station, (b) Sinjhuang (SJ) station, (b) Judong (JD) station.

and submicron particles for the conversion of number
concentrations into mass and surface area concentrations, a
SMPS was collocated with the MOUDI for measuring
UFPs number distributions at ZS station with the time
resolution of 3 minute from Apr. 22 to 25 and May 14 to
18 in 2014. Details of the strategy and methods were
documented in our earlier paper (Chen et al., 2010b) and
are only briefly discussed here.
In the MOUDI, the 3.2 µm cutsize stage was replaced
with 2.5 µm cutsize stage and the 10-th stage was not used.
Thus, the cutsizes of the MOUDI stages were 18, 10, 5.6,
2.5, 1.8, 1.0, 0.56, 0.32, 0.18, and 0.1 µm, respectively,
and the after filter measured UFP concentrations. In the
MOUDI, silicone grease (KF-96-SP, Topco Technologies
Corp., Taiwan) coated aluminum foils were used as the
impaction substrates in 0–9 stages to reduce solid particle
bounce. Teflon filter was used as the impaction substrate
in the 10th stage (Teflon R2PL047, Pall Corp., New York,
2308 Lin et al., Aerosol and Air Quality Research, 15: 2305–2319, 2015 

USA) and after filter (Teflon R2PJ047, Pall Corp., New impactor (ELPI) (Kannosto et al., 2008) or SMPS-MOUDI
York, USA) for chemical analysis for soluble ions and (Hu et al., 2012). The present study used the SMPS-
elements. The samples collected were weighed to determine MOUDI to conduct the field measurement in which ρeff of
mass distributions. The mass distribution function based UFPs in a certain size range was calculated based on the
on particle size dai was calculated by using the multi-modal equation described in Hu et al. (2012) as follows:
size distribution model (Seinfeld and Pandis, 1998) as:
MCi MCi
eff ,i   (4)
dM i j
Mi   logd ai  logd g ,i   VCi  dm 2 3
6 dm1
  exp    d pi  n(d pi ) d d pi
d  logd ai  i 1 2  logd ai  2  log 2 g , j 

(1) where ρeff is the effective density in the size range from dm1
to dm2, i is 9, 10, or after filter representing the 9th stage,
where j is the number of mode under lognormal distribution, 10th stage, and after filter of the MOUDI, respectively; dm
dg,i is the geometric mean diameter (GMD), σg,i is the is the electrical mobility diameter; n(dpi) is the number
geometric standard deviation (GSD), and Mi is the mass concentration of size dpi measured by the SMPS; MCi is the
concentration. mass concentration measured by the MOUDI in the size range
The Dichot (Dichotomous PM10 sampler, Model SA- from da1 to da2 in which da represents the aerodynamic
241, Andersen Inc., Georgia, USA) was used to sample diameter; VCi is the volume concentration calculated from
PM2.5 and coarse particles (PM2.5–10). Teflon filters (Teflo the number distribution measured by the SMPS in the size
R2PL037, Pall Corp., New York, USA) were used in fine range from dm1 to dm2. The range of da1–da2 was changed to
and coarse particle channels for analyzing soluble ions and dm1–dm2 by using the following equations (McMurry et al.,
elements. In this paper, only PM2.5 data will be reported. 2002):
Before chemical analysis, all Teflon samples of MOUDI,
Dichot and filter blanks were conditioned at least 24-h in a
temperature and humidity controlled room (22 ± 1°C, 40 ±
0 C (d ai )
d mi  d ai (5)
5% RH) and then weighed by using a microbalance (Model eff ,i C (dmi )
CP2P-F, Sartorius, Germany). After that, each Teflon filter
was cut in two equal halves using a Teflon coated scissor.
One half was analyzed by an ICP-MS (Model 7500 series, 2    0.999  d pi   
C (d pi )  1  1.142  0.558  exp       (6)
Agilent Technologies, Inc., USA) for elements, including d pi    2   
both crustal materials (CM) (Na, Mg, Al, K, Ca, Fe and Si)
and trace elements (TE) (S, Zn, Ni, Cu, Mn, Sr, Ag, Ba, where C(dmi) is the slip correction factor as the function of
Pb, V, Cr and Ti). The other half was analyzed by an ion dmi; C(dai) is the slip correction factor as the function of dai;
chromatograph (IC, Model DX-120, Dionex Corp, ρ0 is the unit particle density (1 g cm–3); λ is the mean free
Sunnyvale, CA) for ionic species, which are F–, Cl–, NO3–, path air molecules. ρeff,i of UFPs can be calculated by Eq.
SO 4 –2 , NH 4 + , Na + , K + , Mg +2 and Ca +2 . CM can be (4) based on the iteration method.
calculated from elements by the following equations (Chow Eq. (5) is only valid for spherical particles. For non-
et al., 1994a; Marcazzan et al., 2001; Hueglin et al., 2005): spherical particles, the dynamic shape factor (χ ) and the
volume equivalent diameter (dve,i) should be used for
CM = 1.89 × Al + 1.21 × K + 1.43 × Ca + 1.66 × Mg + 1.7 converting the aerodynamic diameter to the mobility diameter
× Ti + 2.14 × Si (2) (DeCarlo et al., 2004). The iteration method was used for
solving χ by the following equations:
Si = 3.41 × Al (3)
MCi
To characterize the effective density and dynamic shape n '  d pi   (7)
factor of UFPs and submicron particles, a SMPS (Model 
d  ρeff ,i
3
mi
3936, TSI Inc., MN, USA) equipped with Nano-DMA (TSI 6
Model 3085) and Ultrafine Water-based Condensation
Particle Counter (UWCPC, TSI Model 3786) was collocated  0 C  d ai   i
with the MOUDI to monitor the number distributions of d ve ,i  d ai (8)
ambient particles from 5.6 to 209.1 nm.  pi C  d ve ,i 

Particle Effective Density (ρeff) and Dynamic Shape C  d mi 

Factor (χ) d mi  dve,i i (9)
Most of previous studies focused on measuring the ρeff C  dve,i 
of submicron particles with a selected diameter (McMurry
et al., 2002; Park et al., 2003; Geller et al., 2006; Spencer where n’(dpi) is the number concentration calculated based
et al., 2007). Only few studies investigated the size-resolved on an assume value of χi; C(dve,i) is the slip correction
ρeff of UFPs by using the SMPS-electrical low pressure factor as the function of dve,i. In the iteration, χi was obtained
 Lin et al., Aerosol and Air Quality Research, 15: 2305–2319, 2015  2309
when n’(dpi) was equal to the measured number concentration
in the size range i. The surface area concentration s’(dpi) in
the size range dpi was computed directly from the number
concentration as s’(dpi) = n’(dpi) (/4 dpi2). UFP surface area
concentration was calculated as the sum of surface area
concentrations in all size ranges below 100 nm.
RESULTS AND DISCUSSION
Meteorological Conditions
Average trace gas concentrations and meteorological
parameters at the three air monitoring stations during the
present study are shown in Table S1 in Supplementary
Materials. The differences in temperature between seasons
are insignificant compared to mid- or high-latitude regions
because Taiwan has a subtropical climate. The largest
difference in temperature between summer and winter was
only 14.7°C occurring at SJ station. The rainfall at three
stations occurred frequently during the sampling period. In
general, the concentrations of criteria pollutants except O3
were lower in JD than the other two stations.
Quality Assurance and Quality Control (QA/QC)
Fig. 2 shows the comparison of mass concentrations
(a)
(c)
Fig. 2. Comparison of PM2.5 mass concentration measured by the MOUDI to those measured by the Dichot at the (a) ZS,
(b) SJ, and (c) JD stations. (PM2.5,D: PM2.5 concentration measured by Dichot, PM2.5,M: PM2.5 concentration measured by
MOUDI.)
measured by the MOUDI with those measured by the Dichot
at the ZS, SJ, and JD stations. Good agreement was obtained
between the MOUDI and the Dichot mass concentrations
with the slope of 1.03 (R2 = 0.94), 0.94 (R2 = 0.94), and 1.0
(R2 = 0.98) at ZS, SJ, and JD stations, respectively. This
indicates that the quality of PM2.5 measurement is good
and the accuracy of UFP concentrations measured by the
MOUDI is guaranteed. Fig. 3 shows the anion-cation balance
of water soluble ions in terms of equivalent concentrations.
For UFPs, the ratios of anion and cation equivalent
concentrations were 1.04 ± 0.23, 1.06 ± 0.20, and 1.03 ±
0.18 at ZS, SJ and JD stations, respectively. For PM2.5, the
ratios were 1.10 ± 0.21 (ZS), 1.11 ± 0.33 (SJ), and 1.05 ±
0.27 (JD), respectively. Good anion-cation balance was
obtained to support of the accuracy and precision of sulfate,
nitrate, and ammonium data in the filter-based aerosol
measurements (Chow et al., 1994b).
Seasonal Variation of PM2.5 and UFPs Mass
Concentration
The seasonal variations of the sampling data at each air
monitoring station are shown in Fig. 4. Four seasons in
Taiwan are spring from March to May, summer from June
to August, autumn from September to November, and winter
(b)
2310 Lin et al., Aerosol and Air Quality Research, 15: 2305–2319, 2015
(a)
Fig. 3. Anion-cation ion balance in terms of equivalent concentration for (a) UFPs (b) PM2.5 at the ZS, SJ, and JD stations.
from December to February, respectively. At ZS station,
the UFPs average mass concentrations in spring (2.2 ± 0.7
µg m–3) and summer (1.9 ± 0.7 µg m–3) are higher than those
in autumn (1.2 ± 0.3 µg m–3) and winter (1.2 ± 0.5 µg m–3).
It could be attributed to the impact by heavy traffic emission
from Xinsheng Highway and NPF due to photochemical
nucleation, which depends on the intense solar radiation
during warm period (Young et al., 2012). Similar results
were also found at SJ and JD stations, where high average
UFPs mass concentrations of 1.6 ± 0.5 and 1.2 ± 0.5 µg m–3
were measured in summer, respectively, followed by those
in spring, autumn, and winter, as shown in Table 1. It is
noted that UFPs mass concentrations measured in JD were
lower than those at ZS and SJ stations because JD station
is surrounded by mountains with less UFPs sources from
traffic emission and anthropogenic activities. In addition to
the primary particles emission, another possible source of
UFPs at the JD station is the NPF produced by the oxidation
of biogenic sources from the forest (O’Dowd et al., 2002)
located in Jianshi Township (~15 km SE from JD station).
For PM2.5, the average mass concentrations in spring,
autumn, and winter at three stations were found to be higher
than those in summer mainly due to the meteorological effect
and partly due to the impact of PMs transported from China
on PM2.5 mass concentration in Taiwan (Lee et al., 2011).
Similar result was also found by Shen et al. (2010), in
which the seasonal highest PM1 mass concentrations was
found in winter due to emissions from coal and biomass
burning, followed by spring, autumn, and summer.
In addition to local sources and long-range transported
PMs, precipitation, wind speed, and wind direction also
affect UFPs and PM2.5. For example, on Feb. 15 and Sep.
13, 2012, the average mass concentration of PM2.5 at ZS
station decreased from 23.0 to 7.2 µg m–3 and 24.5 to 8.8
µg m–3, due to heavy precipitation of 5.8 and 29.8 mm in
rain fall, respectively. Similar results were also found in the
urban area of Pakistan where the heavy monsoon rainfall
during July and August results in lower PM2.5 concentration
in summer than that in winter (Rasheed et al., 2015). A
decrease in UFPs from 1.8 to 0.4 µg m–3 was also observed
 
0.5
PM2.5
ZS
0.4 1:1
SJ
JD
0.3 20%
0.2
0.1
0
0 0.1 0.2 0.3 0.4 0.5
Cation eq. ( mol/m3)
(b)
on Feb. 15, 2012 due to washout effect (Morawska et al.,
2004; 2008). However, an opposite variation trend was
found for PM2.5 and UFPs during rain events of 16.8 and
38.4 mm in rain fall on May 14 and 15, 2011, respectively,
in which PM2.5 mass concentration decreased from 31.9 to
10.3 µg m–3, while UFPs slightly increased from 0.9 to 1.1
µg m–3. It is probably because higher saturation ratio of semi-
volatile species combined with pre-existing particles existed
in reduced temperature and heavy precipitation to form
new particles, resulting in increase in UFPs concentrations
(Charron and Harrison, 2003). Another possible explanation
is that the heavy rain event washed the pre-existing PM out
and thus reduced the coagulation sink and favored the
presence of UFPs. On Aug. 14 and 15 of 2012, the wind
speed (3 m s–1) was larger than the average wind speed
(1.8 m s–1), resulting in minimum PM2.5 and UFPs mass
concentrations during the sampling period due to high
coagulation rate, good air mixing, particle deposition,
scavenging (Morawska et al., 2008).
Table 2 shows 3-year average concentration ratios of
water soluble ions (Ions), organic matters (OM), elementary
carbon (EC), TE and CM concentrations to PM2.5 and UFPs.
The ion concentration accounts for 15.2 ± 1.6, 19.2 ± 1.5,
and 21.0 ± 2.1% of UFPs, while the TE concentration is
3.2 ± 0.9, 3.2 ± 1.3, 4.5 ± 1.0% of UFP concentration at
the ZS, SJ, and JD stations, respectively. The OM in UFPs
was not measured in this study and might contribute
significantly in UFPs.
The TE concentration is 4.3 ± 3.6, 3.0 ± 1.4, and 3.0 ±
1.8% of PM2.5 concentration at the ZS, SJ, and JD stations,
respectively. The ion concentration contributes 37.8 ± 4.1,
40.0 ± 3.0, and 46.4 ± 1.6% to PM2.5, which is similar to that
measured at the roadside in Chen et al. (2010b) (Table 2).
Ion concentration accounted for more fraction in PM2.5
than that in UFPs because UFPs are mostly freshly generated
primary or secondary PMs by vehicles, while PM2.5 are aged
ambient particles, which contain more condensed water to
absorb inorganic salts (Chen et al., 2010a). It is also noted
that PM2.5 sampled at the JD station contains more soluble
ions than those in other stations because of less traffic
 Lin et al., Aerosol and Air Quality Research, 15: 2305–2319, 2015  2311

(a)

(b)

(c)
Fig. 4. PM2.5 and UFPs seasonal mass concentration variation at (a) ZS, (b) SJ, and (c) JD stations.

contribution to PM2.5 at this station, suggesting that particles
are aged through photochemical reaction and thus more
secondary sulfates, nitrates, and other inorganic salts are
formed (Lin et al., 2007; Chen et al., 2010a).
CM including Al, K, Fe, Ca, Mg, Ti, and Si contributed
9.0 ± 7.4, 8.5 ± 7.7, and 9.5 ± 8.3% to UFPs at ZS, SJ, and
JD, respectively, and 8.3 ± 8.0, 8.4 ± 6.2, and 10.6 ± 8.8%
to PM2.5 at ZS, SJ, and JD, respectively. This suggests that
no substantial difference in CM fraction in either UFPs or
PM2.5 and CM is also an important composition in UFPs.
A semi-continuous OC/EC field analyzer (Model-4, Sunset
laboratory, USA) was also used at the ZS, SJ and JD stations
to investigate PM2.5 OM and EC concentration from 2011
to 2013. At ZS station, yearly average of OM and EC is 21.9
2312 Lin et al., Aerosol and Air Quality Research, 15: 2305–2319, 2015 

Table 1. Seasonal average mass concentrations of PM2.5 and UFPs at ZS, SJ, and JD stations.
Spring Summer Autumn Winter
Seasonal Avg.
(Avg. ± S.D.) (Avg. ± S.D.) (Avg. ± S.D.) (Avg. ± S.D.)
ZS UFPs* (µg m–3) 2.2 ± 0.7 1.9 ± 0.7 1.2 ± 0.3 1.2 ± 0.5
SJ UFPs (µg m–3) 1.4 ± 0.6 1.6 ± 0.5 1.2 ± 0.4 1.1 ± 0.6
JD UFPs (µg m–3) 1.2 ± 0.6 1.2 ± 0.4 0.7 ± 0.2 0.9 ± 0.4
ZS PM2.5,M# (µg m–3) 20.5 ± 10.5 17.2 ± 6.2 19.2 ± 5.8 19.4 ± 9.2
SJ PM2.5,M (µg m–3) 19.4 ± 9.2 17.6 ± 7.4 26.3 ± 9.8 15.9 ± 7.0
JD PM2.5,M (µg m–3) 16.5 ± 11.4 15.4 ± 7.0 17.9 ± 9.1 16.6 ± 6.5
*
measured by the after filter below stage 9 of the MOUDI
#
PM2.5,M is the mass concentration measured by MOUDI.

Table 2. 3-year average concentration ratios of chemical species to PM2.5 and UFPs at ZS, SJ, and JD stations.
3-year avg. (%)
UFPs CM TE Ions OM EC Total
ZS 9.0 ± 7.4 3.2 ± 0.9 15.2 ± 1.6 N.A. N.A. 27.9
SJ 8.5 ± 7.7 3.2 ± 1.3 19.2 ± 1.5 N.A. N.A. 30.9
JD 9.5 ± 8.3 4.5 ± 1.0 21.0 ± 2.1 N.A. N.A. 35
PM2.5 CM TE Ions OM EC Total
ZS 8.3 ± 8.0 4.3 ± 3.6 37.8 ± 4.1 21.9 ± 15.5 8.3 ± 8.4 80.6
SJ 8.4 ± 6.2 3.0 ± 1.4 40.0 ± 3.0 30.4 (2011–2012) 6.7 (2011–2012) 88.5
JD 10.6 ± 8.8 3.0 ± 1.8 46.4 ± 1.6 17.6 (2013) 6.5 (2013) 84.1
Roadside (Chen et al., 2010b)
CM+TE Ions OM EC Total
UFPs 11.3 ± 3.3 24.8 ± 9.3 38.7 ± 3.3 16.1 ± 7.5 89.29
PM2.5 7.8 ± 2.0 36.2 ± 6.5 37.5 ± 9.7 8.6 ± 2.3 88.1

± 15.5 and 8.3 ± 8.4% of PM2.5, respectively. Reconstructed
mass concentration is 80.4% of PM2.5 mass concentration.
From 2011 to 2012 at SJ station, 2-year average of OM is
30.4% of PM2.5, while EC contributes 6.7% to PM2.5. Based
on the above results, the summation of CM, TE, Ions, OM,
and EC at SJ station is 88.5% of PM2.5. In 2013 at JD
station, OM and EC is 17.6 and 6.5% of PM2.5, respectively.
The summation of all chemical species is 84.1% PM2.5.
Therefore at all three different stations, the chemical mass
closures for PM2.5 are shown to be good. A slight
disagreement between reconstructed mass and measured
PM2.5 was partly because of negative artifact caused by the
loss of semi-volatile material (SVM) during sampling (Liu
et al., 2013, 2014). The evaporation of PM2.5 concentration
was found to increase with increasing temperature and
decreasing relative humidity, decreasing PM2.5 concentration
and gas-to-particle ratio (Liu et al., 2015). This issue is worth
studying in the future.
PM2.5 and UFPs Seasonal Variation of Mass Distribution
Figs. 5(a)–5(c) and Fig. S1 of Supplementary Materials
show seasonal average mass distributions at ZS, SJ, and JD
stations from 2011 to 2013. In the 3-year average mass
distributions all stations show diurnal bimodal distributions
except those at ZS station in spring 2011 (Fig. 5(b)) and SJ
station in summer 2012 (Fig. 5(c)). In Fig. 5(a), the 3-year
average accumulation and coarse mode mass median
aerodynamic diameters (MMAD) were 0.40 and 5.64 µm
at ZS station, 0.44 and 5.47 µm at SJ station, and 0.42 and
5.38 µm at JD station, respectively. No significant difference
was found all stations. In spring 2011 at ZS station (Fig. 5(b)),
the MMAD was measured to be 0.89 µm, which was larger
than the average MMAD due to the impact of sandstorm
event from Inner Mongolia Autonomous Region which
also transported PM2.5 from China. In summer 2012 at SJ
station (Fig. 5(c)), the mass distribution shows a single coarse
mode with a relatively low mass concentration compared
to other seasons. Large MMAD of 6.34 µm could be
attributed to the influence of sea salt transported by Typhoon
Tembin. Na+ and Cl- concentrations in PM2.5 were both
0.35 µg m–3 in August 2012, which were higher than the
average concentration of 0.19 µg m–3 in 2012, provided
further evidence of sea salt transported by Typhoon Tembin.
At ZS and SJ stations, the peak concentration of the
accumulation mode is slightly higher than that of the coarse
mode, while the coarse mode concentration is higher than
that of the accumulation mode at JD station. Again, it is
because ZS and SJ stations are more influenced by the
UFPs emitted from traffic and industries than JD station.
Number Size Distributions of Particles with dp ≤ 209 nm
Fig. 6 shows calculated ρ eff,i and χi based on the
experimental data measured at ZS station. The average ρeff,i
at ZS station was 0.68 ± 0.16 g cm–3 for UFPs (Fig. 6(a))
and 1.06 ± 0.32 g cm–3 for PM0.1–0.18 (Fig. 6(b)), while χi was
2.06 ± 0.19 and 1.45 ± 0.16 for UFPs (Fig. 6(a)) and
PM0.1–0.18 (Fig. 6(b)), respectively. Calculated χi at ZS were
larger than 1.0, suggesting that the shape of particles was
 Lin et al., Aerosol and Air Quality Research, 15: 2305–2319, 2015  2313

(a) (b)

(c)
Fig. 5. Seasonal average mass distribution at ZS, SJ, and JD stations from 2011 spring to 2013 autumn.

(a) (b)
Fig. 6. ρeff and χ for (a) UFPs and (b) PM0.1–0.18 at ZS station in 2014.
2314 Lin et al., Aerosol and Air Quality Research, 15: 2305–2319, 2015
Fig. 7. TEM images of particles sampled at ZS station on Dec. 9, 2014.
irregular (DeCarlo et al., 2004). This conclusion could be
proven by the TEM images of UFPs sampled by using a
personal nanoparticle sampler (PENS) (Tsai et al., 2012) at
ZS station, as shown in Fig. 7. Results of EDX (Energy-
dispersive X-ray spectroscopy) analysis shown in Table S2
of Supplementary Materials indicated that C was the most
abundant composition of all elements (74.16–90.56% by
weight) in nanoparticles, followed by Cu (4.19–9.03%), O
(1.15–3.67%), Al (0–12.89%), and Si (0.5–2.04%),
suggesting that OM was the major constituent in UFPs. The
chemical compositions of CE at ZS station were different
from those measured by using EDX in India, where the
Mg/Al, Si/Al, K/Al, Ca/Al, Mn/Al, and Fe/Al were 0.44 ±
0.22, 1.96 ± 0.90, 0.65 ± 0.22, 1.52 ± 0.40, 0.84 and 1.54 ±
1.67, respectively (Agnihotri et al., 2015).
Fig. 8 shows daily average particle number concentrations
at ZS (Fig. 8(a)), SJ (Fig. 8(b)), and JD stations (Fig. 8(c)).
ρeff,i and χi obtained at ZS station were assumed applicable
for calculating number concentrations at the other two stations
because the difference in 3-year average concentration ratios
of chemical species to PM2.5 and UFPs (Table 2) and seasonal
average mass distribution among three stations (Fig. 5) were
not significant. In three year period, UFPs daily average
 
number concentration was 1.7 ± 0.8 × 104, 1.4 ± 0.6 × 104,
and 1.2 ± 0.6 × 104 # cm–3, respectively, while PM2.5 daily
average number concentration was 1.8 ± 0.8 × 104, 1.6 ±
0.6 × 104, and 1.3 ± 0.6×104 # cm–3 at ZS, SJ, and JD
stations, respectively. The UFP concentration determined at
ZS station was very close to 1.7 ± 1.4 × 104 # cm–3 measured
at National Taiwan University in 2012 by Cheung et al.
(2013). The variation of UFP number concentrations with
different seasons and stations is apparent in Fig. 8. It shows
UFP concentration is more abundant in ZS than SJ
station and the least abundant in JD station, reflecting the
influence of different traffic emissions at these stations.
The UFP concentration is elevated in summer and spring
than that in winter and autumn in all stations. In
comparison, the trend of PM2.5 mass concentration is
different with summer being the lowest and winter being the
highest. This suggests that secondary aerosol formation in
warm seasons is the major cause for the increase in UFP
number concentrations.
Fig. 9 shows the average ratio of UFPs/PM2.5 for mass,
surface area, and number concentration at ZS (Fig. 9(a)),
SJ (Fig. 9(b)), and JD stations (Fig. 9(c)) from 2011–2013.
Although UFPs mass concentration was only 7.9 ± 4.4% of
 Lin et al., Aerosol and Air Quality Research, 15: 2305–2319, 2015  2315

(a)

(b)

(c)
Fig. 8. Daily average particle number concentration from 2011 spring to 2013 autumn at (a) ZS, (b) SJ, and (c) JD stations.
2316 Lin et al., Aerosol and Air Quality Research, 15: 2305–2319, 2015 

(a)

(b)

(c)
Fig. 9. Average concentration ratio of UFPs to PM2.5 for mass, surface area, and number concentration at ZS (Fig. 9(a)), SJ
(Fig. 9(b)), and JD stations (Fig. 9(c)) from 2011 spring to 2013 autumn.
 Lin et al., Aerosol and Air Quality Research, 15: 2305–2319, 2015  2317
PM2.5 in 3-year average of all stations, the UFPs/PM2.5
ratios for surface area and number concentration were as
high as 42.1 ± 12.8% and 89.0 ± 5.5%, respectively. The
dependence of the ratios on different stations and seasons
is also similar to that in Fig. 8 with ZS having the highest
UFPs/PM2.5 ratio. The 3-year average UFPs/PM2.5 number
concentration ratio was shown to be comparable to 81 ± 8%
and 89.0 ± 5.5% during cold and warm periods, respectively,
measured at urban sampling stations in central Taiwan
(Young et al., 2012). This result reveals that UFPs contribute
significantly to particle number but also to surface area in
PM2.5 in the urban air. Long term measurements for physical
and chemical properties of UFPs in the atmosphere should
be further conducted for better health risk assessment in
the future.
CONCLUSION
This study investigated the long term daily average mass
concentrations UFPs and PM2.5 from 2011 spring to 2013
autumn at Zhongshan (ZS), Sinjhuang (SJ), and Jhudong
(JD) air monitoring stations. Particle number distributions
at ZS station in 2014 were further measured by using a
Scanning Mobility Particle Sizer (Model 3936, TSI
Incorporated, St. Paul, MN, USA, SMPS) to examine the
effective density (ρeff) and dynamic shape factor (χ) of
UFPs. The results showed that heavy traffic emission and
new particle formation event resulted in higher UFPs mass
concentrations in spring and summer than those in autumn
and winter. Based on the calculated average ρeff (0.68 ± 0.16
g cm–3) and χ (2.06 ± 0.19), the number and surface area
concentration ratios of UFPs/PM2.5 at urban air monitoring
stations were found to average 89.0 ± 5.5% and 42.1 ±
12.8%, respectively, and varied by seasons and stations. This
suggests that UFPs contribute significantly to the health-
relevant PM2.5 fraction and warrant serious attention in the
future.
ACKNOWLEDGEMENT
The financial support of the Taiwan Environmental
Protection Agency (EPA-103-1602-02-09) is gratefully
acknowledged.
SUPPLEMENTARY MATERIALS
Supplementary data associated with this article can be
found in the online version at http://www.aaqr.org.
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Received for review, April 29, 2015
Revised, August 16, 2015
Accepted, August 23, 2015