This study was designed to contribute to initiate the researches of nanoparticles in Viet
Nam. Mass concentrations, number concentration and WSOC of NPs at a mixed site of Ha Noi
in the rainy season and the dry season were determined. The mass concentrations of
nanoparticles were 4.76 µg/m3 to 5.42 µg/m3 while the number concentrations of these particles
were 2.59 × 104 – 3.54 × 104 particles/cm3. The average concentrations of WSOC in the rainy
and dry season were 1.51 µg/m3 and 1.09 µg/m3, respectively. The relationship between WSOC
and other components, particularly WIOC, OC, EC, char – EC, soot – EC were used to primarily
identify the sources of emission. The good positive correlations of WIOC with OC, EC, and char
– EC (with R2 = 0.94, 0.71, 0.73, respectively) in the rainy season; and the moderate correlations
of WSOC with OC and EC (R2 = 0.43, 0.58, respectively), and of WIOC with OC (R2 = 0.60) in
the dry season were found. From these findings, a higher SOA was anticipated in the dry season.
These results showed the good agreement with the EC – tracer method, in which SOA was
accounted for 21.67 % and 41.20 % in the rainy and dry season, respectively.
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Vietnam Journal of Science and Technology 55 (6) (2017) 745-755
DOI: 10.15625/2525-2518/55/6/9618
LEVELS AND WATER SOLUBLE ORGANIC CARBON OF
ATMOSPHERIC NANOPARTICLES IN A LOCATION OF HA NOI,
VIET NAM
Nguyen Thi Thu Thuy1, 2, Nghiem Trung Dung1, *, Kazuhiko Sekiguchi3,
Ryosuke Yamaguchi3, Ly Bich Thuy1, Nguyen Thi Thu Hien1
1School of Environmental Science and Technology, Hanoi University of Science and Technology,
1 Dai Co Viet, Ha Noi, Viet Nam
2Faculty of International Training, Thai Nguyen University of Technology, 3/2 Road,
Thai Nguyen, Viet Nam
3Graduate School of Science and Engineering, Saitama University,
225 Shimo-Okubo Sakura, Saitama, Japan
*Email: dung.nghiemtrung@hust.edu.vn
Received: 10 April 2017; Accepted for publication: 16 June 2017
Abstract. Atmospheric nanoparticles (NPs or PM0.1) were investigated at a site inside the
campus of Hanoi University of Science and Technology (HUST) in Hanoi, Viet Nam. The
sampling was conducted during a rainy season (August, 2015) and a dry season (October to
December, 2015). Mass was weighed by an electronic micro-balance, Sartorius ME2, 10-6 g.
Number concentrations were measured by an electrical mobility spectrometer (NanoScan, SMPS
TSI Model 3910). Water soluble organic carbon (WSOC) was analyzed by a total carbon
analyzer (TOC-VCHP, Shimazu). The correlations between WSOC and other components were
studied to primarily identify the sources of atmospheric nanoparticles. Secondary organic carbon
(SOA) was estimated using elemental carbon (EC) – tracer method. Selected characteristics of
nanoparticles including mass concentrations, number concentrations, and WSOC were
determined.
Keywords: nanoparticles, mass concentration, number concentration, WSOC, SOA, Ha Noi.
1. INTRODUCTION
Recently, the scientific community has high concern about nanoparticles (NPs), which are
considered to give probably adverse impacts on human health [1], visibility and climate change
[2]. Such negative impacts could be attributed by: (i) a tiny size that can penetrate deeply and
accumulate in the organs of our bodies, (ii) a very high number concentration, and (iii) a greater
specific surface area that can be bounded by toxic compounds. Therefore, it is important to gain
the best understanding about the species’ concentrations of NPs to assess these effects.
Nguyen Thi Thu Thuy, et al.
746
Organic carbon (OC) is one of the most dominant components of atmospheric
nanoparticles, representing 30 – 73 % of the total mass concentration [3, 4]. Organic aerosols
either can be emitted to the atmosphere as primary organic ones or are formed in the atmosphere
through gas-to-particle conversion processes (secondary organic aerosols - SOA). While it is
complicated to estimate directly the level of SOA, water soluble organic carbon (WSOC) can be
used as an indicator of the formation of SOA because SOA compounds contain polar functional
groups (e.g. hydroxyl, carbonyl, and carboxyl) [5] that attribute to the water-soluble
characteristics of SOA. Although WSOC can come from primary sources such as motor
vehicles, fossil fuel combustion, and biomass burning, WSOC has been used as a tracer for SOA
because the major fraction of SOA is associated with WSOC. In addition to its potential as a
general tracer for biomass burning emission and SOA, WSOC may influence regional climate
[6] and human health [7]. For these reasons, it is important to get the comprehensive knowledge
about WSOC.
Most previous studies of WSOC have generally focused more strongly on suspended
particulate matter (TSP), PM10 and, more recently, on PM2.5 [5, 6]. The investigations on WSOC
of nanoparticles are very few, especially in developing countries. To the best of our knowledge,
publications conducted in Viet Nam on NPs, the higher potential particles to human health and
environment, are very scarce [8 - 10]. Moreover, no data on WSOC of NPs in the country are
available in the open literature. To fill the data gap in mass concentration, number concentration,
and WSOC of NPs in this region, this study is, therefore, aimed at: (i) the determination both
mass and number concentrations of NPs, (ii) the determination of the characteristics of
atmospheric WSOC in NPs in Viet Nam, in which the relationships between WSOC and other
carbonaceous components will be analyzed deeply. These relationships would be valuable to
examine the possible emission sources of NPs in the atmosphere.
2. MATERIALS AND METHODS
2.1. Study area
Ha Noi, located in the Red River delta in the North Viet Nam (21.021N, 105.851E), about
100 km west of the East Sea, is the capital of Viet Nam and the second largest city in the
country. Ha Noi has a tropical monsoon climate with two monsoon seasons. The area is under
the influence of northeast monsoon during winter while being under the influence of southeast
monsoon during summer. From October to December, continental air masses flow coming from
the inland of China brings dry and cold air. From January to March/ April, maritime airflow
traveling a long way over the Pacific Ocean brings warm, humid and better dispersion
conditions. In summer, air masses coming from the Highs over the Indian Ocean and the
subtropical High over the East Sea bring moist air and monsoon rains. However, heavy rains
mainly occur in July and August in association with tropical depressions. The mean annual
rainfall in Ha Noi is 1800 mm, 80 % of which are recorded from May to September [11].
In order to investigate the characteristics of NPs in Ha Noi, a sampling site located at the
3rd floor of the Center of Foreign Languages, Ha Noi University of Science and Technology
(HUST) (21o00.17 N and 105o50.37 E) was chosen (Figure 1). This sampling site can be
considered as a mixed site affected by several activities including transportation, construction,
domestic cooking, and laboratory etc. All those sources can contribute to the levels and
compositions of NPs.
Levels and water soluble organic carbon of atmospheric nanoparticles in a location of Ha Noi...
747
Sampling was conducted during the
wet season and the dry season. These
sampling periods were selected so that the
influence of seasonal reversing winds with
temperature and relative humidity
characteristics corresponding to the seasons
in Ha Noi, Viet Nam, could be observed.
Figure 1. Location of sampling site in Ha Noi.
2.2. Sampling and analytical method
An inertial fibrous filter (INF) sampler (the newest version KU – TSC 26A57C1,
Kanazawa University) with a design airflow of 40.0 L/min was used to collect NPs. The INF
sampler consists of four impaction stages that collect particles with equivalent diameters of 10,
2.5, 1.0, and 0.5 µm. The system also has one inertial filtration stage composed of unwoven
stainless steel fibers for collecting particles larger than 0.1 µm after the four impaction stages.
NPs are collected uniform on to a 55 mm quartz fiber filter (2500 QAT – UP, Pallflex, CT,
USA).
The 24-h sampling duration was conducted in August (rainy season) and from October to
December (dry season) of 2015. Seventeen samples and 3 blank samples were collected for the
rainy season; and 28 samples and 7 blank samples were collected for the dry season,
respectively. Flow rates of the sampler and meteorological parameters, including wind direction
and velocity, temperature and humidity, were measured every hour during sampling. Some
meteorological data are shown in Table 1.
Table 1. Meteorological data.
Average
temperature
(o C)
Average
relative
humidity (%)
Average wind
speed (m/s)
Prevailing
wind
direction
Number of rainy
days
Rainy season 30.0 74.9 2.7 SSE 2/17 sampling days
Dry season 24.7 77.8 2.8 E 8/28 sampling days
Quartz fiber filters were pre-baked at 900 oC for four hours to remove possible
contamination [12]. To determine the mass of NPs, the filters were weighed on an electronic
micro-balance, Sartorius ME2, 10-6 g, before and after field sampling. Prior to being weighed,
the filters were equilibrated in the balance room for at least 24 hours. The balance room’s
relative humidity was maintained at a mean value range of 30 – 40 % and the temperature was
kept from 20 – 23 oC [13]. After weighing, each quartz filter was put in a Petri dish and kept in a
separate airtight bag. The samples were frozen at Ha Noi University of Science and Technology
and were transported in a dry ice box to the Saitama University’s laboratory in Japan for OC/EC,
WSOC analyses.
A quarter of each sample filter was extracted with 10 mL pure water for WSOC analyses.
After the samples were ultrasonically extracted, they were filtered (pore size, 0.2 µgm) and the
solute was injected to total carbon analyzer (TOC-VCHP, Shimazu Corp., Japan) to determine the
concentration of WSOC.
Nguyen Thi Thu Thuy, et al.
748
A 0.503 cm2 sample punched out from the quartz fiber filter was used to determine OC and
EC using a thermal/optical carbon analyzer (DRI model 2001, Atmoslytic Inc, Calabasas, CA,
USA). Temperature was set up with the IMPROVE method with four OC fractions (OC1, OC2,
OC3, OC4 at 120, 250, 450, and 550 oC, respectively in a non-oxidizing helium atmosphere) and
three EC fractions (EC1, EC2, and EC3 at 550, 700, and 800 oC, respectively in an oxidizing
helium atmosphere of 2 % O2 and 98 % of helium). The pyrolysis of OC (POC) was
continuously monitored by reflectance or transmittance of laser signal. OC is operationally
defined as OC1 + OC2 + OC3 + OC4 + POC, and EC is defined as EC1 + EC2 + EC3 – POC.
The EC fraction was divided into char-EC and soot-EC [14-15]. Char-EC is defined as EC1
minus POC, and the soot–EC is defined as the sum of EC2 and EC3 [16].
An electrical mobility spectrometer (NanoScan, SMPS TSI Model 3910; sample flow rate
0.6 L min−1) was utilized to measure the particle mobility size distribution in 13 channels from
10 to 420 nm mobility diameter. Time resolution was 1 minute. During each season, 30 samples
were conducted. The spectrometers generally include an electrostatic classifier, where particles
are electrically charged/neutralized and then classified according to their electrical mobility and
a condensation particle counter, where particles, previously classified, are counted.
3. RESULTS AND DISCUSSIONS
3.1. Levels of PM0.1 and WSOC
Mass concentrations
The mean concentrations of mass, carbonaceous species (EC, OC, and WSOC) are
summarized in Table 2, together with the median, minimum and maximum concentrations of the
chemical species.
Generally, mass and WSOC concentrations of NPs in the rainy season were slightly higher
than those in the dry season. The average mass concentrations of nanoparticles in the rainy season
and the dry season were 5.42 ± 2.24 µg/m3 and 4.76 ± 1.67 µg/m3 respectively, while the WSOC
concentrations of those were 1.51 ± 0.31 µg/m3 and 1.09 ± 0.29 µg/m3. These results might be
explained by the different number of rainy days in the two sampling periods as shown in Table 1.
Table 2. Average mass and carbonaceous concentrations.
Rainy season (4th – 20th Aug. 2015),
n = 17 samples, µg/m3
Dry season (4th Nov – 1st Dec. 2015),
n = 28 samples, µg/m3
Mean Median Range Mean Median Range
Mass 5.42 4.99 2.38 – 11.8 4.76 4.30 1.85 – 9.13
WSOC 1.51 1.57 0.90 – 2.11 1.09 1.06 0.51 – 1.83
WSOC/OC 0.66 0.69 0.24 – 0.97 0.59 0.62 0.28 – 0.76
WIOC 1.06 0.61 0.05 – 4.57 0.76 0.71 0.36 – 2.14
WIOC/OC 0.34 0.31 0.03 – 0.76 0.41 0.38 0.26 – 0.72
(WIOC: water in-soluble organic carbon, WIOC = OC – WSOC).
The nanoparticle concentrations obtained are compared with those of others studies as
shown in Table 3. Disparities of nanoparticle concentrations support the likelihood of site-
specific differences such as sampling period and location. It may be needed to know the
Levels and water soluble organic carbon of atmospheric nanoparticles in a location of Ha Noi...
749
concentrations of nanoparticles at different time periods under various environmental conditions
to get a better understanding about the level of nanoparticles in the atmosphere. However, the
mass concentrations of NPs in Viet Nam were roughly from 2 to 10 times higher than those in
other urban sectors. To answer the questions such as what are the main sources that make the
contribution to the higher concentration of NPs in Viet Nam, what are the effects of these higher
concentrations on human health and environment, the further studies of NPs in Viet Nam are
needed to investigate.
Table 3. Concentrations of NPs at different locations.
Studies Location Site feature Concentration (µg/m3)
This study HUST, Ha Noi Mixed 4.76 – 5.42
Thuy et al. [8] Gia Lam, Ha Noi Traffic 6.40 – 9.70
Cass et al. (2000) [3] California, US Urban – industrial 0.60-1.20
Gugamsetty (2012) [17] Taiwan Urban – industrial 1.40 ±0.60
Pakkanen et al. (2001) [18] Finland Rural 0.52
Pakkanen et al. (2001) [18] Finland Urban 0.49
Mbengue et al. (2014) [19] Dunkrink, France Industrial 0.80
Mbengue et al. (2014) [19] Dunkrink, France Urban – industrial 0.50
Chen et al. (2010) [4] Hsinchu, Taiwan Traffic 2.21± 0.59
Chen et al. (2010) [4] Hsinchu, Taiwan Forest 0.65± 0.31
Chen et al. (2010) [4] Hsinchu, Taiwan Tunnel 33.2±6.5
Kim et al. (2002) [20] Los Angeles, US Riverside 1.34
Kim et al (2002) [20] Los Angeles, US Urban 4.11
Number concentrations
The mass concentrations of the particles smaller than 100 nm, which actually dominate the total
particle number concentrations in urban areas, are negligible. Therefore, accompany with mass
concentration, number concentrations and size distributions are often measured when studying NPs.
Figure 2 shows the distribution of average particle sizes measured at the sampling site.
The average particle number concentrations of the nucleation mode (3–20 nm), Aitken
mode (20–100 nm), and accumulation mode (> 100 nm) are 3,836 particles/cm3, 27,340
particles/cm3, and 3,885 particles/cm3, respectively. The particle number concentration of the
Aitken mode is obviously higher than those of the other modes. Since the majority of particle
number from vehicle exhaust is in the size range of 20 – 130 nm for diesel engines and 20–60
nm for gasoline engines [21-23], the very high number concentration in Aiken mode (71%)
indicates the influence of traffic emissions in the study area.
The average number concentrations in this study were compared with others conducted in
different conditions (Figure 3). Overall, 43 roadside sites, 6 urban sites, and 2 urban background
studies were calculated to get the mean values of each site [4, 21 - 24]. The average
concentration of particles below 100 nm (with an average value of 31,117 particles/cm3) in
HUST is about 2.6 times higher than those in the urban background sites, and was close to those
in the urban sites. The mean value of number concentrations of NPs in this study is lower than
that of roadside sites. However, the number concentrations in reference studies had a huge range
(from 8,020 to 600,000 particles/cm3), in which the values from 20,000 to 40,000 particles/cm3
reached to 48.83 % (21/43 values). One reason might be that these studies were conducted with
Nguyen Thi Thu Thuy, et al.
750
different distances from the road kerb, different duration, and different samplers. Therefore,
results obtained in this study can be considered in the same range with those of other studies in
the urban and roadside environment.
Figure 2. Distribution of number concentration of
NPs.
Figure 3. Mean and median particle number
concentrations for different environments.
3.2. Relationships between WSOC and carbonaceous components
Rainy season Dry season
Figure 4. Temporal variations of WSOC, WIOC, EC, and OC in the rainy and dry season.
WSOC can account for 40 to 80 % of the total organic carbon, depending on the location
and season [5, 6, 16, 25]. As shown in Table 2 and Figure 4, the WSOC concentrations in
aerosols in this study ranged from 0.90 to 2.11 µg/m3 (Av: 1.51 µg/m3) in the rainy season and
0.51 to 1.83 µg/m3 (Av: 1.09 µg/m3) in the dry season, i.e. 1.4 times higher in rainy season. The
WSOC abundance contributes 66.5 % and 58.7 % of OC in the rainy season and the dry season,
respectively. The concentrations of WSOC in the rainy season were higher than those in the dry
season. The relatively low WSOC concentrations observed in the dry season might be due to the
abnormal rainfall during this sampling period. The mass and carbonaceous concentrations of
particles were also relatively low in this season, and that decline might also be due to anomalous
rain showers.
The WSOC/OC ratios ranged from 0.59 µg/m3 to 0.66 µg/m3 while the WIOC/EC ratios were
around 2.30 µg/m3. Typically, both WSOC and WIOC concentrations in this study are two times
higher than those of other studies; whereas the WSOC/OC and ratios can be considered to be stable
at all locations as shown in Table 4.
Levels and water soluble organic carbon of atmospheric nanoparticles in a location of Ha Noi...
751
Table 4. WSOC, WIOC and their ratios with carbonaceous concentrations of NPs of different locations.
Site Sampling location WSOC WIOC WSOC/OC WIOC/EC
This study Ha Noi (mixed site) 1.09 – 1.51 0.76 – 1.06 0.59 – 0.66 2.30
Japan [16] Saitama (roadside) 0.45 – 0.60 0.40 – 0.59 0.47 – 0.62 2.74 – 4.00
Germany [14] Berlin (roadside) 0.54 0.59 0.50 4.6
US [15] New York (rural area) 0.66 N/A N/A N/A
WSOC and WIOC concentrations showed significant site-to-site variability that indicates
the influence of local primary sources of WSOC, such as biomass burning, or differences in the
emissions of precursors to the secondary organic aerosol formation. However, the consistent
WSOC/OC ratios can be found corresponding to a certain location and season.
a) Correlations of WIOC with OC a) Correlations of WSOC and OC
b) Correlations of WIOC and EC b) Correlations of WIOC and EC
c) Correlations of WIOC with char-EC c) Correlations of WIOC and OC
Figure 5. Correlations of WIOC with OC, EC, and
char-EC in the rainy season.
Figure 6. Correlations of WSOC with OC and EC;
WIOC and OC in the dry season.
Nguyen Thi Thu Thuy, et al.
752
In order to primarily identify the sources of NPs, the deeper relationships between WSOC,
WIOC, OC, EC, char – EC, and soot – EC were investigated. While EC originates from the
burning of carbonaceous matter, OC may be emitted directly in the particulate phase or formed
from a gas-to-particle conversion process in the atmosphere [26]. WSOC can be produced from
both primary and secondary emissions, most of WIOC in urban areas were likely formed via
incomplete combustion of fossil fuels [27]. Char – EC is formed when carbonaceous material is
partially burned or heated with a limited supply of air; whereas, soot – EC was formed at high
temperature via gaseous phase processes [28]. Therefore, analysis the relationships between
them will help us have useful indicators for source identification.
The significant positive correlations between WIOC with OC, EC, and char – EC as shown
in Figure 5a, Figure 5b, and Figure 5c, respectively for the rainy season indicates that the main
sources of OC were primary OC; whereas the found correlations between WSOC with OC, and
EC, and between WIOC with OC as presented in Figure 6a, Figure 6b, and Figure 6c,
respectively for the dry season shows the higher contribution of secondary emission in this
season.
3.3. Estimation of secondary OC concentration
OC can be either emitted directly by primary sources (primary OC) or formed by
condensation of low-volatility products from the photochemical oxidation of gaseous organic
precursors [29]. To establish a control strategy for particulate matter pollution, the contributions
of primary and secondary OC to the total OC needs to be estimated.
The SOA fraction in aerosol is either estimated using the EC - tracer method [30] or by
adding up all the oxidation products found in aerosols [25]. In this study, EC – tracer method
was used to estimate the contribution of SOA to the measured OC. This technique has been used
to distinguish primary OC from secondary OC in numerous studies. The underlying hypothesis
is that because EC and primary OC often have the same sources, there is a representative ratio of
primary OC/EC for a given area (hereafter referred to as [OC/EC]pri). Herein, the primary
organic carbon concentrations, [OC]pri, were estimated as follows:
[OC]pri = [OC/EC]pri[EC] + [OC]NC
where [OC]pri is the primary organic aerosol concentration, [OC/EC]pri is the ratio of OC to EC
for the primary sources, and [OC]NC is the non-combustion contribution to the primary OC.
Then, the secondary organic carbon (SOA) concentration, [OC]sec, is simply the difference
between the measured total [OC], [OC]tot, and the estimated primary [OC]pri.
[OC]sec = [OC]tot - [OC]pri
Numerous methods for determining the value of [OC/EC]pri and [OC]NC have been used in
previous studies. Castro et al. (1999) reported that the consistent presence of a clear minimum
ratio for OC/EC in urban and rural areas, in winter and summer, suggests that samples having the
lowest OC/EC ratios contain almost exclusively primary carbonaceous compounds [31]. For this
work, we assumed that the values of 4.45 and 3.35 for (OC/EC)min observed in the rainy and dry
season, respectively were used as [OC]pri and the concentration of primary non-combustion
contribution was negligible. If primary non-combustion OC had contributed to the observed OC,
the estimated secondary OC concentration would be overestimated. Based on this approach,
SOA was been estimated about 0.56 µg/m3 and 0.76 µg/m3 in the rainy and dry season,
respectively, accounting for 21.67 % and 41.20 % of the measured OC. These results showed
good correlations with the primary prediction of sources as presented in Section 3.2.
Levels and water soluble organic carbon of atmospheric nanoparticles in a location of Ha Noi...
753
4. CONCLUSIONS
This study was designed to contribute to initiate the researches of nanoparticles in Viet
Nam. Mass concentrations, number concentration and WSOC of NPs at a mixed site of Ha Noi
in the rainy season and the dry season were determined. The mass concentrations of
nanoparticles were 4.76 µg/m3 to 5.42 µg/m3 while the number concentrations of these particles
were 2.59 × 104 – 3.54 × 104 particles/cm3. The average concentrations of WSOC in the rainy
and dry season were 1.51 µg/m3 and 1.09 µg/m3, respectively. The relationship between WSOC
and other components, particularly WIOC, OC, EC, char – EC, soot – EC were used to primarily
identify the sources of emission. The good positive correlations of WIOC with OC, EC, and char
– EC (with R2 = 0.94, 0.71, 0.73, respectively) in the rainy season; and the moderate correlations
of WSOC with OC and EC (R2 = 0.43, 0.58, respectively), and of WIOC with OC (R2 = 0.60) in
the dry season were found. From these findings, a higher SOA was anticipated in the dry season.
These results showed the good agreement with the EC – tracer method, in which SOA was
accounted for 21.67 % and 41.20 % in the rainy and dry season, respectively.
Acknowledgments. Kanazawa University, Japan is acknowledged for providing the sampler (KU – TSC
26A57C1) for this study.
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