Atmospheric Environment xxx (2012) 1e8

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Atmospheric Environment
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Effects of local, regional meteorology and emission sources on mass and

compositions of particulate matter in Hanoi
Cao Dung Hai 1, Nguyen Thi Kim Oanh*
Environmental Engineering and Management, School of Environment, Resource and Development, Asian Institute of Technology, Thailand

h i g h l i g h t s

< PM2.5 and PM10e2.5 were investigated during polluted winter period in Hanoi.
< Variation in PM mass and composition were analyzed with meteorology and emission.
< Reconstructed mass and PMF model were used for source identication and apportionment.
< Contribution of local sources and long range transport to PM2.5 were analyzed.

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

Article history: Intensive monitoring for PM mass and composition was conducted during December 2006eFebruary
Received 2 October 2011 2007 at a mixed site in Hanoi, Vietnam. Fluctuations in levels of 24 h PM2.5 (26e143 mg m
3) and
Received in revised form PM10 (37e165 mg m
3) were examined in relation to weather conditions and regional synoptic patterns.
26 April 2012
High 24 h PM levels were observed at low wind speeds when a stagnating ridge governed over Northern
Accepted 3 May 2012
Vietnam. Diurnal variations of PM mass and composition, analyzed using 4 h-samples, reected the
inuence of local emissions with peaks of PM mass and EC/OC observed during morning and evening
Keywords:
rush hours. The 24 h EC and OC levels in PM2.5, 1.5e4.9 mg m
3 and 10e39 mg m
3, respectively,
Fine particulate matter


EC/OC
constituted about 90% of the total EC and OC in PM10. Ionic species (SO2
4 , NO3 , NH4 , Cl and K ) were
Diurnal variation the major composition of PM2.5, whereas elements (Ca, Si, Al and Fe) were the major components in the
Meteorology coarse fraction (PM10e2.5). The reconstructed mass, explained 78  11% of PM2.5 and 61  11% of PM10e2.5,


Source apportionment suggested signicant contributions of secondary PM (OM, SO2
4 , NO3 and NH4 ) and combustion
Hanoi (biomass, diesel, etc.) to PM2.5. PMF model revealed 7 source factors of PM2.5: secondary mixed PM (40%),
diesel trafc (10%), residential/commercial cooking (16%), secondary sulfate rich (16%), aged seasalt
mixed (11%), industry/incinerator (6%), and construction/soil (1%). Contributions from local emission
sources and the potential long-range transport were analyzed using the PM compositions and the diurnal
variations in relation to local source activities, location of local sources, winds and air mass HYSPLIT
trajectories. Major part of PM2.5 mass appeared to link to local emission origins. Additional measurement
data are required to characterize the weekendeweekday and inter-seasonal patterns of PM.
2012 Elsevier Ltd. All rights reserved.

1. Introduction of these effects depends on PM size and compositions. Fine parti-

Atmospheric particulate matter (PM) is the most notable air
pollution problem in developing Asian cities (Gupta et al., 2006;
Tsai and Chen, 2006; Hopke et al., 2008; Kim Oanh et al., 2006). PM
gets increasing attention because of the adverse effects on human
health, the atmosphere and climate (Bond et al., 2004). The extent
* Corresponding author.
E-mail address: kimoanh@ait.ac.th (N.T. Kim Oanh).
1
Current address: Petrovietnam Overseas Exploration Production Operating
Company, Hanoi, Vietnam.
cles measured as PM2.5 (particles with the aerodynamic diameter
2.5 mm) can penetrate the lungs deeper than large particles, hence
are more damaging (Pope et al., 2009).
Systematic PM records, however, remain limited in Asian
developing countries, especially for PM2.5. Until recently, available
national monitoring networks focused more on the total suspended
PM (TSP) but at present PM10 (particles with the aerodynamic
diameter  10 mm) is also monitored routinely in many countries
(HEI, 2010). Available data show high levels of PM in Asian cities
that often exceeded the respective national ambient air quality
standards (NAAQS). In particular, PM2.5 and PM10 normally exceed

1352-2310/$ e see front matter 2012 Elsevier Ltd. All rights reserved.
doi:10.1016/j.atmosenv.2012.05.006

Please cite this article in press as: Hai, C.D., Kim Oanh, N.T., Effects of local, regional meteorology and emission sources on mass and compo-
sitions of particulate matter in Hanoi, Atmospheric Environment (2012), doi:10.1016/j.atmosenv.2012.05.006
2 C.D. Hai, N.T. Kim Oanh / Atmospheric Environment xxx (2012) 1e8
the 24 h WHO air quality guidelines by a factor of two or more
(Hopke et al., 2008; Kim Oanh et al., 2006).
In Vietnam, in the past only TSP was measured and over a short
sampling period (e.g. 1 h) but recently PM10 mass is continuously
monitored in some urban areas by a network of automatic stations.
Data on PM2.5 have been made available through research projects
(Hien et al., 2001, 2002; Kim Oanh et al., 2006) and commonly show
high levels in large cities. In Hanoi, the capital city of Vietnam,
higher PM levels are observed during the dry season which can be
explained by high emission strength and limited atmospheric
dispersion (Kim Oanh et al., 2006). Some data on PM2.5 mass and
composition have been reported earlier (Hien et al., 2004; Kim
Oanh et al., 2006) but mainly based on 24 h PM sampling. This
paper presents the results of more time-resolved PM10 and PM2.5
monitoring, with 4 h averaging time (6 samples per day), conducted
at a mixed site in Hanoi during winter. In addition to the water
soluble ions and element compositions that were partly reported in
early studies, this paper also provides the EC and OC data. The
chemical composition of size-segregated atmospheric particles was
used to quantitatively assess contributions from sources using the
reconstructed mass approach and the Positive Matrix Factorization
(PMF) receptor model (Paatero and Tapper, 1994).
2. Monitoring program design
2.1. Study area
The monitoring was conducted during the period of December
2006eFeburary 2007 in the Hanoi capital city of Vietnam. Then the
Hanoi Metropolitan Region (HMR) comprised of 7 inner districts
and 5 suburban districts with a total area of around 921 km2 and
the population of 3.3 million (GSO, 2006). Since 2008, the HMR has
been expanded to cover a total area of 3348 km2 and the population
of over 6.7 million (GSO, 2009). Hanoi is located in Red River delta,
about 100 km from the East Vietnam Sea, and has a tropical climate
with 4 seasons. During winter and early spring, the area is under
the inuence of northeast monsoon while during summer the
inuence of southeast monsoon is pronounced.
The sampling site (20.983 N; 105.784 E) was located in the
Thuong Dinh industrial zone, Hanoi city (Fig. S1, supplementary
information). The PM samplers and meteorology equipment were
placed on the rooftop of a building (15 m above the ground) of the
Hanoi University of Science (HUS) and about 100 m from the
heavily travelled Nguyen Trai road (Fig. S1, SI). This road, 60 m wide
with 6 auto-vehicle and 2 non-auto vehicle lanes, is the main
southwestward transport route from the Hanoi city. The Thuong
Dinh industrial zone is the largest among those located on the right
bank of the Red River in HMR. There are also several large univer-
sities in the area which contribute to the high trafc ow in this
street (Truc and Kim Oanh, 2007). Main air pollution emission
sources in this area include road trafc, residential cooking,
industrial activities and construction activities. Surrounding agri-
cultural areas also contribute emission from agroresidue eld
burning to the site but this is a seasonal emission source, e.g.
intensive rice straw eld burning is observed around June and
November each year. In peri-urban areas around the site, solid
waste open burning is also intensive when weather is dry.
2.2. Sampling and analytical methods
One Andersen dichotomous sampler (dichot) for simultaneous
ne (PM2.5) and coarse (PM10e2.5) fractions, two MiniVol Samplers
(minivol) for PM2.5 and PM10, one Sibata 30 L sampler for PM10, and
one portable weather station (GroWeather Davis) were deployed.
The meteorology conditions (temperature, wind speed and
Please cite this article in press as: Hai, C.D., Kim Oanh, N.T., Effects of local, regional meteorology and emission sources on mass and compo-
sitions of particulate matter in Hanoi, Atmospheric Environment (2012), doi:10.1016/j.atmosenv.2012.05.006
direction) were recorded every 30 min during sampling. Before
sampling all PM samplers were calibrated to obtain the recom-
mended ow rates (15.03 L min
1 for ne and 1.67 L min
1 for
coarse fractions by dichot; 5 L min
1 for Minivols, and 30 L min
1
for Sibata 30 L). The entire sampling period was divided into two
sub-periods: the routine 24 h sampling, 23 December 2006e7
January 2007, when 15 pairs of 24 h PM10 and PM2.5 samples
were collected and the intensive sampling, 12 Januarye11 February
2007, when 92 pairs of 4 h PM samples (6 samples per day) were
collected. Detail on the sampling equipment and on lters used is
given in Table S1, SI.
The QA/QC of the sampling and analysis were following the
same procedures described in Kim Oanh et al. (2009). The lter
conditioning and pre-weighing (using a microbalance) were done
at the Asian Institute of Technology (AIT). Quartz lters were pre-
red at 550  C for about 6 h to remove any carbonaceous/organic
pollutants. After sampling, each quartz lter was put in a Petri dish
and kept in a separate airtight bag. The samples were refrigerated at
HUS and were transported (in an ice box) to the AIT laboratory in
Thailand for subsequent analyses. Immediately after collected, each
mixed cellulose esters lter was cut into 2 equal parts. One part was
kept in a tube containing Milli-Q water and refrigerated while
stored in HUS to minimize the loss of volatile ions. At AIT the tube
content was extracted and analyzed for water soluble ions (Na,
NH
4 , K , Mg
2
and Ca2; Cl
, NO
2

3 and SO4 ) by Ion Chromatog-
raphy (IC). The other part was refrigerated in HUS and upon arriving
at AIT was analyzed for elements (20 species) using the Inductively
Coupled Plasma-Optical Emission Spectroscopy (ICP-OES). The
quartz lters were rst used for mass determination at AIT and then
sent to the University of Illinois at Urbana Champaign for EC/OC
analysis by a Sunset Analyzer (thermal-optical transmittance
method, the NIOSH 5040 protocol). Blank reference lters were
weighed before and after real samples on each weighing day to
ensure that the lter mass was unchanged over time under the
weighing conditions (US EPA, 1998). At least one trip blank was
made for a composition group (EC/OC, ions and elements) in each
sampling sub-period. The blank lters (brought to the site but were
not exposed during a sampling event) were stored and transported
together with the samples. On average, the ion levels in the (mixed
cellulose) blanks were below 1.5 mg per lter for K, Mg2 and Na,


and in the range of 3e4 mg per lter for Cl
, SO2

4 , NO3 , NH4 and
2
Ca . The element content in the mixed cellulose blanks was below
0.03 mg per lter for most of the analyzed species, except for Fe, Si
and Mg that was 0.2e0.5 mg per lter and Ca of 3 mg per lter. OC
content in the quartz blanks was 1.4e3.7 mg per cm2 while EC
blanks were close to zero. The composition results were all blank
corrected. Note that a denuder was not used hence a certain loss of
easily volatile nitrate particles was possible. However, the loss
during sampling was expected to be minimized due to the
moderate ambient air temperatures during the period, 13e20  C,
coupled with the low sampling ow rates and relatively short
sampling period (4 h).
3. Results and discussion
3.1. Daily PM levels in relation to meteorology
The daily (24 h) mass concentrations of PM2.5 and PM10 during
the sampling period were widely uctuating (Fig. 1). The 24 h PM2.5
levels were averaged at 76  32 mg m
3, ranged from 26 to
143 mg m
3, i.e. all measurements were above 24 h WHO guideline
of 25 mg m
3. The 24 h PM10 levels during the period were
98  35 mg m
3 (37e165 mg m
3) which exceeded the 24 h Vietnam
NAAQS of 150 mg m
3 in 2 days and exceeding the WHO guideline
(50 mg m
3) in 27 days (87% of the measurements). The monitoring
 C.D. Hai, N.T. Kim Oanh / Atmospheric Environment xxx (2012) 1e8 3

Fig. 1. 24 h PM mass concentrations (25  C, 1 atm) and daily average wind speed during the monitoring period.

period (DecembereFebruary) includes the months with the highest shows a strong ridge over Northern Vietnam (Fig. S2,a, SI). The
PM levels in Hanoi (Hien et al., 2002). The range obtained by Hien inuence of this stagnating ridge (typically with subsidence and
et al. (2002) for DecembereFebruary in 1998e1999 was compa- radiative inversions) over Northern Vietnam resulted in stagnant
rable with our results for ne PM (PM2.2 w25e150 mg m
3) but air and high PM levels in the initial monitoring days before 2
higher for PM10 (w50e350 mg m
3). January 2007. After that, the ridge was weakening and a low
Our results also show that PM2.5 constituted the major fraction pressure system developed over SEA (Fig. S2,b). The wind speed in
of PM10 (PM2.5/PM10 w0.76  0.08) which emphasizes the impor- Hanoi increased (daily average of 1.5 m s
1) and remained high
tance of the combustion emission and/or secondary particles. The until 7th January due to a relatively large pressure gradient
regression line between PM2.5 and PM10 (PM2.5 0.9 PM10
15) observed over the area that induced a better dispersion hence
had R2 0.92 indicating a strong correlation which further suggests lowered PM levels. During 12the15th January, Northern Vietnam
that the change in PM10 was mostly driven by the change in PM2.5. was again under the inuence of a stagnating ridge (Fig. S2,c) and
Consistently high PM levels during the rst 9 sampling days the PM levels were high. The levels declined from 16th January
(Fig. 1) were observed with the highest levels during the New Year onward when SEA was under inuence of a low pressure system
holiday period (31st December and 1st January). In principle, less and wind speed increased (Fig. S2,d).
activities in the industrial zone and universities (hence less trafc
emission) were expected during the holidays but only on Sunday,
3.2. Diurnal variations of PM and major composition components
31st December a reduction in PM was observed. Examining local
and regional meteorology during the sampling period should help
The 4 h sampling of PM10 and PM2.5 was conducted, starting
to better understand the daily PM variations.
from 6:00 am each day to yield 6 samples per day during the
The weather during the monitoring period was generally dry
intensive sampling, 12the20th January and 05the11th February.
with some drizzle and foggy days typically observed during winter
Fig. 2 presents the average diurnal variations of PM10 and PM2.5
in Hanoi. The wind speeds (30-min averaged) measured at the site
were light, ranging from calm to about 2 m s
1. Only a few obser-
vations recorded speeds of about 3 m s
1 with a maximum of
4.8 m s
1 seen on 7 February 2007. Daily PM mass during the period
appears to inversely proportional to the local wind speed (Fig. 1).
Obviously, lower wind speeds resulted in poor dispersion of air
pollution during the New Year holidays that could offset the
impacts of reduced source activities on the PM levels. In the
following week (2e7 January 2007), when wind speeds increased,
lower PM levels were observed. Daily windroses were examined
and a summary on wind directions together with major features of
regional synoptic meteorology on the sampling days are given in
Table S2, SI. On the regional scale, during winter Northern Vietnam
is frequently inuenced by a high pressure ridge extending from
anticyclones centered in Siberia and China. When such a ridge
reaches Northern Vietnam the sea level pressure increases,
temperature and relative humidity drop, while wind with more
northerly directions and increased speeds are observed. This
principal relationship between the weather conditions and the
synoptic patterns was also observed during the sampling days.
From 25th December 2006 to 7th January 2007 the prevalent wind
directions were gaining more Northerly components and eventu-
ally to predominant Northerly during 27the29th. The pressure was
the highest during 29e31 December 2006 whereas the surface Fig. 2. Diurnal variations of PM mass, major components in PM2.5 and wind speed
temperature dropped to below 20  C. The synoptic chart (0:00 UTC) based on 4 h-sampling in JanuaryeFebruary 2007 (25  C, 1 atm).

Please cite this article in press as: Hai, C.D., Kim Oanh, N.T., Effects of local, regional meteorology and emission sources on mass and compo-
sitions of particulate matter in Hanoi, Atmospheric Environment (2012), doi:10.1016/j.atmosenv.2012.05.006
4 C.D. Hai, N.T. Kim Oanh / Atmospheric Environment xxx (2012) 1e8

mass and major ionic components in PM2.5. High PM levels and EC/OC were observed suggesting that the enhanced dispersion
observed in the morning rush hours (6:00e10:00) and evening by the wind could not offset the increased emission strength. In
rush hours (18:00e22:00) suggested higher contributions of principle, the vertical mixing also changes during a day, better
primary particles especially the road trafc. Note that diurnal around noon and poorer late at night, especially for winter when
variations were clearly seen for PM2.5 while for the coarse fraction radiative inversion frequently exists in Hanoi (Hien et al., 2002).
(PM10e2.5 is the gap between PM10 and PM2.5 in Fig. 2) there was Thus, low levels of PM and EC/OC in the afternoon (14:00e18:00)
only a small reduction in the early morning samples (2:00e06:00). may be attributed to both the enhanced mixing and reduced
This is because these two fractions were originated from different emission strength (a shorter averaging period is desirable as the
sources/processes. The coarse particles are normally emitted evening rush hours in principle start at around 17:00). Note that PM
directly from industrial and construction activities, and/or wind- and EC/OC levels in the samples collected at night and early
blown dust while ne particles are either directly emitted from morning (22:00e02:00 and 2:00e6:00) were still lowest in a day
combustion sources (primary particles) or formed in the atmo- which conrmed the predominant inuence of diurnal variations
sphere (secondary particles) (Chow, 1995). of the local emission.
The diurnal variations of EC and OC also followed the variations Sample-wise PM mass and EC/OC variations (Fig. S3 and S4, SI)
of PM2.5 mass with peaks in the morning and evening rush hours showed two highest EC/OC peaks, both in the Friday evening
(Fig. 2). EC is directly released from incomplete combustion (Bond (18:00e22:00), January 12 (EC 7.3 mg m
3, OC 56 mg m
3)
et al., 2004), mainly in ne PM, and can be used as a marker of this and February 9 (EC 8.8 mg m
3, OC 44 mg m
3). To examine
source. OC includes both primary and secondary particles but they further the weekdayeweekend uctuation, the diurnal variations
were not segregated in our results presented in Fig. 2. Sulfate and for different days of a week were analyzed (Table S3, SI). The-
nitrate, major secondary inorganic PM (ne fraction), did not show highest 4 h average EC level (18:00e22:00) was on Friday
a clear diurnal variation as compared to PM mass and EC/OC (Fig. 2). (5.9  3.7 mg m
3), followed by Sunday (4.5  2.5 mg m
3) and the
Chloride (Cl
), in fact, was following the PM mass diurnal pattern lowest were on other working days (MondayeThursday),
but the peaks were quite small. 2.4  0.5 mg m
3. OC levels largely followed the EC patterns. High
Daily patterns of primary particles were expected to reect daily trafc density on Friday and Sunday evenings, related to personal
variations in the local emission. Truc and Kim Oanh (2007) reported trips from and to Hanoi for the weekend activities, may partly
a very high trafc density in the same road with the daily ow on explain these high PM levels. Overall, the diurnal patterns of EC and
weekdays of 145,000 vehicles (from 7:00 to 19:00) that had high OC on different days of a week were similar to the PM2.5 pattern but
peaks (mainly motorcycles and cars) during morning and evening generally different from the PM10e2.5 pattern. The fact that ne
rush hours. The eet contained 96% motorcycles, 3% gasoline particles contain EC and OC emitted from combustion and that
powered vehicles (taxi, cars, etc.) and about 1% diesel powered majority of EC and OC in our samples were found in PM2.5 explains
vehicles. Two major types of diesel powered vehicles, truck and the similarity in their diurnal patterns. However, the number of
bus, were the principal source of EC at the monitoring site. The bus monitoring days was still small (3 Saturdays, 2 Sundays, 3 Fridays,
hourly density remained quite stable (about 120e180 buses) during and 8 other working days) to properly characterize the
the daytime period of 5:00e19:00, declined afterward (20e30 weekdayeweekend variations. Additional data are required for the
buses) and virtually no buses were observed after 22:30. The purpose, including the time-resolved air pollution, meteorology
truck hourly density was w100 vehicles during the daytime and source activities (i.e. trafc counts, cooking pattern) during
(8:00e17:00) and reduced to about 30 trucks at night but then with different days of a week.
more heavy duty vehicles. In addition, it was observed that cooking
activities for meals at homes and in small restaurants in the 3.3. Daily PM composition
surrounding areas were also coincidentally more intensive during
the morning and evening rush hour periods. The daily patterns of 3.3.1. EC/OC
PM mass and EC/OC thus appear to follow the daily patterns of The 24 h average of EC and OC levels in PM2.5 are presented in
these two major sources in the study area. Fig. 3 which show the same trend as PM presented in Fig. 1. Note that
Other important factors determining the PM diurnal variations EC/OC data were available for all 92 PM2.5 samples as compared to
are related to the meteorology (mixing height, wind, etc.). Average only 30 PM10e2.5 samples, accordingly EC/OC were estimated for only
wind speed was the highest (1.8 m s
1, Fig. 2) around noon 30 PM10 samples. In PM2.5, the average EC levels during the sampling
(10:00e14:00), which to some extent may lower PM levels at this period were 2.7  1.5 mg m
3 (range of 24 h levels: 1.5e4.9 mg m
3)
sampling time (in addition to reduced emission strength). and OC were 18.3  11.9 (10e39 mg m
3). In PM10 the EC levels were
However, the second highest wind speed (1.6 m s
1) was observed 3.0  1.7 mg m
3 (1.5e5.8 mg m
3) and OC levels were
during the morning rush hours (6:00e10:00) when maximum PM 21.5  12.3 mg m
3 (11e43 mg m
3). Majority of EC (about 89  4%)

50
OC EC
40
EC/OC, g m -3

30
20
10
0
20 Jan (Sat)

05 Feb (Mon)

10 Feb (Sat)
13 Jan (Sat)

14 Jan (Sun)

17 Jan (Wed)

07 Feb (Wed)

09 Feb (Fri)

11 Feb (Sun)
12 Jan (Fri)

19 Jan (Fri)

04 Feb (Sun)

08 Feb (Thur)
16 Jan (Tue)
15 Jan (Mon)

18 Jan (Thur)

06 Feb (Tue)

Fig. 3. Daily average EC and OC concentration in PM2.5 calculated from 4 h data for intensive sampling period (whiskers represent one standard deviation).

Please cite this article in press as: Hai, C.D., Kim Oanh, N.T., Effects of local, regional meteorology and emission sources on mass and compo-
sitions of particulate matter in Hanoi, Atmospheric Environment (2012), doi:10.1016/j.atmosenv.2012.05.006
 C.D. Hai, N.T. Kim Oanh / Atmospheric Environment xxx (2012) 1e8
and OC (90  4%) was associated with PM2.5. Overall, EC constituted
only a small fraction of PM2.5 mass (3.4  1.1%) while OC share was
signicant (24.4  7.3%). PM10e2.5 contained only a low level of EC
(0.5  0.3 mg m
3) and OC (2.2  1.3 mg m
3). The ratio between EC
and total carbon (TC EC OC) in PM2.5 also varied during the
monitoring period with lower EC/TC ratios (0.11e0.12) observed
during 12the16th January and the highest ratios (w0.15e0.2) during
7the9th February (Fig. S5, SI). In principle, the diesel exhaust would
have a high ratio (EC/TC w0.7, Kim Oanh et al., 2010) while biomass
open burning would have a lower ratio (w0.15 for rice straw eld
burning, Kim Oanh et al., 2011). The EC and OC absolute levels as well
as EC/TC ratios appeared to change with the main wind directions
despite of the overall low wind speeds. When northerly winds (from
residential and commercial areas to the site, see Fig. S1, SI) were
observed, e.g. 12e16 January (Table S2, SI), higher EC and OC levels
were obtained but lower EC/TC ratios. The cooking in homes and
restaurants and other related activities in the residential area located
just to the north of the site may be the inuencing factor. Winds were
southerly and southeasterly during the rest monitoring period that
brought in more fresh trafc emission from the road to the site hence
during this period higher EC/TC ratios were obtained although the
levels of EC and OC were generally lower.
3.3.2. Ionic species
The results of 8 water soluble anions are summarized in Fig. 4 for
the ne (PM2.5) and coarse fraction (PM10e2.5). The highest levels


were found for SO2
4 , NO3 , and NH4 , predominantly in the ne
fractions, indicating signicant contributions of secondary inor-
ganic particles. Local sources of the gas precursors of these particles
may include the vehicle exhausts (SO2, NOx), residential cooking in
the study area with smoky coal briquettes (SO2), as well agriculture
activities (NOx, NH3). Cl
and K were also found at higher levels in
the ne fraction as compared to the coarse fraction that may be
linked to biomass burning. Na and Cl
may link to seasalt including
fresh table salt from cooking. Hanoi is located about 100 km west to
the Bac Bo (Tonkin) Gulf and the S-SE winds may bring in the aged
seasalt particles through the regional transport. High levels of Ca2
observed in the coarse fraction probably link to construction activ-
ities around the site as well as soil/road dust.
The ion balance was constructed for the QA/QC purpose using
the sum of anions and sum of cations in the molar concentration
unit (equivalents). For PM2.5, the regression line between anions
and cations had a slope of 0.97 (more anions or slightly acidic) and
R2 0.79 while that for PM10 has a slope was 1.1 (slightly alkaline)
and R2 0.62 (Fig. S5, SI).
3.3.3. Element composition
The results of the element analysis are summarized in Fig. 5.
Major elements in PM10e2.5 included Ca (highest, reaching above
2 mg m
3), Si, Fe and Al which indicate the contribution from
soil/road dust and construction activities. PM2.5 contained
Fig. 4. Water soluble ions concentrations in ne and coarse PM (whiskers represent
one standard deviation).
Please cite this article in press as: Hai, C.D., Kim Oanh, N.T., Effects of local, regional meteorology and emission sources on mass and compo-
sitions of particulate matter in Hanoi, Atmospheric Environment (2012), doi:10.1016/j.atmosenv.2012.05.006
5
noticeable levels of most detected elements but mostly below
0.5 mg m
3 in the high level group and below 0.2 mg m
3 in the low
level group (Fig. 5) which indicate a combustion origin. Lead (Pb)
was quite signicant (w0.17 mg m
3) and was mainly found in
PM2.5, also suggesting a combustion origin. The Pb level was well
below the Vietnam 24 h NAAQS (1.5 mg m
3) and that was expected
following the successful phase out of leaded gasoline in the country
in 2001 (ESMAP, 2002).
3.4. Source apportionment of PM
3.4.1. Reconstructed PM mass
The reconstructed mass was done using 8 mass groups
following the method presented previously (Kim Oanh et al.,
2006) to provide information on major contributing sources.
These included (K-biomass K
0.6 Fe), crustal (oxides of
crustal 1.16  (1.9 Al 2.15 Si 1.41 Ca 1.67 Ti 2.09 Fe)),
organic matter (OM 1.4 OC), soot (EC), seasalt (2.54  Na), NH
4,
NO
2

3 and SO4 for secondary organic particles, and trace metals
(remaining analyzed elements) as presented in Table 1. The calcu-
lated mass in principle should be lower than the measured mass
because not all the components were analyzed. However, due to
uncertainties related to sampling and analytical methods, a few
PM2.5 samples (7 samples) had more than 100% mass explained
hence they were excluded from the statistics presented in Table 1.
For the coarse fraction, all samples had mass explained below 100%.
On average, the portion of measured mass explained by the 8
groups was 78  11% for PM2.5 and 61  11% for PM10e2.5. The
K-biomass was used to identify the presence of biomass burning
smoke in the PM and it was not the absolute contribution of the
biomass burning. It was excluded from the sum of the mass
explained to avoid double counting because K was already included
in the trace elements group. The K-biomass group was more
signicant in PM2.5 than PM10e2.5 as most of PM emitted from
biomass burning is expected to be in the ne fraction (Kim Oanh
et al., 2011).
The crustal group was predominantly found in the coarse frac-
tion indicating a signicant contribution from soil/road dust and
construction activities. The seasalt group, estimated based on the
content of Na and Cl
hence indicating fresh seasalt, was small
in both fractions. The trace elements (remaining analyzed
elements) group was generally found at low levels and more in the
ne PM (than the coarse PM fraction) and may be linked to
a combustion origin.
3.4.2. Source apportionment of PM2.5 by PMF
The PMF receptor model (Paatero and Tapper, 1994), used in this
study, assumes non-negativity of the factors, both loadings (source
contributions) and scores (source proles). PMF2, applicable for
two-dimensional arrays, was applied for the PM2.5 source appor-
tionment using the composition data of 92 PM2.5 samples taken
during the intensive sampling sub-period that had complete EC,
OC, ions and element composition data. Due to the lack of EC/OC
data in a large number of coarse PM samples the PMF analysis was
not done for this fraction. The measurement uncertainty of each
species was estimated following the method presented in Kim
Oanh et al. (2009).
PMF was run with Fpeak ranged from
0.6 to 0.6 and Fpeak 0.5
produced seven source factors with the most explainable source
proles. The contributions of these source factors to PM2.5 (Fig. 6)
listed in the reducing order included: 1) secondary mixed (local)
PM (31  15 mg m
3), 2) residential/commercial combustion
(12  10 mg m
3), 3) secondary sulfate rich (LRT) (12  11 mg m
3),
4) aged seasalt mixed (9  7 mg m
3), 5) trafc (diesel)
(8  5 mg m
3), 6) industry/incinerator (4  5 mg m
3), and 7)
6 C.D. Hai, N.T. Kim Oanh / Atmospheric Environment xxx (2012) 1e8

3.0 0.30
High conc. species Low conc. species

Low conc. group (g m -3)

2.5 0.25

High conc. group (g m -3)

Fine fraction Coarse fraction
2.0 0.20

1.5 0.15

1.0 0.10

0.5 0.05

0.0 0.00
Fe Zn Si Al Ca Mg Ni Pb Sr Ti V Be Cd Co Cr Cu Li Mn Mo Tl
Fig. 5. Element compositions of ne fraction and coarse PM (whiskers represent one standard deviation).

construction and soil/road dust (1  1 mg m
3). The scatter plot
between the scaled calculated mass (x) and measured mass (y)
yields a regression equation y 0.97x 2.7 with R2 0.64.
The proles of the identied source factors are presented in
Fig. S7, SI and the temporal variations in the contributions are in
Fig. S8, SI. The residential/commercial had more pronounced
contributions during January 12e16, when the local wind was weak
and had the directions of N-NW, and lower contributions during
the rest of the monitoring period when the wind directions
changed to S-SE. A populated residential area was located to the
north of the site (Fig. S1, SI), food stall/restaurants and commercial
activities were densely distributed along the road and other small
streets inside the residential area. Commercial cooking normally
lasted from 4:00 am to late evening hours with the highest activ-
ities between 18:00e22:00 while residential cooking was normally
more intensive in the evening. Various fuel types were used for
cooking in the area including LPG and wood fuel at home, and
commonly smoky coal briquettes in food stalls/restaurants. The
coal briquettes used for cooking were made of rejected coal parti-
cles which would produce high sulfur and heavy metal emission.
Sawdust or peat mixed in the briquettes, and wood fuel would
contribute high levels of K shown in the source prole. Low
combustion temperature of the residential/commercial cooking as
well as solid/yard waste burning (observed in dry weather) is
expected to emit higher OC than EC. Accordingly, the residential/
commercial combustion had a source prole with specic markers
including high OC and EC (with the ratio EC/OC < 1.0), relative


abundance of NH 4 , sulfate, nitrate, Na , K and Cl , and some


elements (Si, Al, Pb, Cr, Mn). Note that Na and Cl present in this
source prole may directly link to table salt used in cooking that
may also explain the diurnal Cl
variation pattern discussed (Fig. 2).
The trafc (diesel) exhaust prole is characterized by high EC
with the ratio EC/OC > 1.0 (Fig. S7, SI) which is remarkably different
from the residential/commercial source discussed above. A rela-
tively high abundance of V, Zn, Si and Mg2 in this source might be
originated from the fuel additives (Kim Oanh et al., 2010). This
source was quite stable during the monitoring period but was more
pronounced during February 9e11 when the wind (SE, <1 m s
1)
was blowing from the road to the site (Fig. S1, SI). Diesel powered
buses and trucks running in this street were probably the most
important sources of fresh PM2.5 with high EC to the site. A more
clear diurnal contribution pattern was also observed for this source
(Fig. S8, SI) with low emission in the late night and early morning
hours (22:00e6:00) when the public buses stopped operation.
Note that at night heavy trucks were observed traveling in this road
and other side streets in the surrounding area hence the truck
contribution may be not strongly directional.
The secondary mixed PM (local) was identied by a prole with
abundance of sulfate, nitrate, ammonium and high OC but with low
EC (Fig. S7, SI). Overall, its contribution was quite stable during the
sampling period, but showed some dependence on wind speeds
(not on wind directions). This source factor had slightly lower
contributions when higher wind speeds were observed, e.g. January
17e18 and vice versa (Fig. S8 and Table S2, SI). The HYSPLIT (Draxler
and Hess, 1998) 5-day backward trajectories were constructed,
starting at 0:00 UTC and 1000 m above the sampling site for each
sampling day (Fig. S9, SI), and showed that the variations in this
source factor contribution were not strongly associated with the air
mass types. In the dry weather observed during the sampling period
a long atmospheric life of PM was expected that enhanced the
mixing and uniform distribution of the secondary PM in the study
area. This explained why the contributions of this source factor

Table 1
Summary of reconstructed mass for ne and coarse fraction based on 4 h PM
sampling, mg m
3.

Parameters PM2.5 (n 85) PM10e2.5 (n 85/30)b

Max Min Av  std Max Min Av  std

PM mass 162 32 78  33 66 18 29  10
K-biomassa 3.2 0.0 0.9  0.8 2.2 0.0 0.1  0.3
Crustal 5.4 0.38 2.2  1.1 13 0.6 4.8  2.5
OM 54 6.2 21  8.5 5.5 1.5 2.9  1.1
Soot 4.8 0.79 2.2  0.9 1.6 0.1 0.5  0.5
NH 4 19 0.02 7.9  4.8 2.8 0.02 0.9  0.7
NO
3 17 0.02 6.9  3.8 6.4 0.02 1.7  1.8
2

SO4 39 7.2 17  8.1 4.8 0.02 1.2  1.3
Seasalt 2.8 0.04 1.2  0.8 8.1 0.04 1.8  1.8
Trace metals 3.1 0.31 0.8  0.5 1.0 0.05 0.3  0.2
Mass explained, % 99 39 78  11 93 36 61  16
a
K-Biomass is not included in the calculated mass to avoid double counting. Fig. 6. Percentage of average source contributions to PM2.5 at Thuong Dinh, Hanoi
b
Only 30 coarse PM samples had EC/OC data. (based on 4 h sampling, January 12eFebruary 20, 2007).

Please cite this article in press as: Hai, C.D., Kim Oanh, N.T., Effects of local, regional meteorology and emission sources on mass and compo-
sitions of particulate matter in Hanoi, Atmospheric Environment (2012), doi:10.1016/j.atmosenv.2012.05.006
 C.D. Hai, N.T. Kim Oanh / Atmospheric Environment xxx (2012) 1e8
were more depending on local wind speeds than on air mass types
(with characteristic wind directions). To distinguish this source
factor from the secondary sulfate appeared later it is named the
secondary PM (local) although the precursors of this secondary PM
may have both local and regional/LRT emission origins.
The industry/incinerator contribution was identied by higher
levels of several elements (Mg2, Fe, Pb, Zn, Al, Cr and Mn) in the
source prole. This source factor had a relatively small contribution
(6%) and high temporal variations (Fig. S7, SI). A few peaks were
observed at late evening and early morning hours and were in fact
higher on Saturdays and Sundays. Several industrial activities were
located on the opposite side across the road, but in principle should
not have a high contribution at late hours and on weekend. It was
noted that there was a hazardous hospital waste incinerator (stack
height of 20 m) located about 10 km to the NW of the monitoring
site that may explain higher contributions from this source during
12e16 January (NW-N wind predominant). In addition, there is
a waste recycling village (Trieu Khuc, Fig. S1, SI) located about 2 km
to the SW of the site which often had waste burning in the late
evening hours. Further investigation is still required to explain the
detailed source activities of this factor.
The aged seasalt (mixed) was identied by higher levels of Na,
Mg2, as well as nitrate and sulfate in the prole. It contributed
about 11% of PM2.5 mass at the site. Examining the HYSPLIT 5-day
backward trajectories during the period, conrmed that the aged
seasalt (mixed) contribution was higher during the days when
a long marine pathway (15e16, 18 January and 5e7 February) was
observed (Fig. S9, SI). The coastal line of the East Vietnam Sea is
about 100 km away from the site. During the transport to the site,
the marine air masses likely have Cl
depleted (Lee et al., 1999), i.e.
replaced by nitrate and sulfate. Likewise, various secondary and
primary air pollutants were also picked up and brought to the site
hence this aged seasalt mixed was not the same as the (fresh)
seasalt calculated by reconstructed mass (Table 1). Overall, this
source factor was likely associated with the regional/LRT air
pollution that had a marine pathway.
The secondary sulfate rich PM (LRT), with a distinguished high
abundance of sulfate, contributed about 16% to PM2.5 mass. As
compared to the secondary mixed PM (local) this source factor had
a low level of nitrate but more abundance of K, Mg2 and NH 4 . The
temporal variation (Fig. S8, SI) showed higher contributions when
relatively strong winds were recorded at the site, i.e. during 17e19
January and 11 February. The backward trajectories showed that
this source factor had higher contributions when the air masses
arriving at the site with a longer continental pathway, i.e. moving
along the coastal line of Southern China on 13th January and 17th
January, or with a continental pathway over Northern Vietnam and
Southern China, or arriving from the west neighboring countries/
territories (9e11 February). This source factor was likely linked to
the LRT of sulfate-rich PM that was originated from continental
territories on the pathway of air masses before arriving to the site.
The contribution from soil/construction activities to the site was
identied by a source prole with a high abundance of Ca, Si and Al
(Fig. S7, SI). This source contributed only 1% of PM2.5 mass at the
site. As expected, there was no wind direction dependent and a few
peaks (Fig. S8, SI) may be linked to drier weather conditions when
more intensive construction activities and soil/road dust released.
3.4.3. Discussion: contributions from local emission sources and
LRT
For the purpose of the air quality management it is always of
interest to estimate the contribution from the local sources and the
LRT air pollution but this is a challenging task, especially when only
monitoring data are available. This is because PM locally emitted or
formed in a study area is mixed with those of regional and LRT
Please cite this article in press as: Hai, C.D., Kim Oanh, N.T., Effects of local, regional meteorology and emission sources on mass and compo-
sitions of particulate matter in Hanoi, Atmospheric Environment (2012), doi:10.1016/j.atmosenv.2012.05.006
7
origin. The precursors are also both locally and regionally emitted.
At the monitoring site, the most likely part of PM having association
with the regional and LRT origins included the secondary sulfate
rich (LRT) and aged seasalt mixed, that collectively contributed
about 27% of PM2.5 mass. This was estimated using the source
proles, knowledge of local sources and their variations, the vari-
ations in the source contributions in relation to local meteorology
(wind) and pathways of air masses. Nevertheless, it is important to
note that not the entire contributions of these two source factors
(27%) could be attributed to the LRT because the presence of PM of
local origins in the mixture was anticipated.
Likewise, the secondary mixed PM (local), contributing about
40% PM2.5 mass, may also have a part associated with the LRT origin.
However, intensive emission from local sources, for example trafc
and cooking, may contribute signicantly to air pollution, both
primary PM and gaseous precursors for secondary PM, in Hanoi. As
motorcycles have high daily driving activities and scattered over
the city (Phuong, 2009), their contributions would also be widely
scattered. Lack of a source prole of the gasoline powered vehicles
prevents from estimation of this source contribution. Preliminary
results of the emission inventories for Hanoi, using the Interna-
tional Vehicle Emissions modeling, show that in 2008 the total
motorcycle eet in Hanoi contributed 2.4 kt PM10 (Phuong, 2009)
which was about 15% of the PM10 emission estimated from the
diesel bus eet alone in 2010 (Trang, 2011). Thus, the gasoline
vehicles may be more important in the contribution of the gaseous
precursors for secondary PM formation than directly to the primary
PM in the city. An important local source that is observed to dras-
tically increase around the city is the rice straw eld burning.
However, the burning is mainly in June and November after the
harvest of two rice crops, respectively, which was not covered by
our monitoring.
Hien et al. (2004) conducted the PMF modeling for ne and
coarse PM samples collected during 1999e2001 in Hanoi for 3
types of air mass backward trajectories. Majority of the backward
trajectories in our study period (Fig. S9a & b, SI) can be roughly
classied into Type 2 (Northeasterly) of Hien et al. (2004). The
authors identied 6 contributing source factors to ne PM for this
air mass type (LRT, local burning, soil dust, local secondary aerosol,
marine aerosol and Cl-depleted aerosol). These are largely equiva-
lent to our identied source factors except for the trafc (diesel)
exhaust emission that was not identied in their study. With the
available EC/OC data and element composition for the PMF input
our study can identify the contribution from trafc (diesel) emis-
sion, about 10% of PM2.5 mass. Also our study revealed that the LRT
was likely to contribute a smaller part of PM2.5 pollution than the
local emission. The difference between these two studies was large
and may be partly explained by the rapid urbanization and
motorization in Hanoi during the 7e8 year gap. Note that the
average PM2.5 data in our study period was 76  32 mg m
3 that was
about 2 times of the measured levels for Type 2 (43 mg m
3) in Hien
et al. (2004).
4. Conclusions
High PM levels were observed at a mixed site in Hanoi during
the dry winter period with the ne fraction (PM2.5) contributed the
majority (76%) to PM10. The daily PM2.5 levels were found to closely
link to local wind speeds and directions (relative to local emission
sources) and regional synoptic meteorology suggesting that both
local sources and LRT contributed to the high PM levels at the site.
Diurnal variations in PM2.5, EC, OC and EC/TC were similar and can
be largely explained by the uctuations in local source activities.
The coarse fraction (PM10-2.5) was less uctuated during a day.
Reconstructed mass served as useful tool in identifying potential
8 C.D. Hai, N.T. Kim Oanh / Atmospheric Environment xxx (2012) 1e8
source factors for subsequent PMF analysis, although for a site
located 100 km away from the sea like this, the estimated (fresh)
seasalt group may not necessarily relate to the sea spray. PMF
identied seven source factors for PM2.5 that can be explained using
the knowledge on local emission sources and their variations, wind
and HYSPLIT air mass backward trajectories. The major source
factors included the secondary mixed PM (largely with local
origins), local emission (primary PM from cooking, trafc and
industry/incinerator) and LRT (secondary sulfate rich and aged
seasalt mixed). For PM10e2.5, the reconstructed mass suggested that
soil/road dust and construction activities were the main sources.
Overall, the LRT was likely to contribute a smaller part of PM2.5
mass (about 27% have an association with LRT origins) measured at
the site while the majority appears to originate from local emis-
sions. The secondary PM (local) contributed a large part of PM mass
(about 40% of PM2.5) hence to improve PM air quality in the city the
control efforts should also focus on the emission of gaseous
precursors. Cleaner fuel-cookstove systems in residential/
commercial cooking, cleaner diesel vehicles, as well as emission
reduction for the gasoline vehicle eet (including the eet density
reduction) should be addressed. Further studies should be con-
ducted for other periods of the year especially during the rice straw
burning months of June and November to reveal the contribution
from this source.
Acknowledgment
We would like to acknowledge the AIRPET project (http://www.
serd.ait.ac.th/airpet) sponsored by Sida and the ARCP2007-07CMY
project sponsored by the Asia-Pacic Network for Global Change
Research for the partial funding support provided to cover the
consumables for the data collection. Dr. Hoang Xuan Co at Hanoi
University of Science and Dr. Nghiem Trung Dung at Hanoi
University of Technology and their team are specially thanked for
their great assistance extended during the sampling period in
Hanoi. Colleagues at UIUC are highly appreciated for the generous
support for EC/OC analysis.
Appendix A. Supplementary information
Supplementary information related to this article can be found
online at doi:10.1016/j.atmosenv.2012.05.006.
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