Beruflich Dokumente
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Atmospheric Environment
journal homepage: www.elsevier.com/locate/atmosenv
h i g h l i g h t s
This is the rst time to study the VOCs in the remote station in southwest China.
Aromatics and alkanes are the major components of VOC.
The seasonal variation shows higher value in spring and lower value in autumn.
Anthropogenic sources are the most important sources in the remote area.
a r t i c l e i n f o
a b s t r a c t
Article history:
Received 1 November 2012
Received in revised form
4 March 2013
Accepted 18 March 2013
Available online 29 March 2013
The mixing ratio, composition and variability of volatile organic compounds (VOCs) were measured from
2008 through 2011 at Gongga Mountain Forest Ecosystem Research Station (102 000 E, 29 330 N, elevation
1640 m), a remote station in southwest China. Weekly samples were collected in the Gongga Mountain
area and were analyzed using a three-stage preconcentration method coupled with GCeMS. An advance
receptor model positive matrix factorization (PMF) was applied to identify and apportion the sources of
VOCs. The results show that the measured VOC mixing ratio at Gongga Mountain is dominated by aromatics (35.7%) and alkanes (30.8%), followed by halocarbons (21.6%) and alkenes (11.9%). The general
trend of seasonal variation shows higher mixing ratios in spring and lower mixing ratios in autumn. The
effect of alkanes and aromatics on the seasonal variation of total volatile organic compounds (TVOCs) is
signicant. Five sources were resolved by the PMF model: (1) gasoline-related emission (the combination
of gasoline exhaust and gas vapor), which contributes 35.1% of the measured VOC mixing ratios; (2)
solvent use, contributing 21.8%; (3) fuel combustion, contributing 29.1%; (4) biogenic emission,
contributing 5.2%; and (5) industrial, commercial and domestic sources, contributing 8.7%. The effect on
this area of the long-range transport of air pollutants from highly polluted areas is signicant.
2013 Elsevier Ltd. All rights reserved.
Keywords:
VOC sources at Gongga Mountain
Seasonal variation
PMF receptor model
Source apportionment
1. Introduction
There is no doubt of the importance of volatile organic compounds (VOCs) in the atmosphere, because they are the important
precursors of secondary air pollutants and secondary organic
aerosols in photochemical processes. Moreover, most of VOCs are
also impact the environment and human health directly (Leuchner
and Rappenglck, 2010; Prez-Rial et al., 2010).
The study of VOCs is still very limited in China because most
such studies have focused on mega-cities or city clusters, such as
Beijing (Song et al., 2007; Yuan et al., 2009; Su et al., 2011), the Pearl
River Delta (Chan et al., 2006; Guo et al., 2006, 2011; Ling et al.,
2011) and the Yangtze River Delta (Cai et al., 2010; Geng et al.,
2010; Huang et al., 2011). However, information about the source
characteristics of VOCs in remote areas is insufcient because it is
more difcult and more expensive to observe these areas than
observe areas in cities. However, the study of VOC emissions from
remote areas is crucial because these areas occupy more area than
cities worldwide. Thus, the results of such studies are highly useful
for studying the global temporal and spatial variation of VOCs.
Unfortunately, this type of study is rare in China, especially in the
remote area of the underdeveloped southwestern region of China.
Furthermore, it is not sufcient simply to measure the mixing
ratios of VOCs to develop of an effective control strategy. We also
need to obtain and understand accurate information about the
sources of VOCs. One effective method for studying VOC sources
298
involves the use of receptor models (Song et al., 2007; Lanz et al.,
2009; Chan et al., 2011; Ling et al., 2011), such as positive matrix
factorization (PMF). This receptor model has been successfully
tested in comparison with other receptor models for VOCs (Song
et al., 2007; Sauvage et al., 2009; Yuan et al., 2009) and particulate matter (PM) (Leuchner and Rappenglck, 2010; Chan et al.,
2011). A very effective statistical method, it can apportion
ambient concentration data to sources by identifying the intrinsic
characteristics of the data while limiting all of the elements in the
factor score (source proles) and the factor loading (source contributions) matrix to positive values, making this method especially
useful in environmental source analysis (Yuan et al., 2009).
In this paper, the mixing ratios, composition and seasonal variations of VOCs at Gongga Mountain, a station in a remote area of
southwest China, are rst presented. We then use the PMF receptor
model to identify VOC source types and to apportion their contributions. To the best of our knowledge, this paper is the rst to study
VOCs at a remote station in southwest China.
2. Experiment and methods
2.1. VOC sampling and analysis
The measurements were performed at the standard meteorological eld of the Gongga Mountain Forest Ecosystem Research
Station (102 000 E, 29 330 N, elevation 1640 m) in Hailuogou Scenic
Area, a remote site located in southeast Ganzi Tibetan Autonomous
Prefecture in Sichuan province. This scenic area is famous for its
large areas of glaciers and virgin forest and its large number of rare
animal and plant resources. The forest area in Hailuogou is
approximately 70 km2 and the total resort area is approximately
200 km2. The principal tourist seasons are spring and summer. There
are approximately 30,000 inhabitants in the vicinity of the scenic
area. During the tourist seasons, the population is several times
more numerous than the local residents. This station is approximately 130 km to the northeast of Yaan and 250 km from Chengdu,
the capital of Sichuan province (Fig. 1). There are two major roads in
the north and east, 500 m and 400 m from the station, respectively. A
gas station is located 1000 m to the north of the station.
Air samples were collected twice a day every Tuesday from Jan.
2008 to Dec. 2011. A total of 380 samples were collected during the
measurement period (approximately 40 samples were excluded for
various reasons). The monitoring site is shown in Fig. 1. A pump was
used to draw, ambient air samples from a gas inlet through a PFATeon tube (OD: in). These samples were collected in preevacuated 1 L electropolished canisters. A 3 min integrated
sample was taken for each canister sample at 8:00 and 14:00.
Ambient air was collected at a ow rate of 1 L min1. After the
canisters were pressurized to 60 psig, the valve was closed and the
pump turned off. The samples were returned to Beijing for analysis
within 7 days of collection.
Measurements of VOCs were made using an Entech 7100A
preconcentrator (Entech Inc., USA) followed by a GCeMS system
(Finnigan Trace GC/Trace DSQ). The details of the VOC analysis
procedures have been described previously by Mao et al. (2009)
and will be described briey here.
A 500 mL sample was concentrated in an Entech 7100A preconcentrator, a three-stage preconcentration was utilized to
remove the water, carbon dioxide, nitrogen and oxygen in air
samples. The VOCs were further focused with a capillary focusing
trap for rapid injection prior to the analytical column. A DB-5 MS
fused-silica capillary column (60 m 0.25 mm 0.25 mm, Agilent
Technologies Inc.) coupled with a quadrupole mass spectrometer
detector (Finnigan Trace 2000/DSQ. Thermosher Inc. USA) was
used for qualication and quantication.
Forty VOCs were identied and quantied. Each target species
was identied by its retention time, mass spectrum and USEPA
standard gases. The quantication of the target VOCs was performed with multi-point external standard curves and modied
using Relative Responsible Factors (RRFs). The calibration curves
were prepared using 100 ppbv external standard gases (Scott
Specialty, TO14 standard; alkanes and alkenes) and 100 ppbv internal standard gases of dibromomethane at ve different diluted
concentrations plus nitrogen (0e100 ppbv). Internal standard gas
was added to each sample to trace the analytical procedure (Mao
et al., 2009). Five sets of replicate samples were collected to
check the precision and reliability of the sampling and analysis
methods. The RSD was within 10% for the target compounds in all
ve replicates. For most samples, the VOC species were above the
detection limit of 5e10 pptv.
2.2. Positive matrix factorization (PMF)
2.2.1. Principles and application of PMF
The PMF method is comprehensively described by Paatero and
Tapper (1994) and Paatero (1997) and has been used in many
VOC source identication studies (Song et al., 2007; Sauvage et al.,
2009; Yuan et al., 2009). In this paper, PMF 3.0 (USEPA, 2008) was
used to apportion the contributions from emission sources. Several
concepts that are relevant to the understanding of this work are
briey described here. For additional details about the method, the
reader is referred to the publications cited above and to the PMF 3.0
user manual.
An ambient data set can be viewed as an i by j data matrix X in
which i samples and j chemical species are represented. The goal of
multivariate receptor modeling is to identify a number of sources p,
the species prole f of each source and the amount of mass g
contributed by each source to each individual sample as well as the
residuals eij:
Xij
p
X
k1
Q
Fig. 1. Location of the sampling site and some important cities around it.
"
#2
Pp
n X
m x
X
g f
ij
k1 ik kj
uij
i1 j1
299
Table 1
Average mixing ratios of VOCs samples in the air of Gongga Mountain.
Name
Alkanes
Butane
Isopentane
Cyclopentane
Hexane
2-methylhexane
3-methylhexane
Methylcyclohexane
3-methylheptane
Alkenes
1-butene
Isoprene
c-2-pentene
Limonene
Aromatics
Benzene
Ethylbenzene
Styrene
Isopropylbenzene
1,3,5-trimethylbenzene
Halocarbons
Chloromethane
CFC-11 (trichlorouoromethane)
Dichloromethane
1,2-dichloroethane
Name
0.20
0.47
0.11
0.09
0.13
0.18
0.14
0.14
0.16
0.50
0.19
0.12
0.36
0.42
0.32
0.35
Isobutane
Pentane
2-methylpentane
Methylcyclopentane
2,3-dimethylpentane
Heptane
2-methylheptane
0.27
0.22
0.08
0.17
0.18
0.14
0.16
0.38
0.40
0.02
0.06
0.47
0.59
0.04
0.08
1-pentene
t-2-pentene
a-pinene
0.05 0.07
0.04 0.06
0.10 0.18
0.72
0.28
0.23
0.07
0.12
0.64
0.42
0.41
0.14
0.24
Toluene
m/p-xylene
o-xylene
Propylbenzene
1,2,4-trimethylbenzene
0.44
0.28
0.31
0.29
0.39
0.33
0.42
0.43
0.44
0.50
0.62
0.28
0.36
0.25
0.34
0.25
0.42
0.36
CFC-114 (tetrauorodichloroethane)
CFC-113 (trichlorotriuoroethane)
Chloroform
Chlorobenzene
0.02
0.09
0.20
0.08
0.03
0.08
0.35
0.15
0.26
0.23
0.10
0.38
0.35
0.30
0.36
300
Table 2
Comparison of TVOCs or NMHCs measured at Gongga Mountain and at other
stations.
Station
name
Mount Taia
Jianfeng
Mountainb
Dinghu
Mountainb
Shanghaic
Gongga
Mountain
Station
Background Background Background City
Background
type
TVOCs
6.95 5.71
32.35 19.76 8.75 5.76
(ppbv)
NMHCs
4.78 1.85 23.40 9.84
6.33 4.63
(ppbv)
a
b
c
Halocarbons
21.6%
Aromatic
35.7%
Alkanes
30.8%
Alkenes
11.9%
Fig. 2. Contributions of four main hydrocarbon groups to TVOC in the air at Gongga
Mountain.
18
10
Mixing ratio(ppbv)
301
16
14
12
TVOCs
Alkanes
Aromatics
Alkenes
Halocarbons
10
4
3
-1
Jan.Feb.Mar.Apr. MayJun. Jul. Aug.Sep.Oct.Nov.Dec.
Spring
Summer
Autumn
Winter
Fig. 3. Monthly and seasonal average mixing ratios of the total and the four chemical groups of Gongga Mountain.
development of the Gongga area has been rapid. For example, the
number of visitors in the rst seven months of 2009 was 123%
greater than that in the same period in 2008. The tourism zone
requires more hotels, restaurants and other related infrastructure
tracers that are used as solvents (Borbon et al., 2002; Guo et al.,
2004a). In the PMF-derived source prole, 1,2,4-trimethylbenzene
and 1,3,5-trimethylbenzene all account for 75% of the total mass.
This source is therefore assigned to solvent use. In recent years, the
100
Gasoline-related emission
80
60
40
20
0
100
80
Solvent use
60
20
0
100 Fuel combustion
80
60
40
20
0
100 Biogenic emission
80
60
40
20
0
100 Industrial, commercial and domestic
80
60
40
20
-pinene
Limonene
1.2.4-trimethyl-benzene
propyl-benzene
1.3.5-trimethyl-benzene
Isopropylbenzene
Styrene
o-xylene
m/p-xylene
Ethylbenzene
Toluene
Chlorobenzene
Heptane
2,3-dimethyl-pentane
Benzene
2-methyl-hexane
Hexane
1,2-Dichloroethane
Dichloromethane
2-methyl-Pentane
t-2-Pentene
c-2-pentene
Pentane
Isoprene
1-Pentene
Isobutane
Isopentane
0
Chloromethane
% of species
40
302
industrual,
commercial and
domestic, 9%
biogenic
emission, 5%
fuel combustion,
29%
gasoline-related
emission, 35%
solvent use,
22%
limonene were only 0.10 0.18 ppbv and 0.06 0.08 ppbv,
respectively. This nding is similar to those of previous studies in
remote or background sites, such as those at Linan (Guo et al.,
2004b) and Yufa (Yuan et al., 2009).
3.4. The effect of long-range transport
The long-range transport of air pollutants (clean air) from highly
polluted areas (clean areas) could increase (decrease) the VOC
mixing ratios at the study site. This transport will affect the sources
at the sampling site in conjunction with the local sources. The
Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT)
model is a useful air trajectory model, especially for studying the
long-range transport of air masses (Mao et al., 2009; Cheng et al.,
2010). This model was used to calculate 36 h back-trajectories for
each day during different seasons in 2011. The back-trajectories
were calculated every 6 h. The air mass direction can be divided
into four categories in terms of the original direction, namely, 0 e
90 , 90 e180 , 180 e270 and 270 e360 .
Only one air mass in the 0 e90 category was present in spring
(Fig. 6a). It originated from Xian, a large city in central China, and
passed over Hanzhong and several cities of Sichuan, including
Guangyuan, Mianyang, Deyang and Chengdu, before ultimately
arriving at Gongga Mountain. The transport of pollutants from
these cities via the air masses could signicantly promote the level
of VOCs in the air at the study site. Two air masses were associated
with the 180 e270 direction. The air masses originated from the
northeastern part of India and passed over northern Myanmar and
the clean air area in Yunnan province, China. Two air masses were
associated with the 270 e360 direction. These air masses originated from several underdeveloped areas of China, including Qinhai province and the Tibet Autonomous Region. The effect on the
sampling site of the air masses that originate from the latter two
directions was to dilute the mixing ratio of VOCs in the atmosphere.
In summer, two air masses were associated with the 0e90
direction (Fig. 6b). The original and effect of the longer of these two
air masses (7th) was similar to that of the 0e90 air mass in spring.
The shorter air mass originated from and passed several small
counties or towns. Only one air mass was associated with the 90 e
180 direction. This air mass originated from Guizhou province, an
underdeveloped province in China. Three air masses were associated with the 180 e270 direction. The third of these air masses
originated from Yunnan province, a clean area in China. The other
two air masses originated from northern Myanmar, also a clean
area. The effect of the air masses originating from the latter two
directions was to dilute the VOCs in the atmosphere.
One air mass originated from the east of China in autumn
(Fig. 6c). This air mass was very short and may have transported
small amounts of pollutants from nearby towns. However, its effect
was very limited. The major air masses in autumn were associated
303
Fig. 6. The main air masses of different seasons at Gongga Mountain in 2011. a: spring; b: summer; c: autumn; d: winter.
with the 180 e270 and 270 e360 directions. The origins and
effects of these air masses were similar to those of the air masses
identied in spring and summer and associated with the same
directions.
In winter, the air masses were associated with the 180 e270
and 270 e360 directions (Fig. 6d). The origins and effects of these
air masses were the same as those of the air masses associated with
the same directions in spring and autumn.
The air masses can be divided into the following two categories:
(1) contaminated air masses, it only appearing in spring and summer (the 5th air mass in spring and the 7th air mass in summer)
which could transport air pollutants from highly polluted areas and
increase the level of VOCs in the Gongga Mountain area; and (2) the
other air masses, which originated from other directions and
diluted the VOCs at the sampling site. The heights associated with
these two categories of air masses differed signicantly. The height
of the air masses belonging to the rst category was always less
than 500 m. This characteristic was not conducive to the dilution of
pollutants in the vertical direction during the transport process. In
contrast, the height of the air masses belonging to the second
category was not stable. It ranged from more than 3000 m to less
than 500 m for different directions or seasons.
The differences between air masses in different seasons can also
be used to explain the seasonal variation at Gongga Mountain. Air
masses carrying high mixing ratios of pollutants only appeared in
spring and summer, and the associated proportions were all 10%
(the 5th air mass in spring and the 7th air mass in summer). While
the scavenging effect is stronger in summer than spring, due to the
higher temperature and mixing layer. For this reason, the effect of
long-term transport on the VOCs in the Gongga Mountain area is
stronger in spring than in summer. All of the air masses appearing
in autumn and winter can be viewed as dilute air masses. Therefore,
the mixing ratio of VOCs in autumn and winter is lower than in
spring (especially) and summer.
Note that the station at which this study was conducted would
be considered a remote station in a relative sense. The air masses
traveling to the site from several large cities have some effects, as
discussed above. Therefore, the source tracers cannot be used as the
source apportionment if these tracers experienced a loss during
transport. Accordingly, we analyzed the correlations between
304
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