Aerosol and Air Quality Research, 13: 943–956, 2013

Copyright © Taiwan Association for Aerosol Research

ISSN: 1680-8584 print / 2071-1409 online
doi: 10.4209/aaqr.2012.09.0242

A Monitoring and Modeling Study to Investigate Regional Transport and

Characteristics of PM2.5 Pollution

Jianlei Lang1, Shuiyuan Cheng1*, Jianbing Li2, Dongsheng Chen1, Ying Zhou1, Xiao Wei1,
Lihui Han1, Haiyan Wang1
1
College of Environmental & Energy Engineering, Beijing University of Technology, Beijing 100124, China
2
Environmental Engineering Program, University of Northern British Columbia, Prince George, British Columbia V2N
4Z9, Canada

ABSTRACT

In this study, the regional transport and characteristics of PM2.5 pollution were examined through a case study in Beijing,
China. The results from an intensive monitoring program indicate that the inorganic particles (sulfate, nitrate, and
ammonium), organic carbons, and the elements accounted for 35.5, 24.2, and 15.3% of the total PM2.5 on an annual average
basis, respectively. The proportions of such PM2.5 components also showed clear seasonal variations. An integrated MM5-
CMAQ modeling system was then developed to examine the regional transport of PM2.5 and its components in Beijing
within four typical months of 2010. The results indicate that the annual average total trans-boundary contribution ratio
(TBCR) is 42.2, 46.3, 77.4, and 61.6% for the concentrations of PM2.5, sulfate, nitrate, and ammonium, respectively. A
logarithmic relationship was found between the total TBCR and the PM2.5 concentrations in Beijing for different seasons.
Further investigations showed that trans-boundary transport played a major role in Beijing’s PM2.5 concentrations during
the period of high pollution levels, with an annual average TBCR of 54.6%. As a result, the control of PM2.5 pollution in
Beijing needs effective cooperation between Beijing and its surrounding regions, especially during periods of heavy pollution.

Keywords: Trans-boundary transport; Beijing; Emission contribution; MM5-CMAQ; Air quality.

INTRODUCTION atmospheric visibility and the human health. For example,

With continuous rapid economic development and sharp
growth of vehicle population, the pollution of PM2.5 (i.e.,
the fine particles with aerodynamic diameter of ≤ 2.5 μm)
has become one major environmental problem. This problem
has received wide concerns among experts, governments,
media, and the public in China and around the world,
particularly after the occurrence of a severe haze event in
Beijing (i.e., the capital of China) in December 2011 (Lang
et al., 2012; Yuan et al., 2012). It was reported that the
annual average PM2.5 concentrations in Beijing from 2000
to 2010 were 101.0, 93.6, 101.5, 100.0, 102.2, 85.2, 93.5,
84.5, 76.8, 79.6, and 71.9 μg/m3, respectively (Zheng et al.,
2005; Song et al., 2007; Zhao et al., 2009; Wang et al.,
2012). However, the PM2.5 concentrations were only 9.8–
13.6 μg/m3 during the same period in the United States (http://
www.epa.gov/airtrends/pm.html). The high concentration
of PM2.5 could have significant adverse impacts on the
*
Corresponding author. Tel.: +86 10 67391656;
Fax: +86 10 67391983
E-mail address: chengsy@bjut.edu.cn
previous studies indicated that the PM2.5 was the main cause
of reduced visibility in Beijing (Wang et al., 2006; Zhou et
al., 2012a). Such fine particles can also result in serious
human health problems (e.g., cardiovascular diseases,
respiratory irritation, and pulmonary dysfunction) since they
contain microscopic solids or liquid droplets which are toxic
and can get deep into the human body (Cao et al., 2012;
Haberzettl et al., 2012). Consequently, the study of PM2.5
pollution is of great importance for effectively improving
the air quality and the public health. In fact, a new National
Ambient Air Quality Standard (NAAQS) was proposed in
China in the beginning of 2012 (http://www.zhb.gov.cn/gkml
/hbb/bwj/201203/t20120302_224147.htm). This new standard
introduced the control of PM2.5 for the first time in China.
Generally, the pollution of particulate matters (PM) is a
complex regional transport problem as confirmed from
many previous studies (Hatakeyama et al., 2011; Hussein
et al., 2011; Ibn Azkar et al., 2012; Squizzato et al., 2012;
Tao et al., 2012). Particularly, air quality models have been
commonly applied to investigate such regional air pollutant
transport (Chen et al., 2007). Among various models, the
CMAQ/Model-3 developed by US EPA has obtained
extensive applications. For example, Chen et al. (2007)
examined the trans-boundary transport of PM10 to Beijing,
944 Lang et al., Aerosol and Air Quality Research, 13: 943–956, 2013
and obtained the trans-boundary contribution ratios (TBCRs)
from its surrounding regions using a meteorological model
(MM5) and an air quality model (CMAQ). Wang et al.
(2010) utilized the HYSPLIT and MM5-CMAQ models to
study the PM10 pollution problem in Beijing, and found
that the southwest transport pathway was closely associated
with the increasing phase of its PM10 pollution processes.
Zhu et al. (2011) investigated the transport pathways and
potential sources of PM10 concentration in Beijing based
on backward trajectories and PM10 concentration records.
Che et al. (2011) evaluate the effects of different vehicle
emission control measures on the air quality of SO2, NO2,
PM10, and O3. Zhou et al. (2012b) investigated the source-
receptor relationships of PM10 in Tangshan of northern
China using the integrated MM5-CMAQ model. Other
application of CMAQ can be found in Zhang et al. (2007),
Mueller and Mallard (2011) and Han et al. (2012).
Most of the previous studies on the transport of particulate
matters were focused on PM10, and the transport of PM2.5
has received less attention (Streets et al., 2007). As compared
with PM10, the diameter of PM2.5 is much smaller with
more complex components that contain a higher percentage
of inorganic particles, which are mainly secondary pollutants
produced via complex reactions (Ianniello et al., 2011). This
makes the PM2.5 can stay in the atmosphere for a longer
time and facilitates a long distance transport. As a result,
the transport of PM2.5 may be quite different from that of
PM10. However, few previous studies were reported to study
the transport characteristics of PM2.5 components and their
temporal variations (Streets et al., 2007). In fact, the
understanding of such information is very valuable for the
effective decision making of air quality management. The
objective of this study is then to examine the regional
transport of PM2.5 and its components through conducting a
case study in Beijing, which has typical and representative
PM2.5 pollution problem in China. An intensive monitoring
program was implemented in the study area to measure the
concentrations of PM2.5 components within different seasons,
and to provide necessary data for establishing an integrated
MM5-CMAQ modeling system. The modeling system was
then applied to facilitate the investigation of trans-boundary
PM2.5 transport. The concentrations of PM2.5 and three
selected components (sulfate, nitrate, and ammonium) in
Beijing were simulated under various emission reduction
scenarios, and the corresponding trans-boundary contribution
ratios (TBCRs) of Beijing’s surrounding areas were then
calculated. Moreover, the TBCRs associated with different
PM2.5 pollution levels were analyzed. The results can provide
sound decision making basis for the mitigation of PM2.5
pollution in Beijing.
OVERVIEW OF THE STUDY AREA
Beijing is located in northern China, with Tianjin
municipality on its eastern border and Hebei province on
its other three borders as shown in Fig. 1. Topographically,
Beijing is characterized as a semi-basin region, with Taihang
Mountains on its southwest and Yan Mountains on its
northwest. The mean sea level of its land tends to decrease
gradually from its northwest to southeast towards the Bohai
Bay. This basin-like topography plays an important role in
the transport of pollutants from the industrial provinces
(e.g., Hebei, Shanxi) to Beijing. The total population of
Beijing was 19.62 million in 2010, accounting for 1.47%
of the national population. The GDP of Beijing was 213.1
billion US dollars in 2010, accounting for 3.23% of the
national GDP. There are 14 subordinate districts and 2
counties in Beijing as shown in Fig. 1, covering a total area
of 16410.5 km2. The central urban area of Beijing includes
6 subordinate districts (e.g., Dongcheng, Xicheng, Chaoyang,
Haidian, Fengtai, and Shijngshan), covering 8.3% of Beijing’s
geographical area, accounting for 63.2% of Beijing’s total
population, and contributing to 69.7% of the total GDP in
Beijing. As mentioned before, the annual average PM2.5
concentration during the past decade in Beijing was in the
range of 71.9–101.0 μg/m3, which is much higher than the
proposed class II standard of PM2.5 (i.e., 35 μg/m3) in the
new Chinese NAQQS, indicating severe PM2.5 pollution in
Beijing.
METHODOLOGY
MM5-CMAQ Modeling System
The meteorological model MM5 is a limited-area, non-
hydrostatic, terrain-following sigma-coordinate model
designed to simulate meso-scale and regional-scale
atmospheric circulation. It was developed by Penn State
University and National Center for Atmospheric Research
(PSU/NCAR) as a community meso-scale model in 1970s
and has been continuously upgraded since then to its latest
fifth version (Grell et al., 2000). The air quality model
CMAQ/Model-3, which was developed by US EPA, is the
third generation of CMAQ air quality prediction tool. It is
a sophisticated modeling system which can simulate the
concentrations of fine particulate, tropospheric ozone, acid
deposition, visibility, and other atmospheric pollutants at
regional and urban scales (Byun and Ching, 1999). In the
context of “one atmospheric” perspective, the CMAQ model
can well simulate the complex physical and chemical
processes. In addition, the model contains a capacity of
multiple levels nested-grid. The above characteristics of
the model can reduce the uncertainty and increase the
accuracy of the simulation results. In this study, the Carbon
Bond-IV Mechanism (CB-IV) and the AER03 aerosol
mechanism were chosen for the simulations of secondary
particles formation and other relative atmospheric chemical
reactions.
In this study, the MM5 and CMAQ models were coupled
to predict PM2.5 concentrations in Beijing. The MM5
model was used for providing the 4D meteorological data
required by the CMAQ model. The details of the required
data by MM5, such as the topography data, 3D first-guess
meteorological fields, and the meteorological measurements,
as well as the physical options used were the same as those
described in Chen et al. (2007) and Zhou et al. (2012c). As
for the CMAQ model, emission inventory is another
important input data. The county-level air pollutant emission
inventories (including pollutants of PM10, PM2.5, SO2, NOx,
 Lang et al., Aerosol and Air Quality Research, 13: 943–956, 2013 945

0 250
kilometers

Beijing
Do‐2
Do‐1 Tianjin
Hebei
Shanxi
0 750 1,500

kilom eters
Shandong

Henan

N o te:
A.T.: Aoti D .S.: Dongsi 0 25 50 Do‐3
T.T.: Tiantan G.C.: Gucheng kilometers
W.L .: Wanliu G.Y.: Guanyuan
N .Z.G.: Nongzhanguan
F.T.H.Y.: Fengtaihuayuan Yanqing Miyun
W.S.X.G.: Wanshouxigong
Huairou
BN U: Beijing Normal University

Changping Pinggu
B NU A.T.
Shunyi
W.L.
Mentougou H.D.
D.S. S.J.S. X. D. C.Y.
G.Y. C. C. Note:
F.T. Tong D.C. : Dongcheng
G.C. N.Z.G. X.C. : Xicheng
zhou
T.T. Fangshan C.Y. : Chaoyang
F.T.H.Y. Daxing H.D. : Haidian
W.S.X.G. F.T. : Fengtai
S.J.S.: Shijingshan
Evaluation grid cell area (EGC)

Fig. 1. Design of three-level modeling domains.

NH3, VOCs and CO) were obtained from the Environmental
Protection Bureaus (EPBs) of Beijing and its surrounding
regions. These emission inventories were processed by the
modified Sparse Matrix Operator Kernel Emissions Modeling
System (SMOKE) (Houyoux et al., 2000) to generate
emission inputs with high spatial and temporal resolution
as required by the CMAQ model. The space distribution of
PM2.5 emissions in Beijing and surrounding regions was
shown in Fig. 2.
A three-level nested-grid architecture (shown in Fig. 1)
was designed for the implementation of the MM5-CMAQ
modeling system. Modeling domain 1 (only for MM5
simulation) was divided into 43 × 49 grid cells with a spatial
resolution of 36 km × 36 km, covering most areas of
northeastern China; modeling domain 2 (both for MM5
and CMAQ simulation) was divided into 70 × 76 grid cells
with a 12 km × 12 km spatial resolution, covering Beijing
and its surrounding regions (including Tianjin, Hebei, Shanxi,
and parts of Shandong and Henan); modeling domain 3
(both for MM5 and CMAQ simulation) was divided into
49 × 49 grid cells with a spatial resolution of 4 km × 4 km,
covering Beijing. Vertically, 35 sigma levels were designed
for the grid structure in the MM5 simulation, with the top
height being 15 km at the pressure of 100 mbar. The first
20 vertical levels were distributed within 2 km from the
ground level. These 35 vertical layers for the MM5 model
were collapsed into 12 layers for the vertical domain of the
CMAQ model. The MCIP (Meteorology-Chemistry Interface
Processor) was used to process and transform the hourly
MM5 outputs from 35 vertical levels into 12 levels with
the format required by the CMAQ model. More detailed
descriptions of the MM5-CMAQ modeling system and setup
can be found in previous papers (Chen et al., 2007; Zhou
et al., 2012c).
946 Lang et al., Aerosol and Air Quality Research, 13: 943–956, 2013
42.0N
37.0N
113.2E
Fig. 2. Space distributions of PM2.5 emissions in Beijing and surrounding regions.
Observation of PM2.5 Components
The transport of PM2.5 components is of importance as
mentioned above, and was thus investigated in this study.
The observation of PM2.5 components was performed at a
monitoring station located on the rooftop of a building at
Beijing Normal University (BNU), about 45m above the
ground level. The BNU is located between the north second
and third Ring Roads, which is a heavily traffic area of
Beijing. The PM2.5 samples were simultaneously collected
on the Whatmans 41 filters (Whatman Inc., Maidstone, UK)
and the quartz filters (Whatman Inc., Maidstone, UK) using
the medium-volume samplers made by Wuhan Instrument
Co., Ltd., with a flow rate of 40 L/min and 100L/min,
respectively. The samplings were carried out during winter,
spring, summer, and autumn from December 2010 to January
2012 on a 24-h basis. One or two respective months of per
season were selected for the PM2.5 samplings. About 50-60
samples per season and a total number of 212 samples were
collected. All the procedures were strictly quality controlled
to avoid any possible contamination of the samples. Such as,
the samples collected were put in the polyethylene plastic
bags right after sampling and reserved in a refrigerator. All
the filters were weighed before and after sampling using a
One Over Ten-thousand Analytical Balance under constant
temperature (20 ± 5°C) and relative humidity (40 ± 2%).
The samples collected on Whatmans 41 filters were used
for the analysis of 10 selected ions and 22 selected elements,
while the samples collected on the quartz filters were used
for the detection of Organic Carbon (OC) and Element
Carbon (EC). The SO42–, NO3–, NH4+, and other ions
(Mg2+, Ca2+, K+, Na+, PO43–, F–, and Cl–) were analyzed by
ion chromatograph (IC, Metrohm 861 Advanced Compact
IC). The analysis of 22 elements (Na, Mg, Al, Ca, Sc, Ti,
V, Cr, Mn, Fe, Co, Ni, Cu, Zn, As, Se, Sr, Cd, Sb, Ce, Eu,
and Pb) was based on the inductively coupled plasma-mass
spectrometry (ICP-MS, 7500a, Thermo). The OC and EC
120.0E
were measured using a Thermal/Optical Carbon Analyzer
(DRI, Model 2001).
Evaluation of Modeling Performance
The observations from nine air quality monitoring
stations in Beijing were used for modeling performance
assessment of PM2.5 simulation. These stations include
AoTi, NongZhanGuan, DongSi, TianTan, WanShouXiGong,
FengTaiHuaYuan, GuCheng, GuanYuan, and WanLiu, as
illustrated in Fig. 1. As mentioned above, the PM2.5
components were measured at a monitoring station in
Beijing Normal University (BNU). An evaluation grid cell
area (EGC) with a total number of 7 × 10 grid cells was
selected within modeling domain 3 (Fig. 1). It covers the
above ten monitoring stations and most of the central urban
area of Beijing. As a result, the data obtained from these
monitoring stations can well represent the characteristics
of the urban PM2.5 pollution in Beijing. The MM5-CMAQ
model was applied to investigate Beijing’s PM2.5 pollution
within four target months in 2010. These four target months
(January, April, July, and October) were used to represent
winter, spring, summer, and autumn, respectively. In order
to assess the modeling performance, the average simulated
daily concentrations of PM2.5 within the grid cells containing
the nine monitoring stations during different target months
were compared with the average observation results in 2010
from these nine stations. Meanwhile, the simulated monthly
concentrations of the three PM2.5 components (sulfate, nitrate,
and ammonium) within the grid cell containing the BNU
monitoring station during different target months were also
compared with the observation results from that monitoring
station.
Calculation of Trans-boundary Contribution Ratio
(TBCR)
In order to examine the trans-boundary transport of PM2.5,
 Lang et al., Aerosol and Air Quality Research, 13: 943–956, 2013 947

a parameter called trans-boundary contribution ratio (TBCR)
was introduced in this study. A zero-out method was applied
to calculate TBCR using two scenarios, including the Zero
Emission Reduction Scenario (ZERS) and the Emission
Reduction Scenario (ERS) (Chen et al., 2007). The ZERS
was corresponding to the base scenario under which the
MM5-CMAQ model was run using the original emission
inventories. In terms of the ERS, four sub-scenarios were
introduced, including Zero-Surrounding-Emission (S1), Zero-
Beijing-Emission (S2), Zero-Tianjin-Emission (S3), and
Zero-Hebei-Emission (S4). The S1, S2, S3, and S4 scenarios
correspond to the situations where the emissions (including
pollutants of PM10, PM2.5, SO2, NOx, NH3, VOCs and CO)
from Beijing’s surrounding regions, Beijing, Tianjin, and
Hebei were set to zero, respectively.
The average simulated hourly concentrations of PM2.5 and
its three components as well as other fine particles within the
EGC were used to calculate TBCR as described below:
C ZERS  CERS
TBCR   100%
C ZERS
where CZERS represents the simulated hourly concentration
of PM2.5, sulfate, nitrate, ammonium, and other fine particles
under the ZERS scenario; CERS represents the hourly
pollutant concentration under different ERS scenarios. The
CERS under the scenarios of S1, S3, and S4 was used to
calculate the TBCR from all of Beijing’s surrounding regions,
Tianjin, and Hebei, respectively. The CERS under the scenario
of S2 can be used to calculate the contribution ratio of local
emissions within Beijing.
RESULTS AND DISCUSSION
Seasonal Characteristics of PM2.5 in Beijing
Fig. 3 presents the observed proportions of different PM2.5
components in Beijing. It can be found that the inorganic
particles of SO42–, NO3–, and NH4+ were important
components in PM2.5 in Beijing. They accounted for an
annual average percentage of 35.5% of the total PM2.5.
Among these three components, the nitrate (NO3–) had the
highest percentage. In addition to the three inorganic
particles, organic carbons (OC) and elements were another
(1)
two important components in the PM2.5 in Beijing. The
annual average percentages were 24.2 and 15.3% for OC
and elements, respectively. The annual average ratio of

Elements Ammonium Elements

26.2% 11.8% 11.6%

Ammonium
8.5% Nitrate
16.2%
OC OC
20.0% 22.2%
Nitrate
14.2%
Sulfate
EC
14.9%
Sulfate 3.7% EC
6.5% 5.8%
Others Others
21.0% 17.6%
(a) Spring (b) Summer

Elements Elements
10.5% Ammonium 13.0%
Ammonium 9.0%
9.0% OC
30.2%
Nitrate OC
15.5% 24.5%
Nitrate
13.0%

EC
Sulfate EC
Sulfate 4.1%
12.8% 3.3%
10.6%
Others Others
22.6% 21.9%
(c) Autumn (d) Winter
Fig. 3. Proportion of chemical components in PM2.5 during different seasons in Beijing (“Elements” include Na, Mg, Al,
Ca, Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, As, Se, Sr, Cd, Sb, Ce, Eu, and Pb).
948 Lang et al., Aerosol and Air Quality Research, 13: 943–956, 2013

NO3–/SO42– was 1.23, indicating that the motor vehicles
accounted for an important emission source for the formation
of PM2.5 pollution in Beijing (Wang et al., 2005). The
proportion of inorganic particle components also showed
obvious seasonal variation. For example, the proportions
of the three inorganic particles in PM2.5 were higher in
summer and winter, while those for elements were the highest
in spring. The three inorganic components accounted for
29.2, 42.9, 32.5, and 37.2% of the total PM2.5 during
spring, summer, autumn, and winter, respectively. In terms
of the elements, the proportions were 26.2, 11.6, 10.5, and
13.0% in the four seasons, respectively. The reasons for
these seasonal characteristics of PM2.5 components may be
explained as follows: (a) the high O3 concentration in the
atmosphere in summer could facilitate the formation of
secondary particles; (b) the higher emissions of SO2 and
NOx in the heating season of winter could result in a higher
concentrations of inorganic particles as compared to the
spring and autumn, and (c) the higher occurrence frequency
of sandstorms in spring could lead to higher percentage of
elements in the PM2.5.
for all of the four target months. The correlation coefficients
(CCs) between the simulated and observed concentrations
were 0.789, 0.541, 0.641, and 0.591 for January, April,
July, and October, respectively. The correlation coefficients
were generally greater than 0.50. This indicates that the
modeling performance for simulating PM2.5 concentrations
in Beijing is acceptable (Chen et al., 2007).
The modeling performance for simulating the
concentrations of the three inorganic particle components
in PM2.5 (SO42–, NO3–, NH4+) were also evaluated. Table 1
lists the monthly comparison of the simulation and
observation results. Generally, most of the simulation errors
of PM2.5 components were ranging from –30% to 10% for
various seasons. The simulation errors of the annual
average concentrations were –21.8, –15.7, and –18.4% for
sulfate, nitrate, and ammonium, respectively. Considering
the inherent uncertain nature of meteorological and air
quality simulation, the modeling performance of the MM5-
CMAQ for simulating the concentration of inorganic
particle components of PM2.5 is also acceptable (Zhang et
al., 2007; Wang et al., 2011a).

Modeling Performance Emission Contribution to PM2.5 Pollution in Beijing

Fig. 4 presents the scatter plots of the simulated PM2.5 Figs. 5–6 present the hourly emission contribution ratios
concentrations versus the observation results during the four to the PM2.5 concentration in Beijing during the four target
target months in 2010. It can be found that most of the data months from all of Beijing’s surrounding regions, as well
points are adjacently distributed on both sides of the y = x line as from Beijing, Tianjin, and Hebei, respectively. It can be

300 200

250
160
Simulation (g m )
-3

Simulation (g m )
-3

200
120
150
80
100

50 40

0 0
0 50 100 150 200 250 300 0 40 80 120 160 200
-3 -3
　 Observation (g m ) Observation (g m )
(a) January (b) April
150 200

120 160
Simulation (g m )
Simulation (g m )

-3
-3

90 120

60 80

30 40

0 0
0 30 60 90 120 150 0 40 80 120 160 200
-3 -3
Observation (g m ) Observation (g m )
(c) July (d) October
Fig. 4. Scatter plots of the simulated PM2.5 concentrations versus observations during the target months in 2010.
 Lang et al., Aerosol and Air Quality Research, 13: 943–956, 2013 949

Table 1. Comparison of simulated results with observations of inorganic PM2.5 particles (μg/m3)
Spring Summer Autumn Winter Annual average
Observation 4.5 20.7 11.5 13.0 11.9
Sulfate Simulation 4.2 10.2 9.1 13.9 9.3
Relative error –7.8% –50.9% –21.1% 7.1% –21.8%
Observation 9.8 22.6 14.1 15.7 14.7
Nitrate Simulation 8.2 20.4 14.3 6.7 12.4
Relative error –16.9% –9.8% 1.1% –57.5% –15.7%
Observation 5.9 16.4 9.8 9.2 9.4
Ammonium Simulation 4.3 10.9 7.4 8.1 7.7
Relative error –26.3% –33.5% –24.0% –11.4% –18.4%

80 100

60 80
TBCR (%)

TBCR (%)
60
40
40
20 20
0 0
3 6 9 12 15 18 21 24 27 30 3 6 9 12 15 18 21 24 27 30
(a) January (b) April
100 100
80 80
TBCR (%)
TBCR (%)

60 60
40 40
20 20
0 0
3 6 9 12 15 18 21 24 27 30 3 6 9 12 15 18 21 24 27 30
(c) July (d) October
100
Contribution ratio (%)

Contribution ratio (%)

100
80
80
60
60
40
40
20
20
0
3 6 9 12 15 18 21 24 27 30 3 6 9 12 15 18 21 24 27 30
(e) January (f) April
100 100
Contribution ratio (%)

Contribution ratio (%)

80 80
60 60
40 40
20 20
0 0
3 6 9 12 15 18 21 24 27 30 3 6 9 12 15 18 21 24 27 30
(g) July (h) October
Fig. 5. Hourly emission contribution ratio for PM2.5 concentration in Beijing from local emissions and all of Beijing’s
surrounding regions, (a)–(d): TBCR from surrounding regions; (e)–(h): contribution ratios from local Beijing.

found that significant hourly variations of the contribution
ratios exist for all of the study months. Fig. 7 presents the
simulated daily PM2.5 concentrations in the EGC area in
Beijing for the four target months in 2010. By comparing
the daily PM2.5 concentration trend shown in Fig. 7 with
the trend of emission contribution ratio for Beijing’s
surrounding regions (Fig. 5), it can be found that the high
PM2.5 concentration in Beijing generally corresponds to the
high trans-boundary PM2.5 contribution. Meanwhile, the low
PM2.5 concentration in Beijing was corresponding to the low
trans-boundary contribution. Further regression analysis
results showed a logarithmic relationship between the
TBCRs from Beijing’s surrounding regions and the PM2.5
concentrations in Beijing (Fig. 8).
950 Lang et al., Aerosol and Air Quality Research, 13: 943–956, 2013

40 15
12
TBCR (%)

30

TBCR (%)
9
20
6
10 3
0 0
3 6 9 12 15 18 21 24 27 30 3 6 9 12 15 18 21 24 27 30
(a) January (b) April
25 50
20 40

TBCR (%)
TBCR (%)

15 30
10 20
5 10
0 0
3 6 9 12 15 18 21 24 27 30 3 6 9 12 15 18 21 24 27 30
(c) July (d) October
60 100

45 TBCR (%) 80
TBCR (%)

60
30
40
15 20
0 0
3 6 9 12 15 18 21 24 27 30 3 6 9 12 15 18 21 24 27 30
(e) January (f) April
100
100
80
TBCR (%)

80
TBCR (%)

60
60
40
40
20
20
0
0 3 6 9 12 15 18 21 24 27 30
3 6 9 12 15 18 21 24 27 30
(g) July (h) October
Fig. 6. Hourly TBCR to PM2.5 concentration in Beijing from Tianjin and Hebei, (a)–(d): TBCR from Tianjin; (e)–(h): TBCR
from Hebei.

The monthly contribution ratios to PM2.5 concentration
in Beijing were also calculated based on the hourly results
shown in Figs. 5–8, and are listed in Table 2. Table 2 also
lists the calculated annual contribution ratios from different
emission regions based on the simulated hourly PM2.5
concentrations. It can be found that the monthly average
emission contribution ratios from all of Beijing’s surrounding
regions were 24.9, 34.4, 75.2, and 33.6% for January,
April, July, and October, respectively. The trans-boundary
transport from Beijing’s surrounding regions had a much
higher contribution ratio in July as compared to the three
other months. The reasons for this may be explained as
follows. Firstly, North China has a typical temperate and
monsoonal climate with four clearly distinct seasons. In
summer, it is mainly under the control of temperate oceanic
air mass. The prevailing wind directions are south and
southwest (with a frequency about 34%) and this could
facilitate the transport of high PM2.5 emissions from the
southern and southwestern regions (Fig. 2) to Beijing along
the Taihang Mountains. In winter, North China is mainly
under the control of Siberian cold high pressure, the
prevailing wind direction is northwest (with a frequency
about 22%). In this case, the PM2.5 transport is mainly from
the northwest of Hebei, where there has a lower PM2.5
emission (Fig. 2). In addition, the temperature inversion is
universal and the frequency is high in the winter of North
China. This could make the emissions stay in the lower
atmosphere for a long time and facilitates the pollutants
accumulation on the surface. As a result, the PM2.5
concentration is mainly caused by the local emission
sources, and the ratio of transport PM2.5 is lower. However,
in spring and autumn, the wind directions are relative even,
resulting in the intermediate level of PM2.5 TBCRs between
summer and winter. Secondly, the formation of secondary
particles is strongly associated with the O3 concentrations
in July. When the emissions from Beijing’s surrounding
regions were set to zero, the O3 concentrations in Beijing
was declined by about 50%, resulting in the reduction of
secondary fine particles formation. The annual average
contribution ratio to PM2.5 concentration in Beijing from
 Lang et al., Aerosol and Air Quality Research, 13: 943–956, 2013 951

250 150
3 3
g/m g/m
200 120
150 90
100 60
50 30
0 0
6 9 12 15 18 21 24 27 30 6 9 12 15 18 21 24 27 30
(a) January (b) April
120 180 3
3 g/m
100 g/m 150 Daily PM2.5 concentration
3
80 120 Class II level (75 g/m )
3
90 Class I level (35 g/m )
60
60
40
30
20
0
6 9 12 15 18 21 24 27 30 6 9 12 15 18 21 24 27 30
(c) July (d) Octorber
Fig. 7. Simulated daily PM2.5 concentration in the EGC area in Beijing during four target months in 2010.

80% 80%

y = 0.1301ln(x) - 0.2752
60% R² = 0.4796 60%
TBCRs

TBCRs

40% 40%

20% 20% y = 0.2537ln(x) - 0.7128

R² = 0.6191

0% 0%
0 50 100 150 200 250 300 0 30 60 90 120 150 180
PM2.5 concentration (μg/m3) PM2.5 concentration (μg/m3)
(a) January (b) April
100% 100%

80% 80%

60% 60%
TBCRs

TBCRs

y = 0.3719ln(x) - 0.7491
40% R² = 0.6752 40%
y = 0.2032ln(x) - 0.4008
R² = 0.6221
20% 20%

0% 0%
0 30 60 90 120 0 40 80 120 160 200
PM2.5 concentration (μg/m3) PM2.5 concentration (μg/m3)
(c) July (d) October
Fig. 8. Relationship between TBCR from Beijing’s surrounding regions and PM2.5 concentration in Beijing (“x” represents
PM2.5 concentration, “y” represents TBCR).

its surrounding regions was 42.2% as listed in Table 2.
Previous studies based on the MM5/CMAQ modeling system
illustrated that the contribution ratios to PM10 concentration in
Beijing from its surrounding regions were about 34.7%
(annual average) (Chen et al., 2007), 22.0% (in winter) and
40.0% (in summer) (Wang et al., 2008). The result based
on backward trajectories shows that about 26.0% of PM10
concentration in Beijing was contributed from long transport
(Zhu et al., 2011). The differences between the results for
PM10 and PM2.5 can be explained by the fact that the PM2.5
has a smaller aerodynamic size than PM10, and as a result
can stay in the atmosphere for a longer time. This can
facilitate the long-distance transport.
Table 2 also lists the monthly emission contribution ratios
from Beijing, Tianjin, and Hebei. It can be found that the
contribution from Hebei accounted for a major part in the
total contributions from Beijing’s surrounding regions during
all of the study months. This may be explained by the fact
that most part of Beijing is bordered by Hebei province
(Fig. 1) which can facilitate the transport of PM2.5 emitted
952 Lang et al., Aerosol and Air Quality Research, 13: 943–956, 2013

Table 2. The average emission contribution ratio to the concentrations of PM2.5 and inorganic particles in Beijing from
Beijing and its surrounding regions.
Emission regions January April July October Annual
PM2.5
All of the surrounding regions 24.9% 34.4% 75.2% 33.6% 42.2%
Beijing 70.8% 62.5% 30.7% 60.1% 55.4%
Tianjin 1.9% 5.0% 4.4% 9.7% 5.1%
Hebei 19.4% 28.7% 72.3% 28.4% 38.0%
Sulfate
All of the surrounding regions 31.6% 40.8% 79.3% 32.8% 46.3%
Beijing 44.6% 23.8% 8.7% 30.1% 26.5%
Tianjin 3.0% 2.3% 1.3% 2.2% 2.2%
Hebei 25.3% 37.6% 75.5% 30.2% 43.5%
Nitrate
All of the surrounding regions 60.5% 77.2% 96.9% 74.8% 77.4%
Beijing 0.5% 10.1% 21.3% 13.5% 10.7%
Tianjin –3.2% 3.6% 6.6% 2.5% 2.3%
Hebei 27.2% 67.8% 92.0% 66.1% 64.6%
Ammonium
All of the surrounding regions 39.4% 61.1% 90.4% 55.1% 61.6%
Beijing 33.6% 14.6% 15.8% 19.3% 20.4%
Tianjin 1.6% 2.6% 4.4% 2.1% 2.7%
Hebei 26.0% 55.1% 86.1% 49.3% 55.6%
Other particles
All of the surrounding regions 20.6% 29.0% 48.6% 22.6% 30.3%
Beijing 79.0% 70.7% 51.4% 76.6% 69.0%
Tianjin 1.9% 5.3% 4.6% 4.8% 4.2%
Hebei 17.4% 23.1% 42.8% 17.5% 26.0%

and formed in Hebei to Beijing. The annual emission
contribution ratios to the PM2.5 concentration from Beijing,
Tianjin, and Hebei were 55.4, 5.1, and 38.0%, respectively
(Table 2), indicating that nearly half of Beijing’s PM2.5 is
due to trans–boundary transport. The control of Beijing’s
PM2.5 pollution needs coordinated efforts in Beijing and its
surrounding regions, especially Hebei province. The monthly
average contributions for the three inorganic components and
other particles of PM2.5 were also calculated and presented
in Table 2. Similar to PM2.5, the contribution ratios to the
PM2.5 component concentrations from Beijing’s surrounding
regions were much higher in July as compared to the three
other months. The trans–boundary transport impact on nitrate
concentration in Beijing from its surrounding regions was
the greatest (i.e., 77.4%) among all of the fine particles.
This is mainly because that the formation of nitrate can be
affected more strongly by the emission of NH3 as compared
to sulfate and other particles (Behera and Sharma, 2012).
As a result, when the emission of NH3 was reduced, it
would bring more negative influence to the formation of
nitrate. Liu et al.’s (2005) study found that if there were no
NH3 emissions, the sulfate concentration in North China
would reduce about 30%, however the nitrate will nearly
change to zero. In this study, when the NH3 emissions of
Beijing surrounding regions were set to zero, the nitrate in
surrounding regions and transport to Beijing will also
become zero. In addition, the NH3 concentration in Beijing
will decrease by an annual average ratio of about 34%. In
summer, the season during which the nitrate concentration
was highest (more than 20 μg/m3), the NH3 reduction ratio
can even reach more than 50%. This will significantly
decrease the nitrate formation in local Beijing. Both the
nitrate concentration reductions in local Beijing and from a
long distance transport result in the high nitrate TBCR. As a
result, the actual nitrate contributions may be lower than the
results above. The contribution ratios for the concentration
of ammonium (i.e., 61.6%) and sulfate (i.e., 46.3%) in
Beijing from its surrounding regions were also higher than
that for the PM2.5 concentration (i.e., 42.2%). However, the
contribution ratio for the concentration of other particles
from Beijing’s surrounding regions (i.e., 30.3%) was lower
than that for PM2.5 concentration.
It is worth noting that the sum of emission contribution
ratios from Tianjin and Hebei exceeds the contribution
ratio from all of Beijing’s surrounding regions. The sum of
the emission contribution ratios from Beijing and all of its
surrounding regions is also not equal to 100% in this study.
The calculated TBCR from Tianjin in January is less than
zero as well. The following descriptions may explain these
phenomena. Except for the impact of the corresponding
precursors, the formation of sulfate, nitrate, and ammonium
can also be affected by the atmospheric oxidization capacity
and the emissions of other related pollutants. Take sulfate
for an example, its formation can be influenced by the
existence of SO2, NOx, NH3, and oxidizing substance such as
O3 (Wang et al., 2011; Behera and Sharma, 2012b). When
the pollutants emissions of Hebei (for example) were set to
zero, the sulfate in Beijing would changes in the following
 Lang et al., Aerosol and Air Quality Research, 13: 943–956, 2013 953

ways: (1) the primary sulfate (directly emitted from various
sources) transport from Hebei would decrease; (2) the
secondary sulfate formed by chemical reactions in Hebei and
during the transport would decrease, causing a reduction of
sulfate transport to Beijing; (3) the SO2, NOx transport from
Hebei to Beijing would also decrease, and this will reduce
the SO2, NOx concentration and change the O3 formation,
consequently impact the formation of sulfate in local Beijing.
And the influence on the O3 concentration in (3) would be
either positive or negative. It is dependent on the NOx and
VOC concentrations in the receptor district – Beijing (Xing
et al., 2011). As a result, the sulfate concentration changes
in (3) may be plus or minus. But in generally, if the
influence on the O3 formation would be not so significant,
the secondary particles concentration decrease in Beijing
would be plus because of the reduction of NOx, SO2 and
NH3. However, the actual sulfate transport from Hebei to
Beijing just contains (1) and (2). The existence of course (3)
results in the error between the results based on the zero–out
method and the actual sulfate transport contributions. The
zero–out method could make similar influence on nitrate and
ammonium. This is also the reason that results in the
phenomena mentioned in the beginning of this paragraph.
As a result, due to the natural uncertainty, the zero–out
would generally bring higher TBCR of secondary inorganic
particles. And the actual TBCR may be a little lower than
the results in this study. Further studies should be conducted
to avoid the errors brought by the zero–out method for
calculating the emission contribution ratio. This may include
the adoption of source apportionment technology, such as
PSAT (Particulate matter Source Apportionment Technology)
integrated in CAMx (Comprehensive Air Quality Model
with extensions) model (Huang et al., 2010).
Emission Contributions under Different PM2.5 Pollution
Levels
As mentioned before, a new National Ambient Air
Quality Standard (NAAQS) was proposed in China in the
beginning of 2012, with the introduction of two levels of
PM2.5 concentration standard. The class I level corresponds
to the daily average PM2.5 concentration of 35μg/m3, while
the class II level corresponds to the daily average PM2.5
concentration of 75 μg/m3. Based on the PM2.5 standards
and the simulated concentrations (Fig. 7) in Beijing under
emission scenarios S0 and S1, the emission contributions to
PM2.5 and its components in Beijing from its surrounding
regions under different PM2.5 pollution levels were
calculated. The results are listed in Table 3. Three different
PM2.5 pollution levels were examined, namely the daily
PM2.5 concentration of 0–35, 35–75, and greater than 75
μg/m3, respectively. The results of January were discussed
as an example. As shown in Fig. 7(a), the daily PM2.5
concentrations in January were higher than 75μg/m3 for 7
days, including January 8–10 and 16–19. The average trans–
boundary contribution ratio during these periods was 35.4,
56.3, 59.3, 56.4, and 26.8% for the concentrations of PM2.5,
sulfate, nitrate, ammonium, and other particles, respectively
(Table 3). During the periods when the PM2.5 concentrations
were 35–75 μg/m3, the TBCRs in January for PM2.5, sulfate,
nitrate, ammonium, and other particles were 24.2, 25.7, 58.6,
35.8, and 21.5%, respectively. These were 1.1–54.4% lower
than those during the periods with PM2.5 concentration of
over 75 μg/m3. When the air quality was excellent (i.e., the
PM2.5 concentration was lower than 35 μg/m3), the TBCRs
in January were 16.6, 19.5, 61.5, 29.8, and 14.5% for PM2.5,
sulfate, nitrate, ammonium and other particles, respectively.
The results listed in Table 3 confirm the positive correlation
between TBCRs from Beijing’s surrounding regions and
its PM2.5 concentrations.
Based on the PM2.5 standards and the simulated
concentrations in Beijing under emission scenarios S0 and
S2, the annual local emission contribution ratios to PM2.5
in Beijing under different PM2.5 pollution levels were also
calculated, and the results are presented Fig. 9. As different
from the trans–boundary impact from Beijing’s surrounding
regions, a negative correlation exists between the local
emission contribution ratio and the PM2.5 concentration in
Beijing. The annual average emission contribution ratios

Table 3. The average contributions to PM2.5 and inorganic particles in Beijing from its surrounding regions under different
PM2.5 pollution levels.
Daily PM2.5 concentration (μg/m3) January April July October Annual
> 75 35.4% 45.9% 88.3% 51.1% 54.6%
PM2.5 35–75 24.2% 26.6% 71.0% 42.8% 46.1%
0–35 16.6% 10.5% 37.9% 15.3% 17.4%
> 75 56.3% 50.0% 92.3% 50.0% 61.6%
Sulfate 35–75 25.7% 38.8% 76.9% 46.9% 50.6%
0–35 19.5% 5.5% 36.0% 10.2% 15.4%
> 75 59.3% 86.8% 99.3% 80.3% 83.2%
Nitrate 35–75 58.6% 72.3% 94.4% 82.8% 79.1%
0–35 61.5% 55.2% 88.0% 61.7% 63.5%
> 75 56.4% 73.9% 97.1% 66.0% 74.8%
Ammonium 35–75 35.8% 56.4% 89.2% 69.0% 65.7%
0–35 29.8% 23.5% 57.5% 33.2% 33.2%
> 75 26.8% 38.9% 60.9% 29.4% 40.5%
Other particles 35–75 21.5% 20.2% 44.7% 29.1% 30.7%
0–35 14.5% 10.5% 26.3% 11.5% 14.1%
954
PM2.5 contributions from Local Beijing (%)
100
80
60
40
20
0
January
Fig. 9. The average local emission contribution ratio to PM2.5 concentration in Beijing under different PM2.5 pollution levels.
from Beijing were 70.8, 62.5, and 30.7% for the PM2.5
concentration levels of 0–35, 35–75, and over 75 μg/m3,
respectively. However, the corresponding annual average
TBCRs from Beijing’s surrounding regions were 17.4, 46.1,
and 54.6%, respectively. This indicates that the trans–
boundary transport played a major role in Beijing’s PM2.5
concentration during the high pollution levels (i.e., > 75
μg/m3), while the local emission in Beijing played a major
role in its PM2.5 concentration during the lower pollution
levels (i.e., < 75 μg/m3). As a result, the mitigation of PM2.5
pollution in Beijing not only requires the reduction of local
emissions, but also needs the cooperation of its surrounding
regions, especially during the heavy pollution periods.
CONCLUSIONS
An intensive monitoring and modeling program was
implemented to investigate the regional PM2.5 transport
problem, with a case study being conducted in Beijing, China.
It was found that the inorganic components of SO42–, NO3–,
and NH4+ particles accounted for a significant proportion
of the total PM2.5 in Beijing, while the nitrate had the highest
percentage. To further investigate the emission contributions
to Beijing’s PM2.5 from different emission regions, a coupled
MM5–CMAQ modeling system was developed. The
concentrations of PM2.5 and its various components (sulfate,
nitrate, ammonium, and other particles) in Beijing during
four selected months in 2010 were simulated. Acceptable
modeling performance was obtained. A zero–out method
was used to calculate the emission contribution ratio from
different emission regions. It was found that the high PM2.5
concentration in Beijing generally corresponds to the high
trans–boundary emission contribution. And the contribution
from Hebei province accounted for a major part in the total
trans–boundary contributions. It was also found that the
trans–boundary transport from Beijing’s surrounding regions
had the highest contribution to Beijing’s PM2.5 pollution in
July. The trans–boundary transport impact on nitrate
concentration in Beijing was the greatest among all of the
PM2.5 particles. A positive correlation was found between
the trans–boundary emission contribution ratio and the PM2.5
Lang et al., Aerosol and Air Quality Research, 13: 943–956, 2013
3 3 3
>75g/m 35-75g/m 0-35g/m
April July October Annual
concentration in Beijing, but a negative correlation existed
between the local emission contribution ratio and the PM2.5
concentration. The results also illustrated that the trans–
boundary transport played a major role in Beijing’s PM2.5
concentration during the high pollution level period (i.e., >
75 μg/m3), while the local emission in Beijing played a major
role in its PM2.5 concentration during the lower pollution level
period (i.e., < 75 μg/m3). The high PM2.5 concentration in
Beijing may pose serious threats to the public health, and thus
needs effective mitigation. The results obtained from this
study indicated that the control of Beijing’s PM2.5 pollution
should require coordinated efforts in both Beijing and its
surrounding regions. In addition, the natural uncertainty of
zero–out method using for the investigation of secondary
particles transport was discussed. Generally, if the influence
on the O3 formation of the receptor region is not so
significant, the TBCR calculated based on the zero–out
method may be higher than the actual ones.
ACKNOWLEDGMENTS
This research was supported by the Natural Sciences
Foundation of China (No. 51038001 & 51208010), the
"Beijing Science and Technology Project"
(D09040903670801) of the Beijing Municipal Science &
Technology Commission, and the Ministry of Environmental
Protection Special Funds for Scientific Research on Public
Causes (No. 201209003&200909008). The authors would
also like to thank Beijing NOVA Program of China (No.
2009B07), Innovation Team Project of Beijing Municipal
Education Commission (PHR201007105) as well as the
Cultivation Fund of the Key Scientific and Technical
Innovation Project, Ministry of Education of China (708017)
for supporting this work.
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Received for review, September 13, 2012
Accepted, November 27, 2012