Atmospheric Environment 76 (2013) 11e20

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Atmospheric Environment
journal homepage: www.elsevier.com/locate/atmosenv

Emission trends and source characteristics of SO2, NOx, PM10 and

VOCs in the Pearl River Delta region from 2000 to 2009
Qing Lu a, b, Junyu Zheng a, b, *, Siqi Ye a, b, Xingling Shen a, b, Zibing Yuan b, c, Shasha Yin a, b
a

School of Environmental Science and Engineering, South China University of Technology, University Town, Guangzhou 510006, PR China
Pearl River Delta Atmospheric Environmental Research Joint Laboratory, Guangzhou 510006, PR China
c
Atmospheric Research Center, Fok Ying Tung Graduate School, Hong Kong University of Science and Technology, Nansha IT Park,
Guangzhou 511458, PR China
b

h i g h l i g h t s
< PRD emission trends were characterized and validated from 2000e2009.
< Variations in source characteristics were investigated and analyzed.
< SO2 emission began to decrease from 2005, while PM10 emission decreased from 2007.
< NOx and VOCs emissions exhibited upward trends during 2000e2009.
< Immediate control is needed on marine emission source in the PRD region.

a r t i c l e i n f o

a b s t r a c t

Article history:
Received 6 March 2012
Received in revised form
22 October 2012
Accepted 27 October 2012

Emission trends and variations in source contributions of SO2, NOx, PM10 and VOCs in the Pearl River
Delta (PRD) region from 2000 to 2009 were characterized by using a dynamic methodology, taking into
account the economic development, technology penetration, and emission control. The results indicated
that SO2 emissions increased rapidly during 2000e2005 but decreased signicantly afterward. NOx
emissions went up consistently during 2000e2009 except for a break point in 2008. PM10 emissions
increased by 76% during 2000e2007 but started to decrease slightly in the following years. VOCs
emissions presented continuous increase during the study period. Power plants and industrial sources
were consistently the largest SO2 and PM10 emission contributors. The on-road mobile source was the
largest emission contributor for VOCs and NOx emissions with decreasing contributions. The NOx
contribution from power plants and industrial sources kept increasing. Worthy of mention is that the
non-road mobile source is becoming an important SO2 and NOx contributor in this region. Comparisons
with satellite data, ground observations and national trends indicated that emission trends developed in
this study were reasonable. Implications for future air pollution control policies were discussed.
2012 Elsevier Ltd. All rights reserved.

Keywords:
Emission estimation
Source contribution
Control policy
Satellite data
Ground observations

1. Introduction
The PRD region, located in the southern coast of China, covers
cities of Guangzhou, Shenzhen, Zhuhai, Foshan, Dongguan, Zhongshan, Jiangmen, Huizhou and Zhaoqing (see Fig. 1). Beneted from
the implementation of Chinas reform and opening-up policies, the
PRD region has experienced rapid economic growth, with the
surging Gross Domestic Product (GDP) by 280%, fuel consumption by
150% and the population of passenger cars by 530% (GDPBS, 2001e

* Corresponding author. B4-514, School of Environmental Science and Engineering, South China University of Technology, South Campus, University Town,
Guangzhou 510006, PR China. Tel./fax: 86 20 39380021.
E-mail address: zheng.junyu@gmail.com (J. Zheng).
1352-2310/$ e see front matter 2012 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.atmosenv.2012.10.062

2010), respectively, from 2000 to 2009 (Figs. 2 and 8). However,

these dramatic growths have caused serious, complex and regional
air pollution problems (Zhang et al., 2008; Zheng et al., 2010). The
monitoring data showed that the annual average number of haze
days was over 100 and the observed highest ozone concentration
was up to 0.45 mg m
3 in the region (GDEMC and HKEPD, 2005e
2010; Deng et al., 2008), and the ozone background concentrations
increased by an average rate of 0.55 ppbv yr
1 during 1994e2007
(Wang et al., 2009a). These ndings indicated that air pollution
control in this region is challenging.
In order to improve air quality in the PRD region, both national
and local government agencies have made great efforts to formulate and issue various control measures and policies in the past
decade. These policies and control measures were summarized in

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Q. Lu et al. / Atmospheric Environment 76 (2013) 11e20

Fig. 1. The location of the PRD region and air quality monitoring stations.

Table S-1 in the Supplementary Material. These measures already

helped alleviate regional air pollution problems to some extent.
However, the monitoring data indicated that primary pollutant
concentrations still remained at high levels, and secondary ozone
and haze pollution episodes frequently happened (GDEMC and
HKEPD, 2005e2010). Therefore, further control measures and
policies are still needed in order to signicantly improve the air
quality in the PRD region.
Due to the dramatic economic growth, the adjustment of energy
structure, and implementation of emission control measures, it is
expected that source characteristics in this region have greatly
changed during the past ten years. In the meantime, the effectiveness and roles of implemented control measures and policies
have yet to be reviewed or assessed in a systematic and scientic
manner. In order to guide future control policy formulation, there is
a need for analyzing emission trends of primary pollutants (SO2,
NOx, PM10 and VOCs) and identifying variations in source characteristics in the PRD region.
The main objectives of this paper are to characterize emission
trends of primary pollutants from 2000 to 2009 and to assess the
impacts of control measures on source characteristics in the PRD
region. A dynamic methodology, by considering economic development, technology penetration, and emission control, was used to
estimate the emissions. The reliability of this analysis was validated
by comparing emission trends with the satellite data and ground
observations.

Guangdong-Hong Kong air pollution emission inventory handbook

(HG-JWGSDEP, 2008) and Zheng et al. (2009). Due to the absence of
detailed source-based activity data from 2000 to 2009, a top-down
approach was used in this study.
By referring to the technology-based methodology for analyzing
national emission trends (Lu et al., 2010; Zhang et al., 2007; Lei
et al., 2011), in this study, a dynamic approach, considering
economic development, technology penetration, and emission
control, was used to characterize the emission trends in the PRD

Table 1
Emission source categorization in the PRD region.
Category
Power plants
Industrial sources
Industrial solvent use
On-road mobile sources

Non-road mobile sources

2. Data and methods

2.1. Methods for estimating emissions
Non-industrial solvent use

Emission sources in eight major categories and twenty ve subcategories were considered in this study, as listed in Table 1. The
categorization was based on the source classication in the

Biomass burning
Residential fuel consumption

Sub-category

Heavy duty gasoline passenger cars

Heavy duty diesel passenger cars
Light duty gasoline passenger cars
Light duty diesel passenger cars
Heavy duty gasoline trucks
Heavy duty diesel trucks
Light duty gasoline trucks
Light duty diesel trucks
Buses
Taxies
Motorcycles
Marine
Agriculture machinery
Construction machinery
Airport
Railroad
Personal domestic product
Architecture surface coating

Q. Lu et al. / Atmospheric Environment 76 (2013) 11e20

region. The emissions were estimated for different years by the

Equation (1) below:

En

X
i;k;l

Ai;k;l;n

X
 Xh 
i
Zj 1
hj
Xi;k;l;m;n EFk;l;m;n
m

(1)

Where i, k, l, m, n, j represent the city, emission source, the fuel or

product type, the technology type, the year, control technology,
respectively. E represents regional emissions of SO2, NOx, PM10 or
VOCs, A stands for the activity level (such as fuel consumption or
material production), Xm is for the proportion of fuel or production
for a sector that is consumed or produced by technology m. Z is the
proportion of the control technology j, hj is the removal efciency of
control technology j. EF is the emission factor. SO2 emission factors
of fuel combustion sources can be calculated by Equation (2):

EF 2  S  1
SR

(2)

Where S and SR represent the sulfur contents and sulfur retention

in ash, respectively. Besides, emissions from on-road mobile sources were estimated by Equation (3):

En

X

Pi;n  Mi;n  EFi;n

(3)

Where, i, n represent the vehicle class, the year, respectively. P is the

vehicle population, M is the annual mileages traveled. Detailed
methods for estimating emissions from different sources were
described in previous studies (Che et al., 2009) and summarized in
Table S-2 in the Supplementary Material. Table S-2 also listed the
data sources by sectors.
2.2. Activity data and emission factors
2.2.1. Activity data processing
Generally, estimating a long term emission trend is much more
challenging than just developing an annual emission inventory, due
to the limitation of the availability, consistency and accuracy in
activity data and emission factors (Zhang et al., 2007). In this study,
we referred much on ofcial statistics for most activity data (e.g.,
fuel consumption, vehicle population, product output, as shown in
Table S-2 in the Supplementary Material). However, these data
sources were either lack of detailed activity data for some emission
sources or inconsistent among different years, or missing for some
years or emission sources, therefore, surrogate data have to be used
with certain level of data processing. Detailed activity data processing for power plants, industrial combustion sources and onroad mobile sources were presented in the following sections.
The activity data of power plants and industrial combustion
sources at city level were collected from ofcial statistical reports
(BSPRD, 2001e2010). However, in order to reduce the effects of
data gaps on emission trends, we mainly considered three major
fuel types including coal, fuel oil and natural gas consumed in
power plants and industrial combustion sources for all cities during
the study period. Since electricity generation has strong association
with power plant fuel consumptions, we used the electricity
generation data to estimate the missing fuel consumption data by
taking into account changes in fuel structures and improvements in
fuel efciency in power plants. The gross industrial output values
available in the Guangdong Statistical Yearbook (GDPBS, 2001e
2010) were used as conversion factors to estimate the missing
data in industrial combustion sources, by considering the variation
in energy intensity.
For on-road mobile sources, 11 vehicle types were considered
including eight types of passenger cars and trucks (gross weight:

13

heavy or light duty, fueled by diesel or gasoline), buses, taxis and

motorcycles. However, numbers of passenger cars and trucks were
typically collected by gross weight without differentiation of fuel
types in current ofcial statistical yearbooks. In view of this, we
conducted a survey and reviewed previous studies (Che et al., 2009)
to estimate the ratios of gasoline to diesel vehicles with different
gross vehicle weights, and then calculated the numbers of eight
types of passenger cars and trucks based on the above ratios.
2.2.2. Determination of emission factors and control efciencies
Emission factors and control efciencies are greatly inuenced
by control measures, control technologies and emission standards.
In the past ten years, great efforts have been made to reduce
primary air pollutant emissions, such as desulfurization for power
plants and industrial sources and upgraded emission standards for
motor vehicles. In order to reect the possible impacts from these
measures, dynamic emission factors and control efciencies in
different years or cities were used to estimate the emission trends.
In the following paragraphs, we introduced the approach to
determine emission factors and control efciencies for three major
sources across years, including power plants, industrial sources and
on-road mobile sources.
Emission factors of on-road mobile sources were typically estimated by using mobile emission estimation models with inputs of
vehicle technology distribution, fuel types, fuel economy and
annual mileage traveled (He et al., 2005). Due to the lack of detailed
eet and technology information from 2000 to 2009, emission
factors cannot be estimated by mobile emission estimation models
for each year. In this study, we utilized the International Vehicle
Emission (IVE) Model (UCR, 2008) to estimate 2007-based motor
vehicle mission factors in the PRD region with the use of PRD local
emission rates, vehicle emission standards, local ambient conditions and other local data. The emission factors for other years were
estimated based upon 2007-based emission factors by taking into
account the schedule of upgrading vehicle emission standards
(including National 0, I, II and III) in the PRD region, the difference
between vehicle emission factors under different emission standards, and the vehicle numbers by types and years.
Emission factors and control efciencies of power plants and
industrial sources were traditionally determined by the fuel property, combustion equipment and removal technology. The regional
average sulfur content (S) of coal were 0.89% in 2000 (Chen, 2001)
and 0.80% in 2009 (PGGDP, 2010). Since no reliable data were
available, interpolation values were used to calculate the average
sulfur content (S) in each year during 2000e2009 (Lu et al., 2010).
SO2 removal efciencies of power plants and industrial sources
were derived from Equation (4), due to lack of emission control
technology distribution and penetration data from 2000 to 2009

hn Rn =Rn En

(4)

Where R is the regional SO2 removal amount from a specic

emission source, E is the pollutant discharge amount, h is the
average removal efciency of SO2 control technology, n is the year.
The related data were collected from emission source census data,
ofcial statistical reports (EPBGDP, 2001e2009; NBSC, 2003e2009)
and power plant industrial reports (CAEPI-CDDRBK, 2008, 2009,
2010). PM10 removal efciencies were collected from the Environment Statistical Bulletin of Guangdong Province (EPBGDP, 2001e
2009) and national studies (Zhang et al., 2006). Annual average
removal efciencies trends were shown in Figs. 4, 5 and 9 and
Fig. S-4 in the Supplementary material.
NOx and PM10 emission factors of power plants and industrial
sources were obtained from eld investigations conducted on
major point emission sources in the PRD region (HKEPD, 2011) and

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Q. Lu et al. / Atmospheric Environment 76 (2013) 11e20

the emission source census data in 2007 and 2009, with considering the effect of policy implementation on emissions. The NOx
and PM10 emission factors trends of power plants and industrial
sources used in this study were shown in Fig. S-1 in the
Supplementary Material. With respect to VOCs emission factors,
although eld investigations of key VOCs-related industries like
printing, wood furniture manufacturing, shoemaking, paint and
coating manufacturing, and others were conducted in the PRD
Region, VOCs-related control and process technology variations
during the study period were not available, emission factors were
assumed to be xed in this study. Detailed emission factors of major
emission sources were summarized in Tables S-3e6 in the
Supplementary Material.
3. Results and discussion
3.1. Emission trends in the PRD region
SO2, NOx, PM10 and VOCs emission trends from anthropogenic
sources in the PRD region from 2000 to 2009 were shown in Fig. 2.
SO2 emissions increased rapidly from 2000 to 2005 with total
emissions increased by 72% while the GDP increased by 120%,
mainly driven by the rapid growth of fossil fuel consumption
without strict SO2 control. In response to the implementation of
SO2 control measures for power plants and industrial sectors, SO2
emissions decreased signicantly after 2005 and nearly halved in
2009, compared to 2005, indicating the effectiveness of control
measures adopted by governments in recent years. This trend was
basically consistent with Chinese national SO2 trends, in which the
national SO2 emissions increased by 53% from 2000 to 2006 and
began to decrease after 2006 (Lu et al., 2010).
Emission trends of NOx and PM10 exhibited similar patterns as
shown in Fig. 2. During 2000e2009, the GDP in the PRD region
increased by 282%, while NOx and PM10 emissions increased by
96% and 66%, respectively. NOx emissions in the PRD region kept
a consistent growth from 2000 to 2009, with lower growth rates
in recent years, while PM10 emissions kept increasing from 2000
to 2007 with annual growth rates from 2% (in 2006) to 13% (in
2005), but slightly declined after 2007. The reason for differences
in growth rates between emissions and GDP may be the implementation of a series of control measures on vehicles, power
plants and industrial boilers by national and local government
agencies in recent years, and the increased GDP contributions of
non-production sector, from 44% in 2001 to 50% in 2009 (GDPBS,

2001e2010). In comparison with national NOx and PM10 emission

trends, similar upward trend was also identied in the national
NOx emissions with an increase of 55% during 2001e2006 (Zhang
et al., 2009), while the growth rates of PM10 emissions in the PRD
region increased faster than that in the national trend during
2000e2005 (Zhang et al., 2009), probably due to the more rapidly
increasing GDP in this region.
VOCs emissions remained steadily increasing with annual
growth rates ranging from 2% to 10%. The stable growth can be
attributed to the signicant increase of vehicle population and the
increasing use of industrial solvent arising from rapid economic
development. Compared to other three primary pollutants, uctuations of VOCs emission growth rates were much smaller. This
was probably because most of VOCs emission control measures or
policies were targeted on vehicle source with less focus on other
emission sources. Additionally, the VOCs emission trend in the PRD
region was similar to the national one with an upward trend (Zhang
et al., 2009).
3.2. Variations in source characteristics
In this section, we discussed variations in source characteristics
of SO2, NOx, PM10 and VOCs during the past decade and identied
possible impacts of policies and control measures on source characteristics. Besides, differences in source contributions between the
PRD region and the whole China were analyzed.
3.2.1. SO2 emissions
Fig. 3 presented variations in SO2 source contributions from
2000 to 2009. Apparently, although power plants and industrial
sources showed declining trends in contributions, they were still
major contributors, accounting for 92% in 2000 and 82% in 2009. In
addition, the contribution of non-road mobile sources showed an
upward trend, accounting for 6% in 2000 and 15% in 2009 of PRD
regional SO2 emissions. The PRD regional SO2 source characteristics
were similar to national ones, in which power plants and industrial
sources were major contributors with around 90% of total national
SO2 emissions since 2000 (Lu et al., 2010).
Figs. 4 and 5 showed the SO2 emission trends and related data
for power plants and industrial sources. Generally, SO2 emissions of
both power plants and industrial sources shared similar upward
trends from 2000 to 2005, together with energy consumption,
electricity generation and the number of large industrial enterprises. However, although electricity generation and the number of

4.0

1.8
1.6

Normalized emission

Normalized value

3.5
3.0
2.5
2.0

1.4
1.2
1.0
0.8
0.6
0.4

1.5

0.2
1.0

0.0
2000

2001

2002

2003

2004

2005

2006

2007

2008

2009

0.5
2000
GDP

2001

2002

2003

Fuel consumption

2004

2005
SO2

2006
NOx

2007

2008
PM

2009
VOCs

Fig. 2. Trends in pollutant emissions, GDP and fuel consumption (All data are
normalized to the year 2000).

Power plants
On-road mobile sources
Biomass burning

Industrial sources
Non-road mobile sources
Residential fuel consumption

Fig. 3. Contribution trends of SO2 by categories (All data are normalized to the year
2000).

Q. Lu et al. / Atmospheric Environment 76 (2013) 11e20

3.5

70

3.0

60
50

1.5

40
1.0

30

20
0.5
10

2000

2001

2002

2003

2004

2005

2006

2007

2008

1.0

2000

2001

2002

2003

2004

2005

2006

2007

2008

2009

Energy consumption

Marine

Airport

Electricity generation

SO removal efficiencies

Agriculture machinery

Consturction machinery

Railroad

Freight transfer volumes in ports

3.0

70

2.5

60
50

2.0

40
1.5
30

1.0

20

0.5

10

0.0

0
2002

2003

2004

2005

2006

2007

2008

2009

SO emission

Energy consumption

Large industrial enterprises

SO removal efficiencies

Fig. 6. Trends in SO2 emission from marine (non-road) source and related activity data
(All data are normalized to the year 2000).

development of waterway and marine transportation industries in

this region. However, limited control measures were targeted on
non-road mobile sources in this region at present.
3.2.2. NOx emissions
Fig. 7 showed variations of NOx source contributions from 2000
to 2009. Obviously, on-road mobile source was the largest
contributor, although its contribution presented a decreasing trend,
from 41% in 2000 to 38% in 2009. In addition, power plants and
industrial sources also made great contributions to NOx emissions.
Contributions of power plants uctuated around 24e28% from
2000 to 2009 while contributions of industrial sources increased
slightly, from 17% in 2000 and 20% in 2009. The most signicant
increase was the non-road mobile source with doubled emissions
and its contribution reaching 14% in 2009. In comparison with
national NOx source characteristics (Ohara et al., 2007), the largest
NOx contributor was the on-road mobile source in the PRD region,
while nationally it was power plant source.
Fig. 8 showed trends in NOx emissions from on-road mobile
sources and vehicle population from 2000 to 2009. The vehicle
population increased much faster than NOx emissions after 2005,

2.0

SO2 removal efficiencies (%)

Normalized value

1.5

SO emission

large industrial enterprises kept increasing after 2005, the energy

consumption clearly dropped after 2007, and SO2 emissions from
both power plants and industrial sources decreased signicantly.
Installing and operating ue gas desulfurization (FGD) facilities in
power plants and large industrial boilers were main reasons for the
rapid decrease of SO2 emissions. Such decreasing may also be
attributed to the implementation of control measures like shutting
down of small and high-emitting power generation units and
industrial boilers, limiting fuel sulfur contents and increasing the
proportion of clean energy consumption (PGGDP, 2004). As shown
in Figs. 4 and 5, there were higher removal efciencies in power
plants than industrial source, this was mainly because FGD devices
were required to install in all power plants with strict supervision,
while only required in larger industrial boilers for industrial sources, which led to relatively low removal efciencies for industrial
sources on average.
Fig. 6 showed SO2 emission contributions and related activity
data trends for non-road mobile sources. Among non-road mobile
sources, marine was the largest SO2 contributor, accounting for 8%
of total emissions on average and the contribution increased by 12%
per year. This was similar to the trend of freight transfer volumes in
ports, arising from well-developed river systems and the rapid

2001

2.0

0.0

2009

Fig. 4. Trends in SO2 emission from power plants and related activity data (All data
except SO2 removal efciencies are normalized to the year 2000).

2000

2.5

0.5

0.0

Fig. 5. Trends in SO2 emission from industrial sources and related activity data (All
data except SO2 removal efciencies are normalized to the year 2000). Note: Large
industrial enterprises refers to those with the annual main business income over 20
million RMB.

1.8

Normalized emission

Normalized value

2.0

Normalized emission

80

SO2 removal efficiencies (%)

2.5

15

1.6
1.4
1.2
1.0
0.8
0.6
0.4
0.2
0.0
2000

2001

2002

2003

2004

2005

2006

2007

2008

2009

Power plants

Industrial sources

On-road mobile sources

Non-road mobile sources

Biomass burning

Residential fuel consumption

Fig. 7. Contribution trends of NOx by categories (All data are normalized to the year
2000).

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Q. Lu et al. / Atmospheric Environment 76 (2013) 11e20

5.0
2.0

4.0
3.0

1.5

2.0
1.0

1.0

3.0

Normalized emission

2.5

Normalized vehicle population

6.0
Normalized emission

3.5

7.0

3.0

2000

2001

2002

2003

2004

Number of passenger cars

2005

2006

2007

Number of trucks

2008

2.0
1.5
1.0
0.5
0.0

0.0

0.5

2.5

2000

2009

NOx emission

Fig. 8. Trends in NOx emission from on-road mobile sources and vehicle population
(All data are normalized to the year 2000).

2001

2002

2003

2004

2005

2006

2007

2008

2009

Marine

Airport

Agriculture machinery

Consturction machinery

Railroad

Freight transfer volumes in ports

Fig. 10. Trends in NOx emission from marine (non-road) source and related activity
data (All data are normalized to the year 2000).

due to upgraded motor vehicle emission standards, such as the

National II implemented in 2005 and National III implemented in
2008 (PGGDP, 2009b). Additionally, measures like phase-out of
high-emitting vehicles together with the popularization of clean
fuel vehicles such as gas vehicles, hybrid vehicles and electric
vehicles (PGGDP, 2004) have also contributed to the reduced NOx
emission growth rates under the pressure of rapid vehicle population growth.
Fig. 9 showed the relationship between NOx emission trends and
related data of power plants from 2000 to 2009. There were similar
increasing trends in NOx emissions from power plants to those in
energy consumption and electricity generation before 2005.
However, both NOx emissions and energy consumption dropped in
2006 while they resumed to decline after 2007. This may be
probably because the deadline of shutting down small-scale
thermal power units was at the end of year 2005 (PGGDP, 2004),
resulting in the improvement of fuel efciency and the reduced fuel
consumption and NOx emission in 2006. Similar phenomenon was
found in industrial sources and details were provided in the
Supplementary Material (Fig. S-4).
Except for three largest contributors, non-road mobile source
was becoming an important NOx contributor in the PRD region
during the study period. Among non-road mobile sources, as
shown in Fig. 10, marine was the major contributor, accounting for
69% of total non-road mobile sources emission on average with an

2.2

80

2.0

70

increasing trend from 62% to 72%, indicating marine source was

becoming one of major NOx emission sources in this region.
3.2.3. PM10 emissions
Fig. 11 showed variations in PM10 source contributions from
2000 to 2009. Power plants and industrial sources were major
contributors, with average contributions of 37% and 32%, respectively. The contribution of industrial sources presented a relatively
rapid growing trend (29% in 2000 and 36% in 2009), while the
contribution of power plants kept relatively steady (34% in 2000
and 38% in 2009). Besides, biomass burning and on-road mobile
sources were important PM10 contributors. There were similar
PM10 source characteristics in the PRD region, in comparison with
national ones, in which power plants and industrial sources
contributed nearly 70% of total national PM10 emissions in 2000
and 2005 (Lei et al., 2011).
Fig. 9 showed the relationship between PM10 emission trends
and related data of power plants from 2000 to 2009. PM10 emissions from power plants presented similar increasing trends with
those in energy consumption and electricity generation before
2005. However, both PM10 emissions and energy consumption
dropped in 2006 while they resumed to decline after 2007. This can
be attributed to the measures of closing small and high-emit power

2.0

60

1.6
50
1.4

40

1.2
1.0

30

0.8

20

Normalized emission

1.8

PM10 removal efficiencies (%)

Normalized value

1.8
1.6
1.4
1.2
1.0
0.8
0.6
0.4
0.2
2000

2001

2002

2003

2004

2005

2006

2007

2008

2009

0.0
2000

2001

2002

2003

2004

2005

2006

2007

2008

2009

NOx emission

Energy consumption

Power plants

Industrial sources

Electricity generation

PM

On-road mobile sources

Non-road mobile sources

Biomass burning

Residential fuel consumption

PM

emission

removal efficiencies

Fig. 9. Trends in NOx and PM10 emissions from power plants and related activity data
(All data except PM10 removal efciencies are normalized to the year 2000).

Fig. 11. Contribution trends of PM10 by categories (All data are normalized to the year
2000).

Q. Lu et al. / Atmospheric Environment 76 (2013) 11e20

1.6
1.4
1.2
1.0
0.8
0.6
0.4
0.2
0.0
2000

2001 2002 2003 2004

Power plants
Industrial solvent use
Non-road mobile sources
Biomass burning

2005

2006 2007 2008 2009

Industrial sources
On-road mobile sources
Non-industrial solvent use
Residential fuel consumption

Fig. 13. Contribution trends of VOCs by categories (All data are normalized to the year
2000).

presented declining trends, from 10% to 7% and 12% to 5% respectively; while contributions from power plants, non-road mobile
sources and industrial sources kept quite stable during the study
period.
Fig. 14 showed VOCs emission contributions from on-road
mobile sources by vehicle types from 2000 to 2009. Apparently,
motorcycles and passenger cars were major vehicle types for VOCs
emissions, accounting for 56% and 29% of regional on-road mobile
sources emission on average, respectively. The number of motorcycles decreased by 7% from 2005 to 2009, due to the restriction or
prohibition on motorcycles within urban areas in most cities of the
PRD region (Che et al., 2011), with its contributions decreasing from
57% in 2005 to 45% in 2009. The number of passenger car increased
by 530% during the ten years, while its emission contribution just
increased from 17% in 2000 to 41% in 2009, due to the implementation of more strict vehicle emission standards.
As shown in Fig. 13, the VOCs emission from the industrial
solvent use source has tripled during the ten years. Although some
VOCs-related industrial sectors were equipped with VOCs gathering and treatment devices (e.g., activated carbon/water adsorption, catalytic combustion), the removal efciency still remained at

1.4

1.8

1.6

1.2

Normalized emission

Normalized emission

1.4

1.0
0.8
0.6
0.4

1.2

1.0
3
0.8
0.6

0.4
1
0.2

Normalized vehicle population

3.2.4. VOCs emissions

Fig. 13 showed variations in VOCs source contributions from
2000 to 2009. Obviously, the on-road mobile source was the largest
VOCs contributor, accounting for 57% of PRD regional VOCs emissions on average with a slight declining trend from 58% to 53%,
followed by the industrial solvent use source which accounted for
24% of regional total emissions on average, with an increasing trend
from 18% to 33% during the ten years. VOCs emission contributions
of both non-industrial solvent use and biomass burning sources

1.8

Normalized emission

generation units, restricting coal-red power plants, and encouraging the use of hydro-electric power and natural gas (PGGDP,
2004, 2009a). Similar trends were found in industrial sources and
details were provided in the Supplementary Material (Fig. S-4). It
was noteworthy that the emissions of PM10 did not decline significantly as the one of SO2 did. Generally, the two trends were
supposed to be consistent since the installation of desulphurization
system may lead to enhanced PM removal efciency (Zhao et al.,
2008). In our case, the slight inconsistency might be attributed to
the following reasons: (1) since the real removal efciencies were
determined by not only the technology itself but also the operating
conditions and managements (Zhang, 2005), the removal efciencies of PM10 were lower than that of SO2 control, partly due to lack
of strict supervision and management since currently PM10 emission has not been taken into national evaluation index system yet;
(2) the wide use of low sulfur coals in power plants and major
industrial sectors in recent years also led to the large amount of SO2
emission reductions. The monitoring data showed that the
decreasing rates of SO2 and PM10 concentrations from 2005 to 2009
were 19% and 9% respectively (GDEMC and HKEPD, 2005e2010),
indicating the PM10 emission trend developed in this study was
reasonable, though there was inevitable uncertainty.
Fig. 12 showed trends in PM10 emission from the biomass
burning source from 2000 to 2009. Biomass burning included
domestic biofuel combustion, eld burning of crop residues and
forest re (He et al., 2011). The PM10 emission from biomass
burning showed a relatively steady trend, but its contributions
decreased rapidly, from 23% in 2000 to 13% in 2009.
It must be pointed out that road dust and construction sources
were important PM10 emission contributors in the PRD region.
However, due to the lack of detailed activity data and local emission
factors, analysis of PM10 emission trends from road dust and
construction sources were not made in this study. Further investigations and studies were needed for these two sources in the future.

17

0.2
0.0

0
2000

0.0
2000

2001

2002

2003

Domestic biofuel combustion

2004

2005

2006

2007

2008

Field burning of crop residues

2009
Forest fire

Fig. 12. Trends in PM10 emission from biomass burning (All data are normalized to the
year 2000).

2001

2002

2003

2004

Motorcycles
Trucks
Taxies
Number of passenger cars

2005

2006

2007

2008

2009

Passenger cars
Buses
Number of motorcycles

Fig. 14. Trends in VOCs emission from on-road mobile sources and vehicle population
(All data are normalized to the year 2000).

18

Q. Lu et al. / Atmospheric Environment 76 (2013) 11e20

a low level at present due to the limitation of control technology,

ineffective operation, or less supervision.
3.3. Comparison with satellite data and ground observations
In order to validate the reliability of emission trend analysis, NOx
and PM10 emissions trends were compared with satellite data, and
SO2, NOx and PM10 emission trends were compared with ground
observations, depending on data availability. Since the PRD
Regional Air Quality Monitoring Network was established in 2005,
and started to operate in the next half year in 2005 (Zheng et al.,
2010), in order to keep the consistency of ground observation
data used for comparison and to make the comparison scientically
sound, in this study, we only utilized 2005e2009 ground observations for comparisons. The NO2 column concentrations used in
this study were data products by the Institute of Environmental
Physics (IUP), University of Bremen, from GOME (2000e2002) and
SCIAMACHY (2003e2009) satellites, using the Differential Optical
Absorption Spectroscopy-Method (DOAS) (Richter et al., 2005). The
spatial resolutions of GOME and SCIAMACHY are 0.5  0.5 and
0.125  0.125 , respectively. The dry surface extinction coefcient
(SECdry) data with 2-km resolution were used to compare with
PM10 emission trends in this study. The SECdry data were retrieved
from MODIS aerosol optical depth (AOD) data acquired from NASAs
Goddard Earth Sciences Distributed Active Archive Center, using
the aerosol retrieval algorithms developed by Li et al. (2003), with
vertical distribution correction and relative humidity correction (Li
et al., 2005). The domain for retrieved satellite data was the same as
the emission domain used in this study.
Fig. 15 showed trends in NOx emissions and satellite-based NO2
column concentrations from 2000 to 2009. Generally, trends in NOx
emissions and satellite-based NO2 column concentrations presented broad agreement in temporal evolution. Both presented
continuous growths (from 2000 to 2004, increased by 55% and 82%,
respectively; from 2005 to 2007, increased by 13% and 9%, respectively) except that emission in 2008 showed a slight drop. The
growth rates of emissions were lower than those of satellite
observations during 2000e2004, similar to the situation over China
(Zhang et al., 2007). However, the large discrepancy between
emission trends and satellite observations in 2004e2005 can be
attributed to the uncertainty in emission estimates, variability in
meteorology, NOx injection height, and the increasing trend of
sulfate aerosols (Zhang et al., 2007). As shown in Fig. 15, there was
a good agreement between NOx emissions and ground observations

during 2005e2009, indicating the reasonability of NOx emission

trend developed in this study.
Fig. 16 showed trends in PM10 emissions and satellite-based
SECdry values from 2000 to 2009. Basically, PM10 emissions and
satellite-based SECdry values presented similar patterns in temporal
evolution, both of which increased at almost the same rates from
2000 to 2004 except that the SECdry value dropped in 2002.
Another discrepancy occurred during 2004e2006 when PM10
emissions continued to grow but the satellite data started to
decline slightly. Both emissions and the SECdry values presented
downward trends from 2007 to 2009. In comparison, a general
downward trend in PM10 emissions but an upward trend in AOD
was observed over the whole China in 2004e2009 (Lin et al.,
2010). The complex relationship between PM10 emissions and the
satellite data was probably because the AOD generally has a closer
association with PM2.5 than with PM10 (Lin et al., 2010). Besides,
there was a good agreement between PM10 emission trend and
ground observations during 2005e2009. These results indicated
that PM10 emission trend developed in this study was reasonable,
to some extent.
Fig. 17 showed trends in SO2 emission from 2000 to 2009 and
ground observations from 2005 to 2009. There was a very good
agreement between emission and ground observations, both
showing signicant downward trends after 2005. The big discrepancy in 2005 might be attributed to the fact that the PRD regional
monitoring network started the trial operation in the next half year
of 2005, which may not be able to represent regional averaged SO2
concentrations over the whole year.
3.4. Implication for air pollution control policy
The implementation of control policies and measures did reduce
SO2 and PM10 emissions in the PRD region, as shown in this study.
However, concentrations of primary and secondary pollutants still
remain at high levels at present, indicating the importance of
implementing further control measures in this region. In this
section, policy implications for future air pollution control were
discussed based upon the identication of emission trends and the
characterization of source contributions from this study.
Although signicant reductions in SO2 emissions were made in
the past decade, strict control and management of SO2 emissions is
still needed (Xu et al., 2009; Xu, 2011) for further decreasing SO2
concentrations and effectively controlling ne particulate pollutions, a commonly concerned air pollution issue in China. This

2.1

2.1
1.9

Normalized emission

Normalized emission

1.9
1.7
1.5
1.3
1.1

1.7
1.5
1.3
1.1

0.9

0.9

0.7

0.7

0.5

0.5

2000

2001

2002

2003

2004

NOx emissions

2005

2006

2007

2008

2009

Satellite-based NO columns

NOx ground observations

Fig. 15. Trends in NOx emissions, satellite-based NO2 column concentrations, and
ground NO2 concentrations (All data are normalized).

2000

2001

2002

2003

2004

PM10 emissions

2005

2006

2007

2008

2009

Satellite-based SECdry values

PM10 ground observations

Fig. 16. Trends in PM10 emissions, satellite-based SECdry values, and ground PM10
concentrations (All data are normalized).

Q. Lu et al. / Atmospheric Environment 76 (2013) 11e20

precursor for formations of ozone and secondary organic aerosol

(SOA). Thus, controlling VOCs emissions is critical to signicantly
alleviate ozone and ne particulate pollutions in this region. Based
upon this study, VOCs emissions from industrial solvent use source
grew rapidly, implying that control of VOCs emissions from this
source in the PRD region is of great importance in the future. In
addition, control of vehicle emissions should still be on the top
priority in reducing VOCs emissions in this region, since vehicle
source is expected to be still the largest VOCs contributor with
rapidly increasing vehicle population in the next ve or ten years.

1.9
1.7

Normalized emission

19

1.5
1.3
1.1
0.9

0.7

4. Summary and conclusions

0.5
2000

2001

2002

2003

SO emissions

2004

2005

2006

2007

2008

2009

SO ground observations

Fig. 17. Trends in SO2 emissions and ground SO2 concentrations (All data are
normalized).

study showed the effectiveness of current SO2 control measures on

power plants and industrial sources. These measures should be
further promoted under strict supervision and be targeted on other
sources. Specially, marine sources became the third SO2 contributor
with an increasing trend but few measures have been implemented
in the past decade, lowering sulfur contents in fuel of ships or
vessels or installing SO2 control devices is one of top priorities for
reducing marine SO2 emissions in the next few years.
Upgrading motor vehicle emission standards and phasing out
high-emitting vehicles alleviated the growth of NOx emissions in the
PRD region, to some extent. However, this study showed that NOx
emission still presented an upward trend from 2000 to 2009.
National Ministry of Environmental Protection (MEP) listed NOx
control as a top priority during the national Twelfth-Five plan. In
terms of NOx source characteristics in the PRD region from this study,
priority measures for reducing NOx emissions in this region may
include the wide use of low NOx burners and ue gas denitrication
technology on power plants and industrial sources, further
upgrading vehicle emission standards, control of non-road mobile
sources especially the marine source. It must be pointed out that
cautions need to be taken in reducing NOx emissions since there are
complicated non-linear relationships in NOx/VOC ratios for ozone
formation in the PRD region (Zhang et al., 2008). Previous studies
(Wang et al., 2009b; Zhang et al., 2008) showed that ozone formation
was typically under VOC-limited regime in urban areas of the PRD
region, while most likely under NOx-limited regime in surrounding
rural areas. This implies that reducing NOx emissions without
simultaneously controlling VOCs emissions with proper ratios, vice
versa, may lead to elevated ozone concentrations in this region.
Although power plants and large-scale industrial boilers have
been equipped with particulate matter control devices in recent
years, the regional PM10 emission still remained at relatively high
level. Such control devices should be further installed in middle and
small-scale industrial sources. Biomass burning and heavy-duty
diesel vehicles are important PM10 emission contributors in this
region, more strict control measures should be taken on these
sources. Road and construction dust sources made large contributions to PM10 emission in the PRD region, but have not been
effectively controlled. Future work should enhance the control of
dust sources and extend target areas to both urban and rural
regions.
VOCs emissions kept consistently increasing from 2000 to 2009
in the PRD region though restricting motorcycles in urban areas and
upgrading motor vehicle emission standards helped reduce VOCs
emissions from vehicles, to some extent. VOCs is an important

Emission trends and variations in source contributions of SO2,

NOx, PM10 and VOCs in the PRD region from 2000 to 2009 were
characterized by using a dynamic approach. The emission trend
results showed that SO2 emissions increased rapidly during 2000e
2005 but decreased signicantly afterward. NOx emissions went up
consistently during 2000e2009 except for a break point in 2008.
PM10 emissions increased by 76% during 2000e2007 but started to
decrease slightly in the following years, and VOCs emissions presented a continuous increase during the study period. The source
characterization results showed that power plants and industrial
sources were consistently the largest contributors to SO2 and PM10
emissions, the on-road mobile source was the largest NOx and VOCs
contributor, and industrial solvent use source was becoming an
important VOCs emission source. Worthy of attention is that nonroad mobile sources gradually become important SO2 and NOx
emission contributors in the PRD region, which need immediate
control actions on them.
In order to validate the emission trends, comparisons with
satellite data and ground observations were made, where applicable. The results showed that emission trends presented broad
agreements with the satellite data and ground observations, indicating that emission trends developed in this study were reasonable.
Acknowledgments
This work was supported by National Natural Science Foundation of China-Guangdong (NSFC-GD) Key Project (U1033001),
International Technology Cooperation Plan of Guangdong Province
(2011B050300006) and The Fundamental Research Funds for the
Central Universities, South China University of Technology
(2011ZZ0009).
Appendix A. Supplementary material
Supplementary material related to this article can be found
online at http://dx.doi.org/10.1016/j.atmosenv.2012.10.062.
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