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Atmospheric Environment 36 (2002) 49074918

Vertical and horizontal proles of airborne particulate matter


near major roads in Macao, China
Ye Wua, Jiming Haoa,*, Lixin Fua, Zhishi Wangb, Uwa Tangb
a

Department of Environmental Science and Engineering, Tsinghua University, Beijing 100084, Peoples Republic of China
b
Faculty of Science and Technology, University of Macao, Macao, Peoples Republic of China
Received 5 April 2002; accepted 28 June 2002

Abstract
Vertical proles, horizontal proles and size distribution of airborne particulate matter were measured near major
roads in Macao using DustTrak and TEOM monitors. A signicant decrease in the concentrations of PM10, PM2.5 and
PM1, as the height above the ground increases from 2 to 79 m, was found. At the height of 79 m, the concentrations of
PM10, PM2.5 and PM1, decrease to about 60%, 62% and 80% of the maximum occurring at 2 m above the ground,
respectively. However, the horizontal proles near another major road revealed there was no signicant trend of
decrease in concentrations of particulate matter as the distance from the road increases. Over the total measured
distance (0228 m), the maximum decreases of PM10, PM2.5 and PM1 are only 7%, 9% and 10%, of the maximum
occurring at 2 m from the road, respectively. The daytime averaged PM2.5 and PM1 contribute 6667% and 5160%,
respectively, of the total PM10 mass after the particle readings by DustTrak were recalibrated by TEOM. It showed that
ne particles and submicrometer particles contributed a major part of PM10 at the roadside in Macao, which is most
likely attributed to the combinations of local sources including exhausted particulate matter from vehicles and
resuspended ne dust, and secondary particles (sulfate, nitrate and ammonium) of regional scales.
r 2002 Elsevier Science Ltd. All rights reserved.
Keywords: PM10; PM2.5; PM1; Vertical prole; Horizontal prole; Particle size distribution; Trafc

1. Introduction
Throughout the last 30 years, an increasing body of
research has consistently shown statistically signicant
positive associations between ambient PM10 and daily
mortality counts and various indices of morbidity, and
these associations appear stronger for ne particles,
which are generally marked as PM2.5 (US EPA, 1996;
Vedal, 1997; IIASA, 2000a, b). Based on the totality of
evidence, many countries and international organizations issued air quality standards for airborne particulate matter to protect public health. PM10 and PM2.5
were introduced as a standard in the US in 1987 and
*Corresponding author. Tel.: +86-10-6278-2195; fax: +8610-6277-3650.
E-mail address: hjm-den@mail.tsinghua.edu.cn (J. Hao).

1997, respectively. The new EU directive 1999/30/EC of


22 April 1999 also gave limit values for PM10. Since
1996, there have been amendatory National Ambient
Air Quality Standards (NAAQS) in China for TSP and
PM10, and the second class of NAAQS, which pertain to
urban areas, do not permit ambient PM10 concentrations to exceed 100 mg m 3 for an annual arithmetic
average and 150 mg m 3 for a 24-hour average.
Particulate matter pollution in those districts near
major roads was often found to be more severe than
urban background since these districts are affected
directly by various important primary sources, which
are frequently grouped into tailpipe exhaust from motor
vehicles, brake/tire wear, and resuspended road dust
(Lamoree and Turner, 1999). Resuspended road dust is
generally considered to be the most important source of
PM10, especially for the fraction of coarse mode

1352-2310/02/$ - see front matter r 2002 Elsevier Science Ltd. All rights reserved.
PII: S 1 3 5 2 - 2 3 1 0 ( 0 2 ) 0 0 4 6 7 - 3

4908

Y. Wu et al. / Atmospheric Environment 36 (2002) 49074918

(between 2.5 and 10 mm). Motor vehicle emissions,


however, usually constitute the signicant source of ne
and ultrane particles, such as PM2.5 and PM1. Therefore, it is necessary to quantify the particle emission
levels with different size fraction (PM10, PM2.5 and/or
PM1), and also to determine particle behavior after
emissions, as they are transported away from the road.
There have been several studies conducted on
behavior of mass concentrations and elemental composition of airborne particulate matter near the road.
Janssen et al. (1997) compared the mass concentration
and elemental composition of airborne particulate
matter at street and urban background locations in
Netherlands. PM10 and PM2.5 concentrations were
found to be only 1.3 times higher near the road
compared with the background sample, however, black
smoke (elemental carbon) concentrations were 2.6 times
higher. Furthermore, the levels of Si and Fe (abundant
species in road dust) were signicantly higher in PM10,
and to a lesser extent in PM2.5, which suggested that
reentrained road dust, and not vehicle tailpipe exhaust,
was the dominant source for PM10 and PM2.5 in vicinity
of major road. Another study examined street-level
concentrations of PM10, PM2.5 and NO2 in Hong Kong
was conducted by Lam et al.(1999). Although the
correlation between the PM10, PM2.5 and NO2 concentrations and annual average daily trafc volume is
relatively weak, a noticeable trend showing higher
concentrations for higher trafc volumes can be still
found.
Proles of mass concentrations of PM10, PM2.5, NO2,
black smoke and benzene at increasing distances
from a major motorway were conducted by RoordaKnape et al. (1998). Monitoring sites were set up
at approximately 50, 100, 150, and 300 m from a major
motorway at two different locations in the study.
It showed that black smoke and NO2 concentrations
declined with increased distance from the roadside,
however, no gradient was found for PM10, PM2.5
and benzene. A pilot study examined horizontal and
vertical proles of number concentrations of submicrometer particulates in relation to a busy road in
Brisbane, Australia (Morawska et al., 1999). It concluded that the horizontal prole measurements did not
provide any evidence of a statistically signicant
difference in ne particle number concentration with
respect to distance at ground level up to a distance of
200 m with the exception of measurements in close
proximity to the freeway (about 15 m). The vertical
prole measurements also revealed no signicant correlation between particle number concentration and
height. Further study conducted by Hitchins et al.
(2000) measured horizontal prole of concentrations of
ne and ultrane particles from vehicle emissions near a
major road in Brisbane. There was a clear decrease in
ne and ultrane particle number concentration (in the

range 0.0150.697 mm) as distance from the road


increased, as well as the larger particles measured
separately (in the range 0.520 mm). PM2.5 levels also
decreased with distance to around 75% for wind from
the road and to 65% for wind parallel to the road, at a
distance of 375 m in the study.
Macao, one of the Special Administrative Regions in
China (another is Hong Kong), is located in South
China. Macao has three main island components with a
total area of only 19 km2; however, its vehicle population has exceeded 110 thousand in 1999, which resulted
in one of the highest trafc densities in the world. Motor
vehicle emissions are considered to be the main source of
air pollutants in Macao since it is not directly inuenced
by industrial emissions (Hao et al., 2000).
Previous major studies at the Department of Environmental Science and Engineering (DESE) of Tsinghua
University (TU) focused on gaseous vehicle emissions
and determined their behavior as they are transported
away from the road in Macao. These studies presented
information on the real-world trafc activities, emission
inventory of motor vehicles and patterns of dispersion
and transportation of the exhaust air pollutants in
street canyon of Macao (He et al., 1998, 1999; Hao
et al., 2000).
As part of a program to assess emission characteristics
from motor vehicles in Macao, the purpose of this
research was to measure vertical and horizontal proles
of airborne coarse particles (PM10) and ne and
submicrometer particles (PM2.5 and PM1) near major
roads. Also, the study attempts to acquire particle size
distribution, including the contributions of PM2.5 and
PM1 to total PM10 mass, separately, at the roadway.
Due to funding and labor constrains, long-term
monitoring was not an option; instead, the daytime
period from 3 to 12 December in 2001 was chosen for
this monitoring.

2. Experimental techniques and procedures


Monitoring was conducted at four sites near major
roads in Macao. Site 1 at the junction of Avenida de
Horta e Costa Road and Rua de Francisco Xavier
Pereira Road was chosen for vertical prole measurement, site 2 near Avenida da Amizade Road for
horizontal prole measurement, and site 3 and site 4
for single point measurement, at the roadside of
Avenida da Amizade Road and Rua da Ribeira do
Patane Road, respectively. Totally 6 DustTrak monitors
with PM10, PM2.5 and PM1 inlets, respectively, were
used at all of four sites to provide an assessment of the
relationship between particle mass concentration and
vertical and horizontal distance in relation to major
roads. Also, a TEOM 1400a was used at sites 3 and 4 to
recalibrate the readings of the DustTrak, and to acquire

Y. Wu et al. / Atmospheric Environment 36 (2002) 49074918

the TEOM 1400a PM10 Monitor as an equivalent


method for the determination of PM10 concentrations
in ambient air (Designation no. EQPM-1090-079). The
TEOM 1400a monitor collected particles continuously
on a Teons-coated borosilicate glass ber lter
mounted on the tip of a glass element which oscillates
in an applied electric eld. The resonant frequency of the
element decreases as mass accumulations on the lter,
directly measuring inertial mass. Temperatures are
maintained at a constant value, typically 501C, in this
study, to minimize thermal expansion of the tapered
element. At the exit of the PM10 or PM2.5 inlet the
design 16.7 l min 1 ow is isokinetically split into a
3.0 l min 1 sample stream that is sent to the instruments
mass transducer and a 13.7 l min 1 exhaust stream.
Readings of mass concentrations were logged every
10 min and averaged over 1 h in this study.

the PM2.5 and PM1 contributions to PM10 near major


roads.
2.1. Instrumentation
2.1.1. DustTrak
The DustTrak Aerosol Monitor (model #8520, TSI
Inc., St. Paul, MN) is a rugged, portable instrument that
uses particulate light scattering to infer PM concentrations where the amount of scattered light is proportional
to the volume concentration of the aerosol. For particles
smaller than one-third the wavelength of the laser
(780 nm), the scattered light decreases as a function of
the sixth power of the diameter, thus limiting the
smallest detectable particles to approximately 0.1 mm.
The instrument is calibrated using Arizona Test Dust to
relate light scattering intensity to aerosol mass concentrations, and would need to be recalibrated at the
roadside in the study. Different size-selective impactors
are available for the inlet of the DustTrak allowing
measurements of PM10, PM2.5, and PM1. The ow rate
of the instrument is 1.7 l min 1.
DustTrak data can be logged at user-dened intervals
and gives an average reading of mass concentration over
the specied interval. For this study, readings were
logged every minute and averaged over 1 h. Totally
6 DustTraks were used in the study, and labeled as
D1D6, respectively.

2.2. Sites and procedures


Four sites were chosen for this monitoring study. All
of the sites were near major roads: (1) site 1, for vertical
prole measurement, is located at the junction of
Avenida de Horta e Costa Road and Rua de Francisco
Xavier Pereira Road; (2) site 2, for horizontal prole
measurement, is in the vicinity of Avenida da Amizade
Road; (3) site 3, for single point measurement, is located
at the roadside of Avenida da Amizade Road, which is
about 500 m east from site 2; (4) site 4, for single point
measurement also, is located at the roadside of Rua da
Ribeira do Patane Road. Schematic representations of
the four sites selected for measurements are shown in
Figs. 13, respectively.
Hourly meteorological data during the measurement
were obtained from the Macao Meteorological Service.
The meteorological station is located on Taipa Granda

2.1.2. Tapered element oscillating microbalance


(TEOM)
The concentrations of PM10 and PM2.5 were monitored continuously by a TEOM 1400a ambient particulate monitor (Rupprecht & Patashnick Co., Inc.,
Albany, NY) at sites 3 and 4 to recalibrate the readings
of DustTrak in this study. The US EPA has designated

79m

6 (D2)

Building
5 (D4)

59m

Up

4 (D3)

30m
19m
8m
2m

3 (D1)

Site 1
1 (D6)

4909

2 (D5)

Avenida de Horta e Costa Road

Fig. 1. Site 1 for vertical prole measurement.

Y. Wu et al. / Atmospheric Environment 36 (2002) 49074918

4910

Site 2

Building

Avenida da Amizade Road


1 (D1)

2m

2 (D2)

42m

3 (D6)

72m

4 (D4)

120m

5 (D3)

170m

6 (D5)

228m

Fig. 2. Site 2 for horizontal prole measurement.

Building

Site 3
2 (D3, D6, D2)

Avenida da Amizade Road


1 (D1, D5, D4, TEOM1400A)

Building

Site 4

Building
2 (D3, D6, D2)

Rua da Ribeira do Patane Road


1 (D1, D5, D4, TEOM1400A)

Building

Fig. 3. Sites 3 and 4 for single point measurement.

Mount, which is about 34 km south from the monitoring sites. Hourly data of wind speed, wind direction,
temperature, relative humidity and precipitation were
used for this work. Wind directions followed a similar
pattern during most of the sampling period (about 5
days), which were characterized by northerly wind.
However, about 3 days of sampling followed another
directions of southeasterly wind. The sampling roads
were chosen that the winds were perpendicular or nearly
perpendicular to them during most of the sampling
period.
The trafc ow was acquired by counting the number
of cars, light-duty trucks, heavy-duty vehicles (including
buses) and motorcycles for 30 min of each hour from
8:00 a.m. to 20:00 p.m. The average trafc ow per hour

during the measurements for all of the four sites were:


(1) Avenida de Horta e Costa Road: 795 cars, 453 lightduty vehicles, 237 heavy-duty vehicles, 1346 motorcycles, total vehicles 2831; (2) Rua de Francisco Xavier
Pereira Road: cars 365, light-duty vehicles 129, heavyduty vehicles 124, motorcycles 1108, total vehicles 1726;
(3) Avenida da Amizade Road: cars 1029, light-duty
vehicles 145, heavy-duty vehicles 107, motorcycles 352,
total vehicles 1633; (4) Rua da Ribeira do Patane Road:
cars 782, light-duty vehicles 251, heavy-duty vehicles
395, motorcycles 1856, total vehicles 3284.
Measurements at site 1 were taken at different heights:
2, 8, 19, 30, 59 and 79 m. Totally 6 DustTrak monitors
(labeled as D1D6, separately) with PM10, PM2.5 and
PM1 inlets, respectively, were used here during the
sampling period from 8:00 a.m. to 20:00 p.m. on 46
December 2001. Due to constrains of DustTrak
monitors, only one particle size fraction can be
measured each day, i.e., 4 December for PM10, 5
December for PM2.5 and 6 December for PM1,
respectively. Sampling tubes were extended vertically
from the window at least 0.5 m for each DustTrak.
Measurements at site 2 were made at distances of 2,
42, 72, 120, 170 and 228 m from the road. Because the
strongest decrease in concentration was expected to
occur in the rst 100150 m (Leu, 1992), four monitor
locations were situated within 150 m in the study. There
are two small roads crossing the monitoring site,
however, had a negligible amount of trafc (less than
10 vehicles per hour). Six DustTrak monitors were used
here during the sampling period from 8:00 a.m. to 20:00
p.m. on 46 December 2001. Again, each day only one
particle size fraction was measured, i.e., 10th of
December for PM1, 11th of December for PM10 and
the 12th of December for PM2.5, respectively. The
monitoring height of each tube was about 1.52.0 m
above the ground.
As mentioned above, different particle size fraction of
vertical and horizontal proles were measured on
different days due to constraint of DustTraks. It may
cause bias because the characteristics of particles may
be different during variant sampling days. However, as
the measurement were all conducted at workdays, the
pattern of hourly vehicle trafc ow is relatively steady,
which means the emission characterizations of local
sources on the same road, e.g., exhausted particulate
matter from vehicles, could be considered as relatively
steady at the same hour during different sampling days.
Therefore, we assumed that the particle characteristics
were relatively homogeneous on the same road during
the sampling days in the study.
Site 3 is located at the roadside, for single point
measurements. On each side of the site three DustTrak
monitors were installed with 10, 2.5 and 1 mm inlets,
respectively, during the daytime from 8:00 a.m. to 20:00
p.m. on 3 December. A TEOM 1400a was installed at

Y. Wu et al. / Atmospheric Environment 36 (2002) 49074918

4911

Table 1
Results of parallel measurement with 6 DustTrak monitors at the same site
DustTrak

PM10

PM2.5
a

D1
D3
D4
D5
D6

2b

Ratio

0.945
1.030
0.928
0.968
0.984

0.992
0.960
0.946
0.999
0.950

PM1

Ratio

14
6
6
8
6

0.953
0.977
0.918
0.924
0.973

0.997
0.989
0.994
0.989
0.996

Ratio

R2

8
8
8
8
8

0.972
0.972
0.896
0.943
0.994

0.999
1.000
1.000
1.000
1.000

5
8
8
6
8

Ratio=the averaged readings of other DustTraks divided by readings of D2.


R2 =correlation coefcient.
c
n=number of hourly averaged samples.
b

south of the road (Location 1, see Fig. 3) with PM10 and


PM2.5 inlets, separately, used to recalibrate the readings
of DustTrak monitors. Concentrations were measured
simultaneously with these monitors. The sampling
height of DustTraks and TEOM 1400a are about 2.5
and 3 m above the ground level, respectively. Site 4 is
also used for single point measurement, and the same
experimental procedures as those used in site 3 were
applied. Site 4 is located at the roadside of another
major road, and the monitoring period was from 8:00
a.m. to 19:00 p.m. on 7 December.
2.3. Quality assurance and quality control
Parallel measurements were conducted with these 6
DustTrak monitors at the same site with 10, 2.5 and
1 mm inlets, respectively, on 8 and 9 December. The
ratios of averaged readings of other DustTraks (D1,
D3D6) divided by the readings of D2 that was used as a
reference monitor and their linear correlation coefcients are summarized in Table 1. Excellent correlations
(0.951.00) were found for the readings of all of the
DustTraks. There were slight differences of averaged
readings between each other DustTrak and D2 with
10 mm inlets, as well as the 2.5 and 1 mm inlets, which was
probably due to the small shift in the cut-point of these
inlets or other systematic bias from the monitors. The
largest difference found was about 10% for D4 and D2
with 1 mm inlets. In the study, the hourly averaged
concentrations of each DustTrak monitor were normalized to eliminate the systematic bias.

3. Results and discussion


The measurements were conducted between 3 and 12
December 2001. The detailed sampling periods and
meteorological conditions are listed in Appendix A.

3.1. Vertical profiles at site 1


Fig. 4ac present the hourly vertical PM10, PM2.5
and PM1 concentration proles in daytime at the site 1,
respectively, and the vertical proles of the daytime
averaged particulate matter concentrations are summarized in Fig. 5. The concentrations of particulate
matter in Figs. 4 and 5 are measured by DustTraks,
and not recalibrated yet. Although the concentrations
by DustTraks are not real mass concentrations, the
vertical proles measured by DustTraks could be
considered as similar as those measured by other
monitors such as TEOM if we assume that particle
characteristics are relatively homogeneous on the same
road. In this section and followed section on horizontal
proles, the decreasing trends of particle concentrations
are of concern, instead of the detailed concentration
values.
It is clear that there is a signicant decrease in the
concentrations of PM10, PM2.5 and PM1, as the height
above the ground increases.
Those samples collected on 4 December show a strong
decreasing trend in concentrations of PM10 as the height
increases. At the height of 8 m (location 2), the daytime
averaged PM10 concentration decays to 74% of the
maximum occurring at 2 m above the ground (the closest
measurement point above the ground). However, as the
height increases, the attenuation of PM10 concentrations
slows down signicantly. At the height of 79 m (location
6), the concentration of PM10 decreases to about 60% of
the maximum. There is only 14% attenuation over the
measured height from 8 to 79 m. Wind direction
changed during the measuring period (see Appendix
A). It was characterized by northerly winds at about 201
(from the road towards the measuring site) prevailing in
the morning and changing direction to southeasterly
winds at about 1501 (nearly parallel to the road) at noon
and maintained this direction throughout the afternoon.
However, the result demonstrates that there is no

Y. Wu et al. / Atmospheric Environment 36 (2002) 49074918

PM2.5 (12/5/2001)
0.350

0.250

(a)

(b)

TIME

19:00

18:00

17:00

TIME

PM1 (12/6/2001)

0.400

1(D6)
2(D5)
3(D1)
4(D3)
5(D4)
6(D2)

0.350
0.300
CONC. (mgm-3)

16:00

8:00

19:00

18:00

17:00

16:00

15:00

14:00

13:00

12:00

0.000

11:00

0.000
9:00

0.050
10:00

0.100

13:00

0.100

12:00

0.200

0.150

11:00

0.300

0.200

9:00

CONC. (mgm-3)

0.400

8:00

CONC. (mgm-3)

0.500

1(D6)
2(D5)
3(D1)
4(D3)
5(D4)
6(D2)

0.300

15:00

1(D6)
2(D5)
3(D1)
4(D3)
5(D4)
6(D2)

0.600

14:00

PM10 (12/4/2001)

0.700

10:00

4912

0.250
0.200
0.150
0.100

(c)

19:00

18:00

17:00

16:00

15:00

14:00

13:00

12:00

11:00

10:00

9:00

0.000

8:00

0.050

TIME

Fig. 4. Site 1 hourly vertical PM concentration proles in daytime.


0.350
PM10 (12/4/2001)

CONC. (mg m-3)

0.300

PM2.5 (12/5/2001)
PM1 (12/6/2001)

0.250
0.200
0.150
0.100
0.050
0.000
0

10

20

30

40

50

60

70

80

90

100

Height above the ground (m)

Fig. 5. Site 1 vertical proles of the daytime averaged PM


concentrations.

statistically signicant difference between the vertical


proles in the morning and those in the afternoon (see
Fig. 4a).

Those samples collected on 5 December also show a


signicant decreasing trend of in concentrations of
PM2.5 as the height increases, although the attenuation
did not follow the same pattern as PM10. At the height
of 8 m, the daytime averaged PM2.5 concentration
decayed to only 87% of the maximum at the ground
level, not as strong a decrease as for PM10. However, the
concentrations of PM2.5 still decreased signicantly until
the height reached 19 m (location 3), where the
concentration decays to 73% of the maximum. Then,
the decrease of PM2.5 also slows down as the height
increases. At the height of 79 m, the concentration of
PM2.5 decays to 62% of the maximum.
The samples collected on 6 December exhibit a decay
of the PM1 concentrations that is less signicant than
the PM10 and PM2.5s as the height increases. At the
height of 8 m, the daytime averaged PM1 concentration
decays to about 86% of the maximum at the ground
level. The curve of PM1 (see Fig. 5) shows a dip at the
height of 19 m, where the concentration of PM1 decays
to 77% of the maximum. Then, the concentrations of

Y. Wu et al. / Atmospheric Environment 36 (2002) 49074918

PM1 increase slightly, as the height increases from 19 to


79 m. At the height of 79 m, the total decrease of PM1
concentration is about 20%. The reasons for the dip
have not been investigated, but more likely relate to
other source interference at those heights, such as
residential cooking.
The vertical proles of site 1 at the roadside suggest
that PM10, PM2.5 and PM1 concentrations are affected
signicantly by trafc sources at ground level, e.g.,
resuspended road dust for PM10, tailpipe exhaust from
motor vehicles for PM2.5 and PM1, etc., which resulted
in a signicant decrease in the concentration of PM10,
PM2.5 and PM1, as the height above the ground
increases. And, since the particles in the coarse
mode have the much higher settling velocity than those
ne and ultrane particles, attenuation of the concentrations of PM10 is more signicant than the PM2.5
and PM1 at a low height level, e.g., from the location 1
(2 m above the ground) to location 2 (8 m above the
ground).
Furthermore, site 1 is located at the junction of two
major roads, both of which are narrow roads with width
less than 15 m, surrounded by high buildings with height
more than 30 m at both sides of the roads, which
undoubtedly results in signicant street canyon. Special
ow circulation will be generated, and the wind
characteristics including wind speed and wind direction
are height-dependent in general (Hoydysh, 1988; Depaul, 1985). Therefore, the change of wind will
inevitably affect the trend of vertical prole of particle
concentrations. As the aspect ratio (building height to
street width) of site 1 is high, the ow at the bottom of
street canyon is more stable than upper part, which
makes air pollutant accumulate at the bottom (Fu et al.,
2000). However, due to lack of the meteorological
monitors, the wind characteristics in different height
were not measured, and detailed analysis of the inuence
of wind to particle concentrations is not available.
3.2. Horizontal profiles at site 2
Fig. 6ac present the hourly horizontal PM10, PM2.5
and PM1 concentration proles at the site 2, respectively, and the horizontal proles of the daytime
averaged particulate matter concentrations are summarized in Fig. 7. Similarly, the concentrations of particulate matter in Figs. 6 and 7 are measured by DustTraks,
and not recalibrated yet.
The samples collected on 10 December show a weak
trend of decrease in concentrations of PM1 as the
distance from the road increases. The measurement did
not begin until 14:00 p.m. because it rained in the early
morning (see Appendix A and Fig. 6c). At the distance
of 170 m (location 5), the daytime averaged PM1
concentration decays to only 90% of the maximum
occurring at 2 m from the road (the closest measurement

4913

point from the road), which is the maximum decrease in


concentrations of PM1 over the total measured distance.
The samples collected on 11 December shows that the
vertical prole of PM10 follows a similar pattern as
demonstrated by PM1. Over the total measured distance,
the maximum decrease of PM10 is only 7%, which
occurred at the distance of 228 m.
The samples collected on 12 December also show a
weak trend of decrease in concentrations of PM2.5 as
the distance from the road increases. The curve of PM2.5
(see Fig. 7) shows a slightly dip at the distance
of 72 m, where the daytime averaged concentration of
PM2.5 decays to 91% of the maximum occurring at 2 m
from the road. Wind direction changed during the
measurement period on this day (see Appendix A);
it was characterized by northerly winds at about 201
(from the road towards the measuring site) prevailing in
the morning and changing direction to southeasterly
winds at about 1251 (from the measuring site towards
the road) at noon and maintained this direction
throughout the afternoon. The total concentration of
PM2.5 from all of the 6 DustTraks decreased signicantly after the wind direction changed. And, the results
in the afternoon show that the concentrations of PM2.5
at other locations have no statistically signicant
difference except at location 1 (the closest point from
the road); the average concentration of PM2.5 at location
1 is about 12% higher than at other locations in the
afternoon.
The horizontal proles of site 2 at the roadside reveal
there is no signicant trend of decrease in concentrations
of PM10, PM2.5 and PM1 as the distance from the
road increases. The reasons maybe relate to (1) the
sampling heights, which is low above the ground (only
1.52.0 m) resulting in signicant interference from
wind-blown dust near the sampling locations since the
wind speed is high (more than 3 m s 1 in average) during
the sampling period; and (2) the relatively low vehicle
volume at site 2, which is less than 40% of total trafc
volume at site 1, resulting in relatively low particulate
matter emissions from vehicle exhaust and resuspended
road dust. The latter reason revealed that background
particulate matter, e.g., secondary particles and sea salt,
which are relatively steady as the distance from the road
increases, maybe a very important contributor to total
particle mass concentrations near road in Macao. The
ndings from this study can be compared with other
literature data on horizontal proles of particulate
matter near major road. For example, Roorda-Knape
et al (1998) found there was no clear decline for PM10
and PM2.5 concentrations at an increasing distance from
a major motorway; however, Hitchins et al. (2000)
concluded that PM2.5 levels decreased with distance to
around 75% when the wind blew from the road and to
65% for wind parallel to the road, at a distance of 375 m
in their study.

Y. Wu et al. / Atmospheric Environment 36 (2002) 49074918

4914

0.300

0.250

0.250

0.200

0.200

0.150

CONC. (mgm-3)

1(D1)
2(D2)
3(D6)
4(D4)
5(D3)
6(D5)

0.100
0.050

1(D1)
2(D2)
3(D6)
4(D4)
5(D3)
6(D5)

0.150
0.100
0.050

0.000

(a)

(b)

TIME

19:00

18:00

17:00

16:00

15:00

14:00

13:00

12:00

11:00

9:00

8:00

19:00

18:00

17:00

16:00

15:00

14:00

13:00

12:00

11:00

9:00

10:00

8:00

0.000

10:00

CONC. (mgm-3)

PM2.5 (12/12/2001)

PM 10 (12/11/2001)

0.300

TIME

PM1 (12/10/2001)
0.300

1(D1)
2(D2)
3(D6)
4(D4)
5(D3)
6(D5)

CONC. (mgm-3)

0.250
0.200
0.150
0.100
0.050

(c)

19:00

18:00

17:00

16:00

15:00

14:00

13:00

12:00

11:00

10:00

9:00

8:00

0.000

TIME

Fig. 6. Site 2 hourly horizontal PM concentration proles in daytime.

0.200

3.3. Single point measurements at sites 3 and 4

0.180

CONC. (mg m-3)

0.160
0.140
0.120
0.100
PM10 (12/11/2001)
PM25 (12/12/2001)
PM1 (12/10/2001)

0.080
0.060
0.040
0.020
0.000
0

50

100

150

200

250

Distance from the road (m)

Fig. 7. Site 2 horizontal proles of the daytime averaged PM


concentrations.

3.3.1. Particle size distribution near major roads


Table 2 lists the roadside particle size distribution at
sites 3 and 4. The sample arithmetic mean ratios of
PM2.5/PM10 by DustTraks at both sites are between 0.95
and 0.97, and the ratios of PM1/PM10 are also as high as
0.740.87. Since DustTrak is calibrated using Arizona
Test Dust to relate light scattering intensity to aerosol
mass concentrations, its readings were not real mass
concentrations near roads, and need to be recalibrated
by TEOM to acquire the real particle size distribution
and particle concentrations near roads in this study. The
comparisons of hourly PM10 and PM2.5 DustTrak
measurements to TEOM are illustrated in Fig. 8. Good

Y. Wu et al. / Atmospheric Environment 36 (2002) 49074918

4915

Table 2
Size distribution of particulate matter concentrations near major roads
Sampling sites

Site 3 (Avenida da Amizade Road)

Site 4 (Rua da Ribeira do Patane Road)

Location 1

Location 1

Location 2

Location 2

PM2:5 =PM10 PM1 =PM10 PM2:5 =PM10 PM1 =PM10 PM2:5 =PM10 PM1 =PM10 PM2:5 =PM10 PM1 =PM10
Arithmetic mean R% a
0.952
Recalibrated mean R% r b 0.656
Standard deviation sr
0.009
Number of samples n 11

0.833
0.575c
0.013
11

0.970
0.669
0.011
10

0.796
0.549c
0.011
12

0.965
0.665
0.053
9

0.866
0.597c
0.014
10

NAd
NAd
NAd
NAd

0.738
0.509c
0.049
10

%
R=size
fraction by DustTraks only, not recalibrated by TEOM yet.
R% r =readings of DustTraks were recalibrated by TEOM (see Fig. 8).
c
Assumes that PM1 could be recalibrated the same ratio as PM2.5 (0.0029, see Fig. 8b).
d
NA=not available because of the power malfunction of D6.
a

PM10
DUSTTRAK CONC. (mg m-3)

0.250

Avenida da Amizade Road (site 3)


0.200
0.150

y = 0.002x
R2 = 0.8182

0.100
0.050
0.000
0.0

20.0

40.0

60.0

80.0

100.0

TEOM CONC. (ug m-3)

(a)

DUSTTRAK CONC. (mg m-3)

PM2.5
0.350
0.300

Avenida da Amizade Road (site 3)

0.250
0.200

y = 0.0029x
R2 = 0.9114

0.150
0.100
0.050
0.000
0.0

(b)

Ruada Ribeira do Patane Road (site 4)

20.0

40.0
60.0
80.0
TEOM CONC. (ug m-3)

100.0

Fig. 8. Comparison of hourly PM DustTrak measurements to


TEOM.

correlations were found for the readings of DustTrak


monitors and TEOM. It is seen that the slope of the
linear regression is 0.002 and the correlation coefcient
is 0.82 for PM10; and for PM2.5, the slope is 0.0029 with
a correlation coefcient of 0.91. Then, the sample
arithmetic mean ratios of PM2.5/PM10 at both sites

decrease to be between 0.66 and 0.67 after the readings


of PM2.5 and PM10 by DustTrak were recalibrated by
TEOM. If we assume that PM1 could be recalibrated the
same ratio as PM2.5 (0.0029, see Fig. 8b), the sample
arithmetic mean ratios of PM1/PM10 are between 0.51
and 0.60. Because the sample chamber and inlet air are
heated to 501C to measurement in the TEOM system, it
undoubtedly aggravates the particle volatilization bias
for ammonium nitrate and organic compounds, most of
which are ne particles. The ratios of PM2.5/PM10 and
PM1/PM10 will be higher if the volatilization bias
(negative sampling artifact) of TEOM is considered. It
suggests that ne particles and submicrometer particles
contributed major part of PM10 concentrations at
roadside in Macao. The high ratios of ne and
submicrometer particles in total PM10 mass is most
likely attributed to the contribution of local sources
including vehicle tailpipe exhaust and resuspended ne
dust, and, the secondary particles (sulfate, nitrate and
ammonium) of regional scales may be important
contributors to ne particles near roads in Macao too.
3.3.2. Particle concentrations near major roads
Results of the daytime averaged concentrations of
PM10, PM2.5 and PM1 by DustTraks (not recalibrated
by TEOM yet) at sites 3 and 4 are shown in Table 3. The
mean concentrations of PM10, PM2.5 and PM1 at
location 2 are all statistically signicantly lower than
those at location 1 at site 3, but the differences are small
(less than or equal to 10%). The mean concentration of
PM10 at location 2 is statistically signicantly higher
than that at location 1 at site 4, however, the statistically
signicant difference of PM1 between these two locations is not found. Since all of the locations are close to
the road, where are signicantly inuenced by the
sources, e.g., reentrained road dust and vehicle exhausts,
the differences of particle concentrations between
location 1 and location 2 of the roads may be weakened.
Moreover, both site 3 and site 4 are narrow roads (less
than 15 m of road width) surrounded by buildings with

Y. Wu et al. / Atmospheric Environment 36 (2002) 49074918

4916

windward side, which revealed that the effect of street


canyon exactly occurred during the sampling period.
The concentrations of particulate matter in Table 3
are the readings by DustTraks, which are not recalibrated yet. The real mass concentrations will decrease
signicantly after the DustTrak readings are recalibrated
by TEOM (see Fig. 8). The recalibrated daytime

height more than 20 m at both roadsides, which


undoubtedly results in remarkable street canyon. Special
ow circulation will be generated, and result in higher
air pollutant concentrations at leeward side than windward side (Hoydysh, 1988; Depaul, 1985). The arithmetic mean concentrations of PM10, PM2.5 and PM1 at
leeward side of sites 3 and 4 are all higher than those at
Table 3
Daytime averaged particle concentrations near major roads
Sampling sites

Site 3 (Avenida da Amizade Road)

Site 4 (Rua da Ribeira do Patane Road)

Location 1

Location 1

Location 2

Location 2

3 a

PM10 (mg m )
sb/nc

0.116
0.017/11

0.109
0.015/11

0.204
0.047/9

0.258nn
0.045/9

PM2.5 (mg m 3)a


sb/nc

0.111
0.015/11

0.106nn
0.014/11

0.193
0.050/10

NAd
NAd

PM1 (mg m 3)a


sb/nc

0.097
0.013/11

0.086n
0.012/11

0.186
0.049/10

0.195nnn
0.025/10

Arithmetic mean concentration by DustTrak, not recalibrated by TEOM.


s=the standard deviation.
c
n=number of samples.
d
NA=not available because of the power malfunction of D6.
n
Statistically signicant difference compared with location 1 (paired t-test; po0:01).
nn
Statistically signicant difference compared with location 1 (paired t-test; po0:05).
nnn
No statistically signicant difference compared with location 1 (paired t-test; po0:05).

0.600

Ruada Ribeira do Patane Road (site 4)

Ruada Ribeira do Patane Road (site 4)


CONC. (mg m-3)

0.500

Avenida da Amizade Road (site 3)


y = 5E-05x + 0.0388
R2 = 0.6066

Avenida da Amizade Road (site 3)

0.400
y = 6E-05x + 0.0072
R2 = 0.6055

0.300
0.200
0.100
0.000

(a)

PM 2.5

PM 10

0.450
0.400
0.350
0.300
0.250
0.200
0.150
0.100
0.050
0.000

1000

2000

3000

4000

5000

1000

(b)

Hourly traffic flow

2000

3000

Hourly traffic flow

PM 1
0.450

Ruada Ribeira do Patane Road (site 4)

0.400

CONC. (mg m-3)

CONC. (mg m-3)

Avenida da Amizade Road (site 3)

0.350
0.300

y = 5E-05x + 0.0146
R2 = 0.6695

0.250
0.200
0.150
0.100
0.050
0.000
0

(c)

1000

2000
3000
4000
Hourly traffic flow

5000

Fig. 9. Correlations of particle concentrations and hourly trafc ow in daytime.

4000

5000

Y. Wu et al. / Atmospheric Environment 36 (2002) 49074918

averaged mass concentrations of PM10 and PM2.5 at site


3 are 54.558.0 and 36.638.8 mg m 3, respectively. At
site 4, the real mass concentrations of PM10 and PM2.5
are 102.0129.0 and 66.6 mg m 3, respectively. The
particle concentrations at site 4 are much higher than
those at site 3, which is most likely attributed to
the much higher trafc volume at site 4. As mentioned
above, the real mass concentrations of particulate
matter in the study may be underestimated, due to
the thermal loss of volatile material in the TEOM
system.
3.3.3. Relation to vehicular traffic
Since both sites 3 and 4 were located at the roadside,
the local trafc conditions would affect directly the
measured concentration levels of particulate matter. The
correlations of hourly particle concentrations and
hourly trafc ow in daytime at sites 3 and 4 are
presented in Fig. 9ac for PM10, PM2.5 and PM1,
respectively. The obtained correlation coefcients are
equal to 0.61, 0.61 and 0.67, respectively. The results

4917

reveal that correlations between the particulate matter


and the trafc volumes are signicant, showing a clear
trend of higher concentrations for higher trafc
volumes.

4. Summary and conclusions


Vertical and horizontal proles of airborne particulate
matter in daytime were measured near major roads. It is
clear that there is a signicant decrease in the
concentrations of PM10, PM2.5 and PM1, as the height
above the ground increases from 2 to 79 m at site 1. At
the height of 79 m, the concentrations of PM10, PM2.5
and PM1, decrease to about 60%, 62% and 80% of the
maximum occurring at 2 m above the ground, respectively. The vertical proles at the roadside suggest that
particle concentrations are affected signicantly by those
sources at ground level from trafc district, e.g.,
resuspended road dust and tailpipe exhaust from motor
vehicles.

Table 4
Sampling periods and meteorological conditions used in the study
Sampling site

Date

WS (m s 1)a

WDb

P (mm)c

RH (%)d

Site 1 (PM10)

12/4/2001

2.9 (1.73.9)

61 (4879)

Site 1 (PM2.5)

12/5/2001

4.1 (2.85.4)

69 (6474)

Site 1 (PM1)

12/6/2001

6.9 (5.77.9)

64 (6071)

Site 2 (PM10)

12/11/2001

4.3 (3.85.9)

79 (7781)

Site 2 (PM2.5)

12/12/2001

2.9 (1.45.6)

72 (6281)

Site 2 (PM1)

12/10/2001

7.9 (6.99.2)

08:0013:00: Northerly wind at about


201 (from the road towards the
measuring site)
13:0020:00: Southeasterly wind at
about 1501 (nearly parallel to the road)
Southeasterly wind at about 1301 (nearly
parallel to the road)
Northerly wind at about 101 (from the
road towards the measuring site)
Northerly wind at about 201 (from the
road towards the measuring site)
08:0013:00: Northerly wind at about
201 (from the road towards the
measuring site)
13:0020:00: Southeasterly wind at
about 1251 (from the measuring site
towards the road)
Northerly wind at about 201 (from the
road towards the measuring site)

1.6 (08:00)

81 (7590)

Site 3

12/3/2001

3.0 (2.04.1)

0.2 (11:00)
0

72 (6479)

Site 4

12/7/2001

5.2 (3.18.5)

61 (5371)

08:0017:00: Northeasterly and easterly


winds at about 45901 (nearly parallel to
the road)
17:0020:00: Southeasterly wind at
about 1251 (from location 1 towards
location 2)
Northerly wind at about 251 (from
location 2 towards location 1)

WS=wind speed; arithmetic mean (minimummaximum).


WD=wind direction.
c
P=precipitation.
d
RH=relative humidity; arithmetic mean (minimummaximum).
b

4918

Y. Wu et al. / Atmospheric Environment 36 (2002) 49074918

The horizontal proles of site 2 at the roadside reveal


there is no signicant decreasing trend in concentrations
of particulate matter as the distance from the road
increases. Over the total measured distance, the maximum decrease of PM10, PM2.5 and PM1 are only 7%,
9% and 10%, of the maximum values occurring at 2 m
from the road, respectively. The reasons may be related
to low sampling heights, resulting in interference from
other ground-level sources near the sampling locations,
and the relatively low vehicle volume at site 2.
Also, the particle size distribution at the roadside was
acquired in this study. The daytime averaged PM2.5 and
PM1 contributed 6667% and 5160%, respectively, of
the total PM10 mass after the particle readings by
DustTrak were recalibrated by TEOM at both sites 3
and 4 (we assume that PM1 could be recalibrated using
the same ratio as PM2.5). It suggested that ne particles
and submicrometer particles contributed the major part
of PM10 at the roadside in Macao, which may be
attributed to the combinations of sources including
exhaust particulate matter from vehicles and reentrained
ne dust, and secondary particles (sulfate, nitrate and
ammonium) of regional scales.

Acknowledgements
The research described in this paper is funded by the
National Natural Science Foundation of China &
Macao Foundation (Grant No. 40045015). The authors
thank Jingnan Hu and Litao Wang (DESE, TU) for
their contribution to the collection of the samples, and
Mr. Freed, C.N. of US EPA for his helpful advice to
improve our paper.

Appendix A
The detailed sampling periods and meteorological
conditions are listed in Table 4.

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