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  • Atmospheric Environment 36 (2002) 49074918

    Vertical and horizontal proles of airborne particulate matternear major roads in Macao, China

    Ye Wua, Jiming Haoa,*, Lixin Fua, Zhishi Wangb, Uwa Tangb

    aDepartment of Environmental Science and Engineering, Tsinghua University, Beijing 100084, Peoples Republic of ChinabFaculty 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 79m, was found. At the height of 79m, the concentrations of

    PM10, PM2.5 and PM1, decrease to about 60%, 62% and 80% of the maximum occurring at 2m 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 (0228m), the maximum decreases of PM10, PM2.5 and PM1 are only 7%, 9% and 10%, of the maximum

    occurring at 2m 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 organiza-

    tions issued air quality standards for airborne particu-

    late matter to protect public health. PM10 and PM2.5were introduced as a standard in the US in 1987 and

    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 concentra-

    tions to exceed 100mgm3 for an annual arithmeticaverage and 150 mgm3 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

    *Corresponding author. Tel.: +86-10-6278-2195; fax: +86-

    10-6277-3650.

    E-mail address: [email protected] (J. Hao).

    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

  • (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. There-

    fore, 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 compo-

    sition 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 concen-

    trations 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 Roorda-

    Knape et al. (1998). Monitoring sites were set up

    at approximately 50, 100, 150, and 300m 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, PM2.5and benzene. A pilot study examined horizontal and

    vertical proles of number concentrations of submic-

    rometer particulates in relation to a busy road in

    Brisbane, Australia (Morawska et al., 1999). It con-

    cluded 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

    200m with the exception of measurements in close

    proximity to the freeway (about 15m). The vertical

    prole measurements also revealed no signicant corre-

    lation 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 roadincreased, as well as the larger particles measured

    separately (in the range 0.520mm). PM2.5 levels alsodecreased with distance to around 75% for wind from

    the road and to 65% for wind parallel to the road, at a

    distance of 375m 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 popula-

    tion 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 Envir-

    onmental 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 measure-

    ment, 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) 490749184908

  • 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 concentra-

    tions 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 concen-

    trations, 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 lmin1.

    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.

    2.1.2. Tapered element oscillating microbalance

    (TEOM)

    The concentrations of PM10 and PM2.5 were mon-

    itored continuously by a TEOM 1400a ambient parti-

    culate 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

    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 thisstudy, to minimize thermal expansion of the tapered

    element. At the exit of the PM10 or PM2.5 inlet the

    design 16.7 lmin1 ow is isokinetically split into a

    3.0 lmin1 sample stream that is sent to the instruments

    mass transducer and a 13.7 lmin1 exhaust stream.

    Readings of mass concentrations were logged every

    10min and averaged over 1 h in this study.

    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 500m 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

    Avenida de Horta e Costa Road

    Building

    Up

    1 (D6) 2 (D5)

    3 (D1)4 (D3)

    5 (D4)

    6 (D2)

    Site 12m8m

    19m

    30m

    59m

    79m

    N

    Fig. 1. Site 1 for vertical prole measurement.

    Y. Wu et al. / Atmospheric Environment 36 (2002) 49074918 4909

  • Mount, which is about 34 km south from the monitor-

    ing 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 30min 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 light-

    duty vehicles, 237 heavy-duty vehicles, 1346 motor-

    cycles, total vehicles 2831; (2) Rua de Francisco Xavier

    Pereira Road: cars 365, light-duty vehicles 129, heavy-

    duty 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 79m. 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 0.5m for each DustTrak.

    Measurements at site 2 were made at distances of 2,

    42, 72, 120, 170 and 228m from the road. Because the

    strongest decrease in concentration was expected to

    occur in the rst 100150m (Leu, 1992), four monitor

    locations were situated within 150m 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 1.52.0m

    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

    Avenida da Amizade Road

    N Site 2 Building

    2m

    42m

    72m

    120m

    170m

    228m

    1 (D1)

    2 (D2)

    4 (D4)

    3 (D6)

    6 (D5)

    5 (D3)

    Fig. 2. Site 2 for horizontal prole measurement.

    Rua da Ribeira do Patane Road

    N

    Site 4 Building2 (D3, D6, D2)

    Building

    1 (D1, D5, D4, TEOM1400A)

    Avenida da Amizade Road

    N

    Site 3 Building

    1 (D1, D5, D4, TEOM1400A)

    2 (D3, D6, D2)

    Building

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

    Y. Wu et al. / Atmospheric Environment 36 (2002) 490749184910

  • 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 3m 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

    1mm inlets, respectively, on 8 and 9 December. Theratios 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 coef-

    cients 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

    10mm inlets, as well as the 2.5 and 1mm inlets, which wasprobably 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 averagedconcentrations of each DustTrak monitor were normal-

    ized 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, PM2.5and PM1 concentration proles in daytime at the site 1,

    respectively, and the vertical proles of the daytime

    averaged particulate matter concentrations are summar-

    ized 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 8m (location 2), the daytime

    averaged PM10 concentration decays to 74% of the

    maximum occurring at 2m 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 79m (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 79m. 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 noonand maintained this direction throughout the afternoon.

    However, the result demonstrates that there is no

    Table 1

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

    DustTrak PM10 PM2.5 PM1

    Ratioa R2b nc Ratio R2 n Ratio R2 n

    D1 0.945 0.992 14 0.953 0.997 8 0.972 0.999 5

    D3 1.030 0.960 6 0.977 0.989 8 0.972 1.000 8

    D4 0.928 0.946 6 0.918 0.994 8 0.896 1.000 8

    D5 0.968 0.999 8 0.924 0.989 8 0.943 1.000 6

    D6 0.984 0.950 6 0.973 0.996 8 0.994 1.000 8

    aRatio=the averaged readings of other DustTraks divided by readings of D2.bR2=correlation coefcient.cn=number of hourly averaged samples.

    Y. Wu et al. / Atmospheric Environment 36 (2002) 49074918 4911

  • 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 8m, 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 19m (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 79m, 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 8m, 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 19m, where the concentration of PM1 decays

    to 77% of the maximum. Then, the concentrations of

    PM10 (12/4/2001)

    0.000

    0.100

    0.200

    0.300

    0.400

    0.500

    0.600

    0.700

    8:00

    9:00

    10:0

    011

    :00

    12:0

    013

    :00

    14:0

    015

    :00

    16:0

    017

    :00

    18:0

    019

    :00

    TIME

    CON

    C. (m

    gm-3 )

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

    PM2.5 (12/5/2001)

    0.000

    0.050

    0.100

    0.150

    0.200

    0.250

    0.300

    0.350

    8:00

    9:00

    10:0

    011

    :00

    12:0

    013

    :00

    14:0

    015

    :00

    16:0

    017

    :00

    18:0

    019

    :00

    TIME

    CON

    C. (m

    gm-3 )

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

    PM1 (12/6/2001)

    0.000

    0.050

    0.100

    0.150

    0.200

    0.250

    0.300

    0.350

    0.400

    8:00

    9:00

    10:0

    011

    :00

    12:0

    013

    :00

    14:0

    015

    :00

    16:0

    017

    :00

    18:0

    019

    :00

    TIME

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

    CON

    C. (m

    gm-3 )

    (a) (b)

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

    0.000

    0.050

    0.100

    0.150

    0.200

    0.250

    0.300

    0.350

    0 10 2 0 30 4 0 50 60 7 0 80 9 0 100Height above the ground (m)

    CON

    C. (m

    g m-3 )

    PM10 (12/4/2001)PM2.5 (12/5/2001)PM1 (12/6/2001)

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

    concentrations.

    Y. Wu et al. / Atmospheric Environment 36 (2002) 490749184912

  • PM1 increase slightly, as the height increases from 19 to

    79m. At the height of 79m, the total decrease of PM1concentration 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 concen-

    trations of PM10 is more signicant than the PM2.5and PM1 at a low height level, e.g., from the location 1

    (2m above the ground) to location 2 (8m 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 15m, surrounded by high buildings with height

    more than 30m 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; De-

    paul, 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, PM2.5and PM1 concentration proles at the site 2, respec-

    tively, and the horizontal proles of the daytime

    averaged particulate matter concentrations are summar-

    ized in Fig. 7. Similarly, the concentrations of particu-

    late 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 170m (location 5), the daytime averaged PM1concentration decays to only 90% of the maximum

    occurring at 2m from the road (the closest measurement

    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 228m.

    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 72m, where the daytime averaged concentration of

    PM2.5 decays to 91% of the maximum occurring at 2m

    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 towardsthe road) at noon and maintained this direction

    throughout the afternoon. The total concentration of

    PM2.5 from all of the 6 DustTraks decreased signi-

    cantly after the wind direction changed. And, the results

    in the afternoon show that the concentrations of PM2.5at 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

    1.52.0m) resulting in signicant interference from

    wind-blown dust near the sampling locations since the

    wind speed is high (more than 3m s1 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 PM10and 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 375m

    in their study.

    Y. Wu et al. / Atmospheric Environment 36 (2002) 49074918 4913

  • 3.3. Single point measurements at sites 3 and 4

    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

    PM10 (12/11/2001)

    0.000

    0.050

    0.100

    0.150

    0.200

    0.250

    0.300

    8:00

    9:00

    10:0

    011

    :00

    12:0

    013

    :00

    14:0

    015

    :00

    16:0

    017

    :00

    18:0

    019

    :00

    TIME

    CON

    C. (m

    gm-3 )

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

    PM2.5 (12/12/2001)

    0.000

    0.050

    0.100

    0.150

    0.200

    0.250

    0.300

    8:00

    9:00

    10:0

    011

    :00

    12:0

    013

    :00

    14:0

    015

    :00

    16:0

    017

    :00

    18:0

    019

    :00

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

    PM1 (12/10/2001)

    0.000

    0.050

    0.100

    0.150

    0.200

    0.250

    0.300

    8:00

    9:00

    10:0

    011

    :00

    12:0

    013

    :00

    14:0

    015

    :00

    16:0

    017

    :00

    18:0

    019

    :00

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

    TIME

    CON

    C. (m

    gm-3 )

    TIME

    CON

    C. (m

    gm-3 )

    (a) (b)

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

    0.0000.0200.040

    0.0600.0800.1000.1200.140

    0.1600.1800.200

    0 50 100 150 200 250Distance from the road (m)

    CON

    C. (m

    g m-3 )

    PM10 (12/11/2001)PM25 (12/12/2001)PM1 (12/10/2001)

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

    concentrations.

    Y. Wu et al. / Atmospheric Environment 36 (2002) 490749184914

  • 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, itundoubtedly 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 loca-

    tions 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 15m of road width) surrounded by buildings with

    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 2 Location 1 Location 2

    PM2:5=PM10 PM1=PM10 PM2:5=PM10 PM1=PM10 PM2:5=PM10 PM1=PM10 PM2:5=PM10 PM1=PM10

    Arithmetic mean %Ra 0.952 0.833 0.970 0.796 0.965 0.866 NAd 0.738

    Recalibrated mean %Rrb 0.656 0.575c 0.669 0.549c 0.665 0.597c NAd 0.509c

    Standard deviation sr 0.009 0.013 0.011 0.011 0.053 0.014 NAd 0.049

    Number of samples n 11 11 10 12 9 10 NAd 10

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

    y = 0.002xR2 = 0.8182

    0.000

    0.050

    0.100

    0.150

    0.200

    0.250

    0.0 20.0 40.0 60.0 80.0 100.0TEOM CONC. (ug m-3)

    DU

    STTR

    AK

    CO

    NC.

    (mg m

    -3 ) Avenida da Amizade Road (site 3)

    PM10

    y = 0.0029xR2 = 0.9114

    0.000

    0.050

    0.100

    0.150

    0.200

    0.250

    0.300

    0.350

    0.0 20.0 40.0 60.0 80.0 100.0

    DU

    STTR

    AK

    CO

    NC.

    (mg m

    -3 )

    Ruada Ribeira do Patane Road (site 4) Avenida da Amizade Road (site 3)

    PM2.5

    TEOM CONC. (ug m-3)

    (a)

    (b)Fig. 8. Comparison of hourly PM DustTrak measurements to

    TEOM.

    Y. Wu et al. / Atmospheric Environment 36 (2002) 49074918 4915

  • height more than 20m 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 wind-

    ward side (Hoydysh, 1988; Depaul, 1985). The arith-

    metic mean concentrations of PM10, PM2.5 and PM1 at

    leeward side of sites 3 and 4 are all higher than those at

    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 recali-

    brated yet. The real mass concentrations will decrease

    signicantly after the DustTrak readings are recalibrated

    by TEOM (see Fig. 8). The recalibrated daytime

    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 2 Location 1 Location 2

    PM10 (mgm3)a 0.116 0.109n 0.204 0.258nn

    sb/nc 0.017/11 0.015/11 0.047/9 0.045/9

    PM2.5 (mgm3)a 0.111 0.106nn 0.193 NAd

    sb/nc 0.015/11 0.014/11 0.050/10 NAd

    PM1 (mgm3)a 0.097 0.086n 0.186 0.195nnn

    sb/nc 0.013/11 0.012/11 0.049/10 0.025/10

    aArithmetic mean concentration by DustTrak, not recalibrated by TEOM.bs=the standard deviation.cn=number of samples.dNA=not available because of the power malfunction of D6.nStatistically signicant difference compared with location 1 (paired t-test; po0:01).nnStatistically signicant difference compared with location 1 (paired t-test; po0:05).nnnNo statistically signicant difference compared with location 1 (paired t-test; po0:05).

    PM10

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

    0.0000.0500.1000.1500.2000.2500.3000.3500.4000.450

    0 1000 2000 3000 4000 5000Hourly traffic flow

    CON

    C. (m

    g m-

    3 )

    Ruada Ribeira do Patane Road (site 4) Avenida da Amizade Road (site 3)

    PM2.5

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

    0.000

    0.100

    0.200

    0.300

    0.400

    0.500

    0.600

    0 1000 2000 3000 4000 5000

    Ruada Ribeira do Patane Road (site 4) Avenida da Amizade Road (site 3)

    PM1

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

    0.0000.0500.1000.1500.2000.2500.3000.3500.4000.450

    0 1000 2000 3000 4000 5000

    Ruada Ribeira do Patane Road (site 4) Avenida da Amizade Road (site 3)

    Hourly traffic flow

    CON

    C. (m

    g m-

    3 )

    CON

    C. (m

    g m-

    3 )

    Hourly traffic flow

    (a) (b)

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

    Y. Wu et al. / Atmospheric Environment 36 (2002) 490749184916

  • averaged mass concentrations of PM10 and PM2.5 at site

    3 are 54.558.0 and 36.638.8 mgm3, respectively. Atsite 4, the real mass concentrations of PM10 and PM2.5are 102.0129.0 and 66.6 mgm3, respectively. Theparticle 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

    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 79m at site 1. At

    the height of 79m, the concentrations of PM10, PM2.5and PM1, decrease to about 60%, 62% and 80% of the

    maximum occurring at 2m above the ground, respec-

    tively. 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 s1)a WDb P (mm)c RH (%)d

    Site 1 (PM10) 12/4/2001 2.9 (1.73.9) 08:0013:00: Northerly wind at about

    201 (from the road towards themeasuring site)

    0 61 (4879)

    13:0020:00: Southeasterly wind at

    about 1501 (nearly parallel to the road)Site 1 (PM2.5) 12/5/2001 4.1 (2.85.4) Southeasterly wind at about 1301 (nearly

    parallel to the road)

    0 69 (6474)

    Site 1 (PM1) 12/6/2001 6.9 (5.77.9) Northerly wind at about 101 (from theroad towards the measuring site)

    0 64 (6071)

    Site 2 (PM10) 12/11/2001 4.3 (3.85.9) Northerly wind at about 201 (from theroad towards the measuring site)

    0 79 (7781)

    Site 2 (PM2.5) 12/12/2001 2.9 (1.45.6) 08:0013:00: Northerly wind at about

    201 (from the road towards themeasuring site)

    0 72 (6281)

    13:0020:00: Southeasterly wind at

    about 1251 (from the measuring sitetowards the road)

    Site 2 (PM1) 12/10/2001 7.9 (6.99.2) Northerly wind at about 201 (from theroad towards the measuring site)

    1.6 (08:00) 81 (7590)

    0.2 (11:00)

    Site 3 12/3/2001 3.0 (2.04.1) 08:0017:00: Northeasterly and easterly

    winds at about 45901 (nearly parallel tothe road)

    0 72 (6479)

    17:0020:00: Southeasterly wind at

    about 1251 (from location 1 towardslocation 2)

    Site 4 12/7/2001 5.2 (3.18.5) Northerly wind at about 251 (fromlocation 2 towards location 1)

    0 61 (5371)

    aWS=wind speed; arithmetic mean (minimummaximum).bWD=wind direction.cP=precipitation.dRH=relative humidity; arithmetic mean (minimummaximum).

    Y. Wu et al. / Atmospheric Environment 36 (2002) 49074918 4917

  • 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 max-

    imum decrease of PM10, PM2.5 and PM1 are only 7%,

    9% and 10%, of the maximum values occurring at 2m

    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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    Y. Wu et al. / Atmospheric Environment 36 (2002) 490749184918

    Vertical and horizontal profiles of airborne particulate matter near major roads in Macao, ChinaIntroductionExperimental techniques and proceduresInstrumentationDustTrakTapered element oscillating microbalance (TEOM)

    Sites and proceduresQuality assurance and quality control

    Results and discussionVertical profiles at site 1Horizontal profiles at site 2Single point measurements at sites 3 and 4Particle size distribution near major roadsParticle concentrations near major roadsRelation to vehicular traffic

    Summary and conclusionsAcknowledgementsReferences