Science of the Total Environment 338 (2005) 267 – 281

www.elsevier.com/locate/scitotenv

PM2.5 chemical composition in Hong Kong:

urban and regional variationsB
Peter K.K. Louiea,*, Judith C. Chowb, L.-W. Antony Chenb, John G. Watsonb,
Gordon Leunga, Della W.M. Sinc
a
Environmental Protection Department, 33/F, Revenue Tower, 5 Gloucester Rd., Wanchai, Hong Kong Special Administrative
Region of the People’s Republic of China
b
Desert Research Institute, 2215 Raggio Parkway, Reno, NV 89512, USA
c
Government Laboratory, 7/F, Homantin Government Offices, 88 Chung Hau St., Homantin, Hong Kong Special Administrative
Region of the People’s Republic of China
Received 19 February 2004; accepted 7 July 2004

Abstract

Chemically speciated PM2.5 measurements were made at roadside, urban, and rural background sites in Hong Kong for 1
year during 2000/2001 to determine the spatial and temporal variations of PM2.5 mass and chemical composition in this highly
populated region. Annual average PM2.5 concentrations at the urban and rural sites were 34.1 and 23.7 Ag m 3, respectively,
~50–100% higher than the United States’ annual average National Ambient Air Quality Standard (NAAQS) of 15 Ag m 3.
Daily PM2.5 concentrations exceeded the U.S. 24-h NAAQS of 65 Ag m 3 on 19 days, reaching 131F8 Ag m 3 at the roadside
site on 02/28/2001. Carbonaceous aerosol is the largest contributor to PM2.5 mass (explaining 52–75% of PM2.5 mass at the two
urban sites and 32% at the background site), followed by ammonium sulfate (ranging from 23% to 37% at the two urban sites
and 51% at the background site). Ammonium sulfate and crustal concentrations showed more uniform spatial distributions,
while the largest urban—rural contrasts found in carbonaceous aerosol (likely due to emissions from on-road gasoline and
diesel vehicles). Marine influences accounted for 7% of the mass at the background site (more than twice as much as at the two
urban sites). Ternary diagrams are utilized to illustrate the different spatial patterns.
D 2004 Elsevier B.V. All rights reserved.

Keywords: PM2.5; Spatial distribution; Carbonaceous aerosol

B
The content of this paper does not necessarily reflect the views and policies of the Government of the Hong Kong Special Administrative
Region (HKSAR), nor does mention of trade names or commercial products constitute an endorsement or recommendation of their use.
* Corresponding author. Tel.: +852 2594 6426; fax: +852 2827 8040.
E-mail address: plouie@epd.gov.hk (P.K.K. Louie).

0048-9697/$ - see front matter D 2004 Elsevier B.V. All rights reserved.
doi:10.1016/j.scitotenv.2004.07.021
268 P.K.K. Louie et al. / Science of the Total Environment 338 (2005) 267–281
1. Introduction
Concerns have grown through recent decades
regarding health and environmental effects attribut-
able to fine particulate matter (PM) (Vedal, 1997;
National Research Council, 1998, 1999, 2001). Air-
borne fine particles lead to smog and haze formation
that reduces visibility (Watson, 2002a,b; Chow et al.,
2002a). Epidemiological studies have shown statisti-
cal associations between short-term increase in
ambient aerosol concentration and daily mortality/
morbidity (Dockery et al., 1993; Pope et al., 1995).
Recent emission inventories (Streets and Waldhoff,
2000) suggest that Far East Asia, with its large
population and rapidly emerging industrialization
and urbanization, is one of the major source regions
for worldwide anthropogenic PM. Past studies also
indicate consistently higher ambient PM levels in this
region than in North America and Europe (Streets and
Waldhoff, 2000). To minimize further degradation of
the environment, actions must be taken to regulate PM
emissions.
Hong Kong is one of the most developed regions
in Asia. With more than 6.8 million residents living
in a 1100 km2 area, this metropolitan region has
one of the highest population densities in the world.
Potential PM sources in Hong Kong include power
generation, industries, motor vehicle exhaust, road
dust, and commercial and residential heating/cook-
ing. In addition, long-range transport from upwind,
densely populated southeastern China also contrib-
utes to elevated pollution levels. Ho et al. (2002,
2003) investigated the characteristic of major
elements, ions and carbonaceous material in PM10
and PM2.5 (airborne particles with aerodynamic
diameters less than 10 and 2.5 Am, respectively)
during winter months in Hong Kong. Their results
indicated that the majority of the PM10 is in the
PM2.5 fraction, especially in urban and industrial
areas. During winter months, pollutants transported
from the Asian continent result in elevated organic
and elemental carbon (OC, EC) concentrations at
the remote site. Pathak et al. (2003) estimated that
~40% of the PM2.5 ammonium sulfate (NH4SO4) in
Hong Kong originated from long-range transport
and non-local sources. Yu et al. (2004) showed that
the variable EC seasonality in Hong Kong is a
result of two counteracting factors: influence of
marine vessels emissions in summer and northerly
transport of air masses with elevated carbonaceous
aerosol in winter.
A year-long PM2.5 study was carried out during
2000/2001 with the following objectives: (1) to
determine annual average PM2.5 concentrations for
traffic-dominated urban and non-urban parts of Hong
Kong, (2) to investigate the spatial and temporal
variations of PM2.5 inorganic and organic chemical
composition, and (3) to link ambient PM 2.5 to
emission sources. The sampling schedule procedure,
analytical techniques, and quality assurance of this
study were identical or equivalent to those adopted by
major air quality networks in the United States (e.g.,
the U.S. Environmental Protection Agency [EPA]
Speciation Trends Network’ Jayanty et al. (2002)).
Meteorological characteristics on episodic days along
with seasonal variations in PM composition are
addressed by Louie et al. (in review). Since there are
no speciated PM2.5 studies for this region on an annual
basis, this study is a crucial step toward defining
ambient air quality standards and implementing
pollution reduction measures for PM2.5 in Hong Kong.
2. Technical approaches
The Hong Kong metropolitan area includes
Hong Kong Island, Kowloon Peninsula, and the
New Territories, located at the southern end of the
China coastline and facing the South China Sea.
Despite being in the tropics at approximately the
same latitude as Hawaii, United States, the climate
in Hong Kong features a distinct seasonal cycle due
to the Asiatic monsoon. The ambient air quality
monitoring network is shown in Fig. 1. Tsuen Wan
(TW) is an urban, highly populated, residential site
with mixed commercial and industrial developments
in the New Territories. Mong Kok (MK), located 2
km west of the Kowloon Peninsula and southeast
of the TW site, represents population exposure to
heavy traffic and restaurant cooking, in addition to
the urban mixture. Hok Tsui (HT) is a rural
background/transport site located ~20 km southeast
of the MK site, at the southeast end of Hong Kong
Island.
Twenty-four-hour (midnight to midnight LST)
PM2.5 sampling using Partisol samplers (Rupprecht
 P.K.K. Louie et al. / Science of the Total Environment 338 (2005) 267–281 269

Fig. 1. Locations of 12-month (11/06/2000 to 10/26/2001) PM2.5 monitoring sites. Tsuen Wan (TW, latitude 22.388N, longitude 114.18E,
elevation 25 m above mean sea level) is in an urban commercial/residential area. Mong Kok (MK, latitude 22.328N, longitude 114.18E,
elevation 17 m above mean sea level) is a source-oriented roadside site. Hok Tsui (HT, latitude 22.218N, longitude 114.268E, elevation 60 m
above mean sea level) is a rural background/transport site.

and Patashnick, Albany NY, USA) was carried out
every 6th day from 11/06/00 to 10/26/01 at the three
sites. Each Partisol sampler was equipped with an
Andersen SA-246 PM10 size-selective inlet followed
by a PM2.5 WINS (Well Impactor Ninety Six)
impactor, and sampled at a flow rate of 16.7 L min 1
(Watson and Chow, 2001). Two samplers were
collocated at each site: one configured with a ringed
Teflon-membrane filter (#R2PJ047, Pall Life Sciences,
Ann Arbor MI, USA), and the other with a quartz-fiber
filter (#2500QAT-UP, Pall Life Sciences, Ann Arbor
MI, USA). The Teflon-membrane filter collected
particles for mass by gravimetry and for 40 elements
(Na to U) by X-ray fluorescence (XRF) (Watson et al.,
1999). The quartz-fiber filter was analyzed for mass by
gravimetry and for OC and EC following the U.S.
EPA’s Interagency Monitoring of Protected Visual
Environments (IMPROVE) (Chow et al., 1993, 2001)
and Speciation Trends Network (STN) thermal evolu-
tion protocols (Peterson and Richards, 2002). Water
extracts of the quartz-fiber filter were analyzed for
chloride (Cl ), nitrate (NO3 ), and sulfate (SO42 ) by
ion chromatography (IC); for ammonium (NH4+) by
automated colorimetry (AC); for water-soluble sodium
(Na+) and potassium (K+) by atomic absorption
spectrophotometry (AAS) (Chow and Watson, 1999).
Solvent-extractable organic compounds (SEOC) and
organic markers were also measured. These results and
a comparison of carbon fractions between the two
thermal evolution protocols are presented in Sin et al.
(in press) and Chow et al. (in review), respectively.
3. Results and discussion
3.1. Measurement validity
Table 1 summarizes the analytical specifications
for speciated PM2.5. Minimum detection limits
(MDL) and root mean squared (RMS) precisions are
given. Each measurement in this study is associated
with uncertainties from four origins: sample volume,
analytical precision, deposition homogeneity, and
field blank concentration. The uncertainty was esti-
mated (e.g., by flow rate performance test, replicate
analysis, blank variability) and propagated to calcu-
270 P.K.K. Louie et al. / Science of the Total Environment 338 (2005) 267–281

Table 1
Analytical specifications for 24-h PM2.5 measurements at the Mong Kok (MK), Tsuen Wan (TW), and Hok Tsui (HT) sites during the 12-month
PM2.5 characterization Study in Hong Kong from 11/06/00 to 10/26/01
Species Analysis MDL RMS No. of %N
methoda (Ag m 3)b (Ag m 3)c valuesd MDL
Teflon mass Gravimetry N/A 4.6896 176 N/A
Quartz mass Gravimetry N/A 4.7592 176 N/A
Chloride (Cl ) IC 0.0521 0.0573 176 64
Nonvolatilized nitrate (NO3 ) IC 0.0521 0.1226 176 99
Sulfate (SO24 ) IC 0.0521 1.0807 176 100
Ammonium (NH+4 ) AC 0.0521 0.2080 176 99
Soluble sodium (Na+) AAS 0.0104 0.2637 176 93
Soluble potassium (K+) AAS 0.0104 0.0370 176 100

IMPROVE TOR PROTOCOL d

OC1 TOR 0.0958 0.5894 176 81
OC2 TOR 0.0958 0.8606 176 100
OC3 TOR 0.0958 2.3703 176 100
OC4 TOR 0.0958 0.8835 176 100
OPTC TOR 0.0958 0.6400 176 13
OCTC TOR 0.0958 3.3319 176 100
EC1 TOR 0.0958 0.4819 176 100
EC2 TOR 0.0958 0.6511 176 95
EC3 TOR 0.0958 0.2008 176 1
ECTC TOR 0.0958 0.8000 176 100
TCTC TOR 0.0958 3.7332 176 100

STN TOT PROTOCOL e

OCTC TOT 0.0958 3.4675 129 99
ECTC TOT 0.0958 0.7670 129 99
TCTC TOT 0.0958 3.8674 129 99
Sodium (Na) XRF 0.0331 0.0423 176 92
Magnesium (Mg) XRF 0.012 0.0211 176 88
Aluminum (Al) XRF 0.0048 0.0122 176 99
Silicon (Si) XRF 0.003 0.0284 176 100
Phosphorus (P) XRF 0.0027 0.0148 176 55
Sulfur (S) XRF 0.0024 0.1883 176 100
Chlorine (Cl) XRF 0.0048 0.0655 176 51
Potassium (K) XRF 0.0029 0.0368 176 100
Calcium (Ca) XRF 0.0022 0.0114 176 100
Titanium (Ti) XRF 0.0014 0.0317 176 70
Vanadium (V) XRF 0.0012 0.0133 176 88
Chromium (Cr) XRF 0.0009 0.0038 176 38
Manganese (Mn) XRF 0.0008 0.0019 176 96
Iron (Fe) XRF 0.0007 0.0123 176 100
Cobalt (Co) XRF 0.0004 0.0040 176 13
Nickel (Ni) XRF 0.0004 0.0010 176 98
Copper (Cu) XRF 0.0005 0.0013 176 93
Zinc (Zn) XRF 0.0005 0.0105 176 99
Gallium (Ga) XRF 0.0009 0.0026 176 19
Arsenic (As) XRF 0.0008 0.0152 176 77
Selenium (Se) XRF 0.0006 0.0013 176 77
Bromine (Br) XRF 0.0005 0.0015 176 176
Rubidium (Rb) XRF 0.0005 0.0011 176 135
Strontium (Sr) XRF 0.0005 0.0013 176 120
Yttrium (Y) XRF 0.0006 0.0019 176 3
Zirconium (Zr) XRF 0.0008 0.0020 176 43
 P.K.K. Louie et al. / Science of the Total Environment 338 (2005) 267–281 271

Table 1 (continued)
Species Analysis MDL RMS No. of %N
methoda (Ag m 3)b (Ag m 3)c valuesd MDL
Molybdenum (Mo) XRF 0.0013 0.0036 176 21
Palladium (Pd) XRF 0.0053 0.0104 176 6
Silver (Ag) XRF 0.0058 0.0124 176 8
Cadmium (Cd) XRF 0.0058 0.0131 176 22
Indium (In) XRF 0.0062 0.0147 176 12
Tin (Sn) XRF 0.0081 0.0159 176 127
Antimony (Sb) XRF 0.0086 0.0220 176 27
Barium (Ba) XRF 0.0249 0.0805 176 57
Lanthanum (La) XRF 0.0297 0.1101 176 27
Gold (Au) XRF 0.0015 0.0080 176 18
Mercury (Hg) XRF 0.0012 0.0033 176 3
Thallium (Tl) XRF 0.0012 0.0043 176 1
Lead (Pb) XRF 0.0014 0.0060 176 171
Uranium (U) XRF 0.0011 0.0032 176 3
a
IC=ion chromatography; AC=automated colorimetry; AAS=atomic absorption spectrophotometry; TOR=thermal/optical reflectance;
XRF=X-ray fluorescence.
b
Minimum detectable limit (MDL) is the concentration at which instrument response equals three times the standard deviation of the
response to a known concentration of zero. Typical sample volumes are 24.1 m3.
c
Root mean squared precision (RMS) is the square root of the sum of the squared uncertainties of the observations divided by the number
of observations.
d
For thermal/optical reflectance (TOR) carbon analyses following the IMPROVE protocol, the temperature levels in a pure helium (He)
atmosphere are 120 8C (OC1), 250 8C (OC2), 450 8C (OC3), and 550 8C (OC4). Advancing to next stage begins when the flame ionization
detector (FID) response returns to baseline or remains a constant value. The temperature levels in a 98% He/2% O2 atmosphere are 550 8C
(EC1), 700 8C (EC2), and 800 8C (EC3). The fraction of pyrolyzed organic carbon (OPR) is detected in the He/O2 atmosphere at 550 8C prior to
the return of reflectance to its original value. OC is defined as OC1+OC2+OC3+OC4+OPR, and EC is defined as the difference between TC
and OC (Chow et al., 1993, 2001).
e
The STN protocol is similar to the NIOSH protocol (NIOSH, 1996, 1998, 1999). The temperature set points in He are 315 8C (60 s),
480 8C (60 s), 615 8C (60 s), and 900 8C (90 s). Then the temperature is reduced to ~600 8C before a He/O2 atmosphere is introduced. The
temperature set-point in He/O2 are 600, 675, 750, 825, and 920 8C, each for 45 s. In STN protocol, pyrolyzed OC (OPT) is adjusted by laser
transmittance rather than reflectance.

late the measurement precision. Table 1 shows that
RMS uncertainties are typically 2–20 times higher
than analytical MDLs, mainly owing to the variability
of field blanks.
Major mass constituents, including OC, EC, SO42 ,
NO3 , NH4+, and elements (e.g., Al, Si, Ca, Fe, and Zn)
were detected in almost every sample. Species seldom
showing concentrations higher than twice the respec-
tive measurement uncertainties (i.e., 95% confidence
level) include Cr, Co, Ga, As, Y, Zr, Mo, Pd, Ag, Cd,
In, Sb, Ba, La, Au, Hg, Tl, and U. Residual-oil-
combustion-related species Ni and V were detected in
98% and 88% of the samples, respectively, whereas
vehicle-exhaust-related species Br and Pb were
detected in 99% and 95% of the samples, respectively.
Marine-aerosol-related species Na+ and Cl were
detected in 93% and 64% of the samples, respectively.
Phosphorus (P) was detected only at the roadside MK
site, but Sn was detected at both urban sites. These data
show that the analytical protocols established for this
study are adequate for samples acquired.
Fig. 2 shows good agreement between gravimetric
mass measurements from the collocated Teflon-
membrane and quartz-fiber filter samples. PM2.5 mass
concentrations determined from quartz-fiber filters are
7–9% higher than their Teflon counterparts. A
positive intercept of ~3 Ag m 3 is likely due to the
adsorption of organic vapor onto quartz-fiber filters
(Chow et al., 1996). These results are consistent with
the observations of Engelbrecht et al. (2001). The
high correlation (RN0.99) indicates consistent sam-
pling and analysis results from the two Partisol
samplers deployed. Since the adsorbed organic vapor
should not be part of PM2.5, the following discussion
272 P.K.K. Louie et al. / Science of the Total Environment 338 (2005) 267–281
Fig. 2. PM2.5 gravimetric mass acquired from Teflon-membrane and
quartz-fiber filters in Hong Kong during the 12-month PM2.5 study.
Higher PM2.5 mass and a positive intercept (~3 Ag m–3) suggest the
adsorption of organic gases onto quartz-fiber filters (Chow et al.,
1996; Watson and Chow, 2002). These results demonstrate that fiber
losses of quartz-fiber filters during filter handling and transport are
minimal. These results are also consistent with the observations of
Engelbrecht et al. (2001).
refers to Teflon-membrane filter mass unless other-
wise specified.
Ionic species (i.e., Cl , NO3 , SO42 , NH4+, Na+,
+
K ) have been independently measured by the Govern-
ment Laboratory of Hong Kong SAR by IC, and the
results were found to be in good agreement (Relative
Standard Deviation [RSD]b10%) with those measured
at the Desert Research Institute (DRI). Fig. 3 compares
the concentrations of water-soluble potassium (K+)
acquired by AAS on quartz-fiber filters and total
potassium (K) acquired by XRF on Teflon-membrane
filters. The K+ concentration ranged from 0.01 to 2.5
Ag m 3, with an average of ~0.40 Ag m 3. A strong
correlation (r=0.98) indicates consistent sampling and
analysis measurement results between the Teflon-
membrane and quartz-fiber filter samples. On average,
~90% of total potassium is soluble, indicative of
vegetative burning, cooking, or marine aerosol rather
than geological origins. The measurement of K+ for
the two most loaded samples exceeded the K measure-
ment within ~15%. This might result from a larger
analytical uncertainty or inhomogeneous deposition
for heavily loaded samples.
The validity of ion measurements is verified
through anion and cation balances (Chow et al.,
1994). NH4+ appears to be the dominant cation
associated with NO3 and SO42 in PM2.5, but sodium
nitrate (NaNO3) and sodium sulfate (Na2SO4) can be
present in coastal areas due to displacement of Cl in
sea salt by NO3 and SO42 (Finlayson-Pitts and Pitts,
2000; Seinfeld and Pandis, 1998). Ho et al. (2003)
concluded that the major fraction of SO42 in Hong
Kong is non-sea-salt SO42 with substantial anthro-
pogenic origin. The NH4+ concentration can be
calculated assuming that all NO3 is in the form of
ammonium nitrate (NH4NO3) and all SO42 is in the
form of either ammonium sulfate ([NH4]2SO4) or
ammonium bisulfate (NH4HSO4), depending on the
degree of ammoniation. Fig. 4 demonstrates the
agreement between calculated and measured NH4+
concentrations with correlation coefficients exceeding
0.97 for either case. The slope is near unity
(1.05F0.02) when (NH4)2SO4 is assumed, and low
(0.60F0.01) when NH4HSO4 is assumed, consistent
with full neutralization of nitric and sulfuric acid by
gaseous ammonia (NH3). Annual average (NH4)2SO4
concentrations were similar (11.9–13.1 Ag m 3) at the
three sampling sites, indicative of a regional nature of
(NH4)2SO4. (NH4)2SO4 constituted 51% of PM2.5
mass at the HT site, but only 23% of PM2.5 at the MK
site and 37% at the TW site. SO42 mostly originates
from the oxidation of sulfur dioxide (SO2) emitted
during the combustion of sulfur-containing bio- or
fossil fuels. A relatively small fraction of SO42 can be
Fig. 3. A comparison of 24-h-average soluble K+ (by atomic
absorption spectrometry) and total K (by x-ray fluorescence) in
Hong Kong. The dashed line indicates the 1:1 ratio.
 P.K.K. Louie et al. / Science of the Total Environment 338 (2005) 267–281
Fig. 4. A scatter plot of calculated ammonium concentrations versus
measured concentrations from PM2.5 data acquired in Hong Kong.
If all sulfate is assumed to be in the form of ammonium sulfate, then
calculated ammonium=([0.38SO24 ]+[0.29NO3 ]). If all sulfate
is assumed to be in the form of ammonium bisulfate, then calculated
ammonium=([0.192SO24 ]+[0.29NO3 ]).
produced in marine air through oxidation of dimethyl
sulfide (DMS) (Pandis et al., 1994). The strong
correlation (R 2~0.87) of NH4+ with SO42 and a
NH4+/SO42 molar ratio of ~2 suggest that most of
NH4+ is in the form of (NH4)2SO4. In Fig. 4, the
positive intercepts (0.44F0.3 and 0.92F0.7 Ag m 3)
suggest the presence of SO42 and/or NO3 associated
with water-soluble Na+. The median Na+/NH4+ molar
ratio was ~0.15, but it was as high as 1.2 at low NH4+
concentrations.
Reconstructed PM2.5 mass calculated from chem-
ical composition agrees with gravimetric mass, as
shown in Fig. 5. Small differences (b10%) for some
samples may be due to uncertainties in the multipliers
for calculating organic matter (OM, which is assumed
to be 1.4OC) and crustal material (CM) as well as
unquantified species such as water (Turpin and Lim,
2001; Chen et al., 2003). A different empirical formula
(Watson, 2002a) for crustal material is used in the U.S.
IMPROVE network to estimate PM2.5 reconstructed
mass. Differences between the two versions (DRI and
IMPROVE) of reconstructed crustal material, assum-
ing different forms of oxides in major crustal
components, do not result in differences in recon-
structed PM2.5 mass. This is partially due to low crustal
concentrations found in these PM2.5 samples.
273
3.2. Urban and rural contrasts
3.2.1. Annual averages
Annual averages and standard deviations of PM2.5
mass and species concentrations are presented, by site,
in Table 2. The average PM2.5 mass varied by 2.5-fold
among the three sites, with 58.1F18.5 Ag m 3 at the
roadside MK site, 33.9F19.4 Ag m 3 at the urban TW
site, and 23.7F14.8 Ag m 3 at the rural HT site.
Annual averages derived from quarterly averages
(U.S. EPA, 1997) are similar, being 58.4F5.1,
31.4F4.5, and 26.8F4.4 Ag m 3 for the MK, TW,
and HT sites, respectively. Even at the HT background
site, the annual PM2.5 concentration was more than 1.5
times the U.S. EPA’s annual PM2.5 NAAQS of 15 Ag
m 3. Daily PM2.5 concentrations exceeded the U.S.
24-h NAAQS of 65 Ag m 3 three times at the urban
TW site and once at the rural HT site, reaching
131.4F7.7, 122.0F7.4, and 68.3F5.4 Ag m 3 at the
MK, TW, and HT sites, respectively. More than ~70%
of these high levels occurred during winter when the
air was stagnant (Louie et al., in review). A multi-site
Fig. 5. A comparison of 24-h PM2.5 gravimetric (from Teflon) and
reconstructed mass in Hong Kong. Reconstructed mass is derived
from summing SO24 , NO3 , NH+4 , OM, EC, and CM mass. Organic
matter (OM) is determined from 1.4OC in order to account for O, H,
and N atoms in organic compounds (White and Roberts, 1977). DRI
reconstructed mass= ([1.38SO24 ]+ [1.09NO3 ]+[1.4OC]+EC+
[1.89Al]+[2.14Si]+[1.4Ca]+[1.43Fe]) (Solomon et al.,
1989). U.S. IMPROVE reconstructed mass=([1.38 SO 42 ]+
[1.29NO3 ]+ [1.4OC]+EC+[2.2Al]+[2.49Si]+[1.63Ca]+
[2.42Fe]+ [1.94Ti]) (Malm et al., 1994). The dashed line indicates
the 1:1 ratio.
274 P.K.K. Louie et al. / Science of the Total Environment 338 (2005) 267–281

Table 2
Statistical summary of PM2.5 measurements in Hong Kong from 11/6/2000 to 10/26/2001 (24-h samples taken from midnight to midnight every
6th day)
MeanF1r % of samples exceeding two
(Ag m 3) times measurement uncertaintya
MK (56 days)b TW (56 days)b HT (56 days)b MK TW HT
Teflon mass 58.05F18.51 33.89F19.39 23.68F14.82 100 100 82
Quartz mass 62.31F18.57 37.06F18.38 25.94F14.25 100 100 96
Chloride (Cl ) 0.26F0.37 0.14F0.36 0.14F0.21 75 38 45
Nitrate (NO3 ) 1.67F1.70 1.29F1.61 0.70F1.08 100 100 93
Sulfate (SO2-4) 9.44F5.35 9.09F5.13 8.69F5.12 100 100 100
Ammonium (NH+4 ) 3.16F2.18 2.91F2.15 2.17F1.68 100 100 96
Soluble sodium (Na+) 0.39F0.28 0.40F0.29 0.69F0.56 41 39 73
Soluble potassium (K+) 0.46F0.45 0.49F0.48 0.40F0.39 100 100 96
O1TCc 2.51F1.29 0.72F0.58 0.21F0.28 100 86 39
O2TCc 2.49F0.91 1.42F0.59 0.69F0.48 100 100 96
O3TCc 4.56F2.32 2.79F1.81 1.48F1.47 100 100 91
O4TCc 6.946F4.437 3.782F2.635 1.792F1.653 100 100 100
OPTCc 0.187F1.026 0.017F0.082 0.076F0.152 5 2 25
OC (IMPROVE) 16.656F7.627 8.700F5.274 4.215F3.708 100 100 98
E1TCc 20.044F4.285 5.085F1.393 1.539F0.955 100 100 100
E2TCc 0.320F0.428 0.302F0.240 0.224F0.094 80 89 91
E3TCc 0.001F0.005 0.004F0.020 0.000F0.000 2 4 0
EC (IMPROVE) 20.177F4.247 5.374F1.396 1.687F0.923 100 100 100
TCTC (IMPROVE) 36.814F7.492 14.055F5.755 5.883F4.419 100 100 100
Sodium (Na) 0.175F0.104 0.161F0.109 0.284F0.160 84 79 96
Magnesium (Mg) 0.042F0.028 0.039F0.036 0.057F0.042 73 66 79
Aluminum (Al) 0.113F0.111 0.116F0.124 0.109F0.129 98 96 93
Silicon (Si) 0.477F0.331 0.390F0.371 0.348F0.391 100 100 98
Phosphorus (P) 0.009F0.007 0.005F0.005 0.003F0.004 32 4 4
Sulfur (S) 3.454F1.832 3.353F1.814 3.069F1.769 100 100 100
Chlorine (Cl) 0.120F0.275 0.088F0.336 0.146F0.232 45 21 45
Potassium (K) 0.557F0.489 0.582F0.506 0.485F0.447 100 100 100
Calcium (Ca) 0.170F0.106 0.128F0.120 0.103F0.120 100 100 98
Titanium (Ti) 0.009F0.010 0.009F0.011 0.008F0.012 0 4 2
Vanadium (V) 0.014F0.017 0.014F0.012 0.012F0.012 21 27 14
Chromium (Cr) 0.001F0.001 0.001F0.001 0.001F0.001 0 2 0
Manganese (Mn) 0.013F0.010 0.012F0.010 0.008F0.007 91 88 70
Iron (Fe) 0.269F0.137 0.188F0.147 0.122F0.133 100 100 100
Cobalt (Co) 0.000F0.000 0.000F0.000 0.000F0.000 0 0 0
Nickel (Ni) 0.0057F0.0063 0.0054F0.0050 0.0048F0.0041 86 80 89
Copper (Cu) 0.0114F0.0101 0.0089F0.0111 0.0051F0.0071 100 89 63
Zinc (Zn) 0.1784F0.1329 0.1739F0.1749 0.1062F0.1061 100 100 95
Gallium (Ga) 0.0004F0.0007 0.0004F0.0008 0.0005F0.0007 0 0 0
Arsenic (As) 0.005F0.006 0.006F0.008 0.004F0.005 2 4 2
Selenium (Se) 0.002F0.002 0.002F0.002 0.002F0.002 30 36 32
Bromine (Br) 0.013F0.016 0.013F0.020 0.012F0.011 100 96 95
Rubidium (Rb) 0.004F0.005 0.004F0.005 0.003F0.004 55 57 45
Strontium (Sr) 0.001F0.001 0.001F0.001 0.001F0.001 16 13 13
Yttrium (Y) 0.000F0.000 0.000F0.000 0.000F0.000 0 0 0
Zirconium (Zr) 0.001F0.001 0.001F0.001 0.001F0.001 0 0 0
Molybdenum (Mo) 0.001F0.001 0.001F0.001 0.001F0.001 0 0 0
Palladium (Pd) 0.0013F0.0018 0.0017F0.0018 0.0012F0.0017 0 0 0
Silver (Ag) 0.0010F0.0021 0.0016F0.0020 0.0015F0.0023 0 0 0
Cadmium (Cd) 0.0020F0.0022 0.0023F0.0029 0.0021F0.0028 0 0 0
 P.K.K. Louie et al. / Science of the Total Environment 338 (2005) 267–281 275

Table 2 (continued)
MeanF1r % of samples exceeding two
(Ag m 3) times measurement uncertaintya
MK (56 days)b TW (56 days)b HT (56 days)b MK TW HT
Indium (In) 0.002F0.003 0.002F0.003 0.001F0.002 0 0 0
Tin (Sn) 0.0190F0.0140 0.0204F0.0181 0.0113F0.0087 20 23 0
Antimony (Sb) 0.0046F0.0063 0.0050F0.0074 0.0038F0.0051 2 2 0
Barium (Ba) 0.0267F0.0216 0.0159F0.0171 0.0086F0.0125 0 0 0
Lanthanum (La) 0.0130F0.0176 0.0090F0.0131 0.0136F0.0154 0 0 0
Gold (Au) 0.0004F0.0008 0.0005F0.0010 0.0004F0.0010 0 0 0
Mercury (Hg) 0.0001F0.0002 0.0002F0.0004 0.0001F0.0002 0 0 0
Thallium (Tl) 0.0001F0.0002 0.0001F0.0002 0.0001F0.0002 0 0 0
Lead (Pb) 0.0671F0.0770 0.0718F0.0889 0.0568F0.0591 91 88 84
Uranium (U) 0.0002F0.0004 0.0002F0.0003 0.0002F0.0003 0 0 0
a
The percent of samples for which the measurement is greater than twice its uncertainty. This reflects the good signal/noise ratio in the data.
b
11/24/2000, 2/10/2001, 3/30/2001, and 9/8/2001 are not included due to missing data from one or more sites. Sites include: Mong Kok
(MK) roadside site, Tsuen Wan (TW) urban site, and Hok Tsui (HT) rural background/transport.
c
For thermal/optical reflectance (TOR) carbon analyses following the IMPROVE protocol, the temperature levels in a pure helium (He)
atmosphere are 120 8C (OC1), 250 8C (OC2), 450 8C (OC3), and 550 8C (OC4). Advancing to next stage begins when the flame ionization
detector (FID) response returns to baseline or remains a constant value. The temperature levels in a 98% He/2% O2 atmosphere are 550 8C
(EC1), 700 8C (EC2), and 800 8C (EC3). The fraction of pyrolyzed organic carbon (OPR) is detected in the He/O2 atmosphere at 550 8C prior to
the return of reflectance to its original value. OC is defined as OC1+OC2+OC3+OC4+OPR, and EC is defined as the difference between TC
and OC (Chow et al., 1993, 2001).

pollution episode was found on 02/28/01. The road-
side Mong Kok site represents pedestrian exposure in a
source (i.e., vehicle exhaust) dominated environment;
PM2.5 concentrations are frequently 50% higher than
at other urban sites. Approximately one-third of the
samples acquired at the MK site exceed 65 Ag m 3.
In addition to carbon and SO42 , average concen-
trations exceeding 0.1 Ag m 3 (with measurements in
N90% of the samples exceeding two times uncertainty
[2r]) were also observed for all other ions (e.g., NH4+,
NO3 , Cl , Na+, K+) and crustal-related elements
(e.g., Al, Si, K, Ca, Fe, Zn). Motor-vehicle-exhaust-
related elements Br and Pb, averaging 0.01–0.05 Ag
m 3, were present at significant (N2r) levels in more
than 80% of the samples. Ni was present in more than
80% of the samples, as compared to V in only 14–
27% of the samples.
Strong correlations (R 2) of K+ with Pb (0.88) and
Rb (0.92) were found. The Pb/K+ and Rb/K+ ratios of
~0.1 and 0.01, respectively, were about 10 times
higher than those in wood burning profiles reported
by Turn et al. (1997). K+ was moderately correlated
with Mn (0.66), Cu (0.59), Zn (0.62), As (0.74), Se
(0.69), and Br (0.45), consistent with the co-occur-
rence of these elements in incinerator emissions
(Olmez et al., 1988). Only chemical waste is
incinerated in Hong Kong, not domestic waste.
However, waste is commonly incinerated and burned
in neighboring mainland China and the Macao Special
Administrative Region (SAR).
3.2.2. Spatial variations
Annual average total carbon (sum of OC and EC)
differed by more than 6-fold, from 5.9F4.4 Ag m 3 at
the HT site to 36.8F7.4 Ag m 3 at the MK site, and
accounted for 25–63% of the PM2.5 mass. The largest
spatial variations occurred for EC (N10-fold), fol-
lowed by OC (N4-fold). Annual average EC was
20.1F4.2 Ag m 3 at the MK site, 5.4F1.4 Ag m 3 at
the TW site, and 1.7F0.9 Ag m 3 at the HT site. The
overall EC/OC ratio at MK was ~1.2, which is close
to the mean value reported previously for diesel
exhausts (Gertler et al., 1999, 2000). Diesel vehicles
accounted for N60% of the traffic in Hong Kong
during the study, prior to a conversion of diesel taxis
to liquefied petroleum gas (LPG). Elevated PM2.5
concentrations at the roadside MK site were influ-
enced by emissions from on-road gasoline, LPG, and
diesel vehicle exhaust. While most daily activities in
Hong Kong occur within the urban center, elevated
PM2.5 mass and carbonaceous aerosol at this heavily
trafficked location may have significant impact on
276 P.K.K. Louie et al. / Science of the Total Environment 338 (2005) 267–281
human exposure. At the TW and HT sites, the EC/OC
ratios were lower by 50–70% at 0.61 and 0.39,
respectively. The influence of local vehicle exhaust
was least at HT, where a mixture of aged carbon
aerosol from domestic coal burning, biomass burning,
biogenic emissions, and secondary organic aerosol
resulted in lower EC/OC ratios than those observed at
the roadside and urban sites. A similar urban–rural
contrast was found for the solvent extractable organic
compounds (SEOC) by Sin et al. (in press). Distinct
spatial variations in the concentrations of total and
four classes (aliphatic hydrocarbons, polynuclear
aromatic hydrocarbons, fatty acids/alkanoic acids
and alkanols) of SEOC were observed with the
highest concentrations (accounting for 8–18% of
OC) found at the roadside MK site with the lowest
concentrations at the background HT site.
Secondary inorganic aerosols were homogeneously
distributed among the three sites, with the least spatial
variation (F2% in coefficient of variation) found for
SO42 , ranging from 8.7F5.1 Ag m 3 at the HT site to
9.4F5.4 Ag m 3 at the MK site and accounting for
16–37% of PM2.5 mass. Annual average PM2.5 NO3
concentrations were low, in the range of 0.7–1.7 Ag
m 3, and accounted for 2–4% of average PM2.5 mass.
Nitric acid (HNO3) and NO3 are secondary pollutants
formed in the atmosphere predominantly through
oxidation of reactive nitrogen (NOx ). High-temper-
ature combustion in vehicle engines and boilers
dominate NOx production in urban areas (Stehr et
al., 2000), resulting in elevated NO3 levels at the two
urban sites.
Water-soluble K+, ranging from 0.4 to 0.5 Ag
m 3, is 10–20% higher at the two urban sites as
compared to the rural HT site. Water-soluble
sodium (Na+), chloride (Cl ), and bromide (Br )
are markers for marine aerosol. Na+ is often a
better marker for sea salt because volatilization of
Cl and Br by acid displacement or photo-
chemistry may limit their utility as a sea salt
indicator. In addition, vegetative burning, incinerator
operation, and vehicle exhaust may also contribute
to Br concentrations (Dzubay et al., 1988; Malm
and Gebhart, 1997; Chen et al., 2002). Water-
soluble Na+ at the coastal HT site (0.69F0.56 Ag
m 3) was more than 1.5 times the levels found at
the two urban sites, consistent with its location on
the Pacific Ocean shoreline.
A high correlation (0.92) was found between Ni
and V across the three sampling sites, indicative of
residual oil-fired combustion (Olmez et al., 1988).
Power generated through oil-fired plants in Hong
Kong and China may have contributed to this.
However, Ni (0.005–0.006 Ag m 3) and V (0.0012–
0.0014 Ag m 3) were not high and with very little
urban–rural contrast. Residual oil and diesel fuel used
in marine vessels may also contribute to Ni, V, OC,
and EC concentrations (Sinha et al., 2003). It is
estimated that more than 500 seaborne and river ships
per day use the ports shown in Fig. 1 (Yu et al.,
2002).
Concentrations of major crustal components were
low (0.1–0.5 Ag m 3) during this study. Approx-
imately 40–70% of urban–rural contrast was found for
Si, K, Ca, and Zn. The largest difference (N2-fold)
was found for PM2.5 Fe, which was 0.12F0.13 Ag
m 3 at the rural HT site and 0.27F0.14 Ag m 3 at the
roadside MK site. Other elemental levels were low
and variable with very little urban–rural contrast.
Annual average mass fractions of selected species
in PM2.5 are shown, by site, in Fig. 6. The largest
PM2.5 fraction is carbonaceous material, which is
substantially (20–40%) higher at the two urban sites.
OM contributions account for more than a third of
PM2.5 mass (36–40%) at the two urban sites. Fig. 7
compares the average PM2.5 chemical compositions
among the three sites. Carbonaceous aerosol (i.e., the
sum of OM and EC) accounts for 75% and 52% of
PM2.5 mass at the MK and TW sites, respectively.
Even at the background HT site, carbonaceous aerosol
accounted for about one-third (32%) of PM2.5. Due to
the lower PM2.5 mass and carbon concentrations at
HT, most of the trace elements (including SO42 , Na+,
Cl , Al, Si, K+, K, Ca, Ni, Se, Br, Rb, and Pb) had
higher mass percentages at HT. Similarly, SO42 and
NH4+ at the rural HT site are 15–30% higher than those
found at the two urban sites. Urban influences were
stronger on the NO3 , Mn, Fe, Cu, and Zn concen-
trations, which showed higher mass percentages at
TW.
Secondary (NH4)2SO4 was the largest contributor at
the HT site, accounting for 51% of PM2.5 mass, and the
second-largest contributor at the two urban sites,
accounting for 23–37% of PM2.5 mass. Sea salt
accounted for 1–7% of PM2.5 mass at the three sites.
The annual average sea salt concentration (1.7 Ag m 3)
 P.K.K. Louie et al. / Science of the Total Environment 338 (2005) 267–281 277

Fig. 6. Annual average PM2.5 chemical concentrations (species mass fraction) of selected species in Hong Kong (11/2000–10/2001).

at the regional background HT site was nearly twice as itation, and ocean temperature could influence the Na+
high as those at the MK and TW (1.0 Ag m 3) sites, emission rate. No appreciable urban–rural contrast was
indicating a greater marine influence on the coastal found in crustal material, ranging from 1.3 to 1.9 Ag
line. Local meteorology, such as sea breeze, precip- m 3 and accounting for 3–5% of the PM2.5 mass. The

Fig. 7. Annual average (11/2000–10/2001) PM2.5 material balance at three sampling sites (Mong Kok, Tsuen Wai, and Hok Tsui) in Hong Kong.
Negative unidentified mass fraction indicates a greater reconstructed mass than measured gravimetric mass. Ammonium sulfate=1.38SO24 .
Ammonium nitrate=1.29NO3 . OM=1.4OC. Sea salt=2.54Na+. Crustal material=([1.89Al]+[2.14Si]+[1.4Ca]+[1.43Fe]) (Solomon
et al., 1989). Other trace elements include 35 of the 40 elements (Na to U, excluding Al, Si, Ca, Fe, and Na) listed in Table 1.
278 P.K.K. Louie et al. / Science of the Total Environment 338 (2005) 267–281

Fig. 8. Ternary plots for: (a) a conceptual PM2.5 source model, (b) SO24 , EC, OC, and crustal material, and (c) NO3 , Na+, and Ni determined at
the Mong Kok (MK), Tsuen Wan (TW), and Hok Tsui (HT) sites.
 P.K.K. Louie et al. / Science of the Total Environment 338 (2005) 267–281
sum of other trace elements accounts for only 2–4% of
the PM2.5 mass.
3.2.3. Ternary diagrams for source interpretation
Concentrations of a specific PM2.5 species from
the three sampling sites can be compared in a ternary
diagram, which is commonly used for a variety of
applications in Earth Sciences, such as rock classi-
fication and phase transition, to represent the relative
contents of three components. Ternary diagrams
represent the spatial variation of PM2.5 measurements
from the MK, HT, and TW sites, which is indicative
of specific pollution sources. The percentage of a
species distributed among the three sites on a
particular sampling day determines its position in
the ternary plot.
Since the extent of source impact varies by site,
elevated concentrations of a source marker species at
a site explains higher impact by the source, and
therefore it appears closer to the corner representing
the site in the ternary diagram. An intuitive PM2.5
source model is demonstrated in Fig. 8(a), with the
MK, TW, and HT corners noted by mobile, urban,
and marine sources, respectively. Fig. 8(b) shows the
distribution of three major PM2.5 components (SO42 ,
OC, and EC) and crustal material for the study. The
cluster of SO42 located in the center of the diagram
suggests a uniform distribution among the urban and
rural sites, despite substantial day-to-day variations in
SO42 concentrations. This is consistent with the
hypothesis that SO42 is more regional in nature and
partly originates from distant sources. Situated at the
southeast corner of the Pearl River Delta (PRD),
Hong Kong is one of the most populated and
industrialized areas of China, and it is influenced by
the land–sea breeze circulation even under stagnant
conditions. From 10 a.m. to 5 p.m., the land breeze
over western Hong Kong can be as strong as 3–4 ms1
(10.8–13.6 km/h). Under such conditions, pollutants
from the PRD often entrain into Hong Kong through
this land–sea breeze circulation. The impact is less
significant under moderate-to-strong winds that are
not from the west or north.
In contrast, most of the EC measurements are
clustered towards the MK corner in Fig. 8(b),
implying a correspondence between EC concentration
and traffic density. OC is present between the clusters
of EC and SO42 , consistent with a combination of
279
local and regional sources. Most of the crustal
material is also clustered at the center of the diagram
(i.e., regional source), likely due to long-range trans-
port of Asian dust by prevailing winds (Louie et al., in
review). Occasional high crustal material concentra-
tions at the roadside site may result from vehicle-
resuspended road dust.
A broader distribution of NO3 is observed
between the two urban sites in Fig. 8(c). Though
uncertainties in NO3 measurements are higher
because of its volatility (Chow et al., 2002b) and
low ambient concentrations, an overall influence from
Hong Kong urban/on-road sources is indicated. The
marine influence is evident from the elevated Na+
concentrations at the HT site. The distribution of Ni is
consistent with regional contributions, but it shows a
larger scatter than SO42 .
4. Conclusions
The annual average PM2.5 mass concentrations
ranged from 23.7F14.8 to 58.1F18.5 Ag m 3 and are
~1.5–4 times higher than the U.S. EPA’s annual
NAAQS of 15 Ag m 3, indicating a serious fine
particulate pollution over the entire metropolitan
region. Elevated PM2.5 at the roadside MK site is
mostly attributed to elevated OC and EC from vehicle
exhaust in addition to other combustion sources such as
cooking/industrial emissions and vegetative burning.
This might have further impact on population exposure
because the site is located in an urban center where
people work, live, and play. The PM2.5 reconstructed
mass (estimated from SO42 , NO3 , NH4+, OM, EC,
crustal material, and sea salt) closely explains the
gravimetric mass within F10% and confirms the
validity of the mass and chemical measurements.
Carbonaceous material (EC and OM) dominated at
urban and roadside sites (N50%) and exhibited the
largest site-to-site variations. Ammoniated sulfate
concentrations showed limited urban–rural contrasts,
and its contribution to PM2.5 mass ranged from 23% to
37% at the two urban sites and 51% at the rural
background site. The intuitive source model, presented
in a ternary diagram, confirms the local influence of
vehicle exhaust at the urban sites. Long-range transport
of secondary ammonium sulfate and Asian dust cause
regional impacts at all three sites.
280 P.K.K. Louie et al. / Science of the Total Environment 338 (2005) 267–281
Acknowledgments
This study was sponsored by the Hong Kong
Environmental Protection Department under Contract
#90563. The authors wish to thank Steven Kohl of the
Desert Research Institute’s Environmental Analysis
Facility for conducting chemical analyses and per-
forming data validation of PM2.5 measurements, and
Norman Mankim and Eric Dieterle for assembling and
editing the manuscript.
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