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11th Int'l Conference on Chemical, Agricultural, Biological, Healthcare & Environmental Sciences (CABHES-2017) Aug.

12-14, 2017 Batam (Indonesia)

Mix and Match Particle Characterization and


Numerical Methods to Identify the Source of
Particulate Matter Emissions in Ambient Air
Azis Kemal Fauzie, G.V. Venkataramana

 also related to non-exhaust vehicular emissions, such as from


Abstract—Asian countries recently face serious problems related wearing of tire, brake, bearings, car body, and road dust [8].
to particulate pollution. To mitigate the continuous effects, the exact Unlike PM from point source emissions, the origin of
source of particle emissions should be clearly identified. This study is particles dispersed in ambient air is not clearly identified. A
aimed to examine particulate matter (PM) by combining advanced number of comprehensive works using various analytical
laboratory techniques and field data survey. PM concentrations have
been measured and are considerably correlated (p<0.05) with site methods has been published in the examination of atmospheric
temperature and traffic condition. Experimental PM concentrations aerosols [9]. Light and electron microscopes have been found
are correlated significantly with vehicular PM2.5 (p<0.005) and PM10 useful to investigate the microstructural characteristics of
(p<0.0005) emissions estimated numerically using model generated particles. Another important technique, the energy dispersive
from road traffic survey. Light scattering method and electron X-ray spectroscopy, is also helpful to rapidly acknowledge the
microscope image interpretation show that 83-99% of near-roadway elemental composition of particulate matter. In addition to
particles were in the size of PM2.5. Energy dispersive X-ray analysis
explains that roadside PM are carbon-rich particles containing 56% photomicrographical analysis, the size distribution of particles
elemental carbon emitted mostly by fossil-fueled vehicles. The mixed can also be determined using light scattering method by
data from particle characterization and road traffic analysis were dispersing the particles in a specific liquid. Examples have
found matched and similarly suggest that motor vehicles are the most been applied to food science and nanoparticle study [10].
responsible sources for urban PM pollution. The combination of advanced laboratory equipments and
computational graphic analysis has been carried out to study
Keywords—Air pollution, Particle characterization, Particulate the size, shape, morphology, and texture of solid particles
Matter, Vehicular emission
[11]. The schematic diagram has also been introduced to
classify the particulate matter according to the estimation of
I. INTRODUCTION
their element content [12]. But there is still a need to link
Air pollution in urban area is one of serious concern in between the size and chemical composition of ambient
recent times, particularly for Asian developing countries, and particles and their possible sources of emission. In case of
it may further extend from local to global scale [1]. Numerous vehicular pollution, PM emissions can be estimated using data
health effects related to particulate matter (PM) pollution have from road traffic survey [13]. The current study is aimed to
been recorded [2]. The major emissions of total PM in the identify the source of PM emissions by combining the field
atmosphere are mainly from natural sources. However, it is traffic data and experimental analyses of PM collected in
rather difficult to differentiate between natural and man-made urban environment at different spatial and meteorological
sources of emitted PM. Anthropogenic PM are generated from condition. The physico-chemical characterization of particles
vehicles, industries, burning of biomass, and combustion of was conducted comprehensively in full aspects including PM
fossil fuels [3]. The health studies confirm that anthropogenic concentration, size distribution, elemental composition, and
fine particles (PM2.5) are more harmful than coarse particles photomicrographical image interpretation.
(PM10) [4]. Traffic is potential sources of both coarse and fine
particles. Summary of reports explained that PM2.5/PM10 ratios II. MATERIALS AND METHODS
in urban sites are nearly half and less than in rural sites [5].
Ambient PM comprises sulfate, nitrate, chloride, ammonium, A. The Study Area
elemental carbon, and crustal materials [6], whereas the major Mysore is the second largest city in the state of Karnataka,
sources of black carbon are the emissions of diesel and India, after Bangalore metropolitan city. According to the
gasoline vehicles [7]. Other trace elements of heavy metals are 2011 national census, the population of Mysore is 918,225.
Urbanization in Mysore expands continuously due to its
Azis Kemal Fauzie (Author), Environment Management Board, important tourist and heritage sites. Like many other Indian
Government of Karawang Regency, Jl. Lingkar Tanjungpura No. 1 cities, Mysore city has high vehicular growth and emission
Karawang-41316, Indonesia, Email: aziskemalfauzie@gmail.com problem. It has over 520 thousand registered vehicles in 2015
G. V. Venkataramana (Co-Author), School of Forestry and Environmental
Studies, Yale University, New Haven, Connecticut, USA, Email: and is projected to increase about 120% in 2020 [14].
venkataraman_1970@yahoo.co.in

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11th Int'l Conference on Chemical, Agricultural, Biological, Healthcare & Environmental Sciences (CABHES-2017) Aug. 12-14, 2017 Batam (Indonesia)

Sampling site of particulate matter was divided into three C. Laboratory and Computational Analyses
categories namely commercial, industrial and residential area. The Shimadzu AX200 analytical balance with 0.1 mg
Two locations in the city center (Site 1 and Site 2) have been accuracy was used to obtain the gravimetric analysis of the
selected for the commercial area type. One spot in industrial sampled filter mass. The concentration of particulate matter
area (Site 3) has been taken for the second category. Two sites [16] measured by the vacuum air pump sampler is given by:
have been chosen in residential areas; one is in university
campus (Site 4) and the other one is in the newly-developed (2)
village (Site 5). These three categories have different vehicle
traffic and local weather condition as well as pedestrian and where,
vegetation density. Study sites in the city center have the C = particulate concentration (mass/volume);
highly narrow and congested traffic lane with more in high m = net mass collected in the filter (mass);
storey buildings, but less green space. Q = volumetric flow rate of the sampler (volume/time);
T = duration of sampling (time).
B. Sampling Procedures
Particulate matter collected by the sampler is considered as
Euroclean XForce vacuum air pump manufactured by total suspended particles, because no specific attempt was
Aquamall Water Solutions Ltd. was used for the collection of taken to separate the sampled particles in different size
particulate matter. The sampler contains one inlet and outlet categories. Relations between PM concentrations and other
with two types of exchangeable filters (bag filter and screen factors like weather parameters, traffic flows and vehicular
filter). The vacuum pump allows the admission of ambient air PM emissions were analyzed statistically using SPSS version
containing different size of particles with an adjusted flow rate 16.0 and Data Analysis Tool from Microsoft Excel 2007.
of 25 L/min. The sampling was carried out exactly on the Particle size distribution was determined by using dynamic
roadside and in the daytime – about five to six hours per day – light scattering (DLS) method. The technique measures the
when traffic density was relatively high. PM entrapped in the random changes in the intensity of light scattered from a liquid
filters was taken out thoroughly for further analyses. Filter suspension [10]. The samples were dispersed in a liquid and
fibers were removed carefully from the samples to avoid any vortexed to provide a homogeneous solution before transferred
misinterpretation in the analysis of photomicrographical to the DLS instrument. The instrument employed in this work
images and PM elemental composition. is NanotracWaveTM developed by Microtrac, USA.
Outdoor temperature, pressure, humidity, heat index, and A scanning electron microscope (SEM) was used to capture
wind speed were recorded using AcuRite® weather center the image of PM samples. It can obtain information about
model 00615 designed by Chaney Instrument Co. The surface topography, morphology, and volume-size distribution
instrument consists of a sensor and a digital display unit; both of particles [9]. In this work, the high definition Zeiss EVO
are connected using wireless transmission signal that can be LS15 SEM from Germany was employed. SEM produces
monitored in a range up to 330 feet. A sensor containing pseudo-color images that can be saved in digital format and
anemometer was placed on the top of the building to avoid any processed in a computer to adjust their contrast and brightness
obstruction when measuring wind speed. Daily average values and to quantify their size and circularity. The circularity, also
for each weather parameter were measured. known as degree of roundness, is dimensionless. It represents
Road traffic survey has been performed to analyze traffic the shape or form factor of particles [11] and is defined as:
condition at different study areas. Vehicles were classified into
six groups namely two-wheelers (2W), three-wheelers (3W),
(3)
four-wheelers (4W), buses, light commercial vehicles (LCV),
and heavy commercial vehicles (HCV). Each category has
different emission factor depends on type of vehicles, engine By using this formula, a perfectly rounded particle sphere
cylinder volume, vintage, and fuel technology used [15]. should have circularity value of 1. Liquid droplets or aerosols
Emission factors calculated in the previous work [13] are used are almost nearly spherical. More irregular shape will have
in this study. PM2.5 and PM10 emissions are estimated value lesser than that. Scientists use the term „equivalent or
mathematically by the following equation: aerodynamic diameter‟ to characterize the irregular particles.
In this study, length, area, and perimeter of PM were measured
∑ ( ) (1) by employing specific image processing software (Digimizer
version 4.6.0 from MedCalc) before exported to Microsoft
where,
Excel to calculate their size distribution and circularity values.
subscript i represent the study site and subscript j is the
Elemental composition of PM was investigated using
respective vehicle category;
Energy Dispersive X-Ray (EDX) analysis. The instrument
Ei = emission of PM2.5 or PM10, in study site i (g·h–1);
model used is NORAN System 7 X-ray Microanalysis well-
Nj = number of vehicles in category j (h–1);
developed by Thermo Scientific, USA. The data generated by
fj = emission factor of vehicle category j (g·km–1);
EDX machine consists of spectra showing peaks that
di = distance of road segment in study site i (km).
correspond to the specific elements [9]. The higher the peak,
the more abundant the element presents in the sample.

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11th Int'l Conference on Chemical, Agricultural, Biological, Healthcare & Environmental Sciences (CABHES-2017) Aug. 12-14, 2017 Batam (Indonesia)

TABLE I
DESCRIPTIVE STATISTICS OF PM CONCENTRATIONS AND WEATHER CONDITION AT FIVE SAMPLING POINTS
Sampling Concentration Temperature Pressure Humidity Heat Index Wind Speed
Site μg/m3 C kPa % C kph
1 6464 32.09  0.58 1.0110  0.0003 23.82  1.11 30.55  0.45 3.73  0.52
2 2954 30.82  0.35 1.0107  0.0003 18.73  0.97 29.18  0.30 5.91  0.44
3 1808 29.73  0.51 1.0103  0.0004 22.09  0.94 28.36  0.36 10.27  0.80
4 1674 30.62  0.40 1.0117  0.0002 42.00  0.95 30.92  0.35 5.08  0.46
5 1322 29.22  1.10 1.0114  0.0005 31.11  4.24 29.57  0.37 3.56  0.84
All weather condition values are mean  SE

III. RESULTS AND DISCUSSION concentration of ambient particulates. Industrial area with low
traffic flow compared to commercial area still has adequate
A. PM Concentrations and Weather Condition
particle concentration, because of high number of diesel-
Gravimetric analysis of the sampled particles found that fueled vehicles (HCV) that have high emission factors as well
ambient air in Site 1 located in commercial area has the as receive of non-vehicular particles emitted by industrial
highest PM concentration (Table I). The concentration was smoke stacks of neighboring metal and rubber manufacturing
about three times of Site 2 located in the same area type. This industries located not too far from the sampling site.
is due to the sampling location of Site 2 is around the road
circle and has more spacey area than of Site 1. Roadway in TABLE II
Site 2 is about ten meters in width, whereas in Site 1 is only TRAFFIC CONDITION AND HOURLY EMISSIONS OF PM2.5 AND PM10
six meters. Wider space gives more possibility to the Study site i 1 2 3 4 5
dispersion of particles to the atmosphere hence reduces the Traffic flow per hour
concentration. Ambient air in industrial and residential areas 2W 2475 2072 224 188 12
was found to have quite similar concentrations of particulate 3W 794 601 4 1 1
matter, even though the composition might be different. 4W 464 244 25 12 3
It is noted that using statistical data analysis, almost no Bus 73 4 1 0 0
significant correlation was found between any weather LCV 59 67 25 1 1
condition variable and PM concentration for this study, except HCV 3 4 11 1 0
for outdoor temperature. The outdoor temperature may Total Nj 3868 2992 290 203 17
influence ambient PM concentration as they considerably PM2.5 emissions (g/h)
correlated (r = 0.9, p< 0.05; 4 d.f). The relation may be due to 2W 142.02 37.79 13.87 3.57 0.09
3W 89.92 21.64 0.49 0.04 0.01
less vegetation in commercial area resulting less shaded area
4W 42.04 7.03 2.45 0.36 0.03
and higher outdoor temperature. Less vegetation cover also
Bus 85.21 1.48 1.26 0.00 0.00
minimizes the possibility to trap ambient particulates by
LCV 29.58 10.68 13.53 0.17 0.06
leaves stomata. Moreover, commercial area usually has higher HCV 4.96 2.10 19.63 0.55 0.00
traffic volume. Ambient temperature in high traffic area is Total Ei 393.72 80.72 51.23 4.68 0.20
higher due to heat resulted from vehicles‟ engine smokes. PM10 emissions (g/h)
B. PM Concentrations and Road Traffic Condition 2W 310.19 82.55 30.30 7.80 0.19
3W 225.40 54.23 1.23 0.09 0.04
Number of vehicles in urban roadways is presented in Table
4W 122.61 20.50 7.13 1.05 0.10
II. Although two-wheelers have the least emission factor
Bus 62.39 1.09 0.92 0.00 0.00
compared to other vehicle categories, but because of their
LCV 21.29 7.69 9.74 0.12 0.05
significant numbers in urban roadways, they contribute more HCV 2.16 0.92 8.55 0.24 0.00
to the particulate emissions in almost all study sites. Due to Total Ei 744.05 166.97 57.88 9.30 0.37
high traffic density, Site 1 received the largest particle PM2.5/PM10 0.53 0.48 0.89 0.50 0.54
emissions from urban vehicles. On the contrary, motor
vehicles were found less in residential areas; therefore the Linear regression analysis found that ambient PM
areas received lesser PM emissions. PM2.5/PM10 ratios are concentrations measured experimentally by air sampler are
almost nearly half in all sampling sites, except in industrial significantly correlated with PM emissions emitted by motor
area that measured about 0.89. It is because most of the study vehicles, either PM2.5 or PM10. High amount of PM2.5
areas are located in urban sites. These ratios are quite relevant emissions will increase ambient PM concentrations (r = 0.99,
to the studies reported by the scientists elsewhere [5]. 99% CI from 6.7 to 18.8 g/h, p< 0.005; 4 d.f). Similarly,
Considerable correlation was found between PM increase in PM10 emissions will also affect to the high amount
concentration and site traffic flow (r = 0.897, p< 0.05; 4 d.f). of ambient PM concentrations (r = 0.996, 99% CI from 4.6 to
Commercial areas located in the city centre with high traffic 8.8 g/h, p< 0.0005; 4 d.f). It clearly explains that ambient
flows have larger PM concentrations. Conversely, Site 4 and 5 particulates presented in urban roadways are mostly generated
located in residential area were found to have less from vehicles‟ tail end pipe emissions.

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11th Int'l Conference on Chemical, Agricultural, Biological, Healthcare & Environmental Sciences (CABHES-2017) Aug. 12-14, 2017 Batam (Indonesia)

C. Particle Size Distribution abundant in the analysis because most of the compounds
DLS analysis found that only 0.12% of sampled particles usually require one or more oxygen atoms to form anions or as
have aerodynamic diameter above 2,500 nm or in the size of electron receptors on their chemical structures.
PM10 (coarse particles). It means that the remaining 99.88%
have diameter less than 2.5 μm or in the category of fine 35

particles (PM2.5). Peak summary also reported that 97.4% of 30


the total sample volume contains particles with an average
25
diameter of 275.8 nm. The remaining 2.6% has an average

% Distribution
diameter of 1,505 nm. Moreover, the instrument recorded (i) 20
maximum number of particles in the sample container has a
15
mean diameter of 318 nm, (ii) maximum area of scattered
particles has diameter of 1,010 nm, and (iii) maximum volume 10
of suspended particles has an average diameter of 1,728 nm. 5
All results explain that most of the sampled particles were in
the range of PM2.5. Ratio between PM2.5 and PM10 in DLS 0
<0.5 <1 <1.5 <2 <2.5 <3 <3.5 <4 <4.5 <5 <5.5 <6 <6.5 <7
analysis might be different with ratios reported by Table II,
because here ratio is based on particle number, not on weight. Diameter (mm)

D.SEM Image Interpretation Fig. 1 Size distribution of particles analyzed from SEM image
Computational graphic analysis of SEM digital images has 35
generated particle size distribution (Fig. 1) and circularity
30
values of the particles (Fig. 2). According to the result, the
mean size of the particles is 1.66 μm. They were distributed in 25
% Distribution
a variety of size, but majority (83%) of roadway PM is belong
20
to the PM2.5 category, even though 17% of them has diameter
above 2.5 microns (PM10), but due to resolution constraint, 15
image of tiny particles size below 0.5 microns should be more 10
than they have identified in the analysis.
The shape of particles was found close to circular; even 5

they were not exactly spherical. Majority of particles have 0


circularity values up to 0.85 (31%) and 0.8 (27%). However, <0.5 <0.55 <0.6 <0.65 <0.7 <0.75 <0.8 <0.85 <0.9 <0.95 <1
the result could be different if using higher magnification or Circularity value
better contrast images and considering not only large size
particles for shape evaluation [11]. High difficulty was found Fig. 2 Classification data for the circularity of particulate matter
when digitizing smaller objects or random stack of particles. 70
Better analysis would be achieved if the particles are well-
dispersed in a very thin and spacey area while taking 60 56.38
photomicrograph by the electron microscope. Moreover,
50
presence of non-particulate objects like filter fibers, somehow,
obstructed the computational image analysis [9].
Weight %

40
33.66
E. Elemental Composition 30
EDX reading shows that urban roadway particles comprised
20
elements mostly in the form of carbon (above 50%) and
oxygen (above 30%). Other elements were found in smaller 10
fraction such as silicon, iron, aluminium, calcium, sodium, and 3.39 1.97
0.99 1.59 0.56 1.46
potassium; each below 4% in weight (Fig. 3). 0
In nature, particles may present in the form of single C O Na Al Si K Ca Fe

elements or chemical compounds. The only disadvantage of Fig. 3 Weight percentage of elements present in particulate matter
EDX is the unavailability data about which compound that
may compose the particulate matter [9]. The result obtained Chemical compounds that may constitute the particulate
from the instrument only provides elementary basis. In the matter are estimated based on their metal or metalloid cations.
sampled particles, single elements may be found in the form of For example, iron may be assigned as rust (FeO or Fe2O3);
elemental carbon, iron, aluminium, sulfur, etc., whereas aluminium as alumina (Al2O3); calcium as lime (CaO, CaCO3,
compounds are combination of different elements that can be Ca(OH)2) or gypsum (CaSO4); sodium and potassium both as
identified as C-rich, Fe-rich, Si-rich, Al-rich, S-rich, Ca-rich, sea salts (NaCl and KCl, respectively); or other possible forms
K-rich, or other metal-rich particles [12]. Oxygen element is of compound like oxides, hydroxides, chlorides, carbonates,

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11th Int'l Conference on Chemical, Agricultural, Biological, Healthcare & Environmental Sciences (CABHES-2017) Aug. 12-14, 2017 Batam (Indonesia)

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particle samples. Therefore, there is still a need for further About Authors:
study in comparing the results with data in rural or sub-urban
sites where traffic pollution is less or in other sites where Azis Kemal Fauzie is government staff in
various types of natural and industrial emissions may occur. Environment Management Board, Karawang
Regecy, Indonesia. He is now pursuing Ph.D.
research program in the Department of Studies
ACKNOWLEDGMENT in Environmental Sciences, University of
Authors thank to the Institute of Excellence (IOE), Mysore, India.
University of Mysore, India and Yale Tropical Research
Institute, USA for the laboratory and instrumentation supports. G. V. Venkataramana is Assistant Professor in
the Department of Studies in Environmental
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