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ABSTRACT
To determine the chemical compositions and source identification of PM2.5 and PM2.5–10 fractions, airborne particulate
matter (PM) samples were collected from May, 2011 through April, 2012 at three sites: up and downwind and within a
scrap iron and steel smelting industry, Ife–Ibadan highway, south western Nigeria. Samples of PM2.5 (fine) and PM2.5–10
(coarse) were collected on Nuclepore polycarbonate filters using a low volume GENT sampler equipped with a stacked
filter unit (SFU). A total of 200 samples were collected (100 of each fraction). The mass concentration of the sampled
3 3
fine and coarse PM fraction ranged between 14.4–986.5 μg/m and 11.2–3 250 μg/m , respectively. These values
3 3
exceed the permissible daily limit (NAAQS) of 35 μg/m for PM2.5 and 150 μg/m for PM10. The samples were analyzed
for black carbon (BC) using an optical transmissometer and for elemental concentrations using X–Ray Fluorescence
(XRF). The size–resolved data sets were analyzed using Positive Matrix Factorization (PMF) to identify possible sources Corresponding Author:
and estimate the contribution of these sources to the fine and coarse PM mass concentrations. Four source categories,
providing stable profiles, were identified for both fine and coarse fractions. The identified sources and their
Philip K. Hopke
: +1‐315‐268‐3861
contributions for the fine fraction are coking coal (83%), soil (10%), metallurgical industry (6%), and electronic waste
: +1‐315‐268‐6610
processing (1%). For the coarse fraction, the identified sources are metallurgical production plus electronic waste
: phopke@clarkson.edu
(53%), suspended input materials (28%), soil (18%), and galvanized steel scrap with cadmium (1%). Conditional
probability function (CPF) identified the local sources for both the fine and coarse PM samples. This work presents the
first known major use of PMF in Nigeria for source identification in particulate matter (PM) studies. Article History:
Received: 31 May 2014
Keywords: Iron–smelter, Nigeria, black carbon, XRF, PMF, CPF, source apportionment Revised: 31 July 2014
Accepted: 31 July 2014
doi: 10.5094/APR.2015.013
1. Introduction except in the last ten years when iron smelting industries began to
spring up. Iron and steel scrap recycling has been of double
There has been remarkable industrial development in Nigeria advantage to Nigeria in terms of its contribution to secondary steel
over the past two decades resulting in the establishment of many smelting. The scrap is both a raw material source and a waste
cottage industries. This rapid rate of industrialization has not been management method by handling materials that would otherwise
matched with proper planning for the control of environmental have constituted various forms of environmental hazards. The
pollution that is usually associated with such industrial develop‐ production process is a recycling process. It involves melting of the
ment (Adejumo et al., 1994). Previous studies in Nigeria focused on scrap metals at very high temperatures, in the range of 1 200–
the pollutant concentrations in the ambient air (Akeredolu, 1989; 1 700 °C. A prominent source of PM in the production process is
Ogunsola et al., 1995; Obiajunwa et al., 2002) with a knowledge the introduction of additives. A major additive is coke while
gap on the variations in the emission of pollutants from various limestone, soda ash, fluorspar, calcium carbide are also included to
production processes. separate impurities from the molten iron and enhance its strength
(U.S. EPA, 1995).
To design effective reduction strategies for particulate matter
(PM), major sources and their contributions need to be understood The high demand for iron rods and the availability of scrap
(Gu et al., 2011). Source apportionment methods have been metals have been the major drivers for the growth of secondary
developed for this purpose. Positive Matrix Factorization (PMF) iron and steel smelters in Nigeria. This rapid growth has not been
(Paatero, 1997; Kim et al., 2006; Oh et al., 2011) is a powerful and matched with the required strict regulations for environmental and
widely used multivariate method that can resolve the dominant personnel protection. Most of these industries are yet to invest in
source types without a priori knowledge of the sources (Begum et facilities necessary for improving their production processes. These
al., 2010; Cohen et al., 2010; Mooibroek et al., 2011). PMF can industries also lack installed control devices on their production
provide not only the source profiles but also the time series of processes as should be required.
source contributions.
Emissions, which include a range of air pollutants associated
Nigeria has a large capacity for industrial and other economic with the iron smelter production processes has remained a great
activities. Nigerian economy has been majorly dependent on oil concern (Brook et al., 2004; Pope and Dockery, 2006; Zhang et al.,
© Author(s) 2015. This work is distributed under the Creative Commons Attribution 3.0 License.
Owoade et al. – Atmospheric Pollution Research (APR) x
2009; Tai et al., 2010). Each stage of production in steelmaking, As, Cd and Cr, even at trace amounts, are toxic. This has been
using Electric–Arc Furnace (EAF), contributes to the emission of reported to be constituents of particulate matter associated with
pollutants (ACMA, 1999). The pollutants of primary concern are the iron and steel production (Cohen et al., 2004). This study focuses
PM2.5 and PM2.5–10 fractions of the particulate matter (Rickun, on the nature of emissions from a production facility that converts
1993) that is generated at virtually every stage of the production scrap materials into steel products.
process. Given the wide range of pollutants associated with the
production process, there is need to quantify the emission sources 2. Sampling and Data Pretreatment
and their potential impacts on the ambient air concentrations of
the pollutants and human health (Dockery et al., 1993; Brunekreef 2.1. Particulate sampling
and Forsberg, 2005; Katsouyanni, 2005).
After a preliminary assessment of the diurnal and seasonal
Among the PM species emitted from iron and steel production variation of wind direction and speed in the study site, a PM
processes are organic carbon (OC), black carbon (BC), heavy and monitoring sampling point was established near the steel
trace metals, which constitute a major, sometimes dominant, production process within the steel industry (Figure 1). After three
fraction of atmospheric particulate matter. Black carbon is the months of sampling at the point, the sampler was moved to 300 m
principal light–absorbing species in the atmosphere, playing an from the vicinity of the factory to assess the spatial variation of
important role in the aerosol climatic forcing and visibility mass and elemental concentration. A second sampler was
degradation (Tegen et al., 1997; Malm et al., 2000; Jacobson, 2001; deployed in the up and downwind direction, i.e. westerly and
Bond et al., 2013). BC has also been found to contribute large northerly, respectively (Outside – M1 and Outside – M2) based on
fractions to the fine particulate mass (Chow et al., 1996; 8 months of wind direction measurements. Figure 1 shows the
Kirchstetter et al., 1999; Begum et al., 2011). Heavy metals such as map of Nigeria indicating the sampling location.
Figure 1. Maps of study region (upper panel) Nigeria with sampling locations (lower panel).
Owoade et al. – Atmospheric Pollution Research (APR) x
Samples of fine (PM2.5) and coarse (PM2.5–10) airborne partic‐ where, is the number of occurrences of fractional contribution
ulate matter were collected on nuclepore polycarbonate filters exceeding a threshold (e.g., those ranking top up in the total time
using the low–volume GENT Stacked Filter Unit (SFU) samplers series) in direction sector, i and is the total number of wind
with the average flow rate of 15–16 L/min (Maenhaut et al., 1994;
direction occurrences in this sector. The fractional source contri‐
Hopke et al., 1997). The filter holder was placed at the height of
about 1.6 m above the ground. A total of 100 samples were bution is used instead of the original source contribution to avoid
obtained for each of the particulate fractions over the two dry and the influence of atmospheric dilution. In order to ensure statistical
wet seasons. A micrometeorological station at the sampling site reliability, a threshold for the minimal number of wind direction
was operated by the Nigeria Micrometeorological Experiment occurrences in each sector, nt is needed. If <nt, the correspon‐
(NIMEX), Atmospheric Physics unit, Department of Physics and ding CPFi was set to zero. Winds with the speeds below a
Engineering Physics, Obafemi Awolowo University, Ile–Ife. The threshold, wt, were excluded from analysis. The sources are
iron–smelting plant is situated along the Ife–Ibadan busy highway, thought to be located in the direction sectors with high CPF values.
south–western Nigeria. The steel plant occupies a total of 15 It should be noted that CPF is not suitable for distant sources since
hectares of land and is about 5 km away from the University
air particles may travel through circuitous pathways. In this study,
campus in the northeast direction.
the key parameters k, up, nt, and wt, were set to 32, 25%, 15 and
The filters were equilibrated at a relative humidity of between 1.0 m/s, respectively.
32 and 45% and at a temperature of between 20 and 25 °C for at
least 24 hours. They were then weighed using electric micro– 4. Results and Discussion
weighing balance (Sartorius model CP2P–F) with a minimum
resolution of 0.001 mg. After the sampling period, the filters were 4.1. Particulate matter and elemental concentrations
re–equilibrated and reweighed to provide measured mass
concentrations. The summary statistics for the PM, elemental and BC concen‐
trations are listed in Table 1, for the three sampling sites, M1 and
2.2. Chemical analysis M2 and at the production process section of the iron and steel
smelting industry. The annual average (± standard deviation) of
Before elemental concentrations in all the sampled filters particle loadings at the production processes, M1 and M2 for PM2.5
were measured using XRF, black carbon measurements were made are 300, 223, and 243 μg/m3, respectively. These are 20, 15 and 16
using a Magee Scientific Optical Transmissometer (OT21). The times higher than the annual US National Ambient Air Quality
transmitted light intensities at wavelengths of 880 and 370 nm Standard (NAAQS) of 15 μg/m3. The PM10 fractions are 681, 606,
were used to determine absorption. The manufacturer’s recom‐ and 320 μg/m3, respectively and they are 11, 10, and 5 times
mended absorption coefficients, 16.6 and 39.5 m2/g, were used for higher than NAAQS of 60 μg/m3, respectively. During the sampling
880–nm and 370–nm channels, respectively. Black carbon was period, the daily PM2.5 and PM10 also exceeded the NAAQS 24 h
then estimated for each filter in μg/m .
3 standard of 35 and 150 μg/m3, respectively, for some sampling
days.
Samples were analyzed for elemental concentrations using
energy dispersive x–ray fluorescence (Spectro–X–Lab2000) (Raman Also, PM10 and PM2.5 mass concentrations in both rainy and
et al., 2008). The following elements were detected, quantified and dry seasons for the three sampling sites are shown in Table 3. The
average values reported: Na, Mg, Al, Si, S, Cl, K, Ca, Sc, Ti, V, Cr, concentrations of PM10 at the three sites exceed the National
Mn, Fe, Co, Ni, Cu, Zn, Ga, As, Br, Rb, Sr, Cd, Sn, Sm, Pb and Bi. Ambient Air Quality Standard of 150 µg/m3. The average concen‐
trations of PM10 in the rainy season (M1 and M2 sites) were 363
3
3. Data Analysis and 393 µg/m . The values were lower than those of 765 and
3
446 µg/m respectively for the dry season. Sampling was not
3.1. PMF Model carried out at the production site during the dry season because
one of the samplers was not available. A p–value of 0.56 (signifi‐
Source apportionment analysis was performed using EPA PMF cant at the 0.05 level) was obtained for a t–test (2–tailed) carried
v 5.0.5. The model provides a flexible modeling approach that out on the mass concentrations of the PM2.5 in both seasons. The
effectively uses the information in the data. In PMF, the data average concentrations of PM2.5 in the rainy season at the M1 and
matrix X of dimension n rows and m columns, where n and m are M2 sites were 214 and 254 µg/m3. These were not significantly
the number of samples and species, respectively, can be factorized different from that of dry season of 227 and 238 µg/m3, respect‐
into matrices, namely G(n X p) and F(p X m), where p represents ively. The concentrations of PM2.5 in the rainy season exceed the
the number of factors extracted (Paatero et al., 2014). US EPA, (2014) limit of 35 µg/m3 by 6–7 times. These results
indicate high level of airborne particulate pollution contribution by
The solution to the PMF problem depends on estimating the smelter. The ratio of PM2.5/PM10 from the three sampling sites
uncertainties for each of the data values used in the PMF analysis. of 0.44, 0.59 and 0.65 for the rainy season and 0.30 and 0.53 for
The approach of Polissar et al. (1998) has been used to estimate the dry season indicated that fine particles, PM2.5 accounted for
the concentration values and their associated error estimates. above half of the inhalable particles.
3.2. Conditional Probability Function (CPF) Mean elemental concentrations of PM2.5 and PM2.5–10 in the
three sampling sites in Table 1 shows 28 elemental species and BC
The conditional probability function model (Ashbaugh et al., were detected and quantified and that most species concentration
1985; Zhou et al., 2004) is a method used to locate the sources and at production site was higher than at M1 and M2, this might be as
investigate the wind direction effects on each source. The wind a result of high level of contribution by the smelter. The mean
direction range was divided into 32 sectors of 11.25° each. The CPF concentrations range of heavy metals: V, Cr, Mn, Ni, As, Cd and Pb
for each sector is defined as: were shown in Table 2. Using US Environmental Protection Agency
(U.S. EPA, 2014), European Commission Air Quality Standards (EC,
2014) and WHO (2000) guidelines as shown in Table 2, for most of
(1) the sampling periods, there is an index of heavy metals emission by
the industry.
Owoade et al. – Atmospheric Pollution Research (APR) x
3
Table 1. Mean concentrations and standard deviations for the collected samples (µg/m )
PM2.5 PM2.5–10
% %
Mean±SD Mean±SD Mean±SD Mean±SD Mean±SD Mean±SD
Samples Samples
Production Site Outside M1 Site Outside M2 Site Production Site Outside M1 Site Outside M2 Site
>MDL >MDL
Mass 100 300±308 222.7±224.9 242.8±230.5 100 381±456 383±588 177±137
Na 100 45±52 23±20 29±33 100 31±42 33±53 13±12
Mg 80 0.17±0.24 0.29±0.68 0.25±0.38 92.3 0.22±0.20 0.48±0.89 0.18±0.17
Al 98 0.51±0.71 2.6±7.8 2±3 100 2.8±5.8 8±16 3.6±3.8
Si 92 1.29±2.39 5.6±18.1 5±8 97.8 5.8±6.4 15±33 5±7
S 100 2.57±2.14 1.3±1.1 1.3±1.4 100 2.7±2.1 1.40±1.17 1.10±0.63
Cl 100 17±18 7.2±6.0 9±10 100 15±14 10±13 5±4
K 100 1.4±1.3 1.6±3.2 1.7±1.8 100 2.3±2.9 3.80±6.49 1.5±1.1
Ca 100 0.24±0.27 0.72±2.12 0.64±1.23 100 2.5±4.5 2.91±5.79 0.97±0.95
Sc 70 0.004±0.003 0.0022±0.0016 0.0024±0.0033 57.2 0.0037±0.0048 0.0031±0.0054 0.0015±0.0008
Ti 100 0.056±0.082 0.23±0.65 0.19±0.29 100 0.45±0.70 0.86±1.67 0.34±0.41
V 72.2 0.003±0.003 0.0018±0.0026 0.0020±0.0026 69.3 0.0077±0.011 0.008±0.012 0.0028±0.0018
Cr 95.6 0.011±0.014 0.0078±0.0138 0.0081±0.0094 100 0.071±0.106 0.038±0.046 0.025±0.035
Mn 100 0.31±0.39 0.16±0.21 0.20±0.23 100 0.61±0.67 0.71±0.89 0.38±0.43
Fe 100 3±4 3.3±7.8 3.3±4.6 100 11±11 15.7±27.2 6±5
Co 72.2 0.021±0.023 0.018±0.020 0.025±0.038 80.2 0.10±0.16 0.09±0.17 0.029±0.019
Ni 98.9 0.078±0.089 0.045±0.040 0.057±0.069 98.9 0.16±0.21 0.13±0.21 0.051±0.039
Cu 91.1 0.088±0.091 0.036±0.032 0.050±0.054 96.7 0.15±0.19 0.10±0.16 0.041±0.035
Zn 100 58±63 31.1±29.6 42±50 100 119±170 94±164 35±30
Ga 81.1 0.065±0.063 0.030±0.027 0.031±0.028 85.7 0.06±0.074 0.03±0.04 0.016±0.015
As 98.9 0.47±0.45 0.20±0.17 0.24±0.25 100 0.63±0.83 0.36±0.53 0.17±0.12
Br 98.9 0.47±0.50 0.18±0.21 0.26±0.31 100 0.64±1.16 0.40±0.75 0.17±0.13
Rb 94.4 0.018±0.021 0.012±0.019 0.015±0.016 96.7 0.032±0.036 0.04±0.06 0.014±0.010
Sr 92.2 0.009±0.009 0.012±0.026 0.012±0.018 96.7 0.028±0.046 0.037±0.069 0.013±0.012
Cd 66.7 0.20±0.24 0.093±0.072 0.12±0.14 50 0.24±0.65 0.14±0.26 0.070±0.074
Sn 74.5 0.47±0.43 0.29±0.19 0.29±0.32 78.1 0.67±1.42 0.62±1.28 0.20±0.22
Sm 90 0.0089±0.0075 0.0052±0.0046 0.0067±0.0057 90 0.050±0.057 0.017±0.019 0.0091±0.0096
Pb 98.9 6±6 2.4±2.4 3.3±3.7 100 8.7±12.0 5.3±8.9 2.05±1.64
Bi 71.1 0.029±0.032 0.016±0.017 0.019±0.019 57.1 0.025±0.039 0.017±0.030 0.007±0.006
BC 100 1.02±0.91 0.56±0.49 0.61±0.60 100 0.59±0.57 0.48±0.61 0.20±0.12
Delta–C 100 0.036±0.012 0.054±0.028 0.058±0.030 100 0.050±0.041 0.15±0.14 0.10±0.08
Table 2. Comparison of levels of some species concentrations with USEPA, and interpretation of each model run, the optimum number of
3
EU, and WHO guidelines (µg/m ) for PM2.5 factors was chosen based on the most physically reasonable result
and adequate fit of the model to original data for both PM2.5 and
Toxic Elements This Study USEPA EU WHO
PM2.5–10. The optimal factor number chosen was four for both
V 0.001–0.003 1.0 PM2.5 and PM2.5–10 samples. The relatively limited number of
Cr 0.008–0.011 0.000025
b identifiable factors is the result of the very high impact of the scrap
Mn 0.16–0.30 0.15
iron and steel production facility, given its level of emissions and
the proximity of the samplers to the source. A video showing the
Ni 0.045–0.078 0.02 0.0025 dispersion of the plume in the vicinity of the plant is provided in
b
As 0.20–0.47 0.006 0.00066 the Supporting Material (SM). The FPEAK parameter was varied
Cd 0.09–0.20 0.005 0.005 from –0.2 to 1 to refine the source profiles (Santoso et al., 2011).
a The optimum solution was chosen to be that with FPEAK=–0.2
Pb 2.4–6.0 0.15 0.5 0.5
based on G–space edges showing no correlations among the
BC 0.56–1.02 resolved sources.
a
U.S. National Ambient Air Quality Standard (NAAQS) value as a quarterly
average not to be exceeded. Four resolved factors were assigned to each data set. The
b
For a risk of 1:1 000 000 sources were identified as coking coal, crustal/soil, metallurgical
production, and electronic waste processing for PM2.5, while for
4.2. Source apportionment PM2.5–10, the factors were assigned as metallurgical production plus
electronic waste, suspended input materials (coal plus other
PMF was run multiple times for the combined data from the process materials), crustal/soil, and galvanized steel with cadmium
three sampling sites. To obtain optimal number of sources, 4–10 emissions respectively. The profiles are displayed in Figures 2 and 3
factors were tested. The Q values, the resulting source profiles, for the fine and coarse fractions, respectively. The mean contri‐
and the scaled residuals were studied. After a thorough evaluation butions for each of the sources presented in Table 4 shows that
Owoade et al. – Atmospheric Pollution Research (APR) x
83% of the overall mass concentration of PM2.5 was attributed to galvanized steel with cadmium emission of the entire mass
coking coal, 10% to soil, 6% to metallurgical production and 1% to concentration. Figures 4 and 5 present the time series plots of the
electronic waste processing. Also for PM2.5–10, 53% of mass estimated daily contribution for each factor to both PM2.5 and
concentration was attributed to metallurgical production plus PM2.5–10 mass, while Figures 6 and 7 present the CPF plots for the
electronic waste processing, 28% to suspended input materials factors resolved by PMF for both PM2.5 and PM2.5–10, respectively.
(coal, plus other process input materials), 18% to soil and 1% to
3
Table 3. Average mass concentrations (µg/m ) of PM10 and PM2.5 with ratios of PM2.5/PM10 at different sites
Rainy Season Dry Season
Site Species
Mean±SD Min Max N Mean±SD Min Max N
PM10 684.1±613.6 28.1 2 224 18
Production PM2.5 299.7±308.2 14.4 986.5 18
PM2.5/PM10 0.44±0.50 0.51 0.44 18
PM10 363.4±200.1 87.8 753 11 765.4±808.0 167.2 3 449.8 22
Outside M1 PM2.5 214.4±192.7 41.2 632 11 226.9±243.6 23.5 975 22
PM2.5/PM10 0.59±0.96 0.47 0.83 11 0.30±0.30 0.14 0.28 22
PM10 393.0±329.7 124.1 1 016.2 11 446.2±348.9 95.1 1 183 23
Outside M2 PM2.5 253.7±247.7 34.1 712.4 11 237.9±228.1 43.9 765.5 23
PM2.5/PM10 0.65±0.75 0.27 0.7 11 0.53±0.65 0.46 0.64 23
Figure 2. PMF–derived source profiles for the PM2.5 data characterizing the iron and steel smelting industry. The bars represent the
concentrations of the various chemical species in the source profiles while the points represent the amount of explained variation
for each species.
Owoade et al. – Atmospheric Pollution Research (APR) x
Figure 3. PMF–derived source profiles for the PM2.5–10 data characterizing the iron and steel smelting industry. The bars represent
the concentrations of the various chemical species in the source profiles while the points represent the amount of explained
variation for each species.
Table 4. Mean source contribution derived from the PMF modeling for PM2.5 and PM2.5–10
PM2.5 PM2.5–10
Source 3 3
% Mass (µg/m ) % Mass (µg/m )
Soil 10.0 9.94 18.0 24.63
Suspended input materials 28.0 40.01
Galvanized scrap 1.0 1.45
Metallurgical production and electronic waste 53.0 73.97
Coking coal 83.0 87.12
Electronic waste 1.0 0.98
Metallurgy 6.0 6.40
Crustal/soil dust. Crustal elements used as tracers for soil dust except within the production facility. The emissions are deter‐
include Na, Al, Si, Ca, Ti, Mg, Fe, and Sr (Lough et al., 2005; Jaeckels mined by the rate of production as observed in the variations
et al., 2007; Begum et al., 2010; Gu et al., 2011). The crustal/soil shown in Figures 4 and 5. Similar contributions from both fine and
dust factors are dominated by high concentrations of Mg, Al, Si, K, coarse fractions of the PM are observed, particularly between the
Ca, Ti Mn, Fe, and Sr that are the major constituents of soil as months of January to March. The CPF plot in Figures 6 and 7
shown in Figures 2 and 3. Table 4 shows the factor contribution of indicate that this factor originates from within the factory. High
respective 10 and 18% of the fine and coarse PM to the total mass. contributions of coarse PM fraction to the area outside of the
The industrial area is unpaved and dust re–suspension rate is high, smelter can be attributed to road dust from within the unpaved
especially during the peak of the dry season (November to March). industrial site (Balachandran et al., 2000; Srivastava et al., 2009;
The contributions are low in the rainy season (May to October) Chelani et al., 2010).
Owoade et al. – Atmospheric Pollution Research (APR) x
Figure 4. PMF–derived source contributions plotted as a function of sampling date for the PM2.5 data characterizing the iron and
steel smelting industry.
Coking coal. This factor was found only in fine samples. The profile (Vincent and Passant, 2006; NAEI, 2011) and steel metallurgy
has high concentration of Na, Cl, Mn, Ni, Zn, As, Br, Rb, Pb and BC (Tauler et al., 2009). Cu, Mo, Fe, Se, Sb are makers for ferrous
as shown in Figure 2. The major elements used to identify coal metals industry (Kar et al., 2010) while Zn, Cu, and Mn for non–
combustion are As, Cd, Cr, Cu, Pb, Mn, Ni, K and Se (Vincent and ferrous industry (Negi et al., 1987).
Passant, 2006; NAEI, 2011). As, Zn, Cl and Se have been reported to
be good markers for coal combustion (Hien et al., 2001; Almeida et For the fine fractions, major elements identified for electronic
al., 2006; Song et al., 2006; Lee et al., 2008; Alleman et al., 2010). waste processing are Cu, Cd and Sn with high loadings of Cu while
Anthropogenically derived metals (As, Cd, and Cr; Pb and Zn) were that of only metallurgical production are S, Ca, Fe, Zn, As, Pb, BC
used as the marker elements for industrial activities. Among the and Delta–C (Figure 2). The source contributions of the metallur‐
anthropogenically–derived metals, Cd and Pb are known to be gical production and electronic waste processing sources were
emitted by high temperature coal and oil combustion process respectively 6 and 1% of the total fine PM mass (Table 4). For
(Uberol and Shadman, 1991). Most of the coal used in the coking in electronic waste processing, a major determinant of the environ‐
this industry is imported from India and has low sulfur content mental contaminants found in the e–waste depend on the type of
compared to most other coals (Bhanarkar et al., 2008; Chikkatur, items being processed and the time of manufacture (Gullett et al.,
2008). Also, from Figure 4, there is a high contribution of fine 2007; Morf et al., 2007). The major portion of the e–waste is wire
particles from the production processes. The coking coal factor that is typically copper (Bertram et al., 2002). Also, from Figure 2,
contributed 83% of the total mass of fine PM as shown in Table 5. the electronic waste processing factor has a high percentage
The CPF plot (Figures 6), confirmed that the coking coal came from contribution of Ga in addition to Cu, an indication of emissions
the production process within the smelter. from the used Si chips and LCD monitors (Ladou and Lovegrove,
2008). This mixture might occur because most of the scrap is not
Metallurgical production and electronic waste processing. The sorted. So there is varying degree of the mixture of metals such as
major elements associated with these factors are Na, Mg, K, Cu, copper, aluminum, tin, etc. Also, metallurgical production and
Mn, Fe, Zn, Ni, As, Br, Ga, Cd, Sn Pb and BC. The marker elements electronic waste processing contributions to the fine fraction
related to anthropogenic activities such as non–ferrous metal (Figure 4) observed at the Production site is expected, as a result of
industries. Cd is a tracer element for copper alloy manufacture proximity to the emissions.
Owoade et al. – Atmospheric Pollution Research (APR) x
Figure 5. PMF–derived source contributions plotted as a function of sampling date for the PM2.5–10 data characterizing the iron
and steel smelting industry.
For the coarse samples, the elements found for the combined (Song et al., 2006). This factor was found only in coarse fractions
metallurgical production and electronic waste processing sources (Figure 3) and has high factor loadings of Na, K, Si, S, Cl, Fe, Zn, As,
are K, Mn, Fe, Zn, Br, and Pb (Figure 3), while source contributions Br, Pb and BC, indicating coal, plus other process input materials
averaged 53% of total coarse sample PM mass. From Figure 5, the origin. Because of the injection into the slag of input materials such
contributions from metallurgical production/electronic waste as limestone, de–oxidants and alloying elements emissions in high
processing were relative high at the production site and M1 S, Si, Mn and other elements contained in the scrap might result
location because of the melting process in the electric arc furnaces. (Watson et al., 1998; SRI, 2002). The BC might be as a result of
There are indications that the contribution of metallurgical aerosolization of coal dust that contributed to the coarse particles.
production/electronic wastes processing was higher in the dry Figure 5 indicates a sharp increase in time series contribution in
season especially at the M1 site. The pattern may be due to May to June, 2011 at the production site and in January to
seasonal variation and meteorological factors resulting in lower February, 2012. This might be connected with the contribution
emissions in the rainy season, although sampling was not done from the combination of typical piles of input materials, like coal
simultaneously at the production and M1 sites. Similar seasonal and the kind of grinding/shredding process, which crushes the
trends in contributions have been reported in other studies (Liu et scrap to smaller pieces before melting. Also, Table 4 shows that the
al., 2005; Ogulei et al., 2005). factor contributed 28% of the coarse fraction to the total PM. The
presence of Na and Cl indicates the use of salt in the process to
Figures 6 and 7 indicated that this factor originated from remove impurities in the molten steel before casting as well as in
production processes of the smelting industry and contributed to hardening the steel after casting (Jones et al., 1998; Wayman and
both fine and coarse fractions (Begum et al., 2004; Kim et al., 2004; Juleff, 1999). The lower Cl/Na ratio of 0.32 and 0.36 respectively
Lim et al., 2010). for fine and coarse fractions are much lower than the 1.8 value
reported for sea water factors (Goldberg, 1963). This can be as a
Suspended input materials. The major elemental makers include S, result of either unusual lower concentrations of Cl or higher
Zn, As, Cu, Pb, Ni, Mn and BC (Almeida et al., 2006; Lee et al, 2008; concentrations of Na. Figure 7, shows CPF plot showing that the
Yin et al., 2010; Begum et al., 2010; Fujiwara et al., 2011). Other emissions are coming from the scrap metal smelting source.
makers include Al and Si (Bi et al., 2007; Zeng et al., 2010) and Cl
Owoade et al. – Atmospheric Pollution Research (APR) x
(a) (b)
(c) (d)
Figure 6. CPF plots for source contributions resolved by PMF for PM2.5 samples. (a) Crustal/soil, (b) metallurgical production, (c) coking coal,
(d) electronic waste processing.
Galvanized steel scrap with cadmium. This factor occurred only in et al., 2008). There was high contribution to the PM loadings from
coarse samples with the contribution of 1% of the total mass of PM the production area in July, 2011 and between the month of
(Table 4). Metal elements, such as Mg, S, Co, Cd, Sn and BC with February and April, 2012 at M1 (Figure 5), which might be an
high loading of Cd (Figure 3), identified as cadmium source is indication of increased production at that time. Figure 7 shows
attributed to industrial sources – metal manufacturing plants that the north – and easterly emissions from this industry has the
(Chandra Mouli et al., 2006). A range of tracers have been used for largest contribution to cadmium load.
the identification of this type of industrial emissions. These tracers
include Cd–copper alloy manufacture, Al and Zn production, 5. Conclusions
galvanizing, lead acid battery industry; Cr – production of Cr –
based chemicals; Cu and Pb – industrial metal, lead–acid battery; In this study, two size fractions of the airborne particulate
Mn and Ni–Al production, refineries, copper alloy manufacture matter was sampled from May, 2011 to April, 2012 at three
(Vincent and Passant, 2006). Also, there are other studies that sampling sites within and outside an iron and steel smelting
have reported other makers for industrial emissions. Begum et al. industry. The sources of both fractions have been identified using
(2004) used Ni, Pb and S, Song et al. (2006) – Ni, Cr, Fe and Mn, the USEPA’s PMF v5.0.5. The elemental and black carbon concen‐
Yatkin and Bayram (2008) – Fe, Mn, Zn, and Pb, Lestari and trations were obtained using XRF and optical transmissometer,
Mauliadi (2009) – Zn and Fe, for the steel industry, Tauler et al. respectively. The factors affecting their distributions at the industry
(2009) – Zn, Fe, Mn and Cd as tracers for steel metallurgy. These were determined from the PMF analysis. High levels of Mn, Ni, As,
elements might be emitted as a result of different unsorted scrap Cd and Pb indicated that the area within the industry is polluted
used, especially copper alloy metals, in metallic industries (Kothai and should not be neglected.
Owoade et al. – Atmospheric Pollution Research (APR) x
(a) (b)
(c) (d)
Figure 7. CPF plots for source contributions resolved by PMF for PM2.5–10 samples. (a) Soil, (b) suspended input materials, (c) metallurgical
production and electronic waste, (d) galvanized scrap.
Four sources, each, from the ambient PM2.5 and PM2.5–10 mass Acknowledgment
were identified and average contribution of each source was
estimated. For the fine fractions of the PM, these are 83% from The authors want to thank the Centre for Air Resources
coking coal, 10% for soil, 6% from metallurgical production and 1% Engineering and Science, Clarkson University, Potsdam, NY for
from electronic waste processing. For the coarse fraction, the providing all the facilities used in this work.
sources 53% from metallurgical production plus electronic waste
processing, 28% from suspended input materials emission, 18% Supporting Material Available
from soil and 1% from galvanized steel scrap with cadmium–
containing source. We conclude that coking is the major source of A video showing the dispersion of the plume in the vicinity of
fine particles while materials input handling related to the plant the iron–steel plant. This information is available free of charge via
produces the majority of the coarse particles. the internet at http://www.atmospolres.com
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