ORIGINAL PAPER

Determination of total suspended particles and the polycyclicaromatic hydrocarbons concentrations in air of selectedlocations at Kirkuk, Iraq

Moutaz A. Al-Dabbas & Lamyaa Abdulameer Ali & Adnan H. Afaj

Received: 23 September 2013 /Accepted: 26 November 2013# Saudi Society for Geosciences 2013

Abstract The mean concentrations of total suspended parti-cles in air at Kirkuk Oil Refinery and the areas around weredetermined by using low volume air sampler (Sniffer) atselected locations in two periods at October 2010 and March2011. The polycyclic aromatic hydrocarbons concentrationsin air were identified and determined as well as a part of totalsuspended particles. The results obtained from total suspendedparticles were higher in average on March period measure-ment (956.8 ppm) than on October period (818.9 ppm). Thetotal maximum concentration of polycyclic aromatic hydro-carbons in air reached 67.7 μg/m3 in October; while inMarch,it reached 145.3 μg/m3. This increment in concentrations atMarch can be referred to the increasing fuel combustionoperations at the location as well as increasing of dust stormsduring March with relatively higher wind speed that may addanother reason for the effect of meteorological factors on theair quality and on the polycyclic aromatic hydrocarbonsdistribution.

Keywords Suspended particles . Aromatic hydrocarbons .

Air pollution . Kirkuk . Iraq

Introduction

Air pollution is caused by both natural and man-made sources.Major man-made sources include automobiles, power gener-ation, and the industrial activities, which represent the mainsource of air pollution, especially oil industry activities using

huge amount of consumable fuel like power plants and oilrefineries; due the high rate emission of fume, solid particu-lates and toxic gases are more in quantity than every otherindustry. These industries will be more hazardous upon itsexistence inside the limits of the cities, or its existence insideurban area, such as Kirkuk oil refinery (Masitah et al. 2007;Afaj et al. 2008).

Suspended solid particles, which are air pollutants stuck inthe air with a small volume range between 200 and 0.01 μm(WHO 1996; Harrison 1992). Particulate matter is a mixtureof liquid droplets and small particles either organic (such asthe polycyclic aromatic hydrocarbons (PAHs)) or inorganicsubstances. The organic compounds of PAHs have a relativelylow solubility in water, but are highly lipophilic. Most of thePAHs with low vapor pressure in the air are adsorbed onparticles. In the atmosphere, PAHs can react with pollutantssuch as ozone, nitrogen oxides, and sulfur dioxide, yieldingdiones, nitro- and dinitro-PAHs, and sulfuric acids, respective-ly (Jan et al. 2000; Bari et al. 2011; Halek et al. 2006). ThePAHs are predominantly formed as a result of the incompletecombustion of organic fuels such as the burning of petroleumand oil or emissions from automobiles and industrial process-es (petrochemical industry and manufacturing of paints)(Zitka et al. 2012; Ding et al. 2007).

Many researchers had identified 16 different “priority pol-lutants” PAHs which have stronger toxicity than others(Henner et al. 1997; Shihua et al. 2001; Venkataraman et al.2002; Xie et al. 2003). Occupational Safety and HealthAssembly (OSHA) set limits of allowable PAHs in the atmo-spheric air to be 0.2 mg/m3 (WHO 1996; Husain 2003;Ministry of Environment 2008; Hashim 2009; Al-Saadi 2012).

Several researchers had carried out studies on environmen-tal air pollution (Kanbour and Yassin 1985; Afaj et al. 2000;Al- Maliki 2005; Abdel Wahid 2005; Li et al. 2010; Al-Dabbas et al. 2012), but there are very limited studies partic-ularly on the air pollution from oil industrial activities in Iraq.

M. A. Al-Dabbas (*)College of Science, University of Baghdad, Al-Jaderiya, P. O. Box:47138, Baghdad, Iraqe-mail: prof_aldabbas@yahoo.com

L. A. Ali :A. H. AfajMinistry of Science and Technology, Baghdad, Iraq

Arab J GeosciDOI 10.1007/s12517-013-1229-2

The climatic parameters such as the temperature, relativehumidity, wind speed, and rainfall have an important effect onthe concentration of pollutants in the air and lead a key role incontrolling the spread of various air pollutants (Ahrens 2005).The high temperature leads to air movements and the dissem-ination of pollutants vertically to the greatest extent possible,while the low temperature leads to downward air movements.Rain works to purify the air of a lot of solid and gaseouspollutants. Also, a large part of these particles attached to therain drops fall during the rain like dust particles. The relativehumidity percent is depending on temperature; the humiditydecrease in the summer due to high temperature and lowrainfall, while the humidity increase in winter due to lowtemperatures and frequent rainfall; so there is an inverserelationship between humidity and temperature, and directcorrelation between the humidity and rain. The importanteffect of relative humidity is shown by reducing the concen-tration of pollutants in the air. The wind direction plays animportant role in the distribution of pollutants in air, movingthe pollutants with the general direction of the prevailingwinds. When the wind speed increase, the movement andspread of contaminants increase and therefore lack of concen-tration in the air (Ahrens 2005).

The aims of this study were to analyze the climate param-eters of Kirkuk meteorological station and to measure thepollution levels in the air, for total suspended particle (TSP)and PAHs of the area in and around Kirkuk Refinery, betweenlatitudes (35′°24″–35′°29″) to the north and longitude(44′°20″–44′°26″) to the east (Fig. 1).

Materials and methods

Climate

Data of Kirkukmeteorological station and records of the climateelements were studied for the years 1980–2012, such as maxi-mum and minimum temperature (in degrees Celsius), windspeed (in meters per second), and direction, rainfall (in millime-ters), and relative humidity percent (Iraqi MeteorologicalOrganization 2012).

Site selection

The site selection of the air sampling in Kirkuk oil refinerytakes into consideration the prevailing wind direction that isan important factor in pollutants distribution, as well as thenearby populated sectors within Kirkuk city. Fifteen differentsampling sites inside and outside the refinery have beenselected for ambient air samples collection (Fig. 1). The TSPconcentration was determined by using a low-volume airsampler (Sniffer) at a rate of l/min, in two periods October2010 and March 2011. The measurements were done

according to Ali's (2013) procedure. The chemical analysisof the air samples was for measurements of the concentrationsof TSP and the PAHs in the air, and their distribution in thestudied area, using high-performance liquid chromatographyand gas chromatography mass of the polycyclic aromatichydrocarbon compounds (Husain 2003; Ali 2013). The usedstandards for polycyclic aromatic hydrocarbons analysis wereof Sigma-Aldrich Company with high purity (not less than99.5 %). A mixture of the 16 compound with a differentconcentrations for each standard material (naphthalene,acenaphthene, acenaphthylene, fluorene, phenanthrene, fluo-ranthene, chrysene, anthracene, benzo(a)anthracene,benzo(k)fluoranthene, benzo(b)fluoranthene, pyrene,dibenzo(a, h)anthracene, benzo(a)pyrene, benzo(g, h,i)perylene, indeno(1,2,3-cd)pyrene) were used (Ali 2013).

Results and discussion

Climate

Kirkuk meteorological station climatic elements for the years1980–2012 were analyzed (Table 1 and Fig. 2). These resultsreflect that the high value of mean monthly maximum tem-perature was 43.5 °C during July, and the low value was14.0 °C during January. While the high value of mean month-ly minimum temperature was 28.5 °C during July and the lowvalue was 4.8 °C during January (Fig. 2a, b). The hightemperature leads to air movements and the dissemination ofpollutants vertically to the greatest extent possible, while thelow temperature leads to downward air movements.

The high value of mean monthly rainfall was 70.9 mmduring January, while the low value was 0.1 mm duringAugust (Fig. 2c), such results are in accordance with theresults of relative humidity%; the high value of mean monthlyRH% was 73.75 % during January, while the low value was23.07%mmduring July (Fig. 2d). Rain works to purify the airof a lot of solid and gaseous pollutants. Also, a large part ofthese particles attached to the rain drops fall during the rainlike dust particles. The important effect of rainfall and relativehumidity is shown by reducing the concentration of pollutantsin the air.

The high value of mean monthly wind speed was 2.1 m/sduring June, while the low value was 1.1 m/s duringDecember and January (Fig. 2f). Moreover, the prevailingmean monthly wind directions for Kirkuk meteorologicalstation for the period (2002–2012) reflect mainly northwest-erly winds direction (Fig. 2e). The wind direction plays animportant role in the distribution of pollutants in air, movingthe pollutants with the general direction of the prevailingwinds. When the wind speed increases, the movement andspread of contaminants increase.

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Total suspended particles

The results of the average TSP concentration (Table 2) reflectthat five locations (sampling sites) have more than 1,000 μg/m3; these locations were 6, 8, 9, 11, and 15 during October2010, while during March 2011, the locations that had morethan 1,000 μg/m3 are 6, 12, 13, 14, and 15. The results alsoindicate that the highest value recorded for TSP duringOctober 2010 was for sample no. 8 that represents theEternity fire (2,371.8 μg/m3), which is due to the presenceof the gas flares of the refinery nearby. While the lowest valueduring October 2010 was for sample no. 4 that represents theChorao control site (192.3 μg/m3) as shown in Table 2 and

Fig. 3. In March 2011, the highest recorded value was forsample no. 15 that represents Baghdad transport station(3,555.6 μg/m3) due to traffic intensity at this site, while thelowest value was for samples nos. 10 and 11 that represent theCentral Isolation Unit at the refinery and the EnvironmentalDepartment of the Northern Oil Company, respectively, withvalue of 229.9 μg/m3 as shown in Table 2 and Fig. 3. Theaverage concentration of TSP were significantly higher thanthe permissible allowable limits of the Iraqi National standards(350 μg/m3) and the worlds international allowable limits(60–90 μg/m3) (Table 2) for both periods of this study,October 2010 and March 2011; the averages were 818.94and 956.8 μg/m3, respectively. The result shows randomdistribution in the studied sites and did not follow certaingeographic pattern which could be due to the effects of thedust storms and the input of other sources such as the generaluse of local generators to produce electricity. It was alsoobserved that the TSP concentrations increased at the direc-tion away from the refinery (Fig. 3), mostly at the southeastdirection that coincides with the wind direction at the studiedarea which is more correct for March rather than Octoberbecause of increasing dust storms during March with relative-ly higher wind speed that may add another reason for theeffect of the climate in the TSP distribution (Fig. 2f) (Al-Dabbas et al. 2012).

Total PAHs in air

The results of the total PAHs concentrations analysis in airshow the existence of 16 hydrocarbons in air; these are naph-thalene, acenaphthene, acenaphthylene, fluorene, phenan-threne, fluoranthene, chrysene, anthracene, benzo(a)anthracene,

Fig. 1 The topographic map of Iraq showing the site of Kirkuk governorate and the sampling locations

Table 1 The mean monthly values of the climatic parameters of KirkukMeteorological station for years 1980–2012

Months Min temp °C Max temp °C RH% Wind speedm/s

Rainfallmm

October 18.7 31.6 38.5 1.5 14.2

November 11.6 22.3 58.9 1.2 50

December 6.4 15.8 71.3 1.1 62.6

January 4.8 14.0 73.5 1.1 70.9

February 5.6 15.5 67.8 1.4 63.4

March 9.1 19.9 59.7 1.6 54.1

April 14.2 26.5 51.6 1.8 41

May 20.2 33.9 34.9 2.1 13.4

June 25.3 39.9 24.9 1.9 0.2

July 28.5 43.5 23.1 1.8 0.4

August 27.7 42.7 24.6 1.8 0.1

September 23.9 38.7 27.2 1.4 1.2

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benzo(k)fluoranthene, benzo(b)fluoranthene, pyrene,dibenzo(a, h)anthracene, benzo(a)pyrene, benzo(g, h,i)perylene, indeno(1,2,3-cd)pyrene.

The 16 EPAs priority PAHs detected in the studied areawere not all found at all sites of measurements due to theirphysicochemical properties of these compounds.

As a result, naphthalene was detected in refinery and thesites nearby due to the low molecular weight found in gas

phase compared with the compounds of high molecular weightfound in particulate phase detected in the faraway sites fromthe refinery such as benzo(b)flouranthen, benzo(k)flouranthen,benzo(a)pyrene, etc. (Fig. 4).

Most of PAHs minimum values were less than 1.0 μg/m3

during October 2010, except two of them indicate more than1.0 μg/m3 fluoranthene and dibenzo(a, h)anthracene, whilemost of their maximum values were less than 10.0, except for

Fig. 2 The mean monthly meteorological parameters of Kirkuk stationfor the years 1980–2011. a Meanmonthly maximum temperature (°C), bmean monthly minimum temperature (°C), c mean monthly rainfall

(mm), d mean monthly relative humidity %, e the rose diagram of meanmonthly wind directions for Kirkuk Meteorological Station for years(2002–2012), f mean monthly wind speed (m/s)

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naphthalene, phenanthrene, and fluorine which they had morethan 10.0 μg/m3 concentrations (Table 3). The maximumconcentration of PAHs in air during October 2010 as a totalwas 67.7 μg/m3; meanwhile, the minimum concentration was0.03 μg/m3 (Table 3).

During March 2011, most of PAHs minimum concentra-tions were less than 1.0 μg/m3 except that four of them hadconcentrations more than 1.0 μg/m3; these are naphthalene,acenaphthylene, benzo(g, h, i)perylene, and indeno(1,2,3-cd)pyrene. While half of the studied PAHs during March2011 had more than 10.0 μg/m3 maximum values; these arenaphthalene, acenaphthylene, fluoranthene, pyrene,benzo(a)anthracene, benzo(k)fluoranthene, dibenzo(a, h)an-thracene, and benzo(g, h, i)perylene. The total maximum

concentration of PAHs in air during March 2011 was145.3 μg/m3; meanwhile, the total minimum concentrationwas 0.2 μg/m3 (Table 3).

This increment in PAHs concentrations at March 2011period can be referred to the increase of fuel combustionoperations accruing at the location such as the operations ofthe power plant as well as the effect of the intensive duststorms during this period (Table 3 and Fig. 4).

Comparison of the mean values of total PAHs concentra-tions in air with the world limits as indicated by theOccupational Safety and Health Assembly set limits of allow-able PAHs in the atmospheric air to be 0.2 mg/m3 (WHO1996; Husain 2003). Generally, it is noticed that the results ofthis study are higher than this limit (Table 3). However,

Table 2 TSP concentrations(μg/m3) in the studied areacomparing with national andworld limits (WHO 1996)

Sa. no. TSP. in October (μg/m3) TSP. in March (μg/m3) The site name

1 628.9 253.2 Araffa

2 440.3 333.3 First unit ( refinery)

3 273.1 238.1 Third unit (refinery)

4 192.3 238.1 Chorao control

5 833.3 622.5 Market

6 1,635.2 2068.9 Rahim Awa

7 740.7 919.5 Gas separation unit (baba)

8 2,371.8 493.8 Eternity fire

9 1,294.5 238.1 Baba residential area

10 776.7 229.9 Central isolation unit

11 1,111.1 229.9 Environmental department

12 566 2,000 Baba Gurgur hotel

13 433.1 1,666.7 People's action area

14 317.5 1,264.4 K1 control

15 1234.6 3,555.6 Baghdad transport station

Mean 818.94 956.8

Iraqi National standards 350 μg/m3 350 μg/m3

Intern. limits WHO 1996 60–90 μg/m3 60–90 μg/m3

Fig. 3 Total suspended particles (μg/m3) distribution in air of the studied area in October 2010 and March 2011

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Lonneman et al. (1974) studied the total concentration ofPAHs in the air for selected sites within NY and New Jerseycities, and it was ranging from 3.9 to 12.7 ppb, which is inconcordance with the results of this research during October2010 analyses. While Raymond and Guiochon (1974) con-cluded that the naphthalene concentration in the air for select-ed sites within Paris was ranging from 3.8 to 11.2 μg/m3 andHusain (2003) studied the polycyclic aromatic hydrocarbonsin Iraqi environmental air samples and he gave ranges for thedifferent PAHs maximum values from 0.3 to 5.17 μg/m3, bothresults value are too low in comparison with this study results

(Table 3). The same is true comparing with Shihab Aldin andAziz (2013) as they studied the PAHs concentrations in dustsamples of selected locations at Basra City, Iraq.

Dispersion modeling of PAHs in air

The dispersion models of PAHs in air is a numerical tool usedby researchers to describe the causal relationship betweenemissions, meteorology, atmospheric concentrations, deposi-tion, and other factors (Leili et al. 2008; Al- Maliky 2006;Matejicek 2005). In this study, the Geographic Information

Fig. 4 Total PAHs (μg/m3) distribution in air of the studied area in October 2010 and March 2011

Table 3 Total polycyclic aromatic hydrocarbons (PAHs) concentrations (μg/m3) analysis in air of the studied area in October 2010 and March2011,comparing with results of Husain (2003) in air samples of Baghdad City and Shihab Aldin and Aziz (2013) in dust samples at Basra City

No. PAHs October 2010 March 2011 Husain (2003) Shihab Aldin & Aziz (2013)

Min Max Mean Min Max Mean Max. in air Max. in dust

1. Naphthalene NAP 0.4 34.9 10.72 75.9 112.2 95.7 0.3

2. Acenaphthylene ACY 0.0 0.4 – 1.3 109.5 37.5

3. Acenaphthene ACE 0.7 1.75 1.1 0.0 0.0 0.0 5.17

4. Fluorine FLU 0.01 10.1 3.6 0.0 2.8 – 0.3 0.8

5. Phenanthrene PHE 0.01 30.3 8.24 0.0 0.0 0.0 1.53

6. Anthracene ANT 0.01 0.035 0.024 0.15 0.18 0.17

7. Fluoranthene FLUA 1.5 2.1 2.0 0.3 19.2 3.4 0.48 2.2

8. Pyrene PYR 0.0 0.88 – 0.0 27.4 – 0.30 1.1

9. Benzo(a)anthracene B(a)A 0.01 0.2 0.0636 0.26 52.6 15.6 6.9

10. Chrycene CHR 0.05 0.44 0.167 0.0 0.76 – 0.72 7.0

11. Benzo(b)fluoranthene B(b)F 0.03 0.14 0.0653 0.03 3.4 1.3 6.1

12. Benzo(k)fluoranthene B(k)F 0.0 0.07 – 0.16 12.4 3.9 6.0

13. Benzo(a)pyrene B(a)P 0.0 5.7 – 0.51 0.67 0.6 1.71 6.2

14. Dibenzo(ah)antracene Dib(ah)A 1.16 4.7 2.4 0.34 13.6 5.97 0.6 5.2

15. Benzo(ghi)perylene B(ghi)P 0.09 7.0 2.7 4.73 12.2 8.5 3.7 2.1

16. Indino(1,2,3-cd)pyrene Ind P 0.0 1.73 – 3.45 5.24 4.35 3.1 3.7

Total 0.03 67.7 12.5 0.2 145.3 31.2

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Systems (GIS) was applied. Arc GIS 10 modeling of mea-surements of total PAHs in air was applied for both samplingperiods of October 2010 and March 2011 (Fig. 5). The cumu-lative effects of both periods are shown in Fig. 6 that repre-sents the cumulative air model of total PAHs in air of bothperiods. The result show that the concentrations of thesepollutants increase away from the refinery toward the south-west part of the studied area (Ali 2013).

In conclusion, the results show that the effects of the refineryare the most effective factor on the distribution of these pollut-ants. The meteorological condition plays an important role tothe PAHs distribution in air especially the factor of temperatureand wind direction; therefore, the effects of seasonal changesare obviously noticed on the model made (Figs. 5 and 6).

The results of the average total suspended particles con-centration and total PAHs in air of both periods during

Fig. 5 Arc GIS model of PAHs pollutants (μg/m3) in the air of the studied area in October 2010 and March 2011

Fig. 6 Arc GIS model of totalPAHs pollutants (μg/m3) in the airof the studied area

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October 2010 and March 2011 showed a general relativeincrease toward the wind direction (the southeast direction).

It was also observed that the TSP concentrations increasedat the direction away from the refinery (Fig. 4), mostly at thesoutheast direction. The total maximum concentration ofPAHs in air showed a relative increase in concentration duringMarch more than during October which may be referred to theincreasing fuel combustion operations at the location such asthe operations of the power plant as well as increasing of duststorms during March with relatively higher wind speed thatmay add another reason for the effect of meteorological fac-tors on the air quality and on the PAHs distribution (Figs. 5and 6) (Al-Dabbas et al. 2012).

Conclusions

1. The temperature, relative humidity, wind speed, and rain-fall have an important effect on the concentration ofpollutants in the air and lead a key role in controlling thespread of various air pollutants especially during thedifferent months of the year.

2. The average concentration of TSP in this study is higherthan the permissible limits of the Iraqi National determi-nants and the world limits; the little difference between thetwo periods reflects the little effect of the seasonal changes.

3. The results of the total PAHs concentrations analysis inair show the existence of 16 hydrocarbons in air; theseare naphthalene, acenaphthene, acenaphthylene,fluorene, phenanthrene, fluoranthene, chrysene, anthra-cene, benzo(a)anthracene, benzo(k)fluoranthene,benzo(b)fluoranthene, pyrene, dibenzo(a, h)anthracene,benzo(a)pyrene, benzo(g, h, i )perylene, andindeno(1,2,3-cd)pyrene.

4. The 16 EPAs priority PAHs detected in the studied areawere not all found at all sites of measurements due to theirphysicochemical properties of these compounds.

5. The concentration of PAHs in air during March 2011 wasrather higher than during October 2010 which may be dueto the increase of fuel combustion operations as well asincreasing of dust storms during March with relativelyhigher wind speed and relatively low temperature thatmay add another reason for the effect of the climate inthe PAHs distribution (Fig. 2).

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