Polycyclic aromatic hydrocarbons (PAH) in top soil, leachate and ...

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Int. J. Environment and Pollution, Vol. x, No. x, xxxx

Polycyclic aromatic hydrocarbons (PAH) in top soil, leachate and groundwater from Ruseifa solid waste landfill, Jordan Anwar Jiries* Water and Environmental Studies Center, P.O. Box 2, Mutah University, Al-Karak, Jordan E-mail: [email protected] *Corresponding author

Omar Rimawi Faculty of Science, University of Jordan, Amman, Jordan E-mail: [email protected]

Jutta Lintelmann GSF, National Research Center for Environment and Health, D-85764, Neuherberg-Germany E-mail: [email protected]

Mufeed Batarseh Chemistry Department, Mutah University, P.O. Box 7, Al-Karak, Jordan E-mail: [email protected] Abstract: The distribution profiles and pathways of polynuclear aromatic hydrocarbons in the surroundings of Ruseifa landfill area in Jordan were investigated for surface sediments, leachate, and groundwater. The total concentration of 16 polycyclic aromatic hydrocarbons (PAHs) in sediments ranged from 286 to 1704 ppm with an average value of 751 ppm. Meanwhile, concentrations of PAH in groundwater ranged between 7.1 and 12.6 ppm with an average value of 9.1 ppm. The PAH in leachate varied between 0.10 and 0.40 with an average value of 0.29 ppm. The overall PAH distribution profiles appeared to be similar for leachate and groundwater dominated by 2–3 rings system molecules. While, the sediments profile was dominated by 4–6 rings system molecules which indicated the loss of low molecular weight compounds of PAH and accumulation of higher molecular weight of PAH under prevailing semiarid and hot climatic conditions. Keywords: PAH; landfill; Jordan; leachate; sediment; groundwater. Reference to this paper should be made as follows: Jiries, A., Rimawi, O., Lintelmann, J. and Batarseh, M. (xxxx) ‘Polycyclic aromatic hydrocarbons (PAH) in top soil, leachate and groundwater from Ruseifa solid waste landfill, Jordan’, Int. J. Environment and Pollution, Vol. x, No. x, pp.xxx–xxx.

Copyright © 200x Inderscience Enterprises Ltd.

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A. Jiries, O. Rimawi, J. Lintelmann and M. Batarseh Biographical notes: Professor Anwar Jiries is a Hydrogeologist and acting as a Director of the Water and Environment Research Centre at Mutah University, Jordan. Professor Jiries published more than 35 articles in national and International refereed journals in the fields of hydrology, water and environmental quality. Professor Omar Remawi is Hydrogologist and acting as President of Balqa Applied University, published many articles in the fields of hydrology and environment. Dr. Jutta Lintelmann has a PhD in Environmental Chemistry. Dr. Lintelmann is a Researcher at the National Research Centre for Environment and Health, Neuherberg, Germany. Dr. Mufeed Batarseh has a PhD in Environmental Chemistry and Waste Analysis. Dr. Batarseh is a Researcher and Head of Libratory Department at Water and Environment Research Centre at Mutah University, Jordan. Dr. Batarseh published several articles in the fields of environmental analytical chemistry and monitoring of organic pollutants in the environment.

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Introduction

Solid waste dumps are known to be sources of pollutants in their surroundings, especially when they are not properly handled. Accumulation of solid waste generates sufficient energy to start self-combustion. Such process produces various types of priority organic pollutants among them an important group known as polycyclic aromatic hydrocarbons (PAH). However, PAH can be generated by anthropogenic or natural combustion processes, as well as rapid in situ transformation of biogenic precursors during sediment diagenesis (Blumer, 1976; Wakeham and Farrington, 1980). This group of pollutants include potentially carcinogenic compounds such as benzo[a]pyrene (Gelboin, 1980; Denissenko et al., 1996). Consequently, these compounds are subject to various transformation processes including chemical transformation, biodegradation and photochemical degradation (Schwarzenbach et al., 1993). The distribution profiles of such organic pollutants in different environmental compartments has been found to be linearly related to the organic content and soil texture (Kukkonen and Landrum, 1996). However, low molecular weight PAH are exhausted and remobilised in the environment more easily than high molecular weight PAH (Krein and Schorer, 2000; Fu et al., 2001). Solid waste management in Jordan is still primitive. The municipal solid waste collected from the cities of Amman and Zarqa is currently disposed of at Ruseifa landfill located around 15 km north-east of Amman city (Figure 1). The landfill site was originally an abandoned phosphate mining quarry. Overall it can be stated that current landfill operations are causing environmental degradation effects at surrounding areas. At this site, the amount of collected solid waste was estimated to be around 1,200 ton/day with an average composition of 56% kitchen residue, 13% plastics, 16% papers, 1% fibres, 7% glass, 5% metals, and 2% others, respectively (Matouq, 2003).

PAH in top soil, leachate and groundwater Figure 1

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Location map and sampling site

Minimal research has been done on the solid waste disposal sites in Jordan. Jiries et al. (2000) investigated the heavy metals distribution in air and soil at Karak solid waste disposal site. The study showed that the negative impacts of the solid waste burning was limited and controlled by climatic conditions. Rimawi et al. (1999) found high nitrate concentrations in groundwater surrounding Ruseifa landfill. An elevated environmental concentrations of dioxins and furans which emitted from Ruseifa solid waste landfill were detected as consequences of the combustion processes (Alawi et al., 1996). The present work aims at evaluating the environmental impact of the solid waste burning site on surface soil and any groundwater contamination in the area using PAH as tracers. The dumping site is located above the main groundwater basin. However, no investigations were done on the contribution of organic pollutants originating from the landfill in Jordan into groundwater bodies. The present solid waste management is a typical example of the landfill management system of the many metropolitan regions in the Middle East.

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A. Jiries, O. Rimawi, J. Lintelmann and M. Batarseh

Materials and methods

2.1 Sampling The Ruseifa landfill is the largest landfill in Jordan, serving more than two million inhabitants, was selected for this study. Surface sediments, leachate, and groundwater samples were collected from the vicinity of Ruseifa landfill. Duration of sampling activities characterised by arid climatic conditions where no rain and calm wind prevailed at the end of summer season. Therefore, meteorological factors had no impact on the result of this study. Ten grab surface sediment samples (0–5 cm) were collected from different burning sites within the landfill. Leachates were collected from ponds located at different sites within the investigated area using prewashed glass jars. Four groundwater wells located around the dumping site were used for groundwater samples. The samples were stored in the dark at 4oC until analysed. The sample treatment and analysis are described in detail at the end of the paper.

2.2 Sample pretreatment Groundwater: PAH were extracted from water samples using Env. C-18 solid phase extraction columns (SPE) (Varian, USA). The SPE cartridges were conditioned with 5 ml ethyl acetate followed by 5 ml methanol and finally washed two times with 5 ml deionised water. The target compounds were enriched using SPE-apparatus at flow rate of 5 ml/min. Then, the PAH were eluted with 3 ml ethyl acetate. The elute was dried using anhydrous Na2SO4 and concentrated to 1 ml using gentle nitrogen stream. Leachate: a 50 ml of leachate sample was extracted three times successively with 50 ml dichloromethane using a separating funnel and the solvent was removed at 20°C and 14 mm mercury pressure. The residue was dissolved in 5 ml dichloromethane and cleaned up using silica gel chromatography (Batarseh et al., 2003). The analyte was rotary evaporated to dryness and dissolved in 5.5 ml acetonitrile. Surface sediments: a 1–2 g of air-dried and sieved sediment sample was weighed into a Whatmann soxhlet thimble, which has been previously rinsed with dichloromethane. The sample was extracted for three hours with dichloromethane; the extract was taken down at 20°C and reduced at 14 mm mercury pressure to dryness. Then, it was dissolved in 5 ml of acetonitrile. Finally, the same clean up procedures were applied using silica gel chromatography prior to analysis.

2.3 Analysis One ml of the extract was diluted into 5 ml with acetonitrile followed by addition of 5 ml deionised water. The mixture was shaken, allowed to stand for 30 minutes at room temperature and finally filtered through a micro filter (0.2 µm, Brown-Rim-D) obtained from Schleicher and Schuell (Dassel, Germany). Aliquots of 10 µL were injected into the HPLC.

PAH in top soil, leachate and groundwater

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A HPLC system HP series 1,100 was used consisting of a vacuum degasser, a gradient pump, an auto sampler, a column thermostat, a diode array detector, a fluorescence detector and a computer workstation (Hewlett Packard, Waldbronn, Germany). A Bakerbond PAH analytical column (250 mm, 3 mm I.D) was used (Baker, Deventer, Netherlands). The flow velocity was adjusted to 0.5 ml/min. The native fluorescence of the PAH was used for their detection and quantification. The separation gradient was used for 16 PAH at 20°C started with 53% acetonitrile for the first 20 minutes, subsequently linearity programmed to 82% acetonitrile (20–30 minutes) increased to 100% acetonitrile (30–45 minutes) finally held at 53% acetonitrile for the last 15 minutes. The time programme of wavelength pairs were 280, 246, 250, 280, 265, 284, 290, 292 and 294 nm excitation and 330, 370, 406, 450, 390, 380, 430, 420, 410 and 492 nm emission for (Nap, Ace, Fle), Phe, Ant, Fla, Pyr, (BaA & Cry), (BeP & BbF), (DahA & BghiP) and IcdP, respectively. External calibration of six-level-calibration standard solution of 16 PAH was used for quantification. A PAH standard of 100 ng/µL was obtained from Promochem (Wesel, Germany). The overall absolute recoveries of individual PAH compounds were found to be better than 78%. The presented data were corrected accordingly and obtained from the average of duplicate analysis.

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Results and discussion

The United State Environmental Agency (US-EPA) has defined 16 PAH as priority pollutants due to their potential carcinogenic characteristics. Such pollutants occurrence, behaviour, and distribution in different environmental compartments were presented as an important environmental issue in many recent research (Jiries et al., 1996; Lezzari et al., 2000; Krein and Schorer, 2000). The total concentrations of 16 PAH analysed for leachate, surface sediment, and groundwater are presented in Figure 2. The concentration levels of PAH were found to be higher for sediment samples by a factor exceeding 82 and 2590 times than for leachate and groundwater, respectively. The sum value of 16-PAH ranged over 286–1704 ± 751 ppm with an average concentration of 751 ppm for sediments, 7.1–12.6 ± 2.5 ppm with an average 9.1 ppm for leachate, and 0.10–0.40 ± 0.12 ppm with an average of 0.29 ppm for groundwater (Table 1). The differences in the PAH concentrations among the sampling compartments can be attributed to hydrophobic properties of the PAH as they interact more strongly with organic and particulate matter. PAH are more persistently bound to surface sediments (Kukkonen and Landrum, 1996; Tkalin, 1996; Zhou et al., 1998, 1999). The results of this study were in agreement with the findings of Batarseh (2003) in Zarqa River sediments where Σ PAH ranged over 93–3400 µg/kg, despite of low concentration levels were detected in the river waters.

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A. Jiries, O. Rimawi, J. Lintelmann and M. Batarseh

Figure 2

Concentration of 16 PAH for leachate, surface sediments and groundwater

Table 1

Concentration of 16 PAH in ppm for sediments, leachate and groundwater

PAH

Sediment (mg/kg)

Leachate (mg/L)

Groundwater (mg/L)

Name/ abbrev.

Min

Max

Average

Min

Max

Average

Min

Max Average

Naphthalene/NAP

28.3

295.6

117.3

1.19

4.32

2.73

0.03

0.12

0.08

Acenaphthylene/ACE

9.7

29.2

18.9

0.00

0.22

0.07

0.01

0.03

0.02

Fluorene/FLE

7.6

62.6

29.9

0.30

1.61

0.81

0.01

0.04

0.03

Phenanthrene/PHE

27.7

247.2

133.0

0.66

4.25

2.30

0.01

0.11

0.05

Anthracene/ANT

11.9

72.3

39.1

0.10

0.39

0.24

0.00

0.00

0.00

Fluoranthene/FLA

26.5

153.0

64.9

0.34

1.39

0.77

0.02

0.03

0.02

Pyrene/PYR

31.4

205.4

103.5

0.32

1.94

0.96

0.02

0.06

0.04

Benzo(a)anthracene/BaA

7.3

80.7

27.0

0.15

0.33

0.21

0.00

0.00

0.00

Chrysene/CHR

5.1

101.0

43.3

0.00

0.51

0.18

0.00

0.01

0.01

Benzo(e)pyrene/BeP

13.0

204.5

69.1

0.00

0.58

0.33

0.00

0.00

0.00

Benzo(b)fluoranthene/BbF

6.6

54.8

19.5

0.00

0.18

0.06

0.00

0.00

0.00

Benzo(k)fluoranthene/BkF

3.9

32.8

11.7

0.00

0.08

0.03

0.00

0.00

0.00

Benzo(a)pyrene/BaP

8.3

85.1

26.8

0.14

0.19

0.16

0.00

0.00

0.00

Dibenzo(a,h)anthracene/DahA

2.8

15.5

6.0

0.07

0.09

0.08

0.00

0.00

0.00

Benzo(g,h,I)perylene/BghiP

5.2

71.0

22.3

0.13

0.29

0.19

0.01

0.01

0.01

Indo(1,2,3,cd)pyrene/IcdP

3.4

61.1

19.1

0.00

0.10

0.03

0.00

0.00

0.00

Σ PAH

199

1772

751

3.4

16.4

9.2

0.1

0.4

0.26

Naphthalene and phenanthrene were the most abundant PAH existed in all samples composing 55%, 51%, and 33% for leachate, groundwater, and sediment samples, respectively. Such high concentrations of naphthalene and phenanthrene can be attributed to the low degradation under prevailing environments where these two PAH share a common metabolic pathway (Kiyohara et al., 1994). In addition, low molecular weight PAH are able to be mobilised within the liquid phases due to their relative solubility (Kukkonen and Landrum, 1996).

PAH in top soil, leachate and groundwater

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Benzo[a]pyrene (BaP), a five-ring PAH, was intensively investigated due to its high acute toxicity showed on rabbits (LD50 = 50 mg/kg) and human potent carcinogenicity (NTP, 2003). BaP is usually found in smoke and soot, combines with dust particles in air and is carried into water, soil, and crops. People may be exposed to BaP and other PAH via inhalation, ingestion, and skin contact. The concentration of BaP ranged over 0.14–0.19 ± 0.02 ppm with an average value of 0.16 ppm for leachate and 8.3–85.1 ppm ± 26.5 with an average concentration of 26.8 ppm for sediment. However, BaP was not detected in groundwater samples. In addition, pyrene is a typical product of incomplete combustion (Müller et al., 1998), existed in high concentrations with average values of 103, 0.96, and 0.04 ppm for sediment, leachate, and groundwater, respectively. These results are in agreement with other burning sites in the world such as France where high pyrene concentrations existed in waste combusted at low temperature (Besombes et al., 2000). However, previous results have reported that pyrene is also emitted in large amounts by biomass burning such as plants or wood which exists in large amount in the solid waste landfill (Masclet et al., 1995, 2000; Jenkins et al., 1996). The physical and chemical properties of PAH are responsible for their mobility and distribution in the environment. The 2–3 ring systems are exhausted and remobilised in the environment more rapidly than 4–6 ring systems (Krein and Schorer, 2000; Fu et al., 2001). PAH findings were categorised into two structural categories (Figure 3). The overall PAH distribution profiles appeared similar for leachate and groundwater as it was dominated by 2–3 rings system molecules. On the other hand, the sediment PAH profile was dominated by 4–6 ring system molecules. The individual PAH profiles of groundwater, leachate, and sediments are presented in Figure 4. Due to the fact that smaller PAH molecules might be lost due to volatilisation and photo-degradation processes and are able to be mobilised by the leachate contaminating the groundwater resources in the area. Meanwhile, large PAH molecules are strongly retained by sorption on surface sediments material. Figure 3

Distribution pattern of PAH into 2–3 and 4–6 rings system molecules among samples compartments

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A. Jiries, O. Rimawi, J. Lintelmann and M. Batarseh

Figure 4

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Individual 16 PAH distribution profiles (minimum and maximum values) for groundwater, leachate and surface sediments

Conclusions

This work provided significant results on the PAH distribution in leachate, groundwater, and sediments of the Ruseifa landfill. The detected concentration levels of PAH in groundwater were relatively low in comparison to that for leachate and sediment samples in the investigated area. The PAH distribution profiles in groundwater and leachate were similar (dominated with 2–3 rings system) indicating common potential source. On the contradiction, sediments showed the highest concentration levels and dominated by 4–6 rings system.

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The results of the present work indicate that Ruseifa landfill must be monitored continuously in order to prevent hazardous environmental problems. Accordingly, results from the Ruseifa landfill can be considered as a typical example existing in the majority of the Jordanian metropolitan landfills and as consequences of the frequently applied practices of the solid waste management system.

Acknowledgment The authors are very thankful to Mrs Jennet Anderson from Utah, USA for her help in editing the text.

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Lezzari, L., Sperni, L., Bertin, P. and Pavoni, B. (2000) ‘Correlation between inorganic and organic micropollutants concentrations during sewage sludge composting processes’, Chemosph., Vol. 41, pp.427–435. Masclet, P., Cachier, H., Liousse, C. and Wortham, H. (1995) ‘Emissions of polycyclic aromatic hydrocarbons by savanna fires’, J. Atmos. Chem., Vol. 22, pp.41–54. Masclet, P., Hoyau, V., Jaffrezzo, J.L. and Cachier, H. (2000) ‘Polycyclic aromatic hydrocarbon deposition on the ice sheet of Greenland, part I: superficial snow’, Atm. Envir., Vol. 34, pp.3195–3207. Matouq, M. (2003) ‘Waste minimization, separation, collection and transfer methods and technology, case in Jordan’, Workshop on Solid Waste Managment and its Related Health Problems, September, Vols. 4–7, Aqaba-Jordan. Müller, J.F., Hawker, D.W. and Connell, D.W. (1998) ‘Polycyclic hydrocarbons in the atmospheric environment of Brisbane, Australia’, Chemosphere, Vol. 37, pp.1369–1383. NTP (2003) The National Toxicology Program (NTP), within the US Department of Health and Human Services of Health’s National Institute of Environmental Health Sciences (NIEHS), CA, USA, http://ntp-server.niehs.nih.gov. Rimawi, O., Shatanawi, M. and Fayyad, M. (1999) ‘The effect of Ruseifa solid waste disposal site on the groundwater resources of Amman Zarqa Basin’, Abhath Al-Yarmouk Basic Sci. Eng., Vol. 8, pp.73–92. Schwarzenbach, R.P., Gschwend, P.M and Imboden, D.M. (1993) Environmental Organic Chemistry, John Wiley & Sons, New York. Tkalin, A.V. (1996) ‘Chlorinated hydrocarbons in coastal bottom sediments of the Japan sea’, Envir. Poll., Vol. 91, pp.183–185. Wakeham, S.G. and Farrington, J.W. (1980) Hydrocarbons in contemporary aquatic sediments, in Baker, R.A. (Ed.): Contaminants and Sediments, Ann Arbor Science, Vol. 1. Zhou, J.L., Fileman, T.W., Evans, S., Donkin, P., Llewellyn, C., Readman, J.W., Mantoura, R.F.C. and Rowland, S.J. (1998) ‘Fluoranthene and pyrene in the suspended particulate matter and surface sediments of the Humber Estuary, UK’, Marine Poll. Bull., Vol. 36, pp.587–597. Zhou, J.L., Fileman, T.W., Evans, S., Donkin, P., Readman, J.W., Mantoura, R.F.C. and Rowland, S. (1999) ‘The partition of fluoranthene and pyrene between suspended particles and dissolved phase in the Humber Estuary: a study of the controlling factors’, Sci. Total Envir., Vols. 243–244, pp.305–321.

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