Sains Malaysiana 47(5)(2018): 871–882

http://dx.doi.org/10.17576/jsm-2018-4705-02

 

Distribution of Polycyclic Aromatic Hydrocarbons (PAHs) in Surface Sediments of Langkawi Island, Malaysia

(Taburan Hidrokarbon Aromatik Polisiklik (HAP) dalam Permukaan Sedimen di Pulau Langkawi, Malaysia)

 

TERENCE RICKY CHIU1, MD FIROZ KHAN2, MOHD TALIB LATIF1,2, MOHD SHAHRUL MOHD NADZIR1,2, HARIS HAFIZAL ABDUL HAMID1, HAFIDZ YUSOFF1 & MASNI MOHD ALI1,3*

 

1School of Environmental and Natural Resources Sciences, Faculty of Science and Technology, Universiti Kebangsaan Malaysia, 43600 UKM Bangi, Selangor Darul Ehsan, Malaysia

 

2Research Centre for Tropical Climate Change System, Institute of Climate Change, Universiti Kebangsaan Malaysia, 43600 UKM Bangi, Selangor Darul Ehsan, Malaysia

 

3Associate Researcher, Institute of Oceanography and Environment, Universiti Malaysia Terengganu, 21030 Kuala Nerus, Terengganu Darul Iman, Malaysia

 

Received: 15 September 2017/Accepted: 13 December 2017

 

 

ABSTRACT

The individual compounds and sources of polycyclic aromatic hydrocarbon (PAHs) were studied in the surface sediments at 32 locations in the tourism area of Langkawi Island. A total of 15 PAHs were determined and quantified by gas chromatography coupled with mass spectrometry (GC-MS). The total PAH concentrations of surface sediments from Langkawi Island ranged from 228.13 to 990.25 ng/g and they were classified as being in the low to moderate pollution range. All sampling stations were dominated by high molecular weight PAHs with 4 rings (31.59%) and 5-6 rings (42.73%). The diagnostic ratio results showed that in most cases, the sampling stations have pyrogenic input. Further analysis using principal component analysis (PCA) combined with absolute principal component score (APCS) and multiple linear regression (MLR) showed that the natural gas emissions contributed to 57% of the total PAH concentration, 22% from the incomplete combustion and pyrolysis of fuel, 15% from pyrogenic and petrogenic sources and 6% from an undefined source.

 

Keywords: APCS; diagnostic ratio; MLR; PAHs; PCA; surface sediments

 

ABSTRAK

Sebatian individu dan sumber hidrokarbon aromatik polisiklik (HAP) telah dikaji di dalam sedimen permukaan pada 32 lokasi sekitar kawasan pelancongan di Pulau Langkawi. Sebanyak 15 HAP telah dikenal pasti dan dikira dengan menggunakan kromatografi gas yang digabungkan dengan spektometri jisim (GC-MS). Jumlah kepekatan HAP pada sedimen permukaan di Pulau Langkawi berjulat daripada 229.13 sehingga 990.25 ng/g dan diklasifikasikan sebagai pencemaran pada julat tahap rendah sehingga sederhana. Kesemua stesen pensampelan didominasi oleh HAP yang mempunyai berat molekul yang tinggi dengan 4 cincin (31.59%) dan 5-6 cincin (42.73%). Keputusan nisbah diagnosis juga menunjukkan bahawa kebanyakan stesen pensampelan tersebut mempunyai input pirogenik. Analisis selanjutnya menggunakan analisis prinsip komponen (PCA) yang digabungkan dengan prinsip komponen skor mutlak (APCS) dan linear regresi pelbagai (MLR) menunjukkan bahawa pelepasan gas asli menyumbang kepada 57% jumlah keseluruhan kepekatan HAP, 22% daripada pembakaran bahan api yang tidak lengkap dan pirolisis minyak, 15% daripada sumber pirogenik dan petrogenik dan 6% daripada sumber yang tidak diketahui puncanya.

 

Kata kunci: APCS; HAP; MLR; nisbah diagnosis; PCA; sedimen permukaan

REFERENCES

Bathi, J.R., Pitt, R. & Clark, S.E. 2009. Associations of PAHs with size fractioned sediment particles. World Env. & Water Res. Cong. 342: 1-10.

Beyer, J., Jonsson, G., Porte, C., Krahn, M.M. & Ariese, F. 2010. Analytical methods for determining metabolites of polycyclic aromatic hydrocarbon (PAH) pollutants in fish bile: A review. Environ. Toxico. Pharm. 30: 224-244.

Boonyatumond, R., Wattayakorn, G., Togo, A. & Takada, H. 2006. Distribution and origins of polycyclic aromatic hydrocarbons (PAHs) in riverine, estuaries, and marine sediments in Thailand. Mar. Poll. Bull. 52(8): 942-956.

Budzinski, H., Jones, I., Bellocq, J., Pie´ rard, C. & Garrigues, P. 1997. Evaluation of sediment contamination by polycyclic aromatic hydrocarbons in the Gironde estuary. Mar. Chem. 58: 85-97.

Chen, H., Teng, Y. & Wang, J. 2012. Source apportionment of polycyclic aromatic hydrocarbons (PAHs) in surface sediments of the Rizhao coastal area (China) u s i n g diagnostic ratios and factor analysis with nonnegative constraints. Sci. Total Environ. 414: 293-300.

CSIRO Huon Estuary Study Team. 2000. Environmental research for integrated catchment management and aquaculture. Project No. 96/284. Final Report to the Fisheries Research & Development Cooperation. pp. 285-311.

De Luca, G., Furesi, A., Micera, G., Panzanelli, A., Piu, P.C., Pilo, M.I., Spano, N. & Sanna, G. 2005. Distribution and origin of polycylic aromatic hydrocarbons (PAHs) in the sediments of Olbia harbor (northern Sardinia, Italy). Mar. Poll. Bull. 50: 1223-1232.

Dobbins, R.A., Fletcher, R.A., Benner, Jr. B.A. & Hoeft, S. 2006. Polycyclic aromatic hydrocarbons in flames, in diesel fuels, and in diesel emission. Combust Flame 144: 773-781.

Fang, X.Y., Jiang, W.M., Miao, S.G., Zhang, N., Xu, M., Ji, C.P., Chen, X.Y., Wei, J.M., Wang, Z.H. & Wang, X.Y. 2004 The multi-scale numerical modeling system for research on the relationship between urban planning and meteorological environment. Adv. Atm. Sci. 21: 103-112.

Gschwend, P.M. & Hites, R.A. 1981. Fluxes of polycyclic aromatic hydrocarbons to marine and lacustrine sediments in the northeastern US. Geochim. Cosmochim. Acta45: 2359-2367.

Gu, Y., Lin, Q., Lu, T., Ke, C., Sun, R. & Du, F. 2013. Levels, composition profiles and sources of polycyclic aromatic hydrocarbons in surface sediments from Nan’ao Island, a representative mariculture base in south China. Mar. Poll. Bull. 75: 310-316.

Guo, W., He, M.C., Yang, Z.F., Lin, C.Y., Quan, X.C. & Wang, H.Z. 2007. Distribution of polycyclic aromatic hydrocarbons in water, suspended particulate matter and sediment from Daliao river watershed, China. Chemosph. 68: 93-104.

Harrison, R.M., Smith, D.J.T., Pio, C.A. & Castro, L.M. 1996. Source apportionment of atmospheric polycyclic aromatic hydrocarbons collected from an urban location in Birmingham, UK. Environ. Sci. Tech. 30(3): 825-832.

Hopke, P.K. 2003. Recent developments in receptor modeling. J. Chemom. 17: 255-265.

Hosseini, M., Peery, S., Bastami, O.K.A.A. & Monikh, F.A. 2012. Distribution of polycyclic aromatic hydrocarbons in water (Persian Gulf) (Iran). American-Eurasian J. Toxic Sci. 4(2): 94-97.

IARC 1983. Polynuclear aromatic compounds, Part 1, chemical, environmental and experimental data. IARC Monogr. Eval. Carcinog. Risk Chem. Hum. 32: 1-453.

Jamhari, A.A., Sahani, M., Latif, M.T., Chan, K.M., Tan, H.S., Khan, M.F. & Tahir, N.M. 2014. Concentration and source identification of polycyclic aromatic hydrocarbons (PAHs) in PM10 of urban, industrial and semi-urban areas in Malaysia. Atmos. Env. 86: 16-27.

Jiang, Y.F., Wang, X.T., Wang, F., Jia, Y., Wu, M.H., Sheng, G.Y. & Fu, J.M. 2009. Levels, composition profiles and sources of polycyclic aromatic hydrocarbons in urban soil of Shanghai, China. Chemos. 75(8): 1112-1118.

Karickhoff, S.W. 1984. Organic pollutant sorption in aquatic systems. J. Hydra. Eng. 110: 707-735.

Khairy, M.A., Kolb, M., Mostafa, A.R., EL-Fiky, A. & Bahadir, M. 2009. Risk assessment of polycyclic aromatic hydrocarbons in a Mediterranean semi-enclosed basin affected by human activities (Abu Qir Bay, Egypt). J. Hazard Mater. 170: 389- 397.

Khan, M.F., Hirano, K. & Masunaga, S. 2010. Quantifying the sources of hazardous elements of suspended particulate matter aerosol collected in Yokohoma, Japan. Atm. Environ. 44: 2646-2657.

Khim, J.S., Kannan, K., Villeneuve, D.L., Koh, C.H. & Giesy, J.P. 1999. Characterization and distribution of trace organic contaminants in sediment from Masan Bay, Korea. Environ. Sci. Tech. 33: 4199-4205.

Klanova, J., Matykiewiczova, N., Macka, Z., Prosek, P., Laska, K. & Klan, P. 2007. Persistent organic pollutants in soils and sediments from James Ross Island, Antartica. Environ. Poll.8: 1-8.

Ko, F., Chang, C. & Cheng, J. 2014. Comparative study of PAHs in coral tissues and the ambient sediments from Kenting National Park, Taiwan. Environ. Poll.185: 35-43.

Kucuksezgin, F., Pazi, I. & Gohul, L.T. 2012. Marine organic pollutants of the Eastern Aegean: Aliphatic and polycyclic aromatic hydrocarbons in Candarli gulf surficial sediments. Mar. Poll. Bull. 64: 2569-2575.

LADA. 2011. Langkawi Development Authority Report. http:// www.lada.gov.my/v2/en/.

Liu, Y., Chen, L., Huang, Q., Li, W. & Tang, Y. 2009. Source apportionment of polycyclic aromatic hydrocarbons (PAHs) in surface sediments of the Huangpu River, Shanghai, China. Sci. Total Environ. 407: 2931-2938.

Luo, X.S., Yu, S., Zhu, Y.G. & Li, X.D. 2011. Trace metal contamination in urban soils of China. Sci. Total Environ. 421-422: 17-30.

Marr, L.C., Kirchstetter, T.W., Harley, R.A., Miguel, A.H., Hering, S.V. & Hammond, S.K. 1999. Characterization of polycyclic aromatic hydrocarbons in motor vehicle fuels and exhaust emissions. Environ. Sci. Tech. 33: 3091-3099.

Mostafa, A.R., Wade, T.L., Sweet, S.T., Al-Alimi, A.K.A. & Barakat, A.O. 2009. Distribution and characteristics of polycyclic aromatic hydrocarbons (PAHs) in sediments of Hadhramout coastal area, Gulf of Aden, Yemen. J. Mar. Sys. 78: 1-8.

Motelay-Massei, A., Ollivon, D., Garban, B., Tiphagne-Larcher, K., Zimmerlin, I. & Chevreuil, M. 2007. PAHs in the bulk atmospheric deposition of the Seine River basin: Source identification and apportionment by ratios, multivariate statistical techniques and scanning electron microscopy. Chemosphere 67: 312-321.

Murakami, M., Nakajima, F. & Furumai, H. 2005. Size-and density distributions and sources of polycyclic aromatic hydrocarbons in urban road dust. Chemosphere 61: 783-791.

Nasher, E., Lee, Y.H., Zakaria, Z. & Surif, S. 2013. Assessing the ecological risk of polycyclic aromatic hydrocarbons in sediments at Langkawi Island, Malaysia. The Sci. World J. 2013: Article ID. 858309.

Thurston, G.D. & Spengler, J.D. 1985. A quantitative assessment of source contribution to inhalable particulate matter pollution in metropolitan Boston. Atm. Environ. 19: 9-25.

Thurston, G.D., Ito, K. & Lall, R. 2011. A source apportionment of U.S. fine particulate matter air pollution. Atm. Environ. 45: 3924-3936.

Osman, R., Saim, N., Juahir, H. & Abdullah, M.P. 2012. Chemometric application in identifying sources of organic contaminants in Langat river basin. Environ. Monit. Assess. 184(2): 1001-1014.

Page, D.S., Boehm, P.D., Douglas, G.S., Bence, A.E., Burns, W.A. & Mankiewicz, P.J. 1999. Pyrogenic polycyclic aromatic hydrocarbons in sediments record past human activity: A case study in Prince William sound, Alaska. Mar. Poll. Bull. 38: 247-260.

Park, S.U., Kim, J.G., Jeong, M.J. & Song, B.J. 2011. Source identification of atmo-spheric polycyclic aromatic hydrocarbons in industrial complex using diagnostic ratios and multivariate factor analysis. Environ. Contam. Toxico.60: 567-589.

Pierson, W.L., Bishop, K., Van, S., Horton, P.R. & Adamantis, C.A. 2002. Environmental water requirements to maintain estuarine processes. Env. Flows in Tech. Rep. Report no. 3. Commonwealth of Australia.

Prahl, F.G. & Carpenter, R. 1983. Polycyclic aromatic hydrocarbons (PAH)-phase associations in Washington coastal sediment. Geochim. Cosmochim. Acta47: 1013-1023.

Riccardi, C., Filippo, P., Pomata, D., Basilio, M. & Spicaglia, S. 2013. Identification of hydrocarbon sources in contaminated soils of three industrial areas. Sci. Total Environ. 450: 13-21.

Pietzsch, R., Patchineelam, S.R. & Torres, J.P.M. 2010. Polycyclic aromatic hydrocarbons in recent sediments from a subtropical estuary in Brazil. Mar. Chem. 118(1-2): 56-66.

Samat, N. 2010. Assessing land use land cover changes in Langkawi Island: Towards sustainable urban living. Malaysian J. Environ. Management 11(1): 48-57.

Sanders, M., Sivetsen, S. & Scott, G. 2002. Origin and distribution of polycyclic aromatic hydrocarbons in surficial sediments from the Savannah River. Archi. Environ. Contam. Toxicol.43: 438-448.

Sicre, M.A., Marty, J.C., Saliot, A., Aparicio, X., Grimalt, J. & Albaiges, J. 1987. Aliphatic and aromatic hydrocarbons in different sized aerosols over the Mediterranean Sea: Occurrence and origin. Atm. Environ. 21: 2247-2259.

Simenov, V., Stratis, J.A., Samara, C., Zachariadas, G., Voutsa, D., Anthemidis, A., Sofoniou, M. & Kouimtzis, T. 2002. Assessment of the surface water quality in northern Greece. Wat. Res. 37: 4119-4124.

Soclo, H., Garrigues, P.H. & Ewald, M. 2000. Origin of polycyclic aromatic hydrocarbons (PAHs) in coastal marine sediments: Case studies in Cotonou (Benin) and Aquitaine (France) areas. Mar. Poll. Bull. 40: 387-396.

Saha, M., Togo, A., Mizukawa, K., Murakami, M. & Takada, H. 2009. Sources of sedimentary PAHs in tropical Asian waters: Differentiation between pyrogenic and petrogenic sources by alkyl homolog abundance. Mar. Poll. Bull. 58: 189-200.

Sverdrup, L.E., Nielsen, T. & Krogh, P.H. 2002. Soil ecotoxicity of polycyclic aromatic hydrocarbons in relation to soil sorption, lipophilicity and water solubility. Environ. Sci. Tech. 36: 2429-2435.

Tam, N.F.Y., Ke, L., Wang, X.H. & Wong, Y.S. 2001. Contamination of polycyclic aromatic hydrocarbons in surface sediment of mangrove swamps. Environ. Poll. 114: 225-263.

Vaezzadeh, V., Zakaria, M.P., Mustafa, S., Ibrahim, Z.Z. & Shau-Hwai, A.T. 2014. Distribution of polycyclic aromatic hydrocarbons (PAHs) in sediment from Muar River and Pulau Merambong, Peninsular Malaysia. Proceedings Int. Con. Environ. Forensics 8:451-455.

Wang, G., Zhang, Q., Ma, P., Rowden, J., Mielke, H.W., Gonzales, C. & Powell, E. 2009. Sources and distribution of polycyclic aromatic hydrocarbons in urban soils: Case studies of Detroit and New Orleans. Soil Sediment Contam. 17: 547-563.

Ying, L., Chen, L., Jianfu, Z., Qinghui, H., Zhiliang, Z. & Hongwen, G. 2008. Distribution and sources of polycyclic aromatic hydrocarbons in surface sediments of rivers and an estuary in Shanghai, China. Environ. Poll. 154: 298-305.

Yunker, M.B., MacDonald, R.W., Vingarzanc, R., Mitchelld, R.H., Goyettee, D. & Sylvestre, S. 2002. PAHs in the Fraser river basin: A critical appraisal of PAH ratios as indicators of PAH source and composition. Org. Geochem. 33: 489-515.

Zakaria, M.P., Okuda, T. & Takada, H. 2001. Polycyclic aromatic hydrocarbon (PAHs) and hopanes in stranded tar-balls on the coasts of peninsular Malaysia: Applications of biomarkers for identifying sources of oil pollution. Mar. Poll. Bull. 42: 1357-1366.

Zakaria, M.P., Takada, H., Tsutsumi, S., Ohno, K., Yamada, J., Kouno, E. & Kumata, H. 2002. Distribution of polycyclic aromatic hydrocarbons (PAHs) in rivers and estuaries in Malaysia: A widespread input of petrogenic PAHs. Environ. Sci. Tech. 36: 1907-1918.

Zhang, Y., Guo, C.S., Xu, J., Tian, Y.Z., Shi, G.L. & Feng, Y.C. 2012. Potential source contributions and risk assessment of PAHs in sediments from Taihu Lake, China: comparison of three receptor models. Water Resources 46: 3065-3073.

 

 

*Corresponding author; email: masni@ukm.edu.my

 

 

previous