Back
 AJAC  Vol.4 No.4 , April 2013
Safety of Lebanese Bottled Waters: VOCs Analysis and Migration Studies
Abstract: Despite the worldwide increase in the consumption of PET-bottled mineral waters compared to tap waters encouraged by its microbiological and chemical safety for public health, contaminants could migrate from the plastic packaging into the water and induce adverse effects on human health. Volatile organic compounds (VOCs), including benzene, toluene, ethylbenzene, ortho, meta, and para-xylenes (BTEX), styrene, chlorobenzene and benzaldehyde are among the potential contaminants of bottled waters. This study aimed to assess Lebanese PET-bottled waters, in respect of VOCs contents, with comparison to polycarbonate-bottled and tap waters. Both HS-SPME-GC/FID and SPE-GC/FID were optimized and validated for VOCs determination in the waters, and their performances were compared. The HS-SPME-GC/FID was valid (Afnor NF T 90-210 (May 2009)) for all the studied molecules with limits of quantifications (LOQ) far lower the maximum contaminants levels (MCLs) set by both US-EPA and WHO. SPE-GC/FID was valid only for ethylbenzene, m/p-xylenes, o-xylene, and styrene, with poorer LOQs. HS-SPME-GC/FID was used therefore for VOCs monitoring in studied water samples showing the safety of the Lebanese bottled-water. The effects of bottles storage conditions (time, and exposure to sunlight) on VOCs migration were also studied.
Cite this paper: A. Ghanem, J. Maalouly, R. Saad, D. Salameh and C. Saliba, "Safety of Lebanese Bottled Waters: VOCs Analysis and Migration Studies," American Journal of Analytical Chemistry, Vol. 4 No. 4, 2013, pp. 176-189. doi: 10.4236/ajac.2013.44023.
References

[1]   [1] B. Nijssen, T. Kamperman and J. Jetten, “Acetaldehyde in Mineral Water Stored in Polyethylene Terephthalate (PET) Bottles: Odour Threshold and Quantification,” Packaging Technology and Science, Vol. 9, No. 4, 1996, pp. 175-185.

[2]   S. V. Leivadara, A. D. Nikolaou and T. D. Lekkas, “Determination of Organic Compounds in Bottled Waters,” Food Chemistry, Vol. 108, No. 1, 2008, pp. 277-286. doi:10.1016/j.foodchem.2007.10.031

[3]   C. Bach, X. Dauchy, L. David and S. Etienne, “Chemical Compounds and Toxicological Assessments of Drinking Water Stored in Polyethylene Terephthalate (PET) Bottles: A Source of Controversy Reviewed,” Water Research, Vol. 46, No. 3, 2012, pp. 571-583. doi.:10.1016/j.watres.2011.11.062

[4]   A. Ikem, “Measurement of Volatile Organic Compounds in Bottled and Tap Waters by Purge and Trap GC-MS: Are Drinking Water Types Different?” Journal of Food Composition and Analysis, Vol. 23, No. 1, 2010, pp. 70- 77. doi:10.1016/j.jfca.2009.05.005

[5]   M. Farhadian, C. Vachelard, D. Duchez and C. Larroche, “In Situ Bioremediation of Monoaromatic Pollutants in Ground Water: A Review,” Bioresource Technology, Vol. 99, No. 13, 2008, pp. 5296-5308. doi:10.1016/j.biortech.2007.10.025

[6]   M. E. Mahmoud and H. M. AlBishri, “Identification of Dissolved Organic Species in Non-Drinking Tap Water by Solid-Phase Extraction and Gas Chromatography-Mass Spectrometry,” Journal of Saudi Chemical Society, Vol. 14, No. 1, 2010, pp. 105-115. doi:10.1016/j.jscs.2009.12.017

[7]   S. Fakirov, “Handbook of Thermoplastic Polyesters,” Wiley-VCH, Weinheim, 2002. doi:10.1002/3527601961

[8]   P. Westerhoff, P. Prapaipong, E. Shock and A. Hillaireau, “Antimony Leaching from Polyethylene Terephthalate (PET) Plastic Used for Bottled Drinking Water,” Water Research, Vol. 42, No. 3, 2008, pp. 551-556. doi:10.1016/j.watres.2007.07.048

[9]   C. Bach, X. Dauchy, L. David and S. Etienne, “Physico- Chemical Study of PET Bottles and PET Bottled Water,” Matériaux & Techniques, Vol. 99, No. 4, 2011, pp. 391- 408. doi:10.1051/mattech/2011006

[10]   S.-H. Nam, Y.-M. Seo and M.-G. Kim, “Bisphenol A Migration from Polycarbonate Baby Bottle with Repeated Use,” Chemosphere, Vol. 79, No. 9, 2010, pp. 949-952. doi:10.1016/j.chemosphere.2010.02.049

[11]   H. H. Le, E. M. Carlson, J. Chua, P. Belcher and M. Scott, “Bisphenol A Is Released from Polycarbonate Drinking Bottles and Mimics the Neurotoxic Actions of Estrogen in Developing Cerebellar Neurons,” Toxicology Letters, Vol. 176, No. 2, 2008, pp. 149-156. doi:10.1016/j.toxlet.2007.11.001

[12]   J. Ji, C. Deng, W. Shen and X. Zhang, “Field Analysis of Benzene, Toluene, Ethylbenzene and Xylene in Water by Portable Gas Chromatography-Microflame Ionization Detector Combined with Headspace Solid-Phase Microextraction,” Talanta, Vol. 69, No. 4, 2006, pp. 894-899. doi:10.1016/j.talanta.2005.11.032

[13]   D. Li, B. Han, Z. Liu and D. Zhao, “Phase Behavior of Supercritical CO2/Styrene/Poly(ethylene Terephthlate) (PET) System and Preparation of Polystyrene/PET Composites,” Polymer, Vol. 42, No. 6, 2001, pp. 2331-2337. doi:10.1016/S0032-3861(00)00601-7

[14]   M. Dzieciol and J. Trzeszczynski, “Studies of Temperature Influence on Volatile Thermal Degradation Products of Poly(ethylene terephthalate),” Journal of Applied Polymer Science, Vol. 69, No. 12, 1998, pp. 2377-2381. doi:10.1002/(SICI)1097-4628(19980919)69:12<2377::AID-APP9>3.0.CO;2-5

[15]   R. Di Felice, D. Cazzola, S. Cobror and L. Oriani, “Oxygen Permeation in PET Bottles with Passive and Active Walls,” Packaging Technology and Science, Vol. 21, No. 7, 2008, pp. 405-415. doi:10.1002/pts.820

[16]   K. E. Ozlem, “Acetaldehyde Migration from Polyethylene Terephthalate Bottles into Carbonated Beverages in Turkiye,” International Journal of Food Science and Technology, Vol. 43, No. 2, 2008, pp. 333-338. doi:10.1111/j.1365-2621.2006.01443.x

[17]   C. Dutra, P. D. Freire, M. T. de Alvarenga, N. C. Reyes and F. G. Reyes, “Determination of Volatile Organic Compounds in Recycled Polyethylene Terephthalate and High- Density Polyethylene by Headspace Solid Phase Microextraction Gas Chromatography Mass Spectrometry to Evaluate the Efficiency of Recycling Processes,” Journal of Chromatography A, Vol. 1218, No. 10, 2011, pp. 1319- 1330. doi:10.1016/j.chroma.2010.12.099

[18]   S. Fabris, M. T. Freire, W. de Alvarenga, R. Reyes and F. Guillermo, “A Method to Determine Volatile Contaminants in Polyethylene Terephthalate (PET) Packages by HDC-GC-FID and its Application to Post-Consumer Materials,” Ciência e Tecnologia de Alimentos, Vol. 30, No. 4, 2010, pp. 1046-1055. doi:10.1590/S0101-20612010000400033

[19]   F. L. Bayer, “Polyethylene Terephthalate Recycling for Food- Contact Applications: Testing, Safety and Technologies: a Global Perspective,” Food Additives and Contaminants, Vol. 19, No. S1, 2002, pp. 111-134. doi:10.1080/02652030110083694

[20]   A. Lara-Gonzalo, J. E. Sánchez-Uría, E. Segovia-García and A. Sanz-Medel, “Critical Comparison of Automated Purge and Trap and Solid-Phase Microextraction for Routine Determination of Volatile Organic Compounds in Drinking Waters by GC-MS,” Talanta, Vol. 74, No. 5, 2008, pp. 1455-1462. doi:10.1016/j.talanta.2007.09.036

[21]   E. C. Commission Regulation (EU), “No 10/2011 of 14 January 2011 on Plastic Materials and Articles Intended to Come in Contact with Food,” Official Journal of the European Commission, 2011, pp. L12-L89.

[22]   US-EPA, “National Primary Drinking Water Regulations,” 2009. http://www.epa.gov/ogwdw/consumer/pdf/mcl.pdf

[23]   W. H. Organization, “Guidelines for Drinking-Water Quality,” 2008. http://www.who.int/water_sanitation_health/dwq/GDW8rev1and2.pdf

[24]   US-EPA, “Measurement of Purgeable Organic Compounds in Water by Capillary Column Gas Chromatography/ Mass Spectrometry,” 1992.

[25]   H. F. Al-Mudhaf, F. A. Alsharifi and A.-S. I. Abu-Shady, “A Survey of Organic Contaminants in Household and Bottled Drinking Waters in Kuwait,” Science of the Total Environment, Vol. 407, No. 5, 2009, pp. 1658-1668. doi:10.1016/j.scitotenv.2008.10.057

[26]   H. S. Dórea, J. R. L. Bispo, A. A. S. Kennedy, B. B. Cunha, S. Navickiene, J. P. H. Alves, L P. C. Romão and C. A. B. Garcia, “Analysis of BTEX, PAHs and Metals in the Oilfield Produced Water in the State of Sergipe, Brazil,” Microchemical Journal, Vol. 85, No. 2, 2007, pp. 234- 238. doi:10.1016/j.microc.2006.06.002

[27]   P. Kavcar, M. Odabasi, M. Kitis, F. Inal and S. C. Sofuoglu, “Occurrence, Oral Exposure and Risk Assessment of Volatile Organic Compounds in Drinking Water for Ízmir,” Water Research, Vol. 40, No. 17, 2006, pp. 3219-3230. doi:10.1016/j.watres.2006.07.002

[28]   R. M. Cavalcante, M. V. F. de Andrade, R. V. Marins and L. D. M. Oliveira, “Development of a Headspace-Gas Chromatography (HS-GC-PID-FID) Method for the Determination of VOCs in Environmental Aqueous Matrices: Optimization, Verification and Elimination of Matrix Effect and VOC Distribution on the Fortaleza Coast, Brazil,” Microchemical Journal, Vol. 92, No. 2, 2010, pp. 337- 343. doi:10.1016/j.microc.2010.05.014

[29]   K. E. F. Sieg and W. Püttmann, “Analysis of Benzene, Toluene, Ethylbenzene, Xylenes and n-Aldehydes in Melted Snow Water via Solid-Phase Dynamic Extraction Combined with Gas Chromatography/Mass Spectrometry,” Journal of Chromatography A, Vol. 1178, No. 1-2, 2008, pp. 178-186. doi:10.1016/j.chroma.2007.11.025

[30]   C. Aeppli, M. Berg, T. B. Hofstetter, R. Kipfer and R. P. Schwarzenbach, “Simultaneous Quantification of Polar and non-Polar Volatile Organic Compounds in Water Samples by Direct Aqueous Injection-Gas Chromatography/ Mass Spectrometry,” Journal of Chromatography A, Vol. 118, No. 1-2, 2008, pp. 116-124. doi:10.1016/j.chroma.2007.12.043

[31]   H. Jurdáková, A. Kraus, W. Lorenz, R. Kubinec, Z. Krkosová, J. Blasko, I. Ostrovsky, L. Soják and V. Pacáková, “Determination of Gasoline and BTEX in Water Samples by Gas Chromatography with Direct Aqueous Injection,” Petroleum & Coal, Vol. 47, No. 3, 2005, pp. 49-53.

[32]   M. A. Hossain, M. J. Kabir and S. M. Salehuddin, “Determination of Toxic Toluene, Xylene and Cumene in Different Lake Waters,” International Journal of Environmental Research, Vol. 4, No. 2, 2010, pp. 341-346.

[33]   M. K. Meney and C. M. Davidson, “Use of Solid-Phase Extraction in the Determination of Benzene, Toluene, Ethylbenzene, Xylene and Cumene in Spiked Soil and Investigation of Soil Spiking Methods,” Analyst, Vol. 123, No. 2, 1998, pp. 195-200. doi:10.1039/a706258c

[34]   A. Serrano and M. Gallego, “Fullerenes as Sorbent Materials for Benzene, Toluene, Ethylbenzene, and Xylene Isomers Preconcentration,” Journal of Separation Science, Vol. 29, No. 1, 2006, pp. 33-40. doi:10.1002/jssc.200500200

[35]   S. Nakamura and S. Daishima, “Simultaneous Determination of 22 Volatile Organic Compounds, Methyltertbutyl Ether, 1,4-Dioxane, 2-Methylisoborneol and Geosmin in Water by Headspace Solid Phase Microextraction- Gas Chromatography-Mass Spectrometry,” Analytica Chimica Acta, Vol. 548, No. 1-2, 2005, pp. 79-85. doi:10.1016/j.aca.2005.05.077

[36]   I. Arambarri, M. Lasa, R. Garcia and E. Millán, “Determination of Fuel Dialkyl Ethers and BTEX in Water using Headspace Solid-Phase Microextraction and Gas Chromatography-Flame Ionization Detection,” Journal of Chromatography A, Vol. 1033, No. 2, 2004, pp. 193- 203. doi:10.1016/j.chroma.2004.01.046

[37]   V. H. Niri, L. Bragg and J. Pawliszyn, “Fast Analysis of Volatile Organic Compounds and Disinfection by-Products in Drinking Water using Solid-Phase Microextraction—Gas Chromatography/Time-of-Flight Mass Spectrometry,” Journal of Chromatography A, Vol. 1201, No. 2, 2008, pp. 222-227. doi:10.1016/j.chroma.2008.03.062

[38]   T. C. Schmidt, B. H. Stefan, P. Rolf and R. Forster, “Occurrence and Fate Modeling of MTBE and BTEX Compounds in a Swiss Lake used as Drinking Water Supply,” Water Research, Vol. 38, No. 6, 2004, pp. 1520-1529. doi:10.1016/j.watres.2003.12.027

[39]   C. M. Almeida and L. V. Boas, “Analysis of BTEX and Other Substituted Benzenes in Water using Headspace SPME-GC-FID: Method Validation,” Journal of Environmental Monitoring, Vol. 6, No.1, 2004, pp. 80-88. doi:10.1039/b307053k

[40]   A. Gaujac, S. E. Elissandro, N. Sandro, S. L. C. Ferreira and S. D. Haroldo, “Multivariate Optimization of a Solid Phase Microextraction-Headspace Procedure for the Determination of Benzene, Toluene, Ethylbenzene and Xylenes in Effluent Samples from a Waste Treatment Plant,” Journal of Chromatography A, Vol. 1203, No. 1, 2008, pp. 99-104. doi:10.1016/j.chroma.2008.06.022

[41]   J. C. Flórez Menéndez, M. L. Fernández Sánchez, J. E. Sánchez Uría, E. Fernández Martínez and A. Sanz-Medel. “Static Headspace, Solid-Phase Microextraction and Headspace Solid-Phase Microextraction for BTEX Determination in Aqueous Samples by Gas Chromatography,” Analytica Chimica Acta, Vol. 415, No. 1-2, 2000, pp. 9-20. doi:10.1016/S0003-2670(00)00862-X

[42]   F. Bianchi, M. Careri, E. Marengo and M. Musci, “Use of Experimental Design for the Purge-and-Trap-Gas Chromatography?Mass Spectrometry Determination of Methyl Tert.-Butyl Ether, Tert.-Butyl Alcohol and BTEX in Groundwater at Trace Level,” Journal of Chromatography A, Vol. 975, No. 1, 2002, pp. 113-121. doi:10.1016/S0021-9673(02)00881-6

[43]   Water Quality, “Protocol for the Initial Method Performance Assessment in a Laboratory,” AF-NOR NF T90-210, 2009.

[44]   J. Neter, M. H. Kutner, C. J. Nachtsheim and W. Wasserman, “Applied Linear Statistical Models,” McGrawHill, Chicago, 1998.

[45]   M.-R. Lee, C.-M. Chang and J. Dou, “Determination of Benzene, Toluene, Ethylbenzene, Xylenes in Water at sub-ngl-1 Levels by Solid-Phase Microextraction Coupled to Cryo-Trap Gas Chromatography—Mass Spectrometry,” Chemosphere, Vol. 69, No. 9, 2007, pp. 1381-1387. doi:10.1016/j.chemosphere.2007.05.004

[46]   J. Wang and W. Wan, “Application of Desirability Function Based on Neural Network for Optimizing Bio-Hydrogen Production Process,” International Journal of Hydrogen Energy, Vol. 34, No. 3, 2009, pp. 1253-1259. doi:10.1016/j.ijhydene.2008.11.055

[47]   H. H. Nguyen, N. Jang and S. H. Choi, “Multiresponse Optimization Based on the Desirability Function for a Pervaporation Process for Producing Anhydrous Ethanol,” Korean Journal of Chemical Engineering, Vol. 26, No. 1, 2009, pp. 1-6. doi:10.1007/s11814-009-0001-5

[48]   E. M. Thurman and M. S. Mills, “Solid Phase Extraction: Principles and Practice,” Wiley, New York, 1998.

[49]   A. G. González and M. ángeles Herrador, “A Practical Guide to Analytical Method Validation, Including Measurement Uncertainty and Accuracy Profiles,” TrAC Trends in Analytical Chemistry, Vol. 26, No. 3, 2007, pp. 227- 238. doi:10.1016/j.trac.2007.01.009

[50]   L. Al Rayes, C. O. Saliba, A. Ghanem and J. Randon, “BTES and Aldehydes Analysis in PET-Bottled Water in Lebanon,” Food Additives and Contaminants: Part B: Surveillance, Vol. 5, No. 3, 2012, pp. 221-227. doi:10.1080/19393210.2012.698311

[51]   M. Dzie ciol and J. Trzeszczynski, “Volatile Products of Poly(Ethylene Terephthalate) Thermal Degradation in Nitrogen Atmosphere,” Journal of Applied Polymer Science, Vol. 77, No. 9, 2000, pp. 1894-1901. doi:10.1002/1097-4628(20000829)77:9<1894::AID-APP5>3.0.CO;2-Y

[52]   F. Alario, C. Marcilly and M. Barraqué, “BTX: Benzène, Toluène, Xylène,” Techniques de l’ingénieur, 2005, 4p.

 
 
Top