The aim of this study was to provide information on the levels of heavy metals (lead and cadmium) in ed­ible specimens around the Tagarades landfill after a big fire.A total of 49 fruit, vegetable and milk samples were collected, according to the Directive 2001/22/EC. The sampling areas were: < 2.5, 2.5, 3, 4, 5, 6, 7, 8, 9 and 10 km around landfill, as well as, 35-40 km away which served as a blank area that was not affected by the landfill. Care was taken to get samples of the same varieties from different selected sites. The samples were wet digested using concentrated nitric and perchloric acid. Cadmium was analyzed using a Flame Atomic Spectrometer and lead an Atomic Absorption Spectrophotometry with graphite furnace atomization. Our results indicate that there was no apparent effect from the landfill fire on lead and cadmium levels found in the tested food samples. These specimens were safe for consumption according to the Draft Commission Regulation on Setting Maximum Limits for Certain Contaminants in Foodstuffs

Achparaki, Maria

Gerolymou, Ioanna

Mastrogianni, Orthodoxia

Pouliopoulos, Athanasios

Raikos, Nikolaos

Thessalonikeos, Elisavet

Tsoukali, Heleni

English

The aim of this study was to provide information on the levels of heavy metals (lead and cadmium) in ed­ible specimens around the Tagarades landfill after a big fire.A total of 49 fruit, vegetable and milk samples were collected, according to the Directive 2001/22/EC. The sampling areas were:  2.5, 2.5, 3, 4, 5, 6, 7, 8, 9 and 10 km around landfill, as well as, 35-40 km away which served as a blank area that was not affected by the landfill. Care was taken to get samples of the same varieties from different selected sites. The samples were wet digested using concentrated nitric and perchloric acid. Cadmium was analyzed using a Flame Atomic Spectrometer and lead an Atomic Absorption Spectrophotometry with graphite furnace atomization. Our results indicate that there was no apparent effect from the landfill fire on lead and cadmium levels found in the tested food samples. These specimens were safe for consumption according to the Draft Commission Regulation on Setting Maximum Limits for Certain Contaminants in Foodstuffs

Aristotle University of Thessaloniki: Open Journals / ΑΡΙΣΤΟΤΕΛΕΙΟ ΠΑΝΕΠΙΣΤΗΜΙΟ ΘΕΣΣΑΛΟΝΙΚΗΣ

INTRODUCTIONEnvironmental pollution from heavy metals has been established as an ubiquitous problem throughout the world, due to the negative effects of heavy metal tox-icity on human health and the growing concerns by the general public1-3. Toxic metals, such as lead, mer-cury, cadmium, arsenic etc. enter the human body by different routes and in different chemical forms. It has been proven that there is an interrelationship between the contents of trace elements in soil, water, plants and air1. Soils can be contaminated by heavy metals as a result of industrial activities e.g. mining, vehicle emission, landfilling of waste etc.Landfill design and location is such as to minimize impacts to the environment and ensure minimum con-tamination of the surrounding area from the waste degradation4. In many cases, liners are installed to prevent the migration of leachate to the surrounding environment. Municipal solid waste (MSW) landfill leachate contains a number of aquatic pollutants; a specific MSW stream often referred to as household hazardous waste, can be considered as a contributor of a large proportion of these pollutants. Great emphasis is given in assessing the environmental consequences of leachate release from a generic MSW landfill, since heavy metals and organic pollutants were found to mi-grate into the zones beneath a model landfill site over a 20,000-year period5.Landfill fires can be extremely hazardous for the environment since they lead to contamination of soil, water and air by toxic pollutants. Although landfill fires are common in Northern European countries, their effects have gone largely ignored by the scien-tific community. Despite the ease with which landfill fires can occur, the consequences for the environment and human health have yet to be investigated exten-sively and thus still remain poorly understood10.The present study provides data about the effect of Tagarades landfill fire on foodstuffs contamination by lead and cadmium. Such data can be helpful in mak-ing risk assessment and risk management information comprehensible to community groups, local elected Heavy metals in edible specimens around Tagarades  landfill after a big fire.Elisavet Thessalonikeos, Maria Achparaki, Ioanna Gerolymou, Athanasios Pouliopoulos, Heleni Tsoukali, Orthodoxia Mastrogianni, Nikolaos RaikosLaboratory of Forensic Medicine and Toxicology, Medical School, Aristotle University, Thessaloniki, GreeceABSTRACT: The aim of this study was to provide information on the levels of heavy metals (lead and cadmium) in ed-ible specimens around the Tagarades landfill after a big fire.A total of 49 fruit, vegetable and milk samples were collected, according to the Directive 2001/22/EC. The sampling areas were: < 2.5, 2.5, 3, 4, 5, 6, 7, 8, 9 and 10 km around landfill, as well as, 35-40 km away which served as a blank area that was not affected by the landfill. Care was taken to get samples of the same varieties from different selected sites. The samples were wet digested using concentrated nitric and perchloric acid. Cadmium was analyzed using a Flame Atomic Spectrometer and lead an Atomic Absorption Spectrophotometry with graphite furnace atomization. Our results indicate that there was no apparent effect from the landfill fire on lead and cadmium levels found in the tested food samples. These specimens were safe for consumption according to the Draft Commission Regulation on Setting Maximum Limits for Certain Contaminants in Foodstuffs.Key Words: Heavy metals, Landfill, Atomic absorption analysis.Corresponding author: Nikolaos Raikos, Lab. Of Forensic Medicine and Toxicology, Medical School, Aristotle University, 541 24 Thessaloniki, Greece, Tel. +30 2310 999206, Fax: +30 2310 999216, e-mail: raikos@med.auth.gr14 Aristotle University Medical Journal, Vol. 39, Issue 2, June 2012officials, environmentalists etc. in order to assure food safety.Determining traces of heavy metal ions in environ-mental samples and/or foods is restricted by two main factors: their very low concentration -which may be lower than the detection limit of many analytical tech-niques including atomic absorption spectrometry- and the interfering effects of the matrix6.Monitoring the distribution of heavy metals in soil, plants and food of animal origin, facilitates the esti-mation of the extent of foodstuffs contamination. The European Commission has proposed a Regulation which sets maximum limits for lead and cadmium in certain foodstuffs7. These maximum allowable limits result from newly found data in recent literature (epi-demiological data etc.).The aim of the present study was to determine the lead and cadmium levels in fruits, vegetables and milk samples taken at different sites around the Tagarades landfill two months after the big fire in July of 2006 and estimate the consequences the fire had on the lev-els of lead and cadmium in these food samples.SAMPLINGForty nine (49) food samples of fruits, vegetables and milk were collected during September of 2006, about two months after the fire (17-28 July 2006). Sampling was done according to the Directive 2001/22/EC.The sampling areas were: less than 2.5, 2.5, 3, 4, 5, 6, 7, 8, 9 and 10 km around the landfill and about 35-40 km away, which was the blank area. For the analy-sis only the edible portions were included, whereas any bruised or rotten parts were removed. Care was taken to get samples of the same varieties from the selected areas, to the extent that it was possible, while samples from greenhouse cultivation were excluded. Vegetables and fruits samples were collected from dif-ferent parts of the plantation, the size of about one half of an acre, were placed in appropriate bags and were air-dried. All samples were transported to the labora-tory as soon as it was made possible.SAMPLE PREPARATIONFive g of fruit/vegetable sample was mixed with equal volumes (total 15 ml) of concentrated nitric and per-chloric acid into a beaker and kept overnight. Careful digestion of the sample took place on a hot plate. The digestion lasted as long as it was necessary in order to get a clear solution of approximately 2 ml volume, followed by cooling and addition of 2% v/v nitric acid solution, to a final volume of 10 ml.30 g of milk were treated with the method men-tioned above using 10 ml of concentrated nitric acid and 10 ml of concentrated perchloric acid for liquid digestion.MATERIALS AND METHODSStandards solutions of lead and cadmium were pro-vided by Merck (Darmstadt, Germany). All chemicals used were of analytical grade. Analysis for cadmi-um was carried out using a flame atomic adsorption spectrometer (Varian, SpectrAA 300) and for lead an Atomic Absorption Spectrophotometer (Perkin Elmer, 460) with a High Graphite Atomizer system HGA - 2100. VALIDATION  OF THE ANALYTICAL METHODThe instruments were calibrated using Pb, and Cd standards. Reagents blank determinations were used to correct the instrument readings. Blank biological specimens of fruits, vegetables and milk were pro-cessed according to the previously described proce-dure and analyzed as mentioned above. The analyzed biological specimens, with no detectable concentra-tions of Pb and Cd, were homogenized and spiked with various amounts of lead and cadmium standard solutions, and a recovery study was carried out. The recoveries of the spiked biological specimens were between 105% and 120%. The relative standard de-viations were lower than 10%. The limits of detection (LOD) were 0.02 mg/kg for cadmium and 0.002 mg/kg for lead.RESULTS AND DISCUSSIONThe maximum allowable levels for Pb are: 0.02 mg/kg in cow milk, 0.1 mg/kg in vegetables, 0.3 mg/kg in foliar vegetables and 0.1 mg/kg in fruits7. For Cd the upper limits are: 0.05 mg/kg in vegetables and fruits and 0.2 mg/kg in folia vegetables. There are no spe-cific guidelines or statutory limits for Cd in cow milk.The results of lead and cadmium determination in fruits, vegetables and milk samples from various areas around the Tagarades landfill are listed in tables 1-4. Heavy Metals in Edible Specimens Around Tagarades Landfill After a Big Fire 15As shown, no trace of Cd was detected in all of the sampling points. Pb was detected in an olive sample, a cow milk sample and in all goat milk samples. Lead concentrations ranged from 0.002 mg/kg in the cow milk sample to 0.02 mg/kg in a goat milk sample. All concentrations found were below the maximum allowable limit (0.02 mg/kg). Only in one goat milk sample, lead concentration was found equal to the up-per allowable limit.Cd was found in two olive samples with 0.02 and 0.03 mg/kg Cd concentration values which are below the upper accepted limits in the selected area. Lead was not detected in olives, goat milk, apples and water melons, but was found in grapes, melon and sheep’s milk. The determined lead concentrations were also below the maximum allowable limits.Table 1. Lead and cadmium levels in tested samples at a distance less than 2.5 km, 2.5 and 3 km away from landfill.Edible SpecimensSampling Points(km away from landfill)Cd (mg/kg wet weight)Pb (mg/kg wet weight)Grapes < 2.5 <LOD <LODOlives < 2.5 < LOD 0.006Olives < 2.5 < LOD < LODCow milk < 2.5 < LOD 0.002Goat milk < 2.5 < LOD 0.02Goat milk < 2.5 < LOD 0.004Cow milk 2.5 < LOD < LODGoat milk 2.5 < LOD 0.014Goat milk 3 < LOD 0.015Goat milk 3 < LOD 0.015Grapes 3 < LOD < LODTable 2. Lead and cadmium levels in tested samples at a distance of 4 km to 7 km from landfill.Edible SpecimensSampling Points(km-around  landfill)Cd (mg/kg wet weight)Pb (mg/kg wet weight)Olives 4 0.03 <LODGrapes 4 < LOD < LODOlives 5 0.02 < LODSheep’s  milk 5 < LOD 0.002Goat milk 5 < LOD < LODGoat milk 6 < LOD < LODApple 6 < LOD < LODWatermelon 6 < LOD < LODGrapes 7 < LOD 0.02Melon 7 < LOD 0.05Grapes 7 < LOD 0.0216 Aristotle University Medical Journal, Vol. 39, Issue 2, June 2012At a distance of 10 to 35 km away from the Taga-rades landfill no trace of lead and cadmium was found. The distance of the selected suburban sampling area from highways, industries etc. can explain these find-ings.Table 3 indicates that Cd was found in an olive sample and two aubergine samples and Pb in a melon, lettuce and corn samples. All these values were again below the allowable upper limits for both metals.Table 3. Lead and cadmium levels in tested samples at a distance of 7-9 km from Tagarades.Edible SpecimensSampling Points(km-around landfill)Cd (mg/ kg wet weight)Pb (mg/ kg wet weight)Zucchini 7 < LOD < LODGrapes 8 < LOD < LODLettuce 8 < LOD 0.05Onion 8 < LOD < LODGrapes 8 < LOD < LODPomegranate 8 < LOD < LODOlives 8 0.04 < LODTomato 8 < LOD < LODPepper 8 < LOD < LODAubergine (Eggplant) 8 0.02 < LODMelon 9 < LOD 0.09Corn 9 < LOD 0.05Aubergine (Eggplant) 9 0.02 < LODPepper 9 < LOD < LODTable 4. Lead and cadmium levels in tested samples at a distance 10- 35 km away from Tagarades landfill.Edible SpecimensSampling Points(km-around  landfill)Cd (mg/kg wet weight)Pb (mg/kg wet weight)Quince 10 <LOD <LODQuince 10 < LOD < LODOlives 10 < LOD < LODCorn 10 < LOD < LODWatermelon 25 < LOD < LODCorn 25 < LOD < LODZucchini 25 < LOD < LODCorn 25 < LOD < LODCorn 25 < LOD < LODOnion 30 < LOD < LODWatermelon 35 < LOD < LODOlives 35 < LOD < LODCow milk 35 < LOD < LOD Heavy Metals in Edible Specimens Around Tagarades Landfill After a Big Fire 17CONCLUSIONSForty nine food samples of fruits, vegetables and milk were analysed for detection and determination of lead and cadmium levels. The sampling sites vary in dis-tance around the Tagarades landfill. Only 5 samples (10%) had detectable cadmium levels which were however lower than the allowed upper limits. As for the level of lead in the samples, the percentage of sam-ples with detectable concentrations was higher (28%) and the values were also below the maximum allowed limits. Only a goat milk sample taken at a distance less than 2.5 km from the landfill had lead concentra-tion equal to the upper limit for milk. Unfortunately there were not any reported data taken before the fire allowing for comparisons to be made. Another study was also conducted during that same period aiming at analyzing soil and vegetation samples collected 15 days after the ultimate fire extinction, from the sur-rounding area of the same landfill. This study also showed that there was no apparent impact from the landfill fire on the surrounding terrestrial environment and heavy metal concentrations were similar to those reported for vegetation species in other Greek loca-tions8. Another investigation during an accidental fire in a landfill in Western Norway revealed that heavy metals in the leachate showed considerably increased concentrations but the determined levels (except of chromium) appeared to return to normal within one week after the fire was extinguished9. Finally, the re-sults taking into account the conclusions of the two studies mentioned above8,9 indicated that there was no apparent effect of the landfill fire on the lead and cadmium levels of the tested food samples and these specimens were safe for consumption according to the Draft Commission Regulation on Setting Maximum Limits for Certain Contaminants in Foodstuffs. ΠΕΡΙΛΗΨΗ: Στόχος της έρευνας ήταν να παράσχει πληροφορίες για τα επίπεδα των βαρέων μετάλλων (μολύβδου και καδμίου) σε βρώσιμα δείγματα που είχαν συλλεχθεί από περιοχές γύρω από τη χωματερή των Ταγαράδων μετά από την εκδήλωση μεγάλης πυρκαγιάς σε αυτήν. Συνολικά 49 δείγματα από φρούτα, λαχανικά και γάλα συλλέχτηκαν σύμφωνα με την οδηγία 2001/22/EC. Οι περιοχές απ’ όπου ελήφθησαν δείγματα ήταν: < 2.5, 2.5, 3, 4, 5, 6, 7, 8, 9, 10 χιλ. γύρω από τη χωματερή όπως και 35-40 χιλ. μακριά και η οποία θεωρήθηκε ως «τυφλή» περιοχή. Έγινε προσπάθεια να συλλεχθούν δείγματα από τις ίδιες ποικιλίες φρούτων και λαχανικών στις προεπιλεγμένες περιοχές δειγματοληψίας. Τα δείγματα κατεργάστηκαν με θέρμανση με μίγμα πυκνών οξέων (νιτρικό και υπερχλωρικό οξύ), ώστε να καταστραφεί η οργανική δομή τους και να καταστεί δυνατή η ανάλυση τους με φασματομετρία ατομικής απορρόφησης. Η ανάλυση του καδμίου έγινε με φασματομε-τρία ατομικής απορρόφησης φλόγας και του μολύβδου με φασματομετρία ατομικής απορρόφησης με φούρνο γραφίτη. Τα αποτελέσματα έδειξαν πως δεν υπήρξε εμφανής επίδραση της πυρκαγιάς στα δείγματα τροφίμων που εξετάστηκαν, όσον αφοράτα επίπεδα του μολύβδου και του καδμίου. Τα δείγματα τροφίμων ήταν ασφαλή προς κατανάλωση σύμφωνα με το Draft Commission Regulation on Setting Maximum Limits for Certain Contaminants in Foodstuffs.Λέξεις Κλειδιά: Βαρέα μέταλλα, Χωματερή, Ατομική απορρόφηση.Βαρέα μέταλλα σε βρώσιμα δείγματα γύρω από τη χωματερή  των Ταγαράδων έπειτα από μεγάλη πυρκαγιά.Eλισάβετ Θεσσαλονικέως, Mαρία Aχπαράκη, Ιωάννα Γερολύμου, Αθανάσιος Πουλιόπουλος, Eλένη Tσούκαλη, Oρθοδοξία Mαστρογιάννη, Nικόλαος ΡάικοςΕργαστήριο Ιατροδικαστικής και Τοξικολογίας, Ιατρική Σχολή, Α.Π.Θ., Θεσσαλονίκη18 Aristotle University Medical Journal, Vol. 39, Issue 2, June 2012  1. Baranowska I., Barchanska H., Pyrsz A., (2005). Dis-tribution of pesticides and heavy metals in trophic chain. Chemosphere, 60, 1590- 1599.  2. Ebbs S., Talbott J., Sankaran R., (2006). Cultivation of garden vegetables in Peoria Pool sediments from the Illinois River: A case study in trace element accu-mulation and dietary exposures .Environment Interna-tional, 32 (6), 766- 774.  3. LaKind J.S., Wilkins A., Berlin Jr. C., (2004), Envi-ronmental chemicals in human milk: a review of lev-els, infant exposures and health, and guidance for fu-ture research. Toxicology and Applied Pharmacology, 198 (2), 184- 208.  4. Chen C-M, Liu M-C., (2006) Ecological risk assess-ment on a cadmium contaminated soil landfill- a pre-liminary evaluation based on toxicity test on local spe-cies and site- specific information, Science of the Total Environment, 359 (1-30), p.120-129.  5. Slack j. R., Gronow R.J., Hall H.D., Voulvoulis N., (2007), Household hazardous waste disposal to land-fill : Using LandSim to model leachate migration, En-vironmental pollution, 146 (2), 501- 509.  6. Yaman M., (2005), The improvement of sensitivity in lead and cadmium determinations using flame atomic absorption spectrometry, Anal. Biochem., 339 (1), 1-8.  7. European Commission (1997). Draft Commission Regulation Setting Maximum Limits for Certain Con-taminants in Foodstuffs. Doc III/5125/95/Rev.3. http://archive.food.gov.uk/maff/archive/food/infsheet/19/no113.  8. Chrysikou L., Gemenetzis P. , Kouras A., Manoli E., Terzi E., Samara C., (2008), Distribution of persistent organic pollutants, polycyclic aromatic hydrocar-bons and trace elements in soil and vegetation fol-lowing a large scale landfill fire in northern Greece, Environment International, 34 (2), 210-225.  9. Øygard J. K., Måge A., Gjengedal E., Svane T., (2005), Effect of an uncontrolled fire and the subsequent fire fight on the chemical composition of landfill leachate, Waste Management, 25 (7), 712-718.10. Frid F., Doudkinski D., Liskevich G., Shafran E., Averbakh A., Korostishevsky N. and Prihodko L. (2009) Geophysical- geochemical investigation of fire prone landfills. Environ Earth Science.REFERENCES

Heavy metals in edible specimens around Tagarades landfill after a big fire

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Heavy metals in edible specimens around Tagarades landfill after a big fire

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Aristotle University of Thessaloniki: Open Journals / ΑΡΙΣΤΟΤΕΛΕΙΟ ΠΑΝΕΠΙΣΤΗΜΙΟ ΘΕΣΣΑΛΟΝΙΚΗΣ