Waste Management & Research

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Metal leachability, heavy metals, polycyclic aromatic hydrocarbons and polychlorinated biphenyls in fly and bottom ashes of a medical waste incineration facility Athanasios Valavanidis, Nikiforos Iliopoulos, Konstantinos Fiotakis and George Gotsis Waste Management Research 2008; 26; 247 DOI: 10.1177/0734242X07083345 The online version of this article can be found at: http://wmr.sagepub.com/cgi/content/abstract/26/3/247

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Copyright © ISWA 2008 ISSN 0734–242X Waste Management & Research 2008: 26: 247–255

Metal leachability, heavy metals, polycyclic aromatic hydrocarbons and polychlorinated biphenyls in fly and bottom ashes of a medical waste incineration facility Athanasios Valavanidis, Nikiforos Iliopoulos, Konstantinos Fiotakis Department of Chemistry, University of Athens, University Campus Zografou, 15784 Athens, Greece.

George Gotsis NAIAS, Scientific and Analytical Laboratory S.A., Ymittou 44, 18540 Piraeus, Greece.

Medical waste from hospitals and other healthcare institutions has become an imperative environmental and public safety problem. Medical waste in Greece has become one of the most urgent environmental problems, because there are 14 000 tons produced annually, of which only a small proportion is incinerated. In the prefecture of Attica there is only one modern municipal medical waste incinerator (started 2004) burning selected infectious hospital waste (5–6 tons day–1). Fly and bottom residues (ashes) are collected and stored temporarily in barrels. High values of metal leachability prohibit the landfilling of these ashes, as imposed by EU directives. In the present study we determined quantitatively the heavy metals and other elements in the fly and bottom ashes of the medical waste incinerator, by inductively coupled plasma emission spectrometry (ICP) and by energy dispersive X-ray analysis (EDAX). Heavy metals, which are very toxic, such as Pb, Cd, Ni, Cr, Cu and Zn were found in high concentrations in both fly and bottom ashes. Metal leachability of fly and bottom ashes by water and kerosene was measured by ICP and the results showed that toxic metals in both ashes, such as Pb, Cr, Cd, Cu and Zn, have high leaching values. These values indicate that metals can become soluble and mobile if ash is deposited in landfills, thus restricting their burial according to EU regulations. Analysis of polychlorinated biphenyls and polycyclic aromatic hydrocarbons in fly and bottom ashes showed that their concentrations were very low. This is the first known study in Greece and the results showed that incineration of medical waste can be very effective in minimizing the most hazardous and infectious health-care waste. The presence of toxic metals with high leachability values remains an important draw back of incineration of medical waste and various methods of treating these residues to diminish leaching are been considered at present to overcome this serious technical problem. Keywords: medical waste, incineration; heavy metals; metal leachability, polycyclic aromatic hydrocarbons; polychlorinated biphenyls, wmr 1232–9

Introduction Medical waste has become a major environmental problem in terms of pollution and public safety. Hospitals, dental practices, physicians, surgeries and veterinarian practices produce daily a series of infectious and hazardous materials. Medical waste needs proper waste management practices in order to minimize hazards to humans and protect the environment (Blackmann 1995).

In recent years, many efforts have been made by environmental regulatory agencies to manage properly the collection, segregation in various categories, transportation and disposal of hospital waste. The European Union has been making special efforts to classify medical waste and legislated for environmental ways of their disposal (European Union Directive 2000).

Corresponding author: Athanasios Valavanidis, Department of Chemistry, University of Athens, University Campus Zografou, 15784 Athens, Greece. Tel: +30 210 7274479; fax: +30 210 7274761; e-mail: [email protected] DOI: 10.1177/0734242X07083345 Received 23 May 2007; accepted in revised form 25 July 2007

247 Downloaded from http://wmr.sagepub.com at University of Athens on June 2, 2008 © 2008 International Solid Waste Association. All rights reserved. Not for commercial use or unauthorized distribution.

A. Valavanidis, N. Iliopoulos, G. Gotsis, K. Fiotakis

Incineration is the most widely used treatment of medical waste. Infectious medical waste is often burned in incinerators (normally three types: ‘multiple chamber’, ‘controlledair’ and ‘rotary kiln’) which are either located on-site in hospitals or at municipal waste facilities that specialize in handling medical waste (Bontoux 1999). Incineration of medical waste has many advantages, because the infectious waste is burned, resulting in the reduction of waste volume, savings in landfill costs and, at the same time, production of energy. Incineration also has disadvantages, however, mainly emissions of toxic gases, non-degradable chlorinated hydrocarbons, heavy metals in fly ash and residue ash and other toxic substances (Alvim-Ferraz et al. 2003). The main culprit for the production of toxic substances is plastic waste, releasing polycyclic aromatic hydrocarbons (PAHs), dioxins and furans (Lee et al. 2003). To protect human health, incinerators need appropriate equipment to reduce toxic air emissions. As a result, new stringent emission regulations make medical waste incineration very costly. Furthermore, fly and bottom ashes produced from incineration must have low leachability of certain heavy metals and toxic substances in order to be able to be deposited in landfills (Sukandar et al. 2006). In Greece, municipal, toxic and medical waste materials are at present major environmental and public safety problems, which have remained largely unresolved until now. It is estimated that every year 390 000 tons of toxic waste are produced (including refinery and electroplating sludge, asbestos, sludge of waste water treatment facilities, batteries, steel-mill bottom residues, etc), of which only 40% are dealt by various methods (Technical Chamber of Greece 2005). Management of medical waste in Greece is becoming an urgent environmental problem due to new environmental regulations and lack of appropriate facilities (Pantazopoulou & Skordilis 1988). It is calculated that 14 000 tons of medical and healthcare waste are produced every year in Greece, of which 53% in the Athens area. In the prefecture of Attica (Athens, Piraeus and suburbs) there are 46 state hospitals and 105 private hospitals and a number of health-care and veterinary centers (with 36 000 beds), producing 20–25 tons day–1 of infectious medical waste, the majority of which require incineration according to EU Directive (2000/71/EC) (Pantazopoulou & Skordilis 1988). In 2002 a modern pyrolytic rotary kiln incinerator started working in the area of the municipal landfill in Ano Liosia (Athens), able to incinerate up to 30 tons day–1, but due to financial considerations and the lack of incentives to hospital administrators, only 5–6 tons of waste (‘red-bag waste’) per day are collected from hospitals for incineration. The main problem is the high financial cost (2 € kg–1), compared to 0.5 € in other European countries, and the lack of special provisions for hospitals to deal with the problem. A small percentage of the total medical waste is incinerated by old-technology, small-scale hospital incinerators, and some waste is disinfected or mixed with municipal waste, especially in provincial hospitals (Technical Chamber of Greece 2005). Medical waste transported to the Ano Liosia (Athens) incinerator, is initially dried at 100 °C and then is introduced

into the pyrolytic rotary kiln of the incinerator and burned at 800–900 °C. Combustion gases pass through a secondary combustion chamber with an auxiliary natural gas burner at 850– 1000 °C. The gaseous effluents are cooled to 400 °C and then enter a cyclone when they are mixed first with lime slurry, consisting of a solution of Ca(OH)2 and then a solution of NaOH or KOH to neutralize acidic gases and remove dioxins, furans and metallic elements. The remaining gaseous and particular effluents pass through an electrostatic precipitator to remove particulates (fly ash) and activated carbon filters to absorb the finer dust and other volatile chemicals. The solid residue (bottom ash) is continuously recovered by a conveyer from which it is deposited into a skip (Capetanios 1995). Both fly and bottom ashes contain toxic heavy metals, which do not permit their disposal to landfills. This is the result of their metal leachability by water and regulatory controls by the EU in the last few years (European Community 1997). Medical waste problems are also an urgent environmental problem in other big cities in Greece, such as Thessaloniki (14% of the total medical waste), Patras, Heraklion (Crete), Larisa, etc. Most of the medical waste in these areas is incinerated in small-scale incinerators at the individual hospitals or are neutralized by other disinfection techniques (Gidarakos et al. 2006, Tsakona et al. 2007). In this experimental study we used samples of fly ash and bottom ash obtained from the municipal rotary kiln incinerator used of medical waste from the Athens area and measured their heavy metals, metal leachability, PAHs and PCBs contents. This is the first medical waste analysis of its kind in Greece, as far as we know from the published literature. Metals and other elements were determined by inductively coupled plasma emission spectrometry (ICP) and energy dispersive X-ray analysis (EDAX). Metal leachability was determined in water and kerosene by ICP. In addition, polycyclic aromatic hydrocarbons (PAHs) were measured by high-performance liquid chromatography (HPLC) using the EPA standard of 16 most important PAHs (EPA standard) and polychlorinated biphenyls (PCBs) were measured by gas chromatography–electron capture detector (GC-ECD). Finally, various proposals for treating those residues to diminish the leaching of heavy metals are discussed.

Materials and methods Collection and analysis of metal concentrations in fly and bottom ashes At different time periods the chief engineer of the facility collected a number of samples of fly ash and bottom ash from the medical waste incinerator in Ano Liosia as it was being removed from the incinerator to be deposited in barrels. The bottom ash was in the form of coarse particulates (black– grey colour) of unburned carbonaceous material (moisture 6.4%), whereas fly ash (containing ∼ 1% moisture) is collected in electrostatic filters and was a fine powder of grey colour. The composition of the medical waste incinerated in the investigated incinerator was not known, but preliminary studies (results not included) showed that more than 50%


Contents of fly and bottom ashes from a medical waste incineration facility

Table 1: Concentration of metals, non-metallic elements, P, O, S and O in fly and bottom ash samples from the medical waste incineration plant in Ano Liosia. ICP values mg kg–1, mean ± SD. The EDAX values are expressed as percentage weight, % w/w, mean ± SD, of selected elements determined. Elements Mn

ICP method: fly ash

ICP method: bottom ash

Cu > Mg > Cr > N > Cd > Mn. The lithophilic metals were found in decreasing order: Ca > Na > K > Al > Fe. Lead (Pb) was present in bottom ash at a much higher concentration (2000 mg kg–1 compared to 1 mg kg–1) than in fly ash. Furthermore, in the bottom ash copper (Cu) was found at concentrations that are ∼ 50% lower than in fly ash. This fact was probably the result of the high volatility of chlorinated salts. The presence of chlorinated disinfectants and PVC bottles may offer an explanation for the formation of these salts during incineration. Cadmium (Cd) and manganese (Mn) were found at low concentrations in bottom ash. Barium (Ba) was not found in bottom ash. Although there are various studies in the scientific literature on medical waste incineration, we did not find similar analyses of metals and other elements in fly and bottom ashes, with the exception of municipal waste incineration, which has many similarities but different composition. Most of the studies were experimental set-ups under different conditions or using different types of municipal, household and mixed waste (Brunner & Monch 1986, Reimann 1989, Nakamura et al. 1996). The distribution of metals and the factors that influence their concentrations in the fly and bottom ash of various incinerators were described in a recent paper in Japan (Jung et al. 2004). Lithophilic metals, such as Fe, Cu, Cr and Al remained mainly in the bottom ash, whereas atmosphilic metals such as cadmium (Cd) was found mostly in fly ash. Seventy-five percent of Pb and Zn were found in bottom ash, despite their high volatility. The presence of toxic metals such as Cu, Pb, Cr and Zn at high concentrations in both ashes was probably the result of their use as alloys for medical equipment (needles, dissecting equipments). The EDAX results presented another spectrum of values of a different kind (percentages of weight of elements related to the total weight of elements) for the presence of metals and non-metallic elements in fly and bottom ashes. Concentrations by EDAX were higher than those measured by ICP because the sample of ashes were first combusted at 800 °C to burn carbonaceous polymeric residues and tar. The % w/w of elements such as oxygen and chlorine gave an indication of the presence of oxide and chloride salts of metals. Most metallic elements were found in the form of oxides: Na2O, MgO, Al2O3, CaO, Fe2O3, SiO2 and sulfur in the form of SO3. The results in Table 1 (the EDAX method) for the percentage of various elements indicate that in the fly ash, oxygen was 35% of all elements (in the form of oxides), 30% was calcium, 25% chlorine (Cl) and 4% sodium. The bottom ash contained the following order of elements: oxygen 56%, calcium 18%, silicon 11%, aluminium 7%, iron 3%, whereas chlorine was absent. These results showed that elements in fly ash were mainly in the form of calcium oxide and most metals were in the form of oxides or chloride salts.

Chlorine is a reactive chemical compound that may have originated from medical disinfectants and decomposition of plastics (PVC). Some chloride salts, such as CuCl2 are highly volatile. Chloride salts also can be a factor for leaching out of metals more easily, whereas oxides are less soluble in water. This hypothesis was taken from the results of another current study which showed that metals such as Ba, Cd, Pb, and Zn in fly ash demonstrated the tendency to leach out easily (Morf et al. 2000). Reports of analysis of metals and other elements in the fly ash of municipal solid waste incineration (MSWI) by scanning electron microscopy-energy dispersive X-ray spectroscopy (SEM-EDX) in the scientific literature are very limited. One study investigated the distribution of 18 metals and chlorine in MSWI fly ash. The results of this study were aiming to define the role of metals in the formation of polychlorodibenzo-p-dioxins and polychlorodibenzo-furans in fly ash (Gilardoni et al. 2004).

Measurements of metal leachability Metal leachability in water is another very important parameter of the municipal and medical waste incineration process. Heavy and toxic metals showed a tendency to leach easily by water into the surrounding environment during landfilling, thus prohibiting the disposal of fly and bottom ashes. The presence of soluble salts can modify the leaching behaviour, requiring proper management due to the fact that the legal standards for disposal are getting more stringent. Furthermore, leaching of metals is a good indicator for a need to change the operating parameters of the incinerator (temperature, gas composition, residence time). In our measurements of metal leachability (Table 2) we used a ratio of 10 : 1 (ratio liquid : solid ash), which is the usual ratio of leaching tests (EN-12457-2), as well the ratio 2 : 1 (EN-12457-1). The test of leachability by kerosene is important in cases in which organic solvents are present in landfills for deposition of fly and bottom ashes. The results of leachability by water and kerosene from the present study are presented in Table 2. The results of the present study showed that the leachability of metals in fly ash by water was in the following decreasing order: Ca > Na > K > Zn > Pb > Mg > Cu > Ba. Leachability values were much lower for Mn, Cr, Ni, Fe, B, P and Cd. The high leachability of Ca, K and Na (used in the wet scrubbers for the removal of acidic gases) is due to the solubility of their chloride salts. The leachability of metals in the bottom ash was found in the following decreasing order: Al > Ca > K > Na > Mg. Leachability values were very low for other elements, such as Ba, Mn, Pb, Cr, Cu, Zn, Ni, B, Fe, P and Cd. It should be noted that not all the metals leaching out are toxic. Metals such as Ca, K and Na are lithophilic and are useful to the soil. The high leachability values of toxic metals such as Pb, Zn and Cu from fly ash (at much lower values when compared to bottom ash) is an important factor restricting their disposal in landfills. Pb and Cd chlorides are known to



be highly volatile compounds and condense at low temperature. These compounds have been shown to leach out easily. Metals such as Cr, Cu and Hg are slightly more difficult to leach out because their presence is mostly residual (Sukandar et al. 2006). According to a personal communication with the engineer at the Ano Liosia incinerator facility, fly and bottom ashes are kept in barrels from the start of the operations (2004) and a decision is going to be taken concerning their stabilization or use (in cement kilns or for bricks) in building materials. The metal leachability values by kerosene were, as expected due to the low solubility of metals and their oxides or salts, much lower than the ones by water. In the fly ash, the leachability followed the order: Ca > Na > Si > Zn, all other values were much lower. In the bottom ash, the leachability followed the order: Ca > Al and all other values were much lower. The leachability limits for the EU were proposed with the Draft of the Council Directive on the Landfill of wastes [Draft on 3 May 1991, COM (91), 102 Final-SYN 335, EC, Brussels, 1991] are : As: 0.2–1.0 mg L–1; Pb: 0.4–2 mg L–1; Cr: 0.1–0.5 mg L–1; Cd: 0.1–0.5 mg L–1; Cu: 2–10 mg L–1; Zn: 2– 10 mg L–1; Ni: 0.4–2 mg L–1; Hg: 0.02–0.1 mg L–1; chlorine 1.2–6.0 mg L–1. The most toxic metals for environmental disposal were placed in decreasing order: Hg > Cr > Cd > As > Ni > Pb > Cu > Zn. These values are stated in a recent paper by Ibanez et al. (2000). Metal leachability values by water found in the present study showed that fly and bottom ashes of the incinerated medical waste can leach considerable amounts of toxic metals such as Pb, Cu, Zn, but much lower amounts of Cr and Ni. It is obvious that these leachability values exceed the limits imposed by the European Community and can not be disposed in landfills. This is an additional technical problem of medical incineration, which has been overcome by various technical solutions of stabilization or reuse of ashes in cement facilities. Changes in the operating parameters of an incinerator, such as temperature, gas composition, residence time, and the presence of reactive compounds (chlorine, sulfur, aluminum and silicate), which influence the final metal speciation and particle size formation of the residue, are considered by experts as important parameters of an incinerator (Belevi & Moench 2000). Furthermore, other physical processes that may influence the distribution of metals are the particle size of the ash and the formation of the carbonate fraction. The later is of great importance because it affects adsorption phenomena, particle nucleation and agglomeration, which in turn affect the leaching potential (smaller particles have greater leaching potential) (Sukandar et al. 2006). Experimental studies have found that metals such as Ba, Cd, Ni, Pb, and Zn are often found in carbonate and exchangeable fractions of waste solid residues, thus these metals in the fly and bottom ash pose great leaching potential (Abanades et al. 2002). Metal leachability tests showed that toxic metals such as Pb, Zn, Cu and Cr are found in the ash fractions of Fe–Mn

oxides, bound and residual organic matters and can pose a long-term leaching risk with the presence of reducing agents and the change in pH of the surrounding environment (Liu et al. 2005). Heavy metal leaching tests in municipal solid waste incineration from Korea and Japan found that in fly ash the order of leaching was Pb > Cd > Cr, but it was changed to Pb > Cr > Cd in the bottom ash. The leaching concentrations of Pb exceeded the Japanese risk level in all fly ashes from the two countries, but the leaching concentration of Cd exceeded the regulatory level in Korea fly ash only (Shim et al. 2005). One of the solutions proposed for the fly and bottom ash incineration products of hospital waste was to incinerate them at a high temperature (1200 °C). The produced slag was characterized in terms of the metals bound to various fractions. The slag proved to stabilize the metals in the matrix and they were not leached beyond the standard set by US EPA, and so it could be classified as non-hazardous product (Idris & Saed, 2002). Other methods developed to deal with the problem of leachability can be found in the recent scientific literature and in patents. One method involves the mixing of municipal solid waste (MSW) incineration residues with water and FeSO4. The stabilized residues have improved leaching properties (Lundtorp et al. 2002, Jensen et al. 2002). Another method was the reuse of fly ashes from MSW incineration as ‘recycled aggregate’ in concrete production (Collivignarelli & Sorlini, 2002). Chemical stabilization of MSW incinerator fly ashes has been proposed in cement or in asphalt solidification (Youcai et al. 2002). A recent method stabilizes fly ashes from mixed hazardous waste incinerator using ordinary Portland cement which has very law leaching values (Pariatamby et al. 2006). Heavy metals from MSW incinerator fly ashes can be removed and leachates can be reused (Levasseur et al. 2006).

Analysis and results of PCBs Concentrations of PCBs in fly and bottom ashes of the incinerator are presented in Table 3. From the results we can observe that concentrations of PCBs as Arochlor 1242, Arochlor 1254, Arochlor 1260 and total Arochlors are very low in fly and bottom ash. For comparison, other studies for PCBs in fly and bottom ash of medical waste incineration are lacking in the scientific literature.

Analysis and results of PAHs The concentrations of 17 PAHs in the fly and bottom ash of the incinerator are presented in Table 4. The concentrations of PAHs in fly and bottom ashes were very low, the majority of PAHs were not detectable by HPLC. In fly ash the concentrations are extremely low and only B[b}Fl and B[a}P were found at low concentrations. In bottom ash the concentrations (in the range of 10–120 mg kg–1) in decreasing order were: B[b]Fl > B[a]P > B[k]Fl > FLA >> PYR > PHE > ANTH. Another similar study in the scientific literature found that PAHs in solid residues from clinical waste incineration


A. Valavanidis, N. Iliopoulos, G. Gotsis, K. Fiotakis

(measured using HPLC with fluorescence detection) were very low. Fly ash did not produce any identifiable PAHs (detection limit < 0.1 µg kg–1). The authors suggest that some high molecular mass PAHs might have been expected in fly ash, particularly given the amount found in the bottom ash of some PAHs (indicative concentrations FLE 2890 mg kg–1, PHE+ANT 2903, FLA 547, BaA+CRHRYS 642, benzofluoranthenes 167, benzopyrenes 128, and BghiP 152 mg kg–1) (Wheatley & Sandhra, 2004). This is an indicative study with concentrations of PAHs in medical waste.

Conclusion Medical waste is a very important environmental and health safety issue. The European Union has recently advanced legislation concerning the classification and proper disposal of medical waste. Incineration is the most widely used method in member countries for the most infectious and hazardous medical waste materials. Greece is at present in a difficult position and many of the problems of medical waste are unresolved. A high proportion of medical waste in Greek hospitals is not managed by appropriate environmental techniques. The only incinerator of medical waste in the area of Athens is very costly, underutilized and its fly and bottom ashes contain high concentrations of heavy metals. Both fly

and bottom ashes have high values of leachability of toxic metals such as Pb, Cu and Zn and lower values for Cr, Ni and Cd, which restricts their disposal in landfills under the EU regulations. There are at present a number of options for stabilization of fly and bottom ashes of incinerators, as well as using cement or other materials for stabilization/solidification of fly and bottom ashes from incinerators of MSW and other toxic waste, in the scientific literature and in patents. In the case of the incinerator of Ano Liosia various proposals have been considered for the stabilization of ashes in order to diminish their leachability or their use in cement kilns or in the making of bricks, but no firm decision has been taken yet.

Acknowledgements We would like to thank the Special Research Grants committee of the University of Athens for financial support, and the Laboratory of Organic Chemistry of the Department of Chemistry of the University for providing the laboratory facilities and instrumentation for the analysis of samples. Many thanks also to the Association of Communities and Municipalities in the Attica Region and the technical director of the facility for providing the samples of the municipal medical waste incinerator in Ano Liosia (Athens, Greece).

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