Results of the monitoring of non dioxin-like PCBs in food and feed 1

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1 SCIENTIFIC REPORT OF EFSA Results of the monitoring of non dioxin-like PCBs in food and feed 1 ABSTRACT European Food Safety Authority 2, 3 European Food Safety Authority (EFSA), Parma, Italy Non dioxin-like polychlorinated biphenyls (NDL-PCBs) are persistent organic chemicals that accumulate in the environment and humans and are associated with a broad spectrum of health effects. Processing and distribution of PCBs has been prohibited in almost all industrial countries since the late 1980s but they still can be released into the environment from electrical appliances, building paint and sealants and waste sites that contain PCBs. In 2002 the European Commission prescribed a list of actions to be taken to reduce the presence of dioxins and PCBs in food and feed and Member States were recommended to monitor the situation. A total of 12,563 food and feed samples collected in the period from 18 EU Member States, Iceland and Norway were retained for a detailed analysis of the occurrence of the six indicator NDL-PCBs (# 28, 52, 101, 138, 153, and 180). Overall, 18.8% of the results for single congeners were below the limit of quantification (LOQ) but their distribution varied highly between food and feed groups. PCB-153 and PCB-138 were the most commonly detected congeners. In food, the highest mean contamination level was observed in fish and fish derived products followed by eggs, milk and their products, and meat and meat products from terrestrial animals. The lowest contamination was observed in foods of plant origin. A similar pattern was observed in feed where high contamination was reported in feed containing fish derived products and comparatively very low levels in feed of plant or mineral origin. The sum of the six NDL-PCBs was on average close to five times higher than the sum of the 12 dioxin-like PCBs. This relationship varied across food groups and is presumably related to the origin of samples and the contamination source. Country-specific clustering has been observed in several food and feed groups. KEY WORDS Polychlorinated biphenyls, non dioxin-like polychlorinated biphenyls, occurrence, food, feed. 1 On request of EFSA, Question No EFSA-Q , issued on 22 July Correspondence: datex@efsa.europa.eu 3 Acknowledgement: EFSA wishes to thank the EFSA s staff members Valeriu Curtui, Alessandro Carletti, Pietro Ferrari and Stefan Fabiansson for the support provided to this EFSA scientific output. Special thanks to Peter Fürst, and Alexander Kotz for their valuable comments. Suggested citation: European Food Safety Authority; Results of the monitoring of non dioxin-like PCBs in food and feed.. [35 pp.]. doi: /j.efsa Available online: European Food Safety Authority,

2 SUMMARY Polychlorinated biphenyls (PCBs) are a widespread class of persistent organic chemicals that accumulate in the environment and humans and are associated with a broad spectrum of health effects. PCBs were widely used for many applications, especially as dielectric fluids in transformers, capacitors and coolants. Due to their toxicity and classification as persistent organic pollutants, processing and distribution of PCB has been prohibited in almost all industrial countries since the late 1980s but they still can be released into the environment from building paint and sealants and poorly maintained hazardous waste sites that contain PCBs. People are exposed to PCBs primarily through contaminated food. Depending on the number of chlorine atoms and their position, 209 PCB congeners are possible. Based on structural characteristics and toxicological effects, PCBs are divided into dioxin-like PCBs (DL-PCBs) showing toxicological properties similar to dioxins and non dioxin-like PCBs (NDL-PCBs) which do not share the dioxin s toxic mechanism. Some NDL-PCBs have been shown to elicit neurological, endocrine, immunological and carcinogenic effects. Several international agencies classify PCBs as probably carcinogenic to humans. In evaluating the contamination situation, six congeners (# 28, 52, 101, 138, 153, and 180) were chosen as indicators for the occurrence of NDL-PCBs. The Scientific Panel on Contaminants in the Food Chain of EFSA (CONTAM Panel) noted in its Scientific Opinion related to the presence of NDL-PCBs in feed and food that the sum of the six indicator PCBs represented about 50 % of the total NDL-PCB in food. The EU Commission is currently discussing to lay down maximum levels for the sum of the six indicator NDL-PCBs in food and feed. In 2002 the European Commission prescribed a list of actions to be taken to reduce the presence of dioxins and DL-PCBs in food and feed and later introduced regular monitoring by Member States of food and feed, including, if possible, also NDL-PCBs. Data on the presence of dioxins and PCBs in food and feed have been reported on a regular basis to the Commission. In April 2008 the Commission handed the collected information to the European Food Safety Authority (EFSA) for assessment. A total of 11,214 food and 1,349 feed samples collected in the period from 18 EU Member States, Iceland and Norway were retained for a detailed analysis. Overall, 18.8 % of the results for single congeners were below the limit of quantification (LOQ). PCB-153 and PCB-138 contributed the most to the sum of the six NDL-PCB congeners followed by PCB-180, PCB-28, PCB-101 and PCB-52 in that order, but relatively high variations were observed for each congener throughout food and feed groups. The contribution of PCB-153 and PCB-138 together consistently comprised at least 50% of the overall sum of the six congeners in each food group. The highest mean of food contamination levels were observed in several fish and fish product categories followed by products of terrestrial animals. The lowest values were found in fruits and vegetables. Similarly the highest mean of feed contaminations were found in fish oil while most of other feed groups had mean levels below 1 µg/kg. Regression analysis showed that the sum of the six NDL-PCBs were on average close to five times higher than the sum of the 12 DL-PCBs. This relationship varied across food groups and is presumably related to the origin of samples and the contamination source. The current assessment includes results from both random and targeted monitoring but a clear separation of the two sampling groups was not possible. The lack of such sampling information and the irregular coverage of food and feed groups over time did not allow for an accurate time trend analysis to be performed. To improve the validity of any assessment of the presence of dioxins and PCBs in food and feed in Europe it is important to carry out random testing and separate reporting of a sufficient number of samples in each food and feed group. Targeted sampling during contamination incidences should be clearly indicated as such in the reporting. 2

3 TABLE OF CONTENTS Abstract...1 Summary...2 Table of contents...3 Background as provided by the requestor...4 Terms of reference as provided by the requestor...4 Assessment Introduction Objectives Materials and methods Sampling and analytical procedure Data management and validation Expression of results Statistical analysis Results and discussion Number of samples by country and food and feed groups Frequency and descriptive statistics for results below LOQ Contamination level across food and feed groups Contribution of single NDL-PCB congeners to the sum of the six indicators Ratio between NDL-PCBs and DL-PCBs Conclusions and recommendations References Appendix I Glossary and abbreviations

4 BACKGROUND AS PROVIDED BY THE REQUESTOR The term dioxins refers to a group of chemically and structurally related halogenated aromatic hydrocarbons, including 75 polychlorinated dibenzo-p-dioxin (PCDD) and 135 polychlorinated dibenzofuran (PCDF) congeners. Dioxins are widely distributed contaminants formed as unwanted byproducts in a number of anthropogenic activities. The toxicity of individual dioxin and furan congeners differs considerably. From the 210 theoretically possible congeners, only those substituted in each of the 2-, 3-, 7- and 8-positions of the two aromatic rings are of toxicological concern. These 17 congeners exhibit a similar toxicological profile, with 2,3,7,8-tetrachlorodibenzo-p-dioxin (2,3,7,8-TCDD) the most toxic congener. Polychlorinated biphenyls (PCBs) are chlorinated aromatic hydrocarbons, which are synthesised by direct chlorination of biphenyl. Depending on the number of chlorine atom substituents (1-10) and their position on the two rings there are 209 theoretically possible congeners. PCBs can be divided into different groups according to their biochemical and toxicological properties. Non-ortho and mono-ortho substituted PCBs show toxicological properties that are similar to dioxins. They are therefore often termed dioxin-like PCBs. Most other PCBs do not show dioxin-like toxicity. In order to be able to sum up the toxicity of the different congeners of concern (17 dioxins and 12 dioxin-like PCBs), Commission Regulation (EC) No 1881/ lays down the use of toxicity equivalency factors (TEFs) to facilitate risk assessment and regulatory control. The analytical results of all individual dioxin and dioxin-like PCB congeners should be expressed in terms of 2,3,7,8-TCDD toxic equivalents (TEQs) using the TEF values proposed by the World Health Organisation in In 2002, Commission Recommendation 2002/201/EC 5 prescribed a list of actions to be taken to reduce the presence of dioxins and dioxin-like PCBs in food and feed. Target levels for food and feed were recommended based on the opinions produced by the Scientific Committee for Food (SCF, 2000) and the Scientific Committee on Animal Nutrition (SCAN, 2000). In an effort to harmonise the legislation on both dioxins and dioxin-like PCBs in light of more accurate information on their presence in food and feed, a new Commission Recommendation (2006/794/EC) 6 was issued in This Recommendation introduced random monitoring of the presence of dioxins, dioxin-like PCBs and, if possible, non-dioxin-like PCBs, by Member States on the basis of criteria defined by Commission Recommendations 2004/704/EC 7 and 2004/705/EC 8 for feed and food, respectively. Data on the background presence of dioxins, furans, and PCBs in food and feed have been reported on a regular basis to the Commission. In April 2008 the Commission handed the collected information to EFSA for assessment. TERMS OF REFERENCE AS PROVIDED BY THE REQUESTOR The European Food Safety Authority is requested to: 1. Extract from the Member State submissions the original information for each of the 17 dioxins, 12 dioxin-like PCBs and, when relevant, information supplied for non-dioxin-like PCBs. 2. Collate and check the accuracy and details of the submitted information. 4 Commission Regulation (EC) No 1881/2006 of 19 December 2006 setting maximum levels for certain contaminants in foodstuffs. OJ L 364/5, , p Commission Recommendation 2002/201/EC of 4 March 2002 on the reduction of the presence of dioxins, furans and PCBs in feedingstuffs and foodstuffs. OJ L 67, , p Commission Recommendation 2006/794/EC of 16 November 2006 on the monitoring of background levels of dioxins, dioxin-like PCBs and non-dioxin-like PCBs in foodstuffs. OJ L p Commission Recommendation 2004/704/EC of 6 February 2006 on the reduction of the presence of dioxins, furans and PCBs in feedingstuffs and foodstuffs. OJ L , p Commission Recommendation 2004/705/EC of 11 October 2004 on the monitoring of background levels of dioxins and dioxin-like PCBs in foodstuffs. OJ L , p

5 3. Evaluate contamination levels for food and feed categories as nominated in the Commission legislation. 4. Assess the impact of changing the legislation from the current TEF system from 1998 in relation to the new TEFs proposed by the WHO in Document the findings in a report to the Commission and present the results to the Commission Expert Group on persistent organic pollutants (POPs). 6. Provide on-going support in evaluating the annual submissions of data on dioxins, dioxin-like PCBs and non-dioxin-like PCBs. ASSESSMENT 1. Introduction Polychlorinated biphenyls (PCBs) are a class of substances which are synthesised by catalysed chlorination of biphenyl. Depending on the number of chlorine atoms and their position, 209 different compounds (congeners) are possible. PCBs are odourless, tasteless and colourless to pale-yellow oily liquids or solids. Some PCBs are volatile and may exist as a vapour in air. There are no known natural sources of PCBs in the environment (Ballschmiter and Zell, 1980; ATSDR, 2000). Due to their physico-chemical properties, such as chemical stability, low heat conductivity and high dielectric constants, PCBs were widely used in a number of industrial and commercial applications such as hydraulic and heat transfer systems, cooling and insulating fluids in transformers and capacitors, pigments, dyes, repellents and carbonless copy paper or as plasticizers in paints, sealants, plastics and rubber products. For technical purposes, PCBs have been used as complex, technical mixtures and not as single compounds. The different technical mixtures contain in total about 130 individual congeners (Safe, 1990; Dobson and van Esch, 1993; UNEP, 1993; EPA, 2003,). Breivik et al. (2002) estimated an historical global production of 1.3 million tonnes of PCBs of which almost 97% was used in the Northern Hemisphere. PCBs are persistent organic pollutants and have entered the environment through both use and disposal. PCBs were first detected in environmental samples in 1966 (Jensen, 1966). Although the manufacture, processing and distribution of PCBs have been prohibited in almost all industrial countries since the late 1980s, they still can be released into the environment from poorly maintained hazardous waste sites that contain PCBs, illegal or improper dumping of PCB wastes such as old transformer fluids, leaks or releases from electrical transformers containing PCBs, and disposal of PCB-containing consumer products into municipal or other landfills not designed to handle hazardous waste. Other sources include the burning of some wastes in municipal and industrial incinerators and leakage from paint and sealants in older buildings (USDE, 1994; ATSDR, 2000, WHO, 2001). PCBs are globally circulated by atmospheric transport and thus universally present in the environment. Highly chlorinated congeners in particular adsorb strongly to sediment and soil, where they tend to persist with half-lives of months to years. The various PCB congeners differ in their physico-chemical properties and thus demonstrate different behaviour in the environment. Some PCBs are altered through processes such as volatilisation and chemical or biological transformation, which results in a change to the congener pattern compared with the original technical mixtures. This change is even more pronounced when PCB mixtures are ingested by animals, especially mammals, including humans. While certain lower chlorinated PCB congeners are metabolised quickly, higher chlorinated congeners with certain chlorine substitution patterns are more stable and accumulate within the food chain. They are stored in fatty tissues due to their lipophilicity and are highly persistent in the body. The main pathway of human exposure for the majority of the population is via food consumption with the exception of specific cases of accidental or occupational exposure (ATSDR, 2000; WHO, 2003; EFSA, 2005). 5

6 Humans are exposed to PCBs primarily from contaminated food (90%) and through breathing contaminated air. The major dietary sources of PCBs are fish and fish products and meat and meat products (ATSDR, 2000; Baars et al., 2004; Arnich et al., 2009; AFSSA, 2010). High levels of PCBs were found in particular in some specific subpopulations with high dietary PCB exposure such as fishermen from contaminated fishing areas (EFSA, 2005; Turyk et al., 2006). Based on structural characteristics and toxicological effects, PCBs can be divided into two groups. One group consists of 12 congeners that easily can adopt a coplanar structure and has the capability to bind to the Ah receptor, thus showing toxicological properties similar to dioxins (effects on liver, thyroid, immune function, reproduction and behaviour). This group of PCBs is therefore called dioxin-like PCBs (DL-PCB). Non dioxin-like PCBs (NDL-PCBs) refer to PCB congeners (di-ortho or more chlorosubstituted, but including PCB 28 which is mono-ortho) that do not share the dioxin s toxic mechanism (Safe et al., 1985). Some NDL-PCBs elicit different types of responses than the DL-PCBs, including neurological, neuroendocrine, endocrine, immunological and carcinogenic effects. These effects occur via multiple toxicity pathways, not involving the Ah receptors (EPA, 2003). The International Agency for Research on Cancer (IARC) has determined that PCBs are probably carcinogenic to humans (WHO, 1978). PCBs are also classified as probable human carcinogens by the US Environment Protection Agency (EPA, 1996) and the Agency for Toxic Substances and Disease Registry (ATSDR, 2000). It should be noted that in assessing the carcinogenic potential of PCBs no clear distinction was made between DL- PCBs and NDL-PCBs. The Scientific Panel on Contaminants in the Food Chain of EFSA (CONTAM Panel) noted that no published peer-reviewed data were available on the carcinogenic potency of single NDL-PCBs and that PCB mixtures are not mutagenic (EFSA, 2005). The ATHON project funded through the DG Research 6 th Framework program aims to clarify biological mechanisms underlying the various types of toxicity of NDL-PCBs and to evaluate these data from a regulatory toxicology point-of-view ( Data on occurrence of NDL-PCBs in food and feed have been reported in different ways for example as the sum of three congeners (PCB 138, 153 and 180), as the sum of six PCB congeners (PCB 28, 52, 101, 138, 153, 180) often referred to as indicator PCBs or as the sum of seven (sum of six indicator PCBs plus PCB 118). The six PCBs were chosen as indicators not because of their toxicity but because they are easily quantified compared to the other NDL-PCBs and they represent all relevant degrees of chlorination. The EFSA Scientific Panel on Contaminants in the Food Chain (CONTAM Panel) decided to use the sum of the six indicator PCBs as the basis for the evaluation because these congeners are appropriate indicators for different PCB patterns in various sample matrices and are most suitable for a risk assessment of NDL-PCBs on the basis of the available data. The CONTAM Panel noted in its Scientific Opinion related to the presence of non-dioxin-like PCBs in feed and food that the sum of the six indicator PCBs represents about 50 % of the total NDL-PCB in food (EFSA, 2005). Table 1: Congener number and the IUPAC name of the six indicator non dioxin-like PCBs. Congener Number PCB 28 PCB 52 PCB 101 PCB 138 PCB 153 PCB 180 IUPAC Name 2,4,4'-Trichlorobiphenyl 2,2',5,5'-Tetrachlorobiphenyl 2,2',4,5,5'-Pentachlorobiphenyl 2,2',3,4,4',5'-Hexachlorobiphenyl 2,2',4,4',5,5'-Hexachlorobiphenyl 2,2',3,4,4',5,5'-Heptachlorobiphenyl Although there might often be different sources for dioxins/furans (PCDD/Fs), DL-PCBs, and NDL-PCBs some studies have demonstrated that there is a certain correlation between the occurrence of NDL-PCBs and DL-PCBs on the one hand, and between NDL-PCBs and total PCDD/F+DL-PCBs 6

7 on the other (EFSA, 2005; AFSSA, 2009). In the AFSSA opinion it has been demonstrated that in freshwater and marine fish NDL-PCB levels were significantly correlated with total PCDD/F+DL- PCB levels. Schwind et al. (2009) found strong correlations between the level of PCB 153 and DL- PCBs in fish, but no correlation was demonstrated in meat of terrestrial animals. Also, no correlation was observed between NDL-PCBs and PCDD/F in fish. A community strategy for dioxins, furans and PCBs was adopted by the Commission on 24 October 2001, addressing measures to limit or to eliminate their emission into the environment through sourcedirected measures and addressing the way to actively decrease the presence of dioxins, furans and PCBs in food and feed. Maximum levels for PCDD/F and DL-PCBs in food and feed are laid down in Commission Regulation (EC) No 1881/2006 but currently there are no EU maximum limits set up for NDL-PCBs in food and feed. Since 2006, the EU Commission initiated several consultations with the Member States on setting maximum levels for the sum of the six indicator NDL-PCBs in food and feed. The proposed limits are still under discussion. In an effort to harmonise the legislation on dioxins and PCBs Commission Recommendation 2006/794/EC recommends that Member States randomly monitor the presence of dioxins, dioxin-like PCBs and, if possible, non-dioxin-like PCBs. Data on the background presence of dioxins and PCBs in food and feed have been reported on a regular basis to the Commission. In April 2008 the Commission handed the information collected to EFSA for a detailed assessment. 2. Objectives In March 2010, EFSA published the report on the monitoring of dioxin levels in food and feed (EFSA, 2010). The present report is a continuation of the data analysis on dioxins and PCBs with special emphasis on NDL-PCBs and covers the following tasks: 1. Extraction from the Member State submissions of the original information for each of the six indicator NDL-PCBs. 2. Collation and checking of the accuracy and details of the submitted information. 3. Evaluation of contamination levels for food and feed categories as nominated in the EU legislation for dioxins and DL-PCBs. 4. Evaluation of the contribution of single NDL-PCBs to the sum of the six indicators. 5. Assessment of the ratio between the occurrence of the six indicator PCBs and the occurrence of DL-PCBs. 3. Materials and methods 3.1. Sampling and analytical procedure The procedures and requirements for sample collection, preparation and analyses to monitor the levels of dioxins (PCDD), furans (PCDF) and dioxin-like PCBs in foodstuffs are detailed in Commission Regulation (EC) No 1883/2006. The methods of sampling and analysis for the official control of feed are laid down in Commission Regulation (EC) No 152/ It also states that in accordance with the provisions of Regulation (EC) No 882/2004 of the European Parliament and of the Council 10, laboratories shall be accredited by a recognised body operating in accordance with ISO Guide 58 to ensure that they are applying analytical quality assurance. Laboratories shall be accredited following the EN ISO/IEC standard. 9 Commission Regulation (EC) No 152/2009 of 27 January 2009 laying down the methods of sampling and analysis for the official control of feed. OJ L 54, , p Regulation (EC) No 882/2004 of the European Parliament and of the Council of 29 April 2004 on official controls performed to ensure the verification of compliance with feed and food law, animal health and animal welfare rules. OJ L 165, , p

8 Analytical results shall be reported as the upper bound levels of the individual congeners. As there is no specific legislation for NDL-PCBs, a classification was undertaken according to the dioxin and dioxin-like PCB legislation for food in Commission Regulation (EC) No 1881/2006 and feed in Directive 2002/32/EC 11 of the European Parliament and of the Council as amended by Commission Directive 2006/13/EC 12 (see Appendix I). Commission Recommendation 2006/794/EC suggests to adopt nanogram/gram or microgram/kilogram (ng/g or μg/kg) for the non-dioxin-like PCBs. When the information was missing it was assumed that the results were expressed as required by the above legislation. This report includes data from 1995 onwards Data management and validation Out of the 26,600 sets of individual sample results for dioxins and PCBs handed to EFSA, 16,329 contained information on the complete set of the six indicator NDL-PCBs and therefore only these samples were considered for the further evaluation. Data were sent by 19 Member States, Iceland and Norway (Table 2). A list of validation steps (exclusion criteria cover samples with a number of relevant fields left blank, missing food description, or inconsistency between limit of quantification reported and result) was applied to this dataset. Five percent of samples were not complying with the required criteria and were thus excluded. The remaining 15,524 samples were checked for analytical performance criteria developed with the support of the EU Reference Laboratory for Dioxins and PCBs in Feed and Food, Freiburg, Germany, and the European Commission. In a first step, depending on the food or feed group, samples with a LOQ higher than 0.2, 1 or 2 ng/g at the congener level were excluded (Table 3 and 4). The samples were excluded regardless of whether or not only one or more congeners exceeded the maximum accepted LOQ. In a second step, the percentage difference between the upper bound and lower bound of the sum of the six indicators was assessed. Lower and upper bound contamination values were determined by setting to zero and LOQ, respectively, congener-specific analytical results reported to be below the LOQ. In accordance with Commission Regulation (EC) No 1883/2006, Commission Regulation (EC) No 152/2009, and the working document on analytical requirements for determination of non dioxinlike PCBs in food (EU-RL, 2009) samples were excluded when the percentage difference between lower bound and upper bound (reference) estimates of the sum of the six indicators was greater than a pre-defined threshold value set for each food and feed group. By applying the data validation criteria to the cleaned data set a total of 2,961 samples (19%) were excluded and thus 12,563 samples were retained for the final evaluation. The highest proportion of samples (12%) was excluded by applying the specific LOQ cut-off in both food and feed categories (Tables 3 and 4). The criteria based on difference between upper-bound and lower-bound accounted for 7.1% of exclusions. 11 Directive 2002/32/EC of the European Parliament and of the Council of 7 May 2002 on undesirable substances in animal feed. OJ L 140, , p Commission Directive 2006/13/EC of 3 February 2006 amending Annexes I and II to Directive 2002/32/EC of the European Parliament and of the Council on undesirable substances in animal feed as regards dioxins and dioxin-like PCBs. OJ L 32, , p

9 Table 2: Number of country-specific samples analysed for the six indicator NDL-PCBs (initially submitted, retained after a number of validation steps, included in the final database) and their proportion of the total. Country Initial Cleaned Final Percentage Austria Belgium Cyprus Czech Republic Denmark Estonia Finland France Germany 7,230 7,147 6, Greece Iceland Ireland Italy Luxembourg Netherlands Norway Poland Romania Slovenia Sweden United Kingdom 1,580 1,367 1, Not reported Total 16,329 15,524 12,

10 Table 3: Number of samples distributed in food groups before and after applying the exclusion criteria. Food group Initial Cut off* LOQ (µg/kg ) N excl. Concentration range in µg/kg (diff. UB-LB in %) N excl. Concentration range in µg/kg (diff. UB-LB in %) N excl. Concentration range in µg/kg (diff. UB-LB in %) Meat and meat products ruminants (40) (30) 0 >25 (20) Meat and meat products poultry (40) (30) 4 >25 (20) Meat and meat products pigs (40) 4 >10 (20) Liver and products terrestrial animals (40) (30) 1 >40 (20) 0 62 Muscle meat fish and fish products excluding eel 3, >75 (20) ,834 Muscle meat eel >300 (20) Raw milk and dairy products incl. butter 6, (40) (30) 79 >20 (20) 0 5,640 Hen eggs and egg products 1, (40) (30) 144 >40 (20) Fat ruminants (40) (30) 32 >25 (20) Fat poultry (40) (30) 86 >25 (20) 0 53 Fat pigs (40) 15 >10 (20) Mixed animal fats (40) 0 >10 (20) Vegetable oils and fats (40) 7 >10 (20) Marine oils (40) (30) 0 >180 (20) 0 40 Fish liver >75 (20) Other products >30(20) Fruits, vegetables and cereals >1 (20) Infant and baby food >1 (20) Total food 13,942 1, ,214 * Maximum LOQ accepted for each congener N excl. Final data set 10

11 Table 4: Number of samples distributed in feed groups before and after applying the exclusion criteria. Feed group Initial Cut off* LOQ (µg/kg ) N excl. Concentration range in µg/kg (diff. UB- LB in %) N excl. Concentration range in µg/kg (diff. UB-LB in %) N excl. Concentration range in µg/kg (diff. N excl. UB-LB in %) Feed materials of plant origin excl. oils (40) (30) 0 >8 (20) Vegetable oils and their byproducts (40) (30) 0 >8 (20) 0 65 Feed materials of mineral origin (40) (30) 0 >8 (20) Animal fat, including milk fat and egg fat (40) (30) 1 >8 (20) 0 26 Other land animal products including milk, eggs and their (40) (30) 0 >8 (20) 0 32 products Fish oil (40) (30) 0 >100 (20) 0 69 Aquatic animals excl. fish oil and protein (40) (30) 3 >20 (20) Additives binders and anti-caking agents (40) (30) 0 >8 (20) 0 9 Additives compounds of trace elements (40) (30) 0 >8 (20) 0 42 Premixtures (40) (30) 0 >8 (20) 0 73 Compound feed, excl. fur animals, pets and fish (40) (30) 0 >8 (20) Feed for fur animals, pets and fish (40) (30) 3 >30 (20) Other feed additives (40) (30) 0 >8 (20) 0 5 Feed not specified (40) (30) 0 >8 (20) 0 6 Other feed (40) (30) 0 >8 (20) 0 1 Total feed 1, ,349 * Maximum LOQ accepted for each congener Final data set 11

12 3.3. Expression of results Monitoring of Non Dioxin-Like PCBs in Food and Feed Most of the original files handed to EFSA included information on the fat content of the sample, as well as on the method used for fat extraction, as required by the legislation. Commission Recommendation 2006/794/EC of 16 November 2006 on the monitoring of background levels of dioxins, dioxin-like PCBs and non-dioxin-like PCBs in foodstuffs and Commission Recommendation 2004/704/EC of 11 October 2004 on the monitoring of background levels of dioxins and dioxin-like PCBs in feedingstuffs prescribe how the results should be expressed for the respective food and feed groups, either on fat, whole weight basis or feed containing 12% moisture. When not reported, the expression of results was assumed to be compliant with the legislation. On the other hand, when the expression of results was not in agreement with legislation requirements, the PCB concentration was converted to the required expression of results using the reported fat content, where available. For foods which are not covered by the legislation on dioxins (Commission Regulation (EC) No 1881/2006) no assumption was made Statistical analysis Frequency tables and summary statistics were produced to describe the NDL-PCB data (as sum of the six indicator PCBs) by year of collection, country of testing, as well as food and feed group. To compare the occurrence of the individual congeners across food and feed groups summary statistics were also produced at the congener level. The ratio between the occurrence of the six indicator NDL- PCBs and the occurrence of DL-PCBs across food and feed groups was calculated. All analyses were run using the SAS Statistical Software (SAS software, 1999). 4. Results and discussion 4.1. Number of samples by country and food and feed groups The final data set obtained after applying the validation criteria included results from 18 Member States, Iceland and Norway. Most sample results retained in the final data set of NDL-PCBs were from Germany (48%) followed by United Kingdom (9.8%) and Ireland (5.9%). The number of samples distributed in food and feed groups and the basis on what the results have been expressed for each group (fat, whole weight, or 12% moisture basis) are presented in Table 5. The data collection covers results from 1995 to 2008 with the majority of samples collected between 1999 and The number of samples covered for each sampling year in the different countries is detailed in Table 6. The sampled food and feed groups and the number of samples by country and food and feed group are illustrated in Table 7 and 8. There were 11,214 food and 1,349 feed samples classified in categories as defined by Commission Regulation (EC) No 1881/2006 and Directive 2002/32/EC of the European Parliament and of the Council as amended by Commission Directive 2006/13/EC, respectively. The group Raw milk and dairy products including butter contained the largest number of samples (n = 5,640) followed by the group Muscle meat fish and fish products excluding eel (n = 2,834). In the feed area most samples belonged to the group Compound feed, excluding feed for fur animals, pets and fish (n = 398) followed by Feed materials of plant origin, excluding oils. Some food and feed groups e.g. Mixed animal fats, Feed not specified, Other feed additives and Other feed contained only a limited number of samples and therefore these groups were excluded from several statistical evaluations. A general caution is in place in relation to random and targeted sampling. Some of the results reported might have originated from targeted testing during specific dioxin contamination incidences and the overall results might therefore not be a true representation of European background levels of NDL- PCBs. 12

13 Table 5: Number of samples distributed in food and feed groups. Basis indicates on what basis the results have been expressed, whether on fat, whole weight (ww), or 12% moisture basis (12%). Food/feed group Frequency Percent Basis Meat and meat products ruminants fat Meat and meat products poultry fat Meat and meat products pigs fat Liver and products terrestrial animals fat Muscle meat fish and fish products excluding eel 2, ww Muscle meat eel ww Raw milk and dairy products incl. butter 5, fat Hen eggs and egg products fat Fat ruminants fat Fat poultry fat Fat pigs fat Mixed animal fats fat Vegetable oils and fats fat Marine oils fat Fish liver ww Other products * Fruits, vegetables and cereals ww Infant and baby food fat Feed materials of plant origin excl. oils % Vegetable oils and their by-products % Feed materials of mineral origin % Animal fat, including milk fat and egg fat % Other land animal products including milk, eggs and their products % Fish oil % Aquatic animals excl. fish oil and protein % Additives binders and anti-caking agents % Additives compounds of trace elements % Premixtures % Compound feed, excl. fur animals, pets and fish % Feed for fur animals, pets and fish % Other feed additives % Feed not specified % Other feed % *Results in the category Other products were expressed on fat, whole weight or the basis for expression of results was not reported. 13

14 Table 6: Number of accepted samples submitted for each sampling year by the respective country. Country Total Austria Belgium Czech Republic Denmark Estonia Finland France Germany , ,032 Greece Iceland Ireland Italy Luxembourg Netherlands Norway Poland Romania Slovenia Sweden United Kingdom ,232 Total ,598 1,129 1, ,274 1,155 1, ,563 14

15 Table 7: Country ISO code and food group specific sample numbers. Food group AT BE CZ DK EE FI FR DE GR IS IE IT LU NL NO PO RO SI SE UK Total Meat and meat products ruminants Meat and meat products poultry Meat and meat products pigs Liver and products terrestrial animals Muscle meat fish and fish products excluding eel ,834 Muscle meat eel Raw milk and dairy products incl. butter , ,640 Hen eggs and egg products Fat ruminants Fat poultry Fat pigs Mixed animal fats Vegetable oils and fats Marine oils Fish liver Other products Fruits, vegetables and cereals Infant and baby food Total food , ,214 15

16 Table 8: Country ISO code and feed group specific sample numbers. Feed group AT BE CZ DK EE FI FR DE GR IS IE IT LU NL NO PO RO SI SE UK Total Feed materials of plant origin excl. oils Vegetable oils and their byproducts Feed materials of mineral origin Animal fat, including milk fat and egg fat Other land animal products including milk, eggs and their products Fish oil Aquatic animals excl. fish oil and protein Additives binders and anticaking agents Additives compounds of trace elements Premixtures Compound feed, excl. fur animals, pets and fish Feed for fur animals, pets and fish Other feed additives Feed not specified Other feed Total feed ,349 16

17 4.2. Frequency and descriptive statistics for results below LOQ Monitoring of Non Dioxin-Like PCBs in Food and Feed On average, 18.8 % of the results for the individual congeners were below the LOQ (range 15.6 % %). PCB-153 and PCB-138 were the most commonly detected NDL-PCBs with only 15.6% and 15.9%, respectively, of results below the LOQ (Table 9). Table 9: Proportion of results below the LOQ (<LOQ), mean, percentiles, minimum and maximum of LOQ values over the six individual congeners expressed in µg/kg. Congener N <LOQ %* Mean Min P25 P50 P75 Max PCB-153 1, PCB-138 2, PCB-180 2, PCB-101 2, PCB-52 2, PCB-28 2, Overall 14, Expressed on fat basis PCB PCB PCB PCB PCB PCB Expressed on whole weight PCB PCB PCB PCB PCB PCB Expressed on feed 12% moisture PCB PCB PCB PCB PCB PCB Expression of result not reported** PCB PCB PCB PCB PCB PCB *% calculated from the total number of results <LOQ of the respective congener. **Although the basis for expression of results was not reported for a number of samples, in the calculation it was assumed that the results were expressed as required by the legislation. However, for this calculation they were kept separate. 17

18 Results below the LOQ of a specific congener were relatively homogenously distributed within the groups built on the basis of results expressed on fat, whole weight or 12% moisture (range 19.6 % %). Mean LOQs were in the range of µg/kg for results expressed on fat basis, µg/kg for results expressed on whole weight basis and µg/kg for results expressed on 12% moisture basis. However, there was a considerable variation between the minimum and maximum LOQs reported for all groups with minimum LOQ as low as µg/kg to a maximum LOQ as high as 2 µg/kg within the retained results. It is important to note that the maximum LOQ levels mostly reflect the LOQ cut-off applied to a each food and feed group as analytical performance criterion (see section 3.2 Data management and validation). The NDL-PCBs were regularly found in some commonly consumed food commodities with quantifiable levels observed in close to 99% of the tested raw milk and dairy product samples and 94% of hen eggs and hen egg product samples. All of the few foods for infants and babies examined contained some level of NDL-PCB. A majority of products in this group were fish-based. Overall, only 14% of food and feed products did not contain any quantifiable NDL-PCB. The distributions of samples below the LOQ in the different food and feed groups are illustrated in Figures 1 and 2. There is a considerable difference between the groups. Meat and meat products pigs Other products Meat and meat products ruminants Meat and meat products poultry Fruits, vegetables and cereals Muscle meat fish and fish products Vegetable oils and fats Fat pigs Muscle meat eel Hen eggs and egg products Liver and products terrestrial animals Raw milk and dairy products incl. Fat ruminants Fat poultry Marine oils Infant and baby food Fish liver 0% 20% 40% 60% 80% 100% Percentage of samples below the LOQ Figure 1: The proportion of samples with all NDL-PCB congeners below the LOQ across food groups. Additives binders and anti-caking agents Feed not specified Additives compounds of trace elements Other land animal products including milk, Compound feed, excl. fur animals, pets and fish Feed materials of mineral origin Feed materials of plant origin excl. oils Vegetable oils and their by-products Premixtures Feed for fur animals, pets and fish Aquatic animals excl. fish oil and protein Animal fat, including milk fat and egg fat Fish oil 0% 20% 40% 60% 80% 100% Percentage of samples below the LOQ Figure 2: The proportion of samples with all NDL-PCB congeners below the LOQ across feed groups. 18

19 4.3. Contamination level across food and feed groups Monitoring of Non Dioxin-Like PCBs in Food and Feed The lower and upper bound sum of the six indicator NDL-PCBs were calculated for each food and feed group and displayed in Tables 10 and 12. Use of the upper bound is prescribed by the legislation on dioxins to check for compliance. A similar approach has been applied to the NDL-PCBs although there is no legislation in place yet setting maximum limits for this group of compounds. The difference between upper and lower bound results varied from % to 76 %. However, in all groups with mean contamination levels higher than 1 µg/kg the difference was lower than 17%, mostly below 5 %. For a comparison of absolute values of contamination across the different groups, the basis on which the results are expressed must be taken into account. It is important to note that some of the results might have originated from targeted sampling during dioxin and PCB contamination incidents and thus the mean contamination levels might be biased by those samples. Therefore, the European background contamination should be discussed taking also into consideration the median contamination levels (P50). The highest mean levels of NDL-PCBs in food when expressed on a whole weight basis were observed in fish and fish products, with 223 µg/kg in Muscle meat of eel followed by 148 µg/kg in Fish liver, and 23 µg/kg in Muscle meat fish and fish products excluding eel. Among food categories of terrestrial animal origin (results expressed on fat basis) Hen eggs and egg products and Raw milk and dairy products including butter had relatively high mean contamination levels of 16.7 and 9.2 µg/kg fat, respectively. Meat and meat products from ruminants, poultry and pigs had mean contamination levels below 5 µg/kg fat. Among animal fats the highest mean contamination level was observed in fat from ruminants at 8.71 µg/kg fat. Since the results of NDL-PCBs in meat of terrestrial animals are expressed on fat basis theoretically the contamination level in fat and meat of the same animal category should have similar values. In practice fat and meat samples do not originate from the same individuals and the sampling in the Member States might be shifted towards one or other matrix and thus differences between mean contamination level in fat and meat of the same animal category might occur. Although the number of samples for infant and baby food was limited, it seems that the contamination level in this food group is very dependent on the ingredients used. Infant and baby food without meat or containing meat from terrestrial animals presented a mean contamination level of 0.37 µg/kg while infant food containing fish meat had a mean contamination level of 10.9 µg/kg. The lowest contamination levels were observed in foods of plant origin. The category Other products contains foods which are not covered by the provisions of the Commission Regulation (EC) No 1881/2006 regarding the maximum limits for dioxins in food. Therefore, these foods were further classified in ad hoc food groups (Table 11). For several samples the food description was insufficient to accurately classify the foods (meat not specified, fat not specified). The contamination levels in horse meat were similar to levels in meat from ruminants although the number of horse meat samples was very limited. Game meat had a higher mean contamination level than meat from any other terrestrial animals. Levels found in offal and offal products (liver not included) were similar to levels found in meat from terrestrial animals. The apparently not negligible upper-bound mean level found in honey is very much the results of the LOQs applied for this matrix. In fact, NDL-PCBs above the LOQ were reported only in two honey samples and that at a level very close to the LOQ. The relatively high level of contamination reported in some food supplements might be related to the presence of fish oil as an ingredient in those samples. In feed, the highest mean contamination levels were reported in the category Fish oil with 59 µg/kg, followed by 10 µg/kg in Feed for fur animals, pets and fish and 5.95 µg/kg in Aquatic animals, their products excluding fish oil. The mean contamination levels were below 1 µg/kg for most other feed groups. Detailed information on the contamination of feed is presented in Table

20 Table 10: Food group specific means of the sum of indicator PCBs and percentiles (µg/kg) using lower and upper bound. Food/feed group N LB/UB Mean P50 P95 P97.5 P99 Expressed on fat basis Meat and meat products ruminants 132 Meat and meat products poultry 111 Meat and meat products pigs 181 Liver and products terrestrial animals Raw milk and dairy products incl. butter 62 5,640 Hen eggs and egg products 721 Fat ruminants 143 Fat poultry 53 Fat pigs 40 Vegetable oils and fats 51 Marine oils 40 Infant and baby food without fish meat Infant and baby food containing fish meat Expressed on whole weight basis Muscle meat fish and fish products excl. eel ,834 Muscle meat eel 182 Fish liver 22 Fruits, vegetables and cereals 210 Expressed on fat, whole weight or unspecified basis Other products 759 LB UB LB UB LB UB LB UB LB UB LB UB LB UB LB UB LB UB LB UB LB ,084 1,285 UB ,084 1,285 LB UB LB UB LB UB LB , ,517 UB , ,517 LB UB LB UB LB UB

21 Table 11: A split of other foods into more detailed groups and their specific means for the sum of indicator PCBs and percentiles using lower and upper bound (µg/kg fat). Food group N LB/UB Mean P50 P90 P95 P97.5 P99 Horse meat 12 Horse fat 16 Game meat 76 Game fat 19 Meat and meat products not specified 183 Fat not specified 176 Offal and offal products 200 Honey 46 Food supplements 10 Other foods 21 LB UB LB UB LB UB LB UB LB ,765 UB ,765 LB UB LB UB LB UB LB UB LB UB

22 Table 12: Feed group specific means of the sum of indicator PCBs and percentiles (µg/kg fat) using lower and upper bound expressed on12% moisture basis. Feed group N LB/UB Mean P50 P95 P97.5 P99 Feed materials of plant origin excl. vegetable oils 262 Vegetable oils and their by-products 65 Feed materials of mineral origin 111 Animal fat, including milk fat and egg fat Other land animal products including milk, eggs and their products Fish oil 69 Aquatic animals, their products excl. fish oil and fish protein hydrolysates Additives binders and anti-caking agents Additives compounds of trace elements Premixtures 73 Compound feed, excl. feed for fur animals, pets and fish 359 Feed for fur animals, pets and fish 153 Other feed additives 5 Feed not specified 6 LB UB LB UB LB UB LB UB LB UB LB UB LB UB LB UB LB UB LB UB LB UB LB UB LB UB LB UB Contribution of single NDL-PCB congeners to the sum of the six indicators The overall mean contribution of the individual indicator NDL-PCBs (upper-bound) to the sum of the six followed the pattern PCB-153 > PCB-138 > PCB-180 > PCB-28 > PCB-101 > PCB-52 (mean ± SD in %: 31±12, 25±8, 15±7, 12±10, 11±8, 6±8, respectively) but relatively high variation was observed for each PCB as represented in Figure 3. These results are in line with findings reported in other studies which demonstrated that PCB-153 has an average contribution of roughly one third to the sum of the six indicator PCBs (EFSA, 2005; BFR, 2006; Jursa et al., 2006). In food, the mean contribution of PCB-153 and PCB-138 across food groups ranged from 23% to 44% and from 19% to 32%, respectively. Their contribution together was at least 50% in each food group (Table 13; Figure 4). PCB-180 and PCB-101 contributed between 10% and 29%, and 4% and 19%, respectively. PCB-52 and PCB-28 both contributed between 1% and 17% to the sum of the indicator NDL-PCBs. 22

23 Figure 3: Box-plot (whiskers at P5 and P95, box at P25 and P75 with line at P50) of the percentage contribution of the indicator PCBs to the sum in all food and feed samples (n=12,563). A similar pattern to food was observed in compound feed and feed groups containing animal products. However, a somewhat different profile was observed in feed of plant and mineral origin. In these feed groups the mean contribution of the individual PCBs ranged from 12% to 26% without following a specific pattern. It is noteworthy that in these groups the number of samples below LOQ was dominant and thus it was not possible to draw an accurate conclusion on the contribution of the single PCBs to the sum. In conclusion, a high variation in the contribution of each congener was observed throughout food and feed groups as reflected by the percentiles presented in Figures 5 to

24 Meat and meat products ruminants Meat and meat products poultry Meat and meat products pigs Liver and products terrestrial animals Muscle meat fish and fish products excluding eel Muscle meat eel Raw milk and dairy products incl. butter Hen eggs and egg products Fat ruminants Fat poultry Fat pigs Vegetable oils and fats Marine oils Fruits, vegetables and cereals Infant and baby food Fish liver Feed materials of plant origin excl. oils Vegetable oils and their by-products Feed materials of mineral origin Animal fat, including milk fat and egg fat Other land animal products including milk, eggs Fish oil Aquatic animals excl. fish oil and protein Additives binders and anti-caking agents Additives compounds of trace elements Premixtures Compound feed, excl. fur animals, pets and fish Feed for fur animals, pets and fish PCB 153 PCB 138 PCB 180 PCB 101 PCB 28 PCB Percentage Figure 4: Mean contribution (%) of the single NDL-PCBs to the overall sum for each food and feed group (upper-bound) 24

25 Table 13: Table 5. Mean contribution of the single NDL-PCBs to the sum for each food and feed group (upper bound). Basis for expression of results as presented in Food/feed group Sum PCB-28 PCB-52 PCB-101 PCB-138 PCB-153 PCB-180 µg/kg µg/kg % µg/kg % µg/kg % µg/kg % µg/kg % µg/kg % Meat and meat products ruminants Meat and meat products poultry Meat and meat products pigs Liver and products terrestrial animals Muscle meat fish and fish products excluding eel Muscle meat eel Raw milk and dairy products incl. butter Hen eggs and egg products Fat ruminants Fat poultry Fat pigs Vegetable oils and fats Marine oils Fish liver Other products Fruits, vegetables and cereals Infant and baby food Feed materials of plant origin excl. oils Vegetable oils and their by-products Feed materials of mineral origin Animal fat, including milk fat and egg fat Other land animal products including milk, eggs and their products Fish oil Aquatic animals excl. fish oil and protein Additives binders and anti-caking agents Additives compounds of trace elements Premixtures Compound feed, excl. fur animals, pets and fish Feed for fur animals, pets and fish Mean ± SD (calculated from individual data) 12±10 6±8 11±8 25±8 31±12 15±7 25

26 Figure 5: Box-plot (whiskers at P5 and P95, box at P25 and P75 with line at P50) of the percentage contribution of the PCB-28 to the sum of the six indicator PCBs across food and feed groups. Figure 6: Box-plot (whiskers at P5 and P95, box at P25 and P75 with line at P50) of the percentage contribution of the PCB-52 to the sum of the six indicator PCBs across food and feed groups. 26

27 Figure 7: Box-plot (whiskers at P5 and P95, box at P25 and P75 with line at P50) of the percentage contribution of the PCB-101 to the sum of the six indicator PCBs across food and feed groups. Figure 8: Box-plot (whiskers at P5 and P95, box at P25 and P75 with line at P50) of the percentage contribution of the PCB-138 to the sum of the six indicator PCBs across food and feed groups. 27

28 Figure 9: Box-plot (whiskers at P5 and P95, box at P25 and P75 with line at P50) of the percentage contribution of the PCB-153 to the sum of the six indicator PCBs across food and feed groups. Figure 10: Box-plot (whiskers at P5 and P95, box at P25 and P75 with line at P50) of the percentage contribution of the PCB-180 to the sum of the six indicator PCBs across food and feed groups. 28

29 Food/feed group (n) 4.5. Ratio between NDL-PCBs and DL-PCBs Monitoring of Non Dioxin-Like PCBs in Food and Feed For this exercise, samples for which data on both NDL-PCBs and dioxin and dioxin-like PCBs were available in EFSA s dioxin database were selected. Dioxin and DL-PCB data were used in preparing the report Results of the monitoring of dioxin levels in food and feed (EFSA, 2010). A subset of 4,652 samples contained complete information on all six indicator NDL-PCBs as well as on the 29 congeners of PCDD/F and DL-PCBs. The ratio between NDL-PCBs and DL-PCBs has been calculated for each sample. An overview on the ratios across food/feed groups is presented in Fig. 11. The analysis showed that the sum of the six NDL-PCBs were on average close to five times higher than the sum of the 12 DL-PCBs. This relationship varied across food groups and is presumably related to the origin of samples and the contamination source. Meat and meat products ruminants (58) Meat and meat products poultry (52) Meat and meat products pigs (37) Liver and products terrestrial animals (41) Muscle meat fish, fish products excl. eel (1465) Muscle meat eel (107) Raw milk, dairy products incl. butter (419) Hen eggs and egg products (446) Fat ruminants (78) Fat poultry (49) Fat pigs (34) Vegetable oils and fats (33) Marine oils (39) Other products (376) Fruits, vegetables and cereals (178) Infant and baby food (20) Fish liver (20) Feed materials of plant origin excl. oils (253) Vegetable oils and their by-products (65) Feed materials of mineral origin (107) Animal fat, including milk fat and egg fat (24) Other land animal products incl. milk, eggs (27) Fish oil (68) Aquatic animals excl. fish oil and protein (100) Additives binders and anti-caking agents (9) Additives compounds of trace elements (42) Premixtures (71) Compound feed, excl. fur animals, pets and fish (287) Feed for fur animals, pets and fish (141) Ratio NDL-PCB/DL-PCB Figure 11: Box-plot (whiskers at P5 and P95, box at P25 and P75 with line at P50) of the ratio between NDL-PCBs (sum of the six indicators) and DL-PCBs across food and feed groups. 29