DEFINITIVE ANNUAL REPORT Trace elements 2014

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EXPERTISE, SERVICE PROVISION AND CUSTOMER RELATIONS QUALITY OF MEDICAL LABORATORIES CLINICAL BIOLOGY COMMISSION COMMITTEE OF EXPERTS EXTERNAL QUALITY ASSESSMENT IN CLINICAL BIOLOGY DEFINITIVE ANNUAL REPORT Trace elements 2014 IPH-2014/Trace elements/06 Quality of medical laboratories J. Wytsmanstreet, 14 1050 Brussels Belgium www.wiv-isp.be

ISSN: 2294-3471 COMMITTEE OF EXPERTS IPH (secretariat) TEL: 026425521/5522 FAX: 026425645 Scheme coordinator: TEL: 026425385 Bernard China e-mail: bernard.china@wiv-isp.be Alternate coordinator: TEL: 026425535 Mohamed Rida e-mail: Mohamed.Soumali@wiv-isp.be Soumali Experts: Desmet Koen e-mail: koen.desmet@uzleuven.be Dubois Nathalie e-mail: nathalie.dubois@chu.ulg.ac.be Haufroid Vincent e-mail: vincent.haufroid@uclouvain.be Verstraete Alain e-mail: alain.verstraete@ugent.be Committee of experts: 01/07/2015 Authorisation to release report: By Bernard China, scheme coordinator, on 31/07/2015. All the reports are also available on our webpage: https://www.wiv-isp.be/qml/activities/external_quality/rapports/_nl/rapports_annee.htm https://www.wiv-isp.be/qml/activities/external_quality/rapports/_fr/rapports_annee.htm FORM 43/125/E V5 (date of application: 17/06/2015). 2/38

TABLE OF CONTENTS STATISTICS... 4 GRAPHICAL REPRESENTATION... 5 THE SAMPLES AND THE DATA PROCESSING... 6 PARTICIPATION... 6 1. HEAVY METALS IN SERUM... 7 1.1. PARTICIPATION... 7 1.2. GLOBAL RESULTS... 7 1.3. RESULTS PER ELEMENT... 8 1.3.1. Al... 8 1.3.2. Cu... 9 1.3.3. Li... 10 1.3.4. Se... 11 1.3.5. Zn... 12 1.3.6. Non evaluable elements... 13 2. TRACE ELEMENTS IN BLOOD... 15 2.1. PARTICIPATION... 15 2.2. GLOBAL RESULTS... 15 2.3. RESULTS PER ELEMENT... 16 2.3.1. Cd... 16 2.3.2. Co... 17 2.3.3. Hg... 18 2.3.4. Mn... 19 2.3.5. Pb... 20 2.3.6. Tl... 21 2.3.7. Non evaluable elements... 22 2. TRACE ELEMENTS IN URINE... 24 3.1. PARTICIPATION... 24 3.3 RESULTS PER ELEMENT... 25 3.3.1. As.... 25 3.3.2. Cd... 26 3.3.3. Co... 27 3.3.4.Cr... 28 3.3.5. Cu... 29 3.3.6. Hg... 30 3.3.7. Mg... 31 3.3.8. Mn... 32 3.3.9. Ni... 33 3.3.10. Pb... 34 3.3.11. Tl... 35 3.3.12. Zn... 36 3.3.13. Non evaluable elements... 37 FORM 43/125/E V5 (date of application: 17/06/2015). 3/38

Statistics For this annual report the following statistics were performed. The position of your quantitative results is given in comparison with all the results of all the participants and in comparison with the results of all the participants. The following information is given: Your result (R) The global median (M g ): the central value of the results obtained by all the laboratories confounded for all methods. In this report, the global median is considered as the target value. The global standard deviation (SD g ): It mmeasures of the dispersion of the results obtained by all the laboratories confounded for all methods. SD=(P75-P25)/1.349 The Z score: the difference between your result and the global median of your method, expressed as a Z g = (R - M g ) / SD g. NB : some additional information about the used statistics can be found on our web site : https://www.wivisp.be/qml/activities/external_quality/_down/_fr/methodes_statistiques_appliquees_a_eeq.pdf or https://www.wivisp.be/qml/activities/external_quality/_down/_nl/statistische_methoden_gebruikt_voor_eke.p df FORM 43/125/E V5 (date of application: 17/06/2015). 4/38

Graphical representation In addition to the tables of the results is a graphic in "Box et whisker" plot sometimes added. It contains the following elements for the methods with at least 6 participants: a rectangle that ranges from the percentile 25 (P 25 ) to the percentile 75 (P 75 ) a central line that shows the median of the results (P 50 ) a lower limit that shows the smallest value x > P 25-1.5 * (P 75 - P 25 ) an upper limit that shows the largest value x < P 75 + 1.5 * (P 75 - P 25 ) all points outside this interval are represented by a dot. x < P 75 + 1.5 * (P 75 -P 25 ) P 75 P 50 P 25 x > P 25-1.5 * (P 75 -P 25 ) < value < quantification limit FORM 43/125/E V5 (date of application: 17/06/2015). 5/38

The samples and the data processing 24 samples per matrix (Serum, whole blood, urine) were sent to the labs under dry ice (20/03/2014). The samples were purchased at SKML, Winterswijk, Netherlands. Two samples had to be analyzed per month from April 2014 to March 2015. The results were encoded via the web page: www.trace-elements.eu. The laboratories obtained from this site an individual report, a monthly report and an annual report. WIV-ISP produced individual annual reports and this global annual report. Participation 47 Belgian laboratories participated to the EQA (figure 1). 20 laboratories for Serum, blood and urine, 5 laboratoires for Serum and urine, 2 laboratories for blood and urine, 1 laboratory for serum and blood 18 laboratories for serum alone and 1 laboratory for urine alone. Figure 1. repartion (%) of the participants in function of the matrix analysed. FORM 43/125/E V5 (date of application: 17/06/2015). 6/38

1. Heavy metals in Serum 1.1. Participation 44 laboratories participated to the EQA for the quantification of trace elements in serum. Table 1.1. Number of participating laboratories per element Element N Recorded Total percentage Labs results results Al 10 206 240 85.83 Co* 5 103 120 85.83 Cr* 5 109 120 90.83 Cu 26 581 624 93.11 Li 8 170 192 88.54 Mg* 4 112 112 100.00 Se 14 290 336 86.31 Tl* 2 17 48 35.42 Zn 29 652 696 93.68 Total 2225 2472 90.01 *: when n<6, no evaluation was done 1.2. Global results Table 1.2. Global results per element Element Total number Number of of results evaluated results Number of Z citations % citations Al 206 206 25 12.14 Co 103 0 NA NA Cr 110 0 NA NA Cu 581 581 25 4.30 Li 170 170 9 5.29 Mg 96 0 NA NA Se 290 290 15 5.17 Tl 17 0 NA NA Zn 652 652 18 2.76 Total 2225 1899 92 4.84 NA : not applicable In 2014, the overall percentage of Z citation was 4.84. By comparison this percentage was 6.54 and 5.73 in 2012 and 2013, respectively. Nevertheless, those differences were not significant (p>0.05%). Al seems to be the most frequently cited element among the evaluated ones. FORM 43/125/E V5 (date of application: 17/06/2015). 7/38

1.3. Results per element 1.3.1. Al Table 1.3. Results per sample for the quantification of Al in serum Sample Median(µg/ L) SD (µg/l) N Z-citations % 2014.1 77.10 27.04 7 1 14.3 2014.2 98.80 27.28 7 1 14.3 2014.3 28.00 3.45 8 0 0 2014.4 93.38 6.02 8 1 12.5 2014.5 175.18 15.07 7 1 14.3 2014.6 59.00 4.74 7 1 14.3 2014.7 190.28 36.31 8 1 12.5 2014.8 113.40 10.44 9 2 22.2 2014.9 9.40 4.45 9 1 11.1 2014.10 125.50 12.08 9 2 22.2 2014.11 159.00 17.12 9 0 0 2014.12 47.50 1.93 9 2 22.2 2014.13 152.00 12.82 9 0 0 2014.14 185.50 20.68 9 1 11.1 2014.15 49.27 3.30 10 2 20 2014.16 8.10 2.68 10 0 0 2014.17 168.00 13.5 9 1 11.1 2014.18 63.40 8.22 9 1 11.1 2014.19 133.35 11.62 10 1 10 2014.20 196.40 13.27 9 1 11.1 2014.21 153.10 10.85 8 2 25 2014.22 32.00 4.80 7 1 14.3 2014.23 120.10 13.32 10 2 20 2014.24 81.90 9.34 9 0 0 Total evaluated 206 25 12.1 FORM 43/125/E V5 (date of application: 17/06/2015). 8/38

1.3.2. Cu Table 1.4. Results per sample for Cu in serum Sample Median (µg/l) SD (µg/l) N Z-citations % 2014.1 1584.00 106.01 25 2 8 2014.2 1770.00 168.65 25 1 4 2014.3 890.00 88.74 25 1 4 2014.4 1768.00 103.78 25 1 4 2014.5 2839.25 92.66 24 1 4.2 2014.6 1306.57 64.86 24 1 4.2 2014.7 3030.00 198.67 25 0 0 2014.8 1949.00 142.52 26 0 0 2014.9 720.00 53.74 23 1 4.3 2014.10 2238.00 149.33 23 0 0 2014.11 2645.00 269.09 26 0 0 2014.12 1150.00 89.7 26 1 3.8 2014.13 2500.40 160.86 25 0 0 2014.14 2920.00 203.71 25 0 0 2014.15 1124.18 97.7 25 1 4 2014.16 710.00 72.65 25 3 12 2014.17 2657.00 244.03 22 1 4.5 2014.18 1357.00 77.65 22 1 4.5 2014.19 2236.50 122.31 24 1 4.2 2014.20 3055.00 135.06 24 1 4.2 2014.21 2372.00 150.4 23 2 8.7 2014.22 890.00 45.96 23 4 17.4 2014.23 1970.28 121.94 23 0 0 2014.24 1531.00 77.97 23 1 4.3 Total evaluated 581 24 4.1 FORM 43/125/E V5 (date of application: 17/06/2015). 9/38

1.3.3. Li Values not shown on graph : 2014.16 (33.1) Table 1.5. Results per sample for the quantification of Li in Serum Sample Median (mg/l) SD N Z-citations % 2014.1 14.16 0.57 8 0 0 2014.2 12.32 0.8 8 0 0 2014.3 18.74 1.25 7 0 0 2014.4 12.21 0.41 7 0 0 2014.5 3.455 0.3 8 1 12.5 2014.6 15.55 0.29 8 0 0 2014.7 1.46 0.16 7 0 0 2014.8 10.13 0.24 7 1 14.3 2014.9 20.24 0.41 7 1 14.3 2014.10 8.47 0.22 7 1 14.3 2014.11 5.07 0.17 7 1 14.3 2014.12 17.21 1.21 7 1 14.3 2014.13 6.87 0.33 7 0 0 2014.14 3.33 0.17 7 0 0 2014.15 17.84 1.29 7 0 0 2014.16 21.86 1.7 7 1 14.3 2014.17 5.11 0.31 7 0 0 2014.18 15.55 0.36 7 1 14.3 2014.19 8.68 0.36 7 1 14.3 2014.20 1.64 0.3 7 0 0 2014.21 7.01 0.27 7 0 0 2014.22 19.22 0.9 7 0 0 2014.23 10.55 0.28 6 0 0 2014.24 13.92 0.4 6 0 0 Total evaluated 170 9 5.3 FORM 43/125/E V5 (date of application: 17/06/2015). 10/38

1.3.4. Se Values not shown on graph : 2014.16 (408) Table 1.6. Results per sample for the quantification of Se in Serum Sample median SD N Z-citations % 2014.1 176.55 18.01 12 0 0 2014.2 156.25 13.08 12 0 0 2014.3 242.80 10.03 14 1 7.1 2014.4 157.45 10.42 14 0 0 2014.5 46.00 5.34 13 0 0 2014.6 202.75 7.04 14 2 14.3 2014.7 22.15 4.34 10 1 10 2014.8 139.00 8.52 12 1 8.3 2014.9 272.10 30.45 12 0 0 2014.10 111.70 10.01 12 0 0 2014.11 68.00 6.82 13 1 7.7 2014.12 230.00 11.42 13 1 7.7 2014.13 85.00 9.98 13 1 7.7 2014.14 43.67 5.15 12 1 8.3 2014.15 220.40 22.98 12 1 8.3 2014.16 272.35 33.17 12 2 (16.7 2014.17 64.00 4.80 12 1 8.3 2014.18 200.60 16.31 12 0 0 2014.19 108.50 13.65 12 1 8.3 2014.20 24.50 6.13 10 1 10 2014.21 94.00 10.69 12 0 0 2014.22 246.10 15.05 11 0 0 2014.23 135.00 6.63 11 0 0 2014.24 180.60 13.45 10 0 0 Total evaluated 290 15 5.2 % FORM 43/125/E V5 (date of application: 17/06/2015). 11/38

1.3.5. Zn Values not shown on graph 2014.3 : 242.00 ; 2014.1 : 1.97 ; 2014.22 : 340.00 ; 2014.5 : 127.00 ; 2014.6 : 224.00 ; Table 1.7. Results per sample for the quantification of Zn in serum Sample median SD N Z-citations 2014.1 1934.71 179.97 28 1 (3.6 %) 2014.2 1823.50 160.31 28 0 (0 %) 2014.3 2289.50 178.84 28 2 (7.1 %) 2014.4 1820.95 107.12 28 0 (0 %) 2014.5 1225.00 84.32 28 1 (3.6 %) 2014.6 1980.00 113.68 27 1 (3.7 %) 2014.7 1096.50 77.71 28 0 (0 %) 2014.8 1669.00 77.84 29 3 (10.3 %) 2014.9 2377.00 161.37 26 0 (0 %) 2014.10 1559.00 85.06 26 0 (0 %) 2014.11 1346.00 101.56 29 0 (0 %) 2014.12 2160.00 168.28 29 0 (0 %) 2014.13 1464.46 109.9 28 0 (0 %) 2014.14 1228.16 110.82 28 1 (3.6 %) 2014.15 2095.5 133.8 28 1 (3.6 %) 2014.16 2360 142.7 28 1 (3.6 %) 2014.17 1321.08 111.2 25 1 (4 %) 2014.18 2007 200.15 25 1 (4 %) 2014.19 1584 113.34 27 0 (0 %) 2014.20 1102 93.4 27 1 (3.7 %) 2014.21 1432.26 84.6 25 2 (8 %) 2014.22 2212 134.92 25 1 (4 %) 2014.23 1681.5 185.07 26 1 (3.8 %) 2014.24 1893.3 142.2 26 0 (0 %) Total evaluated 652 18 (2.8 %) FORM 43/125/E V5 (date of application: 17/06/2015). 12/38

1.3.6. Non evaluable elements When the number of participants was below 6 for all of the samples, no statistics can be calculated and no evaluation can be done. It is the case in serum for : Co, Cr, Mg and Tl. Nevertheless, the results were plotted in function of the samples (see below). FORM 43/125/E V5 (date of application: 17/06/2015). 13/38

FORM 43/125/E V5 (date of application: 17/06/2015). 14/38

2. Trace elements in blood 2.1. Participation 23 laboratories encoded results for the quantification of trace elements in whole blood. Table 2.1. Number of Participating laboratories per element in whole blood Element N Labs Recorded results Total results Percentage Cd 14 253 336 75.30 Co 6 131 144 90.72 Cr 3* 72 72 100.00 Mg 2* 48 48 100.00 Mn 8 152 192 79.17 Hg 8 161 192 83.85 Pb 19 405 456 88.82 Se 3* 56 72 77.78 Zn 2* 48 48 100.00 Tl 6 140 144 97.22 total 1466 1704 86.03 * : when n<6, no evaluation was done 2.2. Global results Table 2.2. Global results per element for quantification in whole blood Elemen Total number Number of Number of Z citations % citations t of results evaluated results Cd 253 253 31 12.3 Co 131 66 8 12.1 Cr 72 0 NA NA Hg 161 161 12 7.5 Mg 48 0 NA NA Mn 152 134 5 3.7 Pb 405 405 32 7.9 Se 56 0 NA NA Tl 140 132 11 8.3 Zn 48 0 NA NA Total 1466 1151 99 8.6 NA : not applicable In 2014, the overall percentage of Z citations was 48.6. By comparison this percentage was 8.89 and 7.82 in 2012 and 2013, respectively. Nevertheless, those differences were not significant (p>0.05%). Cd and Co seem to be the most frequently cited elements (>12%) among the evaluated ones. FORM 43/125/E V5 (date of application: 17/06/2015). 15/38

2.3. Results per element 2.3.1. Cd Values not shown on graph : 2014.18 (13) Table 2.3. result per sample for the quantification of Cd in blood Sample Median SD N Z-citations % (µg/l) 2014.1 3.66 0.35 9 1 11.1 2014.2 4.14 0.45 9 2 22.2 2014.3 0.82 0.15 13 4 30.8 2014.4 4.36 0.32 14 2 14.3 2014.5 2.85 0.65 12 0 0 2014.6 6.90 1.30 12 0 0 2014.7 4.91 0.34 10 3 30 2014.8 1.49 0.19 10 1 10 2014.9 8.01 0.96 10 2 20 2014.10 7.66 1.18 10 0 0 2014.11 2.18 0.20 9 1 11.1 2014.12 6.15 0.59 9 2 22.2 2014.13 5.42 0.45 10 1 10 2014.14 4.91 0.38 10 1 10 2014.15 0.84 0.26 10 1 10 2014.16 2.13 0.34 10 1 10 2014.17 6.21 0.72 10 2 20 2014.18 8.07 1.12 10 1 10 2014.19 7.05 0.90 12 0 0 2014.20 5.75 0.73 12 0 0 2014.21 1.52 0.16 10 0 0 2014.22 2.85 0.15 10 2 20 2014.23 7.55 0.81 11 2 18.2 2014.24 3.4 0.31 11 2 18.2 Total evaluated 253 31 12.3 FORM 43/125/E V5 (date of application: 17/06/2015). 16/38

2.3.2. Co Values not shown on graph : 2014.10 (30.8) Table 2.4. results per sample for the quantification of Co in blood Sample Median SD N Z-citations % µg/l 2014.1 NA NA 5 NA NA 2014.2 NA NA 5 NA NA 2014.3 NA NA 5 NA NA 2014.4 3.93 0.35 6 1 16.7 2014.5 2.67 0.47 6 0 0 2014.6 7.15 0.52 6 0 0 2014.7 4.41 0.47 6 1 16.7 2014.8 NA NA 5 NA NA 2014.9 NA NA 5 NA NA 2014.10 NA NA 5 NA NA 2014.11 NA NA 5 NA NA 2014.12 NA NA 5 NA NA 2014.13 5.27 0.24 6 2 33.3 2014.14 4.89 0.54 6 0 0 2014.15 NA NA 5 NA NA 2014.16 NA NA 5 NA NA 2014.17 NA NA 5 NA NA 2014.18 NA NA 5 NA NA 2014.19 6.81 0.65 6 2 33.3 2014.20 5.41 0.5 6 1 16.7 2014.21 NA NA 5 NA NA 2014.22 2.60 0.38 6 0 0 2014.23 7.46 0.46 6 0 0 2014.24 3.30 0.26 6 1 16.7 Total evaluated 66 8 12.1 NA : not applicable FORM 43/125/E V5 (date of application: 17/06/2015). 17/38

2.3.3. Hg Value not shown on graph : 2014.2 (364) Table 2.5. results per sample for the quantification of Hg in blood Sample Median (µg/l) SD N Z-citations % 2014.1 50.86 10.01 6 2 33.3 2014.2 58.12 18.89 6 1 16.7 2014.3 1.10 0.29 6 1 16.7 2014.4 63.44 8.64 6 0 0 2014.5 39.45 5.06 6 0 0 2014.6 114.85 18.79 7 0 0 2014.7 73.19 7.52 7 1 14.3 2014.8 12.92 1.59 7 0 0 2014.9 146.55 16.28 6 0 0 2014.10 131.16 27.14 7 0 0 2014.11 25.80 0.98 6 1 16.7 2014.12 102.60 4.87 6 0 0 2014.13 91.00 11.62 7 1 14.3 2014.14 78.62 6.09 7 1 14.3 2014.15 0.83 0.25 6 1 16.7 2014.16 24.30 4.04 7 1 14.3 2014.17 110.00 16.86 7 0 0 2014.18 146.00 22.76 7 0 0 2014.19 123.15 19.94 8 1 12.5 2014.20 91.27 12.9 8 1 12.5 2014.21 12.73 1.27 7 0 0 2014.22 39.80 5.65 7 0 0 2014.23 128.60 21.05 7 0 0 2014.24 53.62 8.27 7 0 0 Total evaluated 161 12 7.5 FORM 43/125/E V5 (date of application: 17/06/2015). 18/38

2.3.4. Mn Table 2.6. Results per sample for the quantification of Mn in blood Sample Median SD N Z-citations (µg/l) 2014.1 NA NA 4 NA NA 2014.2 NA NA 4 NA NA 2014.3 12.1 0.60 7 0 0 2014.4 25.4 2.09 7 0 0 2014.5 20.58 1.58 7 0 0 2014.6 37.17 2.99 7 0 0 2014.7 28.80 0.70 7 0 0 2014.8 15.30 1.48 7 0 0 2014.9 NA NA 5 NA NA 2014.10 NA NA 5 NA NA 2014.11 19.95 2.20 6 0 0 2014.12 35.40 3.81 6 0 0 2014.13 30.43 2.54 7 0 0 2014.14 28.18 1.61 7 0 0 2014.15 12.94 0.78 6 0 0 2014.16 17.66 0.84 6 1 16.7 2014.17 35.10 1.67 7 0 0 2014.18 41.80 1.96 7 0 0 2014.19 35.06 2.67 8 0 0 2014.20 30.85 2.5 8 0 0 2014.21 15.35 0.96 6 1 16.7 2014.22 20.90 1.27 6 1 16.7 2014.23 38.29 3.47 6 1 16.7 2014.24 22.81 1.99 6 1 16.7 Total evaluated 134 5 3.7 NA : not applicable FORM 43/125/E V5 (date of application: 17/06/2015). 19/38

2.3.5. Pb Value not shown on graph : 2014.3 (1200) Table 2.7. Results per sample for the quantification of Pb in whole blood Sample Median (µg/l) SD N Z-citations % 2014.1 501.00 46.15 18 0 0 2014.2 440.75 39.94 18 1 5.6 2014.3 776.00 61.42 19 1 5.3 2014.4 427.00 23.46 19 2 10.5 2014.5 555.86 48.15 18 2 11.1 2014.6 162.50 10.58 18 1 5.6 2014.7 382.75 37.55 18 1 5.6 2014.8 696.17 75.56 18 1 5.6 2014.9 19.56 2.42 16 2 12.5 2014.10 88.65 13.46 16 2 12.5 2014.11 647.50 31.39 15 3 20 2014.12 235.20 35.73 15 0 0 2014.13 297.00 20.98 17 1 5.9 2014.14 369.00 32.36 17 1 5.9 2014.15 722.00 74.2 17 2 11.8 2014.16 614.25 71.91 17 2 11.8 2014.17 227.40 15.2 16 1 6.2 2014.18 19.98 3.17 15 1 6.7 2014.19 157.00 17.05 17 2 11.8 2014.20 286.00 24.46 17 3 17.6 2014.21 692.95 46.53 16 1 6.2 2014.22 555.36 34.45 16 1 6.2 2014.23 87.60 14.69 16 1 6.2 2014.24 492.25 33.86 16 0 0 Total evaluated 405 32 7.9 FORM 43/125/E V5 (date of application: 17/06/2015). 20/38

2.3.6. Tl Table 2.8. Results per sample for the quantification of Tl in whole blood Sample median SD N Z-citations % 2014.1 NA NA 4 NA NA 2014.2 NA NA 4 NA NA 2014.3 0.15 0.12 6 0 0 2014.4 1.90 0.06 6 1 16.7 2014.5 1.10 0.09 6 2 33.3 2014.6 3.05 0.16 6 1 16.7 2014.7 2.04 0.13 6 0 0 2014.8 0.45 0.09 6 0 0 2014.9 3.73 0.18 6 1 16.7 2014.10 3.40 0.17 6 0 0 2014.11 0.73 0.04 6 1 16.7 2014.12 2.65 0.19 6 0 0 2014.13 2.40 0.11 6 0 0 2014.14 2.00 0.07 6 0 0 2014.15 0.10 0.02 6 1 16.7 2014.16 0.75 0.07 6 0 0 2014.17 2.80 0.08 6 0 0 2014.18 3.71 0.20 6 0 0 2014.19 3.07 0.11 6 1 16.7 2014.20 2.37 0.11 6 1 16.7 2014.21 0.42 0.06 6 1 16.7 2014.22 1.09 0.03 6 1 16.7 2014.23 3.42 0.20 6 0 0 2014.24 1.40 0.13 6 0 0 Total evaluated 132 11 8.3 FORM 43/125/E V5 (date of application: 17/06/2015). 21/38

2.3.7. Non evaluable elements When n<6, the statistics where not calculated and no evaluation was performed. In whole blood this was the case for Cr, Mg, Se and Zn. Nevertheless, the individual results are shown here after. FORM 43/125/E V5 (date of application: 17/06/2015). 22/38

FORM 43/125/E V5 (date of application: 17/06/2015). 23/38

2. Trace elements in urine 3.1. Participation 28 laboratories encoded results for the matrix urine. The percentage of response was 84%. Table 3.1. Participation per element Recorded Parameter N Labs results Total results percentage As 6 135 144 93.75 Co 10 204 240 86.44 Cd 11 217 264 85.23 Cr 11 225 264 85.23 Cu 14 287 336 85.42 Se* 4* 78 96 81.25 Hg 7 152 168 84.52 Mg 7 139 168 84.52 Mn 9 187 216 88.42 Ni 10 212 240 88.33 Pb 16 299 384 78.65 Tl 7 134 168 79.76 V* 3 69 72 95.83 I* 2 44 48 100.00 Zn 15 283 360 80.00 Total 2663 3168 84.06 *: when n<6, no evaluation was performed 3.2. Global results Table 3.2. Global results per element for the quantification in urine Elemen Total number Number of Number of Z citations % citations t of results evaluated results As 135 85 6 7.1 Cd 217 217 24 11.1 Co 204 204 14 6.9 Cr 225 225 33 14.7 Cu 287 287 30 10.5 Hg 152 142 14 9.9 Mg 139 124 8 6.5 I 44 0 NA NA Mn 187 187 17 9.1 Ni 212 212 25 11.8 Pb 299 299 30 10 Se 78 0 NA NA Tl 132 72 8 11.1 V 69 0 NA NA Zn 283 283 33 11.7 Total 2663 2337 242 10.4 The global percentage of Z citations for urine in 2014 was 10.4. By comparison, the percentage of Z citations was 9.28 and 9.72 in 2012 and 2013, respectively. Cr seems to be subject to the biggest number of z-citations (14.7%). FORM 43/125/E V5 (date of application: 17/06/2015). 24/38

3.3 results per element 3.3.1. As. Table 3.3. Results per sample for the quantification of As in urine Sample median SD N Z-citations % 2014.1 NA NA 5 NA NA 2014.2 NA NA 5 NA NA 2014.3 NA NA 5 NA NA 2014.4 NA NA 5 NA NA 2014.5 38.1 4.46 6 0 0 2014.6 56.4 6.76 6 0 0 2014.7 82.12 13.54 6 0 0 2014.8 113.05 18.09 6 0 0 2014.9 94.37 5.97 6 1 16.7 2014.10 44.75 3.47 6 1 16.7 2014.11 29.75 2.94 6 0 0 2014.12 109.8 8.11 6 0 0 2014.13 88.26 5.93 6 0 0 2014.14 114.7 5.55 6 0 0 2014.15 NA NA 5 NA NA 2014.16 NA NA 5 NA NA 2014.17 45.2 5.06 7 1 14.3 2014.18 81.9 4.41 6 2 33.3 2014.19 NA NA 5 NA NA 2014.20 NA NA 5 NA NA 2014.21 51.7 4.21 6 1 16.7 2014.22 NA NA 5 NA NA 2014.23 99.85 6.83 6 0 0 2014.24 NA NA 5 NA NA Total evaluated 0 NA NA FORM 43/125/E V5 (date of application: 17/06/2015). 25/38

3.3.2. Cd Table 3.4. Result per sample for the quantification of Cd in urine Sample median SD N Z-citations % 2014.1 3.70 0.3 10 0 0 2014.2 4.39 0.37 10 0 0 2014.3 7.97 0.59 10 0 0 2014.4 4.31 0.28 10 0 0 2014.5 6.40 0.65 11 0 0 2014.6 5.08 0.4 11 1 9.1 2014.7 2.97 0.16 9 3 33.3 2014.8 0.29 0.17 8 1 12.5 2014.9 1.66 0.06 9 1 11.1 2014.10 5.60 0.32 9 1 11.1 2014.11 7.28 0.82 10 0 0 2014.12 0.99 0.19 10 1 10 2014.13 2.40 0.12 10 1 10 2014.14 0.27 0.13 10 1 10 2014.15 2.97 0.07 8 1 12.5 2014.16 6.95 0.35 8 1 12.5 2014.17 5.68 0.2 7 2 28.6 2014.18 2.45 0.63 8 2 25 2014.19 7.43 0.52 8 1 12.5 2014.20 0.93 0.06 7 1 14.3 2014.21 4.84 0.42 8 1 12.5 2014.22 6.10 0.41 9 2 22.2 2014.23 1.66 0.18 8 1 12.5 2014.24 3.55 0.26 9 2 22.2 Total evaluated 217 24 11.1 FORM 43/125/E V5 (date of application: 17/06/2015). 26/38

3.3.3. Co Values not shown on graph 2014.3 52.4 Table 3.5. Results per sample for the quantification of Co in urine Sample Median (µg/l) SD N Z-citations % 2014.1 13.00 0.94 10 0 0 2014.2 15.40 1.73 10 0 0 2014.3 29.56 2.8 8 1 12.5 2014.4 15.26 1.43 8 1 12.5 2014.5 24.10 1.63 9 1 11.1 2014.6 19.45 1.23 8 2 25 2014.7 10.42 1.26 9 2 22.2 2014.8 0.20 0.37 9 1 11.1 2014.9 5.42 0.65 8 1 12.5 2014.10 21.09 2.39 8 2 25 2014.11 26.10 3.26 9 0 0 2014.12 2.85 0.23 8 0 0 2014.13 7.80 0.39 9 2 22.2 2014.14 0.24 0.11 8 0 0 2014.15 10.25 1.04 8 0 0 2014.16 25.89 2.19 8 0 0 2014.17 21.08 2.38 8 0 0 2014.18 8.10 1.07 9 0 0 2014.19 27.70 3.69 8 0 0 2014.20 2.65 0.33 8 0 0 2014.21 17.70 1.98 8 0 0 2014.22 23.00 1.41 9 1 11.1 2014.23 4.92 0.96 8 0 0 2014.24 12.80 2.08 9 0 0 Total evaluated 204 14 6.9 FORM 43/125/E V5 (date of application: 17/06/2015). 27/38

3.3.4.Cr Table 3.6. Results per sample for the quantification of Cr in urine Sample median SD N Z-citations % 2014.1 16.32 1.31 11 0 0 2014.2 13.00 1.1 11 0 0 2014.3 0.34 0.17 8 0 0 2014.4 13.60 1.76 10 1 10 2014.5 5.70 0.49 11 2 18.2 2014.6 10.54 0.74 11 2 18.2 2014.7 18.31 1.95 10 1 10 2014.8 27.91 0.64 9 4 44.4 2014.9 24.30 1.78 9 2 22.2 2014.10 8.70 0.84 9 4 44.4 2014.11 2.87 0.61 10 1 10 2014.12 25.70 3.58 10 1 10 2014.13 21.56 0.57 10 2 20 2014.14 29.70 0.68 10 3 30 2014.15 18.84 0.73 9 1 11.1 2014.16 2.90 0.06 8 2 25 2014.17 8.25 1.11 8 0 0 2014.18 21.90 3.89 9 1 11.1 2014.19 0.33 0.42 8 1 12.5 2014.20 26.09 0.52 10 3 30 2014.21 10.61 0.98 8 0 0 2014.22 5.80 0.74 9 2 22.2 2014.23 24.64 3.57 8 0 0 2014.24 17.50 2.22 9 0 0 Total evaluated 225 33 14.7 FORM 43/125/E V5 (date of application: 17/06/2015). 28/38

3.3.5. Cu Values not shown on graph 2014.10 : 934.38 ; 2014.3 : 901.00 ; 2014.22 : 810.00 ; Table 3.7. Results per sample for the quantification of Cu in urine Sample median SD N Z-citations % 2014.1 212.50 23.43 14 2 14.3 2014.2 242.60 34.36 14 0 0 2014.3 420.79 54.89 11 1 9.1 2014.4 240.55 28.10 11 1 9.1 2014.5 345.00 65.98 11 1 9.1 2014.6 269.00 40.73 11 1 9.1 2014.7 165.70 21.58 12 2 16.7 2014.8 29.14 10.08 12 3 25 2014.9 95.60 8.76 11 3 27.3 2014.10 303.60 34.29 11 2 18.2 2014.11 380.20 17.09 13 3 23.1 2014.12 62.60 12.86 13 0 0 2014.13 133.75 11.60 12 0 0 2014.14 26.03 8.02 12 2 16.7 2014.15 165.00 16.09 12 0 0 2014.16 376.50 25.72 12 0 0 2014.17 301.10 41.81 11 0 0 2014.18 130.30 17.29 12 0 0 2014.19 390.16 40.99 12 2 16.7 2014.20 61.74 8.45 13 1 7.7 2014.21 265.00 32.47 11 1 9.1 2014.22 343.80 29.17 11 1 9.1 2014.23 101.85 16.56 12 1 8.3 2014.24 201.00 15.80 13 3 23.1 Total evaluated 287 30 10.5 FORM 43/125/E V5 (date of application: 17/06/2015). 29/38

3.3.6. Hg Values not shown on graph : 2014.7 (429)-2014.8 (640) Table 3.8. Results per sample for the quantification of Hg in Urine Sample Median SD N Z-citations % 2014.1 74.4 7.15 7 1 14.3 2014.2 61.3 6.82 7 1 14.3 2014.3 NA NA 5 NA NA 2014.4 NA NA 5 NA NA 2014.5 22.48 4.16 6 1 16.7 2014.6 47.03 8.65 6 1 16.7 2014.7 87.00 29.35 7 1 14.3 2014.8 136.48 45.82 7 1 14.3 2014.9 98.66 8.98 6 1 16.7 2014.10 34.98 1.46 6 1 16.7 2014.11 12.05 0.88 6 0 0 2014.12 114.63 3.36 6 1 16.7 2014.13 90.52 7.49 6 0 0 2014.14 122.96 18.53 6 0 0 2014.15 73.05 5.19 6 0 0 2014.16 11.45 0.98 6 1 16.7 2014.17 35.69 2.94 6 1 16.7 2014.18 83.95 16.25 6 1 16.7 2014.19 0.32 0.24 7 1 14.3 2014.20 121.20 31.49 7 0 0 2014.21 45.90 2.06 7 1 14.3 2014.22 23.60 1.20 7 0 0 2014.23 103.6 13.77 7 0 0 2014.24 68.14 7.46 7 0 0 Total evaluated 142 14 FORM 43/125/E V5 (date of application: 17/06/2015). 30/38

3.3.7. Mg Values not shown on graph 2014.9 : 235.32 ; 2014.10 : 409.11 ; 2014.13 : 1035.18 ; Table 3.9. Results per sample for the quantification of Mg in urine Sample Median SD N Z-citations % 2014.1 98.39 2.28 6 0 0 2014.2 100.90 6.01 6 1 16.7 2014.3 NA NA 5 NA NA 2014.4 NA NA 5 NA NA 2014.5 113.36 23.03 6 0 0 2014.6 104.74 18.25 6 0 0 2014.7 90.27 3.69 6 1 16.7 2014.8 73.34 2.32 6 1 16.7 2014.9 84.08 8.13 6 1 16.7 2014.10 110.08 11.51 6 1 16.7 2014.11 NA NA 5 NA NA 2014.12 NA NA 5 NA NA 2014.13 NA NA 5 NA NA 2014.14 72.30 4.47 6 0 0 2014.15 86.86 7.70 6 0 0 2014.16 113.12 1.67 6 1 16.7 2014.17 105.71 10.9 6 1 16.7 2014.18 89.29 5.08 6 0 0 2014.19 118.59 5.29 6 0 0 2014.20 76.67 6.98 6 0 0 2014.21 104.52 4.06 6 0 0 2014.22 112.00 4.48 6 0 0 2014.23 81.77 1.31 6 0 0 2014.24 94.72 3.40 6 0 0 Total evaluated 124 8 FORM 43/125/E V5 (date of application: 17/06/2015). 31/38

3.3.8. Mn n=9 n=6 n=9 n=9 n=6 n=9 n=9 n=7 n=7 n=8 n=7 n=7 2014.1 2014.2 2014.3 2014.4 2014.5 2014.6 2014.7 2014.8 2014.9 2014.10 2014.11 2014.12 2014.13 2014.14 2014.15 2014.16 2014.17 2014.18 2014.19 2014.20 2014.21 2014.22 2014.23 2014.24 Mn (µg/l) 0 5 10 15 20 25 30 35 Tableau 3.10. Results per sample for the quantification of Mn in urine Sample median SD N Z-citations % 2014.1 16.23 3.23 9 0 0 2014.2 13.3 1.97 9 0 0 2014.3 0.195 0.46 6 1 16.7 2014.4 14.07 1.38 6 1 16.7 2014.5 7.13 1.33 9 0 0 2014.6 12.16 1.35 9 2 22.2 2014.7 19.93 1.61 9 1 11.1 2014.8 28.76 2.63 8 1 12.5 2014.9 24.55 4.19 6 0 0 2014.10 8.71 2.87 6 0 0 2014.11 2.83 0.31 9 2 22.2 2014.12 27.47 4.06 8 0 0 2014.13 21.57 0.99 9 1 11.1 2014.14 28.90 1.04 9 1 11.1 2014.15 19.30 1.95 7 0 0 2014.16 2.97 0.74 7 0 0 2014.17 8.70 1.42 7 1 14.3 2014.18 21.94 3.08 8 0 0 2014.19 0.70 0.65 8 1 12.5 2014.20 27.77 3.50 8 0 0 2014.21 10.16 0.62 7 2 28.6 2014.22 5.60 0.86 8 1 12.5 2014.23 23.79 1.99 7 1 14.3 2014.24 16.26 1.20 8 1 12.5 Total evaluated 187 17 9.1 FORM 43/125/E V5 (date of application: 17/06/2015). 32/38

3.3.9. Ni n=10 n=8 n=9 n=10 n=7 n=9 n=10 n=9 n=7 n=9 n=8 n=8 2014.1 2014.2 2014.3 2014.4 2014.5 2014.6 2014.7 2014.8 2014.9 2014.10 2014.11 2014.12 2014.13 2014.14 2014.15 2014.16 2014.17 2014.18 2014.19 2014.20 2014.21 2014.22 2014.23 2014.24 Ni (µg/l) 0 20 40 60 80 Values not shown on graph : 2014.14 (95) and 2014.13 (116.6) Table 3.11. Results per sample for the quantification of Ni in urine Sample median SD N Z-citations % 2014.1 32.60 4.74 10 0 0 2014.2 26.58 2.63 10 1 10 2014.3 0.93 1.63 8 0 0 2014.4 27.34 2.22 8 2 25 2014.5 12.20 2.61 9 0 0 2014.6 21.30 3.39 9 1 11.1 2014.7 35.68 3.55 10 0 0 2014.8 56.41 6.86 10 2 20 2014.9 46.68 5.21 7 0 0 2014.10 16.00 2.74 7 1 14.3 2014.11 6.00 1.19 9 1 11.1 2014.12 49.30 5.97 9 0 0 2014.13 42.61 3.2 10 2 20 2014.14 59.03 3.61 10 3 30 2014.15 35.70 3.71 9 1 11.1 2014.16 5.70 0.66 9 3 33.3 2014.17 16.90 2.26 7 1 14.3 2014.18 41.85 4.67 8 0 0 2014.19 1.46 2.12 9 0 0 2014.20 53.50 4.02 10 1 10 2014.21 21.85 2.61 8 2 25 2014.22 12.30 1.04 9 3 33.3 2014.23 47.55 6.11 8 0 0 2014.24 30.9 3.4 9 1 11.1 Total evaluated 212 25 11.8 FORM 43/125/E V5 (date of application: 17/06/2015). 33/38

3.3.10. Pb n=11 n=14 n=14 n=13 n=12 n=12 n=11 n=12 n=12 n=13 n=12 n=12 2014.1 2014.2 2014.3 2014.4 2014.5 2014.6 2014.7 2014.8 2014.9 2014.10 2014.11 2014.12 2014.13 2014.14 2014.15 2014.16 2014.17 2014.18 2014.19 2014.20 2014.21 2014.22 2014.23 2014.24 Pb (µg/l) 0 50 100 150 Values not shown on graph : 2014.10 (258), 2014.19 (531) Table 3.12. Results per sample for the quantification of Pb in urine Sample median SD N Z-citations % 2014.1 64.40 3.24 11 3 27.3 2014.2 75.50 2.87 11 3 27.3 2014.3 138.50 9.56 14 2 14.3 2014.4 75.00 2.88 14 3 21.4 2014.5 112.25 13.49 14 0 0 2014.6 87.94 7.65 14 1 7.1 2014.7 51.20 7.41 13 0 0 2014.8 1.50 2.97 13 3 23.1 2014.9 27.14 3.66 12 0 0 2014.10 104.45 10.23 12 3 25 2014.11 126.30 20.96 12 1 8.3 2014.12 13.39 1.83 12 1 8.3 2014.13 39.00 3.41 11 0 0 2014.14 1.36 0.92 11 2 18.2 2014.15 52.12 5.54 12 1 8.3 2014.16 123.68 8.95 12 3 25 2014.17 104.00 9.72 12 0 0 2014.18 39.33 3.34 13 1 7.7 2014.19 141.00 16.75 13 2 15.4 2014.20 13.00 2.74 13 1 7.7 2014.21 82.95 10.40 12 0 0 2014.22 112.30 8.15 13 0 0 2014.23 27.85 4.54 12 0 0 2014.24 62.63 5.78 13 0 0 Total evaluated 299 30 0 FORM 43/125/E V5 (date of application: 17/06/2015). 34/38

3.3.11. Tl n=5 n=5 n=6 n=6 n=6 n=6 n=6 n=5 n=5 n=5 n=5 n=5 2014.1 2014.2 2014.3 2014.4 2014.5 2014.6 2014.7 2014.8 2014.9 2014.10 2014.11 2014.12 2014.13 2014.14 2014.15 2014.16 2014.17 2014.18 2014.19 2014.20 2014.21 2014.22 2014.23 2014.24 Tl (µg/l) 0 1 2 3 4 5 Table 3.13. Results per sample for the quantification of Tl in urine Sample median SD N Z-citations % 2014.1 NA NA 5 NA NA 2014.2 NA NA 5 NA NA 2014.3 NA NA 5 NA NA 2014.4 NA NA 5 NA NA 2014.5 1.02 0.24 6 0 0 2014.6 1.67 0.32 6 0 0 2014.7 2.66 0.15 6 2 33.3 2014.8 3.84 0.37 6 0 0 2014.9 3.17 0.31 6 1 16.7 2014.10 1.10 0.26 6 1 16.7 2014.11 0.52 0.16 6 0 0 2014.12 NA NA 5 NA NA 2014.13 2.92 0.09 6 1 16.7 2014.14 4.01 0.21 6 1 16.7 2014.15 NA NA 5 NA NA 2014.16 NA NA 5 NA NA 2014.17 NA NA 5 NA NA 2014.18 2.95 0.12 6 0 0 2014.19 NA NA 5 NA NA 2014.20 NA NA 5 NA NA 2014.21 NA NA 5 NA NA 2014.22 0.93 0.1 6 0 0 2014.23 NA NA 5 NA NA 2014.24 2.27 0.04 6 2 33.3 Total evaluated 72 8 FORM 43/125/E V5 (date of application: 17/06/2015). 35/38

3.3.12. Zn n=13 n=11 n=10 n=13 n=11 n=13 n=12 n=12 n=10 n=12 n=11 n=13 2014.1 2014.2 2014.3 2014.4 2014.5 2014.6 2014.7 2014.8 2014.9 2014.10 2014.11 2014.12 2014.13 2014.14 2014.15 2014.16 2014.17 2014.18 2014.19 2014.20 2014.21 2014.22 2014.23 2014.24 Zn (mg/l) 0 1 2 3 4 Table 3.14. Results per sample for the quantification of Zn in urine Sample median SD N Z-citations % 2014.1 1.75 0.14 13 1 7.7 2014.2 1.95 0.16 13 1 7.7 2014.3 3.38 0.14 11 2 18.2 2014.4 2.03 0.14 12 1 8.3 2014.5 2.75 0.20 10 1 10 2014.6 2.22 0.07 10 1 10 2014.7 1.43 0.05 13 2 15.4 2014.8 0.43 0.03 13 2 15.4 2014.9 0.96 0.15 11 2 18.2 2014.10 2.45 0.30 11 2 18.2 2014.11 3.04 0.21 13 2 15.4 2014.12 0.71 0.03 13 2 15.4 2014.13 1.18 0.05 12 2 16.7 2014.14 0.43 0.03 12 1 8.3 2014.15 1.40 0.03 12 3 25 2014.16 2.90 0.11 12 2 16.7 2014.17 2.33 0.15 10 1 10 2014.18 1.12 0.08 10 0 0 2014.19 3.07 0.27 12 1 8.3 2014.20 0.65 0.06 13 2 15.4 2014.21 2.11 0.13 11 0 0 2014.22 2.62 0.24 10 0 0 2014.23 0.88 0.11 13 1 7.7 2014.24 1.65 0.15 13 1 7.7 Total evaluated 283 33 11.7 FORM 43/125/E V5 (date of application: 17/06/2015). 36/38

3.3.13. Non evaluable elements When the number of participants is lower than 6, no evaluation was performed. It is the case for I, Se and V in urine. Nevertheless, the individual results are shown on graphs here after. n=3 n=3 n=4 n=3 n=4 n=4 n=4 n=4 n=3 n=3 n=4 n=3 n=4 n=4 n=3 n=3 n=4 n=3 n=3 n=3 n=3 n=2 n=2 n=2 2014.1 2014.2 2014.3 2014.4 2014.5 2014.6 2014.7 2014.8 2014.9 2014.10 2014.11 2014.12 2014.13 2014.14 2014.15 2014.16 2014.17 2014.18 2014.19 2014.20 2014.21 2014.22 2014.23 2014.24 Se (µg/l) 0 20 40 60 80 100 120 FORM 43/125/E V5 (date of application: 17/06/2015). 37/38

n=3 n=3 n=3 n=3 n=3 n=3 n=3 n=3 n=3 n=3 n=3 n=3 n=3 n=3 n=3 n=3 n=2 n=3 n=3 n=3 n=2 n=3 n=2 n=3 2014.1 2014.2 2014.3 2014.4 2014.5 2014.6 2014.7 2014.8 2014.9 2014.10 2014.11 2014.12 2014.13 2014.14 2014.15 2014.16 2014.17 2014.18 2014.19 2014.20 2014.21 2014.22 2014.23 2014.24 V (µg/l) 0 5 10 15 20 END. Scientific Institute of Public Health, Brussels 2015. This report may not be reproduced, published or distributed without the consent of the WIV-ISP. FORM 43/125/E V5 (date of application: 17/06/2015). 38/38