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Appendix 1 Trends of persistent organic pollutants (POPs) in humans, food and wildlife Statistical methods and figure legends

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Appendix 1

Trends of persistent organic pollutants (POPs) in humans, food and wildlife

Statistical methods and figure legends

Extreme values may have strong detrimental effect on the statistical power to detect trends but also affect the trend itself if the extreme value are situated in the beginning or at the end of the time series and thus exerting a strong leverage effect. Potential outliers are detected using the Tukey's outer fence (see e.g. Foreman, 2014). The inter- quartile range (IQR) is achieved from a given window of values, this reduce a potential trend (linear or non-linear) to cause deviating concentrations. To make the outlier detection less sensitive, the outer fence was moved from the suggested 3*IQR to 6*IQR. Only really extreme values are reported. Extremes have been excluded after checking the data. If so, this is mentioned in the figures.

Slope = reports the annual change in percent per year with a 95% confidence interval. This change is based on a log- linear regression analysis.

CV(lr) = Coefficient of variation for residuals around the log-linear regression line. A comparison of CV(lr) before and after adjustment for covariates gives information about the effect of adjustment.

LDT(d)= the smallest slope that can be detected with 80% power during a 10-year period, using the average sample size per year. LDT(c)= the smallest slope for the current time-series.

YRQ= minimum n of years required to detect a 5% annual change with a power of 80%

Y(17) = is the estimated geometric mean concentration year 2017, together with a 95% confidence interval

r2=, p= is the Coefficient of Determination (the proportion of the variation, explained by the regression: concentration over time) together with the corresponding p-value.

An alternative to the regression line in order to describe the development over time is a smoothed line. The smoother applied here is a simple 3-point running mean smoother fitted to the annual geometric mean values. In cases where the regression line is badly fitted the smoothed line may be more appropriate. The significance of this line is tested by means of an Analysis of Variance where the variance explained by the smoother and by the regression line is

compared with the total variance. This procedure is used at assessments at ICES and is described by Nicholson et al., 1998.

CV(sm), %, p, %= reports the Coefficient of Variation for the residuals around a smoother (3- or 5 point running mean). If the smoother explains significantly more than the regression line (p<0.05) it is considered significant and is plotted (red smoothed line)

Cp = , p= reports results of a Change-Point analysis (Sturludottir et al., 2014) that tries to detect a significant change- point in the time-series. The year of the change-point and the p-value are reported . The CP-analyses were only carried out for time-series longer than 8 years.

Pw(c) reports the power to detect a yearly change of 5% for current time-series . Pw(d) reports the same thing but estimated for time-series of a fixed period of 10 years (with the same sample sizes as the current time-series) Time series with too few years analysed or with too many analyses below LOQ have been excluded.

************

Foreman J W (2014) Data Smart: Using Data Science to Transform Information into Insight. John Wiley & Sons. 409 p.

Nicholson, M. D., R. J. Fryer, et al. (1998). Temporal trend monitoring: Robust method for analysing contaminant trend monitoring data. ICES Techniques in Marine Environmental Sciences No. 20. Copenhagen, Denmark, ICES: 29.

Sturludottir E, Gunnlaugsdottir H, Jorundsdottir HO, Magnusdottir EV, Olafsdottir K, Stefansson G (2014). Temporal trends of contaminants in cod from Icelandic waters. Science of the Total Environment, 476-477, 181-188.

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Human milk, SLV

Concentrations of environmental contaminant in mothers' milk, varies not only due to changes in exposure from e.g.

food but also from factors like mothers age, (increasing concentrations at higher age), BMI (decreasing), weight gain during pregnancy (decreasing), loss in weight after giving birth (seem to be less important in the current assessment) , education (increasing concentrations).

Trends of confounding factors may affect trends of adjusted time-series in a biased way. Weight gain during

pregnancy would tend to increase a trend (i.e. lower a real decreasing trend) , education would strengthen a decreasing trend in a biased way.

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Polychlorinated biphenyls (PCBs). CB-28

YRQ = minimum n of years required to detect a 5% annual change with a power of 80%.

LDT = the slowest change in concentration that can be detected with a 80% power during a 10-year period with the actual N of the trend.

CP = the year for which a change point in trend has been detected.

HU = human milk from Uppsala. MF=cow´s milk. U8=guillemont eggs.

C1-7, V2, V4= herring muscle. C1=Harufjärden, C2=Änskärsklubb (autumn), V2=Ängskärsklubb (spring), C3=Landsort, C4=Utlängan (autumn), V4=Utlängan (spring), C6=Fladen, C7=Väderöarna.

Fig. 1. CB-28. Individual human milk samples from Uppsala. CB-28 (unadjusted): log-linear regression model with CB-28 concentration as dependent variable and year as independent variable. CB-28 (adj.): log-linear regression model with CB-28 concentration as dependent variable and year of sampling, and maternal age, BMI, weight+, weight-, and education, as independent variables.

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Fig. 2. CB-28. Pooled cow´s milk samples from the Swedish Food Agency´s dioxin control.

Fig. 3. CB-28. Individual guillemot eggs from Stora Karlsö, the Baltic Sea.

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Fig. 4. CB-28. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Harufjärden, Ängskärsklubb, Landsort). “Ängskärskl.” denotes herring sampled in the autumn and “Ängskärskl. spring” denotes herring sampled in the spring.

Fig. 5. CB-28. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Utlängan) and the Swedish Atlantic west coast (Fladen, Väderöarna). “Utlängan” denotes herring sampled in the autumn and “Utlängan, spring”

denotes herring sampled in the spring.

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Polychlorinated biphenyls (PCBs). CB-52

Fig. 6. CB-52. Pooled cow´s milk samples from the Swedish Food Agency´s dioxin control.

Fig. 7. CB-52. Individual guillemot eggs from Stora Karlsö, the Baltic Sea.

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Fig. 8. CB-52. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Harufjärden,

Ängskärsklubb, Landsort). “Ängskärskl.” denotes herring sampled in the autumn and “Ängskärskl. spring” denotes herring sampled in the spring.

Fig. 9. CB-52. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Utlängan) and the Swedish Atlantic west coast (Fladen, Väderöarna). “Utlängan” denotes herring sampled in the autumn and “Utlängan, spring”

denotes herring sampled in the spring.

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Polychlorinated biphenyls (PCBs). CB-77

Fig. 10. CB-77. Pooled human milk samples from Stockholm and Göteborg.

Fig. 11. CB-77. Pooled hen´s egg samples from the dioxin control of the Swedish National Food Agency.

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Fig. 12. CB-77. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Harufjärden,

Ängskärsklubb, Landsort). “Ängskärskl.” denotes herring sampled in the autumn and “Ängskärskl. spring” denotes herring sampled in the spring.

Fig. 13. CB-77. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Utlängan) and from the Swedish Atlantic west coast (Fladen, Väderöarna). “Ulängan” denotes herring sampled in the autumn and “Utlängan, spring” denotes herring sampled in the spring.

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Polychlorinated biphenyls (PCBs). CB-101

Fig. 14. CB-101. Individual guillemot eggs from Stora Karlsö, the Baltic Sea.

Fig. 15. CB-101. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Harufjärden,

Ängskärsklubb, Landsort). “Ängskärskl.” denotes herring sampled in the autumn and “Ängskärskl. spring” denotes herring sampled in the spring.

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Fig. 16. CB-101. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Utlängan) and from the Swedish Atlantic west coast (Fladen, Väderöarna). “Ulängan” denotes herring sampled in the autumn and “Utlängan, spring” denotes herring sampled in the spring.

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Polychlorinated biphenyls (PCBs). CB-105

Fig. 17. CB-105. Individual human milk samples from Uppsala. CB-105 (unadjusted): log-linear regression model with CB-105 concentration as dependent variable and year as independent variable. CB-105 (adj.): log-linear regression model with CB-105 concentration as dependent variable and year of sampling, and maternal age, BMI, weight+, weight-, and education, as independent variables.

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Fig. 18. CB-105. Pooled human milk samples from Stockholm and Göteborg (NRM).

Fig. 19. CB-105. Pooled hen´s egg samples from the dioxin control of the Swedish National Food Agency.

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Fig. 20. CB-105. Pooled cow´s milk, cattle fat and lamb fat samples from the Swedish Food Agency´s dioxin control milk and meat

Fig. 21. CB-105. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Harufjärden,

Ängskärsklubb, Landsort). “Ängskärskl.” denotes herring sampled in the autumn and “Ängskärskl. spring” denotes herring sampled in the spring.

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Fig. 22. CB-105. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Utlängan) and from the Swedish Atlantic west coast (Fladen, Väderöarna). “Ulängan” denotes herring sampled in the autumn and “Utlängan, spring” denotes herring sampled in the spring.

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Polychlorinated biphenyls (PCBs). CB-114

Fig. 23. CB-114. Pooled human milk samples from Stockholm and Göteborg (NRM).

Fig. 24. CB-114. Pooled hen´s egg samples from the dioxin control of the Swedish National Food Agency.

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Fig. 25. CB-114. Pooled cow´s milk, cattle fat and lamb fat samples from the Swedish Food Agency´s dioxin control.

Fig. 26. CB-114. Pooled/Individual autumn samples of herring muscle from the Baltic Sea (Harufjärden,

Ängskärsklubb, Landsort). “Ängskärskl.” denotes herring sampled in the autumn and “Ängskärskl. spring” denotes herring sampled in the spring.

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Fig. 27. CB-114. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Utlängan) and from the Swedish Atlantic west coast (Fladen, Väderöarna). “Ulängan” denotes herring sampled in the autumn and “Utlängan, spring” denotes herring sampled in the spring.

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Polychlorinated biphenyls (PCBs). CB-118

Fig. 28. CB-118. Individual human milk samples from Uppsala. CB-118 (unadjusted): log-linear regression model with CB-118 concentration as dependent variable and year as independent variable. CB-118 (adj.): log-linear regression model with CB-118 concentration as dependent variable and year of sampling, and maternal age, BMI, weight+, weight-, and education, as independent variables.

Fig. 29. CB-118. Pooled human milk samples from Stockholm and Göteborg (NMR).

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Fig.30. CB-118. Pooled hen´s egg samples from the dioxin control of the Swedish National Food Agency.

Fig.31. CB-118. Pooled cow´s milk, cattle fat and lamb fat samples from the Swedish Food Agency´s dioxin control.

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Fig. 32. CB-118. Individual guillemot eggs from Stora Karlsö, the Baltic Sea.

Fig.33. CB-118. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Harufjärden,

Ängskärsklubb, Landsort). “Ängskärskl.” denotes herring sampled in the autumn and “Ängskärskl. spring” denotes herring sampled in the spring.

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Fig. 34. CB-118. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Utlängan) and from the Swedish Atlantic west coast (Fladen, Väderöarna). “Ulängan” denotes herring sampled in the autumn and “Utlängan, spring” denotes herring sampled in the spring.

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Polychlorinated biphenyls (PCBs). CB-123

Fig. 35. CB-123. Pooled human milk samples from Stockholm and Göteborg (NRM).

Fig. 36. CB-123. Pooled hen´s egg samples from the dioxin control of the Swedish National Food Agency.

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Fig. 37. CB-123. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Harufjärden,

Ängskärsklubb, Landsort). “Ängskärskl.” denotes herring sampled in the autumn and “Ängskärskl. spring” denotes herring sampled in the spring.

Fig. 38. CB-123. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Utlängan) and from the Swedish Atlantic west coast (Fladen, Väderöarna). “Ulängan” denotes herring sampled in the autumn and “Utlängan, spring” denotes herring sampled in the spring.

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Polychlorinated biphenyls (PCBs). CB-126

Fig. 39. CB-126. Individual human milk samples from Uppsala. CB-126 (unadjusted): log-linear regression model with CB-126 concentration as dependent variable and year as independent variable. CB-126 (adj.): log-linear regression model with CB-126 concentration as dependent variable and year of sampling, and maternal age, BMI, weight+, weight-, and education, as independent variables.

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Fig. 40. CB-126. Pooled human milk samples from Stockholm and Göteborg (NMR).

Fig. 41. CB-126. Pooled hen´s egg samples from the dioxin control of the Swedish National Food Agency.

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Fig. 42. CB-126. Pooled cow´s milk, cattle fat and lamb fat samples from the Swedish Food Agency´s dioxin control.

Fig. 43. CB-126. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Harufjärden,

Ängskärsklubb, Landsort). “Ängskärskl.” denotes herring sampled in the autumn and “Ängskärskl. spring” denotes herring sampled in the spring.

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Fig. 44. CB-126. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Utlängan) and from the Swedish Atlantic west coast (Fladen, Väderöarna). “Ulängan” denotes herring sampled in the autumn and “Utlängan, spring” denotes herring sampled in the spring.

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Fig. 45. CB-138. Individual human milk samples from Uppsala. CB-138 (unadjusted): log-linear regression model with CB-138 concentration as dependent variable and year as independent variable. CB-138 (adj.): log-linear regression model with CB-138 concentration as dependent variable and year of sampling, and maternal age, BMI, weight+, weight-, and education, as independent variables.

Fig. 46. CB-138. Pooled human milk samples from Stockholm and Göteborg (NMR).

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Fig. 47. CB-138. Pooled hen´s egg samples from the dioxin control of the Swedish National Food Agency.

Fig. 48. CB-138. Pooled cow´s milk, cattle fat and lamb fat samples from the Swedish Food Agency´s dioxin control.

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Fig. 49. CB-138. Individual guillemot eggs from Stora Karlsö, the Baltic Sea.

Fig. 50. CB-138. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Harufjärden,

Ängskärsklubb, Landsort). “Ängskärskl.” denotes herring sampled in the autumn and “Ängskärskl. spring” denotes herring sampled in the spring.

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Fig. 51. CB-138. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Utlängan) and from the Swedish Atlantic west coast (Fladen, Väderöarna). “Ulängan” denotes herring sampled in the autumn and “Utlängan, spring” denotes herring sampled in the spring.

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Polychlorinated biphenyls (PCBs). CB-153

Fig. 52. CB-153. Individual human milk samples from Uppsala. CB-153 (unadjusted): log-linear regression model with CB-153 concentration as dependent variable and year as independent variable. CB-153 (adj.): log-linear regression model with CB-153 concentration as dependent variable and year of sampling, and maternal age, BMI, weight+, weight-, and education, as independent variables.

Fig. 53. CB-153. Pooled human milk samples from Stockholm and Göteborg (NMR).

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Fig. 54. CB-153. Pooled hen´s egg samples from the dioxin control and the contaminant control (RK) of the Swedish National Food Agency.

Fig. 55. CB-153. Individual samples of fat from cattle, swine, lamb and reindeer from the contaminant control (RK) of the Swedish National Food Agency.

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Fig. 56. CB-153. Pooled cow´s milk, cattle fat and lamb fat samples from the Swedish Food Agency´s dioxin control.

Fig. 57. CB-153. Individual guillemot eggs from Stora Karlsö, the Baltic Sea.

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Fig. 58. CB-153. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Harufjärden,

Ängskärsklubb, Landsort). “Ängskärskl.” denotes herring sampled in the autumn and “Ängskärskl. spring” denotes herring sampled in the spring.

Fig. 59. CB-153. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Utlängan) and from the Swedish Atlantic west coast (Fladen, Väderöarna). “Ulängan” denotes herring sampled in the autumn and “Utlängan, spring” denotes herring sampled in the spring.

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Polychlorinated biphenyls (PCBs). CB-156

Fig. 60. CB-156. Individual human milk samples from Uppsala. CB-156 (unadjusted): log-linear regression model with CB-156 concentration as dependent variable and year as independent variable. CB-156 (adj.): log-linear regression model with CB-156 concentration as dependent variable and year of sampling, and maternal age, BMI, weight+, weight-, and education, as independent variables.

Fig. 61. CB-156. Pooled human milk samples from Stockholm and Göteborg (NMR).

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Fig. 62. CB-156. Pooled hen´s egg samples from the dioxin control of the Swedish National Food Agency.

Fig. 63. CB-156. Pooled cow´s milk, cattle fat and lamb fat samples from the Swedish Food Agency´s dioxin control.

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Fig. 64. CB-156. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Harufjärden,

Ängskärsklubb, Landsort). “Ängskärskl.” denotes herring sampled in the autumn and “Ängskärskl. spring” denotes herring sampled in the spring.

Fig. 65. CB-156. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Utlängan) and from the Swedish Atlantic west coast (Fladen, Väderöarna). “Ulängan” denotes herring sampled in the autumn and “Utlängan, spring” denotes herring sampled in the spring.

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Polychlorinated biphenyls (PCBs). CB-157

Fig. 66. CB-157. Pooled human milk samples from Stockholm and Göteborg (NMR).

Fig. 67. CB-157. Pooled hen´s egg samples from the dioxin control of the Swedish National Food Agency.

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Fig. 68. CB-157. Pooled cow´s milk, cattle fat and lamb fat samples from the Swedish Food Agency´s dioxin control.

Fig. 69. CB-157. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Harufjärden,

Ängskärsklubb, Landsort). “Ängskärskl.” denotes herring sampled in the autumn and “Ängskärskl. spring” denotes herring sampled in the spring.

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Fig. 70. CB-157. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Utlängan) and from the Swedish Atlantic west coast (Fladen, Väderöarna). “Ulängan” denotes herring sampled in the autumn and “Utlängan, spring” denotes herring sampled in the spring.

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Polychlorinated biphenyls (PCBs). CB-167

Fig. 71. CB-167. Individual human milk samples from Uppsala. CB-118 (unadjusted): log-linear regression model with CB-118 concentration as dependent variable and year as independent variable. CB-118 (adj.): log-linear regression model with CB-118 concentration as dependent variable and year of sampling, and maternal age, BMI, weight+, weight-, and education, as independent variables.

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Fig. 72. CB-167. Pooled human milk samples from Stockholm and Göteborg (NMR).

Fig. 73. CB-167. Pooled hen´s egg samples from the dioxin control of the Swedish National Food Agency.

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Fig. 74. CB-167. Pooled cow´s milk, cattle fat and lamb fat samples from the Swedish Food Agency´s dioxin control.

Fig. 75. CB-167. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Harufjärden,

Ängskärsklubb, Landsort). “Ängskärskl.” denotes herring sampled in the autumn and “Ängskärskl. spring” denotes herring sampled in the spring.

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Fig. 76. CB-167. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Utlängan) and from the Swedish Atlantic west coast (Fladen, Väderöarna). “Ulängan” denotes herring sampled in the autumn and “Utlängan, spring” denotes herring sampled in the spring.

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Fig. 77. CB-169. Individual human milk samples from Uppsala. CB-169 (unadjusted): log-linear regression model with CB-169 concentration as dependent variable and year as independent variable. CB-169 (adj.): log-linear regression model with CB-169 concentration as dependent variable and year of sampling, and maternal age, BMI, weight+, weight-, and education, as independent variables.

Fig. 78. CB-169. Pooled human milk samples from Stockholm and Göteborg (NMR).

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Fig. 79. CB-169. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Harufjärden,

Ängskärsklubb, Landsort). “Ängskärskl.” denotes herring sampled in the autumn and “Ängskärskl. spring” denotes herring sampled in the spring.

Fig. 80. CB-169. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Utlängan) and from the Swedish Atlantic west coast (Fladen, Väderöarna). “Ulängan” denotes herring sampled in the autumn and “Utlängan, spring” denotes herring sampled in the spring.

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Polychlorinated biphenyls (PCBs). CB-180

Fig. 81. CB-180. Individual human milk samples from Uppsala. CB-180 (unadjusted): log-linear regression model with CB-180 concentration as dependent variable and year as independent variable. CB-180 (adj.): log-linear regression model with CB-180 concentration as dependent variable and year of sampling, and maternal age, BMI, weight+, weight-, and education, as independent variables.

Fig. 82. CB-180. Pooled human milk samples from Stockholm and Göteborg (NMR).

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Fig. 83. CB-180. Pooled hen´s egg samples from the dioxin control of the Swedish National Food Agency.

Fig. 84. CB-180. Pooled cow´s milk, cattle fat and lamb fat samples from the Swedish Food Agency´s dioxin control.

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Fig. 85. CB-180. Individual guillemot eggs from Stora Karlsö, the Baltic Sea.

Fig. 86. CB-180. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Harufjärden,

Ängskärsklubb, Landsort). “Ängskärskl.” denotes herring sampled in the autumn and “Ängskärskl. spring” denotes herring sampled in the spring.

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Fig. 87. CB-180. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Utlängan) and from the Swedish Atlantic west coast (Fladen, Väderöarna). “Ulängan” denotes herring sampled in the autumn and “Utlängan, spring” denotes herring sampled in the spring.

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Polychlorinated biphenyls (PCBs). CB-189

Fig. 88. CB-189. Individual human milk samples from Uppsala. CB-189 (unadjusted): log-linear regression model with CB-189 concentration as dependent variable and year as independent variable. CB-189 (adj.): log-linear regression model with CB-189 concentration as dependent variable and year of sampling, and maternal age, BMI, weight+, weight-, and education, as independent variables.

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Fig. 89. CB-189. Pooled hen´s egg samples from the dioxin control of the Swedish National Food Agency.

Fig. 90. CB-189. Pooled cattle fat and lamb fat samples from the Swedish Food Agency´s dioxin control.

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Fig. 91. CB-189. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Harufjärden,

Ängskärsklubb, Landsort). “Ängskärskl.” denotes herring sampled in the autumn and “Ängskärskl. spring” denotes herring sampled in the spring.

Fig. 92. CB-189. Individual/pooled autumn samples of herring muscle from the Baltic Sea (Utlängan) and from the Swedish Atlantic west coast (Fladen, Väderöarna). “Ulängan” denotes herring sampled in the autumn and “Utlängan, spring” denotes herring sampled in the spring.

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Dioxinlike PCBs toxicity equivalent (TEQ) concentrations

Fig. 93. Mono-ortho PCB TEQ, upper bound (UB) concentrations where concentrations below limit of quantification were set to the concentration at LOQ. Individual human milk samples from Uppsala. moTQUB (unadjusted): log- linear regression model with mono-ortho PCB TEQ concentration as dependent variable and year as independent variable. moTQUB (adj.): log-linear regression model with mono-ortho PCB TEQ concentration as dependent variable and year of sampling, and maternal age, BMI, weight+, weight-, and education, as independent variables.

Fig. 94. Human milk, SLV. Non-ortho PCBs TEQ, upper bound (UB) concentrations where concentrations below limit of quantification were set to the concentration at LOQ. Individual human milk samples from Uppsala. noTQUB (unadjusted): log-linear regression model with non-ortho PCB TEQ concentration as dependent variable and year as independent variable. noTQUB (adj.): log-linear regression model with non-ortho PCB TEQ concentration as dependent variable and year of sampling, and maternal age, BMI, weight+, weight-, and education, as independent variables.

References

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