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Exposure of Humans to Persistent pOrganic Pollutants (POPs):
What is the Relevance of Soil?What is the Relevance of Soil? Olaf Paepke
Eurofins Analytik Am Neuländer Gewerbepark 1Eurofins Analytik, Am Neuländer Gewerbepark 1 D-21097 Hamburg, Germany
Email: olafpaepke@eurofins deEmail: [email protected]
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Outline• General information• Direct intake of soil• Intake via food (milk poultry vegetable• Intake via food (milk-, poultry-, vegetable-
and products R l ti il• Regulations on soil
• Influence of use or origin of soil• Background levels for soil• Examples for elevated levels of soilExamples for elevated levels of soil
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What are POPs?What are POPs?
The term POPs refers to 12 chemicals addressed in the Stockholm Conventionaddressed in the Stockholm Convention (SC) on Persistent Organic Pollutants ,
l b l t t ti t d d tha global treaty negotiated under the auspices of the United Nations pEnvironment Program (UNEP) in order to eliminate the production and use or releaseeliminate the production and use or releaseof POPs.
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12 Stockholm POPs
Chemical Pesticide Industrial Chemical By-productAldrin +Chlordane +Chlordane +DDT +Dieldrin +Endrin +Heptachlor +Mirex +MirexToxaphene +Hexachlorobenzene + + +PCBPCBs + +
Dioxins +Furans +Furans +
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Due to the availability of data, the following will focus on
Dioxins and Dioxin like PCBsDioxins and Dioxin-like PCBs
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Components of QuestionComponents of Question• Polychlorinated • Polychlorinatedy
dioxins and furansPCDDs and PCDFs
Polychlorinated biphenylsPCBsC12HxClyO2 (x+y=8; n=75)
C12HxClyO (x+y=8; n=135)
PCBsC12HxCly (x+y=10; n=209)
• Relevant for Humans:• 17 congeners with 2,3,7,8-
chlorine substitution
• Relevant for Humans:• 12 dioxin-like congeners, 4
chlorine substitutiong
non-ortho, 8 mono-ortho
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Some General Remarks on PCDDs/PCDFsSome General Remarks on PCDDs/PCDFs
Di i d d i t ti ll th• Dioxins were never produced intentionally, they occur as trace contaminants in a variety of industrial and thermal processesthermal processes
• Due to their chemical, physical and biological stability PCDDs/PCDFs are stable to remain in thePCDDs/PCDFs are stable to remain in the environment for long times. As a consequence dioxins from so called “primary sources” (oncedioxins from so called primary sources (once formed in industrial or combustion processes) can be transferred to other matrices and enter the environment. Such “secondary sources” are e.g. sewage sludge/biosludge, composts, or contaminated soils and sediments
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Ch i l & I d t i l SChemical & Industrial Sources for Dioxins
– Waste incineration
– Thermal industrial processes
Metal production– Metal production
– Chlorine industry
– Bleaching of pulp
– TrafficTraffic
– Domestic furnaces
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Exposure Pathways of DioxinsE i i FoodE i t
Incineration
Emission FoodBeef, cow
milk/ products
Environment
IncinerationIndustry
milk/-products
Pork/d t
Rain/deposition
ChlorineIndustry
-products
Chicken/-products
Dump Site/Slude
Unwanted
Thermal MetalProcess
products
Fish/-products
Plants, grasby products
CarExhaust
products
VegetablesSoil / Water
Exhaust
HumansHumansHumansHumans
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Importance of FoodImportance of FoodC ti f f d t ib t ll ith• Consumption of food contributes normally with
>95 %95 %to the daily total PCDD/PCDF and PCB uptake
• Food rich in fat, especially originating from
i l i t i t tanimals, is most important
• Food originating from plants usually shows a• Food originating from plants usually shows a
lower content of PCDDs/PCDFslower content of PCDDs/PCDFs
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Dietary Intake of PCDD/Fs in pg I-TEQ/d from
100Major Food Groups, Adults (≈ 1 pg/day/kg BW)
75Other foods*Fish
50
EggsMeat, poultryDairy products
50
*other foods= cereals,
25 cereal products, vege-tables, fruit, vegetablefats and oils
0Finland France Germany Italy Holland Norway Sweden U.K.
European Commission
The image cannot be displayed. Your computer may not have enough memory to open the image, or the image may have been corrupted. Restart your computer, and then open the file again. If the red x still appears, you may have to delete the image and then insert it again.
The image cannot be displayed. Your computer may not have enough memory to open the image, or the image may have been corrupted. Restart your computer, and then open the file again. If the red x still appears, you may have to delete the image and then insert it again.
European CommissionSCOOP Task 3.2.5June 7, 2000
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Estimated Average Adult Dietary Intakes of Dioxins and dl PCBs in UKDioxins and dl-PCBs in UK
(Upper Bound Calculation)8
678
y
456
O-T
EQ/
eigh
t /da
y
PCBs
234
pg W
HO
g bo
dyw
e CDioxins
UK TDI = 2 pg WHO-TEQ/kg bw/day
12kg
01982 1992 1997 2001
C 02031 FSA Report FD 02/41, 2002
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H E t S ilHuman Exposure to Soil
• Direct Intake: IngestionDirect Intake: Ingestion
• Indirect Intake: FoodMilk d ilk d t- Milk and milk products
- Poultry, eggs- Vegetable, fruit
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Direct Intake: Ingestion
Soil ingsetion in children and adults in the same family (Davis et al., 2005)
Children: 37 – 207 mg/day *)
Adults: 23 – 625 mg/day *)
*) based on titanium as tracer
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Ingestion of Soil, Dependence of Age
0,12
0,14
0 08
0,1
g/da
y)
0,06
0,08
aily
Inta
ke (g
0,02
0,04
Da
0
,
0 to 1 1 to 2 2 to 3 3 to 4 4 to 5 5 to 6 6 to 7Age group (years)Age group (years)
www.epa.gov/superfund/lead/products/ssircolo.pdf
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Influences to POP Levels inMilk ProductsInfluences to POP Levels inMilk Products
EnvironmentalEnvironmental air
Emission
Other FEED STUFF
Grass
Soil
Grass
Soil
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Influence of Soil Contamination on Dioxin C t ti i GConcentration in Grass
Hembrock-Heger 1990
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Effects of Flooding on PCDDs/Fs &Effects of Flooding on PCDDs/Fs & PCBs
• Background: Grazing on milk producing cows on contaminated pastures may result in cont. milk
• During 3 sampling periods (1998-1999) collection of 310 samples (114 milk, 38 feed 79 soil, 79 grass)
• 3 river systems, samples collected from farms with floodplain pastures and nearby control farms
• Results: Milk from flooded prone location show significant higher values for dioxins and PCBs than from control sites Until now data only for milkfrom control sites. Until now, data only for milk available
Reference: Food Standard Agency
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Uptake of Soil by Grazing Animals, Overview
Animal Uptake Method ReferenceAnimal Uptake Method ReferenceCow 6-14% of d. m. Titan Healey, 1968
Cow 1.2-18.6 % of d.m. Titan Mayland et al., 1975
Cow 1-18 % of d.m. Titan Thornton & Abrahams, 1983,
Cow 1-2 % of d.m. Cal. via ash Berende, 1990
Sheep 0.4-14 % of d.m. Titan Field & Purves, 1964
Sheep 75 kg/animal and year Air McGrath et al., 1982
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Transfer of Dioxins by ConsumptionTransfer of Dioxins by Consumption of Poultry and Products
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Influence of Housing on PCDDs/PCDFs in Chicken Eggs n= 285 2005in Chicken Eggs, n= 285, 2005
www.umwelt.nrw.de/verbraucherschutz
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G. Schoeters , R. Hoogenboom, 2006
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Sources of Dioxins in EggsSources of Dioxins in Eggs(G. Schoeters , R. Hoogenboom, 2006)
Cage hensCage hens• Feed
Free range hensFeed• Feed
• Worms and insects11 %
41 %24 %
FoodWorms
Herbs
• Herbs, grasses,vegetables, leavings
HerbsSoilfrom kitchen gardens
• Soil 24 %24 %
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Comparison of “Byker eggs” with levels reported in literature
einf
elde
n
300
350
anta
m P
FHH
ambu
rg Rh e
250
300
g/g
fat
ket
l g t soil
PFH ba
ntam
Wal
es b
a
150
200
DF
I-TEQ
in p
g
e Fa
rm
supe
rmar
ke ow ck an
tam
rura
lny
s du
cken
Pan
teg
uck
rura
len
rura
ldu
ck P
ante
gon
Bac
ott S
tree
ns 4
60 p
pt
orne
rve
r 91
n D
ene
ton
Ath
onys
hen
e Tc
eal
es d
uck
Pra
nxto
n A
b
100
150
PCD
D/P
CD
Haw
thor
neE
U m
inG
erm
any
Cox
lodg
eB
lane
y R
oE
U m
axB
runs
wi c
Wal
es b
aSt
Ant
hoW
ales
he
Wal
es d
uW
ales
hW
ales
dB
ranx
toW
estm
aS
teph
eP
ets
Co
Bol
sov
Den
ton
Bra
nxt
St A
ntH
ulne W
a Br
0
50
0
Pless-Mulloli et al., 2001
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Concentration in Eggs by Allotment:I-TEQ (pg/g fat)I-TEQ (pg/g fat)
50
60
g/g
fat
30
40
TEQ
in p
g
20
30
D/P
CD
F I-T
0
10
k A A
PCD
D
awtho
rne Fa
rmCox
lodg
eBlan
ey R
owBrun
swick
St Anth
onys
Branxto
n Btm
acott
Stre
etPets
Corn
erDen
ton D
ene
Branxto
n ASt A
nthon
ysHuln
e Tce
Branxto
n A
Haw
Westm D
Pless-Mulloli et al., 2001
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Allotment Coxlodge: gI-TEQ (ash) 4224 pg/g, (egg) 2 pg/g fat
14000
16000
30
35
tash egg
10000
12000
-TE
Q in
pg/
g
20
25
TEQ
in p
g/g
faash egg
6000
8000
ratio
n in
ash
I-
15
20
ion
in e
ggs
I-T
2000
4000
Conc
entr
5
10
Conc
entra
t
0
8- T
CDD
8-Pe
CDD
8 Hx
CDDs
8-Hp
CDD
OCDD
7,8-
TCDF
8 Pe
CDFs
8 Hx
CDFs
8 Hp
CDFs
OCDF
0
2, 3
, 7,
1,2,
3,7,
8
Tota
l 2,3
,7,8
1,2,
3,4,
6,7,
8
2,3,
7
Tota
l 2,3
,7,8
Tota
l 2,3
,7,8
Tota
l 2,3
,7,8
Pless-Mulloli et al., 2001
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PCDDs/PCDFs in Exposure MaterialpTotals of ONLY 2.3.7.8-substituted Congeners
100 0
Soil (I-TEQ : 2378 pg/g)
Eggs (I-TEQ : 746 pg/g, lipid)
75,0
100,0Chicken (I-TEQ : 513 pg/g, lipid)
50,0%
0,0
25,0
Tetra-CDD
Penta-CDD
Hexa-CDD
Hepta-CDD
Octa-CDD
Tetra-CDF
Penta-CDF
Hexa-CDF
Hepta-CDF
Octa-CDF
Wuthe et al, 1992
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PCDDs/PCDFs in Human BloodResident of contaminated site
5000Background, Germany, mean (I-TEQ : 43)
Resident No.56 (I-TEQ : 175)
3000
4000
id b
ased
1000
2000
pg/g
, lip
i
0
1000
CD
D
CD
D
CD
D
CD
D
CD
D
CD
F
CD
F
CD
F
CD
F
CD
F
Tetra
-C
Pent
a-C
Hex
a-C
Hep
ta-C
Oct
a-C
Tetra
-C
Pent
a-C
Hex
a-C
Hep
ta-C
Oct
a-C
Wuthe et al, 1992
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Indirect Intake of Soil Contaminants via F d V t blFood: Vegetable
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Increase of PCDD/PCDF in Carrots depending of Soil Concentration Fielddepending of Soil Concentration, Field
Investigation Marsberg
Krause et al., 1993
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Comparison of Dioxin Concentrations (ng TEQ/kg DM) in Food Plants Corresponding Soil(ng TEQ/kg DM) in Food Plants, Corresponding Soil
(0-25 cm) and Deposition (TEQ, m2 /d)
Lettuce Endive Kale Soil Deposition
2.4 28.5 65.6 75.1 56
1.5 5.6 20.8 77.6 20
3.1 14.4 53.7 35.9 51
2.8 5.5 20.3 16.4 21
1.8 2.2 4.0 21.3 7.4
2.2 1.7 2.6 21.8 5.7
MURL, 1995
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Regulations and Special Influences g pon Soil Contamination
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Soil Guideline Concentrations (TEQ, ng/kg d.m.)
• Germany< 5 Target concentration
5 – 40 Control of products if dioxin transfer>100 Soil exchange on children playgrounds>100 Soil exchange on children playgrounds
> 1000 Soil exchange in residential areas> 10,000 Soil exchange independent of the location
• The Netherlands1 Agricultural farming
10 Dairy farming10 Dairy farming• Sweden
10 Sensitive uses250 Non-sensitive uses
• Japan10001000
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Example for Contamination of Soil andExample for Contamination of Soil and Vegetation by a Point Source (MSWI)
(Ch P S t l Di i 2003)(Cheng P.S. et al., Dioxin 2003)
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Nationwide Distribution of PCDD/F levels in Ambient Air of 19 MSWIs in Taiwan
Correspomding locations
Cheng P.S. et al., 2003
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PCDD/Fs Levels in Ambient Air in the Vicinity yof 19 MSWIs in Taiwan. (pg-TEQ/Nm3)
1 60
1,80
2,00
1,20
1,40
1,60
0 60
0,80
1,00
0,20
0,40
0,60
0,00A B C D D E F G H I J K L M N O P Q R S
Cheng P.S. et al., 2003
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PCDD/Fs Levels in Vegetation in the Vicinity
35
of 19 MSWIs in Taiwan. (pg-TEQ/g d.m.)
25
30
20
25
10
15
5
10
0A B C D E F *G I J K L N O P Q R *S
Cheng P.S. et al., 2003
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PCDD/Fs level in soil in the vicinity of 19
70180,0
MSWIs in Taiwan. (pg-TEQ/g d.m.)
50
60
,
40
50
20
30
10
20
0A B C D E F *G H I J K L *M N O P Q R *S
Cheng P.S. et al., 2003
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Nationwide PCDD/Fs Levels in Ambient Air, Vege-tation, and Soil in the Vicinity of 19 MSWIs in Taiwan
12
14
8
10air
vegetation
(* factor 5)
4
6
soil
0
2
4
A B C D E F G H I J K L M N O P Q Rair
soil
0
P Q R S
Cheng P.S. et al., 2003
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Influence of Use/Origin on Soil PCDD/F - Contamination, Bavaria/Germany
TEQ (BGA), ng/kg, d.m.
Type of Soil n Med Range
Farmland 41 0.24 ND -18Grassland 27 0.6 ND - 18Forest top layer 32 10 ND - 50Forest, top layer 32 10 ND 50Forest, soil 30 0.8 ND - 17G 30 1 ND 13Green spaces 30 1 ND - 13ND = Not Detected
Fiedler, 1998
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Influence of Traffic on Soil PCDD/F - Contamination, Bavaria Germany TEQ (BGA) values ng/kg d mBavaria, Germany, TEQ (BGA) values, ng/kg, d.m.
Distance Distance Remark<5 m >5 m
• City of Munich 10 0.3 C.D.• BAB A3 Nürnberg 16 1 6-0 2BAB A3, Nürnberg 16 1.6 0.2• BAB A8, Dachau 7.6 ND• BAB A8 Nürnberg 5 2 1 0 5• BAB A8, Nürnberg 5 2.1-0.5• Local small road 1-0.6 0.5-ND
C.D. = continuous decline till 70 m Fiedler, 1998
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TEQ (PCDD/PCDF only) in Sediment and Soils from EU Member StatesSoils from EU Member States,
ng /kg d. m.S di t S ilSediment Soil
Background, Urban Any Type, Pasture, RuralAustria 1 6 - 14Austria 1.6 - 14Belgium 2.7 - 8.9Finland 0.7 - 100GGermany 1.2 - 73 0.1 - 42Greece 2 - 45Ireland 0.2 - 13Italy 0.1 - 23 0.1 - 43Luxembourg 2.4 - 16 1.4 - 20Netherlands 1 10 2 55Netherlands 1 - 10 2 - 55Spain 0.1 - 8.4Sweden 0.8 - 207 0.1U. Kingdom 2 - 123 0.8 - 87
Fiedler et al., 1999
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Typical Congener/Homolog Distribution of Soil Samples
• Incineration pattern:Increase from TCDD to OCDD, decline from TCDF to OCDF,
• Pentachlorophenol pattern:Increase from HxCDD to OCDD, Increase from HxCDF to OCDF
• Agent Orange pattern:Dominated by 2,3,7,8-TCDD, small 1,2,3,7,8-PeCDD
• Chlorine bleaching pattern:Dominated by 2,3,7,8-TCDD/TCDF, small other Tetra + Penta CDDs/Fs
• “Non anthropogenic” pattern:Increase from HxCDD to OCDD, NO PCDFs
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Examples for Elevated Soil Levels Values in TEQs, pg/g
• Taiwan PCP Production some 1 000 000Taiwan PCP Production some 1,000,000• Vietnam Agent Orange *) about 1,000,000• Seveso TCP Production some 100,000 **)Seveso TCP Production some 100,000 )• Germany Herbicide Production some 100,000• USA Horse Arena some 100,000,• Germany Metal Reclamation some 10,000• Japan MWI vicinity some 1,000• UK Fly ash pathways some 1,000
*) Former air base **) values given in μg/m2
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References for Dietary Intake
• European Commission, SCOOP Task 3.2.5, June 7, 2000• Report FD 02/41, FSA’s Food Survey Information Sheet, 2002
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References for Ingestion of SoilReferences for Ingestion of Soil
• Davis S. and Mirik D., Soil ingestion in Children and adults in the same family, J. of Exposure Analysis and Environmental Epidemiology, 1-13, 2005
• http://www.epa.gov/superfund/lead/products/ssircolo.pdfg
• http://www.sciencedirect.com/science?_ob=ArticleURL&_udi=B6WDM-45M8SWC-2B&_user=10&_rdoc=1&_fmt=&_orig=search&_sort=d&view=c&_acct=C000050221&_version=1&_urlVersion=0&_userid=10&md5=9f47f63ea32790c7a2004714d479c0f5
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References for Transfer of Dioxins to MilkReferences for Transfer of Dioxins to Milk
• Liem et al., Levels and Patterns of dioxins in cows milk in the vicinity of municipal waste incinerators and metal reclamation plants in the Netherlands, OHC, 1, 567-570, (1990)
• Startin et al., Surveillance of British Foods For PCDDs and PCDFs, Chemosphere, 20, 793- 798, (1990)
• Riss et al., Comparison of PCDD/PCDF Levels in Soil, Cow’s milk, Human Blood and Spruce Needles in an Area of PCDD/PCDF Contamination Trough Emissions from a MetalReclamation Plant, Chemosphere, 21, 1451- 1456, (1990)
•
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References for Transfer of Dioxins to EggsReferences for Transfer of Dioxins to Eggs
• http://www.umwelt.nrw.de/verbraucherschutz/pdf/dioxin_eier_bericht.pdf (2005)
• G. Schoeters , R. Hoogenboom ,Contamination of free-range chicken eggs with dioxins and dioxin-like polychlorinated biphenyls, Molekular Nutrition & Food, 50:10, 908 914, 2006p y p y , , , ,
• Pless-Mulloli et al., Transfer of PCDD/F and Heavy Metals from Incinerator Ash onFootpaths in Allotments into Soil and Eggs, OHC, 51, 48-52, (2001)
Fürst et al PCDD/PCDF in Commercial Chicken Eggs Depending on the T pe of• Fürst et al., PCDD/PCDF in Commercial Chicken Eggs – Depending on the Type of Housing, OHC, 13, 31- 34, 1993
• Sagunski et al., Levels and Patterns of PCDD/F in Eggs, Chicken and Human Blood of residents living on a contaminated Area: Investigation of a possible Relationship OHC 13residents living on a contaminated Area: Investigation of a possible Relationship, OHC, 13, 101-104, (1993)
• Wuthe, In Current Views on the impact of dioxins and furans on human health and the environment Berlin Nov 9 11 1992 The Toxicology Forum 252 259 (1992)environment. Berlin Nov. 9-11, 1992. The Toxicology Forum 252-259, (1992)
• Stephens et al., Bioaccumulation of dioxins in food animals II: Controlled exposure studiesChemosphere, 20, 1091- 1096, (1990)
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References for Transfer of Dioxins fom Soil to Grass and Vegetables
• Hembrock-Heger A., PCDD/PCDF levels in soil and plants in North Rhine Westphalia, Organohalogen Compounds,1 475- 478, 1990
MURL 1995 Mi i t i fü U lt R d d L d i t h ft L ft i h lt• MURL, 1995, Ministerium für Umwelt, Raumordnung und Landwirtschaft: Luftreinhalte-planung in Nordrhein-Westfalen, Untersuchungsbericht Ostruhrgebiet, Luftüberwachung
• Krause G.H.M, Delschen T., Fürst P., Hein D., Bewertung der Belastung durch PCDD/F aus der ehemaligen K pferge inn ng im Ra m Marsberg NRW Teil 1 PCDD/F n Bödender ehemaligen Kupfergewinnung im Raum Marsberg, NRW, Teil 1, PCDD/F n Böden, Vegetation und Kuhmilch, UWSF Z .Umweltchemie,5,194-203, 1993
• Healey, W.B, The influence of soil type on ingestion of soil by grazing animals, 9th Inter-national Congress of soil sciences transactions 3:437 445 1968national Congress of soil sciences transactions 3:437-445, 1968
• Mayland H., Flore A., Rosenau R., Turner V., Soil ingestion by cattle on semiarid range as reflected by titanium analysis of feces. J Range Managemant 28:448-452, 1975
• Thornton I., Abrahams O., Soil ingestion- a major pathway of heavy metals into livestock grazing contaminated land. Sci. Total Environ. 28:287-294, 1983
• Berende P., Grondobname door melkoeeien, Institut voor veevoedingsonderzoek (IVVO), , , g ( ),Lelstad, NL, Interim Rapport no., 312, 1990
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References for Transfer of Dioxins fom Soil to Grass and Vegetables (cont.)
• Riss et al., Comparison of PCDD/PCDF Levels in Soil, Cow’s milk, Human Blood and Spruce Needles in an Area of PCDD/PCDF Contamination Trough Emissions from a MetalReclamation Plant, Chemosphere, 21, 1451- 1456, (1990)
• Field A.C., Purves D., Intake of soil by grazing sheep, Poc. Nutr. Soc. 23: 24-24, 1964
• McGrath D, Pool d., Fleming G., Sinnott J., Soil ingestion by grazing sheep, Irish J. Agr. Res., 21:35, 1990
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Thank you for your AttentionThank you for your Attention