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Occurrence and fate of xenobiotic in sewage sludge andin sludge-amended soils

Dominique Patureau, Mireille Laforie, Eric Lichtfouse, Giovanni Caria, ValerieSappin-Didier, Laurence Denaix, Christian Mougin, Nina Christensen,

Katerina Stamatelatou

To cite this version:Dominique Patureau, Mireille Laforie, Eric Lichtfouse, Giovanni Caria, Valerie Sappin-Didier, et al..Occurrence and fate of xenobiotic in sewage sludge and in sludge-amended soils. 15th SETAC EuropeAnnual Meeting, May 2005, Lille, France. 2005. �hal-01600155�

1- SETAC Conference May 2005

Occurrence and fate of xenobiotics

in sewage sludge and in sludge-amended soils

Dominique PATUREAU, M. Laforie, E. Lichtfouse, G. Caria, V. Sappin-Didier, L. Denaix, C. Mougin,

F. Dappozze, N. Christensen, K. Stamatelatou 1LBE-INRA Narbonne, France; 2INRA Avignon, France; 3LAS INRA Arras, France 4INRA Domaine de la Grande-Ferrade, Bordeaux, France ; 5Unit of Phytopharmacy and Semiochemicals, INRA Versailles, France 6Environment & Resources, Technical University of Denmark, Lyngby Denmark; 7Dept. Chemical Engineering, University of Patras, Patras Greece

This work was funded by the EU 5th Framework Program

contract n° QLK5-CT-2002-01138

www.biowaste.dk

Wastewater treatment and sewage sludge production...

• over 50.000 ww treatment plants

• ~ 7.9 millions tons of dry solids (2000)

• Amount will increase

Europe

Dump

40%

Incineration

11%

Spread

on land

37%

Others

6%

Discharge

in sea

6%

… and sewage sludge disposal

France

Incineration

15%

Spread

on land

60%

Dump

25%

Context

2- SETAC Conference May 2005

Are there Xenobiotics in wastewater ????

…and where do they accumulate ???

Storm water

Grey water

Yellow and brown water

Rivers, sediments

Soils, groundwaters

WWTP

because of low water solubility

of high affinity for organic matter

Industrial water

Context

3- SETAC Conference May 2005

4- SETAC Conference May 2005

Xenobiotics Sewage sludge spreading

on agricultural land

Environmental and human risks, public concern

Occurrence of xenobiotics in SS

Litterature survey and analysis of european SS

Fate of xenobiotics in sludge amended soils

From Lab-scale to field experiment

Goals of the project

Contamination of ecosystems and natural ressources

(soil, water, air)?

> Ecotoxicological risk assessment

Drinking polluted waters and eating polluted foods?

> Sanitary risk assessment

Xenobiotics assessed in the project

Context

O

O

O

O OHO

O

Nonylphenol

ethoxylate (NPE)

Polyaromatic hydrocarbon

(PAH)

SO3-,Na+

Linear alkylbenzene

sulfonate (LAS)

Phthalates

• Listed in EU legislation

• Level of concentration

• High toxicity (ED)

• Low biodegradation

• Persistance

5- SETAC Conference May 2005

6- SETAC Conference May 2005

Occurrence of xenobiotics in SS

Litterature survey and analysis

Measurement in water, soil and sediment

Less information in sludge

Various level of concentrations

diverse analytical methodologies (no std)

industrial wastewater

rain runoff collection

population size

type of WW treatment (AS, filters)

type of SS (primary, secondary)

type of SS treatment (AD, composting)

time (date, season, day)

7- SETAC Conference May 2005

Occurrence of xenobiotics in SS

Typically found concentration in EU SS

LAS : 100 - 15000 mg/kg DW

NPE : 25 - 500 mg/kg DW

Phthalates : 10 - 600 mg/kg DW

PAH (16) : 0.1 - 10 mg/kg DW

for other : less than 1 mg/kg to µg/kg

2600

50

100

6

3rd draft

of the SS

EU

Directive

8- SETAC Conference May 2005

Fate of xenobiotics in sludge amended soils

Lab-scale experiments : microcosms and radiolabelled molecules

Unpolluted soil as control

Soil spiked with labelled 14C-xenobiotic

Soil amended with a diverse spiked SS

non-transformed SS

anaerobically treated SS

anaerobically and composted SS

Adsorption - bound residus ?

Volatilization ?

Degradation - metabolites ?

Transfer to water or plant (radish) ?

Impact on bacterial and fungal communities ?

9- SETAC Conference May 2005

Fate of xenobiotics in sludge amended soils

Incubation time (days)

14C

re

co

ve

red

0

20

40

60

80

100Non extractable Extractable Mineralized

0 1 2 4 8 16 32 64 96

27 g dry silt loam sieved at 2 mm

40 mg/kg t-NP*, 80 % MHC, 25°C, darkness

Fast dissipation

mineralization

formation of bound residus

Strong impact of the SS

delay of degradation

higher adsorption

half life of 16 d and more

Low transfer to the plant

less than 9% radioactivity

metabolites ?

Impact on microorganisms

higher PLFA concentration

higher ratio fungi/bacteria

NP spiking on soil

Lab-scale experiments : microcosms and radiolabelled molecules

14C-balance +

HPLC analysis:

T½ ≈ 4 days

10- SETAC Conference May 2005

Fate of xenobiotics in sludge amended soils

Lab-scale experiments : microcosms and radiolabelled molecules

0.00

0.10

0.20

0.30

0.40

0.50

0.60

0.70

0.80

2-B6-T

(128)

3-B6-D

(125)

5-B30-D

(127)

4-B30-T

(126)

1-SD

(130)

dichlo

(122)

dichlo

(121)

dichlo

120

dichlo

119

chloro

118

chloro

117

dichlo

112

chloro

111

fungi / bacteria

Impact of sludge amendment on microorganisms : PLFA analysis

Higher ratio fungi/bacteria

No specific xenobiotic effect

11- SETAC Conference May 2005

Field experiment

Experimental maize crops, Bordeaux, France

Analysis of LAS, NPE,

Phthalates and PAH

Fate of xenobiotics in sludge amended soils

Sludges addition 100 tons sludges/ha/2yr (total 1000 tons)

Sampling

1993 1974 2004

12- SETAC Conference May 2005

Field experiment

Fate of xenobiotics in sludge amended soils

0

0.02

0.04

0.06

0.08

0.1

0.12

1976 1978 1979 1981 1986 1989 1993 1997 1999Time (year)

mg/kg DW Phe BbF Control Phe Control BbF

Results on PAH

SS 1991

Phe 0.9 mg/kg

BbF 0.3 mg/kg

PAH concentration 2-5 x higher in

slugdes-amended soils.

Levels increase during sludges

addition.

Levels still high 7 years after end

of slugdes addition.

Different behaviour towards

molecular weight

Long term impact of high molecular weight PAH

Results on LAS

0

2

4

6

8

10

12

14

16

18

1976

1978

1979

1981

1986

1989

1993

1997

1999

2004

Time (year)

mg/kg DW

LAS-C12

LAS-C13

Sum

Control LAS-C12

Control LAS-C13

Control Sum

Field experiment

Fate of xenobiotics in sludge amended soils

SS 1991

LAS 20 g/kg

13- SETAC Conference May 2005

Higher LAS

concentration in SS

Decrease and

stabilization

Adaptation -

degradation -

mobility?

Decrease to

background level after

10 years

Higher degradability (or mobility?)...

….less residual concentration in soil

14- SETAC Conference May 2005

Conclusions

Development of new methods for Xenobiotics analysis

Overview of occurrence and level of xenobiotics in EU SS

Fate in soil Fate of X in sludge-amended soil is adsorption-degradation dependant

Low transfer to plant and water

Long term soil accumulation of xenobiotics after sludge spreading for

the less degradable and most hydrophobic compounds

Impact Be careful to the mixed effect : sludge and xenobiotics in sludge

Measured effect at even high load of SS. What about at normal load?

15- SETAC Conference May 2005

Last but not least….

Thank you for your attention

» Men walked on the moon, now it’s time they learn how to walk on earth... « [ Henri de la Bretèche ]