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

Dominique Patureau, Mireille Laforie, Eric Lichtfouse, Giovanni Caria, Valerie Sappin-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 Europe Annual Meeting, May 2005, Lille, France. 2005. [hal-01600155](https://hal.science/hal-01600155)

HAL Id: hal-01600155

https://hal.science/hal-01600155

Submitted on 4 Jun 2020

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# 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

This work was funded by the EU 5th Framework Program contract n°QLK5-CT-2002-01138

www.biowaste.dk

<footnote n="1">¹LBE-INRA Narbonne, France; ²INRA Avignon, France; ³LAS INRA Arras, France</footnote>

<footnote n="4">⁴INRA Domaine de la Grande-Ferrade, Bordeaux, France; ⁵Unit of Phytopharmacy and Semiochemicals, INRA Versailles, France</footnote>

<footnote n="6">⁶Environment & Resources, Technical University of Denmark, Lyngby Denmark;</footnote>

<footnote n="7">⁷Dept. Chemical Engineering, University of Patras, Patras Greece</footnote>
Context

Wastewater treatment and sewage sludge production...

<figure><img src="image_2.png" /></figure>

* over 50.000 ww treatment plants

* ~7.9 millions tons of dry solids (2000)

* Amount will increase

... and sewage sludge disposal

<figure><img src="image_3.png" /></figure>

<figure><img src="image_4.png" /></figure>

<figure><img src="image_5.png" /></figure>
Context

Are there Xenobiotics in wastewater ????

<figure><img src="image_6.png" /></figure>

...and where do they accumulate ???

because of low water solubility
of high affinity for organic matter
# Goals of the project

Xenobiotics

<figure><img src="image_7.png" /></figure>

Sewage sludge spreading
on agricultural land

<figure><img src="image_8.png" /></figure>

Environmental and human risks, public concern

* Contamination of ecosystems and natural resources (soil, water, air)?

> *Ecotoxicological risk assessment*

* Drinking polluted waters and eating polluted foods?

> *Sanitary risk assessment*

<figure><img src="image_9.png" /></figure>

**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
Xenobiotics assessed in the project

<figure><img src="image_10.png" /><figcaption>Linear alkylbenzene
sulfonate (LAS)</figcaption></figure>

<figure><img src="image_11.png" /><figcaption>Phthalates</figcaption></figure>

<figure><img src="image_12.png" /><figcaption>Nonylphenol
ethoxylate (NPE)</figcaption></figure>

<figure><img src="image_13.png" /><figcaption>Polyaromatic hydrocarbon
(PAH)</figcaption></figure>

• Listed in EU legislation

• Level of concentration

• High toxicity (ED)

• Low biodegradation

• Persistance
<figure><img src="image_14.png" /></figure>

## 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)
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

3rd draft
of the SS
EU
Directive

2600

50

100

6
<figure><img src="image_15.png" /></figure>

## 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 residues ?

- Volatilization ?

- Degradation - metabolites ?

- Transfer to water or plant (radish) ?

- Impact on bacterial and fungal communities ?

<figure><img src="image_16.png" /></figure>
<figure><img src="image_17.png" /></figure>

# Fate of xenobiotics in sludge amended soils

## Lab-scale experiments : microcosms and radiolabelled molecules
### NP spiking on soil

27 g dry silt loam sieved at 2 mm
40 mg/kg t-NP*, 80 % MHC, 25°C, darkness

<figure><img src="image_18.png" /></figure>

¹⁴C-balance +
HPLC analysis:

T½ ≈ 4 days

* Fast dissipation
  mineralization
  formation of bound residues

* 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
<figure><img src="image_19.png" /></figure>

## Lab-scale experiments : microcosms and radiolabelled molecules

### Impact of sludge amendment on microorganisms : PLFA analysis

<figure><img src="image_20.png" /></figure>
<figure><img src="image_21.png" /></figure>

## Field experiment

### Experimental maize crops, Bordeaux, France

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

<figure><img src="image_22.png" /></figure>

Sampling

<figure><img src="image_23.png" /></figure>

1993

2004

1974

2004

<figure><img src="image_24.png" /></figure>

Analysis of LAS, NPE, Phthalates and PAH

<figure><img src="image_25.png" /></figure>
<figure><img src="image_26.png" /></figure>

## Field experiment

### Results on PAH

<figure><img src="image_27.png" /></figure>

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
<figure><img src="image_28.png" /></figure>

## Field experiment

### Results on LAS

<figure><img src="image_29.png" /></figure>

* 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
# 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 dependent

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?
Thank you for your attention

<figure><img src="image_30.png" /></figure>

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