AARHUSUNIVERSITET
TITEL PÅ PRÆSENTATIONNAVN NAVNESEN
2. MAJ 2011 VERSITETUNI
Dynamics of biocide emissions from buildings in a suburban stormwater catchment Ulla E. Bollmann1, Jes Vollertsen2, Kai Bester1
30. Jan. 2014
1 Aarhus University, Roskilde, Denmark2 Aalborg University, Aalborg, Denmark
www.waterpurification.au.dk
AARHUSUNIVERSITET
TITEL PÅ PRÆSENTATIONNAVN NAVNESEN
2. MAJ 2011DYNAMICS OF BIOCIDE EMISSIONS FROM BUILDINGS IN A SUBURBAN STORMWATER
CATCHMENT U. E. Bollmann, J. Vollertsen, K. Bester
Jan. 20142
Introduction
› State-of-the-art in material protection› Preservatives for polymer based coatings:
façade render and paint› Wood protection, Roof protection (flat roofs)
› Content in exterior renders and paints› 2-4 different biocides, 0.1-1 g kg-1 each› Total: 0.2% in render, 0.2-0.4% in exterior paints
› Different compounds with biocidal effects› Isothiazolinones, carbamates, phenylureas, triazines,
triazoles used as algaecides, fungicides and bactericides
› Hydrophilic molecules with toxic effects
Burkhardt et al., WS&T 2007, 56, (12), 63-67Schoknecht et al., ES&T 2009, 43, (24), 9321-9328
Burkhardt et al., WS&T 2011, 63, (9), 1974-1982
Biocidesin building material
Principal construction of external thermal insulation composite system (ETICS)
AARHUSUNIVERSITET
TITEL PÅ PRÆSENTATIONNAVN NAVNESEN
2. MAJ 2011DYNAMICS OF BIOCIDE EMISSIONS FROM BUILDINGS IN A SUBURBAN STORMWATER
CATCHMENT U. E. Bollmann, J. Vollertsen, K. Bester
Jan. 2014
Introduction
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biocidesBiocidesin building material
Effectson aquatic organisms
Which compounds? Concentrations?
Dynamics? First flush emissions?
Which compounds? Concentrations?
Dynamics? First flush emissions??
Biocidesin building material
› Laboratory experiments:› Constantly soaked test material and dipping experiments (wet
and dry cycles)› Leaching dependent on: Substance & render properties,
Immersion
› Field study:› Concentrations in small Swiss catchment: 0.01-1 µg L-1
(Terbutryn, Carbendazim, Mecoprop)Burkhardt et al. 2007, 2009 & 2012, Schoknecht et al. 2003 & 2009, Wangler et al. 2012, Wittmer et al. 2010
AARHUSUNIVERSITET
TITEL PÅ PRÆSENTATIONNAVN NAVNESEN
2. MAJ 2011DYNAMICS OF BIOCIDE EMISSIONS FROM BUILDINGS IN A SUBURBAN STORMWATER
CATCHMENT U. E. Bollmann, J. Vollertsen, K. Bester
Jan. 2014
Catchment
› Silkeborg (Denmark)› 21.5 ha, 7 ha connected to sewer, separated sewer system› Suburban, residential, 140 well-kept single family houses› 5 % equipped with renders/paints, 20 % (painted) wood, 75 %
brick-facades
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TITEL PÅ PRÆSENTATIONNAVN NAVNESEN
2. MAJ 2011DYNAMICS OF BIOCIDE EMISSIONS FROM BUILDINGS IN A SUBURBAN STORMWATER
CATCHMENT U. E. Bollmann, J. Vollertsen, K. Bester
Jan. 2014
Sampling / Analysis
› Flow proportional high resolution sampling with automatic water sampler› October 2011-June 2012
› Solid phase extraction
› High performance liquid chromatography tandem mass spectrometry (HPLC-MS/MS)
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TITEL PÅ PRÆSENTATIONNAVN NAVNESEN
2. MAJ 2011DYNAMICS OF BIOCIDE EMISSIONS FROM BUILDINGS IN A SUBURBAN STORMWATER
CATCHMENT U. E. Bollmann, J. Vollertsen, K. Bester
Jan. 2014
› 191 samples, 11 biocides
Concentrations
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AA-EQS for fresh water
DIRECTIVE 2013/39/EU
Terbutryn: 65 ng L-1
Cybutryn: 2.5 ng L-1
Diuron: 200 ng L-1Isoproturon: 300 ng L-1
IT: Isothiazolinone Bollmann et al., 2014, submitted
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2. MAJ 2011DYNAMICS OF BIOCIDE EMISSIONS FROM BUILDINGS IN A SUBURBAN STORMWATER
CATCHMENT U. E. Bollmann, J. Vollertsen, K. Bester
Jan. 2014
Mass loads
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IT: IsothiazolinoneBollmann et al., 2014, submitted
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2. MAJ 2011DYNAMICS OF BIOCIDE EMISSIONS FROM BUILDINGS IN A SUBURBAN STORMWATER
CATCHMENT U. E. Bollmann, J. Vollertsen, K. Bester
Jan. 2014
Biocides in buildings
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biocidesBiocidesin building material
Effectson aquatic organisms
Which compounds? Concentrations?
Dynamics? First flush emissions?
Which compounds? Concentrations?
Dynamics? First flush emissions??
AARHUSUNIVERSITET
TITEL PÅ PRÆSENTATIONNAVN NAVNESEN
2. MAJ 2011DYNAMICS OF BIOCIDE EMISSIONS FROM BUILDINGS IN A SUBURBAN STORMWATER
CATCHMENT U. E. Bollmann, J. Vollertsen, K. Bester
Jan. 20149
Emission dynamics
› How are the biocides emitted within the storm event?
› Particle mobilisation in road run-off with first flush
Time
Load
WaterParticles,Heavy metals
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2. MAJ 2011DYNAMICS OF BIOCIDE EMISSIONS FROM BUILDINGS IN A SUBURBAN STORMWATER
CATCHMENT U. E. Bollmann, J. Vollertsen, K. Bester
Jan. 201410
Emission dynamics
› Common event
TB: Terbutryn , CD: Carbendazim, IP: Isoproturon, TBU: Tebuconazole, MCPP: Mecoprop
Bollmann et al., 2014, submitted
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2. MAJ 2011DYNAMICS OF BIOCIDE EMISSIONS FROM BUILDINGS IN A SUBURBAN STORMWATER
CATCHMENT U. E. Bollmann, J. Vollertsen, K. Bester
Jan. 2014
› First flush: occurs irregularly
Emission dynamics
11
First flush
TB: Terbutryn , CD: Carbendazim, IP: Isoproturon, TBU: Tebuconazole, MCPP: Mecoprop
Bollmann et al., 2014, submitted
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2. MAJ 2011DYNAMICS OF BIOCIDE EMISSIONS FROM BUILDINGS IN A SUBURBAN STORMWATER
CATCHMENT U. E. Bollmann, J. Vollertsen, K. Bester
Jan. 2014
Emission dynamics
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First flush for selected biocides
Fast mobilization of biocidesfrom the façade surface
Unnecessary loss of substanceFine tune application?
No first flush for biocides
Constant emissions Partitioning from the facade
No selected stormwatertreatment possible
Common event Special event
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2. MAJ 2011DYNAMICS OF BIOCIDE EMISSIONS FROM BUILDINGS IN A SUBURBAN STORMWATER
CATCHMENT U. E. Bollmann, J. Vollertsen, K. Bester
Jan. 2014
Emission dynamics
› What is influencing the leaching?
› Correlation of the concentration or acc. mass load per event with:
› Rain amount / accumulated flow› Length of the event› Rain intensity› Length of the dry period prior to the event
› Wind driven rain intensity
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TITEL PÅ PRÆSENTATIONNAVN NAVNESEN
2. MAJ 2011DYNAMICS OF BIOCIDE EMISSIONS FROM BUILDINGS IN A SUBURBAN STORMWATER
CATCHMENT U. E. Bollmann, J. Vollertsen, K. Bester
Jan. 2014
Emission dynamics
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Wind Driven Rain (WDR)
WD
R
WIND RAIN
𝐼𝑊𝐷𝑅=29𝐶𝑅𝐶𝑇𝑂𝑊 𝐼𝑅𝑎𝑖𝑛𝑈 cosθ
Blocken & Carmeliet , J. Wind Eng. Ind. Aerodyn. 2004, 92, 1079Burkhardt et al., Environ. Sci. Technol. 2012, 46, 5497
𝐼𝑊𝐷𝑅=𝐶𝐶 𝐼𝑅𝑎𝑖𝑛𝑈with CC = catchment specific factor
𝑀𝑊𝐷𝑅=𝐶𝐶𝐶𝑆 𝐼𝑅𝑎𝑖𝑛𝑈Mass flow M during respective event
with CS = substance specific constant
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TITEL PÅ PRÆSENTATIONNAVN NAVNESEN
2. MAJ 2011DYNAMICS OF BIOCIDE EMISSIONS FROM BUILDINGS IN A SUBURBAN STORMWATER
CATCHMENT U. E. Bollmann, J. Vollertsen, K. Bester
Jan. 2014
Emission dynamics
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CD: Carbendazim, TB: Terbutryn, PPZ: Propiconazole, TBU: TebuconazoleBollmann et al., 2014, submitted
AARHUSUNIVERSITET
TITEL PÅ PRÆSENTATIONNAVN NAVNESEN
2. MAJ 2011DYNAMICS OF BIOCIDE EMISSIONS FROM BUILDINGS IN A SUBURBAN STORMWATER
CATCHMENT U. E. Bollmann, J. Vollertsen, K. Bester
Jan. 2014
Biocides in buildings
16
biocidesBiocidesin building material
Effectson aquatic organisms
Conclusions
AARHUSUNIVERSITET
TITEL PÅ PRÆSENTATIONNAVN NAVNESEN
2. MAJ 2011DYNAMICS OF BIOCIDE EMISSIONS FROM BUILDINGS IN A SUBURBAN STORMWATER
CATCHMENT U. E. Bollmann, J. Vollertsen, K. Bester
Jan. 2014
Conclusions
› Monitoring› Biocides also important pollutants in Danish urban areas› Different footprint than in other European countries
Hard to set-up a sound monitoring strategy
› Emission dynamics› Usually rather constant throughout an event› Irregular first flush phenomena› Indication for correlation between occurrence in
storm water and wind driven rain
› Treatment› Need to take the dynamics of the biocide
emission into account
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AARHUSUNIVERSITET
TITEL PÅ PRÆSENTATIONNAVN NAVNESEN
2. MAJ 2011DYNAMICS OF BIOCIDE EMISSIONS FROM BUILDINGS IN A SUBURBAN STORMWATER
CATCHMENT U. E. Bollmann, J. Vollertsen, K. Bester
Jan. 2014
Acknowledgement
› Scientific cooperation:› Jan Carmeliet and Timothy Wangler (ETH Zurich, Switzerland)› Michael Burkhardt (HSR, Rapperswil, Switzerland)
› Diverse companies in the sector for the willingness to share materials and knowledge
› Financial support:› Danish EPA through the project Methods for the improvement of
scenarios concerning the emission of biocides from buildings (667-00065 & 667-00066)
› AUFF grant: Advanced water purification using bio-inorganic nano catalysts and soil filters (www.waterpurification.au.dk)
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Thank you for your attention!
AARHUSUNIVERSITET
TITEL PÅ PRÆSENTATIONNAVN NAVNESEN
2. MAJ 2011 VERSITETUNI
Dynamics of biocide emissions from buildings in a suburban stormwater catchment Ulla E. Bollmann1, Jes Vollertsen2, Kai Bester1
30. Jan. 2014
1 Aarhus University, Roskilde, Denmark2 Aalborg University, Aalborg, Denmark
www.waterpurification.au.dk