PCDD/Fs are not only generated by copper catalysis: the ......Attempted assassination of Viktor...
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PCDD/Fs are not only generated by copper catalysis: the inconvenient truth about biofuels 6th VERT Forum: Particle Filter Technologies, both for diesel and GDI vehicles Dübendorf, March 20, 2015
Transcript of PCDD/Fs are not only generated by copper catalysis: the ......Attempted assassination of Viktor...
PCDD/Fs are not only generated by copper
catalysis: the inconvenient truth about biofuels
6th VERT Forum: Particle Filter Technologies, both for diesel and GDI vehicles
Dübendorf, March 20, 2015
Yes, biofuels can convert inactive into active filters
Do not generalize here
Three things to remember
Yes, some catalytic DPFs support a PCDD/F formation
PCDD/Fs are not only generated by copper
catalysis: the inconvenient truth about biofuels
Active DPFs: current knowledge
PCDD/F formation with biofuels: the inconvenient truth
The outline
PCDD/Fs two classes of compounds
PCDD/Fs are not only generated by copper
catalysis: the inconvenient truth about biofuels
VERT Secondary emissions test
PCDD/F Formation Potential
Yes, there are risks for a PCDD/F formation in DPFs - they should be assessed!
Soot, O2
Cl, PrecursorsDPF
CO2, H2O
PCDD/Fs?catalyzed
PCDD/Fs: Two classes of compounds
PCDD/Fs are aromatic 3-ring systems related to certain PAHs?
Polychlorinated dibenzodioxins/furans (PCDD/Fs)
2,3,7,8-Tetrachlorodibenzodioxin - the so-called Seveso-dioxin
2,3,7,8-TCDD – the most toxic congener!
PCDD/Fs: toxic at pg-quantities
Thermally stable up to 440°C
Solid, non-volatile, particle-bound
Should be trapped in DPFs unless formed de novo
Highly toxic, bind to Aryl hydrocarbon receptor Persistent, bioaccumulative, ubiquitousRegulated under Stockholm convention on POPs Contaminants in pesticides, e.g. trichlorophenolsfor herbicides, Agent orange (defoliation agent applied in the Vietnam war by U.S. troops)
Unwanted combustion products
PCDD&F Properties:
The dioxin problem
Dioxin formation in Seveso (1976)
Attempted assassination of Viktor Yushchenko,
former President of the UkraineWhat happened during the 2004 presidential election campain in the Ukraine?
Before
Attempted assassination of Viktor Yushchenko,
former President of the UkraineWhat happened during the 2004 presidential election campain in the Ukraine?
Before and after the severe dioxin poisoning
Attempted assassination of Viktor Yushchenko,
former President of the Ukraine1st order decrease of 2,3,7,8-TCDD levels in the months and years after the poisoning
2,3,7,8-TCDD, the only congener found
Serum : TCDD (t) = 106'000 (pg/g lw) e-0.04276 t
t1/2 = 16.2 months
Fat : TCDD (t) = 107'000 (pg/g lw) e-0.04429 t
t1/2 = 15.7 months
Serum and fat TCDD levels (based on lipid weight)
2005
2006
2007
2008
2009
2010
Attempted assassination of Viktor Yushchenko,
former President of the UkraineWhat happened during the 2004 presidential election campain in the Ukraine?
2,3,7,8-TCDD, the only congener found
Serum : TCDD (t) = 106'000 (pg/g lw) e-0.04276 t
t1/2 = 16.2 months
Fat : TCDD (t) = 107'000 (pg/g lw) e-0.04429 t
t1/2 = 15.7 months
Serum and Fat based on lipid weight
Poisoned Sunday, Sept 5, 2004 Dinner with SBU
(Ukrainian National Security)
Uptake of approximately 1-2 mg TCDD !
Second highest TCDD serum level in a human body ever
measured
50‘000 x more than the normal population (2 pg/g lipid)
Nov 23, J. Henry, St. Mary‘s Hospital, London suggests
dioxin poisoning
Dec 17, two independent laboratories confirmed that
exclusively 2,3,7,8-TCDD was found in the blood
(108’000 and 109‘000 ng/kg lipid)
Sorg, O., Zennegg, M. Schmid, P. et al. The Lancet, 2009, 9696, 1179-85
Viktor Yushchenko was poisoned with synthesized material,
PCDD/Fs formed in combustion reactions, e.g. in certain active
DPFs produce quite different pattern!
The dibenzodioxin class of compounds (PCDDs)
We surely assess 2,3,7,8-TCDD, but should have an eye on other congeners as well?
Chemical structures of polychlorinated dibenzodioxins
1x
O
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2,3,7,8-Tetrachlorodibenzofuran
What abuot 2,3,7,8-TCDF?
The dibenzofuran class of compounds (PCDFs)
Why not 2,3,7,8-TCDF or others of the 135 congeners?
Chemical structures of polychlorinated dibenzofurans
0.1x
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The dibenzofuran class of compounds (PCDFs)
Active DPFs: current knowledge
PCDD/F formation with biofuels: the inconvenient truth
Biodiesel can alter the PCDD/F formation potential of Fe-catalyzed DPFs
PCDD/Fs two classes of compounds
PCDD/Fs are not only generated by copper
catalysis: the inconvenient truth about biofuels
Engine out emissions or emissions of inactive DPFs are on average 4 +/- 3 pg/L
Assessment of the PCDD/F-formation potential
10x
Only few filters exceeded the engine out level?
Assessment of the PCDD/F-formation potential
100x
Assessment of the PCDD/F-formation potential
Only 3 of the 37 tested DPFs induced a PCDD/F formation?
Assessment of the PCDD/F-formation potential
These 3 active DPFs exceed the MWI emission limit of 100 pg/m3 exhaust
Cu
Fe/Cu Fe/K
19
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20
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Certain DPFs are not compatible with certain biofuels!
Cu
Fe/Cu
Fe/K
PCDD/F Formation Potential of DPFs:
New Risks with Biofuels?
Fe/B
ioK
Fe
/K
Fe
It’s bio!It’s fossil fuel! (fossilized biofuel)
Possibly thousands of vehicles with Fe-catalyzed DPFs might become active,
when exposed to biofuels, as foreseen by EU legislation!
Fe
Fe
Fe
Fe
Fe
Fe
FeFe Fe
Fe
Fe
PCDD/F Formation Potential of DPFs:
New Risks with Biofuels?
Fe/K
Fe/K
Fe/K
Fe/C
u
Cu
Fe/B
ioK
Potassium, independent of its origin, converts an inactive into an active Fe-DPF
Fold increase compared to reference
PCDD/F Formation Potential of DPFs:
New Risks with Biofuels?
What about 2,3,7,8-TCDF?
Fold increase compared to reference
PCDD/F Formation Potential of DPFs:
New Risks with Biofuels?
Smaller effects on the 17 toxic PCDD/Fs!
Fold increase compared to reference
PCDD/F Formation Potential of DPFs:
New Risks with Biofuels?
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Why not assessing congener classes like Cl4-, Cl5-, Cl6-, Cl7- & Cl8DDs?
Chemical structures of polychlorinated dibenzodioxins
1 Cl82 Cl710 Cl6
22 Cl4
14 Cl5
Assessment of the PCDD/F-formation potential
OCl
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Cl
Cl
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O
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ClCl
O
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Cl
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ClCl
Cl
OCl
ClClCl
OCl
ClCl
Cl
OCl
ClCl
Cl
OCl
ClCl
Cl
Cl
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Cl
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O
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Cl
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Cl
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Cl
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Cl
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Cl
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Cl
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Cl
O
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Cl
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Cl
Cl
Chemical structures of polychlorinated dibenzofurans
1 Cl84 Cl7
16 Cl6
38 Cl4
28 Cl5
Assessment of the PCDD/F-formation potential
Why not assessing congener classes like Cl4-, Cl5-, Cl6-, Cl7- & Cl8DFs?
Pattern changes?
5% PCDDs / 95% PCDFs
Fe/K and Fe/BioK similarl!
Analysis of congener patterns
5% PCDDs / 95% PCDFs
things get red with biofuel!
40% PCDDs / 60% PCDFs
not much change!
Congener-specific effects
Preferential formation of TCDFs!
80 x increase of Cl4-DFs
16 x increase of Cl4-DDs
20 x increase of Cl4-DDs140 x increase of Cl4-DFs
PCDD/F Formation Potential of DPFs:
New Risks with Biofuels?K, bio or not, can promote a PCDD/F formation in certain Fe-catalyzed DPFs
In all Fe-catalyzed DPFs?F
e
Fe
Fe
Fe
Fe
Fe
FeFe Fe
Fe
Fe
PCDD/F Formation Potential of DPFs:
New Risks with Biofuels?
Fe/K
Fe/K
Fe/K
Fe/C
u
Cu
Fe/B
ioK
PCDD/F formation in DPFs is a potential risk
The chemical nature of the catalyst is important
Biofuels can alter the PCDD/F potential of DPFs
There are DPFs out, which may become active over time
when exposed to biofuel exhausts
PCDD/F potential of any new type of DPF has to be
tested, also with biofuels
Conclusions:
Possibly thousands of vehicles with Fe-catalyzed DPFs might become active,
when exposed to biofuels, as foreseen by EU legislation!
PCDD/Fs are not only generated by copper
catalysis: the inconvenient truth about biofuels
A combined effort with many important contributions
Thanks: VERT team: Andreas Mayer, TTM
Jan Czerwinski, Yan Zimmerli, Claudio Chiesura, Sandro Napoli, Tobias Neubert,
Thomas Hilfiker, Jean-Luc Petermann, Peter Bonsack, Samuel Bürki, Uni. Appl. Sci., Biel.
Markus Kasper, Adrian Hess, Thomas Mosimann, Matter Aerosol, Wohlen
Hans Jaeckle, Urs Debrunner, Oliver Schumm, Intertek Caleb Brett.
Empa colleagues: Brigitte Buchmann, Thomas Bührer, Lukas Emmenegger, Anna-Maria Forss,
Urs Gfeller, Maria Guecheva, Peter Graf, Roland Graf, Erika Guyer, Regula Haag, Peter Honnegger, Judith Kobler, Martin Kohler, Peter Lienemann, Alfred Mack, Peter Mattrel, Martin
Mohr, Joachim Mohn, Christof Moor, Andreas Paul, Maria Dolores Rey, Peter Schmid, Cornelia
Seiler, Andrea Ulrich, Heinz Vonmont, Thomas Walter, Max Wolfensberger, Daniela Wenger, Adrian Wichser, Markus Zennegg, Kerstin Zeyer.
Governement: Giovanni D’Urbano, Felix Reutimann, Max Wyser, Gerhard Leutert, Martin Schiess,
Swiss Federal Office for Environment
Thomas Gasser, Heinz Berger, Gerhard Stucki, Swiss Federal Road Office
Filter-, catalyst-, engine & vehicle manufacturers:
PCDD/Fs are not only generated by copper
catalysis: the inconvenient truth about biofuels
Yes, biofuels can convert inactive into active filters
Do not generalize here
Three things to remember
Yes, some catalytic DPFs support a PCDD/F formation
PCDD/Fs are not only generated by copper
catalysis: the inconvenient truth about biofuels
