1 Global Budgets of Atmospheric Glyoxal and Global Budgets of Atmospheric Glyoxal and Methylglyoxal and Implications for Methylglyoxal and Implications for Formation of Secondary Organic Aerosols Formation of Secondary Organic Aerosols Tzung-May Fu, Daniel J. Jacob Department of Earth and Planetary Sciences Harvard University Folkard Wittrock, John P. Burrows, Mihalis Vrekoussis Institute of Environmental Physics and Remote Sensing University of Bremen Fu et al. [2007b] submitted This work is supported by EPRI CHOCHO (glyoxa l) CH 3 C(O)CHO (methylglyox al) US EPA November 8 2007
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Tzung-May Fu, Daniel J. Jacob Department of Earth and Planetary Sciences Harvard University
Global Budgets of Atmospheric Glyoxal and Methylglyoxal and Implications for Formation of Secondary Organic Aerosols. CHOCHO (glyoxal). Tzung-May Fu, Daniel J. Jacob Department of Earth and Planetary Sciences Harvard University. CH 3 C(O)CHO (methylglyoxal). - PowerPoint PPT Presentation
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Global Budgets of Atmospheric Glyoxal and Global Budgets of Atmospheric Glyoxal and
Methylglyoxal and Implications for Formation of Methylglyoxal and Implications for Formation of
3 Acetone: global background and anthropogenic outflow
Fu et al. [2007b]
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Simulated dicarbonyl concentrations are Simulated dicarbonyl concentrations are consistent with available in situ measurementsconsistent with available in situ measurements
Dicarbonyls produce large amounts of SOA!Dicarbonyls produce large amounts of SOA!
6.7
9.0
11
1.8
Reversible partitioning Irreversible uptake by aerosol (10%) and clouds (90%)
SOA production via irreversible uptake of dicarbonyls comparable
to SOA production from reversible partitioning
Glyoxal 2.6
Methyl-gyloxal 8.0
AnthropogenicBiofuel useBiomass burningBiogenic
Fu et al. [2007b]
20%
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Are the reversible / irreversible production of SOA Are the reversible / irreversible production of SOA from isoprene oxidation products additive?from isoprene oxidation products additive?
Kroll et al. [2006], Surrat et al. [2006]
Isoprene
Methacrolein
Methyl vinyl ketone
SOA from reversible partitioningX
It is unclear, BUT
Experiments conducted at RH < 10% no aqueous reaction
(glyoxal and methylglyoxal)
(methylglyoxal)
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Major findings : Global budgets of dicarbonyls Major findings : Global budgets of dicarbonyls and their SOA productionand their SOA production
OH, NO3, O3
CHOCHO+
CH3COCHOIrreversible uptake
SOA production from dicarbonyls 11 Tg C y-1
Current simulated SOA sources from biogenic terpenes (9 Tg C y-1), isoprene (7 Tg C y-1) and aromatics are too small!
20% of SOA produced via dicarbonyls are from non-biogenic emissions, especially in FT
Fu et al. [2007b]
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Contribution of dicarbonyl SOA in U.S.Contribution of dicarbonyl SOA in U.S.
Aircraft measurements during ICARTT (summer 2004)
Water Soluble Organic Carbon by Rodney Weber at Georgia Tech
Samples influenced by biomass burning removed
Observed WSOC
Modelw/ dicarbonyl
SOA
Modelw/o dicarbonyl
SOA
Observed WSOCModel w/ dicarbonyl SOAModel w/o dicarbonyl SOA
Alt
itu
de
[km
]
WSOC [g C m-3 STP][g C m-3 STP]
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Observed WSOC
Model WSOC including SOA from dicarbonyl
Model WSOC without SOA from dicarbonyls
Correlation coefficient (r)
ICARTT WP3 measurements in FT (2 to 6 km), without biomass burning samples
WSOC correlation with other measured tracersWSOC correlation with other measured tracers
Dicarbonyl SOA
captures a lot of the observed variation
correlates with sulfate (aqueous processes) and toluene (anthropogenic precursors)0 0.1 0.2 0.3 0.4 0.5
OBS WSOC
CO
Sulfate
Methanol
Ammonium
Benzene
Toluene
PAN
Acetylene
Methyl nitrate
Ethyl nitrate
Isopropyl nitrate
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WSOC production in cloud – need regional modelWSOC production in cloud – need regional model
Measurements on Twin Otter during ICARTT (summer 2004)Sorooshian et al. [2006]
SO4OxalateNH4 NO3
Power plant plume in cloudsMeasured oxalate consistent with toluene being precursor
SO4 [nmol m-3]
Oxa
late
[
nm
ol
m-3]
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Using suite of satellite observations to diagnose Using suite of satellite observations to diagnose regional pollutant emission and chemistryregional pollutant emission and chemistry