Monoterpene and Sesquiterpene Emissions from Ponderosa Pine: Implications for Secondary Organic Aerosol Formation
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1 Monoterpene and Sesquiterpene Emissions from Ponderosa Pine: Implications for Secondary Organic Aerosol Formation Anita Lee, Gunnar Schade, Allen Goldstein UC Berkeley GCEP Workshop: August 19, 2002
2 What are Monoterpenes? C 10 H 16 : class of volatile organic compound Emitted by all conifers and some flowering plants Used for defense Many different species emitted -pinene -pinene -carene
3 Why Monoterpenes? Biogenic VOC emissions 10 greater than anthropogenic emissions Reactive! Consumes OH radical: Oxidizing capacity of the atmosphere Tropospheric ozone production Secondary organic aerosol (SOA) production
4 Why Sesquiterpenes? C 15 H 24 Heavy VOC particle phase More double bonds more reactive Currently little is known Germacrene D -Caryophyllene
5 Monoterpenes and Sesquiterpenes
6 OH, O 3, NO 3 Monoterpenes and Sesquiterpenes
7 Gas-Phase Oxidation Products: nopinone, pinic acid, pinonic acid OH, O 3, NO 3 Monoterpenes and Sesquiterpenes
8 Secondary Organic Aerosol Gas-Phase Oxidation Products: nopinone, pinic acid, pinonic acid OH, O 3, NO 3 Monoterpenes and Sesquiterpenes
9 Nucleation Secondary Organic Aerosol New Particle Formation Gas-Phase Oxidation Products: nopinone, pinic acid, pinonic acid OH, O 3, NO 3 Monoterpenes and Sesquiterpenes
10 Nucleation Secondary Organic Aerosol New Particle Formation Pre-Existing Aerosol Absorption, Adsorption, Condensation Gas-Phase Oxidation Products: nopinone, pinic acid, pinonic acid OH, O 3, NO 3 Monoterpenes and Sesquiterpenes
11 Ultrafine: d p < 0.1 m Particle Phase Nucleation Secondary Organic Aerosol New Particle Formation Pre-Existing Aerosol Absorption, Adsorption, Condensation Gas-Phase Oxidation Products: nopinone, pinic acid, pinonic acid OH, O 3, NO 3 Monoterpenes and Sesquiterpenes
12 Ultrafine: d p < 0.1 m Particle Phase Accumulation: 0.1 < d p < 2 m Coarse: 2 < d p < 10 m Nucleation Secondary Organic Aerosol New Particle Formation Pre-Existing Aerosol Absorption, Adsorption, Condensation Gas-Phase Oxidation Products: nopinone, pinic acid, pinonic acid OH, O 3, NO 3 Monoterpenes and Sesquiterpenes
13 Water Cloud Condensation Nuclei Radiation Absorption or Reflectance Visible Light Scattering Ultrafine: d p < 0.1 m Particle Phase Accumulation: 0.1 < d p < 2 m Coarse: 2 < d p < 10 m Nucleation Secondary Organic Aerosol New Particle Formation Pre-Existing Aerosol Absorption, Adsorption, Condensation Gas-Phase Oxidation Products: nopinone, pinic acid, pinonic acid OH, O 3, NO 3 Monoterpenes and Sesquiterpenes
14 Regional and Global Effects on Climate Water Cloud Condensation Nuclei Radiation Absorption or Reflectance Visible Light Scattering Ultrafine: d p < 0.1 m Particle Phase Accumulation: 0.1 < d p < 2 m Coarse: 2 < d p < 10 m Nucleation Secondary Organic Aerosol New Particle Formation Pre-Existing Aerosol Absorption, Adsorption, Condensation Gas-Phase Oxidation Products: nopinone, pinic acid, pinonic acid OH, O 3, NO 3 Monoterpenes and Sesquiterpenes
15 Regional and Global Effects on Climate Water Cloud Condensation Nuclei Radiation Absorption or Reflectance Visible Light Scattering Ultrafine: d p < 0.1 m Particle Phase Accumulation: 0.1 < d p < 2 m Coarse: 2 < d p < 10 m Nucleation Secondary Organic Aerosol New Particle Formation Pre-Existing Aerosol Absorption, Adsorption, Condensation Gas-Phase Oxidation Products: nopinone, pinic acid, pinonic acid OH, O 3, NO 3 Monoterpenes and Sesquiterpenes
16 Gas-Phase Oxidation Products: nopinone, pinic acid, pinonic acid OH, O 3, NO 3 Monoterpenes and Sesquiterpenes
17 Outline On-going field measurements of speciated monoterpenes using GC-FID Laboratory chamber measurements of monoterpenes and sesquiterpenes from Ponderosa Pine New field measurements of total monoterpenes using PTR-MS Preliminary Data!
18 Blodgett Forest CO 2, H 2 O, Ozone, VOC, CO and H 2 (Goldstein) NO x, NO y (Cohen) Aerosols (Lunden) Why ponderosa pine? Important tree in Western U.S Major emitter of terpenes, MBO Ozone sensitive Sacramento San Francisco Blodgett Day Night CALIFORNIA Airmass Trajectories Ponderosa Pine Distribution
19 Speciated Terpene Flux 2 channel GC-FID Relaxed Eddy Accumulation v w u
20 Speciated Terpene Flux 2 channel GC-FID Relaxed Eddy Accumulation v w u C u Updrafts
21 Speciated Terpene Flux 2 channel GC-FID Relaxed Eddy Accumulation v w u C d Downdrafts C u Updrafts
22 Speciated Terpene Flux 2 channel GC-FID Relaxed Eddy Accumulation v w u C d Downdrafts One measurement each hour F = bσ w (C up - C down ) C u Updrafts
23 Speciated Monoterpene Mixing Ratios Mixing Ratio (ppb) b-pinene 3-carene a-pinene limonene + b-phellandrene Mixing Ratio (ppb) Day of Year July myrcene camphene a-terpinene g-terpinene terpinolene Day of Year July 27-30
24 New Directions Further understand impact of terpenes on regional air chemistry Link terpene oxidation with SOA production SOA production: 18.5 (30-270) Tg C year -1 Constrain SOA production from mono- and sesquiterpenes Explain observed nucleation events
25 Nucleation Burst on 10/6/ D p (nm) Day dn/dlog(d p ) (cm -3 ) M. Lunden and D. Black, LBNL 2001
26 New Instrumentation Fast real-time measurements of terpenes and their oxidation products Proton Transfer Reaction Mass Spectrometer Quadrupole Mass Spectrometer Chemical ionization using H 3 O + Compounds with proton affinity higher than water trace atmospheric constituents Softer ionization Less Fragmentation
27 PTR-MS
28 Chamber Measurements Test detection of mono- and sesquiterpenes and their oxidation products Compare emissions rates Determine temperature response Quantify emissions from litter and other plant species Preliminary look at ozone oxidation Data analysis still in progress!
29 Ozone Oxidation of Mono- and Sesquiterpenes mass 137 (ug/g dw/h) mass monoterpenes Chamber T (C) Ozone Added Temperature (C) mass 205 (ug/g dw/h) Time (min) mass sesquiterpenes mass norpinic acid? Ozone Added Time (min) mass 173 (ug/g dw/hour)
30 Flux Measurements All monoterpene species share same mass PTR-MS Total monoterpenes Total vs. speciated monoterpene fluxes Total Sesquiterpene Fluxes? Terpene Oxidation Products Lots of other interesting compounds Field deployment last month
31
32
33 New Measurements Flux of total monoterpenes and oxidation products v w u C d Downdrafts PTR-MS 2-8 Hz Eddy Covariance F = w C C u Updrafts
34 Meteorological Controls on Total Monoterpene Mixing Ratios 3.0 PTR-MS Total Monoterpene Co Day of Year July Wind Speed (m/s) 1
35 Meteorological Controls on Total Monoterpene Flux monoterpene flux (mg C m-2 h PTR-MS air temperature (deg C) day of year 2002
36 Speciated measurements miss 30 50% of total emissions 3.0 PTRMS GCFID Total Monoterpene Mix Day of Year July 26-30
37 Observations of Beta-pinene oxidation product? Total Monoterpene Mixing R Day of Year July ppt nopinone observed elsewhere (Calogiou et al. 1999, Yu et al. 1999) 0.0 Mass Nopinone?
38 Take Home Messages! Terpene and oxidation product concentrations and fluxes can be measured by PTRMS-EC Terpenes are a natural but poorly characterized source of aerosol New Particle Formation Events depend on: local meteorology: temperature, depth of BL concentration of pre-existing aerosol terpene and oxidant species and concentrations Complex system! Trees do not cause air pollution!
39 Thanks to... DOE Global Change Education Program Blodgett Forest Research Station Sierra Pacific Industries National Science Foundation California Air Resources Board
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