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Hydrogen Peroxide Methylhydroperoxide Formaldehyde & (Peroxyacetic Acid)

Hydrogen Peroxide Methylhydroperoxide Formaldehyde & (Peroxyacetic Acid). Brian G. Heikes & Haiwei Shen, URI Daniel W. O’Sullivan, USNA Julie A. Snow, Slippery Rock U. Our INTEX Objectives In Measuring Title Compounds. Tropospheric Ozone Radical Oxidants: HO, HO2, CH3OO, CH3C(O)OO ?

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Hydrogen Peroxide Methylhydroperoxide Formaldehyde & (Peroxyacetic Acid)

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  1. Hydrogen PeroxideMethylhydroperoxideFormaldehyde & (Peroxyacetic Acid) Brian G. Heikes & Haiwei Shen, URI Daniel W. O’Sullivan, USNA Julie A. Snow, Slippery Rock U.

  2. Our INTEX Objectives In Measuring Title Compounds • Tropospheric Ozone • Radical Oxidants: HO, HO2, CH3OO, CH3C(O)OO ? • Carbon Processing: • HC’s -> CH2O -> CO ; CH2O lifetime and carbon flux through CH2O • CH3OOH or CH2O ; methane world vs nonmethane world • CH3C(O)OOH (HO2 vs NO2) ; • Extension of Trop-Chem Measurements by Satellite: • CH2O directly • Combined with other compounds and campaigns • Vertical Transport & Mixing • Tracers, Yes • Working on being quantitative • Instrument Development & Comparison • H2O2 : URI, CIT & BAE146 • CH2O: URI, NCAR & WP3

  3. Instrument Changes and Comparison • CH2O – pre-mission, during, & prototype • Simplified FIA system; improved noise • Modified signal processing; noise vs response time • Stability allows for continuous measurements • Last Five Flights (16-20; 8/6,7,11,13 &14) • 1 minute resolution with continuous sampling • 25 pptv level of detection • CH2O Relationships with Other Compounds

  4. ~1.5 ~1.1 Direct comparison, URI & NCAR, 10-s Merge Product red – ascent/descentgreen – levelblue – Xw > 1%

  5. Formaldehyde Relationships with Parents & Daughter Carbon Monoxide, Ethane, Propane, & Benzene

  6. Formaldehyde Relationships Continued Ethyne, Ethene, Isoprene, & Propene

  7. Formaldehyde … Acetaldehyde, Acetone, Methanol, Methylhydroperoxide

  8. Formaldehyde … Perhydroxyl, Ozone, Water, & Hydroxyl

  9. Formaldehyde vs Pressure, RH, Nitrogen Dioxide, Sulfur Dioxide

  10. Instrument Changes & Comparison • H2O2 / CH3OOH / CH3C(O)OOH • Initial setup for H2O2 / CH3OOH alone • StL Samples Indicated 3rd ROOH; PAA on CIT • New HPLC Column online in Portsmouth • Tests for hydroxymethylhydroperoxide – negative • Tests for peroxyacetic acid – positive • Modify mode and run times to resolve PAA, PAA is a work in progress (~3 months more) • Hence, less frequent sampling from NH on.

  11. ~1.2 ~0.65 URI-CIT Direct Comparison – OUTLIERS – Robust Fit Algorithm (MatLab) red – ascent/descentgreen – levelblue – Xv < 1%

  12. Hydrogen Peroxide Relationships Perhydroxyl, Ozone, Water, & Hydroxyl

  13. Hydrogen Peroxide … Pressure, RH, Nitrogen Dioxide, Sulfur Dioxide

  14. Hydrogen Peroxide … Acetaldehyde, Acetone, Methanol, Methylhydroperoxide

  15. Case Study: August 11, 2004; DC-8 Flight 18 2 1 3 4 5 10 6 9 8 7

  16. New Brunswick Far Off N. Carolina St Louis Far Off N. Carolina

  17. New Brunswick Far Off N. Carolina St Louis Far Off N. Carolina

  18. New Brunswick Far Off N. Carolina St Louis Far Off N. Carolina grn – H2O2 blk – CH3OOH red – CH2O(URI)mag – CH2O(NCAR)

  19. New Brunswick Far Off N. Carolina St Louis Far Off N. Carolina grn – H2O2 blk – CH3OOH red – CH2O(URI)mag – CH2O(NCAR)

  20. Summary CH2O Measurements URI to NCAR comparison factor of 1.1 to 1.6 Highly correlated Indicate same functional relationships to other compounds H2O2 Measurements URI to CIT comparison factor of 0.7 to 1.2 Well correlated with outliers, better when Xv<1% Indicate same functional relationships to other compounds

  21. Case Study: August 2, 2004; DC-8 Flight 15 7 8 6 5 4 9 3 10 2 11 14 1 12 13

  22. S. Quebec N. New Foundland S. Maine S. New Foundland

  23. S. Quebec N. New Foundland S. Maine S. New Foundland

  24. S. Quebec N. New Foundland S. Maine S. New Foundland grn – H2O2 blk – CH3OOH red – CH2O(URI)mag – CH2O(NCAR)

  25. S. Quebec N. New Foundland S. Maine S. New Foundland grn – H2O2 blk – CH3OOH red – CH2O(URI)mag – CH2O(NCAR)

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