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Traffic Related Emissions of Radical Precursors HCHO and HONO in Los Angeles During CalNex S. Alvarez 1, B. Rappenglück 1, P.R. Veres 2,3, J.M. Roberts.

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Presentation on theme: "Traffic Related Emissions of Radical Precursors HCHO and HONO in Los Angeles During CalNex S. Alvarez 1, B. Rappenglück 1, P.R. Veres 2,3, J.M. Roberts."— Presentation transcript:

1 Traffic Related Emissions of Radical Precursors HCHO and HONO in Los Angeles During CalNex S. Alvarez 1, B. Rappenglück 1, P.R. Veres 2,3, J.M. Roberts 2, A.K. Cochran 4, C. Afif 5,6, V. Michoud 5, J.F. Doussin 5, A. Borbon 5, H. Osthoff 7 (1) Department of Earth and Atmospheric Sciences, University of Houston, TX/USA (2) NOAA Earth System Research Laboratory, Boulder, CO/USA (3) Max-Planck Institut für Chemie, Mainz, Germany (4) North Carolina Agricultural and Technical State University, Greensboro, NC/USA (5) LISA, UMR-CNRS 7583, Université Paris Est Créteil, Université Paris Diderot, Créteil, France (6) Department of Chemistry, Faculty of Science, Saint Joseph University, Beirut, Lebanon (7) University of Calgary, Canada

2 early morning midmorning afternoon nm –Sources of OH

3 –Secondary formation through photochemical breakdown of anthropogenic and biogenic VOCs. –Primary emission through incomplete combustion. Potential sources: mobile sources (traffic exhaust) point sources (in petrochemical production). Formation of Formaldehyde (HCHO) –Gas phase NO + OH → HONO –Heterogeneous formation 2NO 2 + H 2 O → HONO + HNO 3 Photo-enhanced heterogeneous reactions –Primary emission through combustion processes Formation of Nitrous Acid (HONO)

4 Traffic Related Emissions of HONO and HCHO –So far only scarce traffic emissions data is available which includes both compounds. `

5 Traffic Related Emissions of HONO and HCHO –So far only scarce traffic emissions data is available which includes both compounds. –In particular for HONO traffic related data was obtained more than a decade ago. - mostly in Europe - tunnel measurements (heavy duty vehicles?) `

6 Traffic Related Emissions of HONO and HCHO –So far only scarce traffic emissions data is available which includes both compounds. –In particular for HONO traffic related data was obtained more than a decade ago. - mostly in Europe - tunnel measurements (heavy duty vehicles?) –However, this knowledge is needed to further refine and validate air quality modeling. `

7 Traffic Related Emissions of HONO and HCHO –So far only scarce traffic emissions data is available which includes both compounds. –In particular for HONO traffic related data was obtained more than a decade ago. - mostly in Europe - tunnel measurements (heavy duty vehicles?) –However, this knowledge is needed to further refine and validate air quality modeling. –Primary goal: HCHO/CO, HONO/CO (CO: traffic marker) `

8 Measurements CalNex Pasadena Site

9 Measurements CalNex Pasadena Site

10 Measurements CalNex Pasadena Site ParameterMethod COVacuum ultraviolet (VUV) Fluorescence; AL5001 PANCIMS, (GC) HCHOHantzsch/ Fluorescence; AL4021 HONOSA:NED derivization/ HPLC; NitroMAC

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14 Day (6 am – 8 pm)Night (8 pm – 6 am) CO Night Day

15 Night Day (6 am – 8 pm)Night (8 pm – 6 am) PAN Day

16 Night Day (6 am – 8 pm)Night (8 pm – 6 am) HCHO Day

17 Night Day (6 am – 8 pm)Night (8 pm – 6 am) HONO Day

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19 Morning rush hour Evening rush hour

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21 Morning Morning rush hour

22 Morning Noon Morning rush hour Noon

23 Morning Noon Morning rush hour Evening rush hour Evening Noon

24 Morning Noon Evening

25 Morning Noon Evening

26 Morning Noon Evening Morning rush hour Evening rush hour

27 Morning Evening 4:30-6:00 am 8:00-10:00 pm Time frames taken for correlation analysis

28 4:30-6:00 am (PAN < 300 ppt) HCHO vs CO (weekdays)

29 4:30-6:00 am (PAN < 300 ppt) HCHO vs CO (weekdays) 4:30-6:00 am and 8:00-10:00 pm (PAN < 300 ppt)

30 4:30-6:00 am (PAN < 300 ppt) HCHO vs CO (weekdays) 4:30-6:00 am and 8:00-10:00 pm (PAN < 300 ppt) (i) weekdays (ii) rush hour time 5:00-9:00 am (iii) global radiation < 10 Wm -2 (iv) PAN < 50 ppt (v) no precipitation (vi) RH > 80% Comparison: Houston/TX Highway Junction 07/15-10/15/09 y = 2.66(±0.13) – 140.0(±45.3) R 2 =0.75 y = 2.98(±0.13) + 484.5(±46.1) R 2 =0.69 CalNex-Pasadena “higher”

31 4:30-6:00 am (PAN < 300 ppt) HONO vs CO (weekdays)

32 4:30-6:00 am (PAN < 300 ppt) HONO vs CO (weekdays) 4:30-6:00 am and 8:00-10:00 pm (PAN < 300 ppt)

33 4:30-6:00 am (PAN < 300 ppt) (i) weekdays (ii) rush hour time 5:00-9:00 am (iii) global radiation < 10 Wm -2 (iv) PAN < 50 ppt (v) no precipitation (vi) RH > 80% Comparison: Houston/TX Highway Junction 07/15-10/15/09 y = 2.66(±0.13) – 140.0(±45.3) R 2 =0.75 HONO vs CO (weekdays) 4:30-6:00 am and 8:00-10:00 pm (PAN < 300 ppt) CalNex-Pasadena “higher”

34 –HCHO and HONO traffic related emissions during CalNex; preliminary results: Increase of HCHO and HONO during rush hour(s) HCHO <> CO ratio: slope around 3.5 - 4.9 pptv HCHO/ 1 ppbv CO HONO <> CO ratio: slope around 3.3 - 4.2 pptv HONO/ 1 ppbv CO Higher than in roadside study in Houston But: in Houston: PAN < 50 ppt; in CalNex-Pasadena: PAN < 300 ppt) - CalNex-Pasadena: more aged air masses? - Traffic composition? - Traffic flow?

35 –HCHO and HONO traffic related emissions during CalNex; preliminary results: Increase of HCHO and HONO during rush hour(s) HCHO <> CO ratio: slope around 3.5 - 4.9 pptv HCHO/ 1 ppbv CO HONO <> CO ratio: slope around 3.3 - 4.2 pptv HONO/ 1 ppbv CO Higher than in roadside study in Houston But: in Houston: PAN < 50 ppt; in CalNex-Pasadena: PAN < 300 ppt) - CalNex-Pasadena: more aged air masses? - Traffic composition? - Traffic flow? –What next? HONO: final QA, inclusion of additional HONO data (NOAA) PAN: filling gaps in PAN data (GC?) Merging with VOC and NO x data Source apportionment Comparison with MOBILE6 / MOVES2010 traffic emissions modeling

36 –HCHO and HONO traffic related emissions during CalNex; preliminary results: Increase of HCHO and HONO during rush hour(s) HCHO <> CO ratio: slope around 3.5 - 4.9 pptv HCHO/ 1 ppbv CO HONO <> CO ratio: slope around 3.3 - 4.2 pptv HONO/ 1 ppbv CO Higher than in roadside study in Houston But: in Houston: PAN < 50 ppt; in CalNex-Pasadena: PAN < 300 ppt) - CalNex-Pasadena: more aged air masses? - Traffic composition? - Traffic flow? –What next? HONO: final QA, inclusion of additional HONO data (NOAA) PAN: filling gaps in PAN data (GC?) Merging with VOC and NO x data Source apportionment Comparison with MOBILE6 / MOVES2010 traffic emissions modeling Acknowledgements: -NOAA: Roberts et al., Borbon et al., Osthoff -JJJ: Alvarez, Rappenglück

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