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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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

early morning midmorning afternoon nm –Sources of OH

–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)

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

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?) `

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. `

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) `

Measurements CalNex Pasadena Site

Measurements CalNex Pasadena Site

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

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

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

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

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

Morning rush hour Evening rush hour

Morning Morning rush hour

Morning Noon Morning rush hour Noon

Morning Noon Morning rush hour Evening rush hour Evening Noon

Morning Noon Evening

Morning Noon Evening

Morning Noon Evening Morning rush hour Evening rush hour

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

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

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)

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) (±46.1) R 2 =0.69 CalNex-Pasadena “higher”

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

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)

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”

–HCHO and HONO traffic related emissions during CalNex; preliminary results: Increase of HCHO and HONO during rush hour(s) HCHO <> CO ratio: slope around pptv HCHO/ 1 ppbv CO HONO <> CO ratio: slope around 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?

–HCHO and HONO traffic related emissions during CalNex; preliminary results: Increase of HCHO and HONO during rush hour(s) HCHO <> CO ratio: slope around pptv HCHO/ 1 ppbv CO HONO <> CO ratio: slope around 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

–HCHO and HONO traffic related emissions during CalNex; preliminary results: Increase of HCHO and HONO during rush hour(s) HCHO <> CO ratio: slope around pptv HCHO/ 1 ppbv CO HONO <> CO ratio: slope around 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

weekend