Oxidation of ketone groups in transported biomass burning aerosol from the 2008 Northern California Lightning Series fires |
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| Authors: | Lelia N Hawkins Lynn M Russell |
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| Institution: | 1. Department of Civil and Environmental Engineering, Michigan Technological University, 1400 Townsend Drive, Houghton, MI 49931, USA;2. Atmospheric Sciences Program, Michigan Technological University, 1400 Townsend Drive, Houghton, MI 49931, USA;3. School of Forest Resources and Environmental Science, Michigan Technological University, 1400 Townsend Drive, Houghton, MI 49931, USA;1. School of Environmental and Chemical Engineering, Shanghai University, Shanghai 200444, China;2. Guangzhou Hexin Analytical Instrument Company Limited, Guangzhou 510530, China;3. State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Science, Beijing 100012, China;4. Atmospheric Environment Institute of Safety and Pollution Control, Jinan University, Guangdong 510632, China;1. University of Eastern Finland, Department of Environmental Science, P.O. Box 1627, FI-70211 Kuopio, Finland;2. National Institute for Health and Welfare, Department of Environmental Health, P.O. Box 95, FI-70701 Kuopio, Finland;3. VTT Technical Research Centre of Finland, P.O. Box 1000, FI-02044 VTT, Espoo, Finland;1. Laboratoire de Météorologie Physique, CNRS, Université Blaise Pascal, UMR6016, Aubière cedex, France;2. NASA Langley Research Center, Hampton, VA 23666, USA;3. Institute for Physics of the Atmosphere, Johannes Gutenberg University, Mainz, Germany;4. Centre National de Recherches Météorologiques, URA 1357, Météo-France, Toulouse, France;5. Norwegian Institute for Air Research, Kjeller, Norway;6. Laboratoire des Science du Climat et de l''Environnement, CNRS, France;7. Departement of Atmospheric and Oceanic Sciences, McGill University, Montreal, Canada;8. Laboratoire de Glaciologie et Géophysique de l''Environnement, UMR 5183, Université de Grenoble 1/CNRS, Grenoble, France;1. Department of Environmental Science, Babasaheb Bhimrao Ambedkar University, Lucknow, 226025, Uttar Pradesh, India;2. Environmental Monitoring Division, Indian Institute of Toxicology Research, Mahatma Gandhi Marg, Lucknow, 226 001, Uttar Pradesh, India |
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| Abstract: | Submicron particles were collected from June to September 2008 in La Jolla, California to investigate the composition and sources of atmospheric aerosol in an anthropogenically-influenced coastal site. Factor analysis of aerosol mass spectrometry (AMS) and Fourier transform infrared (FTIR) spectroscopy measurements revealed that the two largest sources of submicron organic mass (OM) at the sampling site were (1) fossil fuel combustion associated with ship and diesel truck emissions near the ports of Los Angeles and Long Beach and (2) aged smoke from large wildfires burning in central and northern California. During non-fire periods, fossil fuel combustion contributed up to 95% of FTIR OM, correlated to sulfur, and consisted mostly of alkane (86%) and carboxylic acid groups (9%). During fire periods, biomass burning contributed up to 74% of FTIR OM, consisted mostly of alkane (48%), ketone (25%), and carboxylic acid groups (17%), and correlated to AMS-derived factors resembling brush fire smoke, wood smoldering and flaming particles, and biogenic secondary organic aerosol. The two AMS-derived biomass burning factors were identified as oxygenated and hydrocarbon biomass burning aerosol on the basis of spectral similarities to smoldering and flaming smoke particles, respectively. In addition, the ratio of oxygenated to hydrocarbon biomass burning OM shows a clear diurnal trend with an afternoon peak, consistent with photochemical oxidation. Back trajectory analysis indicates that 2–4-day old forest fire emissions include substantial ketone groups, which have both lower O/C and lower m/z 44/OM fraction than carboxylic acid groups. Air masses with more than 4-day old emissions have higher carboxylic acid/ketone group ratios, showing that atmospheric processing of these ketone-containing organic aerosol particles results in increased m/z 44 and O/C. These observations may provide functionally-specific evidence for the type of chemical processing that is responsible for biomass burning particle composition in the atmosphere. |
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