Insights into the primary–secondary and regional–local contributions to organic aerosol and PM2.5 mass in Pittsburgh,Pennsylvania |
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| Institution: | 1. Department of Environment and Energy Engineering, Chonnam National University, 77 Yongbong-ro, Gwangju 61186, Republic of Korea;2. Center for Gas Analysis, Korea Research Institute of Standards and Science (KRISS), 267 Gajeong-ro, Yuseong-gu, Daejeon 34113, Republic of Korea;1. Key Laboratory of Geographic Information Science of the Ministry of Education, School of Geographic Sciences, East China Normal University, Shanghai 200241, China;2. Department of Chemistry, Analytical and Testing Center, Capital Normal University, Beijing 100048, China;3. College of Resource Environment and Tourism, Capital Normal University, Beijing 100048, China;4. Beijing Municipal Research Institute of Environmental Protection, Beijing 100037, China;5. State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China;6. Center for Excellence in Regional Atmospheric Environment, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, China;1. Center for Ecological Research & Key Laboratory of Sustainable Forest Ecosystem Management-Ministry of Education, College of Forestry, Northeast Forestry University, Harbin, 150040, China;2. State Environmental Protection Key Laboratory of Urban Ambient Air Particulate Matter Pollution Prevention and Control, College of Environmental Science and Engineering, Nankai University, Tianjin, 300350, China |
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| Abstract: | This paper presents chemical mass balance (CMB) analysis of organic molecular marker data to investigate the sources of organic aerosol and PM2.5 mass in Pittsburgh, Pennsylvania. The model accounts for emissions from eight primary source classes, including major anthropogenic sources such as motor vehicles, cooking, and biomass combustion as well as some primary biogenic emissions (leaf abrasion products). We consider uncertainty associated with selection of source profiles, selection of fitting species, sampling artifacts, photochemical aging, and unknown sources. In the context of the overall organic carbon (OC) mass balance, the contributions of diesel, wood-smoke, vegetative detritus, road dust, and coke-oven emissions are all small and well constrained; however, estimates for the contributions of gasoline-vehicle and cooking emissions can vary by an order of magnitude. A best-estimate solution is presented that represents the vast majority of our CMB results; it indicates that primary OC only contributes 27±8% and 50±14% (average±standard deviation of daily estimates) of the ambient OC in the summer and winter, respectively. Approximately two-thirds of the primary OC is transported into Pittsburgh as part of the regional air mass. The ambient OC that is not apportioned by the CMB model is well correlated with secondary organic aerosol (SOA) estimates based on the EC-tracer method and ambient concentrations of organic species associated with SOA. Therefore, SOA appears to be the major component of OC, not only in summer, but potentially in all seasons. Primary OC dominates the OC mass balance on a small number of nonsummer days with high OC concentrations; these events are associated with specific meteorological conditions such as local inversions. Primary particulate emissions only contribute a small fraction of the ambient fine-particle mass, especially in the summer. |
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