Secondary organic aerosol formation from in-use motor vehicle emissions using a potential aerosol mass reactor. 2014

Daniel S Tkacik, and Andrew T Lambe, and Shantanu Jathar, and Xiang Li, and Albert A Presto, and Yunliang Zhao, and Donald Blake, and Simone Meinardi, and John T Jayne, and Philip L Croteau, and Allen L Robinson
Department of Civil and Environmental Engineering, Carnegie Mellon University , Pittsburgh, Pennsylvania 15213, United States.

Secondary organic aerosol (SOA) formation from in-use vehicle emissions was investigated using a potential aerosol mass (PAM) flow reactor deployed in a highway tunnel in Pittsburgh, Pennsylvania. Experiments consisted of passing exhaust-dominated tunnel air through a PAM reactor over integrated hydroxyl radical (OH) exposures ranging from ∼ 0.3 to 9.3 days of equivalent atmospheric oxidation. Experiments were performed during heavy traffic periods when the fleet was at least 80% light-duty gasoline vehicles on a fuel-consumption basis. The peak SOA production occurred after 2-3 days of equivalent atmospheric oxidation. Additional OH exposure decreased the SOA production presumably due to a shift from functionalization to fragmentation dominated reaction mechanisms. Photo-oxidation also produced substantial ammonium nitrate, often exceeding the mass of SOA. Analysis with an SOA model highlight that unspeciated organics (i.e., unresolved complex mixture) are a very important class of precursors and that multigenerational processing of both gases and particles is important at longer time scales. The chemical evolution of the organic aerosol inside the PAM reactor appears to be similar to that observed in the atmosphere. The mass spectrum of the unoxidized primary organic aerosol closely resembles ambient hydrocarbon-like organic aerosol (HOA). After aging the exhaust equivalent to a few hours of atmospheric oxidation, the organic aerosol most closely resembles semivolatile oxygenated organic aerosol (SV-OOA) and then low-volatility organic aerosol (LV-OOA) at higher OH exposures. Scaling the data suggests that mobile sources contribute ∼ 2.9 ± 1.6 Tg SOA yr(-1) in the United States, which is a factor of 6 greater than all mobile source particulate matter emissions reported by the National Emissions Inventory. This highlights the important contribution of SOA formation from vehicle exhaust to ambient particulate matter concentrations in urban areas.

UI MeSH Term Description Entries
D009566 Nitrates Inorganic or organic salts and esters of nitric acid. These compounds contain the NO3- radical. Nitrate
D009930 Organic Chemicals A broad class of substances containing carbon and its derivatives. Many of these chemicals will frequently contain hydrogen with or without oxygen, nitrogen, sulfur, phosphorus, and other elements. They exist in either carbon chain or carbon ring form. Organic Chemical,Chemical, Organic,Chemicals, Organic
D010084 Oxidation-Reduction A chemical reaction in which an electron is transferred from one molecule to another. The electron-donating molecule is the reducing agent or reductant; the electron-accepting molecule is the oxidizing agent or oxidant. Reducing and oxidizing agents function as conjugate reductant-oxidant pairs or redox pairs (Lehninger, Principles of Biochemistry, 1982, p471). Redox,Oxidation Reduction
D010414 Pennsylvania State bounded on the north by New York and Lake Erie, on the east by Delaware and New Jersey, on the south by Delaware and Maryland, and on the west by Ohio and West Virginia.
D002947 Cities A large or important municipality of a country, usually a major metropolitan center. Municipalities,Towns
D005742 Gasoline Volative flammable fuel (liquid hydrocarbons) derived from crude petroleum by processes such as distillation reforming, polymerization, etc. Diesel Fuel,Diesel Fuels,Fuel, Diesel,Fuels, Diesel,Gasolines
D000336 Aerosols Colloids with a gaseous dispersing phase and either liquid (fog) or solid (smoke) dispersed phase; used in fumigation or in inhalation therapy; may contain propellant agents. Aerosol
D000393 Air Pollutants Any substance in the air which could, if present in high enough concentration, harm humans, animals, vegetation or materials. Substances include GASES; PARTICULATE MATTER; and volatile ORGANIC CHEMICALS. Air Pollutant,Air Pollutants, Environmental,Environmental Air Pollutants,Environmental Pollutants, Air,Air Environmental Pollutants,Pollutant, Air,Pollutants, Air,Pollutants, Air Environmental,Pollutants, Environmental Air
D001272 Atmosphere The gaseous envelope surrounding a planet or similar body. (From Random House Unabridged Dictionary, 2d ed) Atmospheres
D001335 Vehicle Emissions Gases, fumes, vapors, and ODORANTS escaping from the cylinders of a gasoline or diesel internal-combustion engine. (From McGraw-Hill Dictionary of Scientific and Technical Terms, 4th ed & Random House Unabridged Dictionary, 2d ed) Automobile Exhaust,Diesel Exhaust,Engine Exhaust,Vehicle Emission,Vehicular Emission,Traffic-Related Pollutants,Transportation Emissions,Vehicular Emissions,Emission, Vehicle,Emission, Vehicular,Emissions, Transportation,Emissions, Vehicle,Emissions, Vehicular,Exhaust, Automobile,Exhaust, Diesel,Exhaust, Engine,Pollutants, Traffic-Related,Traffic Related Pollutants

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