Browsing by Author "Gaffney, J. S."
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- Sources and transformations of particle-bound polycyclic aromatic hydrocarbons in Mexico CityMarr, Linsey C.; Dzepina, K.; Jimenez, Jose L.; Reisen, F.; Bethel, H. L.; Arey, J.; Gaffney, J. S.; Marley, N. A.; Molina, L. T.; Molina, M. J. (Copernicus Publications, 2006-05-01)Understanding sources, concentrations, and transformations of polycyclic aromatic hydrocarbons (PAHs) in the atmosphere is important because of their potent mutagenicity and carcinogenicity. The measurement of particle-bound PAHs by three different methods during the Mexico City Metropolitan Area field campaign in April 2003 presents a unique opportunity for characterization of these compounds and intercomparison of the methods. The three methods are ( 1) collection and analysis of bulk samples for time-integrated gas- and particle-phase speciation by gas chromatography/ mass spectrometry; ( 2) aerosol photoionization for fast detection of PAHs on particles' surfaces; and ( 3) aerosol mass spectrometry for fast analysis of size and chemical composition. This research represents the first time aerosol mass spectrometry has been used to measure ambient PAH concentrations and the first time that fast, real-time methods have been used to quantify PAHs alongside traditional filter-based measurements in an extended field campaign. Speciated PAH measurements suggest that motor vehicles and garbage and wood burning are important sources in Mexico City. The diurnal concentration patterns captured by aerosol photoionization and aerosol mass spectrometry are generally consistent. Ambient concentrations of particle-phase PAHs typically peak at similar to 110 ng m(-3) during the morning rush hour and rapidly decay due to changes in source activity patterns and dilution as the boundary layer rises, although surface-bound PAH concentrations decay faster. The more rapid decrease in surface versus bulk PAH concentrations during the late morning suggests that freshly emitted combustion-related particles are quickly coated by secondary aerosol material in Mexico City's atmosphere and may also be transformed by heterogeneous reactions.
- Spatial and temporal variability of particulate polycyclic aromatic hydrocarbons in Mexico CityThornhill, D. A.; de Foy, B.; Herndon, S. C.; Onasch, T. B.; Wood, E. C.; Zavala, M.; Molina, L. T.; Gaffney, J. S.; Marley, N. A.; Marr, Linsey C. (Copernicus Publications, 2008)As part of the Megacities Initiative: Local and Global Research Observations (MILAGRO) study in the Mexico City Metropolitan Area in March 2006, we measured particulate polycyclic aromatic hydrocarbons (PAHs) and other gaseous species and particulate properties, including light absorbing carbon or effective black carbon (BC), at six locations throughout the city. The measurements were intended to support the following objectives: to describe spatial and temporal patterns in PAH concentrations, to gain insight into sources and transformations of PAHs and BC, and to quantify the relationships between PAHs and other pollutants. Total particulate PAHs at the Instituto Mexicano del Petroleo (T0 supersite) located near downtown averaged 50 ng m(-3), and aerosol active surface area averaged 80 mm(2) m(-3). PAHs were also measured on board the Aerodyne Mobile Laboratory, which visited six sites encompassing a mixture of different land uses and a range of ages of air parcels transported from the city core. A combination of analyses of time series, back trajectories, concentration fields, pollutant ratios, and correlation coefficients supports the concept of T0 as an urban source site, T1 as a receptor site with strong local sources, Pedregal and PEMEX as intermediate sites, Pico Tres Padres as a vertical receptor site, and Santa Ana as a downwind receptor site. Weak intersite correlations suggest that local sources are important and variable and that exposure to PAHs and BC cannot be represented by a single regional-scale value. The relationships between PAHs and other pollutants suggest that a variety of sources and ages of particles are present. Among carbon monoxide, nitrogen oxides (NO(x)), and carbon dioxide, particulate PAHs are most strongly correlated with NO(x). Mexico City's PAH/BC mass ratio of 0.01 is similar to that found on a freeway loop in the Los Angeles area and approximately 8-30 times higher than that found in other cities. Evidence also suggests that primary combustion particles are rapidly coated by secondary aerosol in Mexico City. If so, their optical properties may change, and the lifetime of PAHs may be prolonged if the coating protects them against photodegradation or heterogeneous reactions.