The impact of temperature on formation of O3 and odd nitrogen photochemistry is investigated using urban‐, regional‐ and global‐scale simulations. Urban and polluted rural environments are explored with a regional simulation derived from a specific episode in the midwestern United States. The simulations predict that O3 increases with temperature in both urban and polluted rural environments. The O3‐temperature relation is driven largely by chemistry of peroxyacetylnitrate (PAN) which represents an increased sink for both NOx and odd hydrogen at low temperatures. Isoprene emissions, H2O, and solar radiation also contribute to the O3‐temperature relation. Possible correlations between temperature and anthropogenic emissions or stagnant meteorology were not included. Observations at urban and rural sites in the United States suggests that O3 increases with temperature at a faster rate than the models predict. Calculations with a one‐dimensional global model suggest that increased temperature in the polluted boundary layer does not lead to increased O3 in the free troposphere, because increased export of O3 is balanced by decreased export of odd nitrogen species.
Ambient levels of particulate matter have been linked to cardiovascular disease. The mechanisms mediating these associations are poorly understood. One candidate mechanism is inflammation. Using data from the Multi-Ethnic Study of Atherosclerosis (2000-2002), the authors investigated the relation between exposure to particulate matter of less than or equal to 2.5 microm in diameter (PM2.5) and C-reactive protein concentration in 5,634 persons aged 45-84 years who were free of cardiovascular disease. Data from US Environmental Protection Agency monitors were used to estimate PM2.5 exposures for the prior day, prior 2 days, prior week, prior 30 days, and prior 60 days. Only the 30-day and 60-day mean exposures showed a weak positive association with C-reactive protein, and confidence intervals were wide: relative increases in C-reactive protein per 10 microg/m3 of PM2.5 adjusted for person-level covariates were 3% (95% confidence interval (CI): -2, 10) for a 30-day mean and 4% (95% CI: -3, 11.0) for a 60-day mean. The means of 7-day, 30-day, and 60-day exposures were weakly, positively, and nonsignificantly associated with the odds of C-reactive protein of greater than or equal to 3 mg/liter: adjusted odds ratios were 1.05 (95% CI: 0.96, 1.15), 1.12 (95% CI: 0.98, 1.29), and 1.12 (95% CI: 0.96, 1.32), respectively. Slightly stronger associations were observed in persons without other risk factors for elevated C-reactive protein, but this heterogeneity was not statistically significant. The authors' results are not compatible with strong effects of particulate matter exposures on population levels of C-reactive protein.
Abnormally high concentrations of O3 have been observed in rural locations on the shore of Lake Michigan and on the Atlantic coast in Maine, at a distance of 300 km or more from major anthropogenic sources. We hypothesize that this O3 is associated with transport from major urban centers and with the suppression of vertical mixing as urban plumes are transported over water. A dynamical/photochemical model is developed that represents formation of O3 in shoreline environments and is used to simulate case studies for Lake Michigan and the northeastern United States. Results suggest that a broad region with elevated O3, NOx and volatile organic carbon (VOC) forms as the Chicago plume travels over Lake Michigan, a pattern consistent with observed O3 at surface monitoring sites. Near‐total suppression of dry deposition of O3 and NOx over the lake is needed to produce high O3. Results for the east coast suggest that the observed peak O3 can only be reproduced by a model that includes suppressed vertical mixing and deposition over water, 2‐day transport of a plume from New York, and superposition of the New York and Boston plumes. An investigation of the sensitivity of O3 to emissions of NOx and VOC suggests that results vary greatly between cities, even when the composition of urban emissions is similar. An index for VOC versus NOx sensitivity is shown to correlate with total reactive nitrogen (NOy) at the time of peak O3.
Cluster analyses of two-dimensional mixed layer back trajectory data were used to determine what fraction of chemical variability in precipitation composition could be related to differences in atmospheric transport. Trajectories arriving at two different sites, Rockport, Indiana, and Gaylord, Michigan, were clustered to identify events occurring with similar transport patterns. It was found that certain transport situations resulted in significantly higher concentrations and depositions of the major ions, H+, SO;, NO; and NHf. At Rockport, the greatest fraction of acid deposition was associated with low wind speeds. At Gaylord, transport direction played a greater role than transport speed in influencing precipitation composition. Results presented here suggest that lo%+% of the variability in ion concentrations may be related to differences in atmospheric transport. The residual variation in concentrations was correlated with differences in the occurrence of upwind precipitation, precipitation type., and variation in precipitation amount.
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