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Ecol Evol ; 6(24): 8785-8799, 2016 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-28035269


Risks associated with exposure of individual plant species to ozone (O3) are well documented, but implications for terrestrial biodiversity and ecosystem processes have received insufficient attention. This is an important gap because feedbacks to the atmosphere may change as future O3 levels increase or decrease, depending on air quality and climate policies. Global simulation of O3 using the Community Earth System Model (CESM) revealed that in 2000, about 40% of the Global 200 terrestrial ecoregions (ER) were exposed to O3 above thresholds for ecological risks, with highest exposures in North America and Southern Europe, where there is field evidence of adverse effects of O3, and in central Asia. Experimental studies show that O3 can adversely affect the growth and flowering of plants and alter species composition and richness, although some communities can be resilient. Additional effects include changes in water flux regulation, pollination efficiency, and plant pathogen development. Recent research is unraveling a range of effects belowground, including changes in soil invertebrates, plant litter quantity and quality, decomposition, and nutrient cycling and carbon pools. Changes are likely slow and may take decades to become detectable. CESM simulations for 2050 show that O3 exposure under emission scenario RCP8.5 increases in all major biomes and that policies represented in scenario RCP4.5 do not lead to a general reduction in O3 risks; rather, 50% of ERs still show an increase in exposure. Although a conceptual model is lacking to extrapolate documented effects to ERs with limited or no local information, and there is uncertainty about interactions with nitrogen input and climate change, the analysis suggests that in many ERs, O3 risks will persist for biodiversity at different trophic levels, and for a range of ecosystem processes and feedbacks, which deserves more attention when assessing ecological implications of future atmospheric pollution and climate change.

Atmos Chem Phys ; 16(5): 3499-3523, 2016.
Artigo em Inglês | MEDLINE | ID: mdl-28649266


The negative impacts of fine particulate matter (PM2.5) exposure on human health are a primary motivator for air quality research. However, estimates of the air pollution health burden vary considerably and strongly depend on the datasets and methodology. Satellite observations of aerosol optical depth (AOD) have been widely used to overcome limited coverage from surface monitoring and to assess the global population exposure to PM2.5 and the associated premature mortality. Here we quantify the uncertainty in determining the burden of disease using this approach, discuss different methods and datasets, and explain sources of discrepancies among values in the literature. For this purpose we primarily use the MODIS satellite observations in concert with the GEOS-Chem chemical transport model. We contrast results in the United States and China for the years 2004-2011. Using the Burnett et al. (2014) integrated exposure response function, we estimate that in the United States, exposure to PM2.5 accounts for approximately 2% of total deaths compared to 14% in China (using satellite-based exposure), which falls within the range of previous estimates. The difference in estimated mortality burden based solely on a global model vs. that derived from satellite is approximately 14% for the U.S. and 2% for China on a nationwide basis, although regionally the differences can be much greater. This difference is overshadowed by the uncertainty in the methodology for deriving PM2.5 burden from satellite observations, which we quantify to be on the order of 20% due to uncertainties in the AOD-to-surface-PM2.5 relationship, 10% due to the satellite observational uncertainty, and 30% or greater uncertainty associated with the application of concentration response functions to estimated exposure.

Chem Rev ; 115(10): 4476-96, 2015 May 27.
Artigo em Inglês | MEDLINE | ID: mdl-25839909
Environ Sci Technol ; 49(7): 4129-37, 2015 Apr 07.
Artigo em Inglês | MEDLINE | ID: mdl-25734883


The high atmospheric concentrations of toxic gases, particulate matter, and acids in the areas immediately surrounding volcanoes can have negative impacts on human and ecological health. To better understand the atmospheric fate of volcanogenic emissions in the near field (in the first few hours after emission), we have carried out real-time measurements of key chemical components of the volcanic plume from Ki̅lauea on the Island of Hawai'i. Measurements were made at two locations, one ∼ 3 km north-northeast of the vent and the other 31 km to the southwest, with sampling at each site spanning a range of meteorological conditions and volcanic influence. Instrumentation included a sulfur dioxide monitor and an Aerosol Chemical Speciation Monitor, allowing for a measurement of the partitioning between the two major sulfur species (gas-phase SO2 and particulate sulfate) every 5 min. During trade wind conditions, which sent the plume toward the southwest site, sulfur partitioning exhibited a clear diurnal pattern, indicating photochemical oxidation of SO2 to sulfate; this enabled the quantitative determination of plume age (5 h) and instantaneous SO2 oxidation rate (2.4 × 10(-6) s(-1) at solar noon). Under stagnant conditions near the crater, the extent of SO2 oxidation was substantially higher, suggesting faster oxidation. The particles within the plume were extremely acidic, with pH values (controlled largely by ambient relative humidity) as low as -0.8 and strong acidity (controlled largely by absolute sulfate levels) up to 2200 nmol/m(3). The high variability of sulfur partitioning and particle composition underscores the chemically dynamic nature of volcanic plumes, which may have important implications for human and ecological health.

Dióxido de Enxofre/análise , Enxofre/análise , Erupções Vulcânicas/análise , Aerossóis/análise , Gases , Hawaii , Humanos , Concentração de Íons de Hidrogênio , Espectrometria de Massas , Oxirredução , Material Particulado/análise , Sulfatos/análise , Enxofre/química , Dióxido de Enxofre/química , Vento
Proc Natl Acad Sci U S A ; 106(22): 8835-40, 2009 Jun 02.
Artigo em Inglês | MEDLINE | ID: mdl-19451635


Remote sensing data over North America document the ubiquity of secondary aerosols resulting from a combination of primary biogenic and anthropogenic emissions. The spatial and temporal distribution of aerosol optical thickness (AOT) over the southeastern United States cannot be explained by anthropogenic aerosols alone, but is consistent with the spatial distribution, seasonal distribution, and temperature dependence of natural biogenic volatile organic compound (BVOC) emissions. These patterns, together with observations of organic aerosol in this region being dominated by modern (14)C and BVOC oxidation products with summer maxima, indicate nonfossil fuel origins and strongly suggest that the dominant summer AOT signal is caused by secondary aerosol formed from BVOC oxidation. A link between anthropogenic and biogenic emissions forming secondary aerosols that dominate the regional AOT is supported by reports of chemicals in aerosols formed by BVOC oxidation in a NO(x)- and sulfate-rich environment. Even though ground-based measurements from the IMPROVE network suggest higher sulfate than organic concentrations near the surface in this region, we infer that much of the secondary organic aerosol in the Southeast must occur above the surface layer, consistent with reported observations of the organic fraction of the total aerosol increasing with height and models of the expected vertical distribution of secondary organic aerosols from isoprene oxidation. The observed AOT is large enough in summer to provide regional cooling; thus we conclude that this secondary aerosol source is climatically relevant with significant potential for a regional negative climate feedback as BVOC emissions increase with temperature.

Aerossóis/química , Poluentes Atmosféricos/química , Carbono/química , Processos Climáticos , Temperatura Baixa , Compostos Orgânicos Voláteis/química , Monitoramento Ambiental , Estados Unidos