Heather Simon

MMP/TIMP expression in spontaneously hypertensive heart failure rats: the effect of ACE- and MMP-inhibition

OBJECTIVE Determine the effect of a matrix metalloproteinase inhibitor (MMPi) and angiotensin converting enzyme inhibitor (ACEi) on collagen, MMP, tissue inhibitors of MMPs (TIMPs) expression in the spontaneously hypertensive heart failure (SHHF) rat. METHODS Six groups were tested: normotensive 9- and 13-month-old Wistar-Furth (WF) rats, 9-month-old SHHFs (compensatory hypertrophy), 13-month-old SHHFs with HF, and 13-month-old SHHFs orally administered with either an MMPi (PD166793, 5 mgkg(-1)day(-1)) or ACEi (quinapril, 10 mgkg(-1)day(-1)) for 4 months. Collagen volume fraction was assessed histomorphometrically. Left ventricular (LV) mRNA [MMP-1,-2,-3,-7,-9,-11,-13,-14; TIMP-1,-2,-3,-4; and collagen alpha1(I) and alpha1(III)] and protein (MMP-2 and MMP-9 zymographic activity; Western blot analysis of MMP-13, and TIMP-1,-2,-4) levels could be quantified. RESULTS Collagen mRNA levels were elevated in SHHFs compared to age-matched controls, but collagen volume fraction was elevated only in 13-month-old SHHFs (approximately 2x). Only MMP-2 mRNA levels increased significantly with HF. However, MMP-2 and MMP-9 zymographic activity, and MMP-13 protein levels increased. TIMP-1 and TIMP-2 mRNA and protein levels increased, and TIMP-4 protein levels decreased in SHHFs vs. controls. Both drug treatments reduced LV dilation; preserved systolic function; and normalized MMP/TIMP expression. Both drug treatments also reduced collagen volume fraction, but only quinapril reduced collagen mRNA levels and LV hypertrophy. CONCLUSIONS The divergent effect of MMPi and ACEi on collagen mRNA levels and hypertrophy indicate that drug efficacy is mediated by different pathways in the SHHF rat.

Ozone Trends Across the United States over a Period of Decreasing NOx and VOC Emissions

In this work, we evaluate ambient ozone trends at urban, suburban, and rural monitoring sites across the United States over a period of decreasing NOx and VOC emissions (1998-2013). We find that decreasing ozone trends generally occur in the summer, in less urbanized areas, and at the upper end of the ozone distribution. Conversely, increasing ozone trends generally occur in the winter, in more urbanized areas, and at the lower end of the ozone distribution. The 95(th) percentile ozone concentrations decreased at urban, suburban, and rural monitors by 1-2 ppb/yr in the summer and 0.5-1 ppb/yr in the winter. In the summer, there are both increasing and decreasing trends in fifth percentile ozone concentrations of less than 0.5 ppb/yr at urban and suburban monitors, while fifth percentile ozone concentrations at rural monitors decreased by up to 1 ppb/yr. In the winter, fifth percentile ozone concentrations generally increased by 0.1-1 ppb/yr. These results demonstrate the large scale success of U.S. control strategies targeted at decreasing peak ozone concentrations. In addition, they indicate that as anthropogenic NOx emissions have decreased, the ozone distribution has been compressed, leading to less spatial and temporal variability.

The development and uses of EPA’s SPECIATE database

SPECIATE is the U.S. Environmental Protection Agency’s (EPA) repository of volatile organic compounds (VOCs) and particulate matter (PM) speciation profiles of air pollution sources. These source profiles can be used to (1) provide input to chemical mass balance (CMB) receptor models; (2) verify profiles derived from ambient measurements by multivariate receptor models (e.g., factor analysis and positive matrix factorization); (3) interpret ambient measurement data; and (4) create speciated emission inventories for regional haze, climate, and photochemical air quality modeling. This paper describes the SPECIATE v4.2 database, provides specific examples of its use, and makes recommendations for future improvements.

Importance of tropospheric ClNO2 chemistry across the Northern Hemisphere

Laboratory and field experiments have revealed that uptake of dinitrogen pentoxide (N2O5) on aerosols containing chloride produces nitryl chloride (ClNO2) and nitric acid. We incorporate heterogeneous ClNO2 formation into the hemispheric Community Multiscale Air Quality model. This heterogeneous chemistry substantially enhances ClNO2 levels in several areas of the Northern Hemisphere and alters the composition of airborne reactive nitrogen, comprising more than 15% of monthly mean values in some areas. Model results suggest that this heterogeneous chemistry reduces monthly mean total nitrate by up to 25% and enhances monthly mean daily maximum 8 h ozone by up to 7.0 ppbv. The pathway also enhances hydroxyl radical by more than 20% in some locations which in turn increases sulfate and other secondary pollutants. The largest ClNO2 concentrations and impacts occur over China and Western Europe, two areas in which few relevant field measurements have been made.

Simulating the Degree of Oxidation in Atmospheric Organic Particles

Modeled ratios of organic mass to organic carbon (OM/OC) and oxygen to carbon (n(O)/n(C)) in organic particulate matter are presented across the US for the first time and evaluated extensively against ambient measurements. The base model configuration systematically underestimates OM/OC ratios during winter and summer months. Model performance is greatly improved by applying source-specific OM/OC ratios to the primary organic aerosol (POA) emissions and incorporating a new parametrization to simulate oxidative aging of POA in the atmosphere. These model improvements enable simulation of urban-scale gradients in OM/OC with values in urban areas as much as 0.4 lower than in the surrounding regions. Modeled OM/OC and n(O)/n(C) ratios in January range from 1.4 to 2.0 and 0.2 to 0.6, respectively. In July, modeled OM/OC and n(O)/n(C) ratios range from 1.4 to 2.2 and 0.2 to 0.8, respectively. Improved model performance during winter is attributed entirely to our application of source-specific OM/OC ratios to the inventory. During summer, our treatment of oxidative aging also contributes to improved performance. Advancements described in this paper are codified in the latest public release of the Community Multiscale Air Quality model, CMAQv5.0.

Fine Particulate Matter Emissions Inventories: Comparisons of Emissions Estimates with Observations from Recent Field Programs

Abstract Emissions inventories of fine particulate matter (PM2.5) were compared with estimates of emissions based on data emerging from U.S. Environment Protection Agency Particulate Matter Supersites and other field programs. Six source categories for PM2.5 emissions were reviewed: on-road mobile sources, nonroad mobile sources, cooking, biomass combustion, fugitive dust, and stationary sources. Ammonia emissions from all of the source categories were also examined. Regional emissions inventories of PM in the exhaust from on-road and nonroad sources were generally consistent with ambient observations, though uncertainties in some emission factors were twice as large as the emission factors. In contrast, emissions inventories of road dust were up to an order of magnitude larger than ambient observations, and estimated brake wear and tire dust emissions were half as large as ambient observations in urban areas. Although comprehensive nationwide emissions inventories of PM2.5 from cooking sources and biomass burning are not yet available, observational data in urban areas suggest that cooking sources account for approximately 5–20% of total primary emissions (excluding dust), and biomass burning sources are highly dependent on region. Finally, relatively few observational data were available to assess the accuracy of emission estimates for stationary sources. Overall, the uncertainties in primary emissions for PM2.5 are substantial. Similar uncertainties exist for ammonia emissions. Because of these uncertainties, the design of PM2.5 control strategies should be based on inventories that have been refined by a combination of bottom-up and top-down methods.

A Direct Sensitivity Approach to Predict Hourly Ozone Resulting from Compliance with the National Ambient Air Quality Standard

In setting primary ambient air quality standards, the EPAs responsibility under the law is to establish standards that protect public health. As part of the current review of the ozone National Ambient Air Quality Standard (NAAQS), the US EPA evaluated the health exposure and risks associated with ambient ozone pollution using a statistical approach to adjust recent air quality to simulate just meeting the current standard level, without specifying emission control strategies. One drawback of this purely statistical concentration rollback approach is that it does not take into account spatial and temporal heterogeneity of ozone response to emissions changes. The application of the higher-order decoupled direct method (HDDM) in the community multiscale air quality (CMAQ) model is discussed here to provide an example of a methodology that could incorporate this variability into the risk assessment analyses. Because this approach includes a full representation of the chemical production and physical transport of ozone in the atmosphere, it does not require assumed background concentrations, which have been applied to constrain estimates from past statistical techniques. The CMAQ-HDDM adjustment approach is extended to measured ozone concentrations by determining typical sensitivities at each monitor location and hour of the day based on a linear relationship between first-order sensitivities and hourly ozone values. This approach is demonstrated by modeling ozone responses for monitor locations in Detroit and Charlotte to domain-wide reductions in anthropogenic NOx and VOCs emissions. As seen in previous studies, ozone response calculated using HDDM compared well to brute-force emissions changes up to approximately a 50% reduction in emissions. A new stepwise approach is developed here to apply this method to emissions reductions beyond 50% allowing for the simulation of more stringent reductions in ozone concentrations. Compared to previous rollback methods, this application of modeled sensitivities to ambient ozone concentrations provides a more realistic spatial response of ozone concentrations at monitors inside and outside the urban core and at hours of both high and low ozone concentrations.

Predicting the effects of nanoscale cerium additives in diesel fuel on regional-scale air quality.

Diesel vehicles are a major source of air pollutant emissions. Fuel additives containing nanoparticulate cerium (nCe) are currently being used in some diesel vehicles to improve fuel efficiency. These fuel additives also reduce fine particulate matter (PM2.5) emissions and alter the emissions of carbon monoxide (CO), nitrogen oxides (NOx), and hydrocarbon (HC) species, including several hazardous air pollutants (HAPs). To predict their net effect on regional air quality, we review the emissions literature and develop a multipollutant inventory for a hypothetical scenario in which nCe additives are used in all on-road and nonroad diesel vehicles. We apply the Community Multiscale Air Quality (CMAQ) model to a domain covering the eastern U.S. for a summer and a winter period. Model calculations suggest modest decreases of average PM2.5 concentrations and relatively larger decreases in particulate elemental carbon. The nCe additives also have an effect on 8 h maximum ozone in summer. Variable effects on HAPs are predicted. The total U.S. emissions of fine-particulate cerium are estimated to increase 25-fold and result in elevated levels of airborne cerium (up to 22 ng/m3), which might adversely impact human health and the environment.

Tropospheric ozone assessment report: Global ozone metrics for climate change, human health, and crop/ecosystem research

Assessment of spatial and temporal variation in the impacts of ozone on human health, vegetation, and climate requires appropriate metrics. A key component of the Tropospheric Ozone Assessment Report (TOAR) is the consistent calculation of these metrics at thousands of monitoring sites globally. Investigating temporal trends in these metrics required that the same statistical methods be applied across these ozone monitoring sites. The nonparametric Mann-Kendall test (for significant trends) and the Theil-Sen estimator (for estimating the magnitude of trend) were selected to provide robust methods across all sites. This paper provides the scientific underpinnings necessary to better understand the implications of and rationale for selecting a specific TOAR metric for assessing spatial and temporal variation in ozone for a particular impact. The rationale and underlying research evidence that influence the derivation of specific metrics are given. The form of 25 metrics (4 for model-measurement comparison, 5 for characterization of ozone in the free troposphere, 11 for human health impacts, and 5 for vegetation impacts) are described. Finally, this study categorizes health and vegetation exposure metrics based on the extent to which they are determined only by the highest hourly ozone levels, or by a wider range of values. The magnitude of the metrics is influenced by both the distribution of hourly average ozone concentrations at a site location, and the extent to which a particular metric is determined by relatively low, moderate, and high hourly ozone levels. Hence, for the same ozone time series, changes in the distribution of ozone concentrations can result in different changes in the magnitude and direction of trends for different metrics. Thus, dissimilar conclusions about the effect of changes in the drivers of ozone variability (e.g., precursor emissions) on health and vegetation exposure can result from the selection of different metrics.

Assessing Temporal and Spatial Patterns of Observed and Predicted Ozone in Multiple Urban Areas

Background: Ambient monitoring data show spatial gradients in ozone (O3) across urban areas. Nitrogen oxide (NOx) emissions reductions will likely alter these gradients. Epidemiological studies often use exposure surrogates that may not fully account for the impacts of spatially and temporally changing concentrations on population exposure. Objectives: We examined the impact of large NOx decreases on spatial and temporal O3 patterns and the implications on exposure. Methods: We used a photochemical model to estimate O3 response to large NOx reductions. We derived time series of 2006–2008 O3 concentrations consistent with 50% and 75% NOx emissions reduction scenarios in three urban areas (Atlanta, Philadelphia, and Chicago) at each monitor location and spatially interpolated O3 to census-tract centroids. Results: We predicted that low O3 concentrations would increase and high O3 concentrations would decrease in response to NOx reductions within an urban area. O3 increases occurred across larger areas for the seasonal mean metric than for the regulatory metric (annual 4th highest daily 8-hr maximum) and were located only in urban core areas. O3 always decreased outside the urban core (e.g., at locations of maximum local ozone concentration) for both metrics and decreased within the urban core in some instances. NOx reductions led to more uniform spatial gradients and diurnal and seasonal patterns and caused seasonal peaks in midrange O3 concentrations to shift from midsummer to earlier in the year. Conclusions: These changes have implications for how O3 exposure may change in response to NOx reductions and are informative for the design of future epidemiology studies and risk assessments. Citation: Simon H, Wells B, Baker KR, Hubbell B. 2016. Assessing temporal and spatial patterns of observed and predicted ozone in multiple urban areas. Environ Health Perspect 124:1443–1452; http://dx.doi.org/10.1289/EHP190