Tropospheric O3 has been decreasing across much of the eastern U.S. but has remained steady or even increased in some western regions. Recent increases in VOC and NOx emissions associated with the production of oil and natural gas (O&NG) may contribute to this trend in some areas. The Northern Front Range of Colorado has regularly exceeded O3 air quality standards during summertime in recent years. This region has VOC emissions from a rapidly developing O&NG basin and low concentrations of biogenic VOC in close proximity to urban‐Denver NOx emissions. Here VOC OH reactivity (OHR), O3 production efficiency (OPE), and an observationally constrained box model are used to quantify the influence of O&NG emissions on regional summertime O3 production. Analyses are based on measurements acquired over two summers at a central location within the Northern Front Range that lies between major regional O&NG and urban emission sectors. Observational analyses suggest that mixing obscures any OPE differences in air primarily influenced by O&NG or urban emission sector. The box model confirms relatively modest OPE differences that are within the uncertainties of the field observations. Box model results also indicate that maximum O3 at the measurement location is sensitive to changes in NOx mixing ratio but also responsive to O&NG VOC reductions. Combined, these analyses show that O&NG alkanes contribute over 80% to the observed carbon mixing ratio, roughly 50% to the regional VOC OHR, and approximately 20% to regional photochemical O3 production.
The influence of stratosphere‐to‐troposphere transport (STT) on surface ozone (O3) concentrations in the greater Los Angeles area during the CalNex and IONS‐2010 measurement campaigns has been investigated. Principal component analysis (PCA) of surface O3measurements from 41 sampling stations indicates that ∼13% of the variance in the maximum daily 8‐h average (MDA8) O3between May 10 and June 19, 2010 was associated with changes of 2–3 day duration linked to the passage of upper‐level troughs. Ozonesondes launched from Joshua Tree National Park and airborne lidar measurements show that these changes coincided with the appearance of stratospheric intrusions in the lower troposphere above southern California. The Lagrangian particle dispersion model FLEXPART reproduces most of these intrusions, and supports the conclusion from the PCA that significant transport of stratospheric air to the surface occurred on May 28–30. This intrusion led to a peak 1‐h O3 concentration of 88 ppbv at Joshua Tree National Monument near the ozonesonde launch site on May 28, and widespread entrainment of stratospheric air into the boundary layer increased the local background O3 over the entire area to ∼55 ppbv on May 29–30. This background was 10–15 ppbv higher than the baseline O3 in air transported ashore from the Pacific Ocean, and when combined with locally produced O3 led to several exceedances of the current National Ambient Air Quality Standard (NAAQS) on the following day.
Abstract. A 3-day period of strong, synoptic-scale stagnation, in which daytime boundary-layer winds were light and variable over the region, occurred in mid July of the 1995 Southern Oxidants Study centered on Nashville, Tennessee. Profiler winds showed light and variable flow throughout the mixed layer during the daytime, but at night in the layer between 100 and 2000 m AGL (which had been occupied by the daytime mixed layer) the winds accelerated to 5-10 m s-1 as a result of nocturnal decoupling from surface friction, which producect inertial oscillations. In the present study, we investigate the effects of these wind changes on the buildup and transport of ozone (03). The primary measurement system used in this study was an airborne differential absorption lidar (DIAL) system that profiled 03 in the boundary layer as the airplane flew along. Vertical cross sections showed that 03 concentrations exceeding 120 ppb extended up to nearly 2 km AGL, but that the 03 hardly moved at all horizontally, instead forming a dome of pollution over or near the city. The analysis concentrates on four meteorological processes that determine the 3-D spatial distribution of 03 and the interaction between urban and rural pollution: (1) daytime buildup of 03 over the urban area, (2) the extent of the drift of pollution cloud during the day as it formed, which controls peak 03 concentrations, (3) nighttime transport by the accelerated winds above the surface, and (4) vertical mixing of pollution layers the next day. Other consequences of very light-wind conditions were intra-regional differences in daytime mixed-layer depth over distances of 50 km or less, and indications of an urban heat-island circulation. IntroductionOver relatively simple topography, such as that found near Nashville, Tennessee, the overriding control on the transport and dispersion of atmospheric pollutants is the large-scale (usually synoptic) wind speed and direction. Occasionally, the larger-scale flow becomes weak, indicating that synoptic controls on flow and transport are weak (except for the large-scale subsidence accompanying these conditions). Two implications of such stagnation are (1) that pollution emissions are confined to a much smaller volume than when stronger flow is present, often leading to the highest pollutant concentrations in a season, and (2) that smaller-mesoscale influences, such as surface heating differences, can express themselves as locally generated flows or variations in mixing properties.Because stagnation periods routinely produce the highest pollution concentrations, it is important to understand the key meteorological processes affecting the distribution and magnitude of the ozone buildup. We identify four processes that control the spread of the urban plume. The first three represent a sequence occurring through different stages of the diurnal heating cycle, and the fourth, advection, represents a daytime control that proved to be significant even under very light wind conditions. The processes are as follows: (1)
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