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Growth in unconventional oil and gas development (UOGD) in the United States has increased airborne emissions, raising environmental and human health concerns. To assess the potential impacts on air quality, we deployed instrumentation in Karnes City, Texas, a rural area in the middle of the Eagle Ford Shale. We measured several episodes of elevated Cl 2 levels, reaching maximum hourly averages of 800 ppt, the highest inland Cl 2 concentration reported to date. Concentrations peak during the day, suggesting a strong local source (given the short photolysis lifetime of Cl 2 ) and/or a photoinitiated production mechanism. Well preproduction activity near the measurement site is a plausible source of these high Cl 2 levels via direct emission and photoactive chemistry. ClNO 2 is also observed, but it peaks overnight, consistent with well-known nocturnal formation processes. Observations of organochlorines in the gas and particle phases reflect the contribution of chlorine chemistry to the formation of secondary pollutants in the area. Box modeling results suggest that the formation of ozone at this location is influenced by chlorine chemistry. These results suggest that UOGD can be an important source of reactive chlorine in the atmosphere, impacting radical budgets and the formation of secondary pollutants in these regions.

Emission rates were estimated for >100 oil and gas production sites with significant liquid-handling equipment (tank battery sites) in the Permian Basin of west Texas. Emission estimates based on equipment counts and emission factors, but not accounting for large uninventoried emission events, led to ensemble average emission rates of 1.8-3.6 kg/h per site. None of the site-specific emission estimates for individual sites, based on equipment counts, exceeded 10 kg/h. On-site drone-based emission measurements led to similar emission estimates for inventoried sources. Multiple aircraft measurement platforms were deployed and reported emissions exceeding 10 kg/h at 14-27% of the sites, and these high-emission rate sites accounted for 80-90% of total emissions for the ensemble of sites. The aircraft measurement systems were deployed asynchronously but within a 5 day period. At least half of the sites with emission rates above 10 kg/h detected by aircraft had emissions that did not persist at a level above 10 kg/h for repeat measurements, suggesting typical high-emission rate durations of a few days or less for many events. The two aircraft systems differed in their estimates of total emissions from the ensembles of sites sampled by more than a factor of 2; however, the normalized distributions of emissions for sites with emission rates of >10 kg/h were comparable for the two aircraft-based methods. The differences between the two aircraft-based platforms are attributed to a combination of factors; however, both aircraft-based emission measurement systems attribute a large fraction of emissions to sites with an emission rate of >10 kg/h.

Ozone formation due to episodic industrial emissions was modeled for the Houston-Galveston-Brazoria (HGB) region in Texas. A total of more than 1000 synthetic emission scenarios were modeled, accounting for different sources, emission magnitudes, emission compositions, duration and timing of the emission events, meteorology at the time of the emissions, and location of the emission source. Episodic emissions consistent with the characteristics of flaring resulted in the greatest amount of ozone formation. An index, based on incremental reactivity, for characterizing the ozone formation potential of flaring emissions was developed using the synthetic scenarios and was applied to the ~4500 flares that report emissions in the state of Texas. The flares with the highest ranking index in the HGB were identified and additional modeling was performed on the ozone formation potential of these flares. If these flares are modeled with their annual average emission rates, the maximum increase in maximum daily 8-h average ozone (MDA8) formation associated with flaring emissions is <1 ppb. If, however, it is assumed that emissions from flaring are episodic, rather than continuous, and temporal patterns consistent with previous data collection on flare emission variability in the HGB are applied, MDA8 enhancements associated with flaring emissions are >10 ppb for multiple scenarios. This analysis suggests that, for flares emissions that have high ozone formation potential, the temporal patterns of flare emissions should be accounted for in developing ozone mitigation plans., Competing Interests: Declaration of competing interest The authors declare the following competing financial interest(s): This work was supported by the 8-Hour Coalition, a group of companies operating facilities, including flares, in the Houston area. One of the authors (DTA) has served and is serving on the Environmental Protection Agency's Science Advisory Board; in this role, he is a paid Special Governmental Employee; DTA has current research support from the National Science Foundation, the Department of Energy, the Texas Commission on Environmental Quality, the Gas Technology Institute's Collaboratory to Advance Methane Science, the National Institute of Clean and Low Carbon Energy (NICE), ExxonMobil Upstream Research Company, Pioneer Natural Resources, and Environmental Defense Fund. He has also worked on air quality projects that have been supported by oil and gas producers and Environmental Defense Fund. DTA has done work as a consultant for multiple companies, including British Petroleum, Cheniere, Eastern Research Group, ExxonMobil, KeyLogic, and SLR International. Ling Huang has also served as a consultant, through Ramboll, to multiple companies., (Copyright © 2022 Elsevier B.V. All rights reserved.)

The methane emission intensity (methane emitted/gas produced or methane emitted/methane produced) of individual unconventional oil and gas production sites in the United States has a characteristic temporal behavior, exhibiting a brief period of decrease followed by a steady increase, with intensities after 10 years of production reaching levels that are 2-10 times the 10 year production-weighted average. Temporal patterns for methane emission intensity for entire production regions are more complex. Historical production data and facility data were used with a detailed basin-wide methane emission model to simulate the collective behavior of tens of thousands of wells and associated midstream facilities. For production regions with few to no new wells being brought to production, and existing wells having reached a mature stage, as in the Barnett Shale production region in north central Texas, the methane emission intensity gradually increases, as natural gas production decreases faster than emissions decrease, following the general pattern exhibited by individual wells. In production regions that are rapidly evolving, either with large numbers of new wells being put into production or with the introduction of source-specific regulations, the behavior is more complex. In the Eagle Ford Shale, which has had both a large number of new wells and the introduction of source-specific regulations, the methane emission intensity stays within relatively narrow bounds but the distribution of sources varies. As source distributions vary, basin-wide propane-to-methane and ethane-to-methane emission ratios vary, impacting methods used in source attribution.

Spatially resolved emission inventories were used with an atmospheric dispersion model to predict ambient concentrations of methane, ethane, and propane in the Eagle Ford oil and gas production region in south central Texas; predicted concentrations were compared to ground level observations. Using a base case inventory, predicted median propane/ethane concentration ratios were 106% higher (95% CI: 83% higher-226% higher) than observations, while median ethane/methane concentration ratios were 112% higher (95% CI: 17% higher-228% higher) than observations. Predicted median propane and ethane concentrations were factors of 6.9 (95% CI: 3-15.2) and 3.4 (95% CI: 1.4-9) larger than observations, respectively. Predicted median methane concentrations were 7% higher (95% CI: 39% lower-37% higher) than observations. These comparisons indicate that sources of emissions with high propane/ethane ratios (condensate tank flashing) were likely overestimated in the inventories. Because sources of propane and ethane emissions are also sources of methane emissions, the results also suggest that sources of emissions with low ethane/methane ratios (midstream sources) were underestimated. This analysis demonstrates the value of using multiple light alkanes in attributing sources of methane emissions and evaluating the performance of methane emission inventories for oil and natural gas production regions.

Unlabelled: Accurate estimates of biogenic emissions are required for air quality models that support the development of air quality management plans and attainment demonstrations. Land cover characterization is an essential driving input for most biogenic emissions models. This work contrasted the global Moderate Resolution Imaging Spectroradiometer (MODIS) land cover product against a regional land cover product developed for the Texas Commissions on Environmental Quality (TCEQ) over four climate regions in eastern Texas, where biogenic emissions comprise a large fraction of the total inventory of volatile organic compounds (VOCs) and land cover is highly diverse. The Model of Emissions of Gases and Aerosols from Nature (MEGAN) was utilized to investigate the influences of land cover characterization on modeled isoprene and monoterpene emissions through changes in the standard emission potential and emission activity factor, both separately and simultaneously. In Central Texas, forest coverage was significantly lower in the MODIS land cover product relative to the TCEQ data, which resulted in substantially lower estimates of isoprene and monoterpene emissions by as much as 90%. Differences in predicted isoprene and monoterpene emissions associated with variability in land cover characterization were primarily caused by differences in the standard emission potential, which is dependent on plant functional type. Photochemical modeling was conducted to investigate the effects of differences in estimated biogenic emissions associated with land cover characterization on predicted ozone concentrations using the Comprehensive Air Quality Model with Extensions (CAMx). Mean differences in maximum daily average 8-hour (MDA8) ozone concentrations were 2 to 6 ppb with maximum differences exceeding 20 ppb. Continued focus should be on reducing uncertainties in the representation of land cover through field validation., Implications: Uncertainties in the estimation of biogenic emissions associated with the characterization of land cover in global and regional data products were examined in eastern Texas. Misclassification between trees and low-growing vegetation in central Texas resulted in substantial differences in isoprene and monoterpene emission estimates and predicted ground-level ozone concentrations. Results from this study indicate the importance of land cover validation at regional scales.

The combined emissions and air quality impacts of electricity generation in the Texas grid and natural gas production in the Eagle Ford shale were estimated at various natural gas price points for the power sector. The increased use of natural gas in the power sector, in place of coal-fired power generation, drove reductions in average daily maximum 8 h ozone concentration of 0.6-1.3 ppb in northeastern Texas for a high ozone episode used in air quality planning. The associated increase in Eagle Ford upstream oil and gas production nitrogen oxide (NOx) emissions caused an estimated local increase, in south Texas, of 0.3-0.7 ppb in the same ozone metric. In addition, the potential ozone impacts of Eagle Ford emissions on nearby urban areas were estimated. On the basis of evidence from this work and a previous study on the Barnett shale, the combined ozone impact of increased natural gas development and use in the power sector is likely to vary regionally and must be analyzed on a case by case basis.

Natural gas use in electricity generation in Texas was estimated, for gas prices ranging from $1.89 to $7.74 per MMBTU, using an optimal power flow model. Hourly estimates of electricity generation, for individual electricity generation units, from the model were used to estimate spatially resolved hourly emissions from electricity generation. Emissions from natural gas production activities in the Barnett Shale region were also estimated, with emissions scaled up or down to match demand in electricity generation as natural gas prices changed. As natural gas use increased, emissions decreased from electricity generation and increased from natural gas production. Overall, NOx and SO2 emissions decreased, while VOC emissions increased as natural gas use increased. To assess the effects of these changes in emissions on ozone and particulate matter concentrations, spatially and temporally resolved emissions were used in a month-long photochemical modeling episode. Over the month-long photochemical modeling episode, decreases in natural gas prices typical of those experienced from 2006 to 2012 led to net regional decreases in ozone (0.2-0.7 ppb) and fine particulate matter (PM) (0.1-0.7 μg/m(3)). Changes in PM were predominantly due to changes in regional PM sulfate formation. Changes in regional PM and ozone formation are primarily due to decreases in emissions from electricity generation. Increases in emissions from increased natural gas production were offset by decreasing emissions from electricity generation for all the scenarios considered.

The impacts of alternative regional development patterns on emissions, dry deposition, and air quality were examined using four visions of future land use in Austin, Texas associated with a doubling of the population in 20-40 years from 2001. Emissions and their spatial allocation were determined based on the development pattern and used to predict hourly ozone concentrations. Differences in hourly ozone concentrations due to changes in anthropogenic emissions between the future case scenarios and a 2007 base case ranged from -14 to 22 ppb and were primarily associated with the implementation of federal mobile source standards; differences due to biogenic emissions and dry deposition due to urbanization ranged from only -1.4 to 0.7 ppb. These differences in the magnitude of emissions produced greater changes in air quality than differences in regional development patterns between the four scenarios. Differences in hourly ozone concentrations between the future development scenarios and a 2007 base case ranged from -14 to 22 ppb, in contrast to differences of -3 to 5 ppb between the future scenarios. The results imply that although the effects of urbanization patterns are non-negligible, the pattern of urban development is not as significant as reductions in emissions per capita.

The Gulf Coast Aerosol Research and Characterization Study ([GC-ARCH], also known as the Houston Fine Particulate Matter [PM] Supersite) examined the spatial and temporal variability in fine PM source contributions and composition and the physical and chemical processes that govern PM formation and transformation in southeastern Texas. This was accomplished through the analysis of data collected in a 16-month field sampling program (August 2000 through November 2001). Three core sites and approximately 15 peripheral sites, jointly operated by the study team and the Texas Commission on Environmental Quality (TCEQ), were used. Key scientific findings related to spatial and temporal variability in fine PM concentrations, sizes and composition of the fine PM, the strength of primary emission sources and causes of secondary fine PM formation are reported.

Emission trading is a market-based approach designed to improve the efficiency and economic viability of emission control programs; emission trading has typically been confined to trades among single pollutants. Interpollutant trading (IPT), as described in this work, allows for trades among emissions of different compounds that affect the same air quality end point, in this work, ambient ozone (O3) concentrations. Because emissions of different compounds impact air quality end points differently, weighting factors or trading ratios (tons of emissions of nitrogen oxides (NO(x)) equivalent to a ton of emissions of volatile organic compounds [VOCs]) must be developed to allow for IPT. In this work, IPT indices based on reductions in O3 concentrations and based on reductions in population exposures to O3 were developed and evaluated using a three-dimensional gridded photochemical model for Austin, TX, a city currently on the cusp of nonattainment with the National Ambient Air Quality Standards for O3 concentrations averaged over 8 hr. Emissions of VOC and NO(x) from area and mobile sources in Austin are larger than emissions from point sources. The analysis indicated that mobile and area sources exhibited similar impacts. Trading ratios based on maximum O3 concentration or population exposure were similar. In contrast, the trading ratios did exhibit significant (more than a factor of two) day-to-day variability. Analysis of the air quality modeling indicated that the daily variability in trading ratios could be attributed to daily variations in both emissions and meteorology.