Quantifying Methane and Ozone Precursor Emissions from Oil and Gas Production Regions across the Contiguous US.

We present an updated fuel-based oil and gas (FOG) inventory with estimates of nitrogen oxide (NOx) emissions from oil and natural gas production in the contiguous US (CONUS). We compare the FOG inventory with aircraft-derived ("top-down") emissions for NOx over footprints that account for ∼25% of US oil and natural gas production. Across CONUS, we find that the bottom-up FOG inventory combined with other anthropogenic emissions is on average within ∼10% of top-down aircraft-derived NOx emissions. We also find good agreement in the trends of NOx from drilling- and production-phase activities, as inferred by satellites and in the bottom-up inventory. Leveraging tracer-tracer relationships derived from aircraft observations, methane (CH4) and non-methane volatile organic compound (NMVOC) emissions have been added to the inventory. Our total CONUS emission estimates for 2015 of oil and natural gas are 0.45 ± 0.14 Tg NOx/yr, 15.2 ± 3.0 Tg CH4/yr, and 5.7 ± 1.7 Tg NMVOC/yr. Compared to the US National Emissions Inventory and Greenhouse Gas Inventory, FOG NOx emissions are ∼40% lower, while inferred CH4 and NMVOC emissions are up to a factor of ∼2 higher. This suggests that NMVOC/NOx emissions from oil and gas basins are ∼3 times higher than current estimates and will likely affect how air quality models represent ozone formation downwind of oil and gas fields.

Development of a Fuel-Based Oil and Gas Inventory of Nitrogen Oxides Emissions.

In this study, we develop an alternative Fuel-based Oil and Gas inventory (FOG) of nitrogen oxides (NO x) from oil and gas production using publicly available fuel use records and emission factors reported in the literature. FOG is compared with the Environmental Protection Agency's 2014 National Emissions Inventory (NEI) and with new top-down estimates of NO x emissions derived from aircraft and ground-based field measurement campaigns. Compared to our top-down estimates derived in four oil and gas basins (Uinta, UT, Haynesville, TX/LA, Marcellus, PA, and Fayetteville, AR), the NEI overestimates NO x by over a factor of 2 in three out of four basins, while FOG is generally consistent with atmospheric observations. Challenges in estimating oil and gas engine activity, rather than uncertainties in NO x emission factors, may explain gaps between the NEI and top-down emission estimates. Lastly, we find a consistent relationship between reactive odd nitrogen species (NO y) and ambient methane (CH4) across basins with different geological characteristics and in different stages of production. Future work could leverage this relationship as an additional constraint on CH4 emissions from oil and gas basins.

Modeling Ozone in the Eastern U.S. using a Fuel-Based Mobile Source Emissions Inventory.

Recent studies suggest overestimates in current U.S. emission inventories of nitrogen oxides (NO x = NO + NO2). Here, we expand a previously developed fuel-based inventory of motor-vehicle emissions (FIVE) to the continental U.S. for the year 2013, and evaluate our estimates of mobile source emissions with the U.S. Environmental Protection Agency's National Emissions Inventory (NEI) interpolated to 2013. We find that mobile source emissions of NO x and carbon monoxide (CO) in the NEI are higher than FIVE by 28% and 90%, respectively. Using a chemical transport model, we model mobile source emissions from FIVE, and find consistent levels of urban NO x and CO as measured during the Southeast Nexus (SENEX) Study in 2013. Lastly, we assess the sensitivity of ozone (O3) over the Eastern U.S. to uncertainties in mobile source NO x emissions and biogenic volatile organic compound (VOC) emissions. The ground-level O3 is sensitive to reductions in mobile source NO x emissions, most notably in the Southeastern U.S. and during O3 exceedance events, under the revised standard proposed in 2015 (>70 ppb, 8 h maximum). This suggests that decreasing mobile source NO x emissions could help in meeting more stringent O3 standards in the future.

Air quality implications of the Deepwater Horizon oil spill.

During the Deepwater Horizon (DWH) oil spill, a wide range of gas and aerosol species were measured from an aircraft around, downwind, and away from the DWH site. Additional hydrocarbon measurements were made from ships in the vicinity. Aerosol particles of respirable sizes were on occasions a significant air quality issue for populated areas along the Gulf Coast. Yields of organic aerosol particles and emission factors for other atmospheric pollutants were derived for the sources from the spill, recovery, and cleanup efforts. Evaporation and subsequent secondary chemistry produced organic particulate matter with a mass yield of 8 ± 4% of the oil mixture reaching the water surface. Approximately 4% by mass of oil burned on the surface was emitted as soot particles. These yields can be used to estimate the effects on air quality for similar events as well as for this spill at other times without these data. Whereas emission of soot from burning surface oil was large during the episodic burns, the mass flux of secondary organic aerosol to the atmosphere was substantially larger overall. We use a regional air quality model to show that some observed enhancements in organic aerosol concentration along the Gulf Coast were likely due to the DWH spill. In the presence of evaporating hydrocarbons from the oil, NO(x) emissions from the recovery and cleanup operations produced ozone.

COVID-19 perturbation on US air quality and human health impact assessment.

The COVID-19 stay-at-home orders issued in the United States caused significant reductions in traffic and economic activities. To understand the pandemic's perturbations on US emissions and impacts on urban air quality, we developed near-real-time bottom-up emission inventories based on publicly available energy and economic datasets, simulated the emission changes in a chemical transport model, and evaluated air quality impacts against various observations. The COVID-19 pandemic affected US emissions across broad-based energy and economic sectors and the impacts persisted to 2021. Compared with 2019 business-as-usual emission scenario, COVID-19 perturbations resulted in annual decreases of 10-15% in emissions of ozone (O3) and fine particle (PM2.5) gas-phase precursors, which are about two to four times larger than long-term annual trends during 2010-2019. While significant COVID-induced reductions in transportation and industrial activities, particularly in April-June 2020, resulted in overall national decreases in air pollutants, meteorological variability across the nation led to local increases or decreases of air pollutants, and mixed air quality changes across the United States between 2019 and 2020. Over a full year (April 2020 to March 2021), COVID-induced emission reductions led to 3-4% decreases in national population-weighted annual fourth maximum of daily maximum 8-h average O3 and annual PM2.5. Assuming these emission reductions could be maintained in the future, the result would be a 4-5% decrease in premature mortality attributable to ambient air pollution, suggesting that continued efforts to mitigate gaseous pollutants from anthropogenic sources can further protect human health from air pollution in the future.

Volatile chemical products emerging as largest petrochemical source of urban organic emissions.

A gap in emission inventories of urban volatile organic compound (VOC) sources, which contribute to regional ozone and aerosol burdens, has increased as transportation emissions in the United States and Europe have declined rapidly. A detailed mass balance demonstrates that the use of volatile chemical products (VCPs)-including pesticides, coatings, printing inks, adhesives, cleaning agents, and personal care products-now constitutes half of fossil fuel VOC emissions in industrialized cities. The high fraction of VCP emissions is consistent with observed urban outdoor and indoor air measurements. We show that human exposure to carbonaceous aerosols of fossil origin is transitioning away from transportation-related sources and toward VCPs. Existing U.S. regulations on VCPs emphasize mitigating ozone and air toxics, but they currently exempt many chemicals that lead to secondary organic aerosols.