Enhancements in Ammonia and Methane from Agricultural Sources in the Northeastern Colorado Front Range Using Observations from a Small Research Aircraft.

Quantifying ammonia (NH3) to methane (CH4) enhancement ratios from agricultural sources is important for understanding air pollution and nitrogen deposition. The northeastern Colorado Front Range is home to concentrated animal feeding operations (CAFOs) that produce large emissions of NH3 and CH4. Isolating enhancements of NH3 and CH4 in this region due to agriculture is complicated because CAFOs are often located within regions of oil and natural gas (O&NG) extraction that are a major source of CH4 and other alkanes. Here, we utilize a small research aircraft to collect in situ 1 Hz measurements of gas-phase NH3, CH4, and ethane (C2H6) downwind of CAFOs during three flights conducted in November 2019. Enhancements in NH3 and CH4 are distinguishable up to 10 km downwind of CAFOs with the most concentrated portions of the plumes typically below 0.25 km AGL. We demonstrate that NH3 and C2H6 can be jointly used to separate near-source enhancements in CH4 from agriculture and O&NG. Molar enhancement ratios of NH3 to CH4 are quantified for individual CAFOs in this region, and they range from 0.8 to 2.7 ppbv ppbv-1. A multivariate regression model produces enhancement ratios and quantitative regional source contributions that are consistent with prior studies.

Coupled Air Quality and Boundary-Layer Meteorology in Western U.S. Basins during Winter: Design and Rationale for a Comprehensive Study.

Wintertime episodes of high aerosol concentrations occur frequently in urban and agricultural basins and valleys worldwide. These episodes often arise following development of persistent cold-air pools (PCAPs) that limit mixing and modify chemistry. While field campaigns targeting either basin meteorology or wintertime pollution chemistry have been conducted, coupling between interconnected chemical and meteorological processes remains an insufficiently studied research area. Gaps in understanding the coupled chemical-meteorological interactions that drive high pollution events make identification of the most effective air-basin specific emission control strategies challenging. To address this, a September 2019 workshop occurred with the goal of planning a future research campaign to investigate air quality in Western U.S. basins. Approximately 120 people participated, representing 50 institutions and 5 countries. Workshop participants outlined the rationale and design for a comprehensive wintertime study that would couple atmospheric chemistry and boundary-layer and complex-terrain meteorology within western U.S. basins. Participants concluded the study should focus on two regions with contrasting aerosol chemistry: three populated valleys within Utah (Salt Lake, Utah, and Cache Valleys) and the San Joaquin Valley in California. This paper describes the scientific rationale for a campaign that will acquire chemical and meteorological datasets using airborne platforms with extensive range, coupled to surface-based measurements focusing on sampling within the near-surface boundary layer, and transport and mixing processes within this layer, with high vertical resolution at a number of representative sites. No prior wintertime basin-focused campaign has provided the breadth of observations necessary to characterize the meteorological-chemical linkages outlined here, nor to validate complex processes within coupled atmosphere-chemistry models.

Importance of Superemitter Natural Gas Well Pads in the Marcellus Shale.

A large-scale study of methane emissions from well pads was conducted in the Marcellus shale (Pennsylvania), the largest producing natural gas shale play in the United States, to better identify the prevalence and characteristics of superemitters. Roughly 2100 measurements were taken from 673 unique unconventional well pads corresponding to ∼18% of the total population of active sites and ∼32% of the total statewide unconventional natural gas production. A log-normal distribution with a geometric mean of 2.0 kg h-1 and arithmetic mean of 5.5 kg h-1 was observed, which agrees with other independent observations in this region. The geometric standard deviation (4.4 kg h-1) compared well to other studies in the region, but the top 10% of emitters observed in this study contributed 77% of the total emissions, indicating an extremely skewed distribution. The integrated proportional loss of this representative sample was equal to 0.53% with a 95% confidence interval of 0.45-0.64% of the total production of the sites, which is greater than the U.S. Environmental Protection Agency inventory estimate (0.29%), but in the lower range of other mobile observations (0.09-3.3%). These results emphasize the need for a sufficiently large sample size when characterizing emissions distributions that contain superemitters.

Methane destruction efficiency of natural gas flares associated with shale formation wells.

Flaring to dispose of natural gas has increased in the United States and is typically assumed to be 98% efficient, accounting for both incomplete combustion and venting during unintentional flame termination. However, no in situ measurements of flare emissions have been reported. We used an aircraft platform to sample 10 flares in North Dakota and 1 flare in Pennsylvania, measuring CO2, CH4, and meteorological data. Destruction removal efficiency (DRE) was calculated by assuming a flare natural gas input composition of 60-100% CH4. In all cases flares were >99.80 efficient at the 25% quartile. Crosswinds up to 15 m/s were observed, but did not significantly adversely affect efficiency. During analysis unidentified peaks of CH4, most likely from unknown venting practices, appeared much larger in magnitude than emissions from flaring practices. Our analysis suggests 98% efficiency for nonsputtering flares is a conservative estimate for incomplete combustion and that the unidentified venting is a greater contributor to CH4 emissions.

Toward a better understanding and quantification of methane emissions from shale gas development.

The identification and quantification of methane emissions from natural gas production has become increasingly important owing to the increase in the natural gas component of the energy sector. An instrumented aircraft platform was used to identify large sources of methane and quantify emission rates in southwestern PA in June 2012. A large regional flux, 2.0-14 g CH4 s(-1) km(-2), was quantified for a ∼ 2,800-km(2) area, which did not differ statistically from a bottom-up inventory, 2.3-4.6 g CH4 s(-1) km(-2). Large emissions averaging 34 g CH4/s per well were observed from seven well pads determined to be in the drilling phase, 2 to 3 orders of magnitude greater than US Environmental Protection Agency estimates for this operational phase. The emissions from these well pads, representing ∼ 1% of the total number of wells, account for 4-30% of the observed regional flux. More work is needed to determine all of the sources of methane emissions from natural gas production, to ascertain why these emissions occur and to evaluate their climate and atmospheric chemistry impacts.