Methane flux from flowback operations at a shale gas site.

We report measurements of methane (CH4) mixing ratios and emission fluxes derived from sampling at a monitoring station at an exploratory shale gas extraction facility in Lancashire, England. Elevated ambient CH4 mixing ratios were recorded in January 2019 during a period of cold-venting associated with a nitrogen lift process at the facility. These processes are used to clear the well to stimulate flow of natural gas from the target shale. Estimates of CH4 flux during the emission event were made using three independent modeling approaches: Gaussian plume dispersion (following both a simple Gaussian plume inversion and the US EPA OTM 33-A method), and a Lagrangian stochastic transport model (WindTrax). The three methods yielded an estimated peak CH4 flux during January 2019 of approximately 70 g s-1. The total mass of CH4 emitted during the six-day venting period was calculated to be 2.9, 4.2 ± 1.4(1σ) and 7.1 ± 2.1(1σ) tonnes CH4 using the simple Gaussian plume model, WindTrax, and OTM-33A methods, respectively. Whilst the flux approaches all agreed within 1σ uncertainty, an estimate of 4.2 (± 1.4) tonnes CH4 represents the most confident assessment due to the explicit modeling of advection and meteorological stability permitted using the WindTrax model. This mass is consistent with fluxes calculated by the Environment Agency (in the range 2.7 to 6.8 tonnes CH4), using emission data provided by the shale site operator to the regulator. This study provides the first CH4 emission estimate for a nitrogen lift process and the first-reported flux monitoring of a UK shale gas site, and contributes to the evaluation of the environmental impacts of shale gas operations worldwide. This study also provides forward guidance on future monitoring applications and flux calculation in transient emission events. Implications: This manuscript discusses atmospheric measurements near to the UK's first hydraulic fracturing facility, which has very high UK public, media, and policy interest. The focus of this manuscript is on a single week of data in which a large venting event at the shale gas site saw emissions of ~4 tonnes of methane to atmosphere, in breach of environmental permits. These results are likely to beresults are likely to be reported by the media and may influence future policy decisions concerning the UK hydraulic fracturing industry.

Characterizing the aging of biomass burning organic aerosol by use of mixing ratios: a meta-analysis of four regions.

Characteristic organic aerosol (OA) emission ratios (ERs) and normalized excess mixing ratios (NEMRs) for biomass burning (BB) events have been calculated from ambient measurements recorded during four field campaigns. Normalized OA mass concentrations measured using Aerodyne Research Inc. quadrupole aerosol mass spectrometers (Q-AMS) reveal a systematic variation in average values between different geographical regions. For each region, a consistent, characteristic ratio is seemingly established when measurements are collated from plumes of all ages and origins. However, there is evidence of strong regional and local-scale variability between separate measurement periods throughout the tropical, subtropical, and boreal environments studied. ERs close to source typically exceed NEMRs in the far-field, despite apparent compositional change and increasing oxidation with age. The absence of any significant downwind mass enhancement suggests no regional net source of secondary organic aerosol (SOA) from atmospheric aging of BB sources, in contrast with the substantial levels of net SOA formation associated with urban sources. A consistent trend of moderately reduced ΔOA/ΔCO ratios with aging indicates a small net loss of OA, likely as a result of the evaporation of organic material from initial fire emissions. Variability in ERs close to source is shown to substantially exceed the magnitude of any changes between fresh and aged OA, emphasizing the importance of fuel and combustion conditions in determining OA loadings from biomass burning.

Impact of alternative fuels on emissions characteristics of a gas turbine engine - part 1: gaseous and particulate matter emissions.

Growing concern over emissions from increased airport operations has resulted in a need to assess the impact of aviation related activities on local air quality in and around airports, and to develop strategies to mitigate these effects. One such strategy being investigated is the use of alternative fuels in aircraft engines and auxiliary power units (APUs) as a means to diversify fuel supplies and reduce emissions. This paper summarizes the results of a study to characterize the emissions of an APU, a small gas turbine engine, burning conventional Jet A-1, a fully synthetic jet fuel, and other alternative fuels with varying compositions. Gas phase emissions were measured at the engine exit plane while PM emissions were recorded at the exit plane as well as 10 m downstream of the engine. Five percent reduction in NO(x) emissions and 5-10% reduction in CO emissions were observed for the alternative fuels. Significant reductions in PM emissions at the engine exit plane were achieved with the alternative fuels. However, as the exhaust plume expanded and cooled, organic species were found to condense on the PM. This increase in organic PM elevated the PM mass but had little impact on PM number.

Impact of alternative fuels on emissions characteristics of a gas turbine engine - part 2: volatile and semivolatile particulate matter emissions.

The work characterizes the changes in volatile and semivolatile PM emissions from a gas turbine engine resulting from burning alternative fuels, specifically gas-to-liquid (GTL), coal-to-liquid (CTL), a blend of Jet A-1 and GTL, biodiesel, and diesel, to the standard Jet A-1. The data presented here, compares the mass spectral fingerprints of the different fuels as measured by the Aerodyne high resolution time-of-flight aerosol mass spectrometer. There were three sample points, two at the exhaust exit plane with dilution added at different locations and another probe located 10 m downstream. For emissions measured at the downstream probe when the engine was operating at high power, all fuels produced chemically similar organic PM, dominated by C(x)H(y) fragments, suggesting the presence of long chain alkanes. The second largest contribution came from C(x)H(y)O(z) fragments, possibly from carbonyls or alcohols. For the nondiesel fuels, the highest loadings of organic PM were from the downstream probe at high power. Conversely, the diesel based fuels produced more organic material at low power from one of the exit plane probes. Differences in the composition of the PM for certain fuels were observed as the engine power decreased to idle and the measurements were made closer to the exit plane.

Polycyclic aromatic hydrocarbon emissions from the combustion of alternative fuels in a gas turbine engine.

We report on the particulate-bound polycyclic aromatic hydrocarbons (PAH) in the exhaust of a test-bed gas turbine engine when powered by Jet A-1 aviation fuel and a number of alternative fuels: Sasol fully synthetic jet fuel (FSJF), Shell gas-to-liquid (GTL) kerosene, and Jet A-1/GTL 50:50 blended kerosene. The concentration of PAH compounds in the exhaust emissions vary greatly between fuels. Combustion of FSJF produces the greatest total concentration of PAH compounds while combustion of GTL produces the least. However, when PAHs in the exhaust sample are measured in terms of the regulatory marker compound benzo[a]pyrene, then all of the alternative fuels emit a lower concentration of PAH in comparison to Jet A-1. Emissions from the combustion of Jet A-1/GTL blended kerosene were found to have a disproportionately low concentration of PAHs and appear to inherit a greater proportion of the GTL emission characteristics than would be expected from volume fraction alone. The data imply the presence of a nonlinear relation between fuel blend composition and the emission of PAH compounds. For each of the fuels, the speciation of PAH compounds present in the exhaust emissions were found to be remarkably similar (R(2) = 0.94-0.62), and the results do provide evidence to support the premise that PAH speciation is to some extent indicative of the emission source. In contrast, no correlation was found between the PAH species present in the fuel with those subsequently emitted in the exhaust. The results strongly suggests that local air quality measured in terms of the particulate-bound PAH burden could be significantly improved by the use of GTL kerosene either blended with or in place of Jet A-1 kerosene.