Unaddressed Uncertainties When Scaling Regional Aircraft Emission Surveys to Basin Emission Estimates.

Wide-area aerial methods provide comprehensive screening of methane emissions from oil and gas (O & G) facilities in production basins. Emission detections ("plumes") from these studies are also frequently scaled to the basin level, but little is known regarding the uncertainties during scaling. This study analyzed an aircraft field study in the Denver-Julesburg basin to quantify how often plumes identified maintenance events, using a geospatial inventory of 12,629 O & G facilities. Study partners (7 midstream and production operators) provided the timing and location of 5910 maintenance events during the 6 week study period. Results indicated three substantial uncertainties with potential bias that were unaddressed in prior studies. First, plumes often detect maintenance events, which are large, short-duration, and poorly estimated by aircraft methods: 9.2 to 46% (38 to 52%) of plumes on production were likely known maintenance events. Second, plumes on midstream facilities were both infrequent and unpredictable, calling into question whether these estimates were representative of midstream emissions. Finally, 4 plumes attributed to O & G (19% of emissions detected by aircraft) were not aligned with any O & G location, indicating that the emissions had drifted downwind of some source. It is unclear how accurately aircraft methods estimate this type of plume; in this study, it had material impact on emission estimates. While aircraft surveys remain a powerful tool for identifying methane emissions on O & G facilities, this study indicates that additional data inputs, e.g., detailed GIS data, a more nuanced analysis of emission persistence and frequency, and improved sampling strategies are required to accurately scale plume estimates to basin emissions.

Identification and health risk evaluation of soil contaminated by polycyclic aromatic hydrocarbons at shale gas extraction sites based on positive matrix factorization.

The impact of shale gas extraction on surrounding environmental media remains unclear. In this study, the current state of contamination by polycyclic aromatic hydrocarbons (PAHs), which are high-frequency contaminants of shale gas, was investigated in the soil surrounding emerging shale gas development sites. The source analysis of PAHs was conducted in the soils of shale gas extraction sites using positive matrix factorization (PMF). The health risk assessment (HRA) was calculated for ingestion, dermal contact, and inhalation exposures, and the priority sources of PAHs in the soil were jointly identified by PMF and HRA to refine the contribution level of different individual PAHs to the carcinogenic risk. The results showed that both Sichuan and Chongqing mining site soils were contaminated to different degrees. Shale gas extraction has an impact on the surrounding soil, and the highest contributing source of PAHs in the mining site soil of Sichuan was anthropogenic activity, accounting for 31.6%, whereas that in the mining site soil of Chongqing was biomass combustion and mixed automobile combustion, accounting for 35.9%. At the two mining sites in Sichuan and Chongqing, none of the three exposure pathways (ingestion, dermal contact, and inhalation) posed a carcinogenic risk to children, whereas the dermal exposure pathway posed a carcinogenic risk to adults. Health risk assessments based on specific source assignments indicate that when managing soil pollution, the control of fossil fuel combustion and vehicular emissions should be prioritized.

Quantifying flare combustion efficiency using an imaging Fourier transform spectrometer.

Mid-wavelength infrared (MWIR) imaging Fourier transform spectrometers (IFTSs) are a promising technology for measuring flare combustion efficiency (CE) and destruction removal efficiency (DRE). These devices generate spectrally resolved intensity images of the flare plume, which may then be used to infer column densities of relevant species along each pixel line-of-sight. In parallel, a 2D projected velocity field may be inferred from the apparent motion of flow features between successive images. Finally, the column densities and velocity field are combined to estimate the mass flow rates for the species needed to calculate the CE or DRE. Since the MWIR IFTS can measure key carbon-containing species in the flare plume, it is possible to measure CE without knowing the fuel flow rate, which is important for fenceline measurements. This work demonstrates this approach on a laboratory heated vent, and then deploys the technique on two working flares: a combustor burning natural gas at a known rate, and a steam-assisted flare at a petrochemical refinery. Analysis of the IFTS data highlights the potential of this approach, but also areas for future development to transform this approach into a reliable technique for quantifying flare emissions.Implications: Our research is motivated by the need to assess hydrocarbon emissions from flaring, which is a critical problem of global significance. For example, recent studies have shown that methane destruction efficiency of flaring from upstream oil may be significantly lower than the commonly assumed figure of 98%; work by Plant et al. , in particular, suggest that this discrepancy amounts to CO2 emissions from 2 to 8 million automobiles annually, considering the US alone. Similarly, the international energy agency (IEA) estimates a global flare efficiency of 92%, which translates in 8 million tons of CH4 emitted by flares in 2020. Highlighted by these studies and supported by the World Bank initiatives toward zero routine flaring emissions, there is an urgent need for oil and gas industry to assess their flare methane emission, and overall hydrocarbon emissions. At the very least, it is critical to identify problematic flare operating conditions and means to mitigate flare emissions. Focusing on remote quantification of plume species, the measurement technique and quantification method presented in this paper is a considerable step forward in that direction by computing combustion efficiency and key components for destruction efficiency.

Methods for Spatial Extrapolation of Methane Measurements in Constructing Regional Estimates from Sample Populations.

Methane emission estimates for oil and gas facilities are typically based on estimates at a subpopulation of facilities, and these emission estimates are then extrapolated to a larger region or basin. Basin-level emission estimates are then frequently compared with basin-level observations. Methane emissions from oil and gas systems are inherently variable and intermittent, which make it difficult to determine whether a sample population is sufficiently large to be representative of a larger region. This work develops a framework for extrapolation of emission estimates using the case study of an operator in the Green River Basin. This work also identifies a new metric, the capture ratio, which quantifies the extent to which sources are represented in the sample population, based on the skewness of emissions for each source. There is a strong correlation between the capture ratio and extrapolation error, which suggests that understanding source-level emissions distributions can mitigate error when sample populations are selected and extrapolating measurements. The framework and results from this work can inform the selection and extrapolation of site measurements when developing methane emission inventories and establishing uncertainty bounds to assess whether inventory estimates are consistent with independent large spatial-scale observations.

Sustainable planning: the case study of the Strait of Messina ports.

The energy and environmental policy carried out by the Port System Authority of the Strait (AdSP), in charge of the management of the ports spread along the Strait of Messina, is reported. The Environmental and Energy Planning Document of Port Systems (DEASP, the Italian acronym) is the document explaining the AdSP sustainable strategy to reduce GHG emissions. It defines specific measures, in order to improve energy efficiency in buildings and infrastructures, promote the use of renewable energy in the port area, and confer environmental benefits for the citizens of neighboring territories and port users. The main actions developed are as follows: photovoltaic solar plants and tidal energy systems, electrification of the docks to allow the shore supply of ships, and the construction of a Liquefied Natural Gas (LNG) storage plant to replace more polluting marine fuels, together with awareness campaigns on "green" issues, involving the 3 million users of these ports. Starting from the socio-economic and environmental analysis of the territorial context managed by AdSP, the DEASP analyses all the activities carried out inside port areas and reports the energy consumptions of the concessionaries, in the way to calculate the carbon footprint and develop an environmental sustainable strategy to reduce pollutant emissions. The interventions foreseen are assessed through the cost-benefit analysis and allow reducing the GHG emissions in 2030 up to 46%.

The Role of Emission Size Distribution on the Efficacy of New Technologies to Reduce Methane Emissions from the Oil and Gas Sector.

Methane emissions from oil and gas operations exhibit skewed distributions. New technologies such as aerial-based leak detection surveys promise cost-effective detection of large emitters (greater than 10 kg/h). Recent policies such as the US Environmental Protection Agency (EPA) methane rule that allow the use of new technologies as part of leak detection and repair (LDAR) programs require a demonstration of equivalence with existing optical gas imaging (OGI) based LDAR programs. In this work, we illustrate the impact of emission size distribution on the equivalency condition between the OGI and site-wide survey technologies. Emission size distributions compiled from aerial measurements include significantly more emitters between 1 and 10 kg/h and lower average emission rates for large emitters compared to the emission distribution in the EPA rule. As a result, we find that equivalence may be achieved at lower site-wide survey frequencies when using technologies with detection thresholds below 10 kg/h, compared to the EPA rule. However, equivalence cannot be achieved with a detection threshold of 30 kg/h at any survey frequency, because most emitters across most US basins exhibit emission rates below 30 kg/h. We find that equivalence is a complex tradeoff among technology choice, design of LDAR programs, and survey frequency that can have more than one unique solution set.

Ground-Based Mobile Measurements to Track Urban Methane Emissions from Natural Gas in 12 Cities across Eight Countries.

To mitigate methane emission from urban natural gas distribution systems, it is crucial to understand local leak rates and occurrence rates. To explore urban methane emissions in cities outside the U.S., where significant emissions were found previously, mobile measurements were performed in 12 cities across eight countries. The surveyed cities range from medium size, like Groningen, NL, to large size, like Toronto, CA, and London, UK. Furthermore, this survey spanned across European regions from Barcelona, ES, to Bucharest, RO. The joint analysis of all data allows us to focus on general emission behavior for cities with different infrastructure and environmental conditions. We find that all cities have a spectrum of small, medium, and large methane sources in their domain. The emission rates found follow a heavy-tailed distribution, and the top 10% of emitters account for 60-80% of total emissions, which implies that strategic repair planning could help reduce emissions quickly. Furthermore, we compare our findings with inventory estimates for urban natural gas-related methane emissions from this sector in Europe. While cities with larger reported emissions were found to generally also have larger observed emissions, we find clear discrepancies between observation-based and inventory-based emission estimates for our 12 cities.

Missing methane emissions from urban sewer networks.

Methane emissions from sewer networks are an important source of anthropogenic greenhouse gases (GHGs) but are not currently reflected in the national GHG inventory. We found significant CH4 emissions of approximately 573 [395-831] CH4 t y-1 from sewer networks in the old residential and commercial areas of Seoul (Gwanak district) using an electric vehicle-based atmospheric GHG monitoring platform. The majority of ethane-to-methane ratios (<0.005) from the observations further suggest that distinctive CH4 emissions from sewer networks are likely related to microbial activity rather than to simple natural gas leakage. Because over 90% of the sewer network in Seoul is a gravity drain type of combined sewer network, where both wastewater and stormwater flow through the same pipes, resulting in the generation of methane emissions from the microbial activity and the manholes and rain gutters, which are directly connected to the combined sewer networks are major sources of atmospheric methane emissions. This study suggests that appropriate treatment of sewer networks can mitigate missing methane emissions in cities that were not originally included in GHG inventory of South Korea.

Quantifying non-steady state natural gas leakage from the pipelines using an innovative sensor network and model for subsurface emissions - InSENSE.

Detecting and quantifying subsurface leaks remains a challenge due to the complex nature and extent of belowground leak scenarios. To address these scenarios, monitoring and evaluating changes in gas leakage behavior over space and time are crucial for ensuring safe and efficient responses to known or potential gas leaks. This study demonstrates the capability of linking environmental and gas concentration data obtained using a low-cost, near real-time methane (CH4) detector network and an inverse gas migration model to capture and quantify non-steady state belowground natural gas (NG) leaks. The Estimating Surface Concentration Above Pipeline Emission (ESCAPE) model was modified to incorporate the impact of soil properties on gas migration. Field-scale controlled NG experiments with leakage rates ranging from 37 to 121 g/h indicate that elevated belowground near-surface (BNS) gas concentrations persist long before elevated surface concentrations are observed. On average, BNS CH4 concentrations were 20%-486% higher than surface CH4 concentrations within the monitoring radius of 4 m from the leak location. An increase in the BNS CH4 concentration was observed within 3 h as the leak rate increased from 37 to 89 g/h. However, due to the atmospheric fluctuations, any changes in surface CH4 concentrations could not be confirmed within this period. The plume area of the BNS CH4 extended approximately two times farther than that of the surface CH4 as the gas leak rate increased from 37 to 121 g/h. The estimated NG leak rates by the modified ESCAPE model agreed well with the experimental NG leak rates (m = 0.99 and R2 = 0.77), demonstrating that including soil characteristics and BNS CH4 measurements can advance estimations of non-steady NG leak rates in low and moderate NG leak rate scenarios. The CH4 detector network and model show potential as an innovative tool to improve operators' risk assessment and NG leakage response.

Environmentally relevant concentrations of chemically complex shale gas wastewater led to reduced fitness of water fleas (Daphnia carinata): Multiple lines of evidence approach.

Shale gas hydraulic fracturing generates flowback waters that pose a threat to aquatic organisms if released into the environment. In order to prevent adverse effects on aquatic ecosystems, multiple lines of evidence are needed to guide better decisions and management actions. This study employed a multi-disciplinary approach, combining direct toxicity assessment (DTA) on the water flea Daphnia carinata and LC-MS metabolomics analysis to determine the impact of a major ion salinity control (SC) and a cumulative flowback shale gas wastewater (SGW) from a well in the Beetaloo Sub-basin, Northern Territory, Australia. The exposures included a culture water control, simply further referred to as 'control', SC at 1% and 2% (v/v) and SGW at 0.125, 0.25, 0.5, 1% and 2% (v/v). The results showed that reproduction was significantly increased at SGW 0.5%, and significantly decreased when exposed to SC 2%. SGW 2% was found to be acutely toxic for the D. carinata (< 48-h). Second generation (F1) of D. carinata exposed to 0.125-1% SGW generally saw reduced activity in four oxidative biomarkers: glutathione S-transferase, lipid peroxidation, reactive oxygen species, and superoxide dismutase. At the metabolomics level, we observed significant changes in 103 metabolites in Daphnia exposed to both SGW and elevated salinity, in comparison to the control group. These changes indicate a range of metabolic disturbances induced by SGW and salinity, such as lipid metabolism, amino acid metabolism, nucleotide synthesis, energy production, and the biosynthesis of crucial molecules like hormones and pigments. These multiple lines of evidence approach not only highlights the complexities of SGW's impact on aquatic ecosystems but also underscores the importance of informed decision-making and management practices to safeguard the environment and its inhabitants.

Characteristics and potential cytotoxicity of halogenated organic compounds in shale gas wastewater-impacted surface waters in Chongqing area， China.

Recent screening surveys have shown the presence of unknown source halogenated organic compounds (HOCs) in shale gas wastewater. However, their occurrence, profile, transport in surrounding surface water and environmental risk potentials remain unclear. Here, a method for the extraction and quantitative determination of 13 HOCs in water by solid phase extraction combined with gas chromatography-mass spectrometry (GC-MS) was established. All of the targeted HOCs were detected and peaked at the outfall, while these contaminants were generally not detected in samples upstream of the outfall, suggesting that these contaminants originated from the discharge of shale gas wastewater; this was further supported by the fact that these pollutants were generally detected in downstream samples, with a tendency for pollutant concentrations to decrease progressively with increasing distance from the outfall. However，different HOCs had different transport potential in water. In addition, the toxicological effects of typical HOCs were evaluated using HepG2 as a model cell. The results indicated that diiodoalkanes suppressed HepG2 cell proliferation and induced ROS generation in a concentration-dependent manner. Mechanistic studies showed that diiodoalkanes induced apoptosis in HepG2 cells via the ROS-mediated mitochondrial pathway, decreasing mitochondrial membrane potential and increasing intercellular ATP and Ca2+ levels. On the other hand, RT-qPCR and Western blot assays revealed that the SLC7A11/GPX4 signaling pathway and HO-1 regulation of ferritin autophagy-dependent degradation (HO-1/FTL) pathway were involved in the ferroptosis pathway induced by diiodoalkane in HepG2 cells. Our study not only elucidates the contamination profiles and transport of HOCs in surface water of typical shale gas extraction areas in China, but also reveals the toxicity mechanism of typical diiodoalkane.

Methane Emissions from Non-producing Oil and Gas Wells and the Potential Role of Seismic Activity: A Case Study in Northeast British Columbia, Canada.

Increasing seismic activity due to fluid injections for oil and gas production may be contributing to leakage along non-producing oil and gas wells and emitting methane, a potent greenhouse gas. However, the extent to which nearby seismicity may drive or exacerbate methane emissions and cause well integrity issues is unknown. Therefore, we analyze field evaluations at 448 non-producing oil and gas wells in Northeast British Columbia (NEBC) and geospatially analyze oil and gas well and fluid injection data alongside locations of 3515 earthquakes from 2001 to 2021 and 130 faults. Through analysis of ground and helicopter-based field evaluations of non-producing wells in NEBC, we show that methane emission rates of non-producing wells average at 8301 mg/h/well but vary by 10 orders of magnitude. We find that higher methane emission rates (milligrams of methane/h/well) are observed at wells with larger flowing pressures at the wellhead during completion (kPa) and with shorter distances (m) to earthquakes, particularly at plugged wells. These results imply that seismicity may increase the likelihood of non-producing well integrity issues and methane leakage, thereby also exacerbating groundwater contamination and environmental degradation risks.

The Futility of Relative Methane Reduction Targets in the Absence of Measurement-Based Inventories.

Under the Global Methane Pledge, Canada is developing oil and gas sector methane regulations targeting 75% reductions from 2012 levels by 2030. Without measured baselines and inventories, such policies are ultimately unverifiable and unenforceable. Using the major oil and gas producing province of Saskatchewan as a case study, we derive first-ever measurement-based methane inventories for the region and comprehensively model previous emissions back to the 2012 baseline. Although relative reductions of 23-69% have likely occurred, the dispersion of modeled possibilities and the high emissions from continuing production illustrate the limits of this approach as a meaningful policy metric. Moreover, nearly 90% of apparent reductions are explained by decreased production at heavy oil facilities, suggesting emissions have potential to rebound if production resumes. By contrast, derived measurement-based methane emissions intensities facilitate quantitative assessment and show that despite any past reductions, Saskatchewan's 0.41 ± 0.03 g/MJ intensity remains among the highest in North America. This highlights how relative reduction targets absent measured baselines and inventories are inherently futile and risk rewarding high emitters while obscuring ongoing mitigation potential. Ultimately, required global methane reductions will only be achieved by adopting objectively and independently verifiable emission metrics while measuring and tracking progress toward a net zero future.

Methane Emissions Show Recent Decline but Strong Seasonality in Two US Northeastern Cities.

Urban methane emissions estimated using atmospheric observations have been found to exceed estimates derived by using traditional inventory methods in several northeastern US cities. In this work, we leveraged a nearly five-year record of observations from a dense tower network coupled with a newly developed high-resolution emissions map to quantify methane emission rates in Washington, DC, and Baltimore, Maryland. Annual emissions averaged over 2018-2021 were 80.1 [95% CI: 61.2, 98.9] Gg in the Washington, DC urban area and 47.4 [95% CI: 35.9, 58.5] Gg in the Baltimore urban area, with a decreasing trend of approximately 4-5% per year in both cities. We also find wintertime emissions 44% higher than summertime emissions, correlating with natural gas consumption. We further attribute a large fraction of total methane emissions to the natural gas sector using a least-squares regression on our spatially resolved estimates, supporting previous findings that natural gas systems emit the plurality of methane in both cities. This study contributes to the relatively sparse existing knowledge base of urban methane emissions sources and variability, adding to our understanding of how these emissions change in time and providing evidence to support efforts to mitigate natural gas emissions.

Assessing the Relative Importance of Satellite-Detected Methane Superemitters in Quantifying Total Emissions for Oil and Gas Production Areas in Algeria.

Methane emissions from oil and gas production provide an important contribution to global warming. We investigate 2020 emissions from the largest gas field in Algeria, Hassi R'Mel, and the oil-production-dominated area Hassi Messaoud. We use methane data from the high-resolution (20 m) Sentinel-2 instruments to identify and estimate emission time series for 11 superemitters (including 10 unlit flares). We integrate this information in a transport model inversion that uses methane data from the coarser (7 km × 5.5 km) but higher-precision TROPOMI instrument to estimate emissions from both the 11 superemitters (>1 t/h individually) and the remaining diffuse area source (not detected as point sources with Sentinel-2). Compared to a bottom-up inventory for 2019 that is aligned with UNFCCC-reported emissions, we find that 2020 emissions in Hassi R'Mel (0.16 [0.11-0.22] Tg/yr) are lower by 53 [24-73]%, and emissions in Hassi Messaoud (0.22 [0.13-0.28] Tg/yr) are higher by 79 [4-188]%. Our analysis indicates that a larger fraction of Algeria's methane emissions (∼75%) come from oil production than national reporting suggests (5%). Although in both regions the diffuse area source constitutes the majority of emissions, relatively few satellite-detected superemitters provide a significant contribution (24 [12-40]% in Hassi R'Mel; 49 [27-71]% in Hassi Messaoud), indicating that mitigation efforts should address both. Our synergistic use of Sentinel-2 and TROPOMI can produce a unique and detailed emission characterization of oil and gas production areas.

A simple method to measure methane emissions from indoor gas leaks.

From wellhead to burner tip, each component of the natural gas process chain has come under increased scrutiny for the presence and magnitude of methane leaks, because of the large global warming potential of methane. Top-down measures of methane emissions in urban areas are significantly greater than bottom-up estimates. Recent research suggests this disparity might in part be explained by gas leaks from one of the least understood parts of the process chain: behind the gas meter in homes and buildings. However, little research has been performed in this area and few methods and data sets exist to measure or estimate them. We develop and test a simple and widely deployable closed chamber method that can be used for quantifying indoor methane emissions with an order-of-magnitude precision which allows for screening of indoor large volume ("super-emitting") leaks. We also perform test applications of the method finding indoor leaks in 90% of the 20 Greater Boston buildings studied and indoor methane emissions between 0.02-0.51 ft3 CH4 day-1 (0.4-10.3 g CH4 day-1) with a mean of 0.14 ft3 CH4 day-1 (2.8 g CH4 day-1). Our method provides a relatively simple way to scale up indoor methane emissions data collection. Increased data may reduce uncertainty in bottom-up inventories, and can be used to find super-emitting indoor emissions which may better explain the disparity between top-down and bottom-up post-meter emissions estimates.

Methane Emissions from Dairy Operations in California's San Joaquin Valley Evaluated Using Airborne Flux Measurements.

State inventories indicate that dairy operations account for nearly half of California's methane budget. Recent analyses suggest, however, that these emissions may be underestimated, complicating efforts to develop emission reduction strategies. Here, we report estimates of dairy methane emissions in the southern San Joaquin Valley (SJV) of California in June 2021 using airborne flux measurements. We find average dairy methane fluxes of 512 ± 178 mg m-2 h-1 from a region of 300+ dairies near Visalia, CA using a combination of eddy covariance and mass balance-based techniques, corresponding to 118 ± 41 kg dairy-1 h-1. These values estimated during our June campaign are 39 ± 48% larger than annual average estimates from the recently developed VISTA-CA inventory. We observed notable increases in emissions with temperature. Our estimates align well with inventory predictions when parametrizations for the temperature dependence of emissions are applied. Our measurements further demonstrate that the VISTA-CA emission inventory is considerably more accurate than the EPA GHG-I inventory in this region. Source apportionment analyses confirm that dairy operations produce the majority of methane emissions in the southern SJV (∼65%). Fugitive oil and gas (O&G) sources account for the remaining ∼35%. Our results support the accuracy of the process-based models used to develop dairy emission inventories and highlight the need for additional investigation of the meteorological dependence of these emissions.

Exceedances of Secondary Aerosol Formation from In-Use Natural Gas Heavy-Duty Vehicles Compared to Diesel Heavy-Duty Vehicles.

This work, for the first time, assessed the secondary aerosol formation from both in-use diesel and natural gas heavy-duty vehicles of different vocations when they were operated on a chassis dynamometer while the vehicles were exercised on different driving cycles. Testing was performed on natural gas vehicles equipped with three-way catalysts (TWCs) and diesel trucks equipped with diesel oxidation catalysts, diesel particulate filters, and selective catalytic reduction systems. Secondary aerosol was measured after introducing dilute exhaust into a 30 m3 environmental chamber. Particulate matter ranged from 0.18 to 0.53 mg/mile for the diesel vehicles vs 1.4-85 mg/mile for the natural gas vehicles, total particle number ranged from 4.01 × 1012 to 3.61 × 1013 for the diesel vehicles vs 5.68 × 1012-2.75 × 1015 for the natural gas vehicles, and nonmethane organic gas emissions ranged from 0.032 to 0.05 mg/mile for the diesel vehicles vs 0.012-1.35 mg/mile for the natural gas vehicles. Ammonia formation was favored in the TWC and was found in higher concentrations for the natural gas vehicles (ranged from ∼0 to 1.75 g/mile) than diesel vehicles (ranged from ∼0 to 0.4 g/mile), leading to substantial secondary ammonium nitrate formation (ranging from 8.5 to 98.8 mg/mile for the natural gas vehicles). For the diesel vehicles, one had a secondary ammonium nitrate of 18.5 mg/mile, while the other showed essentially no secondary ammonium nitrate formation. The advanced aftertreatment controls in diesel vehicles resulted in almost negligible secondary organic aerosol (SOA) formation (ranging from 0.046 to 2.04 mg/mile), while the natural gas vehicles led to elevated SOA formation that was likely sourced from the engine lubricating oil (ranging from 3.11 to 39.7 mg/mile). For two natural gas vehicles, the contribution of lightly oxidized lubricating oil in the primary organic aerosol was dominant (as shown in the mass spectra analysis), leading to enhanced SOA mass. Heavily oxidized lubricating oil was also observed to contribute to the SOA formation for other natural gas vehicles.

Methane Emissions from Abandoned Oil and Gas Wells in Alberta and Saskatchewan, Canada: The Role of Surface Casing Vent Flows.

Abandoned oil and gas wells can act as leakage pathways for methane, a potent greenhouse gas, and other fluids to migrate through the subsurface and to the atmosphere. National estimates of methane emissions remain highly uncertain, and available measurements do not provide details on whether the emissions are associated with well integrity failure (indicating subsurface leaks) or aboveground well infrastructure leaks. Therefore, we directly measured methane emission rates from 238 unplugged and plugged abandoned wells across Alberta and Saskatchewan, Canada, separately quantified emissions from surface casing vents and other emissions from the wellhead (non-surface casing vent), and developed emission factors to estimate Canada-wide emissions from abandoned wells. Our highest measured emission rate (5.2 × 106 mg CH4/hr) from an unplugged gas well was two to three times higher than the largest previously published emission rate from an abandoned well. We estimated methane emissions from abandoned wells in Canada to be 85-93 kilotonnes of methane per year, of which surface casing vent emissions represented 75-82% (70 kilotonnes of methane per year). We found that subsurface leaks, as evidenced by surface casing vent flows, occurred at 32% of abandoned wells in Alberta, substantially higher than previously estimated using provincial data alone (6 and 11%). Therefore, well integrity failures and groundwater contamination are likely to be more common than previous studies suggest.

Determination of intermolecular and intramolecular isotopic compositions of low-abundance gaseous hydrocarbons using an online hydrocarbon gas concentration method.

The stable isotopic composition of natural gas can be used to identify its origin and source. However, low concentrations of gaseous hydrocarbons in high-mature natural and shale gases hinder accurate determination of their compound- and position-specific isotopic compositions. In this study, an online C2+ hydrocarbon gas concentration system combined with gas chromatography-isotope ratio mass spectrometry (GC-IRMS) or gas chromatography-pyrolysis-gas chromatography-isotope ratio mass spectrometry (GC-Py-GC-IRMS) was developed to determine compound- and position-specific isotopic compositions of low-abundance gaseous hydrocarbons. The lower limit of the gas concentration required for isotope ratio determination using the online concentration system is 0.001% (0.003%) for compound-specific carbon (hydrogen) isotopes and 0.005% for position-specific carbon isotopes and is thus applicable to most natural gas samples. The online concentration technique does not cause significant isotopic fractionation effects, and the combination with GC-IRMS and GC-Py-GC-IRMS can accurately and precisely determine the compound-specific δ13C and δD values of low-content C2+ gaseous hydrocarbons and the position-specific δ13C values (δ13Ca, δ13Cb, and SP values) of propane in low-content propane samples, respectively. The application of our method to two natural gas samples from the Ordos and Sichuan basins further confirms that the online concentration method allows simple and rapid determination of the compound- and position-specific isotopic compositions of low-abundance gaseous hydrocarbons.