Improved atmospheric constraints on Southern Ocean CO2 exchange.

We present improved estimates of air-sea CO2 exchange over three latitude bands of the Southern Ocean using atmospheric CO2 measurements from global airborne campaigns and an atmospheric 4-box inverse model based on a mass-indexed isentropic coordinate (Mθe). These flux estimates show two features not clearly resolved in previous estimates based on inverting surface CO2 measurements: a weak winter-time outgassing in the polar region and a sharp phase transition of the seasonal flux cycles between polar/subpolar and subtropical regions. The estimates suggest much stronger summer-time uptake in the polar/subpolar regions than estimates derived through neural-network interpolation of pCO2 data obtained with profiling floats but somewhat weaker uptake than a recent study by Long et al. [Science 374, 1275-1280 (2021)], who used the same airborne data and multiple atmospheric transport models (ATMs) to constrain surface fluxes. Our study also uses moist static energy (MSE) budgets from reanalyses to show that most ATMs tend to have excessive diabatic mixing (transport across moist isentrope, θe, or Mθe surfaces) at high southern latitudes in the austral summer, which leads to biases in estimates of air-sea CO2 exchange. Furthermore, we show that the MSE-based constraint is consistent with an independent constraint on atmospheric mixing based on combining airborne and surface CO2 observations.

Excess methane emissions from shallow water platforms elevate the carbon intensity of US Gulf of Mexico oil and gas production.

The Gulf of Mexico is the largest offshore fossil fuel production basin in the United States. Decisions on expanding production in the region legally depend on assessments of the climate impact of new growth. Here, we collect airborne observations and combine them with previous surveys and inventories to estimate the climate impact of current field operations. We evaluate all major on-site greenhouse gas emissions, carbon dioxide (CO2) from combustion, and methane from losses and venting. Using these findings, we estimate the climate impact per unit of energy of produced oil and gas (the carbon intensity). We find high methane emissions (0.60 Tg/y [0.41 to 0.81, 95% confidence interval]) exceeding inventories. This elevates the average CI of the basin to 5.3 g CO2e/MJ [4.1 to 6.7] (100-y horizon) over twice the inventories. The CI across the Gulf varies, with deep water production exhibiting a low CI dominated by combustion emissions (1.1 g CO2e/MJ), while shallow federal and state waters exhibit an extraordinarily high CI (16 and 43 g CO2e/MJ) primarily driven by methane emissions from central hub facilities (intermediaries for gathering and processing). This shows that production in shallow waters, as currently operated, has outsized climate impact. To mitigate these climate impacts, methane emissions in shallow waters must be addressed through efficient flaring instead of venting and repair, refurbishment, or abandonment of poorly maintained infrastructure. We demonstrate an approach to evaluate the CI of fossil fuel production using observations, considering all direct production emissions while allocating to all fossil products.

Underestimated Dry Season Methane Emissions from Wetlands in the Pantanal.

Tropical wetlands contribute ∼30% of the global methane (CH4) budget. Limited observational constraints on tropical wetland CH4 emissions lead to large uncertainties and disparities in representing emissions. In this work, we combine remote sensing observations with atmospheric and wetland models to investigate dry season wetland CH4 emissions from the Pantanal region of South America. We incorporate inundation maps generated from the Cyclone Global Navigation Satellite System (CYGNSS) satellite constellation together with traditional inundation maps to generate an ensemble of wetland CH4 emission realizations. We challenge these realizations with daily satellite observations for May-July when wetland CH4 emission predictions diverge. We find that the CYGNSS inundation products predict larger emissions in May, in better agreement with observations. We use the model ensemble to generate an empirical observational constraint on CH4 emissions independent of choice of inundation map, finding large dry season wetland CH4 emissions (31.7 ± 13.6 and 32.0 ± 20.2 mg CH4/m2/day in May and June/July during 2018/2019, respectively). These May/June/July emissions are 2-3 times higher than current models, suggesting that annual wetland emissions may be higher than traditionally simulated. Observed trends in the early dry season indicate that dynamics during this period are of importance in representing tropical wetland CH4 behaviors.

In Situ Sampling of NOx Emissions from United States Natural Gas Flares Reveals Heavy-Tail Emission Characteristic.

Natural gas flaring is a common practice employed in many United States (U.S.) oil and gas regions to dispose of gas associated with oil production. Combustion of predominantly hydrocarbon gas results in the production of nitrogen oxides (NOx). Here, we present a large field data set of in situ sampling of real world flares, quantifying flaring NOx production in major U.S. oil production regions: the Bakken, Eagle Ford, and Permian. We find that a single emission factor does not capture the range of the observed NOx emission factors within these regions. For all three regions, the median emission factors fall within the range of four emission factors used by the Texas Commission for Environmental Quality. In the Bakken and Permian, the distribution of emission factors exhibits a heavy tail such that basin-average emission factors are 2-3 times larger than the value employed by the U.S. Environmental Protection Agency. Extrapolation to basin scale emissions using auxiliary satellite assessments of flare volumes indicates that NOx emissions from flares are skewed, with 20%-30% of the flares responsible for 80% of basin-wide flaring NOx emissions. Efforts to reduce flaring volume through alternative gas capture methods would have a larger impact on the NOx oil and gas budget than current inventories indicate.

Temporal Variation and Persistence of Methane Emissions from Shallow Water Oil and Gas Production in the Gulf of Mexico.

Methane emissions from the oil and gas supply chain can be intermittent, posing challenges for monitoring and mitigation efforts. This study examines shallow water facilities in the US Gulf of Mexico with repeat atmospheric observations to evaluate temporal variation in site-specific methane emissions. We combine new and previous observations to develop a longitudinal study, spanning from days to months to almost five years, evaluating the emissions behavior of sites over time. We also define and determine the chance of subsequent detection (CSD): the likelihood that an emitting site will be observed emitting again. The average emitting central hub in the Gulf has a 74% CSD at any time interval. Eight facilities contribute 50% of total emissions and are over 80% persistent with a 96% CSD above 100 kg/h and 46% persistent with a 42% CSD above 1000 kg/h, indicating that large emissions are persistent at certain sites. Forward-looking infrared (FLIR) footage shows many of these sites exhibiting cold venting. This suggests that for offshore, a low sampling frequency over large spatial coverage can capture typical site emissions behavior and identify targets for mitigation. We further demonstrate the preliminary use of space-based observations to monitor offshore emissions over time.

Societal shifts due to COVID-19 reveal large-scale complexities and feedbacks between atmospheric chemistry and climate change.

The COVID-19 global pandemic and associated government lockdowns dramatically altered human activity, providing a window into how changes in individual behavior, enacted en masse, impact atmospheric composition. The resulting reductions in anthropogenic activity represent an unprecedented event that yields a glimpse into a future where emissions to the atmosphere are reduced. Furthermore, the abrupt reduction in emissions during the lockdown periods led to clearly observable changes in atmospheric composition, which provide direct insight into feedbacks between the Earth system and human activity. While air pollutants and greenhouse gases share many common anthropogenic sources, there is a sharp difference in the response of their atmospheric concentrations to COVID-19 emissions changes, due in large part to their different lifetimes. Here, we discuss several key takeaways from modeling and observational studies. First, despite dramatic declines in mobility and associated vehicular emissions, the atmospheric growth rates of greenhouse gases were not slowed, in part due to decreased ocean uptake of CO2 and a likely increase in CH4 lifetime from reduced NO x emissions. Second, the response of O3 to decreased NO x emissions showed significant spatial and temporal variability, due to differing chemical regimes around the world. Finally, the overall response of atmospheric composition to emissions changes is heavily modulated by factors including carbon-cycle feedbacks to CH4 and CO2, background pollutant levels, the timing and location of emissions changes, and climate feedbacks on air quality, such as wildfires and the ozone climate penalty.

Quantifying Regional Methane Emissions in the New Mexico Permian Basin with a Comprehensive Aerial Survey.

Limiting emissions of climate-warming methane from oil and gas (O&G) is a major opportunity for short-term climate benefits. We deploy a basin-wide airborne survey of O&G extraction and transportation activities in the New Mexico Permian Basin, spanning 35 923 km2, 26 292 active wells, and over 15 000 km of natural gas pipelines using an independently validated hyperspectral methane point source detection and quantification system. The airborne survey repeatedly visited over 90% of the active wells in the survey region throughout October 2018 to January 2020, totaling approximately 98 000 well site visits. We estimate total O&G methane emissions in this area at 194 (+72/-68, 95% CI) metric tonnes per hour (t/h), or 9.4% (+3.5%/-3.3%) of gross gas production. 50% of observed emissions come from large emission sources with persistence-averaged emission rates over 308 kg/h. The fact that a large sample size is required to characterize the heavy tail of the distribution emphasizes the importance of capturing low-probability, high-consequence events through basin-wide surveys when estimating regional O&G methane emissions.

Interpreting contemporary trends in atmospheric methane.

Atmospheric methane plays a major role in controlling climate, yet contemporary methane trends (1982-2017) have defied explanation with numerous, often conflicting, hypotheses proposed in the literature. Specifically, atmospheric observations of methane from 1982 to 2017 have exhibited periods of both increasing concentrations (from 1982 to 2000 and from 2007 to 2017) and stabilization (from 2000 to 2007). Explanations for the increases and stabilization have invoked changes in tropical wetlands, livestock, fossil fuels, biomass burning, and the methane sink. Contradictions in these hypotheses arise because our current observational network cannot unambiguously link recent methane variations to specific sources. This raises some fundamental questions: (i) What do we know about sources, sinks, and underlying processes driving observed trends in atmospheric methane? (ii) How will global methane respond to changes in anthropogenic emissions? And (iii), What future observations could help resolve changes in the methane budget? To address these questions, we discuss potential drivers of atmospheric methane abundances over the last four decades in light of various observational constraints as well as process-based knowledge. While uncertainties in the methane budget exist, they should not detract from the potential of methane emissions mitigation strategies. We show that net-zero cost emission reductions can lead to a declining atmospheric burden, but can take three decades to stabilize. Moving forward, we make recommendations for observations to better constrain contemporary trends in atmospheric methane and to provide mitigation support.

Airborne Assessment of Methane Emissions from Offshore Platforms in the U.S. Gulf of Mexico.

Methane (CH4) emissions from oil and gas activities are large and poorly quantified, with onshore studies showing systematic inventory underestimates. We present aircraft measurements of CH4 emissions from offshore oil and gas platforms collected over the U.S. Gulf of Mexico in January 2018. Flights sampled individual facilities as well as regions of 5-70 facilities. We combine facility-level samples, production data, and inventory estimates to generate an aerial measurement-based inventory of CH4 emissions for the U.S. Gulf of Mexico. We compare our inventory and the Environmental Protection Agency Greenhouse Gas Inventory (GHGI) with regional airborne estimates. The new inventory and regional airborne estimates are consistent with the GHGI in deep water but appear higher for shallow water. For the full U.S. Gulf of Mexico our inventory estimates total emissions of 0.53 Tg CH4/yr [0.40-0.71 Tg CH4/yr, 95% CI] and corresponds to a loss rate of 2.9% [2.2-3.8%] of natural gas production. Our estimate is a factor of 2 higher than the GHGI updated with 2018 platform counts. We attribute this disagreement to incomplete platform counts and emission factors that both underestimate emissions for shallow water platforms and do not account for disproportionately high emissions from large shallow water facilities.

Daily Cropland Soil NOx Emissions Identified by TROPOMI and SMAP.

We use TROPOMI (TROPOspheric Monitoring Instrument) tropospheric nitrogen dioxide (NO2) measurements to identify cropland soil nitrogen oxide (NOx = NO + NO2) emissions at daily to seasonal scales in the U.S. Southern Mississippi River Valley. Evaluating 1.5 years of TROPOMI observations with a box model, we observe seasonality in local NOx enhancements and estimate maximum cropland soil NOx emissions (15-34 ng N m-2 s-1) early in growing season (May-June). We observe soil NOx pulsing in response to daily decreases in volumetric soil moisture (VSM) as measured by the Soil Moisture Active Passive (SMAP) satellite. Daily NO2 enhancements reach up to 0.8 × 1015 molecules cm-2 4-8 days after precipitation when VSM decreases to ~30%, reflecting emissions behavior distinct from previously defined soil NOx pulse events. This demonstrates that TROPOMI NO2 observations, combined with observations of underlying process controls (e.g., soil moisture), can constrain soil NOx processes from space.

Direct human influence on atmospheric CO2 seasonality from increased cropland productivity.

Ground- and aircraft-based measurements show that the seasonal amplitude of Northern Hemisphere atmospheric carbon dioxide (CO2) concentrations has increased by as much as 50 per cent over the past 50 years. This increase has been linked to changes in temperate, boreal and arctic ecosystem properties and processes such as enhanced photosynthesis, increased heterotrophic respiration, and expansion of woody vegetation. However, the precise causal mechanisms behind the observed changes in atmospheric CO2 seasonality remain unclear. Here we use production statistics and a carbon accounting model to show that increases in agricultural productivity, which have been largely overlooked in previous investigations, explain as much as a quarter of the observed changes in atmospheric CO2 seasonality. Specifically, Northern Hemisphere extratropical maize, wheat, rice, and soybean production grew by 240 per cent between 1961 and 2008, thereby increasing the amount of net carbon uptake by croplands during the Northern Hemisphere growing season by 0.33 petagrams. Maize alone accounts for two-thirds of this change, owing mostly to agricultural intensification within concentrated production zones in the midwestern United States and northern China. Maize, wheat, rice, and soybeans account for about 68 per cent of extratropical dry biomass production, so it is likely that the total impact of increased agricultural production exceeds the amount quantified here.

Seasonally Resolved Excess Urban Methane Emissions from the Baltimore/Washington, DC Metropolitan Region.

Urban areas are increasingly recognized as an important source of methane (CH4), but we have limited seasonally resolved observations of these regions. In this study, we quantify seasonal and annual urban CH4 emissions over the Baltimore, Maryland, and Washington, DC metropolitan regions. We use CH4 atmospheric observations from four tall tower stations and a Lagrangian particle dispersion model to simulate CH4 concentrations at these stations. We directly compare these simulations with observations and use a geostatistical inversion method to determine optimal emissions to match our observations. We use observations spanning four seasons and employ an ensemble approach considering multiple meteorological representations, emission inventories, and upwind CH4 values. Forward simulations in winter, spring, and fall underestimate observed atmospheric CH4 while in summer, simulations overestimate observations because of excess modeled wetland emissions. With ensemble geostatistical inversions, the optimized annual emissions in DC/Baltimore are 39 ± 9 Gg/month (1 δ), 2.0 ± 0.4 times higher than the ensemble mean of bottom-up emission inventories. We find a modest seasonal variability of urban CH4 emissions not captured in current inventories, with optimized summer emissions ∼41% lower than winter, broadly consistent with expectations if emissions are dominated by fugitive natural gas sources that correlate with natural gas usage.

A Multiplatform Inversion Estimation of Statewide and Regional Methane Emissions in California during 2014-2016.

California methane (CH4) emissions are quantified for three years from two tower networks and one aircraft campaign. We used backward trajectory simulations and a mesoscale Bayesian inverse model, initialized by three inventories, to achieve the emission quantification. Results show total statewide CH4 emissions of 2.05 ± 0.26 (at 95% confidence) Tg/yr, which is 1.14 to 1.47 times greater than the anthropogenic emission estimates by California Air Resource Board (CARB). Some of differences could be biogenic emissions, superemitter point sources, and other episodic emissions which may not be completely included in the CARB inventory. San Joaquin Valley (SJV) has the largest CH4 emissions (0.94 ± 0.18 Tg/yr), followed by the South Coast Air Basin, the Sacramento Valley, and the San Francisco Bay Area at 0.39 ± 0.18, 0.21 ± 0.04, and 0.16 ± 0.05 Tg/yr, respectively. The dairy and oil/gas production sources in the SJV contribute 0.44 ± 0.36 and 0.22 ± 0.23 Tg CH4/yr, respectively. This study has important policy implications for regulatory programs, as it provides a thorough multiyear evaluation of the emissions inventory using independent atmospheric measurements and investigates the utility of a complementary multiplatform approach in understanding the spatial and temporal patterns of CH4 emissions in the state and identifies opportunities for the expansion and applications of the monitoring network.

Large Fugitive Methane Emissions From Urban Centers Along the U.S. East Coast.

Urban emissions remain an underexamined part of the methane budget. Here we present and interpret aircraft observations of six old and leak-prone major cities along the East Coast of the United States. We use direct observations of methane (CH4), carbon dioxide (CO2), carbon monoxide (CO), ethane (C2H6), and their correlations to quantify CH4 emissions and attribute to natural gas. We find the five largest cities emit 0.85 (0.63, 1.12) Tg CH4/year, of which 0.75 (0.49, 1.10) Tg CH4/year is attributed to natural gas. Our estimates, which include all thermogenic methane sources including end use, are more than twice that reported in the most recent gridded EPA inventory, which does not include end-use emissions. These results highlight that current urban inventory estimates of natural gas emissions are substantially low, either due to underestimates of leakage, lack of inclusion of end-use emissions, or some combination thereof.

Methane, Black Carbon, and Ethane Emissions from Natural Gas Flares in the Bakken Shale, North Dakota.

Incomplete combustion during flaring can lead to production of black carbon (BC) and loss of methane and other pollutants to the atmosphere, impacting climate and air quality. However, few studies have measured flare efficiency in a real-world setting. We use airborne data of plume samples from 37 unique flares in the Bakken region of North Dakota in May 2014 to calculate emission factors for BC, methane, ethane, and combustion efficiency for methane and ethane. We find no clear relationship between emission factors and aircraft-level wind speed or between methane and BC emission factors. Observed median combustion efficiencies for methane and ethane are close to expected values for typical flares according to the US EPA (98%). However, we find that the efficiency distribution is skewed, exhibiting log-normal behavior. This suggests incomplete combustion from flares contributes almost 1/5 of the total field emissions of methane and ethane measured in the Bakken shale, more than double the expected value if 98% efficiency was representative. BC emission factors also have a skewed distribution, but we find lower emission values than previous studies. The direct observation for the first time of a heavy-tail emissions distribution from flares suggests the need to consider skewed distributions when assessing flare impacts globally.

Airborne Quantification of Methane Emissions over the Four Corners Region.

Methane (CH4) is a potent greenhouse gas and the primary component of natural gas. The San Juan Basin (SJB) is one of the largest coal-bed methane producing regions in North America and, including gas production from conventional and shale sources, contributed ∼2% of U.S. natural gas production in 2015. In this work, we quantify the CH4 flux from the SJB using continuous atmospheric sampling from aircraft collected during the TOPDOWN2015 field campaign in April 2015. Using five independent days of measurements and the aircraft-based mass balance method, we calculate an average CH4 flux of 0.54 ± 0.20 Tg yr-1 (1σ), in close agreement with the previous space-based estimate made for 2003-2009. These results agree within error with the U.S. EPA gridded inventory for 2012. These flights combined with the previous satellite study suggest CH4 emissions have not changed. While there have been significant declines in natural gas production between measurements, recent increases in oil production in the SJB may explain why emission of CH4 has not declined. Airborne quantification of outcrops where seepage occurs are consistent with ground-based studies that indicate these geological sources are a small fraction of the basin total (0.02-0.12 Tg yr-1) and cannot explain basinwide consistent emissions from 2003 to 2015.

Anthropogenic emissions of methane in the United States.

This study quantitatively estimates the spatial distribution of anthropogenic methane sources in the United States by combining comprehensive atmospheric methane observations, extensive spatial datasets, and a high-resolution atmospheric transport model. Results show that current inventories from the US Environmental Protection Agency (EPA) and the Emissions Database for Global Atmospheric Research underestimate methane emissions nationally by a factor of ∼1.5 and ∼1.7, respectively. Our study indicates that emissions due to ruminants and manure are up to twice the magnitude of existing inventories. In addition, the discrepancy in methane source estimates is particularly pronounced in the south-central United States, where we find total emissions are ∼2.7 times greater than in most inventories and account for 24 ± 3% of national emissions. The spatial patterns of our emission fluxes and observed methane-propane correlations indicate that fossil fuel extraction and refining are major contributors (45 ± 13%) in the south-central United States. This result suggests that regional methane emissions due to fossil fuel extraction and processing could be 4.9 ± 2.6 times larger than in EDGAR, the most comprehensive global methane inventory. These results cast doubt on the US EPA's recent decision to downscale its estimate of national natural gas emissions by 25-30%. Overall, we conclude that methane emissions associated with both the animal husbandry and fossil fuel industries have larger greenhouse gas impacts than indicated by existing inventories.

Airborne Ethane Observations in the Barnett Shale: Quantification of Ethane Flux and Attribution of Methane Emissions.

We present high time resolution airborne ethane (C2H6) and methane (CH4) measurements made in March and October 2013 as part of the Barnett Coordinated Campaign over the Barnett Shale formation in Texas. Ethane fluxes are quantified using a downwind flight strategy, a first demonstration of this approach for C2H6. Additionally, ethane-to-methane emissions ratios (C2H6:CH4) of point sources were observationally determined from simultaneous airborne C2H6 and CH4 measurements during a survey flight over the source region. Distinct C2H6:CH4 × 100% molar ratios of 0.0%, 1.8%, and 9.6%, indicative of microbial, low-C2H6 fossil, and high-C2H6 fossil sources, respectively, emerged in observations over the emissions source region of the Barnett Shale. Ethane-to-methane correlations were used in conjunction with C2H6 and CH4 fluxes to quantify the fraction of CH4 emissions derived from fossil and microbial sources. On the basis of two analyses, we find 71-85% of the observed methane emissions quantified in the Barnett Shale are derived from fossil sources. The average ethane flux observed from the studied region of the Barnett Shale was 6.6 ± 0.2 × 10(3) kg hr(-1) and consistent across six days in spring and fall of 2013.

Aircraft-Based Estimate of Total Methane Emissions from the Barnett Shale Region.

We present estimates of regional methane (CH4) emissions from oil and natural gas operations in the Barnett Shale, Texas, using airborne atmospheric measurements. Using a mass balance approach on eight different flight days in March and October 2013, the total CH4 emissions for the region are estimated to be 76 ± 13 × 10(3) kg hr(-1) (equivalent to 0.66 ± 0.11 Tg CH4 yr(-1); 95% confidence interval (CI)). We estimate that 60 ± 11 × 10(3) kg CH4 hr(-1) (95% CI) are emitted by natural gas and oil operations, including production, processing, and distribution in the urban areas of Dallas and Fort Worth. This estimate agrees with the U.S. Environmental Protection Agency (EPA) estimate for nationwide CH4 emissions from the natural gas sector when scaled by natural gas production, but it is higher than emissions reported by the EDGAR inventory or by industry to EPA's Greenhouse Gas Reporting Program. This study is the first to show consistency between mass balance results on so many different days and in two different seasons, enabling better quantification of the related uncertainty. The Barnett is one of the largest production basins in the United States, with 8% of total U.S. natural gas production, and thus, our results represent a crucial step toward determining the greenhouse gas footprint of U.S. onshore natural gas production.

Demonstration of an ethane spectrometer for methane source identification.

Methane is an important greenhouse gas and tropospheric ozone precursor. Simultaneous observation of ethane with methane can help identify specific methane source types. Aerodyne Ethane-Mini spectrometers, employing recently available mid-infrared distributed feedback tunable diode lasers (DFB-TDL), provide 1 s ethane measurements with sub-ppb precision. In this work, an Ethane-Mini spectrometer has been integrated into two mobile sampling platforms, a ground vehicle and a small airplane, and used to measure ethane/methane enhancement ratios downwind of methane sources. Methane emissions with precisely known sources are shown to have ethane/methane enhancement ratios that differ greatly depending on the source type. Large differences between biogenic and thermogenic sources are observed. Variation within thermogenic sources are detected and tabulated. Methane emitters are classified by their expected ethane content. Categories include the following: biogenic (<0.2%), dry gas (1-6%), wet gas (>6%), pipeline grade natural gas (<15%), and processed natural gas liquids (>30%). Regional scale observations in the Dallas/Fort Worth area of Texas show two distinct ethane/methane enhancement ratios bridged by a transitional region. These results demonstrate the usefulness of continuous and fast ethane measurements in experimental studies of methane emissions, particularly in the oil and natural gas sector.