U.S. Ethane Emissions and Trends Estimated from Atmospheric Observations.

Oil and natural gas (O&G) production and processing activities have changed markedly across the U.S. over the past several years. However, the impacts of these changes on air pollution and greenhouse gas emissions are not clear. In this study, we examine U.S. ethane (C2H6) emissions, which are primarily from O&G activities, during years 2015-2020. We use C2H6 observations made by the NOAA Global Monitoring Laboratory and partner organizations from towers and aircraft and estimate emissions from these observations by using an inverse model. We find that U.S. C2H6 emissions (4.43 ± 0.2 Tg·yr-1) are approximately three times those estimated by the EPA's 2017 National Emissions Inventory (NEI) platform (1.54 Tg·yr-1) and exhibit a very different seasonal cycle. We also find that changes in U.S. C2H6 emissions are decoupled from reported changes in production; emissions increased 6.3 ± 7.6% (0.25 ± 0.31 Tg) between 2015 and 2020 while reported C2H6 production increased by a much larger amount (78%). Our results also suggest an apparent correlation between C2H6 emissions and C2H6 spot prices, where prices could be a proxy for pressure on the infrastructure across the supply chain. Overall, these results provide insight into how U.S. C2H6 emissions are changing over time.

The reduced net carbon uptake over Northern Hemisphere land causes the close-to-normal CO2 growth rate in 2021 La Niña.

La Niña climate anomalies have historically been associated with substantial reductions in the atmospheric CO2 growth rate. However, the 2021 La Niña exhibited a unique near-neutral impact on the CO2 growth rate. In this study, we investigate the underlying mechanisms by using an ensemble of net CO2 fluxes constrained by CO2 observations from the Orbiting Carbon Observatory-2 in conjunction with estimates of gross primary production and fire carbon emissions. Our analysis reveals that the close-to-normal atmospheric CO2 growth rate in 2021 was the result of the compensation between increased net carbon uptake over the tropics and reduced net carbon uptake over the Northern Hemisphere mid-latitudes. Specifically, we identify that the extreme drought and warm anomalies in Europe and Asia reduced the net carbon uptake and offset 72% of the increased net carbon uptake over the tropics in 2021. This study contributes to our broader understanding of how regional processes can shape the trajectory of atmospheric CO2 concentration under climate change.

Implications of Generation Efficiencies and Supply Chain Leaks for the Life Cycle Greenhouse Gas Emissions of Natural Gas-Fired Electricity in the United States.

Uncertainties in supply chain emissions raise questions about the benefits of natural gas as a bridge fuel, but recent efficiency improvements in gas-fired electricity generation remain overlooked. Our comprehensive analysis of supply chain infrastructure and electricity generation across the United States informs spatially and temporally resolved estimates of life cycle greenhouse gas emissions. Results show decreasing life cycle emissions over each year examined: 629, 574, and 525 kg CO2 eq MWh-1 in 2005, 2010, and 2015, respectively. Electricity generation contributed 86% of emissions or greater for each year. Despite concerns over uncertain methane leaks, efficiency improvements make it much more likely that natural gas electricity has an unambiguous greenhouse gas benefit relative to coal. Methane leaks would have to be 4.4 times the Environmental Protection Agency (EPA) value in 2015 to reverse these benefits over 20-year time horizons. With retiring coal plants and scrutinized supply chain emissions, our results show that natural gas can provide a lower emissions option to coal in an increasingly decarbonized power sector.

Potential Uses of Coal Methane in China and Associated Benefits for Air Quality, Health, and Climate.

China is the world's largest producer and consumer of coal, but the country has recently set ambitious targets for cleaner energy sources. These include goals to capture and utilize methane from coal seams as a source of unconventional natural gas. We investigate the impacts of using coal methane to displace coal power plants and residential coal combustion across northern China. We compare the greenhouse gas emissions, air quality, and public health impacts of several scenarios for coal methane utilization. We find that China's existing goals would decrease the country's total carbon emissions by ∼2.3% (284 million tons CO2eq). Furthermore, these reductions are dominated by mitigated methane emissions and therefore confer a much larger climate benefit than would be expected from other forms of natural gas. Our results also indicate that the air quality and health impacts strongly depend on how the methane is utilized. Using the methane to displace coal-fired electricity would reduce annual mean ambient PM2.5 concentrations by up to >2.5 µg/m3 and prevent up to 9290 premature mortalities annually (95% confidence interval: 7862-9992). By contrast, utilizing coal methane in home heating yields smaller changes to ambient air quality (∼0.6 µg/m3), but improvements to indoor air quality could produce comparable reductions in premature mortality.

China's coal mine methane regulations have not curbed growing emissions.

Anthropogenic methane emissions from China are likely greater than in any other country in the world. The largest fraction of China's anthropogenic emissions is attributable to coal mining, but these emissions may be changing; China enacted a suite of regulations for coal mine methane (CMM) drainage and utilization that came into full effect in 2010. Here, we use methane observations from the GOSAT satellite to evaluate recent trends in total anthropogenic and natural emissions from Asia with a particular focus on China. We find that emissions from China rose by 1.1 ± 0.4 Tg CH4 yr-1 from 2010 to 2015, culminating in total anthropogenic and natural emissions of 61.5 ± 2.7 Tg CH4 in 2015. The observed trend is consistent with pre-2010 trends and is largely attributable to coal mining. These results indicate that China's CMM regulations have had no discernible impact on the continued increase in Chinese methane emissions.

Carbon dioxide sources from Alaska driven by increasing early winter respiration from Arctic tundra.

High-latitude ecosystems have the capacity to release large amounts of carbon dioxide (CO2) to the atmosphere in response to increasing temperatures, representing a potentially significant positive feedback within the climate system. Here, we combine aircraft and tower observations of atmospheric CO2 with remote sensing data and meteorological products to derive temporally and spatially resolved year-round CO2 fluxes across Alaska during 2012-2014. We find that tundra ecosystems were a net source of CO2 to the atmosphere annually, with especially high rates of respiration during early winter (October through December). Long-term records at Barrow, AK, suggest that CO2 emission rates from North Slope tundra have increased during the October through December period by 73% ± 11% since 1975, and are correlated with rising summer temperatures. Together, these results imply increasing early winter respiration and net annual emission of CO2 in Alaska, in response to climate warming. Our results provide evidence that the decadal-scale increase in the amplitude of the CO2 seasonal cycle may be linked with increasing biogenic emissions in the Arctic, following the growing season. Early winter respiration was not well simulated by the Earth System Models used to forecast future carbon fluxes in recent climate assessments. Therefore, these assessments may underestimate the carbon release from Arctic soils in response to a warming climate.

Continued emissions of carbon tetrachloride from the United States nearly two decades after its phaseout for dispersive uses.

National-scale emissions of carbon tetrachloride (CCl4) are derived based on inverse modeling of atmospheric observations at multiple sites across the United States from the National Oceanic and Atmospheric Administration's flask air sampling network. We estimate an annual average US emission of 4.0 (2.0-6.5) Gg CCl4 y(-1) during 2008-2012, which is almost two orders of magnitude larger than reported to the US Environmental Protection Agency (EPA) Toxics Release Inventory (TRI) (mean of 0.06 Gg y(-1)) but only 8% (3-22%) of global CCl4 emissions during these years. Emissive regions identified by the observations and consistently shown in all inversion results include the Gulf Coast states, the San Francisco Bay Area in California, and the Denver area in Colorado. Both the observation-derived emissions and the US EPA TRI identified Texas and Louisiana as the largest contributors, accounting for one- to two-thirds of the US national total CCl4 emission during 2008-2012. These results are qualitatively consistent with multiple aircraft and ship surveys conducted in earlier years, which suggested significant enhancements in atmospheric mole fractions measured near Houston and surrounding areas. Furthermore, the emission distribution derived for CCl4 throughout the United States is more consistent with the distribution of industrial activities included in the TRI than with the distribution of other potential CCl4 sources such as uncapped landfills or activities related to population density (e.g., use of chlorine-containing bleach).

A multi-year estimate of methane fluxes in Alaska from CARVE atmospheric observations.

Methane (CH4) fluxes from Alaska and other arctic regions may be sensitive to thawing permafrost and future climate change, but estimates of both current and future fluxes from the region are uncertain. This study estimates CH4 fluxes across Alaska for 2012-2014 using aircraft observations from the Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE) and a geostatistical inverse model (GIM). We find that a simple flux model based on a daily soil temperature map and a static map of wetland extent reproduces the atmospheric CH4 observations at the state-wide, multi-year scale more effectively than global-scale, state-of-the-art process-based models. This result points to a simple and effective way of representing CH4 flux patterns across Alaska. It further suggests that contemporary process-based models can improve their representation of key processes that control fluxes at regional scales, and that more complex processes included in these models cannot be evaluated given the information content of available atmospheric CH4 observations. In addition, we find that CH4 emissions from the North Slope of Alaska account for 24% of the total statewide flux of 1.74 ± 0.44 Tg CH4 (for May-Oct.). Contemporary global-scale process models only attribute an average of 3% of the total flux to this region. This mismatch occurs for two reasons: process models likely underestimate wetland area in regions without visible surface water, and these models prematurely shut down CH4 fluxes at soil temperatures near 0°C. As a consequence, wetlands covered by vegetation and wetlands with persistently cold soils could be larger contributors to natural CH4 fluxes than in process estimates. Lastly, we find that the seasonality of CH4 fluxes varied during 2012-2014, but that total emissions did not differ significantly among years, despite substantial differences in soil temperature and precipitation; year-to-year variability in these environmental conditions did not affect obvious changes in total CH4 fluxes from the state.

Global emissions of refrigerants HCFC-22 and HFC-134a: unforeseen seasonal contributions.

HCFC-22 (CHClF2) and HFC-134a (CH2FCF3) are two major gases currently used worldwide in domestic and commercial refrigeration and air conditioning. HCFC-22 contributes to stratospheric ozone depletion, and both species are potent greenhouse gases. In this work, we study in situ observations of HCFC-22 and HFC-134a taken from research aircraft over the Pacific Ocean in a 3-y span [HIaper-Pole-to-Pole Observations (HIPPO) 2009-2011] and combine these data with long-term ground observations from global surface sites [National Oceanic and Atmospheric Administration (NOAA) and Advanced Global Atmospheric Gases Experiment (AGAGE) networks]. We find the global annual emissions of HCFC-22 and HFC-134a have increased substantially over the past two decades. Emissions of HFC-134a are consistently higher compared with the United Nations Framework Convention on Climate Change (UNFCCC) inventory since 2000, by 60% more in recent years (2009-2012). Apart from these decadal emission constraints, we also quantify recent seasonal emission patterns showing that summertime emissions of HCFC-22 and HFC-134a are two to three times higher than wintertime emissions. This unforeseen large seasonal variation indicates that unaccounted mechanisms controlling refrigerant gas emissions are missing in the existing inventory estimates. Possible mechanisms enhancing refrigerant losses in summer are (i) higher vapor pressure in the sealed compartment of the system at summer high temperatures and (ii) more frequent use and service of refrigerators and air conditioners in summer months. Our results suggest that engineering (e.g., better temperature/vibration-resistant system sealing and new system design of more compact/efficient components) and regulatory (e.g., reinforcing system service regulations) steps to improve containment of these gases from working devices could effectively reduce their release to the atmosphere.

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.

Constraints on carbon monoxide emissions based on tall tower measurements in the US Upper Midwest.

We interpret a full year of high-frequency CO measurements from a tall tower in the U.S. Upper Midwest with a time-reversed Lagrangian Particle Dispersion Model (STILT LPDM) and an Eulerian chemical transport model (GEOS-Chem CTM) to develop top-down constraints on U.S. CO sources in 2009. Our best estimate is that anthropogenic CO emissions in the U.S. Upper Midwest in 2009 were 2.9 Tg, 61% lower (a posteriori scale factor of 0.39) than our a priori prediction based on the U.S. EPA's National Emission Inventory for 2005 (NEI 2005). If the same bias applies across the contiguous U.S., the inferred CO emissions are 26 Tg/y, compared to the a priori estimate of 66 Tg/y. This discrepancy is significantly greater than would be expected based solely on emission decreases between 2005 and 2009 (EPA estimate: 23% decrease). Model transport error is an important source of uncertainty in the analysis, and we employ an ensemble of sensitivity runs using multiple meteorological data sets and model configurations to assess its impact on our results. A posteriori scale factors for the U.S. anthropogenic CO source from these sensitivity runs range from 0.22 to 0.64, corresponding to emissions of 1.6-4.8 Tg/y for the U.S. Upper Midwest and 15-42 Tg/y for the contiguous U.S. The data have limited sensitivity for constraining biomass + biofuel burning emissions and photochemical CO production from precursor organic compounds. Our finding of a NEI 2005 overestimate of CO emissions is consistent with recent assessments for individual cities and with earlier analyses based on the NEI 1999, implying the need for a better mechanism for refining such bottom-up emission estimates in response to top-down constraints.