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Methane emissions from the U.S. oil and natural gas supply chain were estimated by using ground-based, facility-scale measurements and validated with aircraft observations in areas accounting for ~30% of U.S. gas production. When scaled up nationally, our facility-based estimate of 2015 supply chain emissions is 13 ± 2 teragrams per year, equivalent to 2.3% of gross U.S. gas production. This value is ~60% higher than the U.S. Environmental Protection Agency inventory estimate, likely because existing inventory methods miss emissions released during abnormal operating conditions. Methane emissions of this magnitude, per unit of natural gas consumed, produce radiative forcing over a 20-year time horizon comparable to the CO2 from natural gas combustion. Substantial emission reductions are feasible through rapid detection of the root causes of high emissions and deployment of less failure-prone systems. [ABSTRACT FROM AUTHOR]

With China's proposed carbon reduction goals, many carbon monitoring pilot city projects have been launched, involving greenhouse gas (GHG) inverse estimate analysis based on GHG observations. For the evaluation of emissions estimates in a targeted urban area, the contributions of extra-urban fluxes on urban GHG observations must be excluded, especially for core cities within urban agglomerations, which face more severe emission interference from adjacent cities. In this study, we quantified the impact of external emissions on urban carbon dioxide (CO 2 ) mole fraction observations across different seasons in the central downtown area of Zhengzhou, a core city of the Central Plains Urban Agglomeration in China. Results showed that 60% of the CO 2 enhancement from the 500-km square area including the city originated outside the core urban area in autumn and winter, predominantly originating from far-field sources (>50 km) in the northeast, west, and northwest of Zhengzhou. To design an optimal monitoring network that accurately accounts for CO 2 mole fractions entering the urban domain of interest, three different selection methods (distance, meteorological trajectory, and multiple regression) were used to select background station locations, and the resulting background values were evaluated through the application of observing system simulation experiments, including synthetic flux inverse estimate Results indicated that the background stations selected by meteorological trajectories more effectively captured CO 2 variability, introducing the smallest errors to inverse estimate flux (-8%). This study provides a valuable reference for designing background monitoring stations in dense urban agglomerations, thereby improving the accuracy of high-resolution urban GHG emission inverse estimates., Competing Interests: Declaration of Competing Interest ☒ The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper. ☐ The authors declare the following financial interests/personal relationships which may be considered as potential competing interests:, (Copyright © 2024. Published by Elsevier Inc.)

Recent studies have shown that methane emissions are underestimated by inventories in many US urban areas. This has important implications for climate change mitigation policy at the city, state, and national levels. Uncertainty in both the spatial distribution and sectoral allocation of urban emissions can limit the ability of policy makers to develop appropriately focused emission reduction strategies. Top-down emission estimates based on atmospheric greenhouse gas measurements can help to improve inventories and inform policy decisions. This study presents a new high-resolution (0.02 × 0.02°) methane emission inventory for New York City and its surrounding area, constructed using the latest activity data, emission factors, and spatial proxies. The new high-resolution inventory estimates of methane emissions for the New York-Newark urban area are 1.3 times larger than those for the gridded Environmental Protection Agency inventory. We used aircraft mole fraction measurements from nine research flights to optimize the high-resolution inventory emissions within a Bayesian inversion. These sectorally optimized emissions show that the high-resolution inventory still significantly underestimates methane emissions within the New York-Newark urban area, primarily because it underestimates emissions from thermogenic sources (by a factor of 2.3). This suggests that there remains a gap in our process-based understanding of urban methane emissions.

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.

Urban regions emit a large fraction of anthropogenic emissions of greenhouse gases (GHG) such as carbon dioxide (CO 2 ) and methane (CH 4 ) that contribute to modern-day climate change. As such, a growing number of urban policymakers and stakeholders are adopting emission reduction targets and implementing policies to reach those targets. Over the past two decades research teams have established urban GHG monitoring networks to determine how much, where, and why a particular city emits GHGs, and to track changes in emissions over time. Coordination among these efforts has been limited, restricting the scope of analyses and insights. Here we present a harmonized data set synthesizing urban GHG observations from cities with monitoring networks across North America that will facilitate cross-city analyses and address scientific questions that are difficult to address in isolation., (© 2022. The Author(s).)

We analyze airborne measurements of atmospheric CO concentration from 70 flights conducted over six years (2015-2020) using an inverse model to quantify the CO emissions from the Washington, DC, and Baltimore metropolitan areas. We found that CO emissions have been declining in the area at a rate of ≈-4.5 % a -1 since 2015 or ≈-3.1 % a -1 since 2016. In addition, we found that CO emissions show a "Sunday" effect, with emissions being lower, on average, than for the rest of the week and that the seasonal cycle is no larger than 16 %. Our results also show that the trend derived from the NEI agrees well with the observed trend, but that NEI daytime-adjusted emissions are ≈50 % larger than our estimated emissions. In 2020, measurements collected during the shutdown in activity related to the COVID-19 pandemic indicate a significant drop in CO emissions of 16 % relative to the expected emissions trend from the previous years, or 23 % relative to the mean of 2016 to February 2020. Our results also indicate a larger reduction in April than in May. Last, we show that this reduction in CO emissions was driven mainly by a reduction in traffic.

As city governments take steps towards establishing emissions reduction targets, the atmospheric research community is increasingly able to assist in tracking emissions reductions. Researchers have established systems for observing atmospheric greenhouse gases in urban areas with the aim of attributing greenhouse gas concentration enhancements (and thus, emissions) to the region in question. However, to attribute enhancements to a particular region, one must isolate the component of the observed concentration attributable to fluxes inside the region by removing the background, which is the component due to fluxes outside. In this study, we demonstrate methods to construct several versions of a background for our carbon dioxide and methane observing network in the Washington, DC and Baltimore, MD metropolitan region. Some of these versions rely on transport and flux models, while others are based on observations upwind of the domain. First, we evaluate the backgrounds in a synthetic data framework, then we evaluate against real observations from our urban network. We find that backgrounds based on upwind observations capture the variability better than model-based backgrounds, although care must be taken to avoid bias from biospheric carbon dioxide fluxes near background stations in summer. Model-based backgrounds also perform well when upwind fluxes can be modeled accurately. Our study evaluates different background methods and provides guidance determining background methodology that can impact the design of urban monitoring networks.

Since greenhouse gas mitigation efforts are mostly being implemented in cities, the ability to quantify emission trends for urban environments is of paramount importance. However, previous aircraft work has indicated large daily variability in the results. Here we use measurements of CO 2 , CH 4 , and CO from aircraft over 5 days within an inverse model to estimate emissions from the DC-Baltimore region. Results show good agreement with previous estimates in the area for all three gases. However, aliasing caused by irregular spatiotemporal sampling of emissions is shown to significantly impact both the emissions estimates and their variability. Extensive sensitivity tests allow us to quantify the contributions of different sources of variability and indicate that daily variability in posterior emissions estimates is larger than the uncertainty attributed to the method itself (i.e., 17% for CO 2 , 24% for CH 4 , and 13% for CO). Analysis of hourly reported emissions from power plants and traffic counts shows that 97% of the daily variability in posterior emissions estimates is explained by accounting for the sampling in time and space of sources that have large hourly variability and, thus, caution must be taken in properly interpreting variability that is caused by irregular spatiotemporal sampling conditions.

We present the organization, structure, instrumentation, and measurements of the Northeast Corridor greenhouse gas observation network. This network of tower-based in situ carbon dioxide and methane observation stations was established in 2015 with the goal of quantifying emissions of these gases in urban areas in the northeastern United States. A specific focus of the network is the cities of Baltimore, MD, and Washington, DC, USA, with a high density of observation stations in these two urban areas. Additional observation stations are scattered throughout the northeastern US, established to complement other existing urban and regional networks and to investigate emissions throughout this complex region with a high population density and multiple metropolitan areas. Data described in this paper are archived at the National Institute of Standards and Technology and can be found at https://doi.org/10.18434/M32126 (Karion et al., 2019)., Competing Interests: Competing interests. The authors declare that they have no conflict of interest.

Urban areas are increasingly recognized as an important source of methane (CH 4 ), but we have limited seasonally resolved observations of these regions. In this study, we quantify seasonal and annual urban CH 4 emissions over the Baltimore, Maryland, and Washington, DC metropolitan regions. We use CH 4 atmospheric observations from four tall tower stations and a Lagrangian particle dispersion model to simulate CH 4 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 CH 4 values. Forward simulations in winter, spring, and fall underestimate observed atmospheric CH 4 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 CH 4 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.

Urban areas contribute approximately three-quarters of fossil fuel derived CO 2 emissions, and many cities have enacted emissions mitigation plans. Evaluation of the effectiveness of mitigation efforts will require measurement of both the emission rate and its change over space and time. The relative performance of different emission estimation methods is a critical requirement to support mitigation efforts. Here we compare results of CO 2 emissions estimation methods including an inventory-based method and two different top-down atmospheric measurement approaches implemented for the Indianapolis, Indiana, U.S.A. urban area in winter. By accounting for differences in spatial and temporal coverage, as well as trace gas species measured, we find agreement among the wintertime whole-city fossil fuel CO 2 emission rate estimates to within 7%. This finding represents a major improvement over previous comparisons of urban-scale emissions, making urban CO 2 flux estimates from this study consistent with local and global emission mitigation strategy needs. The complementary application of multiple scientifically driven emissions quantification methods enables and establishes this high level of confidence and demonstrates the strength of the joint implementation of rigorous inventory and atmospheric emissions monitoring approaches.

Greenhouse gas emissions mitigation requires understanding the dominant processes controlling fluxes of these trace gases at increasingly finer spatial and temporal scales. Trace gas fluxes can be estimated using a variety of approaches that translate observed atmospheric species mole fractions into fluxes or emission rates, often identifying the spatial and temporal characteristics of the emission sources as well. Meteorological models are commonly combined with tracer dispersion models to estimate fluxes using an inverse approach that optimizes emissions to best fit the trace gas mole fraction observations. One way to evaluate the accuracy of atmospheric flux estimation methods is to compare results from independent methods, including approaches in which different meteorological and tracer dispersion models are used. In this work, we use a rich data set of atmospheric methane observations collected during an intensive airborne campaign to compare different methane emissions estimates from the Barnett Shale oil and natural gas production basin in Texas, USA. We estimate emissions based on a variety of different meteorological and dispersion models. Previous estimates of methane emissions from this region relied on a simple model (a mass balance analysis) as well as on ground-based measurements and statistical data analysis (an inventory). We find that in addition to meteorological model choice, the choice of tracer dispersion model also has a significant impact on the predicted down-wind methane concentrations given the same emissions field. The dispersion models tested often underpredicted the observed methane enhancements with significant variability (up to a factor of 3) between different models and between different days. We examine possible causes for this result and find that the models differ in their simulation of vertical dispersion, indicating that additional work is needed to evaluate and improve vertical mixing in the tracer dispersion models commonly used in regional trace gas flux inversions., Competing Interests: Competing interests. The authors declare that they have no conflict of interest.

The objective of the Indianapolis Flux Experiment (INFLUX) is to develop, evaluate and improve methods for measuring greenhouse gas (GHG) emissions from cities. INFLUX's scientific objectives are to quantify CO 2 and CH 4 emission rates at 1 km resolution with a 10% or better accuracy and precision, to determine whole-city emissions with similar skill, and to achieve high (weekly or finer) temporal resolution at both spatial resolutions. The experiment employs atmospheric GHG measurements from both towers and aircraft, atmospheric transport observations and models, and activity-based inventory products to quantify urban GHG emissions. Multiple, independent methods for estimating urban emissions are a central facet of our experimental design. INFLUX was initiated in 2010 and measurements and analyses are ongoing. To date we have quantified urban atmospheric GHG enhancements using aircraft and towers with measurements collected over multiple years, and have estimated whole-city CO 2 and CH 4 emissions using aircraft and tower GHG measurements, and inventory methods. Significant differences exist across methods; these differences have not yet been resolved; research to reduce uncertainties and reconcile these differences is underway. Sectorally- and spatially-resolved flux estimates, and detection of changes of fluxes over time, are also active research topics. Major challenges include developing methods for distinguishing anthropogenic from biogenic CO 2 fluxes, improving our ability to interpret atmospheric GHG measurements close to urban GHG sources and across a broader range of atmospheric stability conditions, and quantifying uncertainties in inventory data products. INFLUX data and tools are intended to serve as an open resource and test bed for future investigations. Well-documented, public archival of data and methods is under development in support of this objective., Competing Interests: Competing interests The authors have no competing interests to declare.

We report continuous surface observations of carbon dioxide (CO 2 ) and methane (CH 4 ) from the Los Angeles (LA) Megacity Carbon Project during 2015. We devised a calibration strategy, methods for selection of background air masses, calculation of urban enhancements, and a detailed algorithm for estimating uncertainties in urban-scale CO 2 and CH 4 measurements. These methods are essential for understanding carbon fluxes from the LA megacity and other complex urban environments globally. We estimate background mole fractions entering LA using observations from four "extra-urban" sites including two "marine" sites located south of LA in La Jolla (LJO) and offshore on San Clemente Island (SCI), one "continental" site located in Victorville (VIC), in the high desert northeast of LA, and one "continental/mid-troposphere" site located on Mount Wilson (MWO) in the San Gabriel Mountains. We find that a local marine background can be established to within ~1 ppm CO 2 and ~10 ppb CH 4 using these local measurement sites. Overall, atmospheric carbon dioxide and methane levels are highly variable across Los Angeles. "Urban" and "suburban" sites show moderate to large CO 2 and CH 4 enhancements relative to a marine background estimate. The USC (University of Southern California) site near downtown LA exhibits median hourly enhancements of ~20 ppm CO 2 and ~150 ppb CH 4 during 2015 as well as ~15 ppm CO 2 and ~80 ppb CH 4 during mid-afternoon hours (12:00-16:00 LT, local time), which is the typical period of focus for flux inversions. The estimated measurement uncertainty is typically better than 0.1 ppm CO 2 and 1 ppb CH 4 based on the repeated standard gas measurements from the LA sites during the last 2 years, similar to Andrews et al. (2014). The largest component of the measurement uncertainty is due to the single-point calibration method; however, the uncertainty in the background mole fraction is much larger than the measurement uncertainty. The background uncertainty for the marine background estimate is ~10 and ~15 % of the median mid-afternoon enhancement near downtown LA for CO 2 and CH 4 , respectively. Overall, analytical and background uncertainties are small relative to the local CO 2 and CH 4 enhancements; however, our results suggest that reducing the uncertainty to less than 5 % of the median mid-afternoon enhancement will require detailed assessment of the impact of meteorology on background conditions., Competing Interests: Competing interests. The authors declare that they have no conflict of interest.

Methane (CH 4 ) 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 CH 4 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 CH 4 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 CH 4 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 CH 4 observations. In addition, we find that CH 4 emissions from the North Slope of Alaska account for 24% of the total statewide flux of 1.74 ± 0.44 Tg CH 4 ( 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 CH 4 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 CH 4 fluxes than in process estimates. Lastly, we find that the seasonality of CH 4 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 CH 4 fluxes from the state.