Underestimation of Thermogenic Methane Emissions in New York City.

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.

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.

Carbon Monoxide Emissions from the Washington, DC, and Baltimore Metropolitan Area: Recent Trend and COVID-19 Anomaly.

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.

The Impact of COVID-19 on CO2 Emissions in the Los Angeles and Washington DC/Baltimore Metropolitan Areas.

Responses to COVID-19 have resulted in unintended reductions of city-scale carbon dioxide (CO2) emissions. Here, we detect and estimate decreases in CO2 emissions in Los Angeles and Washington DC/Baltimore during March and April 2020. We present three lines of evidence using methods that have increasing model dependency, including an inverse model to estimate relative emissions changes in 2020 compared to 2018 and 2019. The March decrease (25%) in Washington DC/Baltimore is largely supported by a drop in natural gas consumption associated with a warm spring whereas the decrease in April (33%) correlates with changes in gasoline fuel sales. In contrast, only a fraction of the March (17%) and April (34%) reduction in Los Angeles is explained by traffic declines. Methods and measurements used herein highlight the advantages of atmospheric CO2 observations for providing timely insights into rapidly changing emissions patterns that can empower cities to course-correct CO2 reduction activities efficiently.

Wintertime CO2, CH4, and CO Emissions Estimation for the Washington, DC-Baltimore Metropolitan Area Using an Inverse Modeling Technique.

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 CO2, CH4, 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 CO2, 24% for CH4, 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.

Tower-Based Greenhouse Gas Measurement Network Design---The National Institute of Standards and Technology North East Corridor Testbed.

The North-East Corridor (NEC) Testbed project is the 3rd of three NIST (National Institute of Standards and Technology) greenhouse gas emissions testbeds designed to advance greenhouse gas measurements capabilities. A design approach for a dense observing network combined with atmospheric inversion methodologies is described. The Advanced Research Weather Research and Forecasting Model with the Stochastic Time-Inverted Lagrangian Transport model were used to derive the sensitivity of hypothetical observations to surface greenhouse gas emissions (footprints). Unlike other network design algorithms, an iterative selection algorithm, based on a k-means clustering method, was applied to minimize the similarities between the temporal response of each site and maximize sensitivity to the urban emissions contribution. Once a network was selected, a synthetic inversion Bayesian Kalman filter was used to evaluate observing system performance. We present the performances of various measurement network configurations consisting of differing numbers of towers and tower locations. Results show that an overly spatially compact network has decreased spatial coverage, as the spatial information added per site is then suboptimal as to cover the largest possible area, whilst networks dispersed too broadly lose capabilities of constraining flux uncertainties. In addition, we explore the possibility of using a very high density network of lower cost and performance sensors characterized by larger uncertainties and temporal drift. Analysis convergence is faster with a large number of observing locations, reducing the response time of the filter. Larger uncertainties in the observations implies lower values of uncertainty reduction. On the other hand, the drift is a bias in nature, which is added to the observations and, therefore, biasing the retrieved fluxes.

Background conditions for an urban greenhouse gas network in the Washington, D.C. and Baltimore metropolitan region.

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.

Assessment of Planetary Boundary Layer parametrizations and urban heat island comparison: Impacts and implications for tracer transport.

Accurate simulation of planetary boundary layer height (PBLH) is key to greenhouse gas emission estimation, air quality prediction and weather forecasting. This manuscript describes an extensive performance assessment of several Weather Research and Forecasting (WRF) model configurations where novel observations from ceilometers, surface stations and a flux tower were used to study their ability to reproduce planetary boundary layer heights (PBLH) and the impact that the urban heat island (UHI) has on the modeled PBLHs in the greater Washington, D.C. area. In addition, CO2 measurements at two urban towers were compared to tracer transport simulations. The ensemble of models used 4 PBL parameterizations, 2 sources of initial and boundary conditions and 1 configuration including the building energy parameterization (BEP) urban canopy model. Results have shown low biases over the whole domain and period for wind speed, wind direction and temperature with no drastic differences between meteorological drivers. We find that PBLH errors are mostly positively correlated with sensible heat flux errors, and that modeled positive UHI intensities are associated with deeper modeled PBLs over the urban areas. In addition, we find that modeled PBLHs are typically biased low during nighttime for most of the configurations with the exception of those using the MYNN parametrization and that these biases directly translate to tracer biases. Overall, the configurations using MYNN scheme performed the best, reproducing the PBLH and CO2 molar fractions reasonably well during all hours, thus opening the door to future nighttime inverse modeling.

Greenhouse gas observations from the Northeast Corridor tower network.

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).

Intercomparison of atmospheric trace gas dispersion models: Barnett Shale case study.

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.

Microencapsulation of phosphogypsum into a sulfur polymer matrix: physico-chemical and radiological characterization.

The aim of this work is to prepare a new type of phosphogypsum-sulfur polymer cements (PG-SPC) to be utilised in the manufacture of building materials. Physico-chemical and radiological characterization was performed in phosphogypsum and phosphogypsum-sulfur polymer concretes and modeling of exhalation rates has been also carried out. An optimized mixture of the materials was obtained, the solidified material with optimal mixture (sulfur/phosphogypsum=1:0.9, phosphogypsum dosage=10-40 wt.%) results in highest strength (54-62 MPa) and low total porosity (2.8-6.8%). The activity concentration index (I) in the PG-SPC is lower than the reference value in the most international regulations and; therefore, these cements can be used without radiological restrictions in the manufacture of building materials. Under normal conditions of ventilation, the contribution to the expected radon indoor concentration in a standard room is below the international recommendations, so the building materials studied in this work can be applied to houses built up under normal ventilation conditions. Additionally, and taking into account that the PG is enriched in several natural radionuclides as (226)Ra, the leaching experiments have demonstrated that environmental impact of the using of SPCs cements with PG is negligible.