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Uncertainty Quantification of Global Net Methane Emissions From Terrestrial Ecosystems Using a Mechanistically Based Biogeochemistry Model

Quantification of methane (CH4) emissions from wetlands and its sinks from uplands is still fraught with large uncertainties. Here, a methane biogeochemistry model was revised, parameterized, and verified for various wetland ecosystems across the globe. The model was then extrapolated to the global scale to quantify the uncertainty induced from four different types of uncertainty sources including parameterization, wetland type distribution, wetland area distribution, and meteorological input. We found that global wetland emissions are 212 ± 62 and 212 ± 32 Tg CH4 year−1 (1Tg = 1012 g) due to uncertain parameters and wetland type distribution, respectively, during 2000–2012. Using two wetland distribution data sets and three sets of climate data, the model simulations indicated that the global wetland emissions range from 186 to 212 CH4 year−1 for the same period. The parameters were the most significant uncertainty source. After combining the global methane consumption in the range of −34 to −46 Tg CH4 year−1, we estimated that the global net land methane emissions are 149–176 Tg CH4 year−1 due to uncertain wetland distribution and meteorological input. Spatially, the northeast United States and Amazon were two hotspots of methane emission, while consumption hotspots were in the Eastern United States and eastern China. During 1950–2016, both wetland emissions and upland consumption increased during El Niño events and decreased during La Niña events. This study highlights the need for more in situ methane flux data, more accurate wetland type, and area distribution information to better constrain the model uncertainty.

wetland methane emission↗

The Challenges of Measuring Methane from Space with a Lidar

The global and regional quantification of methane fluxes and identification of its sources and sinks has been highlighted as one of the goals of the NASA 2017 Earth Science Decadal Survey. Detecting methane from space and airborne platforms with an active (laser) remote sensing instrument presents several unique technology and measurement challenges. The instrument must have a single frequency, narrow-linewidth light source, and photon-sensitive detector at the right spectral region to make continuous measurements from orbit, day and night, all seasons and at all latitudes. It must have a high signal to noise ratio and must be relatively immune to biases from aerosol/cloud scattering, spectroscopic and meteorological data uncertainties, and instrument systematic errors. At Goddard Space Flight Center (GSFC), in collaboration with industry, we have developed an airborne instrument to measure methane. Our instrument is a nadir-viewing lidar that uses Integrated Path Differential Absorption (IPDA), to measure methane near 1.65 µm. We sample the absorption line using multiple wavelengths from a narrow linewidth laser source and a sensitive photodetector. This measurement approach provides maximum information content about the CH4 column, and minimizes biases in the XCH4 retrieval. In this paper, we will review our progress to date and discuss the technology challenges, options and tradeoffs to measure methane from space and airborne platforms.

airborne instruments↗

Evaluation of GHGSat Methane Emission Estimations of South Side Landfill in Indianapolis, Indiana

As global methane (CH4) continues to grow, accurate quantification of CH4 emission sources has become a high priority for climate management. Urban CH4 emissions in the US could potentially account close to 20% of the national CH4 anthropogenic emissions. While isolated insitu urban CH4 emissions quantification projects have been successful, they require sophisticated planning and prolonged analyses. Such studies are imperative, but they cannot easily operate in every city. An ability to quantify the magnitude of CH4 point sources in a variety of cities with a satellite could support wide scale urban CH4 emissions quantification. Whole-earth scanning satellite instruments such as the TROPOMI and GOSAT are too coarse and noisy to provide meaningful measurements over cities with mid-strength emissions and most point-source emissions in general. It may be possible to address this deficiency utilizing a product with the high spatial resolution of 30-50 m from a private company GHGSat Inc. These sensors are specifically designed to identify and quantify CH4 emissions from diverse types of point sources of varying intensities. In this work we analyze a year (05/2023-05/2024) of GHGSat scans over South Side Landfill in downtown Indianapolis, Indiana and assess the instruments’ accuracy and precision with respect to prior estimations. The results indicate that the data are helpful for estimating landfill’s emissions (~750 kg/hr ± 200 kg/hr) over months-to-a-year time frame but may not be appropriate for identifying daily or even seasonal variations with any trustable degree of certainty, at least not in an urban environment.

Nikolay Balashov↗

Crosscutting Airborne Remote Sensing Technologies for Oil and Gas and Earth Science Applications

Airborne imaging spectroscopy has evolved dramatically since the 1980s as a robust remote sensing technique used to generate 2-dimensional maps of surface properties over large spatial areas. Traditional applications for passive airborne imaging spectroscopy include interrogation of surface composition, such as mapping of vegetation diversity and surface geological composition. Two recent applications are particularly relevant to the needs of both the oil and gas as well as government sectors: quantification of surficial hydrocarbon thickness in aquatic environments and mapping atmospheric greenhouse gas components. These techniques provide valuable capabilities for petroleum seepage in addition to detection and quantification of fugitive emissions. New empirical data that provides insight into the source strength of anthropogenic methane will be reviewed, with particular emphasis on the evolving constraints enabled by new methane remote sensing techniques. Contemporary studies attribute high-strength point sources as significantly contributing to the national methane inventory and underscore the need for high performance remote sensing technologies that provide quantitative leak detection. Imaging sensors that map spatial distributions of methane anomalies provide effective techniques to detect, localize, and quantify fugitive leaks. Airborne remote sensing instruments provide the unique combination of high spatial resolution (<1 m) and large coverage required to directly attribute methane emissions to individual emission sources. This capability cannot currently be achieved using spaceborne sensors. In this study, results from recent NASA remote sensing field experiments focused on point-source leak detection, will be highlighted. This includes existing quantitative capabilities for oil and methane using state-of-the-art airborne remote sensing instruments. While these capabilities are of interest to NASA for assessment of environmental impact and global climate change, industry similarly seeks to detect and localize leaks of both oil and methane across operating fields. In some cases, higher sensitivities desired for upstream and downstream applications can only be provided by new airborne remote sensing instruments tailored specifically for a given application. There exists a unique opportunity for alignment of efforts between commercial and government sectors to advance the next generation of instruments to provide more sensitive leak detection capabilities, including those for quantitative source strength determination.

hyperspectral↗

Quantification of CO2 and CH4 emissions over Sacramento, California, based on divergence theorem using aircraft measurements

Emission estimates of carbon dioxide (CO2) and methane (CH4) and the meteorological factors affecting them are investigated over Sacramento, California, using an aircraft equipped with a cavity ring-down greenhouse gas sensor as part of the Alpha Jet Atmospheric eXperiment (AJAX) project. To better constrain the emission fluxes, we designed flights in a cylindrical pattern and computed the emission fluxes from two flights using a kriging method and Gauss’s divergence theorem. Differences in wind treatment and assumptions about background concentrations affect the emission estimates by a factor of 1.5 to 7. The uncertainty is also impacted by meteorological conditions and distance from the emission sources. The vertical layer averaging affects the flux estimate, but the choice of raw wind or mass-balanced wind is more important than the thickness of the vertical averaging for massbalanced wind for both urban and local scales. The importance of vertical mass transfer for flux estimates is examined, and the difference in the total emission estimate with and without vertical mass transfer is found to be small, especially at the local scale. The total flux estimates accounting for the entire circumference are larger than those based solely on measurements made in the downwind region. This indicates that a closed-shape flight profile can better contain total emissions relative to a one-sided curtain flight because most cities have more than one point source and wind direction can change with time and altitude. To reduce the uncertainty of the emission estimate, it is important that the sampling strategy account not only for known source locations but also possible unidentified sources around the city. Our results highlight that aircraft-based measurements using a closed-shape flight pattern are an efficient and useful strategy for identifying emission sources and estimating local- and city-scale greenhouse gas emission fluxes.

Ju-Mee Ryoo↗

Rapid Expansion of Northern Peatlands and Doubled Estimate of Carbon Storage

Northern peatlands are an integral part of the global carbon cycle—a strong sink of atmospheric carbon dioxide and source of methane. Increasing anthropogenic carbon dioxide and methane in the atmosphere are thought to strongly impact these environments, and yet, peatlands are not routinely included in Earth system models. Here we present a quantification of the sink and stock of northern peat carbon from the last glacial period through the pre-industrial period. Additional data and new algorithms for reconstructing the history of peat carbon accumulation and the timing of peatland initiation increased the estimate of total northern peat carbon stocks from 545 Gt to 1,055 Gt of carbon. Further, the post-glacial increases in peatland initiation rate and carbon accumulation rate are more abrupt than previously reported. Peatlands have been a strong carbon sink throughout the Holocene, but the atmospheric partial pressure of carbon dioxide has been relatively stable over this period. While processes such as permafrost thaw and coral reef development probably contributed some additional carbon to the atmosphere, we suggest that deep ocean upwelling was the most important mechanism for balancing the peatland sink and maintaining the observed stability.

Nichols, Jonathan E.↗

Determination of Combustion Product Radicals in a Hydrocarbon Fueled Rocket Exhaust Plume

The identification of metallic effluent materials in a rocket engine exhaust plume indicates the health of the engine. Since 1989, emission spectroscopy of the plume of the Space Shuttle Main Engine (SSME) has been used for ground testing at NASA's Stennis Space Center (SSC). This technique allows the identification and quantification of alloys from the metallic elements observed in the plume. With the prospect of hydrocarbon-fueled rocket engines, such as Rocket Propellant 1 (RP-1) or methane (CH4) fueled engines being considered for use in future space flight systems, the contributions of intermediate or final combustion products resulting from the hydrocarbon fuels are of great interest. The effect of several diatomic molecular radicals, such as Carbon Dioxide , Carbon Monoxide, Molecular Carbon, Methylene Radical, Cyanide or Cyano Radical, and Nitric Oxide, needs to be identified and the effects of their band systems on the spectral region from 300 nm to 850 nm determined. Hydrocarbon-fueled rocket engines will play a prominent role in future space exploration programs. Although hydrogen fuel provides for higher engine performance, hydrocarbon fuels are denser, safer to handle, and less costly. For hydrocarbon-fueled engines using RP-1 or CH4 , the plume is different from a hydrogen fueled engine due to the presence of several other species, such as CO2, C2, CO, CH, CN, and NO, in the exhaust plume, in addition to the standard H2O and OH. These species occur as intermediate or final combustion products or as a result of mixing of the hot plume with the atmosphere. Exhaust plume emission spectroscopy has emerged as a comprehensive non-intrusive sensing technology which can be applied to a wide variety of engine performance conditions with a high degree of sensitivity and specificity. Stennis Space Center researchers have been in the forefront of advancing experimental techniques and developing theoretical approaches in order to bring this technology to a more mature stage.

Langford, Lester A.↗

Spatiotemporal Methane Emissions from Global Lakes and Reservoirs

Inland aquatic systems, such as lakes and reservoirs, contribute substantially to global methane (CH4) emissions; yet are among the most uncertain components of the total CH4 budget. Lakes and reservoirs have received recent attention as they may generate high CH4 fluxes. Improved quantification of these CH4 fluxes, particularly their spatiotemporal distribution, is key to realistically incorporating them in CH4 modeling and budget studies. Here we report on a new global, gridded (0.25° lat × 0.25° lon) study of lake and reservoir CH4 emissions, accounting for new knowledge regarding lake and reservoir areal extent and distribution, and spatiotemporal emission patterns influenced by diurnal variability, temperature-dependent seasonality, satellite-derived freeze-thaw dynamics, and eco-climatic and physical CH4-centric type classification. The results of this new data set comprise daily CH4 emissions from lake and reservoirs throughout the full annual cycle and are tightly anchored to field observations, in situ measurements, and remote-sensing observations. Results show that reservoirs cover 297 × 103 km2 globally and emit 10.1 Tg CH4 yr-1 from diffusive (1.2 Tg CH4 yr-1) and ebullitive (8.9 Tg CH4 yr-1) emission pathways. On a global scale, CH4 emitting areas of lakes cover 1853 × 103 km2 and emit 37.1 Tg CH4 yr-1 from diffusive (17.1 Tg CH4 yr-1) and ebullitive (23.0 Tg CH4 yr-1) emission pathways and an additional ebullition flux of 5.2 Tg CH4 yr-1 upon ice-melt due to the accumulation of bubbles during the freeze period. This analysis of lakes and reservoir CH4 emission addresses multiple gaps and uncertainties in previous studies and represents an important contribution to studies of the global CH4 budget. The new data sets and methodologies from this study provide a framework to better understand and model the current and future role of lakes and reservoirs in the global CH4 budget and to guide efforts to mitigate inland aquatic system CH4 emissions. This presentation will describe the methodologies applied and the major results of this study focusing on the spatiotemporal distribution of lake and reservoir type classification, processes driving lake and reservoir emission seasonality, and the contribution of individual lake and reservoir types to the annual cycle of inland aquatic CH4 emissions.

Spatiotemporal↗

In-Situ Reaction Monitoring for Lunar Applications Utilizing a Single Quadrupole Residual Gas Analyzer

With a revived focus to create a permeant presence on the moon and in preparation for future Mars exploration, it is imperative that all re-sources are utilized to their fullest potential. In-Situ Resource Utilization (ISRU) will be critical for future mission success as it would enable independent operation of missions while minimally relying on the complex supply chain created between the Earth, moon and Mars. One of the most critical resources that have been identified for ISRU is the creation of liquid oxygen (O2) for not only breathable air, but also for rocket fuel. On the moon and potentially Mars, one of the most O2 rich resources is in the presence of regolith. Although there are numerous minerals within regolith and various processes to extract O2, this is not the scope of this paper. Since the O2 extraction method can vary, a critical standardized analytical method is needed to verify O2 (or oxygenated precursor compounds) for extraction efficiency and purity. Our group utilizes a modified consumer off-the-shelf (COTS), Residual Gas Analyzer (RGA) Single Quadrupole Mass Spectrometer (QMS). Due to the current field mission requirements, the gas analysis module will need to rely only on mass-to-charge ratios (m/z) and peak intensities to differentiate and quantitate targeted gas-phase reactants or products, i.e. carbon monoxide (CO), carbon dioxide (CO2), methane (CH4) and hydrogen (H2). However, due to solar wind implanted volatiles and various other compounds present in lunar regolith, such as nitrogen (N2), helium (He), and deuterium (D2), deconvolution and quantification of isobaric compounds becomes quite difficult. Specifically, the presence of N2 makes quantification of CO, an oxygenated precursor, difficult due to both compounds having a peak at m/z 28. Approaches to differentiate isobaric components: Initially, the solution to overcome isobaric overlap was to use isotopic ratios, particularly be-tween carbon-13 and nitrogen-15. Although limited literature discuss isotopic composition and attempt to quantify the ratios, variation is particularly high and limited to a few lunar regolith samples. The following were identified as potential approaches to quantify isobaric species, N2 and CO, using our RGA. Threshold Ionization. CO and N2 both have peaks at m/z 28, but only N2 is capable of producing a peak at m/z 7. While a N2 peak at m/z 7 is generally rare, instrument parameters can be optimized in order to maximize the peak intensity. Typically a standard ionization energy of 70 eV is used to monitor a batch process and would produce reliable results for a majority of the reactants or products that we are interested in quantifying. However, to analyze the rare molecular fragment of N2 (N2+ at m/z 7), a different ionization energy may be beneficial. Threshold Ionization Mass Spectrometry (TIMS) will be explored to optimize the N2+ peak at m/z 7 by varying parameters such as ionization energy and pressure. Therefore, a quantitative value at m/z 7 will be used to determine the product gas concentration of N2, which will be subtracted from the total concentration determined at m/z 28 enabling us to approximate the amount of CO. Secondary Detector (infrared gas detector, IR). Another approach to quantitate and differentiate be-tween isobaric components is to leverage alternative modes of detection. Unlike mass spectrometry, which generally uses a separation step prior to analysis (i.e. gas chromatography), IR produces energy that is specifically absorbed depending on the bond and configuration of the molecule. This technique could be leveraged since it is generally only active on non-symmetric molecules, i.e. CO. Utilizing concentrations of CO determined from another detector could help correct concentrations of CO obtained from the QMS. However, the inclusion of another detector adds additional mission requirements, such as power, software changes and avionics updates that add additional cost and schedule requirements.

mass spectrometry↗

In-Situ Reaction Monitoring for Lunar Applications Utilizing a Single Quadrupole Residual Gas Analyzer

With a revived focus to create a permanent presence on the moon and in preparation for future Mars exploration, it is imperative that all resources are utilized to their fullest potential.[1] In-Situ Resource Utilization (ISRU) will be critical for future mission success as it would enable independent operation of missions while minimally relying on the complex supply chain created between the Earth, moon and Mars. One of the most critical resources that have been identified for ISRU is the creation of liquid oxygen(LO2) for not only breathable air, but also for rocket propellant. On the moon and potentially Mars, one of the most O2 rich resources is in the presence of regolith.[2],[3] Although there are numerous minerals within regolith and various processes to extract O2,this is not the scope of this paper. Since the O2 extraction method can vary, a critical standardized analytical method is needed to verify O2(or oxygenated precursor compounds) for extraction efficiency and purity. Our group utilizes a modified consumer off-the-shelf (COTS), Residual Gas Analyzer (RGA) Single Quadrupole Mass Spectrometer (QMS). Due to the current field mission requirements, the gas analysis module will need to rely only on mass-to-charge ratios (m/z) and peak intensities to differentiate and quantitate targeted gas-phase reactants or products, i.e. carbon monoxide(CO), carbon dioxide (CO2), methane (CH4) and hydrogen (H2). However, due to solar wind implanted volatiles and various other compounds present in lunar regolith, such as nitrogen (N2), helium (He), and deuterium (D2), deconvolution and quantification of isobaric compounds becomes quite difficult. Specifically, the presence of N2 makes quantification of CO, an oxygenated precursor, difficult due to both compounds having a peak at m/z 28.

Mass Spectrometry↗

Pulling Results Out of Thin Air: Four Years of Ozone and Greenhouse Gas Measurements by the Alpha Jet Atmospheric Experiment (AJAX)

The Alpha Jet Atmospheric eXperiment (AJAX) has been measuring atmospheric ozone, carbon dioxide, methane and meteorological parameters from near the surface to 8000 m since January 2011. The main goals are to study photochemical ozone production and the impacts of extreme events on western US air quality, provide data to support satellite observations and aid in the quantification of emission sources e.g. wildfires, urban outflow, diary and oil and gas. The aircraft is based at Moffett Field and flies multiple times a month to sample vertical profiles at selected sites in California and Nevada, providing long-term data records at these sites. AJAX is also uniquely positioned to launch with short notice sampling flights in rapid response to extreme events e.g. the 2013 Yosemite Rim fire. This talk will focus on the impacts of vertical transport on surface air quality, and investigation of emission sources from diaries and wildfires.

AJAX↗

Quantifying Methane Leak Emissions by Fused Airborne Imaging Spectroscopy with in Situ Surface Mobile and Airborne Observations of a California Producing Oil Field

Methane (CH4) emission budgets remain uncertain and are projected to grow as oil and gas production from short-lived wells increases and their subsequent transport through aging gas distribution networks. Orders-of-magnitude variations in temporal, spatial, and emission scales present a key challenge to leak detection and quantification. Also, the probability distributions for large and stochastic, leaky systems such as geological reservoirs (by natural migration-seeps) and petroleum production from those reservoirs remain largely unknown, needed to address current approach limitations. The scale of many petroleum systems favors remote sensing, but the sensitivity of such systems often precludes detection of weak emissions. Consequently, an accurate evaluation requires that the relative contribution from the emission "tails" of small leaks also be quantified, which is best carried out using high-sensitivity in situ methods. Fusion of remote sensing and in situ approaches leverages complementary capabilities to address these limitations. We show results from mobile surface (AMOG) and airborne in situ (AJAX) and thermal-infrared (TIR) hyperspectral imaging spectroscopy (Mako) data applied to a producing oil field in the California Central Valley near Bakersfield. AMOG is an automobile-based mobile lab that measures 13 trace gases, aerosol size distributions and vertical profiles, 3D winds and other meteorology, and atmospheric column measurements by solar spectroscopy at highway speeds. AJAX measures 5 trace gases and 3D winds at ~140 m/s. Mako is a broad-area TIR imaging spectrometer that can discriminate multiple gases present in each pixel acquired. In situ-derived, total field emissions were 31±16 Gg/yr CH4. This was compared with Mako-derived emissions from all plumes identified across the study site. We found that super-emitters were not the dominant emissions mode and the spatial pattern of plume locations from production infrastructure was correlated to geological structures.

Leifer, Ira↗

Quantitative Measurements of CH* Concentration in Normal Gravity and Microgravity Coflow Laminar Diffusion Flames

With the conclusion of the SLICE campaign aboard the ISS in 2012, a large amount of data was made available for the analysis of the effect of microgravity on laminar coflow diffusion flames. Previous work focused on the study of sooty flames in microgravity as well as the ability of numerical models to predict its formation in a simplified buoyancy-free environment. The current work shifts the investigation to soot-free flames, putting an emphasis on the chemiluminescence emission from electronically excited CH (CH*). This radical species is of significant interest in combustion studies: it has been shown that the CH* spatial distribution is indicative of the flame front position and, given the relatively simple diagnostic involved with its measurement, several works have been done trying to understand the ability of CH* chemiluminescence to predict the total and local flame heat release rate. In this work, a subset of the SLICE nitrogen-diluted methane flames has been considered, and the effect of fuel and coflow velocity on CH* concentration is discussed and compared with both normal gravity results and numerical simulations. Experimentally, the spectral characterization of the DSLR color camera used to acquire the flame images allowed the signal collected by the blue channel to be considered representative of the CH* emission centered around 431 nm. Due to the axisymmetric flame structure, an Abel deconvolution of the line-of-sight chemiluminescence was used to obtain the radial intensity profile and, thanks to an absolute light intensity calibration, a quantification of the CH* concentration was possible. Results show that, in microgravity, the maximum flame CH* concentration increases with the coflow velocity, but it is weakly dependent on the fuel velocity; normal gravity flames, if not lifted, tend to follow the same trend, albeit with different peak concentrations. Comparisons with numerical simulations display reasonably good agreement between measured and computed flame lengths and radii, and it is shown that the integrated CH* emission scales proportionally to the computed total heat release rate; the two-dimensional CH* spatial distribution, however, does not appear to be a good marker for the local heat release rate.

microgravity↗

Quantitative Measurements of Electronically Excited CH Concentration in Normal Gravity and Microgravity Coflow Laminar Diffusion Flames

With the conclusion of the SLICE campaign aboard the ISS in 2012, a large amount of data was made available for the analysis of the effect of microgravity on laminar coflow diffusion flames. Previous work focused on the study of sooty flames in microgravity as well as the ability of numerical models to predict its formation in a simplified buoyancy-free environment. The current work shifts the investigation to soot-free flames, putting an emphasis on the chemiluminescence emission from electronically excited CH (CH*). This radical species is of significant interest in combustion studies: it has been shown that the electronically excited CH spatial distribution is indicative of the flame front position and, given the relatively simple diagnostic involved with its measurement, several works have been done trying to understand the ability of electronically excited CH chemiluminescence to predict the total and local flame heat release rate. In this work, a subset of the SLICE nitrogen-diluted methane flames has been considered, and the effect of fuel and coflow velocity on electronically excited CH concentration is discussed and compared with both normal gravity results and numerical simulations. Experimentally, the spectral characterization of the DSLR color camera used to acquire the flame images allowed the signal collected by the blue channel to be considered representative of the electronically excited CH emission centered around 431 nm. Due to the axisymmetric flame structure, an Abel deconvolution of the line-of-sight chemiluminescence was used to obtain the radial intensity profile and, thanks to an absolute light intensity calibration, a quantification of the electronically excited CH concentration was possible. Results show that, in microgravity, the maximum flame electronically excited CH concentration increases with the coflow velocity, but it is weakly dependent on the fuel velocity; normal gravity flames, if not lifted, tend to follow the same trend, albeit with different peak concentrations. Comparisons with numerical simulations display reasonably good agreement between measured and computed flame lengths and radii, and it is shown that the integrated electronically excited CH emission scales proportionally to the computed total heat release rate; the two-dimensional electronically excited CH spatial distribution, however, does not appear to be a good marker for the local heat release rate.

chemiluminescence↗