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NASA NTRS2016

Cometary Origin of Atmospheric Methane Variations on Mars Unlikely

The detection of methane in the atmosphere of Mars was first reported in 2004. Since then a number of independent observations of methane have been reported, all showing temporal variability. Up until recently, the origin of methane was attributed to sources either indigenous to Mars or exogenous, where methane is a UV degradation byproduct of organics falling on to the surface. Most recently, a new hypothesis has been proposed that argues that the appearance and variation of methane are correlated with specific meteor events at Mars. Indeed, extraplanetary material can be brought to a planet when it passes through a meteoroid stream left behind by cometary bodies orbiting the Sun. This occurs repeatedly at specific times in a planet's year as streams tend to be fairly stable in space. In this paper, we revisit this latest hypothesis by carrying out a complete analysis of all available data on Mars atmospheric methane, including the very recent data not previously published, together with all published predicted meteor events for Mars. Whether we consider the collection of individual data points and predicted meteor events, whether we apply statistical analysis, or whether we consider different time spans between high methane measurements and the occurrence of meteor events, we find no compelling evidence for any correlation between atmospheric methane and predicted meteor events.

methane↗
NASA NTRS2013

Preindustrial to Present-Day Changes in Tropospheric Hydroxyl Radical and Methane Lifetime from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

We have analysed time-slice simulations from 17 global models, participating in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), to explore changes in present-day (2000) hydroxyl radical (OH) concentration and methane (CH4) lifetime relative to preindustrial times (1850) and to 1980. A comparison of modeled and observation-derived methane and methyl chloroform lifetimes suggests that the present-day global multi-model mean OH concentration is overestimated by 5 to 10% but is within the range of uncertainties. The models consistently simulate higher OH concentrations in the Northern Hemisphere (NH) compared with the Southern Hemisphere (SH) for the present-day (2000; inter-hemispheric ratios of 1.13 to 1.42), in contrast to observation-based approaches which generally indicate higher OH in the SH although uncertainties are large. Evaluation of simulated carbon monoxide (CO) concentrations, the primary sink for OH, against ground-based and satellite observations suggests low biases in the NH that may contribute to the high north–south OH asymmetry in the models. The models vary widely in their regional distribution of present-day OH concentrations (up to 34%). Despite large regional changes, the multi-model global mean (mass-weighted) OH concentration changes little over the past 150 yr, due to concurrent increases in factors that enhance OH (humidity, tropospheric ozone, nitrogen oxide (NOx) emissions, and UV radiation due to decreases in stratospheric ozone), compensated by increases in OH sinks (methane abundance, carbon monoxide and non-methane volatile organic carbon (NMVOC) emissions). The large inter-model diversity in the sign and magnitude of preindustrial to present-day OH changes (ranging from a decrease of 12.7% to an increase of 14.6%) indicate that uncertainty remains in our understanding of the long-term trends in OH and methane lifetime. We show that this diversity is largely explained by the different ratio of the change in global mean tropospheric CO and NOx burdens (Delta CO/Delta NOx, approximately represents changes in OH sinks versus changes in OH sources) in the models, pointing to a need for better constraints on natural precursor emissions and on the chemical mechanisms in the current generation of chemistry-climate models. For the 1980 to 2000 period, we find that climate warming and a slight increase in mean OH (3.5 +/- 2.2%) leads to a 4.3 +/- 1.9% decrease in the methane lifetime. Analysing sensitivity simulations performed by 10 models, we find that preindustrial to present-day climate change decreased the methane lifetime by about four months, representing a negative feedback on the climate system. Further, we analysed attribution experiments performed by a subset of models relative to 2000 conditions with only one precursor at a time set to 1860 levels. We find that global mean OH increased by 46.4 +/- 12.2% in response to preindustrial to present-day anthropogenic NOx emission increases, and decreased by 17.3 +/-2.3%, 7.6 +/- 1.5%, and 3.1 +/- 3.0% due to methane burden, and anthropogenic CO, and NMVOC emissions increases, respectively.

nitrogen oxides↗
NASA NTRS2020

Hiatus of wetland methane emissions associated with recent La Niña episodes in the Asian monsoon region

The variability of methane emissions from wetlands in the tropics and northern temperate regions can explain more than 70% of the interannual variation in global wetland methane emissions, which are largely driven by climate variability. We use climate reanalysis, remote sensing wetland area dataset and simulations from 11 land models contributing to Global Methane Budget to investigate the interannual variation and anomalies of wetland methane emissions in the Asian Monsoon region. Methane emissions in this region steadily increased over 2000–2012. However, abnormally low methane emissions were found in equatorial fully humid (Af), warm temperate winter dry (Cw), and warm temperate fully humid (Cf) Asian Monsoon climate sub-regions in 2008, 2009 and 2011, respectively. These spatially-shifting low emissions occurred simultaneously with observed wetland area shrinkage due to abnormally low precipitation. Interannual variability of wetland methane emissions in Asian Monsoon region are primarily driven by South Asian Monsoon system. However, the abnormally low emissions are related to strong La Niña events, and its accompanying effect of weakened East Asian Monsoon system and eastward Western Pacific subtropical high, which drives the shifting pattern of rainfall, and thus the spatial pattern of methane emission anomalies.

wetlands↗
NASA NTRS2020

The Global Methane Budget 2000–2017

Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. Atmospheric emissions and concentrations of CH4 continue to increase, making CH4 the second most important human-influenced greenhouse gas in terms of climate forcing, after carbon dioxide (CO2). The relative importance of CH4 compared to CO2 depends on its shorter atmospheric lifetime, stronger warming potential, and variations in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in reducing uncertainties in the atmospheric growth rate arise from the variety of geographically overlapping CH4 sources and from the destruction of CH4 by short-lived hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. Following Saunois et al. (2016), we present here the second version of the living review paper dedicated to the decadal methane budget, integrating results of top-down studies (atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up estimates (including process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). For the 2008–2017 decade, global methane emissions are estimated by atmospheric inversions (a top-down approach) to be 576 Tg CH4/yr (range 550–594, corresponding to the minimum and maximum estimates of the model ensemble). Of this total, 359 Tg CH4/yr or ∼ 60 % is attributed to anthropogenic sources, that is emissions caused by direct human activity (i.e. anthropogenic emissions; range 336–376 Tg CH4/yr or 50 %–65 %). The mean annual total emission for the new decade (2008–2017) is 29 Tg CH4/yr larger than our estimate for the previous decade (2000–2009), and 24 Tg CH4/yr larger than the one reported in the previous budget for 2003–2012 (Saunois et al., 2016). Since 2012, global CH4 emissions have been tracking the warmest scenarios assessed by the Intergovernmental Panel on Climate Change. Bottom-up methods suggest almost 30 % larger global emissions (737 Tg CH4/yr, range 594–881) than top-down inversion methods. Indeed, bottom-up estimates for natural sources such as natural wetlands, other inland water systems, and geological sources are higher than top-down estimates. The atmospheric constraints on the top-down budget suggest that at least some of these bottom-up emissions are overestimated. The latitudinal distribution of atmospheric observation-based emissions indicates a predominance of tropical emissions (∼ 65 % of the global budget, < 30° N) compared to mid-latitudes (∼ 30 %, 30–60° N) and high northern latitudes (∼ 4 %, 60–90° N). The most important source of uncertainty in the methane budget is attributable to natural emissions, especially those from wetlands and other inland waters. Some of our global source estimates are smaller than those in previously published budgets (Saunois et al., 2016; Kirschke et al., 2013). In particular wetland emissions are about 35 Tg CH4/yr lower due to improved partition wetlands and other inland waters. Emissions from geological sources and wild animals are also found to be smaller by 7 Tg CH4/yr by 8 Tg CH4/yr, respectively. However, the overall discrepancy between bottom-up and top-down estimates has been reduced by only 5 % compared to Saunois et al. (2016), due to a higher estimate of emissions from inland waters, highlighting the need for more detailed research on emissions factors. Priorities for improving the methane budget include (i) a global, high-resolution map of water-saturated soils and inundated areas emitting methane based on a robust classification of different types of emitting habitats; (ii) further development of process-based models for inland-water emissions; (iii) intensification of methane observations at local scales (e.g., FLUXNET-CH4 measurements) and urban-scale monitoring to constrain bottom-up land surface models, and at regional scales (surface networks and satellites) to constrain atmospheric inversions; (iv) improvements of transport models and the representation of photochemical sinks in top-down inversions; and (v) development of a 3D variational inversion system using isotopic and/or co-emitted species such as ethane to improve source partitioning.

methane budget↗
NASA NTRS2021

Half of global methane emissions come from highly variable aquatic ecosystem sources

Atmospheric methane is a potent greenhouse gas that plays a major role in controlling the Earth’s climate. The causes of the renewed increase of methane concentration since 2007 are uncertain given the multiple sources and complex biogeochemistry. Here, we present a metadata analysis of methane fluxes from all major natural, impacted and human-made aquatic ecosystems. Our revised bottom-up global aquatic methane emissions combine diffusive, ebullitive and/or plant-mediated fluxes from 15 aquatic ecosystems. We emphasize the high variability of methane fluxes within and between aquatic ecosystems and a positively skewed distribution of empirical data, making global estimates sensitive to statistical assumptions and sampling design. We find aquatic ecosystems contribute (median) 41% or (mean) 53% of total global methane emissions from anthropogenic and natural sources. We show that methane emissions increase from natural to impacted aquatic ecosystems and from coastal to freshwater ecosystems. We argue that aquatic emissions will probably increase due to urbanization, eutrophication and positive climate feedbacks and suggest changes in land-use management as potential mitigation strategies to reduce aquatic methane emissions.

aquatic ecosystem↗
DOE OSTI2024

Multi-Scale Integrated Monitoring System for Enhancing Methane Emission Detection, Quantification & Prediction

This report details the progress and findings of a comprehensive study on reviewing existing solutions, identifying technology gaps, and formulating an “all-in-one” integrated strategy for developing the next-generation multiscale methane monitoring and modeling platform, conducted under grant number DE-FE0032292. Co-led by Dr. David Ebert, Dr. Binbin Weng, and Dr. Chenghao Wang at the University of Oklahoma, the project’s goal was to develop an integrated approach for building this engineering platform to detect, quantify, and mitigate methane emissions across various temporal scale, spatial scales, and sectors. The planning grant study began with an extensive review of various methane sensing and monitoring technologies and systems, surveying over 100 technology providers globally. This review revealed the prevalence of optical methods over chemical methods in commercially available sensors, with Non-Dispersive Infrared (NDIR), Tunable Diode Laser Absorption Spectroscopy (TDLAS), and Optical Gas Imaging (OGI) cameras being the most prevalent options. A trend towards more advanced optical techniques was observed, driven by increased regulatory focus and technological advancements. The technical evaluation of these sensing technologies provided crucial insights into their capabilities and limitations. The study examined emerging technologies such as Differential Absorption LiDAR (DIAL), which show promise for high-precision and long-range detection. The team then investigated the features and application bandwidth of various sensing platforms, including handheld, fixed/stationary, mobile, aerials, and spaceborne monitors. Pilot field studies were conducted to assess the capabilities of solutions for different emission scenarios. Field work with sensor deployments was conducted at three distinct site types: an oil & gas industry site, a cattle ranching operation, and a waste processing facility. The team also conducted a thorough review of methane flux inverse modeling approaches, focused on physically based methods. These approaches were categorized into simple, intermediate, and advanced methods. A realtime WRF-GHG (Weather Research and Forecasting-Greenhouse Gas) modeling system was developed and applied, incorporating multiple data sources to guide field experiments and inform methane plume detection. The project identified and analyzed numerous categories of methane data sources, including satellite measurements, ground-based sensors, and inventory databases. Key platforms examined include EDGAR, EPA GHGI, NASA TROPOMI, Carbon Mapper, and Climate TRACE, among others. The team proposed an architecture for a comprehensive methane monitoring platform. This system incorporates multi-source data acquisition, advanced data processing and assimilation, interactive visualization tools, and analytical capabilities for emissions forecasting and scenario analysis. The proposed platform aims to provide a user-friendly interface catering to various stakeholders, from researchers to policymakers. The architecture includes sophisticated data ingestion methods, a centralized data warehouse, and advanced analytical tools for data fusion and interpretation. To ensure the relevance and effectiveness of the proposed system, a comprehensive survey was conducted to gather stakeholder input on system requirements. Key findings include a strong need for integrating various data types and formats, a preference for real-time data updates and advanced visualization tools, and a demand for user-friendly interfaces catering to different expertise levels.

03 NATURAL GAS↗
DOE OSTI2026

Mapping the soil microbiome functions shaping wetland methane emissions

Accounting for only 8% of Earth’s land cover, freshwater wetlands remain the foremost contributors to global methane emissions. Yet the microorganisms and processes underlying methane emissions from wetland soils remain poorly understood. Over a five-year period, we surveyed the microbial membership and in situ methane measurements from over 700 samples in one of the most prolific methane-emitting wetlands in the United States. We constructed a catalog of 2,502 metagenome-assembled genomes (MAGs), with more than half of the 70 bacterial and archaeal phyla sampled containing novel lineages. Integration of these data with 133 soil metatranscriptomes provided a genome-resolved view of the biogeochemical specialization and versatility expressed over wetland soil spatial and temporal gradients. Centimeter-scale depth differences best explained patterns of microbial community structure and transcribed functionalities, even more than land cover or temporal information. Moreover, while extended flooding restructured soil redox, this perturbation failed to reconfigure the transcriptional profiles of methane-cycling microorganisms, contrasting with theoretically expected responses to hydrological perturbations. Co-expression analyses, coupled with depth-resolved methane measurements, revealed the metabolisms and trophic structures most predictive of methane hotspots. Mapping the spatiotemporal transcriptional patterns on this compendium of biogeochemically classified soil-derived genomes begins to untangle the microbial carbon, energy, and nutrient processing contributing to wetland methane production.

MAG↗
DOE OSTI2024

Development of prechamber enabled mixing-controlled combustion strategy for ultra-low methane emissions from lean burn natural gas engines

This numerical study explores the optimization of Prechamber Enabled Mixing-Controlled Combustion (PC-MCC) using natural gas in heavy-duty engines, aiming to enhance combustion efficiency to minimize methane slip and NOx emissions. The approach involves a prechamber ignition system, distinct from conventional spark ignition (SI) systems, to initiate combustion of direct injected natural gas. By leveraging the robust ignition characteristics of the prechamber, the PC-MCC method demonstrates significant potential in achieving efficient combustion akin to diesel engines but with lower greenhouse gas emissions. The research evaluates the effects of various geometric and operational parameters on the combustion process and emissions, including prechamber volume, nozzle diameter, direct injector (DI) geometry, and engine operating strategies. Computational Fluid Dynamics (CFD) simulations are utilized, focusing on a heavy-duty, single-cylinder engine modeled after the Caterpillar C9.3B engine. Key findings indicate that a prechamber volume of 3 cc, coupled with a nozzle diameter of 2.75 mm for two prechamber holes, strikes an optimal balance between combustion efficiency and emissions reduction. This configuration ensures robust combustion across a range of operating conditions while maintaining methane slip within targeted limits. Further investigation into DI geometry shows the significance of the injector umbrella angle and nozzle diameter in shaping the fuel-air mixing and combustion dynamics. An umbrella angle of 130° and a nozzle diameter of 300 microns are identified as optimal, promoting rapid and efficient combustion with minimized methane and NOx emissions. The study also investigates the impact of injection timing and pressure, highlighting their roles in controlling combustion timing and influencing emissions levels. Advanced injection timing is found to be crucial in achieving the desired low methane slip, whereas retarded injection timing assists to reduce NOx emissions while having a slight increase in methane emissions. Operating strategies incorporating various levels of Exhaust Gas Recirculation (EGR) are assessed for their effectiveness in further reducing emissions. The research demonstrates that a judicious combination of internal hot EGR and careful calibration of DI pressure and SOI timing can achieve significant reductions in NOx emissions while keeping methane slip under control. Specifically, an internal EGR level of 15%–25%, combined with DI pressures of 200–300 bar and injection timings at or after top dead center, is recommended. These findings contribute valuable insights into the development of advanced combustion techniques for natural gas engines, offering a viable pathway to reduce methane slip without compromising engine efficiency or performance. The PC-MCC system presents a promising solution for the future of heavy-duty natural gas engine technology to reduce methane emissions.

Nsaif, Osama↗
NASA NTRS1986

Stable carbon isotope ratios in atmospheric methane and some of its sources

Ratios of C-13/C-12 have been measured in atmospheric methane and in methane collected from sites and biota that represent potentially large sources of atmospheric methane. These include temperate marshes (about -48 percent to about -54 percent), landfills (about -51 percent to about -55 percent), and the first reported values for any species of termite (-72.8 + or - 3.1 percent for Reticulitermes tibialis and -57.3 + or - 1.6 percent for Zootermopsis angusticollis). Numbers in parentheses are delta C-13 values with respect to PDB (Peedee belemnite) carbonate. Most methane sources reported thus far are depleted in C-13 with respect to atmospheric methane (-47.0 + or - 0.3 percent). Individual sources of methane should have C-13/C-12 ratios characteristic of mechanisms of CH4 formation and consumption prior to release to the atmosphere. The mass-weighted average isotopic composition of all sources should equal the mean C-13 of atmospheric methane, corrected for a kinetic isotope effect in the OH attack of CH4. Assuming the kinetic isotope effect to be small (about -3.0 percent correction to -47.0), as in the literature, the new values given here for termite methane do not help to explain the apparent discrepancy between C-13/C-12 ratios of the known CH4 sources and that of atmospheric CH4.

Tyler, Stanley C.↗
NASA NTRS1991

A study of the sources and sinks of methane and methyl chloroform using a global three-dimensional Lagrangian tropospheric tracer transport model

Sources and sinks of methane and methyl chloroform are investigated using a global three-dimensional Lagrangian tropospheric tracer transport model with parameterized hydroxyl and temperature fields. Using the hydroxyl radical field calibrated to the methyl chloroform observations, the globally averaged release of methane and its spatial and temporal distribution were investigated. Two source function models of the spatial and temporal distribution of the flux of methane to the atmosphere were developed. The first model was based on the assumption that methane is emitted as a proportion of net primary productivity (NPP). The second model identified source regions for methane from rice paddies, wetlands, enteric fermentation, termites, and biomass burning based on high-resolution land use data. The most significant difference between the two models were predictions of methane fluxes over China and South East Asia, the location of most of the world's rice paddies, indicating that either the assumption that a uniform fraction of NPP is converted to methane is not valid for rice paddies, or that NPP is underestimated for rice paddies, or that present methane emission estimates from rice paddies are too high.

Taylor, John A.↗
NASA NTRS2011

Liquid Methane Conditioning Capabilities Developed at the NASA Glenn Research Center's Small Multi- Purpose Research Facility (SMiRF) for Accelerated Lunar Surface Storage Thermal Testing

Glenn Research Center s Creek Road Cryogenic Complex, Small Multi-Purpose Research Facility (SMiRF) recently completed validation / checkout testing of a new liquid methane delivery system and liquid methane (LCH4) conditioning system. Facility checkout validation was conducted in preparation for a series of passive thermal control technology tests planned at SMiRF in FY10 using a flight-like propellant tank at simulated thermal environments from 140 to 350K. These tests will validate models and provide high quality data to support consideration of LCH4/LO2 propellant combination option for a lunar or planetary ascent stage.An infrastructure has been put in place which will support testing of large amounts of liquid methane at SMiRF. Extensive modifications were made to the test facility s existing liquid hydrogen system for compatibility with liquid methane. Also, a new liquid methane fluid conditioning system will enable liquid methane to be quickly densified (sub-cooled below normal boiling point) and to be quickly reheated to saturation conditions between 92 and 140 K. Fluid temperatures can be quickly adjusted to compress the overall test duration. A detailed trade study was conducted to determine an appropriate technique to liquid conditioning with regard to the SMiRF facility s existing infrastructure. In addition, a completely new roadable dewar has been procured for transportation and temporary storage of liquid methane. A new spherical, flight-representative tank has also been fabricated for integration into the vacuum chamber at SMiRF. The addition of this system to SMiRF marks the first time a large-scale liquid methane propellant test capability has been realized at Glenn.This work supports the Cryogenic Fluid Management Project being conducted under the auspices of the Exploration Technology Development Program, providing focused cryogenic fluid management technology efforts to support NASA s future robotic or human exploration missions.

Bamberger, Helmut H.↗
NASA NTRS2012

Isotopic Ratios in Titan's Methane: Measurements and Modeling

The existence of methane in Titan's atmosphere (approx. 6% level at the surface) presents a unique enigma, as photochemical models predict that the current inventory will be entirely depleted by photochemistry in a timescale of approx 20 Myr. In this paper, we examine the clues available from isotopic ratios (C-12/C-13 and D/H) in Titan's methane as to the past atmosphere history of this species. We first analyze recent infrared spectra of CH4 collected by the Cassini Composite Infrared Spectrometer, measuring simultaneously for the first time the abundances of all three detected minor isotopologues: (13)CH4, (12)CH3D, and (13)CH3D. From these we compute estimates of C-12/C-13 = 86.5 +/- 8.2 and D/H = (1.59 +/- 0.33) x 10(exp -4) , in agreement with recent results from the Huygens GCMS and Cassini INMS instruments. We also use the transition state theory to estimate the fractionation that occurs in carbon and hydrogen during a critical reaction that plays a key role in the chemical depletion of Titan's methane: CH4 + C2H yields CH3 + C2H2. Using these new measurements and predictions we proceed to model the time evolution of C-12/C-13 and D/H in Titan's methane under several prototypical replenishment scenarios. In our Model 1 (no resupply of CH4), we find that the present-day C-12/C-13 implies that the CH4 entered the atmosphere 60-1600 Myr ago if methane is depleted by chemistry and photolysis alone, but much more recently-most likely less than 10 Myr ago-if hydrodynamic escape is also occurring. On the other hand, if methane has been continuously supplied at the replenishment rate then the isotopic ratios provide no constraints, and likewise for the case where atmospheric methane is increasing, We conclude by discussing how these findings may be combined with other evidence to constrain the overall history of the atmospheric methane.

Nixon, C. A.↗
NASA NTRS2016

Martian Atmospheric Methane Plumes from Meteor Shower Infall: A Hypothesis

Methane plumes in the martian atmosphere have been detected using Earth-based spectroscopy, the Planetary Fourier Spectrometer on the ESA Mars Express mission, and the NASA Mars Science Laboratory. The methane's origin remains a mystery, with proposed sources including volcanism, exogenous sources like impacts and interplanetary dust, aqueous alteration of olivine in the presence of carbonaceous material, release from ancient deposits of methane clathrates, and/or biological activity. To date, none of these phenomena have been found to reliably correlate with the detection of methane plumes. An additional source exists, however: meteor showers could generate martian methane via UV pyrolysis of carbon-rich infall material. We find a correlation between the dates of Mars/cometary orbit encounters and detections of methane on Mars. We hypothesize that cometary debris falls onto Mars during these interactions, depositing freshly disaggregated meteor shower material in a regional concentration. The material generates methane via UV photolysis, resulting in a localized "plume" of short-lived methane.

Fries, M.↗
NASA NTRS2017

Methane Metabolism by Yeast for Solar System Exploration

Exploration of the solar system is constrained by the cost of moving mass off Earth. Producing materials in situ will reduce the mass that must be delivered from earth. CO2 is abundant on Mars and manned spacecraft. On the ISS, NASA reacts excess CO2 with H2 to generate CH4 and H2O using the Sabatier System. The resulting water is recovered into the ISS, but the methane is vented to space. Thus, there is a capability need for systems that convert methane into valuable materials. Methanotrophic bacteria consume methane but these are poor synthetic biology platforms. Thus, there is a knowledge gap in utilizing methane in a robust and flexible synthetic biology platform. The yeast Pichia pastoris is a refined microbial factory that is used widely by industry because it efficiently secretes products. Pichia could produce a variety of useful products in space. Pichia does not consume methane but robustly consumes methanol, which is one enzymatic step removed from methane. Our goal is to engineer Pichia to consume methane thereby creating a powerful methane-consuming microbial factory.

Galazka, Jonathan M.↗
NASA NTRS2022

XSP Methane Sensors Test and Evaluation Project “M-Step”

Methane sensor technology is employed in industry sectors from oil and gas to agriculture, landfills, and monitoring of natural emissions. The US oil and gas sector is extensive in scale, critical to fulfilling US energy needs, and deals with commodities presenting enormous challenges for personnel safety and the environment. Thus, it is imperative that they have accurate and responsive sensors to detect hazardous gases such as methane. US space launch systems will increasingly also use liquefied methane and liquefied natural gas (LNG), which is mostly methane, in quantities large and small, as main and auxiliary propulsion and power. Some of these systems will be reusable, which adds the unique challenge of processing a vehicle that has residual commodities and has returned to its launch site to be readied for its next launch. The methane sensors test and evaluation project (M-STEP) began within the context of a reusable launch system, the Defense Advanced Research Projects Agency (DARPA) Experimental Spaceplane (XSP) program, which would have employed a high-pressure gaseous methane and gaseous oxygen reaction control system. Although the XSP partnership between Boeing and DARPA was terminated by Boeing in early 2020, DARPA and KSC have continued to collaborate in the area of gas sensors with the hydrogen sensor test and evaluation project (H-STEP) and with M-STEP. The NASA Launch Services program (LSP) invested in M-STEP in FY 2021 “to evaluate and understand the state-of-the-art in methane gas sensors”. M-STEP and the LSP effort was complementary, pushing in the same direction to understand US launch system stakeholder needs and approaches, requirements internal (NASA) and external, and commercially available or forthcoming methane sensing technologies, practices, and approaches. In addition, M-STEP (as with H-STEP) enhances KSC capabilities and understanding of these technologies, informing agency investments and further research in these areas.

Tracy L. Gibson↗
NASA NTRS2022

Wetland Emission and Atmospheric Sink Changes Explain Methane Growth in 2020

Atmospheric methane growth reached an exceptionally high rate of 15.1 ± 0.4 parts per billion per year in 2020 despite a probable decrease in anthropogenic methane emissions during COVID-19 lockdowns(1). Here we quantify changes in methane sources and in its atmospheric sink in 2020 compared with 2019. We find that, globally, total anthropogenic emissions decreased by 1.2 ± 0.1 teragrams of methane per year (Tg CH4 yr−1), fire emissions decreased by 6.5 ± 0.1 Tg CH4 yr−1 and wetland emissions increased by 6.0 ± 2.3 Tg CH4 yr−1. Tropospheric OH concentration decreased by 1.6 ± 0.2 per cent relative to 2019, mainly as a result of lower anthropogenic nitrogen oxide (NOx) emissions and associated lower free tropospheric ozone during pandemic lockdowns(2). From atmospheric inversions, we also infer that global net emissions increased by 6.9 ± 2.1 Tg CH4 yr−1 in 2020 relative to 2019, and global methane removal from reaction with OH decreased by 7.5 ± 0.8 Tg CH4 yr−1. Therefore, we attribute the methane growth rate anomaly in 2020 relative to 2019 to lower OH sink (53 ± 10 per cent) and higher natural emissions (47 ± 16 per cent), mostly from wetlands. In line with previous findings(3,4,) our results imply that wetland methane emissions are sensitive to a warmer and wetter climate and could act as a positive feedback mechanism in the future. Our study also suggests that nitrogen oxide emission trends need to be taken into account when implementing the global anthropogenic methane emissions reduction pledge(5).

Shushi Peng↗
DOE OSTI2025

Engineering PdAu/CeO 2 Alloy/Oxide Interfaces for Selective Methane‐to‐Methanol Conversion with Water

The direct conversion of methane-to-methanol remains a critical challenge in methane valorization. In this study, we unveil the crucial role of PdAu/CeO 2 catalysts in enabling selective methane transformation under mild conditions, using only water as the sole oxidant. Through a combination of experimental techniques, including XPS and catalytic testing, alongside density functional theory (DFT) calculations, we demonstrate that a Pd 0.3 Au 0.7 /CeO 2 catalyst, which predominantly exposes isolated Pd atoms, achieves remarkable methanol selectivity (∼80%) at 500 K with a 1:1 methane-to-water ratio. While Pd/CeO 2 efficiently activates methane, its tendency for overreaction leads to complete methanol decomposition, thereby limiting selectivity. Alloying Pd with Au on ceria mitigates this over-reactivity, preventing methanol degradation while maintaining sufficient catalytic activity. The PdAu/CeO 2 composite exhibits a synergistic effect: Pd in contact with the ceria support facilitates methane activation and water dissociation, while Au fine-tunes reactivity to promote methanol formation. DFT calculations confirm that isolated Pd sites at the PdAu/CeO 2 interface play a key role in balancing activity and selectivity. This work underscores the importance of alloy/oxide interfaces in controlling selective methane conversion with water and offers valuable insights for designing highly efficient catalysts for methanol synthesis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Insights into Designing an Efficient and Reliable Microwave-Assisted Methane Dehydroaromatization Process: Effect of Microwave Absorber on Catalyst Performance

Microwave-assisted methane dehydroaromatization has the potential to address challenges of traditional dehydroaromatization reactions. However, catalysts for microwave-enhanced reaction systems require effective coupling of fields with the catalyst to produce heat and reach reaction temperatures. Here, this work presents an in-depth understanding of the effect of the addition of silicon carbide as a microwave absorber on catalyst performance among other variables, the viability of the microwave reactor configuration, and insights into designing an effective and reliable microwave-based methane dehydroaromatization process. The effect of other parameters including temperature, weight hourly space velocity, role of microwave absorber, and methane concentration during microwave-assisted methane dehydroaromatization reaction are studied. Mo/ZSM-5 was found to suffer from low permittivity and nonuniform heating under microwave conditions. Mixing silicon carbide powder as a microwave absorber with the catalyst was found to provide more uniform heating. When assessing the catalytic performance of the mixture, it was found that higher methane partial pressures at 2000 cc/g cat .h and a temperature range of 500-600°C produced the highest amount of benzene. The formation of graphitic carbon on the spent catalyst increased with temperature, gas-solid contact period, and methane concentration, which resulted in higher methane conversion and benzene selectivity. The study indicates that under microwave heating the presence of localized carbon enhanced catalyst life by coupling with microwave energy, leading to localized heating, and improving benzene selectivity.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗