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NASA NTRS1979

Concentration-time data in toxicity tests and resulting relationships

Periodic analyses for carbon monoxide and methane in the animal exposure chamber during pyrolysis of polyethylene at 800 C without forced air flow showed that the concentrations of these compounds increased with exposure time. These observations, and similar observations for polyurethane flexible foam, permitted the calculation of carbon monoxide toxicity in terms of a DP (Death Product Concentration) value, in addition to flammability in terms of HC (Hydro Carbon) value. Observed DP values exceeding the critical DP(CO) value of 47,200 ppm-min for carbon monoxide may indicate that lethal exposures were reached earlier but not immediately manifested because of the time delay involved in physiological processes. On the basis of this DP(CO) value, carbon monoxide could have been the sole toxicant in the case of polyethylene, polypropylene, polyoxymethylene, polystyrene, polycarbonate, ethylene propylene diene rubber, and wood.

Hilado, C. J.↗

DOE OSTI2025

COMPASS-FME Terrestrial Ecosystem Manipulation to Probe the Effects of Storm Treatments (TEMPEST) Soil Greenhouse Gas Fluxes 04/2020-06/2024

Both raw and processed data measured using a LI-COR 7810 Greenhouse Gas Analyzer in the TEMPEST experiment, part of COMPASS-FME (https://compass.pnnl.gov/FME/COMPASSFME), at Smithsonian Environmental Research Center. This ecosystem-scale experiment probes the effects of saltwater versus freshwater flooding in a coastal deciduous forest.The data consist of both concentrations and fluxes of carbon dioxide and methane measured using static chambers on the soil surface, approximately every two weeks from early 2020 to mid 2024. Some of the measurement points are controls, and some subject to root-exclusion techniques; all measurements are embedded in the TEMPEST control, freshwater, and saltwater plots (see Hopple et al. 2023). These data were generated to understand changing soil greenhouse gas (CO2 and CH4) production and consumption. File types are comma-separated value (.csv) for data, and markdown (.md) for supplementary information.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1990

Burning trees and bridges

Most burning of biomass is the result of human activity, and on a global scale it is increasing. Tropospheric concentrations of CO2, CO, CH4, non-methane hydrocarbons, and ozone are all increasing with time; global biomass burning may make an important contribution to this increase and thus to potential global climate change. The nitrogen cycle also can have important climatic effects. Nitrous oxide put into the atmosphere by biomass burning is a greenhouse gas 250 times more powerful (molecule for molecule) than carbon dioxide. Nitric oxide, as well as being a photochemical precursor of ozone, a major pollutant in the troposphere, produces nitric acid, the fastest-growing component of acid rain. Hence, the new bridge in the nitrogen cycle is of more than mere technical interest.

Levine, Joel S.↗

NASA NTRS2005

High-temperature catalyst for catalytic combustion and decomposition

A robust, high temperature mixed metal oxide catalyst for propellant composition, including high concentration hydrogen peroxide, and catalytic combustion, including methane air mixtures. The uses include target, space, and on-orbit propulsion systems and low-emission terrestrial power and gas generation. The catalyst system requires no special preheat apparatus or special sequencing to meet start-up requirements, enabling a fast overall response time. Start-up transients of less than 1 second have been demonstrated with catalyst bed and propellant temperatures as low as 50 degrees Fahrenheit. The catalyst system has consistently demonstrated high decomposition effeciency, extremely low decomposition roughness, and long operating life on multiple test particles.

Mays, Jeffrey A.↗

NASA NTRS2010

Operation of a Third Generation JPL Electronic Nose in the Regenerative ECLSS Module Simulator at MSFC

An electronic nose has been developed at the Jet Propulsion Laboratory (JPL) to monitor spacecraft cabin air for anomalous events such as leaks and spills of solvents, coolants or other fluids with near-real-time analysis. It is designed to operate in the environment of the US Lab on ISS and was deployed on the International Space Station for a seven-month experiment in 2008-2009. In order improve understanding of ENose response to crew activities, an ENose was installed in the Regenerative ECLSS Module Simulator (REMS) at Marshall Space Flight Center (MSFC) for several months. The REMS chamber is operated with continuous analysis of the air for presence and concentration of CO, CO2, ethane, ethanol and methane. ENose responses were analyzed and correlated with logged activities and air analyses in the REMS.

Electronic Nose (ENose)↗

NASA NTRS2011

Atmospheric Composition Change: Climate-Chemistry Interactions

Chemically active climate compounds are either primary compounds such as methane (CH4), removed by oxidation in the atmosphere, or secondary compounds such as ozone (O3), sulfate and organic aerosols, formed and removed in the atmosphere. Man-induced climate-chemistry interaction is a two-way process: Emissions of pollutants change the atmospheric composition contributing to climate change through the aforementioned climate components, and climate change, through changes in temperature, dynamics, the hydrological cycle, atmospheric stability, and biosphere-atmosphere interactions, affects the atmospheric composition and oxidation processes in the troposphere. Here we present progress in our understanding of processes of importance for climate-chemistry interactions, and their contributions to changes in atmospheric composition and climate forcing. A key factor is the oxidation potential involving compounds such as O3 and the hydroxyl radical (OH). Reported studies represent both current and future changes. Reported results include new estimates of radiative forcing based on extensive model studies of chemically active climate compounds such as O3, and of particles inducing both direct and indirect effects. Through EU projects such as ACCENT, QUANTIFY, and the AEROCOM project, extensive studies on regional and sector-wise differences in the impact on atmospheric distribution are performed. Studies have shown that land-based emissions have a different effect on climate than ship and aircraft emissions, and different measures are needed to reduce the climate impact. Several areas where climate change can affect the tropospheric oxidation process and the chemical composition are identified. This can take place through enhanced stratospheric-tropospheric exchange of ozone, more frequent periods with stable conditions favouring pollution build up over industrial areas, enhanced temperature-induced biogenic emissions, methane releases from permafrost thawing, and enhanced concentration through reduced biospheric uptake. During the last 510 years, new observational data have been made available and used for model validation and the study of atmospheric processes. Although there are significant uncertainties in the modelling of composition changes, access to new observational data has improved modelling capability. Emission scenarios for the coming decades have a large uncertainty range, in particular with respect to regional trends, leading to a significant uncertainty range in estimated regional composition changes and climate impact.

Atmosphere climate chemistry↗

NASA NTRS2014

Climate Change in New York State Updating the 2011 ClimAID Climate Risk Information Supplement to NYSERDA Report 11-18 (Responding to Climate Change in New York State)

In its 2013-2014 Fifth Assessment Report (AR5), the Intergovernmental Panel on Climate Change (IPCC) states that there is a greater than 95 percent chance that rising global average temperatures, observed since the mid-20th century, are primarily due to human activities. As had been predicted in the 1800s, the principal driver of climate change over the past century has been increasing levels of atmospheric greenhouse gases associated with fossil-fuel combustion, changing land-use practices, and other human activities. Atmospheric concentrations of the greenhouse gas carbon dioxide are now approximately 40 percent higher than in preindustrial times. Concentrations of other important greenhouse gases, including methane and nitrous oxide, have increased rapidly as well.

New York↗

NASA NTRS2013

Analyzing Carbon Dioxide and Methane Emissions in California Using Airborne Measurements and Model Simulations

Greenhouse gas (GHG) concentrations have increased over the past decades and are linked to global temperature increases and climate change. These changes in climate have been suggested to have varying effects, and uncertain consequences, on agriculture, water supply, weather, sea-level rise, the economy, and energy. To counteract the trend of increasing atmospheric concentrations of GHGs, the state of California has passed the California Global Warming Act of 2006 (AB-32). This requires that by the year 2020, GHG (e.g., carbon dioxide (CO2) and methane (CH4)) emissions will be reduced to 1990 levels. To quantify GHG fluxes, emission inventories are routinely compiled for the State of California (e.g., CH4 emissions from the California Greenhouse Gas Emissions Measurement (CALGEM) Project). The major sources of CO2 and CH4 in the state of California are: transportation, electricity production, oil and gas extraction, cement plants, agriculture, landfills/waste, livestock, and wetlands. However, uncertainties remain in these emission inventories because many factors contributing to these processes are poorly quantified. To alleviate these uncertainties, a synergistic approach of applying air-borne measurements and chemical transport modeling (CTM) efforts to provide a method of quantifying local and regional GHG emissions will be performed during this study. Additionally, in order to further understand the temporal and spatial distributions of GHG fluxes in California and the impact these species have on regional climate, CTM simulations of daily variations and seasonality of total column CO2 and CH4 will be analyzed. To assess the magnitude and spatial variation of GHG emissions and to identify local “hot spots”, airborne measurements of CH4 and CO2 were made by the Alpha Jet Atmospheric eXperiment (AJAX) over the San Francisco Bay Area (SFBA) and San Joaquin Valley (SJV) in January and February 2013 during the Discover-AQ-CA study. High mixing ratios of GHGs were observed in-flight with a high degree of spatial variability. To provide an additional method to quantify GHG emissions, and analyze AJAX measurement data, the GEOS-Chem CTM is used to simulate SFBA/SJV GHG measurements. A nested-grid version of GEOS-Chem will be applied and utilizes varying emission inventories and model parameterizations to simulate GHG fluxes/emissions. The model considers CO2 fluxes from fossil fuel use, biomass/biofuel burning, terrestrial and oceanic biosphere exchanges, shipping and aviation, and production from the oxidation of carbon monoxide, CH4, and non-methane volatile organic carbons. The major sources of CH4 simulated in GEOS-Chem are domesticated animals, rice fields, natural gas leakage, natural gas venting/flaring (oil production), coal mining, wetlands, and biomass burning. Preliminary results from the comparison between available observations (e.g., AJAX and CALGEM CH4 emission maps) and GEOS-Chem results will be presented, along with a discussion of CO2 and CH4 source apportionment and the use of the GEOS-Chem-adjoint to perform inverse GHG modeling.

Johnson, Matthew S.↗

DOE OSTI2022

An Assessment of Current Understanding of the Greenhouse Gas Impacts from H 2 Emissions

With the anticipated growth in hydrogen generation and use as part of a broad shift in energy use away from fossil fuels, concerns have been raised regarding the impact of increased H 2 emissions on global warming. Atmospheric scientists have long recognized that H 2 emissions into the atmosphere do have an indirect impact on global warming, largely because a portion of emitted H 2 is consumed by the hydroxyl radical (OH), which is the primary reactant that removes the potent greenhouse gas methane from the atmosphere. Therefore, increases in H 2 emissions will result in decreases in the average OH concentrations in the atmosphere and an increase in the atmospheric lifetime of methane. Various assessments of the impact of H 2 emissions on global warming have been performed over the past couple of decades. These assessments have yielded significant variability and recognized uncertainty in the magnitude of the warming effect of a given quantity of emitted H 2 , and an even greater uncertainty in the magnitude of H 2 leakage and releases that can be anticipated with an expanded H 2 infrastructure. Consequently, definitive estimates of the magnitude of the warming effect of additional emitted H 2 are lacking. However, given the current understanding of the warming potential of emitted H 2 and given reasonable expectations of the emission rate of an expanded H 2 infrastructure, it is anticipated that warming effects from emitted H 2 will offset no more than 5% of the reduction in warming associated with avoided CO 2 emissions from using clean H 2 . Further, it is highly unlikely that the warming effects from emitted H 2 will offset more than 10% of the benefit from avoided CO 2 emissions, at least as considered over a typical 100-year accounting period. Because of the short atmospheric lifetimes of H 2 and methane, however, the warming effect of emitted H 2 is enhanced over the first few years following increases in H 2 emission.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Role of ring-enlargement reactions in the formation of aromatic hydrocarbons

Ring-enlargement reactions can provide a fast route towards the formation of six-membered single-ring or polycyclic aromatic hydrocarbons (PAHs). To investigate the participation of the cyclopentadienyl (C 5 H 5 ) radical in ring-enlargement reactions in high-temperature environments, a mass-spectrometric study was conducted. Experimental access to the C 5 H 5 high-temperature chemistry was provided by two counterflow diffusion flames. Cyclopentene was chosen as a primary fuel given the large amount of resonantly stabilized cyclopentadienyl radicals produced by its decomposition and its high tendency to form PAHs. In a second experiment, methane was added to the fuel stream to promote methyl addition pathways and to assess the importance of ring-enlargement reactions for PAH growth. The experimental dataset includes mole fraction profiles of small intermediate hydrocarbons and of several larger species featuring up to four condensed aromatic rings. Results show that, while the addition of methane enhances the production of methylcyclopentadiene and benzene, the concentration of larger polycyclic hydrocarbons is reduced. The increase of benzene is probably attributable to the interaction between the methyl and the cyclopentadienyl radicals. However, the formation of larger aromatics seems to be dominated only by the cyclopentadienyl driven molecular-growth routes which are hampered by the addition of methane. Furthermore, in addition to the experimental work, two chemical mechanisms were tested and newly calculated reaction rates for cyclopentadiene reactions were included. In an attempt to assess the impact of cyclopentadienyl ring-enlargement chemistry on the mechanisms’ predictivity, pathways to form benzene, toluene, and ethylbenzene were investigated. Results show that the updated mechanism provides an improved agreement between the computed and measured aromatics concentrations. Nevertheless, a detailed study of the single reaction steps leading to toluene, styrene, and ethylbenzene would be certainly beneficial.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Temporal and spatial characterization of a thermogenic, fault-controlled gas hydrate system, Woolsey Mound, Gulf of Mexico

Woolsey Mound, located at Mississippi Canyon Lease Block 118 (MC118), is the site of the Gulf of Mexico hydrate research consortium’s seafloor observatory, where gas hydrates outcrop at the seafloor. The presence of gas hydrates in the mound is confirmed directly by coring and indirectly by 3D seismic reflection data. Craters, pockmarks, chemosynthetic communities, and authigenic carbonates populate the seafloor at Woolsey Mound. Each crater is characterized by a network of shallow crestal faults that connect the hydrate mound to the underlying allochthonous salt body. We characterize the temporal and spatial evolution of gas hydrates at Woolsey Mound under natural perturbations using four collocated 3D seismic reflection data sets that span over 14 years. Data acquisition differences embedded in the data sets arising from variation in geometry, sample rate, and phase are minimized using the “cross-equalization” method. Our results indicate that hydrate formation and dissociation vary temporally and spatially in close connection to the shallow crestal faults. Evidence of gas hydrate dissociation is observed over a period of three years (2000–2003), where major dissociation occurred along the southern portion of the crestal fault in the southeast crater. The dissociation is less prominent in the southwest crater. Evidence of methane venting is observed between 2000 and 2010, which is mostly concentrated in the southeast crater. The residual amplitude anomalies observed between 2000 and 2014 in the mound are mostly positive, implying that the methane venting had increased significantly. The positive anomalies are correlated with the methane seepage recorded in 2011. Our results indicate the evolution of a fault-controlled gas hydrate system in the northern Gulf of Mexico, which would aid in assessing its impact on the seafloor.

Geochemistry & Geophysics↗

NASA NTRS2001

Mapping Rice Production in China with AVHRR Imagery

The study of rice agriculture is necessary for both the importance of rice as a vital food source and because of the fact that cultivating it has an unfortunate byproduct, namely methane gas. As a food source, rice is a staple for a large majority of the world's population, especially in Asia. Because the populations of many Asian nations are increasing at rapid rates, the production of rice will need to similarly increase. In 1989, it was estimated that the demand for rice would increase by 65% by the year 2019. Rice crops are considered to be one of the primary anthropogenic sources of methane gas. A reason for concern is that this gas is a so-called "greenhouse" trace gas and given its increasing levels in the atmosphere, is thought to contribute to the suspected global warming phenomenon. Some estimate that methane may contribute up to 20% to the global warming effect. Trace gas emissions from anthropogenic sources is an issue that generates great worldwide interest because of the fact that mankind is very likely affecting the current and future climate in potentially negative ways. In an effort to better understand these effects, scientists and engineers are conducting research on all of the varied fronts which relate to climate change and biosphere/atmosphere interactions. The study of global warming through increasing concentrations of greenhouse gases is one area which has received much media and scientific attention. Research fueled by debates on this topic is being conducted on numerous, interrelated fronts in an effort to better understand the complex relationship between human activities and the earth's climate. The research ranges from attempting to verify if the observed data even supports the existence of an anthropogenically generated global-warming phenomenon, to identification of sources and sinks of the trace gases, to measuring the source strengths, to studies which focus on modeling the processes which generate the gases, and finally, to trying to project their impact on the global climatic system. Some of the more commonly known sources of greenhouse gases are related to industry and transportation. Carbon dioxide, CO2, from automobile emissions is one such example. Lesser known are sources from natural and cultivated vegetation, such as the methane, CH4, resulting from rice cropping. While the concentration of atmospheric methane is significantly less than that of carbon dioxide, CH4 has been estimated to have up to 32 times the insulating capability of carbon dioxide, making it an important gas to monitor. The remainder of this chapter will provide some additional background information on the effects of atmospheric methane, and the role that rice agriculture plays as a source in the methane budget. This will be followed by a brief description of efforts to model this source of atmospheric methane. Finally, this chapter will end with a statement of the hypotheses of this thesis, at which time a description of the information contained in the rest of this document will be provided.

Paliouras, Eleni J.↗

DOE OSTI2022

Experimental Investigation of Gaseous Mixtures of Ethane, Methane, and Carbon Dioxide as an Alternative to Conventional Fuel in Spark Ignition Engines

This study investigates the viability and performance of certain synthetic fuels in spark ignition internal combustion engine based stationary power generation wherein the fuel comprises a mixture of methane and ethane in high dilutions of carbon dioxide (CO 2 ). The fuel of concern is a byproduct of a novel method for producing ethylene from ethane. The byproduct gas mixture has a concentration of approximately 41% CO 2 , 40% ethane, and 5% methane by weight along with other minor compounds. Varying mixtures of ethane and methane combined with between 42% and 46% by weight CO 2 were used to evaluate the viability and efficiency of this fuel to operate in existing internal combustion engines as a means of reducing emissions and increasing industrial process efficiency. A 13 hp gasoline generator was repurposed as a test stand by incorporating a modified fuel induction system and instrumentation for data collection. A gas metering and mixing system was installed to precisely control the mass flow of gases induced into the engine. Various instrumentations were installed to monitor in-cylinder pressure, temperature at various locations, emissions, and fuel and airflow rates. Varying fuel mixtures and loads were tested and compared to gasoline. It was found that under a high load, the mixed gas was able to generate comparable thermal efficiency and power to gasoline. But under no load or a part load condition the indicated thermal efficiency was found to be about 21% lower than that of gasoline. Further, the mixed gas also resulted in up to 50% reduction in CO and NOx emissions when compared to gasoline.

42 ENGINEERING↗

DOE OSTI2025

Changuinola peat soil characteristics and gas emission raw data October 2019

This dataset comprises radiocarbon and geochemical measurements from peat and porewater samples collected across various depths at a site in Bocas del Toro, Panama. The study focuses on carbon cycling dynamics in tropical peatlands by examining carbon isotopic signatures (¹⁴C and ¹³C) and elemental compositions of bulk peat, dissolved organic carbon (DOC), carbon dioxide (CO₂), and methane (CH₄). Key parameters include radiocarbon ages and isotopic ratios (δ¹³C) of bulk peat, concentrations of carbon (%C) and nitrogen (%N), and radiocarbon content of porewater gases and dissolved organic carbon (DOC). The data provide insights into the vertical and spatial distribution of carbon sources and possible preservation and decomposition processes within tropical peat profiles, offering critical information for understanding carbon storage and greenhouse gas emissions in these ecosystems.This dataset is comprised of one main data folder containing (1) file-level metadata; (2) data dictionary; (3) field metadata; (4) carbon isotopic signatures (¹⁴C and ¹³C); (5) concentrations of carbon (%C) and nitrogen (%N); (6) radiocarbon content of porewater carbon dioxide (CO₂), and methane (CH₄) ; (7) porewater DOC; (8) bulk peat sampling protocol; (9) porewater sampling protocol; (10) porewater gas collection methods; and (11) gas extraction methods. All files are in .csv format and can be opened with any software that supports this file types.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Comparison of Sub-Ppm Instrument Response Suggests Higher Detection Limits Could Be Used to Quantify Methane Emissions from Oil and Gas Infrastructure

Quantifying and controlling fugitive methane emissions from oil and gas facilities remains essential for addressing climate goals, but the costs associated with monitoring millions of production sites remain prohibitively expensive. Current thinking, supported by measurement and simple dispersion modelling, assumes single-digit parts-per-million instrumentation is required. To investigate instrument response, the inlets of three trace-methane (sub-ppm) analyzers were collocated on a facility designed to release gas of known composition at known flow rates between 0.4 and 5.2 kg CH 4 h –1 from simulated oil and gas infrastructure. Methane mixing ratios were measured by each instrument at 1 Hertz resolution over nine hours. While mixing ratios reported by a cavity ring-down spectrometer (CRDS)-based instrument were on average 10.0 ppm (range 1.8 to 83 ppm), a mid-infrared laser absorption spectroscopy (MIRA)-based instrument reported short-lived mixing ratios far larger than expected (range 1.8 to 779 ppm) with a similar nine-hour average to the CRDS (10.1 ppm). We suggest the peaks detected by the MIRA are likely caused by a micrometeorological phenomenon, where vortex shedding has resulted in heterogeneous methane plumes which only the MIRA can observe. Further analysis suggests an instrument like the MIRA (an optical-cavity-based instrument with cavity size ≤10 cm3 measuring at ≥2 Hz with air flow rates in the order of ≤0.3 slpm at distances of ≤20 m from the source) but with a higher detection limit (25 ppm) could detect enough of the high-concentration events to generate representative 20 min-average methane mixing ratios. Even though development of a lower-cost, high-precision, high-accuracy instrument with a 25 ppm detection threshold remains a significant problem, this has implications for the use of instrumentation with higher detection thresholds, resulting in the reduction in cost to measure methane emissions and providing a mechanism for the widespread deployment of effective leak detection and repair programs for all oil and gas infrastructure.

03 NATURAL GAS↗

DOE OSTI2024

Simulation of metal nanoparticles growth in methane atmosphere of arc discharge: comparison to experiment

A direct current arc discharge in a methane atmosphere is a scalable and sustainable method to produce metal-carbon core–shell nanoparticles and single-walled carbon nanotubes, where a metal catalyst can be continuously supplied through evaporation of an anode made from the catalyst material. The size of catalyst particles is of critical importance as it can affect the synthesis yield and properties of nanotubes and core–shell nanoparticles. This study presents a numerical model describing the formation and growth of metal particles for the conditions representative of the arc discharge with an evaporating iron anode at near-atmospheric pressure of a methane-rich atmosphere. The model incorporates carbon adsorption to the metal surface and explains the limiting effect of carbon coverage on the size of metal nanoparticles. The predicted particle sizes are compared with experimental observations. The model also predicts higher concentrations of metal particles with the increasing partial pressure of methane.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

NASA NTRS1977

High pressure flame system for pollution studies with results for methane-air diffusion flames

A high pressure flame system was designed and constructed for studying nitrogen oxide formation in fuel air combustion. Its advantages and limitations were demonstrated by tests with a confined laminar methane air diffusion flame over the pressure range from 1 to 50 atm. The methane issued from a 3.06 mm diameter port concentrically into a stream of air contained within a 20.5 mm diameter chimney. As the combustion pressure is increased, the flame changes in shape from wide and convex to slender and concave, and there is a marked increase in the amount of luminous carbon. The height of the flame changes only moderately with pressure.

Miller, I. M.↗

NASA NTRS1985

Combustion efficiency of a premixed continuous flow combustor

Exhaust gas temperature, velocity, and composition measurements at various radial locations at the combustor exit are presented for a swirling-flow continuous combustor of a confined concentric jet configuration operating on premixed propane or methane and air. The main objective of the study is to determine the effect of fuel substitution and of changes in outer flow swirl conditions on the combustor performance. It is found that there is no difference in observed properties for propane and methane firing; the use of either of the fuels results in nearly the same exit temperature and velocity profiles and the same efficiency for a given operating condition. A mechanism for combustion is proposed which explains qualitatively the changes in efficiency and pollutant emissions observed with changing swirl.

Anand, M. S.↗