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At least 469 records · Page 26
All sourcesNASA NTRSDOE OSTI
DOE OSTI2013

A metagenomic insight into freshwater methane-utilizing communities and evidence for cooperation between the Methylococcaceae and the Methylophilaceae

We investigated microbial communities active in methane oxidation in lake sediment at different oxygen tensions and their response to the addition of nitrate, via stable isotope probing combined with deep metagenomic sequencing. Communities from a total of four manipulated microcosms were analyzed, supplied with 13 C-methane in, respectively, ambient air, ambient air with the addition of nitrate, nitrogen atmosphere and nitrogen atmosphere with the addition of nitrate, and these were compared to the community from an unamended sediment sample. We found that the major group involved in methane oxidation in both aerobic and microaerobic conditions were members of the family Methylococcaceae, dominated by species of the genus Methylobacter, and these were stimulated by nitrate in aerobic but not microaerobic conditions. In aerobic conditions, we also noted a pronounced response to both methane and nitrate by members of the family Methylophilaceae that are non-methane-oxidizing methylotrophs, and predominantly by the members of the genus Methylotenera. The relevant abundances of the Methylococcaceae and the Methylophilaceae and their coordinated response to methane and nitrate suggest that these species may be engaged in cooperative behavior, the nature of which remains unknown.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2014

Retrieval of Methane Source Strengths in Europe Using a Simple Modeling Approach to Assess the Potential of Spaceborne Lidar Observations

We investigate the sensitivity of future spaceborne lidar measurements to changes in surface methane emissions. We use surface methane observations from nine European ground stations and a Lagrangian transport model to infer surface methane emissions for 2010. Our inversion shows the strongest emissions from the Netherlands, the coal mines in Upper Silesia, Poland, and wetlands in southern Finland. The simulated methane surface concentrations capture at least half of the daily variability in the observations, suggesting that the transport model is correctly simulating the regional transport pathways over Europe. With this tool we can test whether proposed methane lidar instruments will be sensitive to changes in surface emissions. We show that future lidar instruments should be able to detect a 50% reduction in methane emissions from the Netherlands and Germany, at least during summer.

surface fluxes↗
NASA NTRS2020

Increasing anthropogenic methane emissions arise equally from agricultural and fossil fuel sources

Climate stabilization remains elusive, with increased greenhouse gas concentrations already increasing global average surface temperatures 1.1°C above pre-industrial levels (World Meteorological Organization 2019). Carbon dioxide (CO2) emissions from fossil fuel use, deforestation, and other anthropogenic sources reached ~ 43 billion metric tonnes in 2019 (Friedlingstein et al 2019, Jackson et al 2019). Storms, floods, and other extreme weather events displaced a record 7 million people in the first half of 2019 (IDMC 2019). When global mean surface temperature four million years ago was 2°C–3°C warmer than today (a likely temperature increase before the end of the century), ice sheets in Greenland and West Antarctica melted and parts of East Antarctica’s ice retreated, causing sea levels to rise 10–20 m (World Meteorological Organization 2019). Methane (CH4) emissions have contributed almost one quarter of the cumulative radiative forcings for CO2, CH4, and N2O (nitrous oxide) combined since 1750 (Etminan et al 2016). Although methane is far less abundant in the atmosphere than CO2, it absorbs thermal infrared radiation much more efficiently and, in consequence, has a global warming potential (GWP) ~86 times stronger per unit mass than CO2 on a 20-year timescale and 28- times more powerful on a 100-year time scale (IPCC 2014). Global average methane concentrations in the atmosphere reached ~1875 parts per billion (ppb) at the end of 2019, more than two-and-a-half times preindustrial levels (Dlugokencky 2020). The largest methane sources include anthropogenic emissions from agriculture, waste, and the extraction and use of fossil fuels as well as natural emissions from wetlands, freshwater systems, and geological sources (Kirschke et al 2013, Saunois et al 2016a, Ganesan et al 2019). Here, we summarize new estimates of the global methane budget based on the analysis of Saunois et al (2020) for the year 2017, the last year of the new Global Methane Budget and the most recent year data are fully available. We compare these estimates to mean values for the reference ‘stabilization’ period of 2000–2006 when atmospheric CH4 concentrations were relatively stable. We present data for sources and sinks and provide insights for the geographical regions and economic sectors where emissions have changed the most over recent decades.

fossil fuel sources↗
NASA NTRS2020

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↗
NASA NTRSDate not supplied

A New Laser Transmitter for Methane and Water Vapor Measurements at 1.65 μm

Atmospheric methane trends over the last few years have been increasing at a rate of 7-12 parts per billion (ppb) per year after brief a pause in the first decade of this century. The reasons for the pause and subsequent increase remains unclear. Thus, there is a critical need for additional, precise and accurate methane observations to understand the natural and anthropogenic processes that drive the trends in atmospheric methane and to constrain its sources, and sinks. At NASA Goddard Space Flight Center (GSFC), in collaboration with Freedom Photonics Inc., we have been developing a lidar to measure atmospheric methane using Integrated Path Differential Absorption (IPDA) from an airborne platform as a precursor to a future space mission. In this paper we present the design of a laser transmitter operating at ~1651 nmbased on a newly developed Distributed Bragg Grating (DBR) seed laser and an Optical parametric oscillator (OPO). The DBR is rapidly step-tuned over the methane absorption at several discrete wavelengths. This multi-wavelength approach enables us to sample the entire methane lineshape and reduce systematic errors.

Atmospheric methane trends↗
DOE OSTI2015

Surface Assisted Formation of methane Hydrates on Ice and Na Montmorillonite Clay

Methane hydrates are extremely important naturally-occurring crystalline materials that impact climate change, energy resources, geological hazards, and other major environmental issues. Whereas significant experimental effort has been completed to understanding the bulk thermodynamics of methane hydrate assemblies, little is understood on heterogeneous nucleation and growth of methane hydrates in clay-rich environments. Controlled synthesis experiments were completed at 265-285 K and 6.89 MPa to examine the impact of montmorillonite surfaces in clay-ice mixtures to nucleate and form methane hydrate. The results suggest that the hydrophilic and methane adsorbing properties of Namontmorillonite reduce the nucleation period of methane hydrate formation in pure ice systems.

clathrate hydrate↗
DOE OSTI2016

A large increase in U.S. methane emissions over the past decade inferred from satellite data and surface observations

Abstract The global burden of atmospheric methane has been increasing over the past decade, but the causes are not well understood. National inventory estimates from the U.S. Environmental Protection Agency indicate no significant trend in U.S. anthropogenic methane emissions from 2002 to present. Here we use satellite retrievals and surface observations of atmospheric methane to suggest that U.S. methane emissions have increased by more than 30% over the 2002–2014 period. The trend is largest in the central part of the country, but we cannot readily attribute it to any specific source type. This large increase in U.S. methane emissions could account for 30–60% of the global growth of atmospheric methane seen in the past decade.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2016

Dry Reforming of Methane on a Highly‐Active Ni‐CeO 2 Catalyst: Effects of Metal‐Support Interactions on C−H Bond Breaking

Abstract Ni‐CeO 2 is a highly efficient, stable and non‐expensive catalyst for methane dry reforming at relative low temperatures (700 K). The active phase of the catalyst consists of small nanoparticles of nickel dispersed on partially reduced ceria. Experiments of ambient pressure XPS indicate that methane dissociates on Ni/CeO 2 at temperatures as low as 300 K, generating CH x and CO x species on the surface of the catalyst. Strong metal–support interactions activate Ni for the dissociation of methane. The results of density‐functional calculations show a drop in the effective barrier for methane activation from 0.9 eV on Ni(111) to only 0.15 eV on Ni/CeO 2− x (111). At 700 K, under methane dry reforming conditions, no signals for adsorbed CH x or C species are detected in the C 1s XPS region. The reforming of methane proceeds in a clean and efficient way.

Liu, Zongyuan↗
DOE OSTI2014

Single iron sites for catalytic, nonoxidative conversion of methane

In this paper we discuss how the availability of inexpensive natural gas from the fracturing of shale and as a byproduct of oil production has stimulated the investigation of catalytic processes for the direct conversion of methane to products. Efforts in this direction are further driven by the desire to avoid the generation of CO 2 and its emission to the atmosphere, as occurs when methane is steam-reformed to produce synthesis gas, a mixture of CO and H 2 that can be used for the production of fuels and chemicals via Fischer-Tropsch synthesis. During the past forty years, numerous investigators have attempted to convert methane to higher value products by either thermal dehydrogenation or by oxidative dehydrogenation. While methane can be converted to benzene and hydrogen via thermal dehydrogenation, this process is accompanied by the deposition of large amounts of coke, leading to rapid catalyst deactivation. The oxidative coupling of methane has focused on the formation of ethylene, but this chemistry is not selective and also results in a substantial combustion of methane to CO 2 and water.

Bell, Alexis T.↗
DOE OSTI2025

Methane pyrolysis by Joule heating for graphitic carbon and hydrogen production

The global energy transition toward sustainability requires technologies that can decarbonize energy carriers and fuels while producing valuable materials. Methane, a primary component of natural gas, is both a high-energy-density fuel and a significant greenhouse gas. This study reports an approach for methane pyrolysis utilizing Joule heating within the deposition substrate to drive the endothermic reaction. With electric current passing through a resistive porous carbon cloth, heat is generated to break C-H bonds of methane molecules. Here, the decomposition of methane as it flows through the cloth results in hydrogen production and the formation of conformally layered graphite around the carbon fibers. The effects of input power, chamber pressure, feedstock flow rate, and process duration on hydrogen and graphite production are characterized via in situ mass spectrometry and laser absorption spectroscopy, resulting in methane conversion rates up to 88%, with hydrogen and carbon yields of 82% and 72%, respectively. Material characterization verifies uniform high-quality graphite deposition, with a Raman I D /I G ratio of 0.1 and 3.38 Å d-spacing. This Joule heating method for catalyst-free methane pyrolysis offers the potential for advancing hydrogen production technology by simultaneously producing valuable materials such as solid graphite, thus enhancing the economic viability of the fuel decarbonization process.

Energy Resources↗
DOE OSTI2021

Effect of Ni particle size on the production of renewable methane from CO 2 over Ni/CeO 2 catalyst

Production of ‘renewable Methane’ has attracted renewed research interest as a fundamental probe reaction and process for CO 2 utilization through potential use in C1 fuel production and even for future space exploration technologies. CO 2 methanation is a structure sensitive reaction on Ni/CeO 2 catalysts. To precisely elucidate the size effect of the Ni metal center on the CO 2 methanation performance, we prepared 2%Ni/CeO 2 catalysts with pre-synthesized uniform Ni particles (2, 4 and 8 nm) on a high surface area CeO 2 support. Transmission electron microscopy (TEM) and ambient pressure X-ray photo spectroscopy (AP-XPS) characterization have confirmed that the catalyst structure and chemical state was uniform and stable under reaction conditions. The 8 nm sized catalyst showed superior methanation selectivity over the 4 and 2 nm counterparts, and the methanation activity in term of TOF is 10 times and 70 times higher than for the 4 and 2 nm counterparts, respectively. Here, the DRIFTS studies revealed that the larger Ni (8 nm particles) over CeO 2 efficiently facilitated the hydrogenation of the surface formate intermediates, which is proposed as the rate determining step accounting for the excellent CO 2 methanation performance.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Historic and modern approaches for discovery of abandoned wells for methane emissions mitigation in Oil Creek State Park, Pennsylvania

Hundreds of oil wells were drilled along Oil Creek in Pennsylvania in the mid-16 1800s, birthing the modern oil industry. No longer in operation, many wells are now classified as abandoned, and, due to their age, their locations are either unknown or inaccurately recorded. These historic well sites present environmental, safety, and economic concerns in the form of possible methane leaks and physical hazards. Airborne magnetic and LiDAR surveys were conducted in the Pioneer Run watershed in Oil Creek State Park to find abandoned wells in a historically significant but physically challenging location. Wells were drilled in this area prior to modern geolocation and legal documentation. Although a large number of old wells were abandoned summarily without remediation of the site, much of the land area within Oil Creek State Park is now covered in trees and dense underbrush, which can obscure wellheads. The thick vegetation and steep terrain limited the possibility of ground-based surveys to easily find well sites for methane emissions studies. The data from remote sensing surveys were used to corroborate potential well locations from historic maps and photographs. Potential well sites were verified in a ground-based field survey and monitored for methane emissions. Two historic photographs documenting oil activity in the late 1800s were georeferenced using a combination of magnetic and LiDAR data. LiDAR data, which were more useful in georeferencing and in field verification, identified 290 field locations in the Pioneer Run watershed, 86% of which were possible well sites. Sixty-two percent of the ground-verified wells remained unplugged and comprised the majority of leaking wells. The mean methane emissions factor for unplugged wells was 0.027 ± 0.099 kg/day, lower than other Appalachian Basin methane emissions estimates. LiDAR was used for the first time, in combination with an airborne magnetic survey, to reveal underground oil industry features and inform well identification and remediation efforts in difficult-to-navigate regions. In the oldest oil fields, where well casing has been removed or wood conductor casing was installed, historic photographs provide additional lines of evidence for oil wells where ground disturbances have concealed surface features. Identification of well sites is necessary for mitigation efforts, as unplugged wells emit methane, a potent greenhouse gas.

02 PETROLEUM↗
DOE OSTI2021

Methane Exhaust Measurements at Gathering Compressor Stations in the United States

Unburned methane entrained in exhaust from natural gas-fired compressor engines (“combustion slip”) can account for a substantial portion of station-level methane emissions. A novel in-stack, tracer gas method was coupled with Fourier transform infrared (FTIR) species measurements to quantify combustion slip from natural gas compressor engines at 67 gathering and boosting stations owned or managed by nine “study partner” operators in 11 U.S. states. The mean methane emission rate from 63 four-stroke, lean-burn (4SLB) compressor engines was 5.62 kg/h (95% CI = 5.15–6.17 kg/h) and ranged from 0.3 to 12.6 kg/h. The mean methane emission rate from 39 fourstroke, rich-burn (4SRB) compressor engines was 0.40 kg/h (95% CI = 0.37– 0.42 kg/h) and ranged from 0.01 to 4.5 kg/h. Study results for 4SLB engines were lower than both the U.S. EPA compilation of air pollutant emission factors (AP-42) and Inventory of U.S. Greenhouse Gas Emissions and Sinks (GHGI) by 8 and 9%, respectively. Study results for 4SRB engines were 43% of the AP-42 emission factor and 8% of the GHGI emission factor, the latter of which does not distinguish between engine types. Total annual combustion slip from the U.S. natural gas gathering and boosting sector was modeled using measured emission rates and compressor unit counts from the U.S. EPA Greenhouse Gas Reporting Program. Modeled results [328 Gg/y (95% CI = 235–436 Gg/y) of unburned methane] would account for 24% (95% CI = 17–31%) of the 1391 Gg of methane emissions for “Gathering and Boosting Stations”, or 6% of the net emissions for “Natural Gas Systems” (5598 Gg) as reported in the 2020 U.S. EPA GHGI. In conclusion, gathering and boosting combustion slip emissions reported in the 2020 GHGI (374 Gg) fall within the uncertainty of this model.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Plasma-Catalyst Synergy in the One-Pot Nonthermal Plasma-Assisted Synthesis of Aromatics from Methane

Electrification of the methane dehydroaromatization reaction with the use of nonthermal plasmas could alleviate the high-temperature requirement for this process while promoting the formation of valuable aromatics. Here, in this work, we evaluate the use of nonthermal plasma to investigate methane activation and conversion to aromatics by systematically varying bulk gas temperature in a one-pot, plasma-stimulated catalytic reactor over Mo/H-ZSM-5 and metal-free H-ZSM-5 catalysts. We report that Mo is not required for methane activation under low-temperature plasma conditions (573–773 K), and methane conversions up to ~15% with a 1:1 methane/N 2 feed are obtained under a 10 W plasma. However, Mo contributes to the formation of aromatics in the presence of a plasma at 773 K, achieving close to a 2-fold increase in the production of aromatics when compared to unmodified H-ZSM-5. Further, the exposure of as-prepared Mo/H-ZSM-5 to the methane plasma feed induces the formation of Mo-carbide phases in the temperature range studied. These findings highlight the complex roles of nonthermal plasmas in the direct activation of methane and the importance of plasma-catalyst design to facilitate aromatization reactions under plasma-assisted reaction conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

Mechanism of Methane Chemical Looping Combustion with Hematite Promoted with CeO 2

Chemical looping combustion (CLC) is a promising technology for fossil fuel combustion that produces sequestration-ready CO{sub 2} stream, reducing the energy penalty of CO{sub 2} separation from flue gases. An effective oxygen carrier for CLC will readily react with the fuel gas and will be reoxidized upon contact with oxygen. This study investigated the development of a CeO{sub 2}-promoted Fe{sub 2}O{sub 3}-hematite oxygen carrier suitable for the methane CLC process. Composition of CeO{sub 2} is between 5 and 25 wt % and is lower than what is generally used for supports in Fe{sub 2}O{sub 3} carrier preparations. The incorporation of CeO{sub 2} to the natural ore hematite strongly modifies the reduction behavior in comparison to that of CeO{sub 2} and hematite alone. Temperature-programmed reaction studies revealed that the addition of even 5 wt % CeO{sub 2} enhances the reaction capacity of the Fe{sub 2}O{sub 3} oxygen carrier by promoting the decomposition and partial oxidation of methane. Fixed-bed reactor data showed that the 5 wt % cerium oxides with 95 wt % iron oxide produce 2 times as much carbon dioxide in comparison to the sum of carbon dioxide produced when the oxides were tested separately. This effect is likely due to the reaction of CeO{sub 2} with methane forming intermediates, which are reactive for extracting oxygen from Fe{sub 2}O{sub 3} at a considerably faster rate than the rate of the direct reaction of Fe{sub 2}O{sub 3} with methane. These studies reveal that 5 wt % CeO{sub 2}/Fe{sub 2}O{sub 3} gives stable conversions over 15 reduction/oxidation cycles. Lab-scale reactor studies (pulsed mode) suggest the methane reacts initially with CeO{sub 2} lattice oxygen to form partial oxidation products (CO + H{sub 2}), which continue to react with oxygen from neighboring Fe{sub 2}O{sub 3}, leading to its complete oxidation to form CO{sub 2}. The reduced cerium oxide promotes the methane decomposition reaction to form C + H{sub 2}, which continue to react with Fe{sub 2}O{sub 3}/Fe{sub 3}O{sub 4} to form CO/CO{sub 2} and H{sub 2}O. This mechanism is supported by the characterization studies, which also suggest that the formation of carbonaceous intermediates may affect the reaction rate and selectivity of the oxygen carrier.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Variations in Gas and Water Pulses at an Arctic Seep: Fluid Sources and Methane Transport

Methane fluxes into the oceans are largely dependent on the methane phase as it migrates upward through the sediments. Here we document decoupled methane transport by gaseous and aqueous phases in Storfjordrenna (offshore Svalbard) and propose a three-stage evolution model for active seepage in the region where gas hydrates are present in the shallow subsurface. In a preactive seepage stage, solute diffusion is the primary transport mechanism for methane in the dissolved phase. Fluids containing dissolved methane have high 87 Sr/ 86 Sr ratios due to silicate weathering in the microbial methanogenesis zone. During the active seepage stage, migration of gaseous methane results in near-seafloor gas hydrate formation and vigorous seafloor gas discharge with a thermogenic fingerprint. In the postactive seepage stage, the high concentration of dissolved lithium points to the contribution of a deeper-sourced aqueous fluid, which we postulate advects upward following cessation of gas discharge.

58 GEOSCIENCES↗
DOE OSTI2020

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 = 10 12 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 CH 4 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 CH 4 year -1 , we estimated that the global net land methane emissions are 149–176 Tg CH 4 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.

58 GEOSCIENCES↗
DOE OSTI2020

Anaerobic methane oxidation coupled to manganese reduction by members of the Methanoperedenaceae

Abstract Anaerobic oxidation of methane (AOM) is a major biological process that reduces global methane emission to the atmosphere. Anaerobic methanotrophic archaea (ANME) mediate this process through the coupling of methane oxidation to different electron acceptors, or in concert with a syntrophic bacterial partner. Recently, ANME belonging to the archaeal family Methanoperedenaceae (formerly known as ANME-2d) were shown to be capable of AOM coupled to nitrate and iron reduction. Here, a freshwater sediment bioreactor fed with methane and Mn(IV) oxides (birnessite) resulted in a microbial community dominated by two novel members of the Methanoperedenaceae, with biochemical profiling of the system demonstrating Mn(IV)-dependent AOM. Genomic and transcriptomic analyses revealed the expression of key genes involved in methane oxidation and several shared multiheme c-type cytochromes (MHCs) that were differentially expressed, indicating the likely use of different extracellular electron transfer pathways. We propose the names “Candidatus Methanoperedens manganicus” and “Candidatus Methanoperedens manganireducens” for the two newly described Methanoperedenaceae species. This study demonstrates the ability of members of the Methanoperedenaceae to couple AOM to the reduction of Mn(IV) oxides, which suggests their potential role in linking methane and manganese cycling in the environment.

54 ENVIRONMENTAL SCIENCES↗