Highly active Ni/CeO2 catalyst for CO2 methanation: Preparation and characterization
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99 GENERAL AND MISCELLANEOUS↗
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Methane oxidation activity and nanoscale characterization of Pd/CeO2 catalysts prepared by dry milling Pd acetate and ceria
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99 GENERAL AND MISCELLANEOUS↗
Creating Accurate Methane Emission Inventories through Data-Driven Airborne Survey Strategies
Because natural gas emits less carbon than other fossil fuels, it holds promise as a green energy transition fuel. However, the overall carbon footprint of natural gas is significantly elevated by methane emissions that occur during its production and transmission (Cusworth et al. 2022). Methane “super-emitters,†while comprising only about 1% of sites, are responsible for the majority of oil- and gas-sourced methane emissions, making their detection and mitigation critical in reducing the climate impact of natural gas and in meeting national and global sustainability goals (Sherwin et al. 2024). Yet, despite advancements in detection, significant uncertainties remain regarding the size, frequency, and duration distributions of methane emissions (e.g., Frankenberg et al. 2016, Cusworth et al. 2022, Chen, Sherwin et al. 2022, Conrad et al. 2023, Johnson et al. 2023, Sherwin et al. 2024) underscoring the need for comprehensive emissions inventories segmented by basin across the US. Airborne surveys are well-suited for collecting data to build these comprehensive, basin-level inventories because they allow for extensive spatial coverage, and have the spatial resolution, and the sensitivity to pinpoint individual methane sources. As remote sensing technologies enable rapid basin-scale surveys, it is imperative to establish scientifically and statistically robust standards to generate reliable and actionable emissions inventories. Recent work has shown that differences in airborne sampling strategies, detection technologies, and analysis can lead to large differences between survey conclusions if not correctly accounted for (Chen et al. 2024). This elevates the importance of incorporating proper sampling and analysis techniques when designing a methane emissions monitoring campaign to produce accurate results and facilitate cross-study comparisons. In this paper, we describe a survey strategy designed using the latest conclusions from the literature to align results from different aerial surveys. We identify several sampling and analysis principles, including large sample sizes, balanced sampling across oil and gas production, careful survey area definition, and a unified protocol for analysis, to be vital to producing an unbiased estimate of basin-scale emissions. We present results from a Department of Energy-funded project that deployed this survey strategy in two understudied oil and gas- producing regions in the United States: the Haynesville Basin in Texas and Louisiana, and the Woodford Shale in the Anadarko Basin in Oklahoma.
03 NATURAL GAS↗
Three-Dimensional Free Gas Flow Focuses Basin-Wide Microbial Methane to Concentrated Methane Hydrate Reservoirs in Geological System
Here, we present a systematic model that links the generation, migration, phase partitioning, and accumulation of methane into a closed loop as the sediment is deposited from the seafloor and buried through the base of hydrate stability zone (BHSZ). In our model, methane is generated by biodegradation of organic carbon in muds. Hydrate does not form and methane is not trapped until a coarse-grained layer is deposited, because the small pores prevent hydrate formation in muds. Instead, methane diffuses into sands/silts where methane solidifies into hydrate. As hydrate-bearing sands/silts pass through the BHSZ during sediment burial, methane hydrate dissociates, and releases free gas. The released and the newly generated free gas below the BHSZ concentrates into a vertical/dipping zone with low capillary entry pressure and high permeability and flows upward driven its buoyancy. When free gas reaches the hydrate stability zone (HSZ), capillary forces drive free gas to flow laterally, preferentially enter sands/silts, feed hydrate growth, and elevate hydrate saturation. With three-dimensional focused free gas flow, microbial methane that is generated from a much larger fetch area of the entire basin, both above and below the BHSZ, is concentrated into coarse-grained layers at structural closures for hydrate formation. Our model illustrates how geological evolution, microbial methane generation, and gas flow by buoyancy couple to generate concentrated hydrate deposits in geological system. These insights can be used to explore for high-concentration methane hydrate and are important for understanding the methane budget and carbon cycle under the seafloor.
58 GEOSCIENCES↗
Carbonate-hosted microbial communities are prolific and pervasive methane oxidizers at geologically diverse marine methane seep sites
At marine methane seeps, vast quantities of methane move through the shallow subseafloor, where it is largely consumed by microbial communities. This process plays an important role in global methane dynamics, but we have yet to identify all of the methane sinks in the deep sea. Here, we conducted a continental-scale survey of seven geologically diverse seafloor seeps and found that carbonate rocks from all sites host methane-oxidizing microbial communities with substantial methanotrophic potential. In laboratory-based mesocosm incubations, chimney-like carbonates from the newly described Point Dume seep off the coast of Southern California exhibited the highest rates of anaerobic methane oxidation measured to date. After a thorough analysis of physicochemical, electrical, and biological factors, we attribute this substantial metabolic activity largely to higher cell density, mineral composition, kinetic parameters including an elevated V max , and the presence of specific microbial lineages. Our data also suggest that other features, such as electrical conductance, rock particle size, and microbial community alpha diversity, may influence a sample’s methanotrophic potential, but these factors did not demonstrate clear patterns with respect to methane oxidation rates. Based on the apparent pervasiveness within seep carbonates of microbial communities capable of performing anaerobic oxidation of methane, as well as the frequent occurrence of carbonates at seeps, we suggest that rock-hosted methanotrophy may be an important contributor to marine methane consumption.
58 GEOSCIENCES↗
Surface Interactions and Nanoconfinement of Methane and Methane plus CO2 Revealed by High-Pressure Magic Angle Spinning NMR Spectroscopy and Molecular Dynamics
This study explores the fundamental, molecular- to microscopic-level behavior of methane gas confined into nanoporous silica proxies with different pore diameters and surface-to-volume (S/V) ratios. Surfaces and pore walls of nanoporous silica matrices are decorated with hydroxyl (-OH) groups, resembling natural heterogeneity. High-pressure MAS NMR was utilized to characterize the interactions between methane and the engineered nanoporous silica proxies under various temperature and pressure regimes. There was a change in the chemical shift position of confined methane slightly in the mixtures with nanoporous silica up to 393 K, as shown by high-pressure 13C-NMR. The 13C-NMR chemical shift of methane was changed by pressure, explained by the densification of methane inside the nanoporous silica materials. The influence of pore diameter and S/V of the nanoporous silica materials on the behaviors and dynamics of methane were studied. The presence of CO2 in mixtures of silica and methane needs analysis with caution because CO2 in a supercritical state and gaseous CO2 change the original structure of nanoporous silica and change surface area and pore volume. According to simulation, the picosecond scale dynamics of methane confined in larger pores of amorphous silica is faster. In the 4 nm pore, the diffusivity obtained from MD simulations in the pore with a higher S/V ratio is slower due to the trapping of methane molecules in adsorbed layers close to the corrugated pore surface. In contrast, relaxation measured with NMR for smaller pores (higher S/V) exhibits larger T1, indicating slower relaxation.
03 NATURAL GAS↗
Plant‐mediated methane transport in emergent and floating‐leaved species of a temperate freshwater mineral‐soil wetland
Abstract Methane flux from freshwater mineral‐soil (FWMS) wetlands and its variability among sites is largely modulated by plant‐mediated transport. However, plant‐mediated transport processes are rarely resolved in land surface models and are poorly parametrized for plants commonly found in FWMS wetlands. Here, relationships between methane flux and CO 2 uptake, as well as plant conductance of methane were evaluated for three plant species and two characteristic functional types: emergent (narrow‐leaved cattail) and floating‐leaved (American lotus and water lily). We found significant but contrasting correlations between methane flux and CO 2 uptake in cattails ( r 2 = 0.51, slope = −0.16, during morning) and water lily ( r 2 = 0.32, slope = 0.064, after midday). This relationship was not significant in American lotus, showing that stomata regulation of methane fluxes is species‐specific and not generalizable across the floating‐leaved plant functional type. Conductance of methane per leaf area showed distinct seasonal dynamics across species. Conductance was similar among the floating‐leaved species (6.2 × 10 −3 m d −1 in lotus and 7.2 × 10 −3 m d −1 in water lily) and higher than conductance in the emergent species (2.7 × 10 −3 m d −1 ). Our results provide direct observations of plant conductance rates and identify the vegetation parameters (leaf area, stomatal conductance) that modify them. Our results further suggest that models of methane emissions from FWMS should parameterize plant‐mediated transport in different plant functional types, scaled by leaf area and with variable seasonal phenological dynamics, and consider possible species‐specific mechanisms that control methane transport through plants.
Villa, Jorge A.↗
Large reductions in Permian Basin methane intensity shown in multi-year comparison of aerially-visible methane emissions
Spanning the US states of Texas and New Mexico, the Permian Basin has been a hotspot of methane emissions from oil and natural gas activity 1–4, although studies disagree over the magnitude of these emissions. The most comprehensive measurement campaigns published were conducted in 2019 1–5 .There have been large changes in the energy industry since then, including in the prices of oil and gas, both state and federal regulatory environments, investor and activist pressure over methane emissions, and the adoption of new technologies and policies by energy operators. Understanding how any or all of these might influence methane emissions is important for policy makers, oil and gas operators, and other stakeholders. We characterize the time evolution of Permian Basin methane emissions using a series of comprehensive aerial surveys conducted every year from 2020-2023 and compare them to the 2019 results cited above. To maintain comparability, all the data sets are from surveys using Insight M point source methane sensing technology. The scope of these surveys expanded over time: from 33-46% of wells, oil production, and gas production in 2020 to 60-65% in 2021, to 84% of wells and over 90% of both oil and gas production in 2023. These surveys by Insight M also include hundreds of gas processing plants and compressor stations as well as 1000s of km of gathering and transmission pipelines. Considering only the aerially detected portion of emissions (typically the majority of the total in such surveys 4), we find reductions of more than 70% in methane emissions intensity compared to the 2019 New Mexico-only Insight M survey, with variation depending on the year 3,4. Notably, although sources below 100 kg/hr contributed less than 10% of aerially measured emissions the 2019 New Mexico survey 3, these smaller sources constitute a larger proportion of total aerially measured emissions (although not the majority) in 2020-2023. Production facilities and gathering pipelines are responsible for the larges shares of total emissions, followed by compressor stations and gas processing plants. Permian methane emissions were also measured in a comprehensive 2019 Permian-wide survey by the Carbon Mapper team 2. That analysis led to a lower total emissions estimate at the time 4. These new Insight M-based emission rates are still roughly 30-70% lower than the aerially measured portion of the 2019 Carbon Mapper-based estimates 4. Further work is needed to harmonize these surveys in space and time to create the most intercomparable numbers possible 5. Additional analysis is needed to compare our findings to the more spatially constrained 2020, 2021, and 2023 Carbon Mapper surveys in the Permian 4,6. The evidence is strong from these two survey teams that emissions intensity has declined significantly since 2019. Reasons for this trend are currently unclear but point to possible success of emissions control programs. Future work investigating frequency, source, and operator-specific intensities could provide insights into the causes of this promising trend.
methane, oil and gas, data science, remote sensing↗
Combined Experimental and Modeling Study of Microwave-Assisted Methane Dehydroaromatization Process
ACS Fall Meeting 2022, Chicago, IL, August 21-25, 2022
Bai, Xinwei↗
On the Relationship Between Methane Production in Anaerobic Incubations of Peat Material and In Situ Methane Emissions
Anaerobic incubations of peat have been widely used to explore soil processes, but this in vitro technique raises many questions as to how well it reproduces in situ conditions. To investigate this, we conducted 60–100 days (+25 days pre‐incubation) anaerobic, temperature‐controlled incubation experiments across a temperature range of 1–26°C on samples from bog and fen habitats, at two different depths (9–19 and 25–35 cm). Here, we observed exponential increases in CO 2 and methane production with temperature in all conditions. We then compared field‐based measurements of methane emission with modeled expectations by extrapolating incubation‐determined methane production rates based on (a) soil temperature profiles, (b) the observed incubation temperature‐methane production relationship, and (c) seasonal thaw depth from each site. The resulting incubation‐extrapolated methane production agreed with measured emission rates within a factor of two at both sites and corresponded to 182 ± 54% and 59 ± 14% of the measured average yearly fluxes from the field for the bog and fen, respectively. The underestimation of fen methane fluxes may be due to the lack of living plant root‐derived dissolved organic carbon inputs in incubations, a key process in fens. Conversely, the overestimation in bogs could be attributed to methane oxidation in the field, which is absent in anaerobic incubation conditions. Nonetheless incubations predicted greenhouse gas emissions from a northern peatland within a factor of two.
Biological and medical sciences,Geosciences,Enviro↗
Global methane emissions from coal mining to continue growing even with declining coal production
This paper presents projections of global methane emissions from coal mining under different coal extraction scenarios and with increasing mining depth through 2100. The paper proposes an updated methodology for calculating fugitive emissions from coal mining, which accounts for coal extraction method, coal rank, and mining depth and uses evidence-based emissions factors. A detailed assessment shows that coal mining-related methane emissions in 2010 were higher than previous studies show. This study also uses a novel methodology for calculating methane emissions from abandoned coal mines and represents the first estimate of future global methane emissions from those mines. The results show that emissions from abandoned mines increase faster than those from active ones. Using coal production data from six integrated assessment models, this study shows that by 2100 methane emissions from active underground mines increase by a factor of 4, while emissions from abandoned mines increase by a factor of 8. Abandoned mine methane emissions continue through the century even with aggressive mitigation actions.
coal mine methane, abandoned coal mine methane, em↗
Methane, ethane, and propane production in Greenland ice core samples and a first isotopic characterization of excess methane
Air trapped in polar ice provides unique records of the past atmospheric composition ranging from key greenhouse gases such as methane (CH 4 ) to short-lived trace gases like ethane (C 2 H 6 ) and propane (C 3 H 8 ). Recently, the comparison of CH 4 records obtained using different extraction methods revealed disagreements in the CH 4 concentration for the last glacial in Greenland ice. Elevated methane levels were detected in dust-rich ice core sections measured discretely, pointing to a process sensitive to the melt extraction technique. To shed light on the underlying mechanism, we performed targeted experiments and analyzed samples for methane and the short-chain alkanes ethane and propane covering the time interval from 12 to 42 kyr. Here, we report our findings of these elevated alkane concentrations, which scale linearly with the amount of mineral dust within the ice samples. The alkane production happens during the melt extraction step of the classic wet-extraction technique and reaches 14 to 91 ppb of CH 4 excess in dusty ice samples. We document for the first time a co-production of excess methane, ethane, and propane, with the observed concentrations for ethane and propane exceeding their past atmospheric background at least by a factor of 10. Independent of the produced amounts, excess alkanes were produced in a fixed molar ratio of approximately 14 : 2 : 1, indicating a shared origin. The measured carbon isotopic signature of excess methane is (-47.0 ± 2.9) ‰ and its deuterium isotopic signature is (-326 ± 57) ‰. With the co-production ratios of excess alkanes and the isotopic composition of excess methane we established a fingerprint that allows us to constrain potential formation processes. This fingerprint is not in line with a microbial origin. Moreover, an adsorption–desorption process of thermogenic gas on dust particles transported to Greenland does not appear very likely. Instead, the alkane pattern appears to be indicative of abiotic decomposition of organic matter as found in soils and plant leaves.
54 ENVIRONMENTAL SCIENCES↗
Enhanced CO 2 Methanation Activity of Sm 0.25 Ce 0.75 O 2-δ –Ni by Modulating the Chelating Agents-to-Metal Cation Ratio and Tuning Metal–Support Interactions
Highly active and selective CO 2 methanation catalysts are critical to CO 2 upgrading, synthetic natural gas production, and CO 2 emission reduction. Wet impregnation is widely used to synthesize oxide-supported metallic nanoparticles as the catalyst for CO 2 methanation. However, as the reagents cannot be homogeneously mixed at an atomic level, it is challenging to modulate the microstructure, crystal structure, chemical composition, and electronic structure of catalysts via wet impregnation. In this work, a scalable and straightforward catalyst fabrication approach has been designed and validated to produce Sm 0.25 Ce 0.75 O 2-δ -supported Ni (SDC–Ni) as the CO 2 methanation catalyst. By varying the chelating agents-to-total metal cations ratio (C/I ratio) during the catalyst synthesis, we can readily and simultaneously modulate the microstructure, metallic surface area, crystal structure, chemical composition, and electronic structure of SDC–Ni, consequently fine-tuning the oxide–support interactions and CO 2 methanation activity. The optimal C/I ratio (0.1) leads to an SDC–Ni catalyst that facilitates C–O bond cleavage and significantly improves CO 2 conversion at 250 °C. A CO 2 -to-CH 4 yield of >73% has been achieved at 250 °C. Furthermore, a stable operation of >1500 hours has been demonstrated, and no degradation is observed. Extensive characterizations were performed to fundamentally understand how to tune and enhance CO 2 methanation activity of SDC–Ni by modulating the C/I ratio. The correlation of physical, chemical, and catalytic properties of SDC–Ni with the C/I ratio is established and thoroughly elaborated in this work. This study could be applied to tune the oxide–support interactions of various catalysts for enhancing the catalytic activity.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Direct methane activation by atomically thin platinum nanolayers on two-dimensional metal carbides
We report efficient and direct conversion of methane to value-added products has been a long-term challenge in shale gas applications. Here, we show that atomically thin nanolayers of Pt with a single or double atomic layer thickness, supported on a two-dimensional molybdenum titanium carbide (MXene), catalyse non-oxidative coupling of methane to ethane/ethylene (C 2 ). Kinetic and theoretical studies, combined with in-situ spectroscopic and microscopic characterizations, demonstrate that Pt nanolayers anchored at the hexagonal close-packed sites of the MXene support can activate the first C–H bond of methane to form methyl radicals that favour desorption over further dehydrogenation and thus suppress coke deposition. At 750 °C and 7% methane conversion, the catalyst runs for 72 hours of continuous operation without deactivation and exhibits >98% selectivity towards C 2 products, with a turnover frequency of 0.2–0.6 s -1 . Our findings provide insights into the design of highly active and stable catalysts for methane activation and create a platform for developing atomically thin supported metal catalysts.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Comparative study of oxygen-limited and methane-limited growth phenotypes of Methylomicrobium buryatense 5GB1
Not provided.
Biotechnology & Applied Microbiology↗
SPRUCE Anaerobic oxidation of methane mitigates net methane production and responds to long-term experimental warming in a northern bog: Supporting data
This data set contains measurements of anaerobic oxidation of methane (AOM), net methane (CH4) production, carbon dioxide (CO2) production, and gross CH4 production measurements from the SPRUCE experiment (Hanson et al. 2017). CH4 is greenhouse gas with 45 times the sustained global warming potential of CO2 over 100 years, which may have significant implications on global climate change. The process of AOM plays a large role in the extent of CH4 emissions from wetland environments like those at the SPRUCE experiment site. This study conducted two on different dates. In experiment 1, net CH4 and CO2 production were measured with a gas chromatograph through the peat profile at in situ temperatures of the SPRUCE plots four times from May to October, 2016 (2016-05 to 2016-10). Two treatments were examined, a Porewater Treatment that was a 1:1 volumetric peat:porewater slurry and a No Porewater Treatment that was field-moist peat with no porewater added. Additionally, net CH4 production were measured at frequent intervals (from 4 hr to 9 d) in peat from selected SPRUCE plots from soil collected on October 16, 2016 (2016-10-16). Samples were collected from the SPRUCE plots, immediately made anaerobic, and transported to the University of Oregon for rate measurements within several days of collection. In experiment 2, AOM, net CH4 production, CO2 production, and gross CH4 production were measured through the peat profile at in situ field temperatures once from samples collected in July, 2021 (2021-07). The same two porewater treatments were examined. AOM was measured with a 13CH4 tracer method using a Picarro G2201-i analyzer for isotopic CO2/CH4 quantification with a small stable isotope module attached. This data set contains three data files in comma separate (*.csv) format. This data set is associated with the following publication: Barney, M, AM Hopple, LL Gregory, JK Keller, and SD Bridgham. 2024. Anaerobic oxidation of methane mitigates net methane production and responds to long-term experimental warming in a northern bog. Soil Biology and Biochemistry, 190, 109316. https://doi.org/10.1016/j.soilbio.2024.109316.
SPRUCE Experiment, Marcell Experimental Forest, Me↗
Experimental Insights into the Coupling of Methane Combustion and Steam Reforming in a Catalytic Plate Reactor in Transient Mode
The microstructured reactor concept is very promising technology to develop a compact reformer for distributed hydrogen generation. In this work, a catalytic plate reactor (CPR) is developed and investigated for the coupling of methane combustion (MC) and methane steam reforming (MSR) over Pt/Al 2 O 3 -coated microchannels in cocurrent and counter-current modes in transient experiments during start-up. A three-dimensional (3D) computational fluid dynamics (CFD) simulation shows uniform velocity and pressure distribution profiles in microchannels. For a channel velocity from 5.1 to 57.3 m/s in the combustor, the oxidation of methane is complete and self-sustainable without explosion, blow-off, or extinction; nevertheless, flashbacks are observed in counter-current mode. In the reformer, the maximum methane conversion is 84.9% in cocurrent mode, slightly higher than that of 80.2% in counter-current mode at a residence time of 33 ms, but at the cost of three times higher energy input in the combustor operating at ~1000 °C. Nitric oxide (NO) is not identified in combustion products, but nitrous oxide (N 2 O) is a function of coupling mode and forms significantly in cocurrent mode. Furthermore, this research would be helpful to establish the start-up strategy and environmental impact of compact reformers on a small scale.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗