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At least 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Active Thermochemical Tables: Sequential Bond Dissociation Enthalpies of Methane, Ethane, and Methanol and the Related Thermochemistry

Active Thermochemical Tables (ATcT) thermochemistry for the sequential bond dissociations of methane, ethane, and methanol systems were obtained by analyzing and solving a very large thermochemical network (TN). Values for all possible C–H, C–C, C–O, and O–H bond dissociation enthalpies at 298.15 K (BDE298) and bond dissociation energies at 0 K (D0) are presented. The corresponding ATcT standard gas-phase enthalpies of formation of the resulting CHn, n = 4–0 species (methane, methyl, methylene, methylidyne, and carbon atom), C2Hn, n = 6–0 species (ethane, ethyl, ethylene, ethylidene, vinyl, ethylidyne, acetylene, vinylidene, ethynyl, and ethynylene), and COHn, n = 4–0 species (methanol, hydroxymethyl, methoxy, formaldehyde, hydroxymethylene, formyl, isoformyl, and carbon monoxide) are also presented. The ATcT thermochemistry of carbon dioxide, water, hydroxyl, and carbon, oxygen, and hydrogen atoms is also included, together with the sequential BDEs of CO2 and H2O. The provenances of the ATcT enthalpies of formation, which are quite distributed and involve a large number of relevant determinations, are analyzed by variance decomposition and discussed in terms of principal contributions. The underlying reasons for periodic appearances of remarkably low and/or unusually high BDEs, alternating along the dissociation sequences, are analyzed and quantitatively rationalized. The present ATcT results are the most accurate thermochemical values currently available for these species.

Active Thermochemical Tables↗
DOE OSTI2019

Simulating Enhanced Methane Deliverable Capacity of Guest Responsive Pores in Intrinsically Flexible MOFs

In this work, a novel computational procedure, based on the principles of flat-histogram Monte Carlo, is developed for facile prediction of the adsorption thermodynamics of intrinsically flexible adsorbents. We then demonstrate how an accurate prediction of methane deliverable capacity in a metal–organic framework (MOF) with significant intrinsic flexibility requires use of such a method. Dynamic side chains in the framework respond to methane adsorbates and reorganize to exhibit a more conducive pore space at high adsorbate densities while simultaneously providing a less conducive pore space at low adsorbate densities. This “responsive pore” MOF achieves ~20% higher deliverable capacity than if the framework were rigid and elucidates a strategy for designing high deliverable capacity MOFs in the future.

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

Observationally derived rise in methane surface forcing mediated by water vapour trend

Atmospheric methane (CH4) mixing ratios exhibited a plateau between 1995 and 2006 and have subsequently been increasing. While there are a number of competing explanations for the temporal evolution of this greenhouse gas, these prominent features in the temporal trajectory of atmospheric CH4 are expected to perturb the surface energy balance through radiative forcing, largely due to the infrared radiative absorption features of CH4. However, to date this has been determined strictly through radiative transfer calculations. Here, we present a quantified observation of the time series of clear-sky radiative forcing by CH4 at the surface from 2002 to 2012 at a single site derived from spectroscopic measurements along with line-by-line calculations using ancillary data. There was no significant trend in CH4 forcing between 2002 and 2006, but since then, the trend in forcing was 0.026?±?0.006 (99.7%?CI)?W?m2?yr-1. The seasonal-cycle amplitude and secular trends in observed forcing are influenced by a corresponding seasonal cycle and trend in atmospheric CH4. However, we find that we must account for the overlapping absorption effects of atmospheric water vapour (H2O) and CH4 to explain the observations fully. Thus, the determination of CH4 radiative forcing requires accurate observations of both the spatiotemporal distribution of CH4 and the vertically resolved trends in H2O.

Feldman, Daniel R.↗
DOE OSTI2021

Engineering catalyst supports to stabilize PdO x two-dimensional rafts for water-tolerant methane oxidation

The treatment of emissions from natural gas engines is an important area of research since methane is a potent greenhouse gas. The benchmark catalysts, based on Pd, still face challenges such as water poisoning and long-term stability. In this work, we report an approach for catalyst synthesis that relies on the trapping of metal single atoms on the support surface, in thermally stable form, to modify the nature of further deposited metal/metal oxide. By anchoring Pt ions on a catalyst support we can tailor the morphology of the deposited phase. In particular, two-dimensional (2D) rafts of PdO x are formed, resulting in higher reaction rates and improved water tolerance during methane oxidation. The results show that modifying the support by trapping single atoms could provide an important addition to the toolkit of catalyst designers for controlling the nucleation and growth of metal and metal oxide clusters in heterogeneous catalysts.

2D raft↗
DOE OSTI2016

Development of Low-Intermediate Temperature Fuel Cells for Direct Conversion of Methane to Methanol Fuel

The objective of this project is development of a durable, low-cost, and high performance Low Temperature Solid Oxide Fuel Cell (LT-SOFC) for direct conversion of methane to methanol and other liquids, characterized by: a) operating temperature < 500oC, b) current density of > 100 mA/cm2 in liquid hydrocarbon production mode, c) continuous operation of > 100 h, d) cell area >100 cm2, e) cell cost per rate of product output < 100,000/bpd, f) process intensity of > 0.1 bpd/ft3, g) product yield and carbon efficiency > 50%, and h) volumetric output per cell > 30 L/day.

Torabi, Alireza↗
NASA NTRS1989

Carbon-14 in methane sources and in atmospheric methane - The contribution from fossil carbon

Measurements of carbon-14 in small samples of methane from major biogenic sources, from biomass burning, and in clean air samples from both the Northern and Southern hemispheres reveal that methane from ruminants contains contemporary carbon, whereas that from wetlands, peat bogs, rice fields, and tundra, is somewhat depleted in carbon-14. Atmospheric (C-14)H4 seems to have increased from 1986 to 1987, and levels at the end of 1987 were 123.3 + or - 0.8 percent modern carbon in the Northern Hemisphere and 120.0 + or - 0.7 percent modern carbon in the Southern Hemisphere.

Wahlen, M.↗
DOE OSTI2019

Plant Root Exudates Increase Methane Emissions through Direct and Indirect Pathways

The largest natural source of CH4 to the atmosphere is wetlands, which produce 20% to 50% of total global emissions. Vascular plants play a key role regulating wetland CH4 emissions through multiple mechanisms. They often contain aerenchymatous tissues which act as a diffusive pathway for CH4 to travel from the anoxic soil to the atmosphere and for O2 to diffuse into the soil and enable methanotrophy. Plants also exude carbon from their roots which stimulates microbial activity and fuels methanogenesis. This study investigated these mechanisms in a laboratory experiment utilizing rootboxes containing either Carex aquatilis plants, silicone tubes that simulated aerenchymatous gas transfer, or only soil as a control. CH4 emissions were far greater from planted boxes than from control boxes or simulated plants, indicating that the physical transport pathway of aerenchyma was of little importance when not paired with other effects of plant biology. Plants were exposed to 13CO2 at two time-points and subsequent enrichment of root tissue, rhizosphere soil, and emitted CH4 was used in an isotope mixing model to determine the proportion of plant-derived versus soil-derived carbon supporting methanogenesis. Results showed that carbon exuded by plants was converted to CH4 but that plants also increased emission of soil-derived carbon relative to the other experimental treatments. This result signifies that plants and root exudates altered the soil chemical environment and microbial community such that microbial utilization of soil carbon was increased (e.g. microbial priming) and/or oxidation of soil-derived CH4 was decreased (e.g., by microbial competition for oxygen).

methane, wetlands, microbial priming, root exudate↗
DOE OSTI2018

Synthesis of Titanium Oxycarbide from Titanium Slag by Methane-Containing Gas

In this study, reaction steps of a process for synthesis of titanium oxycarbide from titanium slag were demonstrated. This process involves the reduction of titanium slag by a methane-hydrogen-argon mixture at 1473 K (1200 °C) and the leaching of the reduced products by hydrofluoric acid near room temperature to remove the main impurity (Fe{sub 3}Si). Some iron was formed by disproportionation of the main M{sub 3}O{sub 5} phase before gaseous reduction started. Upon reduction, more iron formed first, followed by reduction of titanium dioxide to suboxides and eventually oxycarbide.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Low diffusive methane emissions from the main channel of a large Amazonian run-of-the-river reservoir attributed to high methane oxidation

The global development of hydropower dams has rapidly expanded over the last several decades and has spread to historically non-impounded systems such as the Amazon River's main low land tributaries in Brazil. Despite the recognized significance of reservoirs to the global methane (CH4) emission, the processes controlling this emission remain poorly understood, especially in Tropical reservoirs. Here we evaluate CH4 dynamics in the main channel and downstream of the Santo Antônio hydroelectric reservoir, a large tropical run-of-the-river (ROR) reservoir in Amazonia. This study is intended to give a snapshot of the CH4 dynamics during the falling water season at the initial stage after the start of operations. Our results show substantial and higher CH4 production in reservoirs' littoral sediment than in the naturally flooded areas downstream of the dam. Despite the large production in the reservoir or naturally flooded areas, high CH4 oxidation in the main channel keep the concentration and fluxes of CH4 in the main channel low. Similar CH4 concentrations in the reservoir and downstream close to the dam suggest negligible degassing at the dam, but stable isotopic evidence indicates the presence of a less oxidized pool of CH4 after the dam. ROR reservoirs are designed to disturb the natural river flow dynamics less than traditional reservoirs. If enough mixing and oxygenation remain throughout the reservoir's water column, naturally high CH4 oxidation rates can also remain and limit the diffusive CH4 emissions from the main channel. Nevertheless, it is important to highlight that our results focused on emissions in the deep and oxygenated main channel. High emissions, mainly through ebullition, may occur in the vast and shallow areas represented by bays and tributaries. However, detailed assessments are still required to understand the impacts of this reservoir on the annual emissions of CH4.

Amazon, aquatic, biogeochemistry, carbon cycling, ↗
DOE OSTI2015

Enhanced Dry Reforming of Methane on Ni and Ni-Pt Catalysts Synthesized by Atomic Layer Deposition

Atomic layer deposition (ALD) was used to deposit Ni and Pt on alumina supports to form monometallic and bimetallic catalysts with initial particle sizes of 1–2.4 nm. The ALD catalysts were more active (per mass of metal) than catalysts prepared by incipient wetness (IW) for dry reforming of methane (DRM), and they did not form carbon whiskers during reaction due to their sufficiently small size. Catalysts modified by Pt ALD had higher rates of reaction per mass of metal and inhibited coking, whereas NiPt catalysts synthesized by IW still formed carbon whiskers. Temperature-programmed reduction of Ni catalysts modified by Pt ALD indicated the presence of bimetallic interaction. Density functional theory calculations suggested that under reaction conditions, the NiPt surfaces form Ni-terminated surfaces that are associated with higher DRM rates (due to their C and O adsorption energies, as well as the CO formation and CH4 dissociation energies).

Environmental Molecular Sciences Laboratory↗