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At least 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Carbon Scaffold Architectures for Stable Lithium Metal Anodes

In light of the skyrocketing demand for electric vehicles and consequent need for high-performing lithium-ion batteries, there has been significant research into the creation of a battery with a lithium metal anode due to its high theoretical capacity and energy density. Unfortunately, nonuniform lithium deposition and consequent dendrite growth diminish performance and pose a safety risk. To combat this, lightweight carbon scaffolds are being developed to stabilize the electric field of these batteries and induce uniform deposition through rational design at the nano-, micro-, and meso- scales. However, there is a paucity of research on the impacts of macroscale scaffold topology on lithium cycling performance. Here, we report the creation of two graphite-based scaffolds with distinct 3D topologies: one a series of triangular prisms and one a series of rectangular prisms. Coin cells were made using these scaffolds and cycled at a current of 1mA/cm2 for 50 cycles to test the performance. The triangular topology was found to outperform the rectangular topology in terms of both potential magnitude and stability during cycling. Disassembling the cells revealed more even lithium deposition on the rectangular scaffold; however, some of the rectangular prisms were broken while all the triangular prisms remained intact. Last, future experiments are proposed regarding the scaffold spacing and mass of the cells in order to isolate the topological impact.

25 ENERGY STORAGE↗
NASA NTRS2005

Ion Neutral Mass Spectrometer Measurements from Titan

Introduction: The Ion Neutral Mass Spectrometer (INMS) aboard the Cassini orbiter has obtained the first in situ composition measurements of the neutral densities of molecular nitrogen, methane, argon, and a host of stable carbon-nitrile compounds in its first flyby of Titan. The bulk composition and thermal structure of the moon s upper atmosphere do not appear to be changed since the Voyager flyby in 1979. However, the more sensitive techniques provided by modern in-situ mass spectrometry also give evidence for large-spatial-scale large-amplitude atmospheric waves in the upper atmosphere and for a plethora of stable carbon-nitrile compounds above 1174 km. Furthermore, they allow the first direct measurements of isotopes of nitrogen, carbon, and argon, which provide interesting clues about the evolution of the atmosphere. The atmosphere was first accreted as ammonia and ammonia ices from the Saturn sub-nebula. Subsequent photochemistry likely converted the atmosphere into molecular nitrogen. The early atmosphere was 1.5 to 5 times more substantial and was lost via escape over the intervening 4.5 billion years due to the reduced gravity associated with the relatively small mass of Titan. Carbon in the form of methane has continued to outgas over time from the interior with much of it being deposited in the form of complex hydrocarbons on the surface and some of it also being lost to space.

Waite, J. H., Jr.↗
NASA NTRS2013

Carbonate Mineral Formation on Mars: Clues from Stable Isotope Variation Seen in Cryogenic Laboratory Studies of Carbonate Salts

The geologic history of water on the planet Mars is intimately connected to the formation of carbonate minerals through atmospheric CO2 and its control of the climate history of Mars. Carbonate mineral formation under modern martian atmospheric conditions could be a critical factor in controlling the martian climate in a means similar to the rock weathering cycle on Earth. The combination of evidence for liquid water on the martian surface and cold surface conditions suggest fluid freezing could be very common on the surface of Mars. Cryogenic calcite forms readily when a rise in pH occurs as a result of carbon dioxide degassing quickly from freezing Ca-bicarbonate-rich water solutions. This is a process that has been observed in some terrestrial settings such as arctic permafrost cave deposits, lakebeds of the Dry Valleys of Antarctica, and in aufeis (river icings) from rivers of N.E. Alaska. We report here the results of a series of laboratory experiments that were conducted to simulate potential cryogenic carbonate formation on the planet Mars. These results indicate that carbonates grown under martian conditions (controlled atmospheric pressure and temperature) show enrichments from starting bicarbonate fluids in both carbon and oxygen isotopes beyond equilibrium values with average delta13C(DIC-CARB) values of ~20.5%0 which exceed the expected equilibrium fractionation factor of [10(sup 3) ln alpha = ~13%0] at 0 degC. Oxygen isotopes showed a smaller enrichment with delta18O(H2O-CARB) values of ~35.5%0, slightly exceeding the equilibrium fractionation factor of [10(sup 3) ln alpha = ~34%0 ] at 0degC. Large kinetic carbon isotope effects during carbonate precipitation could substantially affect the carbon isotope evolution of CO2 on Mars allowing for more efficient removal of 13C from the Noachian atmosphere enriched by atmospheric loss. This mechanism would be consistent with the observations of large carbon isotope variations in martian materials despite the relative paucity of carbonate minerals in the martian crust.

Socki, Richard↗
NASA NTRS2004

Stable Isotope Composition of Carbonates Formed in Low-Temperature Terrestrial Environments as Martian Analogs

We examine the carbon and oxygen isotope composition of carbonate minerals that formed in two low-temperature terrestrial environments. Field locations were chosen to represent environments where microcrystalline carbonates (caliches) form. Samples include caliche crusts collected from the tsekel zone of N. Yucatan, Mexico, as well as carbonate mud from the edge of a near-by salt pan, representing both ancient and modern-precipitated carbonates. Additional field samples of surface-coating caliche were collected from two volcanic fields in Arizona. Preliminary results indicate that there is an overall depletion of 18O and 13C as a function of the extent of meteoric diagenesis. These data are used as terrestrial analogs to gauge whether carbonates that have been found within Martian meteorites could possibly have formed under these or similar conditions on Mars.

Socki, Richard A.↗
NASA NTRS1995

Stable isotopic compositions of carbonates from the Mesoproterozoic Bangemall Group, northwestern Australia

Marine carbonate rocks from the Mesoproterozoic Bangemall Group of northwestern Australia show little deviation (+/-1.3%) in whole-rock delta 13C(carb)-values about a mean of -0.5%. This narrow range persists despite close sampling (every 10-20 m) through long sections (up to 2500 m) that are geographically widespread (up to 250 km apart), over many depositional environments (supralittoral to outer shelf), sediment sources (stromatolitic bioherms to detrital calcilutites) and rock types (pure limestones to dolomitic shales). The only major excursions from the norm seem related to unusual environmental or post-depositional processes, as they are correlated with large enrichments (to -3%) or depletions (to -16%) in 18O. Relatively heavy delta 13C-values, up to +2.5%, occur in a single bed of brecciated ferruginous dolostone at a single locality; these abnormal values may result from local evaporitic conditions. Limey and shaley nodular dolostones have delta 13C-values as low as -4.3%, probably caused by remineralization of organic matter during late and patchy dolomitization. Most notably, sharp negative excursions in delta 13C, up to -8.4%, occur in bleached kerogen-free rocks with mineral assemblages of dolomite + quartz + calcite +/- tremolite + talc, reflecting isotopic re-equilibration in thick metamorphic aureoles around dolerite intrusions. General environmental variations are minor, with delta 13C-values of peritidal facies tending to be slightly positive whereas those of subtidal facies are slightly negative. There are no strong secular trends, but subtle fluctuations within the range -2 to +l% can be correlated along the northwestern margin of the basin. This resembles the pattern seen in other Mesoproterozoic successions, but is markedly unlike the heavy background (> +5%) and extreme variations (up to l0%) in delta 13C evident in Neoproterozoic successions of similar thickness and environmental setting. Hence, in contrast to the Neoproterozoic, the global rate of organic carbon burial was probably fairly constant during deposition of the Bangemall Group, and perhaps generally during the Mesoproterozoic, as was the redox state of the atmosphere and hydrosphere.

Non-NASA Center↗
NASA NTRS1993

Stable isotopic biogeochemistry of carbon and nitrogen in a perennially ice-covered Antarctic lake

Lake Hoare (77 degrees 38' S, 162 degrees 53' E) is an amictic, oligotrophic, 34-m-deep, closed-basin lake in Taylor Valley, Antarctica. Its perennial ice cover minimizes wind-generated currents and reduces light penetration, as well as restricts sediment deposition into the lake and the exchange of atmospheric gases between the water column and the atmosphere. The biological community of Lake Hoare consists solely of microorganisms -- both planktonic populations and benthic microbial mats. Lake Hoare is one of several perennially ice-covered lakes in the McMurdo Dry Valleys that represent the end-member conditions of cold desert and saline lakes. The dry valley lakes provide a unique opportunity to examine lacustrine processes that operate at all latitudes, but under an extreme set of environmental conditions. The dry valley lakes may also offer a valuable record of catchment and global changes in the past and present. Furthermore, these lakes are modern-day equivalents of periglacial lakes that are likely to have been common during periods of glacial maxima at temperate latitudes. We have analyzed the dissolved inorganic carbon (DIC) of Lake Hoare for delta 13C and the organic matter of the sediments and sediment-trap material for delta 13C and delta 15N. The delta 13C of the DIC indicates that 12C is differentially removed in the shallow, oxic portions of the lake via photosynthesis. In the anoxic portions of the lake (27-34 m) a net addition of 12C to the DIC pool occurs via organic matter decomposition. The dissolution of CaCO3 at depth also contributes to the DIC pool. Except near the Canada Glacier where a substantial amount of allochthonous organic matter enters the lake, the organic carbon being deposited on the lake bottom at different sites is isotopically similar, suggesting an autochthonous source for the organic carbon. Preliminary inorganic carbon flux calculations suggest that a high percentage of the organic carbon fixed in the water column is remineralized as it falls through the water column. At nearby Lake Fryxell, the substantial (relative to Lake Hoare) glacial meltstream input overprints Fryxell's shallow-water biological delta 13C signal with delta 13C-depleted DIC. In contrast, Lake Hoare is not significantly affected by surface-water input and mixing, and therefore the delta 13C patterns observed arise primarily from biological dynamics within the lake. Organic matter in Lake Hoare is depleted in 15N, which we suggest is partially the result of the addition of relatively light inorganic nitrogen into the lake system from terrestrial sources.

NASA Program Exobiology↗
NASA NTRS1985

Millimeter-scale variations of stable isotope abundances in carbonates from banded iron-formations in the Hamersley Group of Western Australia

Several diamond drill cores from formations within the Hamersley Group of Western Australia have been studied for evidence of short-range variations in the isotopic compositions of the carbonates. For a set of 32 adjacent microbands analyzed in a specimen from the Marra Mamba Iron Formation, carbon isotope compositions of individual microbands ranged from -2.8 to -19.8 per mil compared to PDB and oxygen isotope compositions ranged from 10.2 to 20.8 per mil compared to SMOW. A pattern of alternating abundances was present, with the average isotopic contrasts between adjacent microbands being 3.0 per mil for carbon and 3.1 per mil for oxygen. Similar results were obtained for a suite of 34 microbands (in four groups) from the Bruno's Band unit of the Mount Sylvia Formation. Difficulties were experienced in preparing samples of single microbands from the Dales Gorge Member of the Brockman Iron Formation, but overall isotopic compositions were in good agreement with values reported by previous authors. Chemical analyses showed that isotopically light carbon and oxygen were correlated with increased concentrations of iron. The preservation of these millimeter-scale variations in isotopic abundances is interpreted as inconsistent with a metamorphic origin for the isotopically light carbon in the BIF carbonates. A biological origin is favored for the correlated variations in 13C and Fe, and it is suggested that the 13C-depleted carbonates may derive either from fermentative metabolism or from anaerobic respiration. A model is presented in which these processes occur near the sediment-water interface and are coupled with an initial oxidative precipitation of the iron.

NASA Program Exobiology↗
DOE OSTI2023

Stable isotopes contain substantial additive information about terrestrial carbon and water cycling

Abstract Stable isotope ratios of H ( δ 2 H ), O ( δ 18 O), and C ( δ 13 C) are linked to key biogeochemical processes of the water and carbon cycles; however, the degree to which isotope-associated processes are reflected in macroscale ecosystem flux observations remains unquantified. Here through formal information assessment, new measurements of δ 13 C of net ecosystem exchange ( NEE ) as well as δ 2 H and δ 18 O of latent heat ( LH ) fluxes across the United States National Ecological Observation Network (NEON) are used to determine conditions under which isotope measurements are informative of environmental exchanges. We find all three isotopic datasets individually contain comparable amounts of information about NEE and LH fluxes as wind speed observations. Such information from isotope measurements, however, is largely unique. Generally, δ 13 C provides more information about LH as aridity increases or mean annual precipitation decreases. δ 2 H provides more information about LH as temperatures or mean annual precipitation decreases, and also provides more information about NEE as temperatures decrease. Overall, we show that the stable isotope datasets collected by NEON contribute non-trivial amounts of new information about bulk environmental fluxes useful for interpreting biogeochemical and ecohydrological processes at landscape scales. However, the utility of this new information varies with environmental conditions at continental scales. This study provides an approach for quantifying the value adding non-traditional sensing approaches to environmental monitoring sites and the patterns identified here are expected to aid in modeling and data interpretation efforts focused on constraining carbon and water cycles’ mechanisms.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1989

Analytical electron microscopy of biogenic and inorganic carbonates

In the terrestrial sedimentary environment, the mineralogically predominant carbonates are calcite-type minerals (rhombohedral carbonates) and aragonite-type minerals (orthorhombic carbonates). Most common minerals precipitating either inorganically or biogenically are high magnesium calcite and aragonite. High magnesium calcite (with magnesium carbonate substituting for more than 7 mole percent of the calcium carbonate) is stable only at temperatures greater than 700 C or thereabouts, and aragonite is stable only at pressures exceeding several kilobars of confining pressure. Therefore, these carbonates are expected to undergo chemical stabilization in the diagenetic environment to ultimately form stable calcite and dolomite. Because of the strong organic control of carbonate deposition in organisms during biomineralization, the microchemistry and microstructure of invertebrate skeletal material is much different than that present in inorganic carbonate cements. The style of preservation of microstructural features in skeletal material is therefore often quite distinctive when compared to that of inorganic carbonate even though wholesale recrystallization of the sediment has taken place. Microstructural and microchemical comparisons are made between high magnesium calcite echinoderm skeletal material and modern inorganic high magnesium calcite inorganic cements, using analytical electron microscopy and related techniques. Similar comparisons are made between analogous materials which have undergone stabilization in the diagenetic environment. Similar analysis schemes may prove useful in distinguishing between biogenic and inorganic carbonates in returned Martian carbonate samples.

Blake, David F.↗
DOE OSTI2020

Implementation of Ion Exchange Processes for Carbon Dioxide Mineralization Using Industrial Waste Streams

Sequestration of CO 2 within stable mineral carbonates (e.g., CaCO 3 ) represents an attractive emission reduction strategy because it offers a leakage-free alternative to geological storage of CO 2 in an environmentally benign form. However, the pH of aqueous streams equilibrated with gaseous streams containing CO 2 (pH < 4) are typically lower than that which is required for carbonate precipitation (pH > 8). Traditionally, alkalinity is provided by a stoichiometric reagent (e.g., NaOH) which renders these processes environmentally hazardous and economically unfeasible. This work investigates the use of regenerable ion-exchange materials to induce alkalinity in CO 2 -saturated aqueous solutions such that the pH shift required for mineralization occurs without the need for stoichiometric reagents. Na + -H + exchange isotherms (at [H + ] = 10 −8 –10 −1 M) and rates were measured for 13X and 4A zeolites and TP-207 and TP-260 organic exchange resins in batch equilibrium and fixed-bed exchange experiments, respectively. At solutions equilibrated with CO 2 at 1.0 atm (pH = 3.9), H + exchange capacities for the materials were similar (1.7–2.4 mmol H + /g material) and resulted in pH increases from 3.9 to greater than 8.0. Multi-component mixtures using Ca 2+ and Mg 2+ cations (at 10 −3 –10 −1 M) in CO 2 -saturated water were used to probe competitive ion exchange. The presence of divalent cations in solution inhibited H + exchange, reducing capacities to as low as 0.2 mmol H + /g for both resins and zeolites. Dynamic H + exchange capacities in fixed-bed ion exchange columns were similar to equilibrium values for resins (∼1.5 mmol/g) and zeolites (∼0.8 mmol/g) using inlet solutions that were equilibrated with gaseous streams of CO 2 at 1.0 atm. However, exchange kinetics were limited by intraparticle diffusion as indicated by the increased rate parameters with increasing inlet flow rates (20–160 cm 3 min −1 ). Experimental calcite precipitation from mixing the alkaline CO 3 2− -rich water solution obtained from the ion-exchange column with a simulated liquid waste stream solution achieved thermodynamic maximum yields. The results from these studies indicate that ion exchange processes can be used as an alternative to the addition of stoichiometric bases to induce alkalinity for the precipitation of CaCO 3 , thereby opening a pathway toward sustainable and economic mineralization processes.

42 ENGINEERING↗
DOE OSTI2021

Modified carbon nanotubes and methods of forming carbon nanotubes

In this invention, processes which can be used to achieve stable doped carbon nanotubes are disclosed. Preferred CNT structures and morphologies for achieving maximum doping effects are also described. Dopant formulations and methods for achieving doping of a broad distribution of tube types are also described.

Heintz, Amy M.↗
DOE OSTI2024

Adding labile carbon to peatland soils triggers deep carbon breakdown

Peatlands store vast amounts of carbon, with deep peat carbon remaining stable due to limited thermodynamic energy and transport. However, climate change-induced increases in labile carbon inputs could destabilize these stores. Here, we combined DNA stable isotope probing with stable isotope-assisted metabolomics employing a multi-platform approach to investigate microbial dynamics driving deep peat carbon degradation upon labile carbon (e.g., glucose) amendment. Our findings highlight the vulnerability of deep peat carbon, as glucose addition triggers the breakdown of older organic matter. By uniquely integrating these techniques, we identified active glucose metabolizers to specific microbial populations and mapped carbon flow through microbial networks, elucidating their role in priming recalcitrant carbon mineralization. This multi-omics approach offers crucial insights into how changing resources reshape the peatland microbiome, enhancing our understanding of deep carbon processing, and refining model parameterization to predict microbial responses and carbon cycle feedbacks under global change pressures.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2020

29 Si solid state MAS NMR study on leaching behaviors and chemical stability of different Mg-silicate structures for CO 2 sequestration

Silicon is one of the most earth abundant elements, and thus, the fate and reactivity of silicate materials are often important for various energy and environmental technologies including carbon sequestration, where CO 2 is captured and stored as a thermodynamically stable solid carbonate phase. Thus, understanding the structures and chemistries of different silicate phases has become an important research aim. Here in this study, the changes in the silicate structures (Q 0 –Q 4 ) of heat-treated Mg-bearing mineral (serpentine) exposed to a CO 2 -water system (carbonic acid) was investigated using 29 Si MAS NMR, XRPD and ICP-OES and the identified structures were employed to explain complex leaching behaviors of silicate materials. The 29 Si MAS NMR and XRPD analysis indicated that the heat-treated serpentine is a mixture of amorphous (Q 1 : dehydroxylate I, Q 2 : enstatite, Q 4 : silica) and crystalline (Q 0 : forsterite, Q 3 : dehydroxylate II and serpentine) phase, while natural serpentine mineral has single crystalline Q 3 silicate structure. The leaching experiments showed that both Mg and Si in the amorphous silicate structures (Q 1 : dehydroxylate I, Q 2 : enstatite) are more soluble than those in crystalline phase (Q 0 : forsterite, Q 3 : dehydroxylate II and serpentine). Therefore, tuning the silicate structure towards Q 1 and Q 2 would significantly improve carbon sequestration potential of silicate minerals, whereas silicate materials with Q 3 structure would provide great chemical stabilities in acidic conditions. The solubilities of silicate structures were in the order of Q 1 (dehydroxylate I) > Q2 (enstatite) >> Q0 (forsterite) > Q3 (dehydroxylate II) > Q 3 (serpentine) and this finding can be used to better design a wide range of energy and environmental materials and reaction systems.

25 ENERGY STORAGE↗
NASA NTRS2012

Compound-Specific Carbon, Nitrogen, and Hydrogen Isotopic Ratios for Amino Acids in CM and CR Chondrites and their use in Evaluating Potential Formation Pathways

Stable hydrogen, carbon, and nitrogen isotopic ratios (oD, 013C, and olSN) of organic compounds can revcal information about their origin and formation pathways. Several formation mechanisms and environments have been postulated for the amino acids detected in carbonaceous chondrites. As each proposed mechanism utilizes different precursor molecules, the isotopic signatures of the resulting amino acids may indicate the most likely of these pathways. We have applied gas chromatography with mass spectrometry and combustion isotope ratio mass spectrometry to measure the compound-specific C, N, and H stable isotopic ratios of amino acids from seven CM and CR carbonaceous chondrites: CM1I2 Allan Hills (ALH) 83100, CM2 Murchison, CM2 Lewis Cliff (LEW) 90500, CM2 Lonewolf Nunataks (LON) 94101, CRZ Graves Nunataks (GRA) 95229, CRZ Elephant Moraine (EET) 92042, and CR3 Queen Alexandra Range (QUE) 99177. We compare the isotopic compositions of amino acids in these meteorites with predictions of expected isotopic enrichments from potential formation pathways. We observe trends of decreasing ODC and increasing oD with increasing carbon number in the aH, (l-NH2 amino acids that correspond to predictions made for formation via Streckercyanohydrin synthesis. We also observe light ODC signatures for ~-alanine, which may indicate either formation via Michael addition or via a pathway that forms primarily small, straight-chain, amine-terminal amino acids (n-ro-amino acids). Higher deuterium enrichments are observed in amethyl amino acids, indicating formation of these amino acids or their precursors in cold interstellar or nebular environments. Finally, individual amino acids are more enriched in deuterium in CR chondrites than CM chondrites, reflecting different parent-body chemistry.

Elsila, Jamie E.↗
DOE OSTI2024

Biomolecular budget of persistent, microbial-derived soil organic carbon: The importance of underexplored pools

The details of how soil microorganisms contribute to stable soil organic carbon pools are a pressing knowledge gap with direct implications for soil health and climate mitigation. It is now recognized that microbial necromass contributes substantially to the formation of stable soil carbon. However, the quantification of necromass in soils has largely been limited to model molecules such as aminosugar biomarkers. The abundance and chemical composition of other persistent microbial residues remain unresolved, particularly concerning how these pools may vary with microbial community structure, soil texture, and management practices. We use yearlong soil incubation experiments with an isotopic tracer to quantify the composition of persistent residues derived from microbial communities inhabiting sand or silt dominated soil with annual (corn) or perennial (switchgrass) monocultures. Persistent microbial residues were recovered in diverse soil biomolecular pools including metabolites, proteins, lipids, and mineral-associated organic matter (MAOM). The relative abundances of microbial contributions to necromass pools were consistent across cropping systems and soil textures. The greatest residue accumulation was not recovered in MAOM but in the light density fraction of soil debris that persisted after extraction by chemical fractionation using organic solvents. Necromass abundance was positively correlated with microbial biomass abundance and revealed a possible role of cell wall morphology in enhancing microbial carbon persistence; while gram-negative bacteria accounted for the greatest contribution to microbial-derived carbon by mass at one year, residues from gram-positive Actinobacteria and Firmicutes showed greater durability. Together these results offer a quantitative assessment of the relative importance of diverse molecular classes for generating durable soil carbon.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Nanostructured carbon as highly efficient and stable anodes for ethylene production and power generation in protonic ceramic electrochemical cells

Protonic ceramic electrochemical cells (PCECs) have the potential in reducing the energy input and carbon emissions in ethylene production from ethane dehydrogenation. The performance of conventional perovskite-based anode materials for ethane conversion in PCECs is limited by their low active surface area and proneness to coke deposition. In this work, for the first time, we demonstrate the use of aligned carbon nanotube forests (CNTFs) as a novel anode material for an ethane fueled PCEC to co-produce ethylene and electricity. The CNTF electrode was grown on the electrolyte by the chemical vapor deposition (CVD) method. Highly dispersed iron carbide nanoparticles are formed in situ on the CNTFs during the CVD process, acting as highly active catalysts for ethane dehydrogenation. The novel PCECs show superior catalytic and electrochemical performances to that using conventional perovskite-based anodes. The cell also exhibits excellent durability and anti-coking abilities within 100 h test. This work showcases the promising application of nanostructured carbon, a new class of non-perovskite materials, as the multifunctional electrode materials for PCECs.

03 NATURAL GAS↗