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At least 379 records · Page 21
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Effect of Cd on the Nucleation and Transformation of Amorphous Calcium Carbonate

Qualitative measurements observations and field observations measurements indicate mineral coatings are one of the most abundant ways earth materials form, including in sedimentary deposits and certain biominerals. Formation of amorphous carbonates and other metastable intermediates in such these mixed cation systems is poorly understood, however. Using in situ PDF and SAXS, along with ICP-MS and SEM, results from this study 1) determines identify a novel short-range ordered Cd-ACC phase and 2) finds determine amorphous carbonate is stabilized by Cd2+, and 3) support formation of Cd-substituted vaterite, a polymorph of Ca that is not natively formed by Cd CO3. Results are highly dependent on ACC supersaturation, suggesting Cd-induced stability of Cd-ACC are is dependent primarily very sensitive on amorphous phase kinetics rather than thermodynamics to the rate of Cd-ACC nucleation and transformation. Findings provide a quantitative understanding of precursor intermediate phase structure and stability in mixed cation carbonate systems and aggregation that impact and suggest alternate pathways to forming the chemical heterogeneities frequently observed in natural mineral coatings.

Mergelsberg, Sebastian T.↗
DOE OSTI2024

Photolytic Degradation of Water‐Soluble Organic Carbon in Snowmelts: Changes in Molecular Characteristics, Brown Carbon Chromophores, and Radiative Effects

Abstract Water‐soluble organic carbon (WSOC) deposited in ambient snowpack play key roles in regional carbon cycle and surface energy budget, but the impacts of photo‐induced processes on its optical and chemical properties are poorly understood yet. In this study, melted samples of the seasonal snow collected from northern Xinjiang, northwestern China, were exposed to ultraviolet (UV) radiation to investigate the photolytic transformations of WSOC. Molecular characteristics and chemical composition of WSOC and its brown carbon (BrC) constituents were investigated using high‐performance liquid chromatography interfaced with a photodiode array detector and a high‐resolution mass spectrometer. Upon illumination, formation of nitrogen‐ and sulfur‐containing species with high molecular weight was observed in snow samples influenced by soil‐ and plant‐derived organics. In contrast, the representative sample collected from remote region showed the lowest molecular diversity and photolytic reactivity among all samples, in which no identified BrC chromophores decomposed upon illumination. Approximately 65% of chromophores in urban samples endured UV irradiation. However, most of BrC composed of phenolic/lignin‐derived compounds and flavonoids disappeared in the illuminated samples containing WSOC from soil‐ and plant‐related sources. Effects of the photochemical degradation of WSOC on the potential modulation of snow albedo were estimated. Apparent half‐lives of WSOC estimated as albedo reduction in 300–400 nm indicated 0.1–0.4 atmospheric equivalent days, which are shorter than typical photolysis half‐lives of ambient biomass smoke aerosol. This study provides new insights into the roles of WSOC in snow photochemistry and snow surface energy balance.

Meteorology & Atmospheric Sciences↗
DOE OSTI2021

Silica-copper catalyst interfaces enable carbon-carbon coupling towards ethylene electrosynthesis

Membrane electrode assembly (MEA) electrolyzers offer a means to scale up CO 2 -to-ethylene electroconversion using renewable electricity and close the anthropogenic carbon cycle. To date, excessive CO 2 coverage at the catalyst surface with limited active sites in MEA systems interferes with the carbon-carbon coupling reaction, diminishing ethylene production. With the aid of density functional theory calculations and spectroscopic analysis, here we report an oxide modulation strategy in which we introduce silica on Cu to create active Cu-SiO x interface sites, decreasing the formation energies of OCOH* and OCCOH*—key intermediates along the pathway to ethylene formation. We then synthesize the Cu-SiO x catalysts using one-pot coprecipitation and integrate the catalyst in a MEA electrolyzer. By tuning the CO 2 concentration, the Cu-SiO x catalyst based MEA electrolyzer shows high ethylene Faradaic efficiencies of up to 65% at high ethylene current densities of up to 215 mA cm -2 ; and features sustained operation over 50 h.

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

Emerging concepts in intermediate carbon dioxide emplacement to support carbon dioxide removal

Substantial upscaling of carbon dioxide capture is possible in the coming decades but existing solutions for storage are projected to be limited in annual capacity by as much as 2–10 GtCO 2 per year until mid-century. Temporary storage of CO 2 in a solid or liquid state could prove useful for filling this gap in capacity, until more permanent and ideally lucrative CO 2 sequestration options come online. There are several concepts for reversible solid-state and chemical CO 2 storage, but their advantages and limitations have yet to be reviewed in this context. This article focuses on the physical and chemical aspects of CO 2 storage via liquid and solid chemical carriers and sorbents, and gives an overview of the energetics around their use, as well as prospects for their future development. Exciting opportunities for coupling capture and medium to high maturity multi-year storage technologies could support carbon removal in the coming decades. Highlights of the analysis are the remarkable storage capacity of oxalic acid and formic acid (CO 2 -density of 1857 kg m –3 and 1152 kg m –3 , compared with condensed liquid CO 2 at 993–1096 kg m –3 , respectively), the relative scalability and compatibility of carbonate salts for stationary storage with direct air capture, and the potential promise of multiple carriers for CO 2 transportation. Solid sorbents do not achieve such ultra-high storage capacities, but could improve storage over compressed gas tanks on a capacity and energetics basis.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Extending tetrahedral network similarity to carbon: A type-I carbon clathrate stabilized by boron

Clathrates are guest/host framework compounds composed of polyhedral cages, yet despite their prevalence among tetrahedral network formers, clathrates with a carbon host lattice remain unrealized synthetic targets. Here, we report a type-I carbon-based framework—a ubiquitous clathrate structure type found throughout compounds containing tetrahedral building blocks. Following a boron-stabilization scheme based on first-principles predictions in the Ca–B–C system at high pressure, type-I Ca 8 B x C 46−x (x ≈ 9) was synthesized in the archetypal $Pm\bar{3}n$ lattice with stability derived from substitutionally disordered boron atoms on hexagonal ring framework positions. The synthesized clathrate, which is recoverable to ambient conditions, expands topological network similarity across tetrahedral systems and opens possibilities for a broad family of diamond-like, carbon-based compounds with tunable properties based on the wide potential for guest/host-atom substitutions and framework versatility.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Carbonate Management to Enable Energy- and Carbon-Efficient CO 2 Electrolysis (Final Technical Report)

The rapid growth and plummeting cost of solar energy have created great interest in using CO 2 electrolysis to produce chemical feedstocks and fuels such as carbon monoxide, ethylene, ethanol, and propanol. While research in CO 2 electrolysis has yielded substantial progress in both fundamental understanding of the requisite electrocatalytic reactions and design of prototype devices, the energy efficiency (electrical energy to-product) and carbon efficiency (CO 2 -to-product) of CO 2 electrolysis remain far too low for large-scale deployment. A preponderance of evidence indicates that the principal reason for these low efficiencies is the rapid and thermodynamically favorable reaction of CO 2 with hydroxide (OH–) to form carbonate , which forces CO 2 electrolysis cells to operate under conditions that result in large voltage and CO 2 losses. This “CO 3 2 – problem” presents a fundamental scientific barrier to creating a viable electrochemical option for converting solar energy into chemicals and fuels.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Stoichiometrically coupled carbon and nitrogen cycling in the MIcrobial-MIneral Carbon Stabilization model version 1.0 (MIMICS-CN v1.0)

Explicit consideration of microbial physiology in soil biogeochemical models that represent coupled carbon–nitrogen dynamics presents opportunities to deepen understanding of ecosystem responses to environmental change. The MIcrobial-MIneral Carbon Stabilization (MIMICS) model explicitly represents microbial physiology and physicochemical stabilization of soil carbon (C) on regional and global scales. Here we present a new version of MIMICS with coupled C and nitrogen (N) cycling through litter, microbial, and soil organic matter (SOM) pools. The model was parameterized and validated against C and N data from the Long-Term Inter-site Decomposition Experiment Team (LIDET; six litter types, 10 years of observations, and 13 sites across North America). The model simulates C and N losses from litterbags in the LIDET study with reasonable accuracy (C: R 2 =0.63; N: R 2 =0.29), which is comparable with simulations from the DAYCENT model that implicitly represents microbial activity (C: R 2 =0.67; N: R 2 =0.30). Subsequently, we evaluated equilibrium values of stocks (total soil C and N, microbial biomass C and N, inorganic N) and microbial process rates (soil heterotrophic respiration, N mineralization) simulated by MIMICS-CN across the 13 simulated LIDET sites against published observations from other continent-wide datasets. We found that MIMICS-CN produces equilibrium values in line with measured values, showing that the model generates plausible estimates of ecosystem soil biogeochemical dynamics across continental-scale gradients. MIMICS-CN provides a platform for coupling C and N projections in a microbially explicit model, but experiments still need to identify the physiological and stoichiometric characteristics of soil microbes, especially under environmental change scenarios.

58 GEOSCIENCES↗
NASA NTRS1983

Eikonal phase shift analyses of carbon-carbon scattering

A high-energy double-folding optical potential approximation to the exact nucleus-nucleus multiple-scattering series is used in determining eikonal phase shifts for carbon-carbon scattering at 204.2, 242.7, and 288.6 MeV. The double-folding potentials are derived by folding the energy-dependent free nucleon-nucleon interaction with densities for the projectile and target; these latter are obtained by unfolding the finite nucleon charge density from harmonic-well carbon charge distributions. The charge parameters for these distributions are taken from the results of electron scattering experiments. Predictions are made for total, reaction, and elastic differential cross sections using standard partial wave analysis for the scattering of identical particles and are then compared with recent experimental results. Excellent agreement is obtained despite the absence of arbitrarily adjusted parameters in the theory.

Townsend, L. W.↗
NASA NTRS1987

Abundances in red giant stars - Carbon and oxygen isotopes in carbon-rich molecular envelopes

Millimeter-wave observations have been made of isotopically substituted CO toward the envelopes of 11 carbon-rich stars. In every case, C-13O was detected and model calculations were used to estimate the C-12/C-13 abundance ratio. C-17O was detected toward three, and possibly four, envelopes, with sensitive upper limits for two others. The CO-18 variant was detected in two envelopes. New results include determinations of oxygen isotopic ratios in the two carbon-rich protoplanetary nebulae CRL 26688 and CRL 618. As with other classes of red giant stars, the carbon-rich giants seem to be significantly, though variably, enriched in O-17. These results, in combination with observations in interstellar molecular clouds, indicate that current knowledge of stellar production of the CNO nuclides is far from satisfactory.

Wannier, P. G.↗
NASA NTRS1989

The formation of weathering products on the LEW 85320 ordinary chondrite - Evidence from carbon and oxygen stable isotope compositions and implications for carbonates in SNC meteorites

Isotopic analysis of nesquehonite recovered from the surface of the LEW 85320 H5 ordinary chondrite shows that the delta C-13 and delta O-18 values of the two generations of bicarbonate (Antarctic and Texas) are different: delta C-13 = + 7.9 per mil and + 4.2 per mil; delta O-18 = + 17.9 per mil and + 12.1 per mil, respectively. Carbon isotopic compositions are consistent with equilibrium formation from atmospheric carbon dioxide at - 2 + or - 4 C (Antarctic) and + 16 + or - 4 C (Texas). Oxygen isotopic data imply that the water required for nesquehonite precipitation was derived from atmospheric water vapor or glacial meltwater which had locally exchanged with silicates, either in the meteorite or in underlying bedrock. Although carbonates with similar delta C-13 values have been identified in the SNC meteorites EETA 79001 and Nakhla, petrographic and temperature constraints argue against their simply being terrestrial weathering products.

Grady, Monica M.↗
NASA NTRS1989

The production of low mass carbon stars - Carbon-rich dredge up or oxygen-rich mass loss?

Conventional theory explains the origin of carbon stars as due to dredge up of carbon enriched material from the stellar core during helium flash events late in the life of solar mass AGB stars. This relatively efficient process, however, seems to produce a larger C/O ratio than observed (Lambert et al., 1987). A secondary effect which could contribute to the appearance of carbon stars, is the selective removal of oxygen from the atmosphere by radiative force expulsion of oxygen-rich dust grains. Calculations for this scenario are presented, which evaluate the degree of momentum coupling between the grains and gas under the thermodynamical conditions of AGB star atmospheres.

Stencel, R. E.↗
NASA NTRS1991

Spectral evidence for carbonates on Mars: Hydrous carbonates

Although many of the spectral features of the Martian samples studied are not unique mineralogical indicators, much of the current spectral data is consistent with (possibly abundant) hydrous carbonates on the surface of Mars. The absorption features in the measured samples were quite weak compared with those of anhydrous carbonates. The weak features imply that significantly more hydrous carbonates can be incorporated onto the surface before becoming spectrally evident; however, exact limits have yet to be determined. The stability of these materials in the Martian environment is not known, but their formation and occurrence in low temperature terrestrial environments makes them appealing candidates for weathering products on Mars.

Calvin, W. M.↗
NASA NTRS1992

The cyclic carbonates of the Latemar Massif: Evidence for the orbital forcing of a carbonate platform during the Middle Triassic

The Latemar Massif is an exhumed carbonate platform in the Dolomites of Northern Italy that was deposited during the Ladinian stage of the Middle Triassic. The platform interior is comprised of hundreds of vertically stacked, meter scale, subtidal limestone/vadose cap carbonate cycles ('Latemar couplets') arranged into upward thinning bundles of 5. The individual couplets are interpreted as the products of sea level oscillations occurring with an approximately 20,000 year periodicity; the 5:1 bundling is indicative of a lower order approximately 100,000 year modulating component. This combination of cycling is interpreted as a platform response to precession forcing with the 5:1 bundling an expression of modulation by the eccentricity. Spectral analysis confirms the significance of the 5:1 bundling, and identifies other significant bundling components related to other components of the eccentricity. The results show that the Latemar bundling spectrum is complex, with a splitting of components around the 1 percent bundling frequency, suggestive of the multiple component eccentricity in the 100,000 year range. On the other hand, there is no direct evidence for the major 400,000 year eccentricity component, although there is a dominant approximately 700,000 year cycling in the buildup (a 35:1 bundling period). Other higher frequency bundling components may be related to obliquity forcing. Simple models are presented to argue for and against an astronomical origin of these cyclic platform carbonates.

Hinnov, Linda↗
NASA NTRS1993

Carbon-carbon grid for ion engines

A method and apparatus of manufacturing a grid member for use in an ion discharge apparatus provides a woven carbon fiber in a matrix of carbon. The carbon fibers are orientated to provide a negatibe coefficient of thermal expansion for at least a portion of the grid member's operative range of use.

Garner, Charles E.↗
NASA NTRS1995

Carbon-carbon grid for ion engines

A method and apparatus of manufacturing a grid member for use in an ion discharge apparatus provides a woven carbon fiber in a matrix of carbon. The carbon fibers are orientated to provide a negatibe coefficient of thermal expansion for at least a portion of the grid member's operative range of use.

Garner, Charles E.↗
NASA NTRS1996

Studies of the Surface Treatment and Sizing of Carbon Fiber Surfaces on the Mechanical Properties of Composites Containing Carbon Fibers

Carbon fiber reinforced composites are materials where carbon fibers are used to reinforce a matrix to produce a light and strong material with important applications in the aerospace industry. There are many aspects of the preparation of these materials that would benefit from a study which combines the research of groups involved in the production, testing and analysis of these materials, and studies of the basic surface chemistry involved. This final reports presents the results of a project that has developed a collaboration between groups in all three of the major research universities in the State of Kansas, and promises to lead to a collaborative program that covers the major aspects of composite development and application. Sherwood has provided initial fiber surface treatment and sizing together with fiber and composite surface analysis; Lease, Tomblin and Wang have worked together toward the goal of preparing pre-preg and fabrication of laminated panels; Locke has developed computational models to evaluate the effect of surface treatment (and chemistry) on mechanical properties; Lease, Tomblin and Wang have worked together to perform all necessary mechanical testing. The research has been focused on materials that would benefit the High Speed Civil Transport (HSCT) program. The group has visited Dr. Howard Maars and his colleagues at NASA Langley, and has focused their studies on the NASA requirements discussed in this meeting. An important development, requested by NASA scientists, has been the acquisition and study of K3B as a matrix material for the composites. The project has led to the successful acquisition and surface analysis of K3B, together with the successful deposition of this material onto surface oxidized carbon fibers. Mechanical testing, modelling and the construction of composite preparation equipment has been achieved during the grant period.

Sherwood, Peter M. A.↗
NASA NTRS1994

Durability of Carbon-Carbon Composites to a Simulated Martian Atmosphere

A new facility was designed and constructed to investigate the effects of the Martian atmosphere on high temperature radiator components. Preliminary experimental results from carbon-carbon composite radiator samples suggest that carbon is unstable in the simulated Martian atmosphere at a temperature of 600 C, consistent with previous thermodynamic modeling. However, more work is needed to identify the exact mechanism. The versatile design of the facility permits additional study of materials stability in the presence of other atmospheres.

Jaworske, D. A.↗