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Results for “CARBONIZATION”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Evidence for Carbonate Surface Complexation during Forsterite Carbonation in Wet Supercritical Carbon Dioxide

Continental flood basalts are attractive formations for geologic sequestration of carbon dioxide because of their reactive divalent-cation containing silicates, such as forsterite (Mg2SiO4), suitable for long-term trapping of CO2 mineralized as metal carbonates. The goal of this study was to investigate at a molecular level the carbonation products formed during the reaction of forsterite with supercritical CO2 (scCO2) as a function of the concentration of H2O adsorbed to the forsterite surface. Experiments were performed at 50 °C and 90 bar using an in situ IR titration capability, and post-reaction samples were examined by ex situ techniques, including SEM, XPS, FIB-TEM, TGA-MS, and MAS-NMR. Carbonation products and reaction extents varied greatly with adsorbed H2O. We show for the first time evidence of Mg-carbonate surface complexation under wet scCO2 conditions. Carbonate is found to be coordinated to Mg at the forsterite surface in a predominately bidentate fashion at adsorbed H2O concentrations below 27 µmol/m2. Above this concentration and up to 76 µmol/m2, monodentate coordinated complexes become dominant. Beyond a threshold adsorbed H2O concentration of 76 µmol/m2, crystalline carbonates continuously precipitate as magnesite, and the particles that form are hundreds of times larger than the estimated thicknesses of the adsorbed water films of about 7 to 15 Å. At an applied level, these results suggest that mineral carbonation in scCO2 dominated fluids near the wellbore and adjacent to caprocks will be insignificant and limited to surface complexation, unless adsorbed H2O concentrations are high enough to promote crystalline carbonate formation. At a fundamental level, the surface complexes and their dependence on adsorbed H2O concentration give insights regarding forsterite dissolution processes and magnesite nucleation and growth.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2017

Carbon Inputs From Riparian Vegetation Limit Oxidation of Physically Bound Organic Carbon Via Biochemical and Thermodynamic Processes: OC Oxidation Processes Across Vegetation

In light of increasing terrestrial carbon (C) transport across aquatic boundaries, the mechanisms governing organic carbon (OC) oxidation along terrestrial-aquatic interfaces are crucial to future climate predictions. Here, we investigate biochemistry, metabolic pathways, and thermodynamics corresponding to OC oxidation in the Columbia River corridor. We leverage natural vegetative differences to encompass variation in terrestrial C inputs. Our results suggest that decreases in terrestrial C deposition associated with diminished riparian vegetation induce oxidation of physically-bound (i.e., mineral and microbial) OC at terrestrial-aquatic interfaces. We also find that contrasting metabolic pathways oxidize OC in the presence and absence of vegetation and—in direct conflict with the concept of ‘priming’—that inputs of water-soluble and thermodynamically-favorable terrestrial OC protects bound-OC from oxidation. Based on our results, we propose a mechanistic conceptualization of OC oxidation along terrestrial-aquatic interfaces that can be used to model heterogeneous patterns of OC loss under changing land cover distributions.

Graham, Emily B.↗
DOE OSTI2019

Analysis of the origins of black carbon and carbon monoxide transported to Beijing, Tianjin, and Hebei in China

A novel back-trajectory approach was adopted to determine the origins of black carbon (BC) and carbon monoxide (CO) transported to Beijing, Tianjin and Hebei. Results showed that the transport efficiency was controlled mainly by mid-latitude westerlies in winter, the South Asian monsoon in summer and prevailing westerly and northwesterly winds in spring and autumn. Hebei was identified as the most important source region of both BC (respectively accounting for 55% and 49%) and CO (39% and 38%) transported to Beijing and Tianjin. Inner Mongolia contributed more to the effective emission intensity (EEI) in winter than in summer for both BC and CO transported to Beijing and Tianjin. Shandong was responsible for higher EEI in summer than in winter. The six provinces making the greatest contributions to BC transported to Hebei were Shandong (19%), Shanxi (19%), Inner Mongolia (17%), Beijing (11%), Henan (11%), and Tianjin (10%), whereas thosemaking the greatest contributions to CO transported to Hebei were Shandong (20%), Inner Mongolia (10%), Tianjin (9%), Henan (9%), Shanxi (9%), and Beijing (8%). In summary, Hebei, Inner Mongolia, Shandong, Tianjin and Shanxi were determined as the dominant source regions of not only BC but also CO transported to Beijing. Hebei, Shandong, Beijing, Inner Mongolia, Henan, Liaoning and Shanxi were relatively important source regions for Tianjin. Shandong, Shanxi, Inner Mongolia, Beijing, Henan, Tianjin, Liaoning, Jiangsu and Anhui were the main source regions for Hebei. Residential and industrial sectors were the dominant sectors for BC and CO transported to the receptors, respectively. These results are consistent with the results of previous studies. Finally, comparing the observed.BC/.CO ratiowith the enhancement ratio of the EEI of BCwith that of CO (Delta EEIBC/Delta EEICO) atMiyun site, we further confirmed that the EEI can be used to represent the amounts of BC and CO reaching receptors. (c) 2018 Published by Elsevier B.V.

black carbon↗
DOE OSTI2011

Amorphous Diamond: A High-Pressure Superhard Carbon Allotrope

Compressing glassy carbon above 40 GPa, we have observed a new carbon allotrope with a fully sp{sup 3}-bonded amorphous structure and diamondlike strength. Synchrotron x-ray Raman spectroscopy revealed a continuous pressure-induced sp{sup 2}-to-sp{sup 3} bonding change, while x-ray diffraction confirmed the perseverance of noncrystallinity. The transition was reversible upon releasing pressure. Used as an indenter, the glassy carbon ball demonstrated exceptional strength by reaching 130 GPa with a confining pressure of 60 GPa. Such an extremely large stress difference of >70 GPa has never been observed in any material besides diamond, indicating the high hardness of this high-pressure carbon allotrope.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Copper carbon composite wire with a uniform carbon dispersion made by friction extrusion

Copper-carbon composites are a group of materials with excellent mechanical, electrical, thermal, and tribological properties. However, bulk size copper-carbon composites made by the traditional manufacturing processes, like rolling or extrusion, fall short of reaching some of these properties predicted by theory or demonstrated only by samples at centimeter scale or smaller. The two main challenges to the successful scaling-up are: 1) to uniformly disperse carbon in the metal matrix; 2) to avoid degradation due to oxidation or reaction from overheating. In this work, we first demonstrate friction extrusion as a new method to make bulk-size void-free copper-carbon composite wires with homogenized carbon dispersion. Three different carbon varieties, graphite powder, graphene nanopowder, and carbon nanotubes, were added to the copper matrix with the concentration ranging from 0.5 wt% to 15 wt%. Special tooling, processing parameters, and procedures were developed, especially for high carbon content samples. Ten-fold reductions of both copper grain size and carbon particle size were achieved and attributed to the high shear deformation. Energy dispersive X-ray spectrometry indicates the carbon powder was refined to a sub-micron level and uniformly dispersed in the copper matrix. Compared with that of pure copper, the thermal capacity of the composite wire increases by 30 % while density reduces by 29 %.

Friction extrusion, Metal matrix composite, Graphe↗
DOE OSTI2020

Quantitative Determination of Biomass-derived Renewable Carbon in Fuels from Coprocessing of Bio-oils in Refinery Using a Stable Carbon Isotopic Approach

Increasing renewable carbon incorporation into conventional fuels through coprocessing with vacuum gas oil (VGO, a petroleum refining feedstock) is a critical step in biofuels development, scaling-up, adoption and associated GHG reduction. Optimization of the co-processing parameters maximizes incorporation of the renewable carbon in the fuel products. Quantitative determination of the renewable carbon content in the co-processed products provides direct evaluation of the parameters. The co-processing bio-oil with VGO through hydrocracking (HC) or fluid catalytic cracking (FCC) system resulted in carbon isotopic fractionation that prevented the direct use of the isotope mixing model for quantifying the renewable carbon. Here, we report an algorithm of using a stable carbon isotope approach to quantify the renewable carbon content in co-processing biofuel products through high-precision ?13C analysis. A controlled experiment carried out by blending a fossil diesel (-29.013‰) with a bio-diesel (-30.099‰) at various blending levels up to 98.0/2.0 wt% is presented and has demonstrated the applicability of this approach. The carbon isotope fractionation factors for the bio-oil co-processing were obtained by using a 14C-derived isotope-mixing model. The ?13C method was tested by co-processing 13C-labeled bio-crude and natural woody biomass-derived fast pyrolysis (FP) and catalytic fast pyrolysis (CFP) bio-oils with VGO. The results were verified by 14C accelerator mass spectrometry (AMS) method (ASTM-D6866) and compared with the yield mass balance (YMB) method. Strong agreement between d13C and 14C AMS methods demonstrated the applicability of the ?13C method to quantify renewable carbon content in co-processing fuel products and guide the co-processing optimization

Li, Zhenghua↗
DOE OSTI2011

Spherical carbon particles and carbon nanotubes prepared by autogenic reactions : evaluation as anodes in lithium electrochemical cells.

Autogenic reactions, based on the decomposition of one or more precursors at elevated temperatures with self generated pressures can be used to prepare a wide range of materials with interesting structural, morphological and technological properties. Recent reports that spherical carbon particles and carbon nanotubes can be prepared by this technique from waste products, such as used plastic bags, have highlighted this environmentally-attractive approach to synthesize new or modified carbon-based materials. In this paper, we report the synthesis of spherical carbon particles and carbon nanotubes and their evaluation as negative electrodes (anodes) in lithium electrochemical cells. A steady reversible capacity of approximately 240 mAh/g for hundreds of cycles was achieved from both types of carbon, when cycled at a 1C rate between 1.5 V and 5 mV. A reversible capacity of 372 mAh/g, i.e., the theoretical value for graphite, was obtained from the carbon nanotube electrodes by raising the upper voltage limit to 3 V. To increase the graphitic order in the carbon spheres, the particles were heated to 2400 C in an inert atmosphere. This treatment reduced the first cycle irreversible capacity loss of Li/C half cells from 60 to 20%, the spherical carbon electrodes yielding a stable 252 mAh/g discharge capacity for numerous cycles. Structural and morphological information about the parent and cycled carbon electrodes, obtained by powder X-ray diffraction, Raman spectroscopy, high-resolution scanning electron microscopy, and electron dispersive analysis of X-rays is provided.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2011

Convert Graphene Sheets to Boron Nitride and Boron Nitride-carbon Sheets via a Carbon-substitution Reaction

Here we discuss our synthesis of highly crystalline pure boron nitride (BN) and BN-carbon (BN-C) sheets by using graphene sheets as templates via a carbon-substitution reaction. Typically, these sheets are several micrometers wide and have a few layers. The composition ratios of BN-C sheets can be controlled by the post-treatment (remove carbon by oxidation) temperature. We also observed pure BN and BN-C nanoribbons. We characterized the BN-C sheets via Raman spectroscopy and density functional theory calculations. The results reveal that BN-C sheets with an armchair C-BN chain, and embedded C2 or C6 units in BN-dominated regions energetically are the most favorable.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Experimental and modeling study of calcium carbonate precipitation and its effects on the degradation of oil well cement during carbonated brine exposure

Decalcification of cement in solutions of carbonated brine is important to a host of engineering applications, especially in subsurface service environments where cementitious materials are frequently utilized as engineered barriers for wellbore seals, as well as shaft and drift seals and waste forms for nuclear waste disposal. Analysis of leaching simulations and experiments shows that, depending on solution compositions (dissolved CO{sub 2} concentration, pH, Ca ion concentration), calcite precipitation occurring during leaching of cement in contact with carbonated brine can have a significant impact on cement reactivity, in some instances leading to complete arrest of reactivity via calcium carbonate ''pore-clogging''. We present modeling and experimental results that examine the range of solution conditions that can lead to pore-clogging. Analysis of the results shows that distinct regimes of leaching behavior, based on pH and pCO2, can be used to form a framework to better understand the occurrence of pore-clogging.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2013

CARBON-ENHANCED METAL-POOR STARS IN SDSS/SEGUE. I. CARBON ABUNDANCE ESTIMATION AND FREQUENCY OF CEMP STARS

We describe a method for the determination of stellar [C/Fe] abundance ratios using low-resolution (R = 2000) stellar spectra from the Sloan Digital Sky Survey (SDSS) and its Galactic sub-survey, the Sloan Extension for Galactic Understanding and Exploration (SEGUE). By means of a star-by-star comparison with a set of SDSS/SEGUE spectra with available estimates of [C/Fe] based on published high-resolution analyses, we demonstrate that we can measure [C/Fe] from SDSS/SEGUE spectra with S/N ≥ 15 Å{sup –1} to a precision better than 0.35 dex for stars with atmospheric parameters in the range T {sub eff} = [4400, 6700] K, log g = [1.0, 5.0], [Fe/H] = [–4.0, +0.5], and [C/Fe] = [–0.25, +3.5]. Using the measured carbon-to-iron abundance ratios obtained by this technique, we derive the frequency of carbon-enhanced stars ([C/Fe] ≥ +0.7) as a function of [Fe/H], for both the SDSS/SEGUE stars and other samples from the literature. We find that the differential frequency slowly rises from almost zero to about 14% at [Fe/H] ∼ –2.4, followed by a sudden increase, by about a factor of three, to 39% from [Fe/H] ∼ –2.4 to [Fe/H] ∼ –3.7. Although the number of stars known with [Fe/H] < –4.0 remains small, the frequency of carbon-enhanced metal-poor (CEMP) stars below this value is around 75%. We also examine how the cumulative frequency of CEMP stars varies across different luminosity classes. The giant sample exhibits a cumulative CEMP frequency of 32% for [Fe/H] ≤ –2.5, 31% for [Fe/H] ≤ –3.0, and 33% for [Fe/H] ≤ –3.5; a roughly constant value. For the main-sequence turnoff stars, we obtain a lower cumulative CEMP frequency, around 10% for [Fe/H] ≤ –2.5, presumably due to the difficulty of identifying CEMP stars among warmer turnoff stars with weak CH G-bands. The dwarf population displays a large change in the cumulative frequency for CEMP stars below [Fe/H] = –2.5, jumping from 15% for [Fe/H] ≤ –2.5 to about 75% for [Fe/H] ≤ –3.0. When we impose a restriction with respect to distance from the Galactic mid-plane (|Z| < 5 kpc), the frequency of the CEMP giants does not increase at low metallicity ([Fe/H] < –2.5), but rather decreases due to the dilution of C-rich material in stars that have undergone mixing with CNO-processed material from their interiors. The frequency of CEMP stars near the main-sequence turnoff, which are not expected to have experienced mixing, increases for [Fe/H] ≤ –3.0. The general rise in the global CEMP frequency at low metallicity is likely due to the transition from the inner-halo to the outer-halo stellar populations with declining metallicity and increasing distance from the plane.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2015

Effect of Vinylene Carbonate and Fluoroethylene Carbonate on SEI Formation on Graphitic Anodes in Li-Ion Batteries

Binder free (BF) graphite electrodes were utilized to investigate the effect of electrolyte additives fluoroethylene carbonate (FEC) and vinylene carbonate (VC) on the structure of the solid electrolyte interface (SEI). The structure of the SEI has been investigated via ex-situ surface analysis including X-ray Photoelectron spectroscopy (XPS), Hard XPS (HAXPES), Infrared spectroscopy (IR) and transmission electron microscopy (TEM). The components of the SEI have been further investigated via nuclear magnetic resonance (NMR) spectroscopy of D2O extractions. The SEI generated on the BF-graphite anode with a standard electrolyte (1.2 M LiPF6 in ethylene carbonate (EC) / ethyl methyl carbonate (EMC), 3/7 (v/v)) is composed primarily of lithium alkyl carbonates (LAC) and LiF. Incorporation of VC (3% wt) results in the generation of a thinner SEI composed of Li2CO3, poly(VC), LAC, and LiF. Incorporation of VC inhibits the generation of LAC and LiF. Incorporation of FEC (3% wt) also results in the generation of a thinner SEI composed of Li2CO3, poly(FEC), LAC, and LiF. The concentration of poly(FEC) is lower than the concentration of poly(VC) and the generation of LAC is inhibited in the presence of FEC. The SEI appears to be a homogeneous film for all electrolytes investigated.

25 ENERGY STORAGE↗