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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

Measurement of Neutrino Absolute Deep Inelastic Scattering Cross Section in Iron, Lead, Carbon, and Plastic Using MINERvA Detector at $E_{\nu} = 6$ \GeV

A deep inelastic sample is selected from the nuclear charged current inclusive analysis, by requiring reconstructed $Q^{2} \geq 1.0$ (GeV/c)$^{2}$ and $W \geq 2.0$ GeV/c$^{2}$. The neutrino energy range of $5 < E_{\nu} < 50$ previously applied to this analysis in the Low Energy (LE) analysis is removed and the energy range cut is imposed on the muon energy from $2 < E_{\mu} < 50$ GeV. Machine learning vertexing is used to improve the track-based vertexing resulting in higher purity and efficiency of the sample. A local sideband method is utilized to remove the plastic background for the events reconstructed in the target. After plastic backgrounds and non-DIS backgrounds are subtracted, the reconstructed neutrino energy and Bjorken-x are unsmeared to their true quantities via Bayesian unfolding. The unfolded distributions of carbon, iron, lead, and plastic are efficiency corrected and then divided by the flux and the number of nucleons in the target to produce the absolute cr oss section as a function of $E_{\nu}$ and differential cross section as function of $x_{bj}$. The results of the analysis show good agreement between data and MC for $E_{\nu}$ and $x_{bj}$ (see Figures \ref{fig:xsecEnuC} through \ref{fig:xsecXCH}). None of the distributions displayed significant differences with the theoretical models underlying MINERvAs MC.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Operando tribochemical formation of onion-like-carbon leads to macroscale superlubricity

High contact pressure and shear during relative movement of the sliding interfaces are known to cause structural or chemical modification or complete phase transformation due to the stress induced chemical reaction. Such reactions can manifest either formation of tribofilm or induce enhanced wear at the tribological interface. The nature of these stress-induced reactions at the atomistic level and formation of byproducts at the tribological interface, however, remain poorly understood and pose uncertainties in predicting the tribological performance of the tribosystem. In this paper we demonstrate that, when pristine molybdenum disulfide layers in their two dimensional form are coupled with nanodiamonds, the catalytic interaction of sulfur with the nanodiamond through a stress-induced tribocatalytic reaction under high pressure and shear conditions induces amorphization of nanodiamond and eventually formation of onion like carbon structures (OLCs). This leads to near-zero friction, superlubricity, when sliding against diamond like carbon (DLC) ball in dry nitrogen environment at room temperature. Furthermore, the large size (20-30 nm in diameter) and stiffness of the resulting OLCS allow sustaining high contact pressures, while graphitic lattice provides an incommensurate contact with the DLC surface, thus allowing for successful demonstration of the superlubricity conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Engineering the Si Anode Interface via Particle Surface Modification: Embedded Organic Carbonates Lead to Enhanced Performance

Si nanoparticles (SiNPs) are recognized as a promising anode material for next-generation high-energy lithium-ion batteries. However, due to the more stringent requirements resulting from severe volume change, the solid-electrolyte interphase (SEI) on SiNPs plays a critical role in determining their cycling performance. Engineering the interface for higher stability has become an effective yet challenging approach to accommodate the deterioration of the silicon anode from the repeated lithiation/delithiation process. Herein, we report a novel approach of engineering a covalently bonded organic monolayer of ethylene carbonates onto the surface of the SiNPs that can help form a sturdy SEI. Finally, this molecule-level surface modification provides an effective approach to enable high-energy lithium-ion batteries with Si anodes.

25 ENERGY STORAGE↗

Test and Analysis of a Hyper-X Carbon-Carbon Leading Edge Chine

During parts production for the X43A Mach 10 hypersonic vehicle nondestructive evaluation (NDE) of a leading edge chine detected on imbedded delamination near the lower surface of the part. An ultimate proof test was conducted to verify the ultimate strength of this leading edge chine part. The ultimate proof test setup used a pressure bladder design to impose a uniform distributed pressure field over the bi-planar surface of the chine test article. A detailed description of the chine test article and experimental test setup is presented. Analysis results from a linear status model of the test article are also presented and discussed. Post-test inspection of the specimen revealed no visible failures or areas of delamination.

Smith, Russell W.↗

Determination of the cross section of the proton, pion and neutron inelastic interaction with lead and carbon nuclei at 0.5 - 5.0 TeV energies (PION experiment)

Experimental results on the cross section of the single pion, proton and neutron inelastic interaction with carbon and lead nuclei in the 0.5 to 5.0 TeV energy interval obtained on the PION installation (Mount Aragats, Armenia, 3250 m) are presented. For this purpose the (N pi)/(N p) and inelastic (p Fe)/(pi Fe) ratios measured directly on the installation as well as the calculated inelastic (p A)/(pi A) dependence on the target nucleus atomic numbers were used.

Avakian, V. V.↗

DNP-enhanced ultrawideline 207 Pb solid-state NMR spectroscopy: an application to cultural heritage science

Dynamic nuclear polarization (DNP) is used to enhance the (ultra)wideline 207 Pb solid-state NMR spectra of lead compounds of relevance in the preservation of cultural heritage objects. The DNP SSNMR experiments enabled, for the first time, the detection of the basic lead carbonate phase of the lead white pigment by 207 Pb SSNMR spectroscopy. Variable-temperature experiments revealed that the short T'2 relaxation time of the basic lead carbonate phase hinders the acquisition of the NMR signal at room temperature. We additionally observe that the DNP enhancement is twice as large for lead palmitate (a lead soap, which is a degradation product implicated in the visible deterioration of lead-based oil paintings), than it is for the basic lead carbonate. As a result, this enhancement has allowed us to detect the formation of a lead soap in an aged paint film by 207 Pb SSNMR spectroscopy; which may aid in the detection of deterioration products in smaller samples removed from works of art.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Positive and negative contribution to birefringence in a family of carbonates: A Born effective charges analysis

It is an important topic to investigate the birefringence and reveal the contribution from ions to birefringence because it plays an important role in nonlinear optical materials. In this paper, the birefringence of carbonates with coplanar CO{sub 3} groups were investigated using the first-principles method. The results show that the lead carbonates exhibit relative large birefringence. After detailed investigate the electronic structures, and Born effective charges, the authors find out that anisotropic electron distribution in the CO{sub 3} groups and Pb atoms give positive contribution, while the negative contribution was found from fluorine atoms, meanwhile the Ca, Mg, and Cd atoms give very small contribution to birefringence. - Graphical abstract: Using the DFT and Born effective charges, the birefringence and the contribution of ions were investigated, the positive and negative contribution was found from Pb and F ions, respectively. - Highlights: • Optical properties and Born effective charges of carbonates are investigated. • Lead carbonates exhibit relative large birefringence. • Coplanar CO{sub 3} groups and Pb atoms give positive contribution. • F atoms give negative contribution. • Ca, Mg, and Cd atoms give very small contribution.

36 MATERIALS SCIENCE↗

Aligned FTICR-MS, Respiration, and Biochemical Transformation Data from Columbia River Sediment Incubations Associated with: “Carbon Limitation Leads to Thermodynamic Regulation of Aerobic Metabolism”

Columbia River hyporheic zone sediments from the Hanford Site 300 Area in eastern Washington were incubated in a full factorial design with different organic matter (OM) amendments. The aim of the experiment was to test the influence of OM thermodynamics on aerobic respiration across different organic carbon pools and concentrations. This dataset is comprised of (1) a csv with high resolution characterization of dissolved organic matter via 12 Tesla Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS) analyzed through the Environmental Molecular Sciences Laboratory (EMSL; https://www.pnnl.gov/environmental-molecular-sciences-laboratory), (2) a csv with sample IDs, replicates, amendments, dissolved oxygen (DO) measurements, and sampling time points, (3) a csv with sample IDs, replicates, respiration rates, FTICR summary metrics, and relative abundance of chemical classes; and (4) a csv with the number of chemical transformations in each sample replicate (microcosm). The data are associated with the publication “Carbon Limitation Leads to Thermodynamic Regulation of Aerobic Metabolism” published in ES&T Letters (Garayburu-Caruso et al., 2020). Please use the data package’s DOI to cite the data package. We ask that you acknowledge the U.S. Department of Energy (DOE) Biological and Environmental Research (BER) Subsurface Biogeochemical Research (SBR) program when using the data. All data are free to be used for any purpose, such as for manuscripts, presentations, and grant proposals. There is no obligation to include data package authors as co-authors.

54 ENVIRONMENTAL SCIENCES↗

Catalysts by pyrolysis: Direct observation of transformations during re-pyrolysis of transition metal-nitrogen-carbon materials leading to state-of-the-art platinum group metal-free electrocatalyst

Transition metal-nitrogen-carbon (M-N-C) materials have been the focus of scientists’ efforts to address the rising need for earth-abundant materials solutions for energy technology and decarbonization of the economy. They are viewed as one of the most promising candidates to replace platinum group metal (PGM) catalysts in the fuel cell and energy conversion fields, including the application of oxygen reduction reaction, carbon dioxide reduction reaction, and nitrogen reduction reaction. In the effort to improve M-N-C materials properties and achieve atomic dispersity of the transition metal in the carbonaceous matrix, a re-pyrolysis process has been proposed. This secondary heat treatment process of already obtained primary pyrolysis-derived M-N-C materials has been widely reported to substantially improve the electrochemical performance and operational stability of the catalysts. Here, we report a systematic investigation of this process used on samples of templated M-N-C catalysts to obtain state-of-the-art catalysts via in situ heating X-ray photoelectron spectroscopy (XPS), scanning transmission electron microscopy (STEM), energy-dispersive X-ray spectroscopy (EDS), electron energy loss spectroscopy (EELS), X-ray diffraction (XRD), and X-ray computed tomography (CT) characterization methods. It is found that the re-pyrolysis of M-N-C materials could result in the partial amorphization of the carbonaceous substrate. It causes the rearrangement and transformation of multitudinous N moieties, leading to optimization of their morphological display and association with atomically dispersed transition metal dopants. Ultimately, the re-pyrolysis results in an increase in uniformity of the active Fe-Nx sites distribution without the formation of nano-crystalline phases (metallic or carbide) and with overall preservation of the morphology of the carbonaceous framework achieved during the first formative pyrolysis step of the templated synthesis. Finally, these observations provide confirmation that empirically established re-pyrolysis is recommended to be used on all M-N-C materials despite the different synthesis routes to obtain a practical advanced catalytic material.

36 MATERIALS SCIENCE↗

Coupling FeNi alloys and hollow nitrogen-enriched carbon frameworks leads to high-performance oxygen electrocatalysts for rechargeable zinc–air batteries

A dual-template strategy for facile preparation of a bifunctional oxygen electrocatalyst for high-performance rechargeable zinc–air batteries has been reported. Coupling FeNi alloys with hollow nitrogen-doped carbon frameworks concludes in exceptionally high electrocatalytic oxygen reduction and evolution activities. In 1 M KOH, the resulting new material exhibits a superior oxygen evolution activity with a low overpotential of 250 mV to deliver 10 mA cm -2 current density, at which the obtained oxygen reduction performance is also comparable to that of commercial Pt/C and the half-wave potential reaches as high as 0.87 V. As a result, the bifunctional oxygen electrocatalysis performance thus obtained (0.61 V, 1 M KOH) ranks among the best of non-precious oxygen electrocatalysts. Using this new catalyst as an air electrode, the as-prepared rechargeable Zn–air battery shows a high current density of 215 mA cm -2 at a voltage of 1.0 V, large peak power density (310 mW cm -2 ), high potential efficiency (64.7% at 10 mA cm -2 ) and prolonged operation durability. This method provides a means to control the surface features, thereby tuning the catalytic properties of the material, and may open up new possibilities for the rational design and synthesis of new materials for electrochemical applications.

25 ENERGY STORAGE↗

Carbon Limitation Leads to Thermodynamic Regulation of Aerobic Metabolism

Organic matter (OM) metabolism in freshwater ecosystems is a critical source of uncertainty in global biogeochemical cycles, yet the processes regulating aerobic respiration in aquatic environments remain poorly understood. Aerobic respiration is typically predicted through kinetic controls such as organic carbon and oxygen concentrations, while assuming thermodynamic regulation has no influence. The role of OM thermodynamics has been mainly explored under anaerobic conditions; however, recent observations have suggested that thermodynamic properties of OM may influence aerobic respiration rates. Here, we explicitly test OM thermodynamics as a key regulator of aerobic respiration. We pair controlled microcosm experiments with ultrahigh-resolution OM characterization to show that aerobic respiration increases with OM thermodynamic favorability under carbon limitation. We also demonstrate a shift in the regulation of aerobic respiration from OM thermodynamics to nitrogen content when carbon is in excess, highlighting a central role for OM thermodynamics particularly in carbon-limited ecosystems. This illuminates a structural gap in aquatic biogeochemical models by demonstrating that both kinetic and thermodynamic constraints can modulate aerobic respiration. Our work therefore proposes a new conceptual model in which thermodynamic and nutrient limitations dually control aerobic respiration.

54 ENVIRONMENTAL SCIENCES↗

An Effective Approach to the Synthesis of Nanocrystalline PbMoO{sub 4} in Na{sub 2}Mo{sub 4}O{sub 13}–PbCO{sub 3} Melts

This paper presents thermodynamic analysis of reactions of sodium tetramolybdate with Pb{sub 3}O{sub 4}, PbO{sub 2}, PbO, and lead carbonate and describes an effective approach to PbMoO{sub 4} synthesis in melts of the Na{sub 2}Mo{sub 4}O{sub 13}–PbCO{sub 3} system, which offers a low synthesis temperature, waste-free character of the process, high rate, and high yield of a reagent-grade synthesis product in a nanocrystalline state. The synthesis product has been identified by chemical analysis, X-ray diffraction, and particle size measurements.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Elucidation of Local Ordering and Atomic-Scale Structure in Polymer-Derived SiOC

Silicon oxycarbide (SiOC) is a versatile ceramic material with tunable microstructure and compositions that can be modulated through precursor chemistry and processing conditions. Though there are several noteworthy uses of SiOC across a range of application spaces, the difficulties in elucidating the short- to medium-range order within these materials have limited the maturation of strategies to precisely control SiC x O 4–x compositions for user-tailored applications. In this contribution, we implement a range of synchrotron scattering and spectroscopy methods coupled with stochastic modeling techniques to elucidate changes in local chemistry and structure associated with the pyrolysis of a commercially available SiOC polymer precursor. Stochastic modeling approaches provide valuable insights into decoupling local Si–O and Si–C environments while confirming predominate heterogeneous phases in materials. Using pyrolysis temperatures between 250 to 800 °C results in a heterogeneous material predominately composed of SiOC and amorphous SiO 2 domains. At 1100 °C, redistribution of Si–C pairs in the SiOC network and Si–O from the SiO 2 domains create a more ordered SiOC phase with local cubic SiC-like ordering. In addition, residual carbon leads to a detectable carbon phases at 1100 °C that persist at higher temperatures. These efforts address the difficulties of obtaining atomic-scale insights into the local structure and nanoscale heterogeneities in SiOC, providing pathways toward establishing structure–property relationships for future materials development.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Recycling of Lead Pastes from Spent Lead–Acid Batteries: Thermodynamic Constraints for Desulphurization

Lead–acid batteries are important to modern society because of their wide usage and low cost. The primary source for production of new lead–acid batteries is from recycling spent lead–acid batteries. In spent lead–acid batteries, lead is primarily present as lead pastes. In lead pastes, the dominant component is lead sulfate (PbSO 4 , mineral name anglesite) and lead oxide sulfate (PbO•PbSO 4 , mineral name lanarkite), which accounts for more than 60% of lead pastes. In the recycling process for lead–acid batteries, the desulphurization of lead sulfate is the key part to the overall process. In this work, the thermodynamic constraints for desulphurization via the hydrometallurgical route for recycling lead pastes are presented. The thermodynamic constraints are established according to the thermodynamic model that is applicable and important to recycling of lead pastes via hydrometallurgical routes in high ionic strength solutions that are expected to be in industrial processes. The thermodynamic database is based on the Pitzer equations for calculations of activity coefficients of aqueous species. The desulphurization of lead sulfates represented by PbSO 4 can be achieved through the following routes. (1) conversion to lead oxalate in oxalate-bearing solutions; (2) conversion to lead monoxide in alkaline solutions; and (3) conversion to lead carbonate in carbonate solutions. Among the above three routes, the conversion to lead oxalate is environmentally friendly and has a strong thermodynamic driving force. Oxalate-bearing solutions such as oxalic acid and potassium oxalate solutions will provide high activities of oxalate that are many orders of magnitude higher than those required for conversion of anglesite or lanarkite to lead oxalate, in accordance with the thermodynamic model established for the oxalate system. An additional advantage of the oxalate conversion route is that no additional reductant is needed to reduce lead dioxide to lead oxide or lead sulfate, as there is a strong thermodynamic force to convert lead dioxide directly to lead oxalate. As lanarkite is an important sulfate-bearing phase in lead pastes, this study evaluates the solubility constant for lanarkite regarding the following reaction, based on the solubility data, PbO•PbSO 4 + 2H + ⇌ 2Pb 2+ + SO 4 2– + H 2 O(l).

25 ENERGY STORAGE↗

Origins of interstellar and solar system: Carbonaceous materials

Carbon is a crucial atom in cosmochemistry. It is well-established that carbon is synthesized in stellar interiors after the main sequence, is ejected by red giants as small carbonaceous grains during their 'carbon star' phase, resides in the interstellar medium, and was later incorporated into the solar system. The mechanisms of carbon grain formation and later chemical processing are complex because, with only small thermodynamic differences, carbon can take on a bewildering variety of forms: diamond; oxides; carbides; graphite; aliphatic hydrocarbons; polycyclic aromatic hydrocarbons (PAH's); fullerenes; amorphous carbon; and other compounds. These are evidence for many of the forms of carbon found in astronomical observations. We seek to understand the possible astrophysical sites and conditions of the origins of different forms of carbon by combining state-of-the-art capabilities of carbon chemistry with astrophysical modeling. The work is a collaboration between Prof. Frenklach, a leading carbon materials scientist with both laboratory and computer modeling expertise and Prof. Feigelson, an astrophysicist with interests in star formation. The largest effort under this grant was devoted to developing this concept into a comprehensive quantitative model. In addition to explaining the astronomical properties of red giants producing carbonaceous grains, our model also can incorporate recent meteoritic findings. Finally, our induced nucleation grain formation model provides a natural explanation for the widespread presence of PAH emission bands in the Galactic interstellar medium. A brief synopsis of other activities sponsored under this grant and a list of publications from this grant is included.

Feigelson, Eric D.↗

Three-dimensional Pentagon Carbon with a genesis of emergent fermions

Carbon, the basic building block of our universe, enjoys a vast number of allotropic structures. Owing to its bonding characteristic, most carbon allotropes possess the motif of hexagonal rings. Here, with first-principles calculations, we discover a new metastable three-dimensional carbon allotrope entirely composed of pentagon rings. The unique structure of this Pentagon Carbon leads to extraordinary electronic properties, making it a cornucopia of emergent topological fermions. Under lattice strain, Pentagon Carbon exhibits topological phase transitions, generating a series of novel quasiparticles, from isospin-1 triplet fermions to triply degenerate fermions and further to Hopf-link Weyl-loop fermions. Its Landau level spectrum also exhibits distinct features, including a huge number of almost degenerate chiral Landau bands, implying pronounced magneto-transport signals. In conclusion, our work not only discovers a remarkable carbon allotrope with highly rare structural motifs, it also reveals a fascinating hierarchical particle genesis with novel topological fermions beyond the Dirac and Weyl paradigm.

36 MATERIALS SCIENCE↗