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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 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Structural Characteristics and Graphitizability of Tars from Thermal versus Microwave Plasma Pyrolysis of Coals

This work investigates the structural characteristics and graphitizability of tars obtained from thermal pyrolysis versus the reactive microwave (MW) plasma pyrolysis of coals. Powder River Basin (PRB) coal tars obtained by thermal pyrolysis have been compared with tars obtained from MW plasma pyrolysis containing H 2 . To study the effect of coal rank and MW plasma environment, the PRB tars have been compared with Middle Kittanning (MK) coal tars obtained from an argon–hydrogen MW plasma (hp) and an argon-CO 2 MW plasma (cdp) environment. Fourier transform infrared spectroscopy has been used for investigating the structural differences among the tar samples. The tars have been graphitized (GR-) at 2500 °C and the graphitic quality assessment has been performed using X-ray diffraction and transmission electron microscopy. MW plasma-derived tars have higher aromaticity, lower condensation, and lower oxygenated molecules compared to thermally derived tars. These advantageous features of MW plasma-derived tars lead to the formation of crystallites several times larger than thermally derived tars after graphitization. When considering coal of the same rank (bituminous), the choice of the MW plasma environment has a substantial impact on the graphitic quality of the tars. The utilization of MW plasma containing H 2 leads to a significant increase in both the crystallite diameter (by 60%) and stacking height (by 40%) compared to MW plasma containing CO 2 . Furthermore, within the same MW plasma environment, the coal rank plays a significant role in determining the crystallite diameter and stacking height of the GR-tars. In particular, GR-MK tar obtained from hp exhibits a 135% larger crystallite diameter and 85% larger stacking height compared with GR-PRB tar obtained from hp. These findings demonstrate the potential to tailor the composition of coal-derived tars and consequently influence their graphitizability by adjusting the reactive environment during MW plasma treatment.

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

Boson Fermion Nuclei Energy Levels In The Third Period Of The Periodic Table Of Elements (Monograph No.5)

The boson fermion nucleus (BFN) energy level is shown for sodium, magnesium, aluminum, silicon, phosphorus, sulphur, chlorine, and argon. The BFN energy levels are compared to the energy levels in the shell nuclear model. Individual nucleon fermions in the BFN make minor contributions to the nucleus energy level. Nucleons rearrange into boson structures during stellar nucleosynthesis and condense into the lowest-level energy state. Deconstruction of the BFN structure and conversion to a shell or liquid-drop model brings about a higher energy state. This is not favored in nature.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Science & Technology Review: March 2026 - The Future of Lasers

At Lawrence Livermore National Laboratory, we focus on science and technology research to ensure our nation’s security. We also apply that expertise to solve other important national problems in energy, bioscience, and the environment. Science & Technology Review is published eight times a year to communicate, to a broad audience, the Laboratory’s scientific and technological accomplishments in fulfilling its primary missions. The publication’s goal is to help readers understand these accomplishments and appreciate their value to the individual citizen, the nation, and the world.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Modular Plasma Microreactor for Intensified Hydrogen Peroxide Production

Sustainable and decentralized manufacturing of hydrogen peroxide (H 2 O 2 ) has been extensively sought to replace the energy- and waste-intensive anthraquinone process. We introduce a helical biphasic microreactor in a coaxial dielectric barrier discharge (DBD) configuration as a modular, adaptable, and scalable intensified unit for H 2 O 2 production. Geometric and operating parameters such as electrode length, applied voltage, and gas and liquid flow rates can be tuned to regulate the residence time, delivered power, and gas–liquid interfacial area. In turn, these affect the key output parameters, i.e., H 2 O 2 concentration, production rate, and energy yield. We found a direct correlation between the H 2 O 2 production rate and the product of the interfacial area and residence time in the plasma region. We investigated the H 2 O 2 formation pathways using DMSO as an ·OH radical scavenger and found that H 2 O 2 forms by the dissolution of gaseous H 2 O 2 at low interfacial areas and is enhanced probably due to the interfacial recombination of ·OH radicals at a large gas–liquid interfacial area. The reactor temperature can also be externally controlled to intensify the production rate and energy yield of H 2 O 2 . Concentrations of up to 33 mM can be attained with a small footprint reactor that features a maximum energy yield of 4 g kWh –1 . Here, the plasma microreactor could epitomize a powerful process intensification tool for sustainable and distributed chemical manufacturing.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

High-Fidelity Computational Studies of Intermediate Pressure Capacitively Coupled Plasmas

This report discussed progress made in the development of a computational model for intermediate pressure capacitively coupled plasma discharge. A new full fidelity argon chemistry model has been developed that includes electron, argon ion, three lumped states for electronically excited species, and the background ground state argon. As such the mechanism has been validated over a wide range of intermediate pressure conditions from 100 mTorr to a few Torr. Uncertainties in the electron impact cross sections and the rate coefficients for the reactions are propagated through the model to establish uncertainties that emerge in the model due the reaction mechanism and its impact on the discharge properties. The model is therefore validated in face of uncertainties.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Oxidative Functionalization of Long-Chain Liquid Alkanes by Pulsed Plasma Discharges at Atmospheric Pressure

In this work, we introduce the oxidation of long aliphatic alkanes using non-thermal, atmospheric plasma processing as an eco-friendly route for organic synthesis. A pulsed dielectric barrier discharge in He/O 2 gas mixtures was employed to functionalize n-octadecane. C 18 secondary alcohols and ketones were the main products, with an optimal molar yield of ~29.2%. Prolonged treatment resulted in the formation of dialcohols, diketones, and higher molecular weight oxygenates. Lighter hydrocarbon products and decarboxylation to CO 2 were also observed at longer treatment times and higher power inputs. A maximum energy yield of 5.48 × 10 –8 mol/J was achieved at short treatment times and high powers, associated with higher selectivity to primary oxygenates. Direct hydroxylation of alkyl radicals, as well as disproportionation reactions, are proposed as the main pathways to alcohols and ketones. The results hold promise for functionalizing long hydrocarbon molecules at ambient conditions using catalyst-free plasma discharges.

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

Changes in environmental and engineered conditions alter the plasma membrane lipidome of fractured shale bacteria

ABSTRACT Microorganisms that persist in fractured shale reservoirs cause several problems including secreting foul gases and forming biofilms. Current biocontrol measures often fail due to limited knowledge of their in situ activities. The plasma membrane protects the cell, mediates many of its critical functions, and responds to intracellular cues and ecological perturbations through physicochemical modifications. As such, it provides valuable insight into the physiological adaptation of microorganisms in disturbed environmental systems. Here, we (i) demonstrate how changes in salinity and hydraulic retention time (HRT) influence the plasma membrane intact polar lipid (IPL) chemistry of model bacterium, Halanaerobium congolense WG10, and mixed microbial consortia enriched from shale-produced fluids and (ii) elucidate adjustments in membrane IPL chemistry during biofilm growth relative to planktonic cells. We incubated H. congolense WG10 in chemostats under three salinities (7%, 13%, and 20% NaCl), operated under three HRTs (19.2, 24, and 48 h), and in drip flow biofilm reactors under the same salinity gradients. Also, mixed microbial consortia in produced fluids were enriched in triplicate chemostat vessels under three HRTs (19.2, 24, and 72 h) and biofilm reactors. Lipids were analyzed by ultra high performance liquid chromatography-tandem mass spectrometry (UPLC-MS/MS). Our results show that phosphatidylglycerols, cardiolipins, and phosphatidylethanolamines were predominantly enriched in planktonic H. congolense WG10 cells grown at hypersalinity (20%) compared to optimum (13%). In addition, several zwitterionic phosphatidylcholines and phosphatidylethanolamines were higher in abundance during biofilm growth. These observations suggest that microbial adaptation and biofilm formation in fractured shale are enabled by strategic plasma membrane IPL chemistry adjustments. IMPORTANCE Microorganisms inadvertently introduced into the shale reservoir during fracturing face multiple stressors including brine-level salinities and starvation. However, some anaerobic halotolerant bacteria adapt and persist for long periods of time. They produce hydrogen sulfide, which sours the reservoir and corrodes engineering infrastructure. In addition, they form biofilms on rock matrices, which decrease shale permeability and clog fracture networks. These reduce well productivity and increase extraction costs. Under stress, microbes remodel their plasma membrane to optimize its roles in protection and mediating cellular processes such as signaling, transport, and energy metabolism. Hence, by observing changes in the membrane lipidome of model shale bacteria, Halanaerobium congolense WG10, and mixed consortia enriched from produced fluids under varying subsurface conditions and growth modes, we provide insight that advances our knowledge of the fractured shale biosystem. We also offer data-driven recommendations for improving biocontrol efficacy and the efficiency of energy recovery from unconventional formations.

03 NATURAL GAS↗
DOE OSTI2022

Analysis, identification and confirmation of synthetic opioids using chloroformate chemistry: Retrospective detection of fentanyl and acetylfentanyl in urine and plasma samples by EI-GC-MS and HR-LC-MS

Electron Impact Gas Chromatography-Mass Spectrometry (EI-GC-MS) and High Resolution Liquid Chromatography-Mass Spectrometry (HR-LC-MS) have been used in the analysis of products arising from the trichloroethoxycarbonylation of fentanyl and acetylfentanyl in urine and plasma matrices. The method involves the initial extraction of both synthetic opioids separately from the matrices followed by detection of the unique products that arise from their reaction with 2,2,2-trichloroethoxycarbonyl chloride (Troc-Cl), namely Troc-norfentanyl and Troc-noracetylfentanyl. The optimized protocol was successfully evaluated for its efficacy at detecting these species formed from fentanyl and acetylfentanyl when present at low and high levels in urine (fentanyl: 5 and 10 ng/mL and acetylfentanyl: 20 and 100 ng/mL) and plasma (fentanyl: 10 and 20 ng/mL and acetylfentanyl: 50 and 200 ng/mL), values that reflect levels reported in overdose victims. The HR-LC-MS method’s LOQ (limit of quantitation) for the Troc-norfentanyl and Troc-noracetylfentanyl products was determined to be ~10 ng/mL for both species. Even though the superiority in the detection of these species by HR-LC-MS over EI-GC-MS, the latter method proved to be important in the detection of the second product from the reaction, namely 2-phenylethyl chloride that is crucial in the determination of the original opioid. This observation highlights the importance of using complimentary analytical techniques in the analysis of a sample, whether biological or environmental in nature. The method herein serves as a complementary, qualitative confirmation for the presence of a fentanyl in collected urine, plasma and by extension other biological samples amenable to the common extraction procedures described for opioid analysis. More importantly, the method’s main strength comes from its ability to react with unknown fentanyls to yield products that can be not only detected by EI-GC-MS and HR-LC-MS but can then be used to retrospectively identify an unknown fentanyl.

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

Effects of Surface Roughness on the Electrochemical Reduction of CO 2 over Cu

We have investigated the role of surface roughening on the CO 2 reduction reaction (CO 2 RR) over Cu. The activity and product selectivity of Cu surfaces roughened by plasma pretreatment in Ar, O 2 , or N 2 were compared with that of electrochemically polished Cu samples. Differences in total and product current densities, the ratio of current densities for HER (the hydrogen evolution reaction) to CO 2 RR, and the ratio of current densities for C 2+ to C 1 products depend on the electrochemically active surface and are nearly independent of plasma composition. Theoretical analysis of an electropolished and roughened Cu surface reveals a higher fraction of undercoordinated Cu sites on the roughened surface, sites that bind CO preferentially. Roughened surfaces also contain square sites similar to those on a Cu(100) surface but with neighboring step sites, which adsorb OC-COH, a precursor to C 2+ products. Here, these findings explain the increases in the formation of oxygenates and hydrocarbons relative to CO and the ratio of oxygenates to hydrocarbons observed with increasing surface roughness.

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

Graphitizable Pitch from Microwave Plasma Pyrolysis of Natural Gas

An innovative approach of microwave plasma was utilized to convert natural gas into tar, from which a highly graphitizable pitch was derived using fractional distillation. The natural gas-derived pitch (NGDP) was thoroughly characterized, and the graphitizability of the carbonized NGDP was assessed using polarized light microscopy. The NGDP and, for comparison, needle coke, petroleum coke, and shot coke were subjected to graphitization heat treatment (GR) at 2500 °C. Results indicate that the graphitizability of the NGDP exceeds those of all industrial standard cokes. The GR-NGDP showed the highest degree of graphitization and crystallite size among all samples.

03 NATURAL GAS↗
DOE OSTI2022

Plasma thermal-chemical instability of low-temperature dimethyl ether oxidation in a nanosecond-pulsed dielectric barrier discharge

Plasma stability in reactive mixtures is critical for various applications from plasma-assisted combustion to gas conversion. To generate stable and uniform plasmas and control the transition towards filamentation, the underlying physics and chemistry need a further look. Here, this work investigates the plasma thermal-chemical instability triggered by dimethyl-ether (DME) low-temperature oxidation in a repetitive nanosecond pulsed dielectric barrier discharge. First, a plasma-combustion kinetic mechanism of DME/air is developed and validated using temperature and ignition delay time measurements in quasi-uniform plasmas. Then the multi-stage dynamics of thermal-chemical instability is experimentally explored: the DME/air discharge was initially uniform, then contracted to filaments, and finally became uniform again before ignition. By performing chemistry modeling and analyzing the local thermal balance, it is found that such nonlinear development of the thermal-chemical instability is controlled by the competition between plasma-enhanced low-temperature heat release and the increasing thermal diffusion at higher temperature. Further thermal-chemical mode analysis identifies the chemical origin of this instability as DME low-temperature chemistry. This work connects experiment measurements with theoretical analysis of plasma thermal-chemical instability and sheds light on future chemical control of the plasma uniformity.

repetitive nanosecond pulses↗
DOE OSTI2026

Experimental Investigation of Uranium and Iron Condensation from High-Temperature Plasma Conditions

We used a plasma flow reactor (PFR) to generate synthetic fallout nanoparticles from vapor-phase condensation of two different input concentrations of uranium and iron analytes (U/Fe = 1:1 and 1:2). Synthetic fallout from complex chemical matrices (e.g., mixtures of U and Fe) has not been generated in this setup before and allows for the observation of relative condensation and fractionation of nuclear debris. Experiments were conducted under two different temperature histories with variations in particle flow patterns along the PFR. Transmission electron microscopy (TEM) observation and analysis of the nanoparticles revealed variations in speciation of uranium oxides (UO 2 and α-UO 3 ) depending on the competition between flow mixing and oxygen sequestration by iron. A ternary metal oxide, UFeO 4 , was observed in addition to iron oxides (e.g., FeO and Fe 3 O 4 ), which suggests that fallout models should account for chemical speciation of ternary metal oxides (i.e., UFeO 4 ) and their relative condensation behaviors in addition to those of singular metal oxides (e.g., FeO and UO 2 ). X-ray Energy Dispersive Spectroscopy (EDS) elemental maps showed that some particles had Fe-rich cores surrounded by U-rich regions. This suggests that either condensed U oxides coagulate onto molten Fe oxides or that the increase in iron analyte concentration might drive the system toward a higher degree of supersaturation, leading to earlier formation of iron oxide particles and providing an energetically favored pathway for nucleation of uranium oxides around iron oxide particles.

and nuclear chemistry↗
DOE OSTI2022

Plasma‐driven biocatalysis: In situ hydrogen peroxide production with an atmospheric pressure plasma jet increases the performance of OleT JE when compared to adding the same molar amount of hydrogen peroxide in bolus

Abstract Enzymes like fatty acid peroxygenase OleT JE are desirable enzymes for the industry. While they require inexpensive hydrogen peroxide for activity, the same hydrogen peroxide also causes overoxidation of their reactive heme center. Here, we generate hydrogen peroxide slowly in situ using the Cooperation in Science and Technology (COST)‐Jet, an atmospheric pressure plasma jet, to avoid overoxidizing OleT JE . The COST‐Jet was operated in helium with a water admixture to provide hydrogen peroxide for OleT JE activity. This helium/water admixture produced the highest enzyme turnover numbers after 2 min of treatment. These turnover numbers were even superior to using an equimolar amount of hydrogen peroxide to treat the enzymes exogenously, showing that this plasma source can provide a reliable amount of reaction mediator to support OleT JE activity.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Time-domain modelling and thermometry of the CH 4 v 1 Q-branch using hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering

Here, we present time-domain measurements and modelling of the CH 4 v 1 vibrational Q-branch, as well as simultaneous temperature acquisition from the CH 4 and N 2 vibrational Q-branches using broadband hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps CARS). Accurate measurements with fs/ps CARS require knowledge of the time-domain response of the probed molecule at different temperatures and pressures. In this work, a fs/ps CARS model was developed for theCH 4 v 1 Q-branch and validated using time-resolved probe delay scans at pressures between 70 and 600 Torr and temperatures between 295 and 1000 K. A simplified modified exponential energy gap model was used to determine the linewidths of the Raman transitions within the Q-branch. Total Q-branch linewidths for the entire explored parameter space were also determined from the probe delay scans. This enabled quantitative measurements of CH 4 with fs/ps CARS as well as the temperature through the hot bands of the CH 4 v 1 Q-branch. With a broadband fs laser pulse in a two-beam phase matching scheme, the N 2 Q-branch and CH 4 v 1 Q-branch were simultaneously measured in a heated cell, and the temperatures from each molecule's spectra was evaluated. Here, the fitted temperatures corresponded well with differences ranging from 4 to 17%. It was also shown that exchanging 90% of CH 4 for N 2 or Ar at 295 K and 500 Torr did not significantly impact the normalized time-domain signal prior to a 100 picosecond probe delay. Spatially resolved one-dimensional (1-D) thermometry using the CH 4 Q-branch was also demonstrated with an imaged spatial resolution of 40 µm. With the developed model, 1-D quantitative measurements of CH 4 concentration and temperature can be measured with time resolution of tens of picoseconds.

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

ASGarD: Adaptive Sparse Grid Discretization

Many areas of science exhibit physical processes that are described by high dimensional partial differential equations (PDEs), e.g., the 4D, 5D and 6D models describing magnetized fusion plasmas, models describing quantum chemistry, or derivatives pricing. Such problems are affected by the so-called “curse of dimensionality” where the number of degrees of freedom (or unknowns) required to be solved for scales as N D where N is the number of grid points in any given dimension D. A simple, albeit naive, 6D example is demonstrated in the left panel of Figure 1. With N = 1000 grid points in each dimension, the memory required just to store the solution vector, not to mention forming the matrix required to advance such a system in time, would exceed an exabyte - and also the available memory on the largest of supercomputers available today. The right panel of Figure 1 demonstrates potential savings for a range of problem dimensionalities and grid resolution. While there are methods to simulate such high-dimensional systems, they are mostly based on Monte-Carlo methods, which rely on a statistical sampling such that the resulting solutions include noise. Since the noise in such methods can only be reduced at a rate proportional to $\sqrt{N_p}$ where N p is the number of Monte-Carlo samples, there is a need for continuum, or grid/mesh-based methods for high-dimensional problems, which both do not suffer from noise and bypass the curse of dimensionality. We present a simulation framework that provides such a method using adaptive sparse grids.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2020

Dr. Ian Hutcheon Award: Spectroscopic Fingerprinting of Vapor-Phase Uranium Species

The Dr. Ian Hutcheon Post-Doctoral Fellowship provides resources to fund a TNFapplicable research project as well as promote mentorship, career development, and relevant training for the recipient. The two-year proposal incorporated a research plan to investigate uranium chemistry relevant to post-detonation nuclear forensics and a mentorship plan to address career development for the recipient in TNF-relevant areas.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗