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At least 271 records · Page 15

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NASA NTRS1977

Development and testing of a wet oxidation waste processing system

The wet oxidation process is considered as a potential treatment method for wastes aboard manned spacecraft for these reasons: (1) Fecal and urine wastes are processed to sterile water and CO2 gas. However, the water requires post-treatment to remove salts and odor; (2) the residual ash is negligible in quantity, sterile and easily collected; and (3) the product CO2 gas can be processed through a reduction step to aid in material balance if needed. Reaction of waste materials with oxygen at elevated temperature and pressure also produces some nitrous oxide, as well as trace amounts of a few other gases.

Weitzmann, A. L.↗

NASA NTRS1992

Innovative techniques for the production of energetic radicals for lunar processing including cold plasma processing of local planetary ores

Hydrogen reduction of ilmenite has been studied by a number of investigators as a potential means for recovery of oxygen from lunar soil. Interest in this process has always rested with the simplicity of the flow diagram and the utilization of established technology. Effective utilization of hydrogen in the reduction process at temperatures of 1200 C and below has always been disappointing and, as such, has led other investigators to focus attention on other systems. Effective utilization of hydrogen in the reduction of ilmenite can be significantly enhanced in the presence of a non-equilibrium hydrogen plasma. Ilmenite at solid specimen temperatures of 600 C to 970 C were reacted in a hydrogen plasma. Those experiments revealed that hydrogen utilization can be significantly enhanced. At a specimen temperature of 850 C the fraction of H2 reacted was 24 percent compared to the 7 percent theoretical limit calculated with thermodynamic theory for the same temperature. An added advantage for a hydrogen plasma involves further reduction of TiO2. Reduction of the iron oxide in ilmenite yields TiO2 and metallic iron as by products. Titanium forms a number of oxides including TiO, Ti2O3, Ti3O5 and the Magneli oxides (Ti4O7 to Ti50O99). In conventional processing of ilmenite with hydrogen it is possible to reduce TiO2 to Ti7O13 within approximately an hour, but with poor utilization of hydrogen on the order of one mole of H2 per thousand. In the cold or non-equilibrium plasma TiO2 can be rapidly reduced to Ti2O3 with hydrogen utilization exceeding 10 percent. Based on design considerations of the plasma reactor greater utilization of the hydrogen in the reduction of TiO2 is possible.

Bullard, D.↗

DOE OSTI2020

Modular Electrochemical Synthesis Using a Redox Reservoir Paired with Independent Half-Reactions

Electrochemical synthesis of high-value chemicals using renewable electricity could lead to sustainability advantages over conventional chemical manufacturing. The tight coupling between paired anodic and cathodic reactions in conventional electrochemical processes, however, constrains the products and their efficiencies. Here, we demonstrate a strategy to achieve modular electrochemical synthesis (ModES) of different chemicals by decoupling and pairing the oxidative and reductive half-reactions with a heterogeneous redox reservoir (RR). Specifically, sodium nickel hexacyanoferrate (NaNiHCF) can serve as a robust and reversible RR that enables the modular production of several strong oxidants, hydrogen peroxide (H 2 O2) and sodium persulfate (Na 2 S 2 O 8 ) or active chlorine, in separate RR-coupled electrochemical processes. The system’s excellent performance and operational stability is demonstrated by continuous operation over 100 cycles (~36 h) to produce H 2 O 2 and Na 2 S 2 O 8 with a high voltage efficiency. The concept presented here highlights the prospects for using RRs to enable efficient, modular, and on-demand electrochemical synthesis of valuable chemicals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Novel Modular Electrocatalytic Processing for Simultaneous Conversion of Carbon Dioxide and Wet Shale Gas into Valuable Products (Final Report)

This report examines solid oxide electrolyzer cell (SOEC) technology as an alternative process for the manufacture of carbon monoxide (CO) and the separation of ethane (C 2 H 6 ) from wet natural gas (WNG). SOEC cathodes for the electrochemical reduction of carbon dioxide (CO 2 ) to CO and SOEC anodes for the selective electrochemical oxidation of C 2 H 6 to ethylene (C 2 H 4 ) are described and presented. Lifecycle and techno-economic analyses (LCA and TEA) utilizing SOEC technology for the production of CO are also reported.

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2023

Novel Modular Electrocatalytic Processing for Simultaneous Conversion of Carbon Dioxide and Wet Shale Gas into Valuable Products

03 NATURAL GAS↗

DOE OSTI2025

Mechanistic Insights into Oxygen Reduction Reaction on Metal Cathode Over BaZrO 3 -Based Electrolyte under Moist Atmosphere: Interfacial Interactions and Reaction Pathways

The oxygen reduction reaction (ORR) is a critical process that often governs the overall performance of electrochemical systems such as proton conducting solid oxide fuel cells. Despite its significance, the current understanding about the ORR, especially when it involves H 2 O is still limited. In this study, the proton involved ORR (PI-ORR) on metal cathode (e.g., Pt) over BaZrO 3 (BZO) electrolyte is investigated using density functional theory (DFT) under moist atmosphere. Two scenarios are considered: one at relatively high temperature (900 K) in the presence of oxygen vacancy in BZO substrate and one at relatively low temperature (700 K) without oxygen vacancy. We systematically explored oxygen vacancy effects on adsorption sites and proton transfer pathways, calculated energy profiles and Gibbs free energies for elementary steps along the O 2 dissociated and the O 2 concerted reaction pathways. We also evaluated H 2 O impacts on intermediate oxygen species (*O and *OH) through Ab Initio molecular dynamics. These analyses revealed pathway-dependent reaction mechanisms and hydration effects at triple-phase boundary, advancing fundamental understanding of PI-ORR in metal cathode/Ba-based electrolyte systems for energy applications.

08 - HYDROGEN↗

DOE OSTI2026

Iron as a driver of organic carbon fate in permafrost regions

Iron (Fe) and its biogeochemical interactions with organic carbon (OC) exert critical controls over carbon storage and water quality across Arctic and sub-Arctic landscapes. Permafrost thaw affects Fe–organic carbon interactions by exposing thawed material and driving shifts in hydrologic regimes. Here we propose a conceptual framework describing how Fe–OC interactions respond to permafrost thaw and the implications for global carbon cycling. The framework builds on current understanding of hydrologically driven processes that are altered by permafrost thaw, including microbial Fe reduction that influences OC decomposition and carbon emissions; Fe cycling through redox transformations and sulfide oxidation; dissolution and reprecipitation of Fe–OC assemblages; and Fe export to river networks. We put forward four testable hypotheses—on topics from Fe supply to its role in soil OC storage and transfer to rivers—to advance understanding of the coupled environmental controls on pore-scale reactions (that is, microscale reactions at mineral–water–microorganism interfaces) that are central to global Fe–OC cycling. Our framework highlights how soil-profile- and landscape-scale processes, such as hydrologic connectivity and redox dynamics, regulate pore-scale Fe–OC reactions.

Herndon, Elizabeth [ORNL] (ORCID:0000000291945493)↗

DOE OSTI2024

Interfacial Reactivity-Triggered Oscillatory Lattice Strains of Nanoalloys

Understanding the structure evolution of nanoalloys under reaction conditions is vital to the design of active and durable catalysts. Herein, we report an operando measurement of the dynamic lattice strains of dual-noble-metal alloyed with an earth-abundant metal as a model electrocatalyst in a working proton-exchange membrane fuel cell using synchrotron high-energy X-ray diffraction coupled with pair distribution function analysis. Additionally, the results reveal an interfacial reaction-triggered oscillatory lattice strain in the alloy nanoparticles upon surface dealloying. Analysis of the lattice strains with an apparent oscillatory irregularity in terms of frequency and amplitude using time-frequency domain transformation and theoretical calculation reveals its origin from a metal atom vacancy diffusion pathway to facilitate realloying upon dealloying. This process, coupled with surface metal partial oxidation, constitutes a key factor for the nanoalloy's durability under the electrocatalytic oxygen reduction reaction condition, which serves as a new guiding principle for engineering durable or self-healable electrocatalysts for sustainable fuel cell energy conversion.

Wu, Zhi-Peng [State University of New York (SUNY),↗

DOE OSTI2022

High-entropy boride–carbide ceramics by sequential boro/carbothermal synthesis

We report a dual-phase high-entropy boride/carbide ceramic with fine grain size was synthesized by a sequential boro/carbothermal process. In the first step, a Hf-Nb-Ta-Ti-Zr-containing carbide was synthesized by carbothermal reduction of oxides followed by reaction of the carbide with B4C and ZrH2 to convert part of the carbide to boride. The resulting composition was ~29 vol% high-entropy boride with an average grain size of ~1.1 µm. Solid solution formation occurred at the densification temperature of 1900°C resulting in a relative density higher than 99%. The Vickers’ hardness was 26.5 ± 1.4 GPa. This is the first report of synthesizing dual-phase boride-carbide high-entropy ceramics from carbothermally synthesized, high-entropy carbide powders.

36 MATERIALS SCIENCE↗

NASA NTRS1983

Methods of reducing energy consumption of the oxidant supply system for MHD/steam power plants

An in-depth study was conducted to identify possible improvements to the oxidant supply system for combined cycle MHD power plants which would lead to higher thermal efficiency and reduction in the cost of electricity, COE. Results showed that the oxidant system energy consumption could be minimized when the process was designed to deliver a product O2 concentration of 70 mole percent. The study also led to the development of a new air separation process, referred to as liquid pumping and internal compression. MHD system performance calculations show that the new process would permit an increase in plant thermal efficiency of 0.6 percent while allowing more favorable tradeoffs between magnetic energy and oxidant system capacity requirements.

A. J Juhasz↗

NASA NTRS1983

Methods of reducing energy consumption of the oxidant supply system for MHD/steam power plants

An in-depth study was conducted to identify possible improvements to the oxidant supply system for combined cycle MHD power plants which would lead to higher thermal efficiency and reduction in the cost of electricity, COE. Results showed that the oxidant system energy consumption could be minimized when the process was designed to deliver a product O2 concentration of 70 mole percent. The study also led to the development of a new air separation process, referred to as 'liquid pumping and internal compression'. MHD system performance calculations show that the new process would permit an increase in plant thermal efficiency of 0.6 percent while allowing more favorable tradeoffs between magnetic energy and oxidant system capacity requirements.

Juhasz, A. J.↗

DOE OSTI2025

Robust measurement of microbial reduction of graphene oxide nanoparticles using image analysis

ABSTRACT Shewanella oneidensis ( S. oneidensis ) has the capacity to reduce electron acceptors within a medium and is thus used frequently in microbial fuel generation, pollutant breakdown, and nanoparticle fabrication. Microbial fuel setups, however, often require costly or labor-intensive components, thus making optimization of their performance onerous. For rapid optimization of setup conditions, a model reduction assay can be employed to allow simultaneous, large-scale experiments at lower cost and effort. Since S. oneidensis uses different extracellular electron transfer pathways depending on the electron acceptor, it is essential to use a reduction assay that mirrors the pathways employed in the microbial fuel system. For microbial fuel setups that use nanoparticles to stimulate electron transfer, reduction of graphene oxide provides a more accurate model than other commonly used assays as it is a bulk material that forms flocculates in solutions with a large ionic component. However, graphene oxide flocculates can interfere with traditional absorbance-based measurement techniques. This study introduces a novel image analysis method for quantifying graphene oxide reduction, showing improved performance and statistical accuracy over traditional methods. A comparative analysis shows that the image analysis method produces smaller errors between replicates and reveals more statistically significant differences between samples than traditional plate reader measurements under conditions causing graphene oxide flocculation. Image analysis can also detect reduction activity at earlier time points due to its use of larger solution volumes, enhancing color detection. These improvements in accuracy make image analysis a promising method for optimizing microbial fuel cells that use nanoparticles or bulk substrates. IMPORTANCE Shewanella oneidensis ( S. oneidensis ) is widely used in reduction processes such as microbial fuel generation due to its capacity to reduce electron acceptors. Often, these setups are labor-intensive to operate and require days to produce results, so use of a model assay would reduce the time and expenses needed for optimization. Our research developed a novel digital analysis method for analysis of graphene oxide flocculates that may be utilized as a model assay for reduction platforms featuring nanoparticles. Use of this model reduction assay will enable rapid optimization and drive improvements in the microbial fuel generation sector.

Bennett, Danielle T. (ORCID:0009000188748827)↗

DOE OSTI2022

Redox chemistry of plutonium and plutonium surrogates in vitrified nuclear wastes

Lanthanide borosilicate glasses containing Pu and the analog element, Ce, were subjects of an X-ray absorption spectroscopy investigation to quantify the +3/+4 ratio of the redox-sensitive element. The data show that the dominant oxidation states are +4 for Pu and +3 for Ce. The data also indicate that the reductive potential of glasses can be quantified, although allowances must be made for glass composition, from a solution chemistry method adapted to glass chemistry. These data can therefore be used to formulate glass compositions and processing schedules that lead to knowledge of the oxidation state of Pu in melts. Furthermore, the data show that Ce is a poor analog for Pu behavior in melt and that the suitability of surrogates can be evaluated by this method. The methods demonstrated in this paper can be used to estimate the oxidation states of a range of multi-valent elements as functions of temperature and composition with data from only a single redox couple.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2025

Burning conditions and transportation pathways determine biomass-burning aerosol properties in the Ascension Island marine boundary layer

Abstract. African biomass-burning aerosol (BBA) in the southeast Atlantic Ocean (SEA) marine boundary layer (MBL) is an important contributor to Earth's radiation budget, yet its representation remains poorly constrained in regional and global climate models. Data from the Layered Atlantic Smoke Interactions with Clouds (LASIC) field campaign on Ascension Island (7.95° S, 14.36° W) provide insight into how burning conditions, fuel type, transport pathways, and atmospheric processing affect the chemical, microphysical, and optical properties of BBA between June and September 2017. A total of 10 individual plume events characterize the seasonal evolution of the BBA properties. Early-season inefficient fires, determined by low refractory black carbon to above-background carbon monoxide mixing ratios (rBC : ΔCO), led to enhanced concentrations of organic- and sulfate-rich aerosols. Mid-season efficient fires, determined by higher rBC : ΔCO values, led to rBC-enriched BBA. A mix of efficient and inefficient fires later in the season resulted in conflicting BBA properties. Prolonged transport (∼ 10 d) through the MBL and lower free troposphere (FT) facilitated chemical and aqueous-phase processing, which led to a reduction in organic aerosol mass concentrations. This resulted in lower organic aerosol (OA) to rBC (OA : rBC) mass ratios (2–5) in the MBL compared to higher values (5–15) in the nearby FT. These atmospheric and cloud oxidation processes yield more light-absorbing BBA and explain the notably low single-scattering albedo at 530 nm (SSA530) values (< 0.80) observed in the MBL. This study establishes a robust correlation between SSA530 and OA : rBC across the MBL and FT, underscoring the dependency of optical properties on chemical composition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Operando High-Energy-Resolution X-ray Spectroscopy of Evolving Cu Nanoparticle Electrocatalysts for CO 2 Reduction

Advances in electrocatalysis research rely heavily on building a thorough mechanistic understanding of catalyst active sites under realistic operating conditions. Only recently have techniques emerged that enable sensitive spectroscopic data collection to distinguish catalytically relevant surface sites from the underlying bulk material under applied potential in the presence of an electrolyte layer. Here, we demonstrate that operando high-energy-resolution fluorescence detected X-ray absorption spectroscopy (HERFD-XAS) is a powerful spectroscopic method which offers critical surface chemistry insights in CO 2 electroreduction with sub-electronvolt energy resolution using hard X-rays. Combined with the high surface area-to-volume ratio of 5 nm copper nanoparticles, operando HERFD-XAS allows us to observe with clear evidence the breaking of chemical bonds between the ligands and the Cu surface as part of the ligand desorption process occurring under electrochemical potentials relevant for the CO 2 reduction reaction (CO 2 RR). In addition, the dynamic evolution of oxidation state and coordination number throughout the operation of the nanocatalyst was continuously tracked. With these results in hand, undercoordinated metallic copper nanograins are proposed to be the real active sites in the CO 2 RR. In conclusion, this work emphasizes the importance of HERFD-XAS compared to routine XAS in catalyst characterization and mechanism exploration, especially in the complicated electrochemical CO 2 RR.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Chemical and electrochemical pathways to low-carbon iron and steel

Currently, the iron and steel industry is responsible for 7% of global CO 2 emissions. In this review, we summarize the operational principles of current emissions-intensive steelmaking technologies and review emerging low- and zero-carbon technologies that could substantially reduce emissions. Current technologies that are discussed include blast furnaces, electric arc furnaces, and smelting. Promising low-carbon routes include use of alternative reductants for ore processing (hydrogen direct reduction, hydrogen plasma-smelting, hydrogen smelting, and ammonia-based reduction), electrolytic iron production (with aqueous and molten oxide electrolytes) and biocarbon-based electric arc furnace operation. Advantages of each approach are presented, and remaining research hurdles are identified.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Integration of Concentrating Solar Power with High Temperature Electrolysis for Hydrogen Production: Preprint

Hydrogen (H2) has been identified as a leading sustainable contender to replace fossil fuels in transportation and electricity generation. H2 production can be achieved by concentrating solar thermal power (CSP) systems collecting thermal energy from the sun to various chemical processes for fuel production. Fuel production via solar thermal chemical processes integrated with CSP uses the full spectrum of sunlight compared with photovoltaic power conversion and stores solar energy directly and efficiently [1]. The solar fuel production can be realized by thermochemical processes (e.g., water splitting for H2 production, carbon dioxide reduction, or methane reforming) or thermal electrochemical methods (e.g., integration with solid oxide electrolysis cell). Technology development for CSP-integrated solar fuel production requires broad technological bases from solar energy collection to chemical energy conversion. H2 generated from renewable sources can be an energy carrier for a carbon-free economy. Integrating CSP with high temperature electrolysis (HTE) using solid oxide electrolysis cells (SOEC) provides a renewable path for H2 generation. The CSP-HTE integration approach provides the benefit of thermal energy storage (TES) for continuous operation, improved capacity, and SOEC life. H2 gas has low energy density for transportation, pipeline networks are expensive, and H2 liquefaction is energy intensive. However, an alternative method for H2 distribution is to use carbon dioxide (CO2) capture and liquid hydrocarbon synthesis to convert solar energy into liquid fuels that are compatible with the existing fossil fuel infrastructure.

concentrating solar thermal power↗

NASA NTRS2017

Mirror coatings for large aperture UV optical infrared telescope optics

Large space telescope concepts such as LUVOIR and HabEx aiming for observations from far UV to near IR require advanced coating technologies to enable efficient gathering of light with important spectral signatures including those in far UV region down to 90nm. Typical Aluminum mirrors protected with MgF2 fall short of the requirements below 120nm. New and improved coatings are sought to protect aluminum from oxidizing readily in normal environment causing severe absorption and reduction of reflectance in the deep UV. Choice of materials and the process of applying coatings present challenges. Here we present the progress achieved to date with experimental investigations of coatings at JPL and at GSFC and discuss the path forward to achieve high reflectance in the spectral region from 90 to 300nm without degrading performance in the visible and NIR regions taking into account durability concerns when the mirrors are exposed to normal laboratory environment as well as high humidity conditions. Reflectivity uniformity required on these mirrors is also discussed.

Quijada, Manuel↗