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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 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Methods for carbon dioxide hydrogenation

A method of carbon dioxide hydrogenation comprises introducing gaseous water to a positive electrode of an electrolysis cell comprising the positive electrode, a negative electrode, and a proton-conducting membrane between the positive electrode and the negative electrode. The proton-conducting membrane comprises an electrolyte material having an ionic conductivity greater than or equal to about 10-2 S/cm at one or more temperatures within a range of from about 150° C. to about 650° C. Carbon dioxide is introduced to the negative electrode of the electrolysis cell. A potential difference is applied between the positive electrode and the negative electrode of the electrolysis cell to generate hydrogen ions from the gaseous water that diffuses through the proton-conducting membrane and hydrogenates the carbon dioxide at the negative electrode. A carbon dioxide hydrogenation system is also described.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

System and method for carbon dioxide reactor control

A system preferably including a carbon dioxide reactor. A method for carbon dioxide reactor control, preferably including selecting carbon dioxide reactor aspects based on a desired output composition, running a carbon dioxide reactor under controlled process conditions to produce a desired output composition, and/or altering the process conditions to alter the output composition.

Kuhl, Kendra↗
DOE OSTI2023

Mission Analysis for Marine Renewable Energy to Provide Power for Marine Carbon Dioxide Removal

The mission of this project was to provide a preliminary feasibility assessment of powering different marine carbon dioxide removal (mCDR), marine carbon capture, and marine carbon sequestration strategies with marine energy. In this report, carbon capture refers to methods that can separate or capture carbon dioxide (CO 2 ) from the air or ocean; carbon sequestration refers to methods that store CO 2 obtained by capture methods out of the atmosphere for long periods of time; and carbon dioxide removal (CDR) refers to methods that do both. The project found that mCDR powered by marine energy and offshore wind energy available in the United States could meet global CDR scales needed by 2040 and 2050 to limit warming to 1.5 degrees C by 2100. Note that this preliminary estimate assumes that it is possible to harvest all the marine and offshore wind resources available in the United States with existing technology options, and it does not account for the power needed for monitoring these methods, as these power needs are not yet well defined and require further research. Additionally, these CDR scales will still require emissions reductions.

16 TIDAL AND WAVE POWER↗
DOE OSTI2020

Hydrometeorological sensitivities of net ecosystem carbon dioxide and methane exchange of an Amazonian palm swamp peatland

Here, we report ecosystem-scale CO 2 and CH 4 flux observations for an Amazonian palm swamp peatland over a two-year period in relation to hydrometeorological forcings. Seasonal and short-term variations in hydrometeorological forcing had a strong effect on carbon dioxide and methane fluxes. High air temperature and vapor pressure deficit exerted an important limitation on photosynthesis during the dry season, while latent heat flux appeared to be insensitive to these climate drivers. Evidence from light-response analyses and flux partitioning support that photosynthetic activity was downregulated during dry conditions, while ecosystem respiration was either inhibited or enhanced depending on water table position. The cumulative net ecosystem carbon dioxide exchange indicated that the peatland was a significant carbon dioxide sink ranging from –465 (–279 to –651) g C m -2 y -1 in 2018 to –462 (–277 to –647) g C m -2 y -1 in 2019. The forest was a methane source of 22 (20 to 24) g C m -2 y -1 , similar in magnitude to other tropical peatlands and larger than boreal and arctic peatlands. Furthermore, the annual carbon budget of this Amazonian palm swamp peatland appears to be a major carbon sink under current hydrometeorological conditions, but evidence indicates that the sink strength is vulnerable to future climate change.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Landfilled coal ash for carbon dioxide capture and its potential as a geopolymer binder for hazardous waste remediation

In this report, the legacy of global fossil fuel usage is not just the increase in global warming due to CO 2 production, but also the billions of tons of toxic coal ash disposed in landfills. This investigation evaluates the merits of using high-calcium landfilled coal fly ash of different disposal durations and granulated blast furnace (GBF) slag as primary raw materials for production of a new class of geopolymer binder. Processing of landfilled coal fly ash, GBF slag and supplementary raw materials into a geopolymer binder was accomplished by a simple, scalable milling process in the absence of heating under a carbon dioxide environment. The resultant geopolymer cement binders were tested for carbon dioxide uptake, compressive strength, and heavy metal stabilization. The geopolymer binder demonstrated a desired balance of carbon dioxide uptake, strength and safety. These results also indicate that the performance of the geopolymer binder depends on the landfill disposal age of the coal fly ash.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2021

Engineering Second Sphere Interactions in a Host–Guest Multicomponent Catalyst System for the Hydrogenation of Carbon Dioxide to Methanol

Many enzymes utilize interactions extending beyond the primary coordination sphere to enhance catalyst activity and/or selectivity. Such interactions could improve the efficacy of synthetic catalyst systems, but the supramolecular assemblies employed by biology to incorporate second sphere interactions are challenging to replicate in synthetic catalysts. Herein, a strategy is reported for efficiently manipulating outer sphere influence on catalyst reactivity by modulating host–guest interactions between a noncovalently encapsulated transitionmetal-based catalyst guest and a metal–organic framework (MOF) host. This composite consists of a ruthenium PNP pincer complex encapsulated in the MOF UiO-66 that is used in tandem with the zirconium oxide nodes of UiO-66 and a ruthenium PNN pincer complex to hydrogenate carbon dioxide to methanol. Due to the method used to incorporate the complexes in UiO-66, structure–activity relationships could be efficiently determined using a variety of functionalized UiO-66-X hosts. These investigations uncovered the beneficial effects of the ammonium functional group (i.e., UiO-66-NH 3 + ). Mechanistic experiments revealed that the ammonium functionality improved efficiency in the hydrogenation of carbon dioxide to formic acid, the first step in the cascade. Isotope effects and structure–activity relationships suggested that the primary role of the ammonium functionality is to serve as a general Brønsted acid. Importantly, the cooperative influence from the host was effective only with the functional group in close proximity to the encapsulated catalyst. Here, reactions carried out in the presence of molecular sieves to remove water highlighted the beneficial effects of the ammonium functional group in UiO-66-NH 3 + and resulted in a 4-fold increase in activity. As a result of the modular nature of the catalyst system, the highest reported turnover number (TON) (19 000) and turnover frequency (TOF) (9100 h –1 ) for the hydrogenation of carbon dioxide to methanol are obtained. Moreover, the reaction was readily recyclable, leading to a cumulative TON of 100 000 after 10 reaction cycles.

08 HYDROGEN↗
DOE OSTI2020

The influence of lattice defects, recombination, and clustering on thermal transport in single crystal thorium dioxide

Thermal transport is a key controlling property for thorium dioxide in many applications where defect-generating radiation fields are present. An understanding of the effect of nanoscale lattice defects on thermal transport in this material is currently unavailable due to a lack of high-quality, single crystal material from which unit processes may be investigated. In this work, a series of thorium dioxide single crystals are exposed to 2 MeV proton irradiation at room temperature and 600°C to create microscale regions with varying densities and types of point and extended defects. Defected regions are investigated using spatial domain thermoreflectance to quantify the change in thermal conductivity as a function of ion fluence as well as transmission electron microscopy and Raman spectroscopy to interrogate the structure of the generated defects. Together, this com- bination of methods provides important initial insight into defect formation, recombination, and clustering in thorium dioxide and the effect of those defects on thermal transport. These methods also provide a promising pathway for the quantification of the smallest-scale defects which cannot be captured using traditional microscopy techniques and play and outsized role in degrading thermal performance.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

Temperature-dependent elastic constants of thorium dioxide probed using time-domain Brillouin scattering

Herein we report the adiabatic elastic constants of single-crystal thorium dioxide over a temperature range of 77–350 K. Time-domain Brillouin scattering, an all-optical, non-contact picosecond ultrasonic technique, is used to generate and detect coherent acoustic phonons that propagate in the bulk perpendicular to the surface of the crystal. These coherent acoustic lattice vibrations have been monitored in two hydrothermally grown single-crystal thorium dioxide samples along the (100) and (311) crystallographic directions. The three independent elastic constants of the cubic crystal (C 11 , C 12 , and C 44 ) are determined from the measured bulk acoustic velocities. The longitudinal wave along the (100) orientation provided a direct measurement of C 11 . Measurement of C 44 and C 12 was achieved by enhancing the intensity of quasi-shear mode in a (311) oriented crystal by adjusting the polarization angle relative to the crystal axes. We find the magnitude of softening of the three elastic constants to be ~2.5% over the measured temperature range. Good agreement is found between the measured elastic constants with previously reported values at room temperature, and between the measured temperature-dependent bulk modulus with calculated values. We find that semi-empirical models capturing lattice anharmonicity adequately reproduce the observed trend. We also determine the acoustic Grüneisen anharmonicity parameter from the experimentally derived temperature-dependent bulk modulus and previously reported temperature-dependent values of volumetric thermal expansion coefficient and heat capacity. This work presents measurements of the temperature-dependent elasticity in single-crystal thorium dioxide at cryogenic temperature and provides a basis for testing ab initio theoretical models and evaluating the impact of anharmonicity on thermophysical properties.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

A formaldehyde and nitrogen dioxide toxics monitor for environmental justice

DOE’s Integrated Field Laboratories (IFLs) require a vast array of measurements to measure urban air quality. Nitrogen dioxide (NO2) and formaldehyde (HCHO) are ubiquitous pollutants with numerous sources, most notably vehicle exhaust. High-spatial density measurements are critical to understanding how certain neighborhoods are more adversely impacted by pollutants. This report describes the results of a Phase I SBIR project to develop and demonstrate a rapid, affordable, low-power monitor to provide high spatial resolution mobile measurements of formaldehyde and nitrogen dioxide at street-level, where people live and walk. The spatial density will be achieved via rapid measurements on a mobile platform. This sensor will quantify spatial disparities in cities of the toxics, HCHO and NO2, as well as carbon monoxide and carbon dioxide for better source identification. These species are detected in the mid infrared by laser absorption spectroscopy, and fiberoptics are used. Tasks accomplished include identification and testing of the appropriate spectroscopic regions; coupling of laser light into a fiberoptic system; development of software to control miniature electronics to scan and control two lasers simultaneously; coupling of the mid infrared fiber into a multipass cell for enhanced pathlength and sensitivity; characterization of sources of instrument noise; and design work for a Phase II prototype.

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

Linking the Dynamic Response of the Carbon Dioxide-Concentrating Mechanism to Carbon Assimilation Behavior in Fremyella diplosiphon

ABSTRACT Cyanobacteria use a carbon dioxide (CO 2 )-concentrating mechanism (CCM) that enhances their carbon fixation efficiency and is regulated by many environmental factors that impact photosynthesis, including carbon availability, light levels, and nutrient access. Efforts to connect the regulation of the CCM by these factors to functional effects on carbon assimilation rates have been complicated by the aqueous nature of cyanobacteria. Here, we describe the use of cyanobacteria in a semiwet state on glass fiber filtration discs—cyanobacterial discs—to establish dynamic carbon assimilation behavior using gas exchange analysis. In combination with quantitative PCR (qPCR) and transmission electron microscopy (TEM) analyses, we linked the regulation of CCM components to corresponding carbon assimilation behavior in the freshwater, filamentous cyanobacterium Fremyella diplosiphon . Inorganic carbon (C i ) levels, light quantity, and light quality have all been shown to influence carbon assimilation behavior in F. diplosiphon . Our results suggest a biphasic model of cyanobacterial carbon fixation. While behavior at low levels of CO 2 is driven mainly by the C i uptake ability of the cyanobacterium, at higher CO 2 levels, carbon assimilation behavior is multifaceted and depends on C i availability, carboxysome morphology, linear electron flow, and cell shape. Carbon response curves (CRCs) generated via gas exchange analysis enable rapid examination of CO 2 assimilation behavior in cyanobacteria and can be used for cells grown under distinct conditions to provide insight into how CO 2 assimilation correlates with the regulation of critical cellular functions, such as the environmental control of the CCM and downstream photosynthetic capacity. IMPORTANCE Environmental regulation of photosynthesis in cyanobacteria enhances organismal fitness, light capture, and associated carbon fixation under dynamic conditions. Concentration of carbon dioxide (CO 2 ) near the carbon-fixing enzyme RubisCO occurs via the CO 2 -concentrating mechanism (CCM). The CCM is also tuned in response to carbon availability, light quality or levels, or nutrient access—cues that also impact photosynthesis. We adapted dynamic gas exchange methods generally used with plants to investigate environmental regulation of the CCM and carbon fixation capacity using glass fiber-filtered cells of the cyanobacterium Fremyella diplosiphon . We describe a breakthrough in measuring real-time carbon uptake and associated assimilation capacity for cells grown in distinct conditions (i.e., light quality, light quantity, or carbon status). These measurements demonstrate that the CCM modulates carbon uptake and assimilation under low-C i conditions and that light-dependent regulation of pigmentation, cell shape, and downstream stages of carbon fixation are critical for tuning carbon uptake and assimilation.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2022

Basic Energy Sciences Roundtable: Foundational Science for Carbon Dioxide Removal Technologies (Brochure)

Basic research to identify and understand the fundamental principles governing carbon dioxide removal processes of capture, conversion, and storage is essential for achieving zero carbon emissions by 2050. In March 2022, the Office of Basic Energy Sciences (BES)—in coordination with the US Department of Energy (DOE) technology Offices of Energy Efficiency and Renewable Energy, Fossil Energy and Carbon Management, and Nuclear Energy—held a roundtable titled, “Foundational Science for Carbon Dioxide Removal Technologies,” to discuss the scientific and technical barriers for CO 2 capture, conversion, and storage. Five priority research opportunities were identified to address these scientific and technical challenges and accelerate progress toward the realization of zero carbon emissions. The PROs are as follows: 1) Master Interfacial Processes of CO2 Transport and Reactivity Across Multiple Length and Time Scales; 2) Create Materials that Simultaneously Exhibit Multiple Properties for CO 2 Capture and Release or Conversion; 3) Discover Unconventional Pathways for Energy-Efficient CO 2 Capture, Release, and Conversion; 4) Control Multiphase Interactions Required for CO 2 Conversion into Minerals and Materials; and 5) Achieve Predictive Understanding of Coupled Processes in Complex Subsurface Geologic Systems for Secure Carbon Storage.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Photosynthesis | Photosynthetic Carbon Dioxide Fixation

Carbon dioxide is reduced to make the molecules of life such as proteins, lipids, carbohydrates, and nucleic acids and as the primary mechanism of energy storage for the biosphere. Reduction of fully oxidized carbon, carbon dioxide, occurs following carboxylation of preexisting molecules rather than direct reduction of carbon dioxide to formic acid or formaldehyde. Furthermore, the primary pathway is called the Calvin Benson cycle and proceeds mostly as a series of gluconeogenic (reversal of glycolytic) reactions plus a few pentose phosphate pathway reactions.

Aldolase reaction↗
DOE OSTI2020

A new approach of reduction of carbon dioxide emission and optimal use of carbon and hydrogen content for the desired syngas production from coal

We report this research is designed to make progress in overcoming the challenges through the development of a two-stage coal processing. Specifically, a two-stage process was used to maximize the use of the carbon in coal or increase the carbon monoxide yield or lower carbon dioxide and methane yields. Carbon dioxide-char gasification in the absence of water can generate carbon monoxide with near-zero methane, which is desired to produce high-carbon and low-hydrogen chemicals such as oxalic acid through catalytic carbon monoxide coupling and hydrolysis. The technology is applicable to any coal, although Power River Basin (PRB) coal is used as an example feedstock in this research Also, the sodium-iron catalyst can accelerate not only the reaction kinetics in both stages but also increase the hydrogen/carbon monoxide ratio in the syngas produced in the second stage. In other words, the catalyst is a multifunctional agent, which can not only intensify the overall coal process efficiency but also improve the qualities of the desired syngas products and reduce carbon dioxide emission. Thus, In the 1st stage, the catalysts can significantly reduce the CO 2 -char gasification by as high as 75.00%. In the 2nd stage, the H 2 /CO ratio of ideal syngas is ~2:1 with near-0 CH 4 generation and the CH4 production can be reduced as high as 61.29% for the CO 2 –H 2 O-Char coal gasification. The activation energy for the 2nd stage is reduced by as high as 35.43% than that of raw coal without use Na–Fe catalyst. The overall carbon footprint reduction for the study is reduced by 87.33% in the 1st stage and 96.77% compared to the direct coal combustion.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2024

Formation of uranium oxy-carbide and uranium carbide via conversion of polymer covered uranium dioxide by laser-based thermal processing

Conventional formation of carbonaceous uranium compounds requires bulk processing using furnace-based approaches. Here, a methodology employing polymer covered uranium dioxide and laser-based heating is explored to enable rapid, localized formation of carbonaceous uranium compounds. Specifically, heating of poly(methyl methacrylate) covered uranium dioxide powder to high temperatures using laser irradiation in argon and methane gaseous environments was investigated. Decomposition of material and reactions induced by laser irradiation were probed in situ by residual gas analysis using a benchtop mass spectrometer. In this study, to determine the effect on the resultant material phase, three different process parameters were varied: gaseous atmosphere, laser power, and laser irradiation time. Material processed under varying conditions was analyzed using powder X-ray diffraction and scanning electron microscopy. This work realized the conversion of uranium dioxide into uranium oxy-carbide(s) and uranium carbide(s) phases, at over 60 wt.%, via the polymer surface application and laser-based thermal decomposition methodology.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Hydrolysis of Metal Dioxides Differentiates d-block from f-block Elements: Pa(V) as a 6d Transition Metal; Pr(V) as a 4f “Lanthanyl”

Gas-phase reactions of pentavalent metal dioxide cations M V O 2 + with water were studied experimentally for M = V, Nb, Ta, Pr, Pa, U, Pu, and Am. Addition of two H 2 O can occur by adsorption to yield hydrate (H 2 O) 2 M V O 2 + or by hydrolysis to yield hydroxide M V (OH) 4 + . Displacement of H 2 O by acetone indicates hydrates for Pr V , U V , Pu V , and Am V , whereas nondisplacement indicates hydroxides for Nb V , Ta V , and Pa V . Computed potential energy profiles agree with the experimental results and furthermore indicate that acetone unexpectedly induces dehydrolysis and displaces two H 2 O from (H 2 O)VO(OH) 2 + to yield (acetone) 2 VO 2 + . Structures and energies for several M V , as well as for Th IV and U VI , indicate that hydrolysis is governed by the involvement of valence f versus d orbitals in bonding: linear f-element dioxides are more resistant to hydrolysis than bent d-element dioxides. Accordingly, for early actinides, hydrolysis of Th IV is characteristic of a 6d-block transition metal; hydration of U V and U VI is characteristic of 5f actinyls; and Pa V is intermediate between 6d and 5f. The praseodymium oxide cation Pr V O 2 + is assigned as an actinyl-like lanthanyl with properties governed by 4f bonding.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Microcarbonation of Naphthalene: An Experimental and Computational Study of Photoionization in Naphthalene-Carbon Dioxide Clusters

The photoionization of naphthalene (N)-carbon dioxide (CO 2 ) clusters was studied using tunable vacuum ultraviolet (VUV) radiation from a synchrotron in the photon range of 8.0 to 13.7 eV, in combination with time-of-flight mass spectrometry. Clusters of monomer, dimer, and trimer naphthalene with CO 2 (N­(CO 2 ) 0–6 , N 2 ­(CO 2 ) 0–3 , N3) were observed. The lowest-energy conformers were obtained via a conformer search, followed by geometry optimizations at the ωB97X-V2/aug-cc-pVTZ (monomer) and ωB97X-V2/aug-cc-pVDZ (dimer) levels of theory. Carbon dioxide was found to preferentially cluster on top of the naphthalene molecule (in an out-of-plane configuration). From the mass spectra, photoionization intensity curves (PICs) were constructed, and appearance energies (AEs) were determined. No substantial trend in AE was observed with increasing size of the naphthalene-carbon dioxide clusters; rather, AE oscillations around the value for pure naphthalene were observed. These AE oscillations are also observed in a recently studied naphthalene-water cluster system, though in this system a slight downward trend in AE for pure naphthalene clusters (N1/2/3/4) was observed. The differences between the two systems are attributed to differing interaction strengths. In conclusion, understanding these differences may aid in determining how photoprocessing can proceed differently depending on the dominant matrix component in interstellar ices.

Wannenmacher, Anna [Lawrence Berkeley National Lab↗
DOE OSTI2024

Capturing carbon dioxide from air with charged-sorbents

Emissions reduction and greenhouse gas removal from the atmosphere are both necessary to achieve net-zero emissions and limit climate change. There is thus a need for improved sorbents for the capture of carbon dioxide from the atmosphere, a process known as direct air capture. In particular, low-cost materials that can be regenerated at low temperatures would overcome the limitations of current technologies. In this work, we introduce a new class of designer sorbent materials known as ‘charged-sorbents’. These materials are prepared through a battery-like charging process that accumulates ions in the pores of low-cost activated carbons, with the inserted ions then serving as sites for carbon dioxide adsorption. We use our charging process to accumulate reactive hydroxide ions in the pores of a carbon electrode, and find that the resulting sorbent material can rapidly capture carbon dioxide from ambient air by means of (bi)carbonate formation. Unlike traditional bulk carbonates, charged-sorbent regeneration can be achieved at low temperatures (90–100 °C) and the sorbent’s conductive nature permits direct Joule heating regeneration using renewable electricity. Given their highly tailorable pore environments and low cost, we anticipate that charged-sorbents will find numerous potential applications in chemical separations, catalysis and beyond.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Uncertainty in determining carbon dioxide removal potential of biochar

A quantitative and systematic assessment of uncertainty in life-cycle assessment is critical to informing sustainable development of carbon dioxide removal (CDR) technologies. Biochar is the most commonly sold form of CDR to date and it can be used in applications ranging from concrete to agricultural soil amendments. Previous analyses of biochar rely on modeled or estimated life-cycle data and suggest a cradle-to-gate range of 0.20–1.3 kg CO 2 net removal per kg of biomass feedstock, with the range reported driven by differences in energy consumption, pyrolysis temperature, and feedstock sourcing. Herein, we quantify the distribution of CDR possible for biochar production with a compositional life-cycle inventory model paired with scenario-aware Monte Carlo simulation in a 'best practice' (incorporating lower transportation distances, high pyrolysis temperatures, high energy efficiency, recapture of energy for drying and pyrolysis energy requirements, and co-generation of heat and electricity) and 'poor practice' (higher transportation distances, lower pyrolysis temperatures, low energy efficiency, natural gas for energy requirements, and no energy recovery) scenarios. In the best-practice scenario, cradle-to-gate CDR (which is representative of the upper limit of removal across the entire life cycle) is highly certain, with a median removal of 1.4 kg of CO 2 e/kg biomass and results in net removal across the entire distribution. In contrast, the poor-practice scenario results in median net emissions of 0.090 kg CO 2 e/kg biomass. Whether this scenario emits (66% likelihood) or removes (34% likelihood) carbon dioxide is highly uncertain. The emission intensity of energy inputs to the pyrolysis process and whether the bio-oil co-product is used as a chemical feedstock or combusted are critical factors impacting the net carbon dioxide emissions of biochar production, together responsible for 98% of the difference between the best- and poor-practice scenarios.

54 ENVIRONMENTAL SCIENCES↗