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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

Microwave-Assisted Reactive CO 2 Capture with the SrCO 3 -Graphite System

This study details the initial development of a microwave heat-driven reactive CO 2 capture (RCC) process using the SrO/SrCO 3 cycle and graphitic carbon to absorb ppm-levels of CO 2 from humidified room temperature air and selectively convert it into CO. By combining first-principles density functional theory (DFT) simulations with thermogravimetric analysis (TGA) and X-ray diffraction (XRD) verification, it is demonstrated that SrO spontaneously absorbs moisture to generate Sr(OH) 2 followed by Sr(OH) 2 *1H 2 O, which then can spontaneously react with atmospheric levels of CO 2 to form SrCO 3 . The resulting SrCO 3 can then react with solid carbon at elevated temperatures to selectively produce CO and regenerate SrO. Graphitic carbon is an excellent microwave absorber that can quickly generate temperatures approaching 1000 °C and then cool to room temperature within minutes, potentially allowing for integration with intermittent electricity. It is shown that using microwaves to selectively heat a mixture of graphitic carbon and SrCO 3 produced CO with 85 ± 3% selectivity and stable performance over ten cycles. The rapid heating for release and room temperature CO 2 uptake processes appeared to prevent performance loss from particle sintering typically observed with traditional thermal systems. In conclusion, these results demonstrate a new RCC approach that adds to the growing number of potential technologies available for converting CO 2 to useful chemicals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Benchmark Exercise for the Control Rod Swelling Evaluation

The VTR core has six reactivity control assemblies and three safety assemblies. The control assemblies or primary control rods are adjusted during the normal operation to balance the core reactivity and to control the reactor power. A typical control assembly radial layout is presented in Figure 1. The figure shows the swelled absorber (B 4 C) rod. Initially, helium gas fills the gap between the pin and the cladding before irradiation swelling takes place. For VTR, HT9 steel was selected as the cladding and duct material. The main neutron absorbing material used in the VTR is B 4 C. When residing in the core, the neutronics, thermophysical, and mechanical properties of the materials used in a control assembly will degrade due to accumulated neutron damage. Material degradation limits how long a control assembly can reside in the core. Many phenomena affect the control assembly lifetime, such as the loss of reactivity worth due to B 4 C depletion, the mechanical interaction of the absorber rod and the cladding due to B 4 C swelling, the helium gas buildup in the pin due to B-10 capture, etc. B 4 C swelling, which causes closure of the gap between the absorber rod and the cladding, is usually considered as the main limiting factor from past experience. An initial study was conducted at PNNL to evaluate the irradiation behavior of a VTR control assembly. The evaluation was performed using the CNRD2 code that was initially developed for the FFTF. The study also included an assessment of the VTR control assembly and focused on a 61-pin control assembly design, which is different from that used (37-pin design) in the core design study. The study conducted by PNNL was reviewed independently by ANL. A Python script referred to as the Control Assembly Evaluation Script (CAES) was developed for the independent review and additional assessment of 37-pin control assembly design. The script has focused on the assessment of the absorber rod swelling for its importance in determining the control assembly lifetime. CAES uses geometry, neutronics, materials data as input to predict the swelling of the absorber rod during its residence in the reactor core. The results from CAES showed some non-negligible differences against the PNNL results. Some of the differences can be attributed to the different interpretation of the control rod assembly dimensions. To resolve this issue, a benchmark exercise was proposed. The benchmark specification was developed by PNNL. The benchmark exercise was performed independently at PNNL and ANL using different codes/scripts (CRND2 and CAES). This memo documents the results calculated using the different codes. However, this report is limited to presenting the results obtained. Further investigation of the cause of the observed difference will be performed as part of future activities, pending continuation of the VTR program.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Nanoscale Measurements of Charge Transfer at Cocatalyst/Semiconductor Interfaces in BiVO 4 Particle Photocatalysts

Semiconductor photocatalyst particles convert solar energy to fuels like H 2 . The particles are often assumed to provide crystalline-facet-dependent electron-hole separation. A common strategy is to deposit HER electrocatalyst on electron-selective facets and OER electrocatalyst on hole-selective facets. A precise understanding of how charge-carrier-selective contacts emerges and how they rationally designed, however, is missing. Using a combination of ex-situ and in-situ conducting-AFM experiments and new ionomer/catalyst-semiconductor test structures, we show how heterogeneity in charge-carrier selectivity can be measured at the nanoscale. We discover that the presence of interface water/electrolyte is critical to induce hole selectivity between the CoO x water-oxidation catalyst and the BiVO 4 light absorber. pH-dependent measurements suggest that negative surface charge on the semiconductor is central to inducing hole selectivity. Furthermore, the work also demonstrates a new approach to control local pH and introduce water using thin-film ionomers compatible with conductive-AFM measurements.

14 SOLAR ENERGY↗

Absolute decay counting of 146 Sm with 4π cryogenic microcalorimetry

We present a methodology for absolute activity counting of long-lived isotopes based on cryogenic Decay Energy Spectroscopy. A 146 Sm source was produced at the TRIUMF Laboratory and then processed and purified at Lawrence Livermore National Laboratory, yielding a pure sample. The source was embedded within a 4π thermal absorber coupled to a magnetic microcalorimeter achieving nearly 100% counting efficiency. Experimental uncertainties were studied and modeled, including thermal coupling of the source to the absorber, pulse pile-up, trigger, and event selection efficiencies. Here, the absolute activity of the pure 146 Sm source was measured to better than 1% uncertainty.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Direct Air Capture-Compatible Azolate and Amino Acid Ionic Liquids for Electrochemical CO 2 Reduction to CO on a Silver Cathode

Direct air capture (DAC) compatible ionic liquids (ILs) are attractive for integrating CO 2 capture and conversion due to their high CO 2 solubility at low partial pressures, tunable chemisorption mechanisms, low volatility, and wide electrochemical windows. However, very few ILs have high CO 2 uptake at DAC conditions (420 ppm CO 2 ), and even fewer have been evaluated for chemical compatibility and mechanistic continuity for combined capture and electrochemical CO 2 reduction (eCO 2 RR). We demonstrate that two representative DAC-capable ILs, [P 4444 ][Val] (amino acid-based) and [P 66614 ][5-Me-Imd] (azolate-based), exhibit favorable electrochemical reduction behavior. CO and H 2 were the dominant gas-phase products by GC, while 1 H and 13 C NMR confirmed negligible liquid-phase HCOOH. Chronoamperometry at moderate applied potentials (−2.0 to −2.5 V vs Ag/AgCl) in a two-compartment H-cell with a Ag coated carbon paper as the working electrode yielded steady-state current densities of ∼10 mA cm −2 with CO FE of 96% for [P 4444 ][Val] and 95% for [P 66614 ][5-Me-Imd], highlighting the role of viscosity and chemically absorbed CO 2 -IL species to provide highly selective CO formation while suppressing H 2 evolution.

amino acid ionic liquid↗

Isotope-selective radiography and material assay using high-brilliance, quasi-monochromatic, high-energy photons

We demonstrate the possibility to directly detect microgram amounts of the isotope 7 Li using a quasi-monochromatic high-energy photon beam. The isotope selective detection is based on a witness scatterer absorbing and re-emitting photons via nuclear resonance fluorescence. This enables the detection of isotopes with microgram accuracy at long distances from the actual sample. Further, we demonstrate that the technique can deliver quantitative information without specific knowledge of the photon flux and no spectral capabilities or knowledge of the resonance fluorescence cross section. Detection of low-atomic-weight isotopes screened by heavy shielding is also shown. The techniques described are applicable to all next-generation, ultrahigh brilliance, laser-Compton light sources currently under construction.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Decoupling absorption and radiative cooling in mid-wave infrared bolometric elements

We present a spectrally selective, passively cooled mid-wave infrared bolometric absorber engineered to spatially and spectrally decouple infrared absorption and thermal emission. The structure leverages an antenna-coupled metal–insulator–metal resonance for mid-wave infrared normal incidence photon absorption and a long-wave infrared optical phonon absorption feature, aligned closer to peak room temperature thermal emission. The phonon-mediated resonant absorption enables a strong long-wave infrared thermal emission feature limited to grazing angles, leaving the mid-wave infrared absorption feature undisturbed. The two independently controlled absorption/emission phenomena demonstrate decoupling of the photon detection mechanism from radiative cooling and offer a new design approach enabling ultra-thin, passively cooled mid-wave infrared bolometers.

Ware, Alexander (ORCID:0009000256937727)↗

Fundamental Science for Enhancing the Durability of Photoelectrodes for Solar Fuels Production

During the award period, we performed a series of investigations to address a key bottleneck in solar-driven fuel production, which is materials stability. Regardless of the activity of electrocatalysts or selectivity of products, or efficiency of the light absorbers, if the systems are not stable then there is no ultimate technological relevance for solar fuels production. Degradation of semiconductor photoelectrodes is a well-known, long-recognized impediment to implementation of practical stable solar fuels systems. Thus, we aimed to define the thermodynamics and kinetics of the (electro)chemical processes that underpin corrosion of semiconductor photoelectrodes. We also sought to develop protective coatings and kinetic control strategies to extend durability of semiconductor photoelectrodes.

14 SOLAR ENERGY↗

DESI Survey Validation Data in the COSMOS/Hyper Suprime-Cam Field: Cool Gas Trace Main-sequence Star-forming Galaxies at the Cosmic Noon

We present the first result in exploring the gaseous halo and galaxy correlation using the Dark Energy Spectroscopic Instrument survey validation data in the Cosmic Evolution Survey (COSMOS) and Hyper Suprime-Cam field. We obtain multiphase gaseous halo properties in the circumgalactic medium by using 115 quasar spectra (signal-to-noise ratio > 3). We detect Mg ii absorption at redshift 0.6 < z < 2.5, C iv absorption at 1.6 < z < 3.6, and H i absorption associated with the Mg ii and C iv. By crossmatching the COSMOS2020 catalog, we identify the Mg ii and C iv host galaxies in 10 quasar fields at 0.9< z < 3.1. We find that within the impact parameter of 250 kpc, a tight correlation is seen between the strong Mg ii equivalent width and the host galaxy star formation rate. The covering fraction f c of the strong Mg ii selected galaxies, which is the ratio of the absorbing galaxy in a certain galaxy population, shows significant evolution in the main-sequence galaxies and marginal evolution in all the galaxy populations within 250 kpc at 0.9 < z < 2.2. The f c increase in the main-sequence galaxies likely suggests the coevolution of strong Mg ii absorbing gas and the main-sequence galaxies at the cosmic noon. Furthermore, Mg ii and C iv absorbing gas is detected out of the galaxy virial radius, tentatively indicating the feedback produced by the star formation and/or the environmental effects.

79 ASTRONOMY AND ASTROPHYSICS↗

CIGS photovoltaics: reviewing an evolving paradigm

Copper indium selenide chalcopyrite-structure alloys with gallium (CIGS) are unique among the highest performing photovoltaic (PV) semiconductor technologies. They are structurally disordered, nonstoichiometric materials that have been engineered to achieve remarkably low bulk nonradiative recombination levels. Nevertheless, their performance can be further improved. This review adopts a fundamental thermodynamic perspective to comparatively assess the root causes of present limitations on CIGS PV performance. The topics of selectivity and passivation of contacts to CIGS and its multinary alloys are covered, highlighting pathways to maximizing the electrochemical potential between those contacts under illumination. Further, an overview of absorber growth methods and resulting properties is also provided. We recommend that CIGS researchers consider strategies that have been successfully implemented in the more mature wafer-based GaAs and Si PV device technologies, based on the paradigm of an idealized PV device design using an isotropic absorber with minimal nonradiative recombination, maximal light trapping, and both electron-selective and hole-selective passivated contacts. We foresee that CIGS technology will reach the 25% efficiency level within the next few years through enhanced collection and reduced recombination. To significantly impact power-generation applications, cost-effective, manufacturable solutions are also essential.

14 SOLAR ENERGY↗

IER-499 Final Design of a TEX Variant: Chlorine to Support NNSA Operations [Slides]

This presentation concludes the final design of TEX with chlorine absorbers is complete. 5 configurations were identified, expected to down select to three experimental configurations. Great comparison to Y-12 and good comparison to INL sensitivities. Fastest configuration touches on the 35 Cl(n,p) cross section (continuing to work with Terrapower for faster configurations). Extensive density studies performed to ensure understanding of the salt in the plates. Reactivity studies performed to assist with experiment. Finally, the fabrication of the chlorine absorbers is ongoing (with LANL), and the experiment is scheduled to be completed this year.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Investigation of the Selectivity of Carrier Transport Layers in Wide-Bandgap Perovskite Solar Cells

Excellent contact passivation and selectivity are prerequisites to realize the full potential of high-material-quality perovskite solar cells, first to maximize the internal voltage (or quasi-Fermi-level separation) iV within the absorber, then to translate this high internal voltage into a high external voltage V. Experimental quantification of contact passivation and selectivity is, thus, key to improving device performance. Here, open-circuit measurements of iV oc and V oc , combined with surface photovoltage measurements, are used to systematically quantify the passivation—using iVoc as a metric—and the selectivity—defined as Soc=V oc /iV oc —of a range of common carrier transport layers to wide-bandgap (1.67 eV) perovskite absorbers. The resulting solar cells suffer from large voltage deficits, particularly when NiO x is used as the hole transport layer, even though it provides better passivation than its polymer-based counterparts (PTAA and PTAA/PFN). This indicates a poor selectivity of NiO x (Soc<0.81 for NiO x -based devices), whereas devices using polymer-based hole transport layers exhibit high selectivity (S oc =0.94–0.95). In agreement with recent reports, this low selectivity is attributed to the formation of an interlayer of non-perovskite material with high resistance to holes at the perovskite/NiO x interface. These measurements also imply that the selectivity of the C60-based electron transport layers is relatively good.

carrier transport layers↗

Selective sulfur removal from semi-dry flue gas desulfurization coal fly ash for concrete and carbon dioxide capture applications

High-sulfur mixed fly ash residues from semi-dry flue gas desulfurization units in coal-fired power plants are unsuitable for use as supplementary cementitious material (SCM) for concrete production or carbon dioxide utilization. In this work, we explore the potential for upcycling a representative spray dry absorber ash (10.44 wt% SO 3 ) into concrete-SCM by selective sulfur removal via weak acid dissolution while simultaneously exploring the possibility for CO 2 capture. Towards this effort, parametric studies varying liquid-to-solid ratio, acidity, and CO 2 pressure were conducted in a batch reactor to establish the sulfur removal characteristics in de-ionized water, nitric acid, and carbonic acid, respectively. The dissolution studies show that the leaching of sulfur from calcium sulfite hemihydrate, which is the predominant S phase, is rapid and achieves a concentration plateau within 5 min, and subsequently, appears to be controlled by the primary mineral solubility. Here, preferential S removal was sufficient to meet SCM standards (e.g., 5.0 wt% as per ASTM C618) using all three washing solutions with 0.62–0.72 selectivity (S^), defined as the molar ratio of S to Ca in the leachate, for a raw fly ash with bulk S^ = 0.3. Acid dissolution with 1.43 meq/g of ash or under 5 atm CO 2 retained > 18 wt% CaO and other Si-, Al-rich phases in the fly ash. Based on the experimental findings, two sulfur removal schemes were suggested for either integration with CO 2 capture and utilization processes using flue gas or to produce fly ash for use as a SCM.

01 COAL, LIGNITE, AND PEAT↗

Molecular catalyst coordinatively bonded to organic semiconductors for selective light-driven CO 2 reduction in water

The selective photoreduction of CO 2 in aqueous media based on earth-abundant elements only, is today a challenging topic. Here we present the anchoring of discrete molecular catalysts on organic polymeric semiconductors via covalent bonding, generating molecular hybrid materials with well-defined active sites for CO 2 photoreduction, exclusively to CO in purely aqueous media. The molecular catalysts are based on aryl substituted Co phthalocyanines that can be coordinated by dangling pyridyl attached to a polymeric covalent triazine framework that acts as a light absorber. This generates a molecular hybrid material that efficiently and selectively achieves the photoreduction of CO 2 to CO in KHCO 3 aqueous buffer, giving high yields in the range of 22 mmol g -1 (458 μmol g -1 h -1 ) and turnover numbers above 550 in 48 h, with no deactivation and no detectable H 2 . The electron transfer mechanism for the activation of the catalyst is proposed based on the combined results from time-resolved fluorescence spectroscopy, in situ spectroscopies and quantum chemical calculations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Bicarbonate-Carbonate Selectivity through Nanofiltration for Direct Air Capture of Carbon Dioxide

Direct air capture (DAC) of carbon dioxide is one approach among many proposed that is capable of offsetting hard-to-avoid emissions. In previous work, we developed the alkalinity concentration swing (ACS) method, which is driven through concentrating an alkaline solution that has been loaded with atmospheric CO 2 by desalination technologies, such as reverse osmosis or capacitive deionization. Though the ACS is promising in terms of energy usage and implementation, its absorption rate and water requirements are infeasible for a large-scale DAC process. Here, we propose an improvement on the ACS, the bicarbonate-enriched alkalinity concentration swing (BE-ACS), which selects bicarbonate ions from a stream of aqueous alkaline solution that has absorbed atmospheric CO 2 . The bicarbonate-rich stream is then concentrated, which greatly increases its CO 2 partial pressure, and then CO 2 is extracted from solution. We experimentally investigate the use of pressure-driven nanofiltration (NF) membrane-based separation to select bicarbonate ions over carbonate ions. We screen commercial membranes and select one high-performance membrane for detailed studies, quantifying its bicarbonate-carbonate selectivity factor and bicarbonate-passage factor. Feed pH, the combined concentration of aqueous CO 2 , bicarbonate, and carbonate species (or dissolved inorganic carbon), alkalinity, and permeation flux are systematically varied to study NF separation properties. We find that the selectivity factor, which exceeds 30 times in certain regimes, increases with higher feed pH and higher alkalinity. Lastly, the performance metrics of the selected NF membrane are input into a theoretical BE-ACS cycle analysis, and the required energy input and cycle capacity output are evaluated. Ideal cycle energy is found to be as low as around 250 kJ/mol, with opportunities identified for further decreases through process engineering and forward osmosis energy recovery.

animal feed↗

Towards non-contact pollution monitoring in sewers with hyperspectral imaging

Monitoring water quality in sewers is challenging, particularly because state-of-the-art technologies require contact with the raw wastewater. The presence of fat, oil, grease, and solids makes automated grab sampling difficult and causes sensor fouling. To overcome these limitations, non-contact methods based on light reflectance, such as hyperspectral imaging (HSI), are gaining attention. However, HSI has never been tested for raw wastewater. To assess its accuracy for measuring pollution, we developed a laboratory setup and performed targeted experiments with a combination of raw and diluted wastewater, as well as synthetic turbidity stock solutions. We measured seven pollution variables: chemical oxygen demand, turbidity, dissolved organic compounds, ammonium, total nitrogen, phosphate, and sulphates. We used automated pixel selection and partial least squares regression to retrieve pollution information from the hyperspectral images. Our results, based on 144 samples, suggest that HSI can estimate pollution levels with a precision in the range of state-of-the-art absorbance spectrophotometric methods. Additionally, we found that the combination of pixel and wavelength selection, enabled by the hyperspectral data structure, significantly influences the performance of partial least square modelling. Overall, our findings indicate that HSI is a promising technology for non-contact monitoring of water quality in raw wastewater.

54 ENVIRONMENTAL SCIENCES↗

EPCAPE-PT-LANL Measurements: Single Particle Soot Photometer

Coastal cities offer a unique environment for studying aerosol-cloud interactions and the effects of urban emissions on cloud properties. As part of the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE), the Partitioning Thrust by Los Alamos National Laboratory (EPCAPE-PT-LANL) was conducted. Our campaign focused on measuring the optical and chemical properties of aerosols and their interactions within marine stratocumulus clouds in La Jolla, California. EPCAPE-PT-LANL enhances the primary goals of EPCAPE through innovative observations of vapor-phase transitions between aerosols and cloud droplets, the impact of black carbon on aerosol-cloud dynamics, and the effects of cloud processing on aerosol optical properties. Instrument: Single Particle Soot Photometer (Droplet Measurements Technology) Data Notes: Contact us if you want additional data products from this instrument. Reported data is the black carbon (rBC) number and mass concentration with diagnostic flags. The SP2 measures incandescence from particles that is induced with a 1064 Nd-YAG laser. Particles that absorb the laser energy and then emit radiation is assumed to contain black carbon. The amount of intensity of radiation is related to the mass of absorbing material in the particle. Here, we calibrate the incandescence intensity to size selected Regal Black (Cabot) nebulized from solution. Data provided for the EPCAPE campaign used the combined broadband high-gain + low-gain channels (BHBL). Each channel has a lower threshold of detection equivalent to 2-s of the respective channel noise. Thresholding has been applied to select between the high-gain and low-gain channels. The detection limit is 80-540 nm (Deq) or 0.36- 55 fg. It is assumed that rBC is the only aerosol type that is in significant concentration in the sampled atmosphere that absorbs the laser energy. Particle data are integrated over 10 second windows to calculate a rBC number and mass concentration. QC/QA: • Diagnostic flags that impacted measured concentration: - Sample, Sheath, and Purge Flow Rates: Despite observing fluctuations in all flows, the rBC detection and mass quantification are generally observed to be stable, although large changes in sample flow rate did impact detection efficiency. A flag was implemented for sample flow deviations >12 cm3/min from the set point averaged over 30 seconds - Laser Power: Detection efficiency decreases with laser power and deviations in laser power also affect mass quantification. Flag for laser power is set for deviations in laser current from the set value >5 mA. - Primary Detector Threshold: Primary thresholding is the signal value which determines whether a “particle” is recorded. Thresholding errors occur when the threshold value is too HIGH and real particles are ignored. • Several periods without data: - 16-18 Nov: Ultra Zero Air generator failure, flows deviated significantly from set points. rBC # conc recovered but questionable. - 20-21 Nov: Offline for calibrations for several hours each day. - 25-27 Nov: Data is missing. - 30 Nov: Power outage 3 Dec: SP2 hard-drive full. - 3 Dec: Power Outage Header: - BHBL_NumbConc[#/cc]: Refers to the number concentration of refractory black carbon (rBC) measured from combined broadband high-gain and low-gain channels, expressed in particles per cubic centimeter. - BHBL_BCMass_Conc[ug/m3]: Refers to the mass concentration of refractory black carbon (rBC) measured from combined broadband high-gain and low-gain channels, expressed in micrograms per cubic meter. - NoData_Flag[bool]: A boolean flag that indicates whether no data was recorded during a measurement. - NoBC_Flag[bool]: A boolean flag indicating whether no black carbon particles were recorded during the measurement. - Laser_Flag[bool]: A boolean flag indicating deviations in laser current during the measurement. - SampleFlow_Flag[bool]: A boolean flag indicating deviations from the set sample flow rate during the measurement. - PrimThresh_Flag[bool]: A boolean flag indicating deviations from the set primary threshold during the measurement, potentially ignoring real particles. - Manual_Flag[bool]: A boolean flag indicating manual intervention or adjustments during the measurement. - CVI_Flag[bool]: A boolean flag indicating whether the Counterflow Virtual Impactor (CVI) was active or inactive during the measurement.

54 ENVIRONMENTAL SCIENCES↗