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All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Suggestions on the Vapor Pressure Determination of Molten Salts

The knowledge of the thermophysical properties of coolant and fuel in molten salts nuclear reactors (MSRs), such as thermal stability and vapor pressure, are of remarkable interest, particularly for simulating safe reactor operations. Molten salt reactorsMSRs use molten salt mixtures as the primary coolant and/or fuel and are expected to operate up to 800 °C. With the revival of interest in deploying MSRs, complete thermophysical and thermochemical characterization of these materials is of interest to industry, regulators, and researchers. Vapor pressure data for molten salts are scarce in the literature, both for pure salts but especially for eutectic mixtures. This report describes the effusion method, which consist of measuring the rate of escape of vapor molecules through a small orifice for the determination of the vapor pressure of compounds and may be useful on compounds such as molten salts. Thermogravimetric analysis records the mass loss as a function of time and temperature. There are two equations that can be used to relate the mass loss rate with the vapor pressure: (1) the Knudsen equation and (2) the Langmuir equation. To apply these equations, the system needs to reach a pseudo (or near) equilibrium condition. Therefore, the experimental conditions must be such that allow the condensed and the vapor/gas phases to be in equilibrium. In order to accomplish equilibrium like conditions, the sample must be in an almost-sealed cell except for a small orifice, from where the vapor escapes. In the Knudsen method vacuum is applied to eliminate the effect that the presence of other gas molecules could have on the evaporation rate of the sample. However, Langmuir alleged that in certain conditions, such as at low temperatures and/or when the vapor pressure is low, the rate of evaporation of a substance is independent of the presence of vapor around it. For that reason, some researchers, when measuring the mass loss of a substance with a predictable low vapor pressure, do not apply vacuum when using the Langmuir equation. However, they use a standard substance to parameterize the experimental setup. The use of one equation or the other will depend on the characteristics of the sample and the availability of an appropriate standard. Some important aspects related to the nature of the samples and vapor pressure measurements are described for future consideration.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

SCALE 6.2.4 Validation: Reactor Physics

This report is the third volume in a report series documenting the validation of SCALE 6.2.4, which is used herein with ENDF/B-VII.1 libraries, for nuclear criticality safety, reactor physics, and radiation shielding applications. This report focuses on validating SCALE capabilities that affect reactor physics applications. The experimental data used as basis for validation consists of measurement data for nuclide inventory, decay heat, and full-core experiments and include the following: 1. radiochemical assay measurements of 40 nuclides of importance to burnup credit, decay heat, and radiation shielding in 169 light-water reactor (LWR) spent nuclear fuel samples that cover burnups up to 70 GWd/MTU and initial enrichments up to 4.9% 235 U; 2. full-assembly decay heat measurements for 236 LWR assemblies with: a. initial fuel enrichments up to 4% 235 U, b. assembly burnups of 5–51 GWd/MTU, and c. cooling times after discharge in the 2- to 27-year range (of importance to spent nuclear fuel storage, transportation, and disposal); and 3. pulse fission irradiations for fissionable materials at cooling times of interest to severe accident analyses (<10 5 s). Validation examples for full-core analysis are based on startup experiments for the Watts Bar Nuclear Unit 1 (WBN1) pressurized water reactor (PWR) and two high-temperature gas-cooled reactor (HTGR) benchmarks for the HTR-10 pebble bed and the prismatic HTTR reactor.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2022

Models to Incorporate Reaction Mechanisms into DG-OSPREY: Fixed-Bed Simulations for Organic Iodides Capture Using Ag 0 Z

As one of the most potent radioisotopes released during spent nuclear fuel reprocessing, 129 I is strictly regulated and must be removed before discharge. Organic iodides (primarily alkyl iodides with different chain lengths, i.e., CH 3 I, C 4 H 9 I, and C 12 H 25 I) comprise ~2% of the total iodine in the reprocessing off-gases and are primarily present in vessel off-gas (VOG). Reduced silver mordenite (Ag 0 Z) is predominantly considered for the removal of radioiodine; however, its capture performance and underlying interaction processes with long-chain organic iodides are not fully understood. Two major tasks were accomplished in this study. First, to improve upon the previous experimental studies where Ag 0 Z was used to capture CH 3 I, C 4 H 9 I, and C 12 H 25 I at different concentrations, we comprehensively investigated the corresponding capture mechanisms by characterizing fully loaded Ag 0 Z samples. Second, computational codes were implemented to perform fixed-bed simulations that account for transport and reaction mechanisms. Scanning electron microscopy with energy dispersive X-ray analysis (SEM-EDX), powder X-ray diffraction (PXRD), UV-visible diffuse reflectance spectroscopy (UV-vis DRS), and thermogravimetric analysis (TGA) were conducted on Ag 0 Z samples that are saturated with I 2 , CH 3 I, C 4 H 9 I, and C 12 H 25 I), respectively. Results indicate that AgI is the predominant adsorption product regardless of the adsorbed iodine species, yet alkyl iodides with different carbon chain lengths may have different compositions of α- and γ-AgI. Synchrotron pair distribution function (PDF) measurements and TGA coupled with a Fourier transformed infrared detector (TGA FTIR) have been performed, and experimental data are currently analyzed. Results are expected to provide further insights into the adsorption mechanisms. The fixed-bed capture performance for CH 3 I was successfully simulated by solving mathematical equations that describe the underlying transport processes and adsorption reactions. The computational framework, Catalytic After Treatment System (CATS), that was originated in our research group, was used to solve the governing equations. Kinetic parameters, including the pore diffusivity and reaction rate constant were obtained by optimization techniques using data from thin-bed experiments performed at Oak Ridge National Laboratory. The performance of a deep bed predicted using the optimized parameters showed promising agreement with the experimental data.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2018

Preferential flow systems amended with biogeochemical components: imaging of a two-dimensional study

The vadose zone is a highly interactive heterogeneous system through which water enters the subsurface system by infiltration. This paper details the effects of simulated plant exudate and soil component solutions upon unstable flow patterns in a porous medium (ASTM silica sand; US Silica, Ottawa, IL, USA) through the use of two-dimensional tank light transmission method (LTM). The contact angle (θ) and surface tension (γ) of two simulated plant exudate solutions (i.e., oxalate and citrate) and two soil component solutions (i.e., tannic acid and Suwannee River natural organic matter, SRNOM) were analyzed to determine the liquid–gas and liquid–solid interface characteristics of each. To determine if the unstable flow formations were dependent on the type and concentration of the simulated plant exudates and soil components, the analysis of the effects of the simulated plant exudate and soil component solutions were compared to a control solution (Hoagland nutrient solution with 0.01 M NaCl). Fingering flow patterns, vertical and horizontal water saturation profiles, water saturation at the fingertips, finger dimensions and velocity, and number of fingers were obtained using the light transmission method. Significant differences in the interface properties indicated a decrease between the control and the plant exudate and soil component solutions tested; specifically, the control (θ = 64.5° and γ = 75.75mNm -1 ) samples exhibited a higher contact angle and surface tension than the low concentration of citrate (θ = 52.6° and γ = 70.8mNm -1 ). Wetting front instability and fingering flow phenomena were reported in all infiltration experiments. The results showed that the plant exudates and soil components influenced the soil infiltration as differences in finger geometries, velocities, and water saturation profiles were detected when compared to the control. Among the tested solutions and concentrations of soil components, the largest finger width (10.19cm) was generated by the lowest tannic acid solution concentration (0.1mgL -1 ), and the lowest finger width (6.00cm) was induced by the highest SRNOM concentration (10mgL -1 ). Similarly, for the plant exudate solutions, the largest finger width (8.36cm) was generated by the lowest oxalate solution concentration (0.1mgL -1 ), and the lowest finger width (6.63cm) was induced by the lowest citrate concentration (0.1mgL -1 ). The control solution produced fingers with average width of 8.30cm. Additionally, the wettability of the medium for the citrate, oxalate, and SRNOM solutions increased with an increase in concentration. Our research demonstrates that the plant exudates and soil components which are biochemical compounds produced and released in soil are capable of influencing the process of infiltration in soils. The results of this research also indicate that soil wettability, expressed as cosθ 1/2 , should be included in the scaling of the finger dimension, i.e., finger width, when using the Miller and Miller (1956) scaling theory for the scaling of flow in porous media.

58 GEOSCIENCES↗
NASA NTRS2013

Materials Combustion Testing and Combustion Product Sensor Evaluations in FY12

NASA Centers continue to collaborate to characterize the chemical species and smoke particles generated by the combustion of current space-rated non-metallic materials including fluoropolymers. This paper describes the results of tests conducted February through September 2012 to identify optimal chemical markers both for augmenting particle-based fire detection methods and for monitoring the post-fire cleanup phase in human spacecraft. These studies follow up on testing conducted in August 2010 and reported at ICES 2011. The tests were conducted at the NASA White Sands Test Facility in a custom glove box designed for burning fractional gram quantities of materials under varying heating profiles. The 623 L chamber was heavily instrumented to quantify organics (gas chromatography/mass spectrometry), inorganics by water extraction followed by ion chromatography, and select species by various individual commercially-available sensors. Evaluating new technologies for measuring carbon monoxide, hydrogen cyanide, hydrogen fluoride, hydrogen chloride and other species of interest was a key objective of the test. Some of these sensors were located inside the glovebox near the fire source to avoid losses through the sampling lines; the rest were located just outside the glovebox. Instruments for smoke particle characterization included a Tapered Element Oscillating Microbalance Personal Dust Monitor (TEOM PDM) and a TSI Dust Trak DRX to measure particle mass concentration, a TSI PTrak for number concentration and a thermal precipitator for collection of particles for microscopic analysis. Materials studied included Nomex®, M22759 wire insulation, granulated circuit board, polyvinyl chloride (PVC), Polytetrafluoroethylene (PTFE), Kapton®, and mixtures of PTFE and Kapton®. Furnace temperatures ranged from 340o to 640o C, focusing on the smoldering regime. Of particular interest in these tests was confirming burn repeatability and production of acid gases with different fuel mixture compositions, as well as the dependence of aerosol concentrations on temperature.

Smoke↗
NASA NTRS2013

Materials Combustion Testing and Combustion Product Sensor Evaluations in FY12

NASA Centers continue to collaborate to characterize the chemical species and smoke particles generated by the combustion of current space-rated non-metallic materials including fluoropolymers. This paper describes the results of tests conducted February through September 2012 to identify optimal chemical markers both for augmenting particle-based fire detection methods and for monitoring the post-fire cleanup phase in human spacecraft. These studies follow up on testing conducted in August 2010 and reported at ICES 2011. The tests were conducted at the NASA White Sands Test Facility in a custom glove box designed for burning fractional gram quantities of materials under varying heating profiles. The 623 L chamber was heavily instrumented to quantify organics (gas chromatography/mass spectrometry), inorganics by water extraction followed by ion chromatography, and select species by various individual commercially-available sensors. Evaluating new technologies for measuring carbon monoxide, hydrogen cyanide, hydrogen fluoride, hydrogen chloride and other species of interest was a key objective of the test. Some of these sensors were located inside the glovebox near the fire source to avoid losses through the sampling lines; the rest were located just outside the glovebox. Instruments for smoke particle characterization included a Tapered Element Oscillating Microbalance Personal Dust Monitor (TEOM PDM) and a TSI Dust Trak DRX to measure particle mass concentration, a TSI PTrak for number concentration and a thermal precipitator for collection of particles for microscopic analysis. Materials studied included Nomex(R), M22759 wire insulation, granulated circuit board, polyvinyl chloride (PVC), Polytetrafluoroethylene (PTFE), Kapton(R), and mixtures of PTFE and Kapton(R). Furnace temperatures ranged from 340 to 640 C, focusing on the smoldering regime. Of particular interest in these tests was confirming burn repeatability and production of acid gases with different fuel mixture compositions, as well as the dependence of aerosol concentrations on temperature.

Combustion↗
NASA NTRS2017

Thermochemistry of CaO-MgO-Al2O3-SiO2 (CMAS) and Advanced Thermal and Environmental Barrier Coating Systems

CaO-MgO-Al2O3-SiO2 (CMAS) oxides are constituents in a broad number of materials and minerals which have recently inferred to discussions in materials science, planetary science, geochemistry and cosmochemistry communities. In materials science, there is increasing interest in the degradation studies of thermal (TBC) and environmental (EBC) barrier coatings of gas turbines by molten CMAS. CMAS minerals usually are carried by the intake air into gas turbines, e.g. in aircraft engines, and their deposits react at high temperatures (1000C) with the coating materials. This causes degradation and accelerated failure of the static and rotating components of the turbine engines. We discuss some preliminary results of the reactions between CMAS and Rare-Earth (RE Y, Yb, Dy, Gd, Nd and Sm) oxide stabilized ZrO2 or HfO2 systems, and the stability of the resulting oxides and silicates. Plasma sprayed hollow tube samples ( 2.2 mm and 26 mm height) were half filled with CMAS powder, wrapped and sealed with platinum foil, and heat treated at 1310 C for 5h. Samples were characterized by differential scanning calorimetry, X-ray diffraction and cross section electron microscopy analysis.

degradation↗
DOE OSTI2016

5 kHz thermometry in a swirl-stabilized gas turbine model combustor using chirped probe pulse femtosecond CARS. Part 2. Analysis of swirl flame dynamics

We have performed a detailed analysis of the temperature field in a turbulent swirl flame operating with a self-excited thermo-acoustic instability. The temperature field was measured using 5 kHz chirped-probe-pulse (CPP) femtosecond (fs) coherent anti-Stokes Raman scattering (CARS). The measurements are described in detail in the part 1 companion article. In this paper, part 2, a detailed analysis of the time-resolved temperature measurements and simultaneous pressure measurements is performed to provide insight into the dynamics and structure of the swirl-stabilized flame. Here this work is the first to capture the dynamics of the flame, flow, and coupled flow-flame processes using high-fidelity, spatially- and temporally-resolved thermometry in a flame of practical relevance. The time-averaged contour plot of the temperature field indicates that the flame is very flat and stabilizes approximately 10 mm downstream of the burner face. In this region, there are very significant temperature fluctuations indicating a very high level of unsteadiness. The temperature probability distribution functions (PDFs) are clearly bimodal in this region near the injector face. A Fourier analysis of the temperature time series revealed multiple coherent oscillatory modes. The strongest oscillation was found to be coherent and in-phase with an acoustic resonance at 314 Hz, as expected from the Rayleigh criteria for the unstable flame. An analysis of the phase-conditioned average temperature fields clearly shows an axial pumping of low-temperature reactants, which are consumed after a convective delay and result in a spike in the global heat-release rate. Continued analysis also revealed a 438 Hz oscillation that was found to correspond with the dynamics of convective transport by a helical precessing vortex core (PVC). The structure of the PVC, and its interaction with the flame, were studied based on the presence of this characteristic frequency in the power spectral densities computed throughout the flow. The precision and time-resolution of the CPP fsCARS measurements was also sufficient to enable computation of the integral time-scales as well as the PDFs of the temporal temperature gradients. A sample of state space trajectories were used to provide insight into the nature of coupling between the narrowband acoustic resonance and the broadband spectrum of turbulent flame processes.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2016

Experimental Studies and Model Analysis of Noble Gas Fractionation in Porous Media

Core Ideas Ambient noble gases in porous media fractionate from through‐flow of other gases. CO 2 fluxes and noble‐gas fractionation are measured in simple sandbox experiments. Modeled fractionation provides indirect proxy, e.g., of steady CO 2 leakage fluxes. The noble gases, which are chemically inert under normal terrestrial conditions but vary systematically across a wide range of atomic mass and diffusivity, offer a multicomponent approach to investigating gas dynamics in unsaturated soil horizons, including transfer of gas between saturated zones, unsaturated zones, and the atmosphere. To evaluate the degree to which fractionation of noble gases in the presence of an advective–diffusive flux agrees with existing theory, a simple laboratory sand column experiment was conducted. Pure CO 2 was injected at the base of the column, providing a series of constant CO 2 fluxes through the column. At five fixed sampling depths within the system, samples were collected for CO 2 and noble gas analyses, and ambient pressures were measured. Both the advection–diffusion and dusty gas models were used to simulate the behavior of CO 2 and noble gases under the experimental conditions, and the simulations were compared with the measured depth‐dependent concentration profiles of the gases. Given the relatively high permeability of the sand column (5 × 10 −11 m 2 ), Knudsen diffusion terms were small, and both the dusty gas model and the advection–diffusion model accurately predicted the concentration profiles of the CO 2 and atmospheric noble gases across a range of CO 2 flux from ∼700 to 10,000 g m −2 d −1 . The agreement between predicted and measured gas concentrations demonstrated that, when applied to natural systems, the multi‐component capability provided by the noble gases can be exploited to constrain component and total gas fluxes of non‐conserved (CO 2 ) and conserved (noble gas) species or attributes of the soil column relevant to gas transport, such as porosity, tortuosity, and gas saturation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2019

Advanced FIB-based Preparation of Cryogenically-prepared Specimens for APT Analysis

The utilization of the focused ion beam scanning electron microscope (FIB-SEM) has aided the application of Atom Probe Tomography (APT) to a continually-growing variety of materials, including soft biological materials. However, the regular application of APT to hydrated interfaces such as those found in biological and environmental materials is lacking in large part due to difficulties in specimen preparation under high and ultra-high vacuum conditions. Although a FIB-SEM based cryogenic specimen preparation approach offers a rational route to the preparation of such specimens for APT analysis, many practical aspects such as welding and limitations in the cryo stage manipulation makes it challenging for routine liftout of site-targeted specimens. In this work, we describe our recent efforts in the development of a site-specific liftout and attachment scheme for cryogenically cooled specimens involving a combination of redeposition and overcoating of organic and organometallic molecules, as shown in Fig. 1a-d for a cryogenically-frozen corroded glass sample containing a hydrated porous gel surface layer. Application of an annular milling pattern to the frozen specimens leads to a needle-shaped morphology necessary for APT analysis with the targeted water-ice filled porous corroded silicate glass region of interest near the apex. Using a custom shuttle device and environmental transfer hub at PNNL to facilitate environmentally-protected specimen transfer, APT analysis was applied to directly map, for the first time, a water/solid interface in 3D to reveal the complex nanoscale water-filled porous network of corroded glass. Application of this unique specimen preparation approach to biological specimens will also be discussed, as well as the application of a unique cryo nanomaniupulator with integrated gas injection system to enable controlled FIB-based welding under cryogenic temperatures.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2024

Electricity and natural gas tariffs at United States wastewater treatment plants

Abstract Wastewater treatment plants (WWTPs) are large electricity and natural gas consumers with untapped potential to recover carbon-neutral biogas and provide energy services for the grid. Techno-economic analysis of emerging energy recovery and management technologies is critical to understanding their commercial viability, but quantifying their energy cost savings potential is stymied by a lack of well curated, nationally representative electricity and natural gas tariff data. We present a dataset of electricity tariffs for the 100 largest WWTPs in the Clean Watershed Needs Survey (CWNS) and natural gas tariffs for the 54 of 100 WWTPs with on-site cogeneration. We manually collected tariffs from each utility’s website and implemented data checks to ensure their validity. The dataset includes facility metadata, electricity tariffs, and natural gas tariffs (where cogeneration is present). Tariffs are current as of November 2021. We provide code for technical validation along with a sample simulation.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2016

Multi-Column Xe/Kr Separation with AgZ-PAN and HZ-PAN

Previous multi-column xenon/krypton separation tests have demonstrated the capability of separating xenon from krypton in a mixed gas feed stream. The results of this initial testing with AgZ-PAN and HZ-PAN indicated that an excellent separation of xenon from krypton could be achieved. Building upon these initial results, a series of additional multi-column testing were performed in FY-16. The purpose of this testing was to scale up the sorbent beds, test a different composition of feed gas and attempt to improve the accuracy of the analysis of the individual capture columns’ compositions. Two Stirling coolers were installed in series to perform this testing. The use of the coolers instead of the cryostat provided two desired improvements, 1) removal of the large dilution due to the internal volume of the cryostat adsorption chamber, and 2) ability to increase the sorbent bed size for scale-up. The AgZ-PAN sorbent, due to its xenon selectivity, was loaded in the first column to capture the xenon while allowing the krypton to flow through and be routed to a second column containing the HZ-PAN for capture and analysis. The gases captured on both columns were sampled with evacuated sample bombs and subsequently analyzed via GC-MS for both krypton and xenon. The results of these tests can be used to develop the scope of future testing and analysis using this test bed for demonstrating the capture and separation of xenon and krypton using sorbents, for demonstrating desorption and regeneration of the sorbents, and for determining compositions of the desorbed gases. They indicate a need for future desorption studies in order to better quantify co-adsorbed species and final krypton purity.

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

End-Use Savings Shapes Measure Documentation: Console Water-to-Air Geothermal Heat Pump

Executive Summary Building on the successfully completed effort to calibrate and validate the U.S. Department of Energy’s ResStock™ and ComStock™ models over the past several years, the objective of this work is to produce national datasets that empower analysts working for federal, state, utility, city, and manufacturer stakeholders to answer a broad range of analysis questions. The goal of this work is to develop energy efficiency, electrification, and demand flexibility end-use load shapes (electricity, gas, propane, or fuel oil) that cover most of the high-impact, market-ready (or nearly market-ready) measures. An end-use savings shape is the difference in energy consumption between a baseline building and a building with an energy efficiency, electrification, or demand flexibility measure applied. It results in a time series profile that is broken down by end use and fuel (electricity or on-site gas, propane, or fuel oil use) at each time step. ComStock is a highly granular, bottom-up model that uses multiple data sources, statistical sampling methods, and advanced building energy simulations to estimate the annual sub-hourly energy consumption of the commercial building stock across the United States. The baseline model intends to represent the U.S. commercial building stock as it existed in 2018. This measure models the conversion of an existing heating, ventilating, and air-conditioning (HVAC) system to a series of “console” water-to-air heat pumps served by a ground heat exchanger. Console water-to-air geothermal heat pumps (GHP) are all-in-one packages that have no or minimal ductwork and serve individual spaces. Properly designed ground heat exchanger-coupled systems can offer benefits in energy efficiency relative to “conventional” HVAC systems, as well as facilitating beneficial electrification. Console GHPs can be coupled to a ground loop on the source side and can directly replace electric baseboard heaters or air-source packaged terminal heat pumps. Console GHPs can also bring in outdoor air for ventilation. This measure will be referred to throughout the document as the “Console GHP” upgrade.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
NASA NTRS1973

Radiative coupled viscous flow with massive blowing

An analysis of the fully-coupled viscous, radiating flow past an ablating blunt body at hyperbolic entry conditions is presented. A detailed thermodynamics computation, as well as a realistic radiation transport model, is included. A locally nonsimilar approach is employed to solve the conservation equations away from the stagnation point. The validity of the locally nonsimilar approach is demonstrated for some nonablating cases. Sample calculations are made for the typical flight condition of a Jovian entry probe. The effects of the downstream injection of the ablation products of a carbon heat shield on the flux distribution around the body are discussed in detail. It is found that most of the radiative energy is absorbed by the injected carbon gas and dumped into the wake.

Chou, Y. S.↗
NASA NTRS2012

Thermal and Evolved Gas Analysis of "Nanophase" Carbonates: Implications for Thermal and Evolved Gas Analysis on Mars Missions

Data collected by the Mars Phoenix Lander's Thermal and Evolved Gas Analyzer (TEGA) suggested the presence of calcium-rich carbonates as indicated by a high temperature CO2 release while a low temperature (approx.400-680 C) CO2 release suggested possible Mg- and/or Fe-carbonates [1,2]. Interpretations of the data collected by Mars remote instruments is done by comparing the mission data to a database on the thermal properties of well-characterized Martian analog materials collected under reduced and Earth ambient pressures [3,4]. We are proposing that "nano-phase" carbonates may also be contributing to the low temperature CO2 release. The objectives of this paper is to (1) characterize the thermal and evolved gas proper-ties of carbonates of varying particle size, (2) evaluate the CO2 releases from CO2 treated CaO samples and (3) examine the secondary CO2 release from reheated calcite of varying particle size.

Lauer, Howard V., Jr.↗
DOE OSTI2015

SUPERMASSIVE BLACK HOLES WITH HIGH ACCRETION RATES IN ACTIVE GALACTIC NUCLEI. III. DETECTION OF Fe ii REVERBERATION IN NINE NARROW-LINE SEYFERT 1 GALAXIES

This is the third in a series of papers reporting on a large reverberation-mapping campaign aimed to study the properties of active galactic nuclei (AGNs) with high accretion rates. We present new results on the variability of the optical Fe ii emission lines in 10 AGNs observed by the Yunnan Observatory 2.4 m telescope from 2012 to 2013. We detect statistically significant time lags, relative to the AGN continuum, in nine of the sources. This accurate measurement is achieved using a sophisticated spectral fitting scheme that allows for apparent flux variations of the host galaxy, and several narrow lines, due to the changing observing conditions. Six of the newly detected lags are indistinguishable from the Hβ lags measured in the same sources. Two are significantly longer and one is slightly shorter. Combining these findings with the Fe ii lags reported in previous studies, we find an Fe ii radius–luminosity relationship similar to the one for Hβ, although our sample by itself shows no clear correlation. The results support the idea that Fe ii emission lines originate in photoionized gas, which, for the majority of the newly reported objects, is indistinguishable from the Hβ-emitting gas. We also present a tentative correlation between the lag and intensity of Fe ii and Hβ and comment on its possible origin.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Radiocarbon analysis as a method for verifying atmospheric CO 2 uptake during carbon mineralization

Sequestration of atmospheric CO 2 is required to constrain the warming of Earth’s climate. Carbon mineralization refers to the precipitation of carbonate minerals by reaction of CO 2 and Mg- and Ca-rich rocks; if the source of the CO 2 is atmospheric and the precipitated carbonate is protected from subsequent dissolution, this process at sufficient scale may be able to reliably draw down atmospheric greenhouse gas levels. Such reactions occur passively in ultramafic settings and previous work has demonstrated that they actively draw down local CO 2 (g) concentrations. However, a method for unambiguously attributing the sequestered carbon solid product to atmospheric sources is still lacking. Here, we test if radiocarbon can be used to verify that the carbon being incorporated into carbonate minerals during carbon mineralization is atmospheric in origin. Additionally, samples from recently exposed ultramafic sites are analyzed and the results demonstrate the utility of this technique for verifying true atmospheric carbon reduction.

58 GEOSCIENCES↗
DOE OSTI2025

Operando XPS in reactive plasmas: The importance of the wall reactions

In this article, advancements in differential pumping and electron optics over the past few decades have enabled x-ray photoelectron spectroscopy (XPS) measurements at (near-)ambient pressures, bridging the pressure gap for characterizing realistic sample chemistries. Recently, we have demonstrated the capabilities of an ambient pressure XPS setup for in situ plasma environment measurements, allowing plasma-surface interactions to be studied in operando rather than using the traditional before-and-after analysis approach. This new “plasma-XPS” technique facilitates the identification of reaction intermediates critical for understanding plasma-assisted surface processes relevant to semiconductor nanomanufacturing, such as physical vapor deposition, etching, atomic layer deposition, and many other plasma applications. In this paper, we apply the plasma-XPS approach to monitor real-time surface chemical changes on a model Ag(111) single crystal exposed to oxidizing and reducing plasmas. We correlate surface-sensitive data with concurrent gas-phase XPS measurements and residual gas mass-spectrum analysis of species generated during plasma exposure, highlighting the significant role of plasma-induced chamber wall reactions. Ultimately, we demonstrate that plasma-XPS provides comprehensive insights into both surface and gas-phase chemistry, establishing it as a versatile and dynamic characterization tool with broad applications in microelectronics research. Finally, we outline potential enhancements and future metrology directions to advance plasma-XPS investigations further.

36 MATERIALS SCIENCE↗