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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 271 records · Page 15
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

A Bayesian approach to time-domain photonic Doppler velocimetry analysis

Photonic Doppler velocimetry (PDV) is an established technique for measuring the velocities of fast-moving surfaces in high-energy-density experiments. In the standard approach to PDV analysis, the short-time Fourier transform (STFT) is used to generate a spectrogram from which the velocity history of the target is inferred. The user chooses the form, duration, and separation of the window function. Here, in this study, we present a Bayesian approach to infer the velocity directly from the PDV oscilloscope trace, without using the spectrogram for analysis. This is clearly a difficult inference problem due to the highly periodic nature of the data, but we find that with carefully chosen prior distributions for the model parameters, we can accurately recover the injected velocity from synthetic data. We validate this method using PDV data collected at the STAR two-stage light gas gun at Sandia National Laboratories, recovering shock-front velocities in quartz that are consistent with those inferred using the STFT-based approach and are interpolated across regions of low signal-to-noise data. Although this method does not rely on the same user choices as the STFT, we caution that it can be prone to misspecification if the chosen model is not sufficient to capture the velocity behavior. Analysis using posterior predictive checks can be used to establish whether a better model is required, although more complex models come with additional computational cost, often taking more than several hours to converge when sampling the Bayesian posterior. We, therefore, recommend it be viewed as a complementary method to that of the STFT-based approach.

Allison, James R. [First Light Fusion Ltd., Yarnto↗
DOE OSTI2024

Broad absorption line quasars in the Dark Energy Spectroscopic Instrument Early Data Release

Broad absorption line (BAL) quasars are characterized by gas clouds that absorb flux at the wavelength of common quasar spectral features, although blueshifted by velocities that can exceed $0.1c$. BAL features are interesting as signatures of significant feedback, yet they can also compromise cosmological studies with quasars by distorting the shape of the most prominent quasar emission lines, impacting redshift accuracy and measurements of the matter density distribution traced by the Lyman $\alpha$ forest. We present a catalogue of BAL quasars discovered in the Dark Energy Spectroscopic Instrument (DESI) survey Early Data Release, which were observed as part of DESI Survey Validation, as well as the first two months of the main survey. We describe our method to automatically identify BAL quasars in DESI data, the quantities we measure for each BAL, and investigate the completeness and purity of this method with mock DESI observations. We mask the wavelengths of the BAL features and re-evaluate each BAL quasar redshift, finding new redshifts which are $243\, {\rm km}\, {\rm s}^{-1}$ smaller on average for the BAL quasar sample. These new, more accurate redshifts are important to obtain the best measurements of quasar clustering, especially at small scales. Finally, we present some spectra of rarer classes of BALs that illustrate the potential of DESI data to identify such populations for further study.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Promise of nonthermal plasmas in addressing emerging environmental and health problems: Present and future

Nonthermal atmospheric pressure plasmas transform input electrical energy efficiently into reactive species, charged particles, and photons. This “activated gas” is being investigated as solutions for a range of environmental and health problems facing society today. In this Perspective, we take a cursory look at a few of these societal problems and the reflected role that plasmas may play in charting the pathway to a solution buoyed by supporting research. Here, we survey the plasma-based opportunities in the removal of trace contaminants in water supporting methodologies such as water reuse, which addresses scarcity and pollution, the opportunity posed by plasmas-based chemical depolymerization for plastics recycling, and the application of plasmas for food security, which includes sterilization of foodstuffs and the improvement of crop yield. Finally, we also included a short review on how plasmas may help control disease spread. In each case, the scope of the problem is presented along with the potential plasma-based solution.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

The history of metal enrichment traced by X-ray observations of high-redshift galaxy clusters

ABSTRACT We present the analysis of deep X-ray observations of 10 massive galaxy clusters at redshifts 1.05 < z < 1.71, with the primary goal of measuring the metallicity of the intracluster medium (ICM) at intermediate radii, to better constrain models of the metal enrichment of the intergalactic medium. The targets were selected from X-ray and Sunyaev–Zel’dovich effect surveys, and observed with both the XMM–Newton and Chandra satellites. For each cluster, a precise gas mass profile was extracted, from which the value of r500 could be estimated. This allows us to define consistent radial ranges over which the metallicity measurements can be compared. In general, the data are of sufficient quality to extract meaningful metallicity measurements in two radial bins, r < 0.3r500 and 0.3 < r/r500 < 1.0. For the outer bin, the combined measurement for all 10 clusters, Z/Z⊙ = 0.21 ± 0.09, represents a substantial improvement in precision over previous results. This measurement is consistent with, but slightly lower than, the average metallicity of 0.315 solar measured at intermediate-to-large radii in low-redshift clusters. Combining our new high-redshift data with the previous low-redshift results allows us to place the tightest constraints to date on models of the evolution of cluster metallicity at intermediate radii. Adopting a power-law model of the form Z ∝ (1 + z)γ, we measure a slope $\gamma = -0.5^{+0.4}_{-0.3}$, consistent with the majority of the enrichment of the ICM having occurred at very early times and before massive clusters formed, but leaving open the possibility that some additional enrichment in these regions may have occurred since a redshift of 2.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2025

Techno-economic design of a linear Fresnel reflector for industrial process heat

A techno-economic model of a Concentrating Solar Thermal (CST) system using a Linear Fresnel Reflector (LFR) has been developed. LFRs can deliver process heat suitable for a range of industries, including food and beverage production. This model uses an adaptive algorithm to calculate the optimal secondary reflector shape given the geometry and optical properties of the rest of the system. A ray-tracing program is used to calculate optical efficiency over a wide range of longitudinal and transversal incidence angles and subsequently evaluate the annual efficiency at a given geographical location. A specific LFR design developed by Hyperlight Energy was modelled, and this industrial partner provided a detailed cost breakdown which was used as the basis of an economic model. Combining the technical and economic data facilitates the calculation of the Levelized Cost of Heat (LCOH). The influence of a number of parameters on the annual efficiency and LCOH is explored; notable parameters include the absorber height, the number, width, and spacing of the primary mirrors, the aim point, and the secondary reflector shape and width. By identifying an optimal combination of these parameters, we reduce the LCOH of the industry partner’s system design by 9.2%, from 14.4 $\$/MWh_{th}$ to 13.0 $\$/MWh_{th}$. In comparison, the LCOH of a natural gas boiler delivering the same annual quantity of heat is 29 $\$/MWh_{th}$, which indicates that LFRs can be a competitive heat source for industrial processes.

14 SOLAR ENERGY↗
DOE OSTI2020

Viscosity of glass-forming melt at the bottom of high-level waste melter feed cold caps: Effects of temperature and incorporation of solid components

At the final stages of conversion of melter feed (glass batch) to molten glass, the transient glass-forming melt becomes a continuous liquid phase encapsulating dissolving solid particles and gas bubbles that produce primary foam at the bottom of the cold cap (the reacting melter feed in an electric glass melting furnace). The glass-forming melt viscosity plays a dominant role in primary foam formation, stability, and eventual collapse, thus affecting the rate of melting (the glass production rate per cold cap area). For several melter feeds designed for nuclear waste vitrification, we have traced the glass-forming melt viscosity during the final stages of feed-to-glass conversion as it changes in response to changing temperature and composition (resulting from dissolving solid particles). Starting with a relatively low values at the moment when the melt connects, melt viscosity reaches maximum within the primary foam layer and then decreases to its final melter-operating temperature value. We paid a particular attention to the cold-cap bottom—the boundary between the primary foam layer and the thermal boundary layer—where the melt viscosity affects the rate of melting predominantly through its effect on the temperature at which primary foam is collapsing.

Lee, Seung Min↗
DOE OSTI2022

Thermite and intermetallic projectiles examined experimentally in air and inert gas environments

Intermetallic (aluminum and zirconium) and thermite (aluminum and molybdenum trioxide) projectiles were launched using a high velocity impact ignition testing system. The experiments were designed to simulate reactivity in high (argon) and low (air) altitude environments. The projectiles were launched into a chamber that included a steel target plate for projectile penetration before impacting a rear witness plate. The chamber was semi-sealed and instrumented for quasi-static pressure data. The results provide an understanding of energy release from the projectile materials and of the environmental influence on performance. The transient pressure traces provide insight into reaction kinetics. A bifurcation in transient pressure rise was an indication of a shift in reaction kinetics from the inherent reactive material to metal oxidation with the environment. The bifurcation was delayed by about 0.15 ms for the intermetallic relative to the thermite, evidence that the thermite reaction proceeded faster upon impact than the intermetallic. The two-step process (impact ignition of the reactive material followed by metal oxidation) was shown to produce higher energy conversion efficiencies than projectiles composed of pure fuel (i.e., aluminum) reported previously. Both reactive materials showed energy conversion efficiencies greater than 30% (for air) and 50% (for argon), and an explanation of underestimated efficiency and energy losses is provided. These results have implications for advancing formulations for ballistic applications. Structural reactive materials can be used to modify the effective reactivity of metal-containing formulations in varied atmospheric environments.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Tracing the transient reaction kinetics of adsorbed species by in situ/operando infrared spectroscopy

The dynamic reaction behavior (i.e., transient responses) of IR-observable adsorbed species and gaseous products obtained from transient kinetic studies provide valuable kinetic and mechanistic information, namely: the abundance of active intermediates and their reactivity distribution, the chemical structure of IR-observable active and spectator species, the sequence of their formation, and the kinetically significant and rate-determining step under reaction conditions of practical catalysis. We discuss the use of transient response data to elucidate the reaction mechanisms of several gas-solid reactions: CO/H 2 , CO/H 2 /C 2 H 4 , photocatalytic oxidation of ethanol, and the CO 2 -amine reaction. The IR coupled with transient kinetic techniques is especially useful for investigating the mechanisms of photocatalytic reactions because both photogenerated electrons and many adsorbed species are IR-active (exhibiting measurable IR bands), and their evolution occurs on a time scale of seconds at ambient temperature. We highlight the key features and limitations of in situ IR with transient kinetics, as well as their significance in catalyst design.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Experimental determinations of carbon and hydrogen isotope fractionations and methane clumped isotope compositions associated with ethane pyrolysis from 550 to 600°C

Methane clumped isotope compositions signify the relative natural abundances of rare, doubly substituted isotopic species of methane ( 13 CH 3 D and 12 CH 2 D 2 ) and have emerged as a new isotopic tool to trace the sources, sinks, and lifecycles of methane in the environment. Such measurements can identify equilibration (or reequilibration) temperatures if found to be in isotopic equilibrium or non-equilibrium processes (e.g., kinetically controlled reactions or mixing) if not in isotopic equilibrium. Naturally occurring thermogenic methane—formed by the thermally activated breakdown of larger organic molecules—has been found to have clumped isotope compositions consistent with equilibrium at reasonable gas formation temperatures in some settings and non-equilibrium processes occurring during either formation, migration, storage, or extraction in others. To explore the potential controls on the isotopic composition of thermogenic methane, we conducted isothermal time-series ethane pyrolysis experiments at 550 and 600 °C to measure methane and ethane 13 C/ 12 C and D/H fractionations and methane clumped isotope compositions (resolved 13 CH 3 D and 12 CH 2 D 2 ). We explore the effects of modifying the initial clumped isotope composition of ethane and the addition of water vapor to pyrolysis experiments. We observe that ethane and methane 13 C/ 12 C are controlled by kinetic isotope effects and Rayleigh distillation processes. In contrast, ethane and methane D/H and methane clumped isotope compositions appear to be controlled by a combination of these processes and hydrogen isotope exchange. The hydrogen isotope exchange processes lead to isotopic equilibrium as reaction completion is approached for both D/H (ethane/methane) and methane clumped isotope compositions. Here, we develop a chemical model based on a mass balance approach that accounts for inheritance vs. hydrogen-abstraction formation pathways for singly and doubly substituted isotopologues of ethane and methane that is compared to the experimental data. The model allows the determination of carbon and hydrogen kinetic isotope effects associated with ethane cracking and hydrogen abstraction reactions that, where applicable, we compare to prior theoretical constraints. From the comparison of the model to the experimental data, we infer that the kinetically controlled ethane and methane bulk isotope compositions and methane clumped isotope compositions are controlled by kinetic isotope effects (both primary and secondary) associated with both C–C bond and C–H bond cleavage reactions. Specifically, the methane clumped isotope compositions likely result from a combination of clumped isotope effects associated with ethane breakdown and/or assembly of methane isotopologues (expressed in terms of γ-factor parameters ≠ 1) and combinatorial effects that arise probabilistically. We discuss our experimental results in the context of recent pyrolysis experiments and observations of naturally occurring thermogenic methane. We consider a proposal consistent with observations from nature that the hydrogen isotope exchange reactions that promote equilibration of methane isotopic molecules at or near formation temperature may be facilitated by free radicals generated by pyrolysis reactions. In this framework, isotope exchange effectively ceases when pyrolysis effectively ceases locking in compositions that can be consistent with peak formation temperatures.

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

System code evaluation of near-term accident tolerant claddings during pressurized water reactor station blackout accidents

Following the Fukushima Daiichi nuclear accident in 2011, researches on Accident-tolerant fuels (ATFs) are currently of high interest in not only the nuclear industry but also governmental and international organizations. In this work, a quantitative evaluation of the performance of monolithic FeCrAl cladding and Cr-coated Zircaloy cladding has been performed for Pressurized Water Reactor (PWR) Station Blackout (SBO) accidents. A generic PWR model has been built in system thermal-hydraulics code TRACE based on the Surry Nuclear Power Station with counter-current natural circulation modelling capability for hotleg and steam generator U-tube components during the accidents. The base model results are then compared to MELCOR and RELAP simulations to verify the system component implementation in TRACE. Two PWR SBO scenarios were investigated, including: short-term SBO and long-term SBO with early reactor coolant pump (RCP) seal failure. These scenarios are defined to be very similar to the accidents studied in the State-of-the-Art Reactor Consequence Analysis (SOARCA) project. TRACE code is modified to reflect the oxidation kinetics of FeCrAl and Cr-coating. Larson-Miller creep rupture model is also implemented in TARCE using its built-in control systems to simulate the creep rupture of hotlegs. Additionally, the comparison between the TRACE models with and without the counter-current flow modeling resulted in significant difference when comparing ATF cladding to Zircaloy for short term SBO, while it marginal impacted the performance during long term SBO with RCP seal failure. For short term SBO, both ATF cladding underwent hot leg creep rupture ~20 min after Zircaloy cladding. While Zircaloy and Cr-coated cladding had generated significant amount of hydrogen gas (>10 kg) before the creep rupture event, FeCrAl cladding had only generated <0.5 kg of hydrogen gas. For long term SBO with RCP seal failure, significant hydrogen generation and fuel melting was predicted before hot leg creep rupture for the ATF cladding while providing only 10–20 min additional coping time compared to Zircaloy.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

A new aerial approach for quantifying and attributing methane emissions: implementation and validation

Methane (CH 4 ) is a powerful greenhouse gas that is produced by a diverse set of natural and anthropogenic emission sources. Biogenic methane sources generally involve anaerobic decay processes such as those occurring in wetlands, melting permafrost, or the digestion of organic matter in the guts of ruminant animals. Thermogenic CH 4 sources originate from the breakdown of organic material at high temperatures and pressure within the Earth's crust, a process which also produces more complex trace hydrocarbons such as ethane (C 2 H 6 ). Here, we present the development and deployment of an uncrewed aerial system (UAS) that employs a fast (1 Hz) and sensitive (1–0.5 ppb s -1 ) CH 4 and C 2 H 6 sensor and ultrasonic anemometer. The UAS platform is a vertical-takeoff, hexarotor drone (DJI Matrice 600 Pro, M600P) capable of vertical profiling to 120 m altitude and plume sampling across scales up to 1 km. Simultaneous measurements of CH 4 and C 2 H 6 concentrations, vector winds, and positional data allow for source classification (biogenic versus thermogenic), differentiation, and emission rates without the need for modeling or a priori assumptions about winds, vertical mixing, or other environmental conditions. The system has been used for direct quantification of methane point sources, such as orphan wells, and distributed emitters, such as landfills and wastewater treatment facilities. With detectable source rates as low as 0.04 and up to ~1500 kg h -1 , this UAS offers a direct and repeatable method of horizontal and vertical profiling of emission plumes at scales that are complementary to regional aerial surveys and localized ground-based monitoring.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Vapor detection and vapor pressure measurements of fentanyl and fentanyl hydrochloride salt at ambient temperatures

There is a need for non-contact, real-time vapor detection of drugs to combat illicit transportation and help curb the opioid epidemic. The low-volatility of drugs, like fentanyl, makes room temperature vapor detection of illicit drugs challenging, but feasible by atmospheric flow tube-mass spectrometry (AFT-MS). AFT-MS is a non-contact vapor detection approach capable of ultra-trace detection of drugs, including fentanyl and its analogs at low parts-per-quadrillion (ppqv) levels. The determination of vapor pressure values of fentanyl is necessary to understand potential vapor concentrations that may be available for detection. In this paper, vapor pressures of fentanyl free base and fentanyl hydrochloride salt (a common form of the illicit drug) were measured as a function of temperature at or near ambient conditions using the transpiration (gas saturation) method and AFT-MS. Based on our measurements, the vapor pressure of fentanyl at 25 °C is 9.0 × 10-14 atm (90 ppqv), and the vapor pressure of fentanyl hydrochloride at 25 °C is 1.8 x 10-17 atm (0.018 ppqv). We also demonstrate non-contact, real-time vapor detection of fentanyl. Preconcentration of vapors can further extend the detection capabilities. The collection, desorption, and detection of fentanyl vapors at ambient conditions was demonstrated for sampling times of seconds to an hour resulting in increased signal. AFT-MS is a viable detection method of fentanyl and other drugs for screening of packages and cargo.

atmospheric flow tube-mass spectrometry (AFT-MS), ↗
DOE OSTI2021

NACHOS, a CubeSat-based high-resolution UV-Visible hyperspectral imager for remote sensing of trace gases: system overview and science objectives

Here, the Nano-satellite Atmospheric Chemistry Hyperspectral Observation System (NACHOS) is a high-throughput (f/2.9), high spectral resolution (~1.3 nm optical resolution, 0.6 nm sampling) Offner-design hyperspectral imager operating in the 300-500 nm spectral region. The 1.5U instrument payload (1U optical system, 0.5U electronics module) is hosted by a 1.5U LANL-designed CubeSat bus to comprise a 3U complete satellite. Spectroscopically similar to NASA’s Ozone Monitoring Instrument (OMI), which provides wide-field global mapping of ozone and other gases at coarse spatial resolution, NACHOS fills the complementary niche of targeted measurements at much higher spatial resolution. With 350 across-track spatial pixels and a 15-degree across-track field of view, NACHOS will provide spectral imaging at roughly 0.4 km per pixel from 500 km altitude. NACHOS incorporates highly streamlined gas-retrieval algorithms for rapid onboard processing, alleviating the need to routinely downlink massive hyperspectral data cubes. We will discuss the instrument design, challenges in achieving mechanical robustness to launch vibration in such a compact instrument, the onboard calibration system, and gas-retrieval data downlink strategy. We will also discuss potential science missions, including monitoring of NO 2 as an easily detected proxy for anthropogenic fossil-fuel greenhouse gases, monitoring lowlevel SO 2 degassing at pre-eruptive volcanoes, H 2 CO from wildfires, and characterization of aerosols. The long-term vision is for a many-satellite constellation that could provide both high spatial resolution and frequent revisits for selected targets of interest. As an initial technology demonstration of this vision, the NACHOS project is currently slated to launch two CubeSats in early 2022.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2021

Ribulose-1,5-Bisphosphate Carboxylase/Oxygenase (RubisCO) Is Essential for Growth of the Methanotroph Methylococcus capsulatus Strain Bath

The importance of RubisCO and CO 2 in M. capsulatus Bath metabolism is unclear. In this study, we demonstrated that both CO 2 and RubisCO are essential for M. capsulatus Bath growth. 13 CO 2 tracing experiments supported that RubisCO mediates CO 2 fixation and that a noncanonical Calvin cycle is active in this organism.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2021

Observing correlations between dark matter accretion and galaxy growth: II. testing the impact of galaxy mass, star formation indicator, and neighbour colours

A crucial question in galaxy formation is what role new accretion has in star formation. Theoretical models have predicted a wide range of correlation strengths between halo accretion and galaxy star formation. Previously, we presented a technique to observationally constrain this correlation strength for isolated Milky Way mass galaxies at z ~ 0.12, based on the correlation between halo accretion and the density profile of neighbouring galaxies. By applying this technique to both observational data from the Sloan Digital Sky Survey and simulation data from the UNIVERSEMACHINE , where we can test different correlation strengths, we ruled out positive correlations between dark matter accretion and recent star formation activity. In this work, we expand our analysis by (1) applying our technique separately to red and blue neighbouring galaxies, which trace different infall populations, (2) correlating dark matter accretion rates with D n 4000 measurements as a longer-term quiescence indicator than instantaneous star-formation rates, and (3) analysing higher-mass isolated central galaxies with 10 11.0 < M * /M ⊙ < 10 11.5 out to z ~ 0.18. Finally, in all cases, our results are consistent with non-positive correlation strengths with ≳ 85 percent confidence, which is most consistent with models where processes such as gas recycling dominate star formation in massive z = 0 galaxies.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2024

An exploration of anomalous electrical noise in shocked cyclotrimethylenetrinitramine (RDX)-based explosives

Gas gun shock experiments on cyclotrimethylenetrinitramine (RDX)-based explosive compositions that employ embedded gauge particle velocity tracers have noted a significant amount of electrical noise when compared to other explosive formulations. This paper reexamines previously published embedded gauge data on Cyclotols (60–80 wt. % RDX) to quantify the electromagnetic behavior of these materials. The primary observation is a fourfold increase in the electrical noise when Cyclotols are shocked above 4.22 ± 0.08 GPa. Electromagnetic gauge noise is also observed within particle velocity traces in reactive growth and off-Hugoniot shocks, although at higher pressures than the direct shock case, suggesting a temperature- or kinetically dependent transition. In all cases, the electrical noise disappears upon detonation. By comparing with the static high-pressure phase diagram of RDX, we interpret this change in electromagnetic behavior to be a change in the RDX crystal structure to a piezoelectric phase, although it is uncertain whether the γ or ε phase is responsible for the observed behavior.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Transport and chemistry of isoprene and its oxidation products in deep convective clouds

Deep convective clouds can transport trace gases from the planetary boundary layer into the upper troposphere where subsequent chemistry may impact aerosol particle formation and growth. In this modelling study, we investigate processes that affect isoprene and its oxidation products injected into the upper troposphere by an isolated deep convective cloud in the Amazon. We run a photochemical box model with coupled cloud microphysics along hundreds of individual air parcel trajectories sampled from a cloud-resolving model simulation of a convective event. The box model simulates gas-phase chemical reactions, gas scavenging by liquid and ice hydrometeors, and turbulent dilution inside a deep convective cloud. The results illustrate the potential importance of gas uptake to anvil ice in regulating the intensity of the isoprene oxidation and associated low volatility organic vapour concentrations in the outflow. Isoprene transport and fate also depends on the abundance of lightning-generated nitrogen oxide radicals (NO x = NO + NO 2 ). If gas uptake on ice is efficient and lightning activity is low, around 30% of the boundary layer isoprene will survive to the cloud outflow after approximately one hour of transport, while all the low volatile oxidation products will be scavenged by the cloud hydrometeors. If lightning NO x is abundant and gas uptake by ice is inefficient, then all isoprene will be oxidised during transport or in the immediate outflow region, while several low volatility isoprene oxidation products will have elevated concentrations in the cloud outflow. Reducing uncertainties associated with the uptake of vapours on ice hydrometeors, especially HO 2 and oxygenated organics, is essential to improve predictions of isoprene and its oxidation products in deep convective outflows and their potential contribution to new particle formation and growth.

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

Ambient Mass Spectrometry Rapid Analysis Methods for Trace Inorganics

The ability to rapidly detect and characterize the chemistry of trace quantities of inorganic species has multiple potential applications, including nuclear safeguards, nuclear forensics, and environmental monitoring. Some mass spectrometric methods currently exist, but they are costly and time-intensive, often destroying chemical information in the process of ionization. Ambient mass spectrometry is a relatively new analytical method in which samples are introduced to the mass spectrometer from atmospheric pressure, rather than from high vacuum. Ambient MS can operate with gentler ionization methods such as electrospray ionization (ESI) and paper-spray ionization (PSI), reducing fragmentation and preserving the chemical information of the analyte. This may be useful for determining the intended purpose of material in a sample. Strontium, part of nuclear fallout, is analyzed here to test these new analytical methods for viability. Electrospray ionization mass spectrometry functions by spraying the sample as a solution through a needle charged to a few kV. A nebulizing gas flows out along with the sample to create the spray before droplets enter a drying chamber with heated drying gas to remove the solvent molecules. From there bare analyte ions enter the mass spectrometer. This method has the advantage of relatively fast sample preparation and stable ionization. More stable ionization produces higher-quality data. Paper-spray ionization mass spectrometry operates by applying sample to a paper triangle. The paper triangle is then electrified in a metal clamp to a few kV before spray solvent is applied. The spray solvent transports analyte in the sample to the tip, where it is ionized and enters the mass spectrometer. One advantage of this method is reduced sample preparation - an analyst can even swipe a surface and cut a triangle directly from the swipe. The data analysis serves to rapidly process tens of samples all at once. The mass spectrometer outputs a file containing a few hundred spectra for each sample. The pipeline processes each one to identify peaks of interest. A full palette of data analysis metrics are generated, including plots of the raw data and plots of calculated values such as isotopic ratios. The pipeline filters the raw data to remove noise and background peaks, as well as peaks representing detector saturation. A heat map is generated to show the overall spectrum in mass-time- intensity space. Post-processing, we obtained the desired calibration curves, demonstrating that both ESI-MS and PSI-MS are viable methods for quantifying trace amounts of inorganics while retaining their chemical speciation information. ESI-MS demonstrated a linear response region of 100 ppb to 20 ppm, with a limit-of-detection of around 100 ppb. At top left is an example spectrum with the {sup 88}SrNO{sub 3} peak identified to show the retention of chemical speciation. PSI-MS showed a linear response region of around 1 ppb to 1 ppm, with a limit-of-detection of near 1 ppb. PSI-MS produced more erratic results than ESI-MS, likely due to the variability in ionization resulting from manual positioning of the paper triangle near the MS inlet. Future efforts will focus on improving the repeatability of PSI-MS as well as analyzing other species of interest such as cerium and uranium. Improvements will also be made to create more reliable data extraction and intelligent data filtering.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗