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All sourcesNASA NTRSDOE OSTI
NASA NTRS2016

Evaluation of Observed and Modelled Aerosol Lifetimes Using Radioactive Tracers of Opportunity and an Ensemble of 19 Global Models

Aerosols have important impacts on air quality and climate, but the processes affecting their removal from the atmosphere are not fully understood and are poorly constrained by observations. This makes modelled aerosol lifetimes uncertain. In this study, we make use of an observational constraint on aerosol lifetimes provided by radionuclide measurements and investigate the causes of differences within a set of global models. During the Fukushima Dai-Ichi nuclear power plant accident of March 2011, the radioactive isotopes cesium-137 (Cs-137) and xenon-133 (Xe-133) were released in large quantities. Cesium attached to particles in the ambient air, approximately according to their available aerosol surface area. Cs-137 size distribution measurements taken close to the power plant suggested that accumulation mode (AM) sulfate aerosols were the main carriers of cesium. Hence, Cs-137 can be used as a proxy tracer for the AM sulfate aerosol's fate in the atmosphere. In contrast, the noble gas Xe-133 behaves almost like a passive transport tracer. Global surface measurements of the two radioactive isotopes taken over several months after the release allow the derivation of a lifetime of the carrier aerosol. We compare this to the lifetimes simulated by 19 different atmospheric transport models initialized with identical emissions of Cs-137that were assigned to an aerosol tracer with each model's default properties of AM sulfate, and Xe-133 emissions that were assigned to a passive tracer. We investigate to what extent the modelled sulfate tracer can reproduce the measurements, especially with respect to the observed loss of aerosol mass with time. Modelled Cs-137and Xe-133 concentrations sampled at the same location and times as station measurements allow a direct comparison between measured and modelled aerosol lifetime. The e-folding lifetime e, calculated from station measurement data taken between 2 and 9 weeks after the start of the emissions, is 14.3 days (95% confidence interval 13.1-15.7 days). The equivalent modelled e lifetimes have a large spread, varying between 4.8 and 26.7 days with a model median of 9.42.3 days, indicating too fast a removal in most models. Because sufficient measurement data were only available from about 2 weeks after the release, the estimated lifetimes apply to aerosols that have undergone long-range transport, i.e. not for freshly emitted aerosol. However, modelled instantaneous lifetimes show that the initial removal in the first 2 weeks was quicker (lifetimes between 1 and 5 days) due to the emissions occurring at low altitudes and co-location of the fresh plume with strong precipitation. Deviations between measured and modelled aerosol lifetimes are largest for the northernmost stations and at later time periods, suggesting that models do not transport enough of the aerosol towards the Arctic. The models underestimate passive tracer (Xe-133) concentrations in the Arctic as well but to a smaller extent than for the aerosol (Cs-137) tracer. This indicates that in addition to too fast an aerosol removal in the models, errors in simulated atmospheric transport towards the Arctic in most models also contribute to the underestimation of the Arctic aerosol concentrations.

Radioactive isotopes↗
NASA NTRS2017

US Navy Submarine Sea Trial of NASA developed Multi-Gas Monitor

During a successful 2 year technology demonstration of the tunable diode laser spectroscopy (TDLS) based Multi-Gas Monitor (MGM) on the International Space Station (ISS), we began discussing with the US Navy the possibility of conducting a sea trial of an MGM on a submarine. The sea trial would also include a gas chromatography/differential mobility spectrometer based Air Quality Monitor (AQM), which is used operationally on ISS for select volatile organic compounds. AQM results will be the subject of a separate paper. The Navy’s interest in testing NASA equipment is in a planned update to the environmental monitoring equipment used aboard submarines. NASA’s goal is studying submarines as closed environment analogs to spacecraft. MGM’s core technology was developed by Vista Photonics Inc using Small Business Innovation Research (SBIR) grants and expanded for various applications using NASA program funding. The MGM measures oxygen, carbon dioxide, ammonia and water vapor in ambient air, displays concentrations with temperature and pressure, and stores 30 second moving averages. The sea trial involves colocating the instrument with the Central Air Monitor (CAM) and connecting it to rack power prior to departure, and letting it run during the entire sea trial of a few months duration. All data stored is inside MGM, with no connection to the vessel data bus. Crew intervention is limited to checking MGM periodically to see that it is working and power cycling if the display is OFF. After the trial is over, the unit with its data will be retrieved. Post sea trial calibration check and data analysis are planned and results will be compared with both CAM data and results from MGM’s ISS technology demonstration.

Mudgett, Paul D.↗
NASA NTRS1991

Annular denuder systems: Precision and applicability to stratospheric sampling

Annular denuder systems (ADS) are designed to sample both gases and particles from ambient air without cross interference. The ADS's were used to detect chemical gradients over rural forest canopies. Accurate and precise methods for the sampling and analysis of low concentrations of gaseous and particulate species over short sampling periods were developed. Typical analytical precision data for nitrate and sulfate are shown. Both sampling and analytical precision data for a 2 hour test using four collocated ADS's are presented. On this particular day, the overall precision for HNO3 was unusually poor. The overall precision for the major constituents of interest is generally about 3 to 5 percent for typical ambient concentrations. The ADS's could potentially be used to determine the concentrations of HNO3 and fine-particle nitrate in the stratosphere, and to simultaneously characterize the chemical composition of stratospheric aerosols. Assuming 50 mb pressure, a 2 hour sampling time, a 50 Lpm sampling rate, and a low blank value, an overal precision of about 15 percent should be possible for 1 ppbv of HNO3 or nitrate, which would include nitric-acid trihydrate (NAT); and pump-driven systems could accommodate more complex systems involving denuders and filter packs in sequence. Alternate coatings could possibly be developed to selectively sample species such as Cl2 and ClNO3. The ADS's might also be useful in laboratory studies of heterogeneous chemical reactions involving NAT aerosols.

Randtke, Stephen J.↗
NASA NTRS1987

Optimization of the tungsten oxide technique for measurement of atmospheric ammonia

Hollow tubes coated with tungstic acid have been shown to be of value in the determination of ammonia and nitric acid in ambient air. Practical application of this technique was demonstrated utilizing an automated sampling system for in-flight collection and analysis of atmospheric samples. Due to time constraints these previous measurements were performed on tubes that had not been well characterized in the laboratory. As a result the experimental precision could not be accurately estimated. Since the technique was being compared to other techniques for measuring these compounds, it became necessary to perform laboratory tests which would establish the reliability of the technique. This report is a summary of these laboratory experiments as they are applied to the determination of ambient ammonia concentration.

Brown, Kenneth G.↗
DOE OSTI2021

Fog Formation Related to Gravity Currents Interacting with Coastal Topography

An interesting mixing-fog event was identified during IOP7 of the C-FOG project, where a cold front arriving from the north-east collided with the Downs peninsula in Ferryland, Newfoundland, to produce foggy conditions. A comprehensive set of field observations suggests that this collision caused turbulent mixing of nearly saturated ambient air with an almost saturated cold front, creating conditions for mixing fog. Additionally, laboratory experiments were performed to study the interaction of lock-exchange induced gravity currents with a (rectangular) obstacle to delve into physical processes underlying this phenomenon. Instantaneous velocity and density fields were obtained using particle image velocimetry and planar laser-induced fluorescence. The observations suggest that the obstacle starts affecting the approaching gravity-current propagation at an upstream distance of 2 H and, upon collision, the mixing is taking place over a spatial scale of 0.83 H , where H is the depth of the ambient fluid layer. The time for largerscale turbulent stirring to permeate to the smallest scales of turbulence and activate the condensation nuclei was estimated as 3t * , where t* = √H/g' is the intrinsic time scale of the gravity current and g' the reduced gravity. Extrapolation of results to IOP7 showed a good agreement with observations.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

What does it take to “see” air leakage through a building envelope?

Unwanted air leakage in buildings can cause health and comfort issues for the building occupants and contribute to rot and mold growth in building materials. Leakage also contributes to unnecessary energy consumption ~4 quads (1172 TWh) per year in the buildings sector in the United States. Finding and repairing leaks through the building envelope can improve the energy efficiency, comfort, air-quality, and moisture durability of the building stock. Typical methods of locating air leakage, such as infrared imaging or smoke tracing, rely on concurrent blower door operation which also measures the total leakage rate of the building. These methods can be disruptive to occupants and can’t measure the contribution of individual leaks to prioritize sealing efforts. ORNL is working on a refraction-based fluid flow imaging technique that can measure the leakage rate of individual leaks from the outside of the building. The working principle of this device is based on the refraction of light caused by the exfiltration because there is a small difference in density between the exfiltration and ambient air. We will discuss the operation of the air leak detector and key variables that affect its performance. We will also present preliminary results showing the visualization capability of this new air leak detector under different conditions. Experiments were completed with different claddings, air temperatures, and lighting conditions.

Boudreaux, Philip↗
DOE OSTI2020

Half‐Fused Diketopyrrolopyrrole‐Based Conjugated Donor–Acceptor Polymer for Ambipolar Field‐Effect Transistors

Abstract A novel building block, denoted as half‐fused diketopyrrolopyrrole (DPP) (9‐(3‐octadecylhenicosyl)‐8‐(thiophen‐2‐yl)‐7 H ‐pyrrolo[3,4‐ a ]thieno[3,2‐ g ]indolizine‐7,10(9 H )‐dione), in which one of the flanking thiophene units is fused to one of the DPP rings via a carbon‐carbon double bond at the N‐position is reported. The half‐fused DPP is successfully utilized as an electron acceptor to prepare the conjugated donor–acceptor polymer PTFDFT , which exhibits ambipolar semiconducting behavior in ambient air. Theoretical calculations and absorption spectral studies show that the backbone of PTFDFT is more planar compared to the reference polymer with conventional DPP units. As a result, PTFDFT shows a narrow bandgap and low lowest unoccupied molecular orbital level. The more planar backbone with fewer side chains favors the dense packing of the polymer chains of PTFDFT with a short π–π stacking distance (3.49 Å). Grazing‐incidence wide‐angle X‐ray scattering data further confirm the predominant edge‐on packing mode of the PTFDFT polymer chains on the substrate. As expected, the PTFDFT thin film shows excellent ambipolar semiconducting properties under ambient conditions, reaching 2.23 and 1.08 cm 2 V −1 s −1 for the n‐ and p‐channels, respectively. In addition, complementary‐like inverter with gain value as high as 141 is successfully constructed using the PTFDFT thin film.

Shi, Dandan↗
DOE OSTI2024

Capturing carbon dioxide from air with charged-sorbents

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

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

High performance ionic-liquid-gated air doped diamond field-effect transistors

Here we report successful fabrication of high performance ion-gated field-effect transistors (FETs) on hydrogenated diamond surface. Investigations on the hydrogen (H)-terminated diamond by Hall effect measurements shows Hall mobility as high as ~200 cm 2 V –1 s –1 . In addition we demonstrate a rapid fabrication scheme for achieving stable high performance devices useful for determining optimal growth and fabrication conditions. We achieved H-termination using hydrogen plasma treatment with a sheet resistivity as low as ~1.3 kΩ/sq. Conductivity through the FET channel is studied as a function of bias voltage on the liquid ion-gated electrode from –3.0 to 1.5 V. Stability of the H-terminated diamond surface was studied by varying the substrate temperature up to 350 °C. It was demonstrated that the sheet resistance and carrier densities remain stable over 3 weeks in ambient air atmosphere even at substrate temperatures up to 350 °C, whereas increasing temperature beyond this limit has effected hydrogenation. This study opens new avenues for carrying out fundamental research on diamond FET devices with ease of fabrication and high throughput.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
NASA NTRS1999

Summary of HEAT 1 Aeroacoustics Installation Effects

A critical part of the NASA High-Speed Research (HSR) program is the demonstration of satisfactory suppression of the jet noise present at low airspeeds. One scheme for reducing jet exhaust noise generated by a future High-Speed Civil Transport (HSCT) is the use of a mixer/ ejector system which would entrain large quantities of ambient air into the exhaust flow from the powerplant in order to cool and slow the jet exhaust before it leaves the tailpipe. Of the variety of factors which can affect the noise suppression characteristics of the mixer/ejector system, the influence of the wing flow field and high-lift devices is not well understood. The effectiveness of the noise suppression device must be evaluated in the presence of the wing/high-lift system before definitive assessments can be made concerning HSCT noise. Of nearly equal importance is the evaluation of the performance of the high-lift system(s) in the presence of realistic propulsion units which feature high ambient flow entrainment rates and jet thrust coefficients. These noise suppressors must provide the required acoustic attenuation while not overly degrading the thrust efficiency of the propulsion system or the lift enhancement of the high-lift devices on the wing. The overall objective of the NASA High-lift Engine Aeroacoustics Technology program is to demonstrate satisfactory interaction between the jet noise suppressor and the high-lift system at airspeeds and angles of attack consistent with takeoff, climb, approach, and landing. In support of this program, an isolated aeroacoustic test of a 13.5%-scale, candidate mixer/ejector nozzle was performed in the Ames' Research Center 40- by 80-Foot Wind Tunnel. The purpose of the test was to measure the baseline aeroacoustic performance characteristics of this nozzle in isolation from the aerodynamic flowfield induced by an HSCT airframe. The test documented the acoustic signature of the nozzles with treated and hardwall ejector surfaces and with changes in the ratio of ejector-duct-to-jet-area over a wide range range of nozzle pressure ratios and freestream Mach numbers. The test also measured the thrust performance, ambient-flow aspiration ratio, and internal and external static pressures on the nozzles. The isolated aeroacoustic performance data has been compared with results obtained with this nozzle installed on a 13.5% Boeing Reference H HSCT configuration, semi-span model. The semi-span, aeroacoustics integration test documented the first-order effects of the airframe flowfield on the acoustic performance of the nozzle and the effect of the nozzle secondary inlet flows on the aerodynamic performance of the wing high-lift systems. This investigation is critical to understanding the mutual installation effects of mixer/ejector nozzles and wing high-lift systems.

Smith, Brian E.↗
DOE OSTI2023

Evolution of titanium particle combustion in potassium perchlorate and air

Understanding titanium particle combustion processes is critical not only for characterizing existing pyrotechnic systems but also for creating new igniter designs. In order to characterize titanium particle combustion processes, morphologies, and temperatures, simultaneous spatially-resolved electric field holography and imaging pyrometry techniques were used to capture post-ignition data at up to 7 kHz. Due to the phase and thermal distortions present in the combustion cloud, traditional digital in-line holography techniques fail to capture accurate data. Here in this work, electric field holography techniques are used in order to cancel distortions and capture the three-dimensional spatial locations and diameters of the particles. In order to estimate the projected surface temperatures of the titanium particles, an imaging pyrometry method that ratios emission at 750 and 850 nm is utilized. Using these diagnostics, joint statistics are collected for particle size, morphology, velocity, and temperature. Results show that, early in the combustion process, the titanium particles are primarily oxidized by potassium perchlorate inside the igniter cup, resulting in projected surface temperatures near 3000 K. Later in the process, the particles interact with ambient air, resulting in lower surface temperatures around 2400 K and the formation of flame zones. These results are consistent with adiabatic flame temperature predictions as well as particle morphology observations of a titanium core with a TiO 2 surface. Late stage particle expansion, star fragmentation, and molten droplet breakup events are also observed using the time-resolved morphology and temperature diagnostics. These results illustrate the different stages of titanium particle combustion in pyrotechnic environments, which can be used to inform improvements in next-generation igniters.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Response of marine post-frontal clouds to Gulf Stream variability

Understanding how Gulf Stream variation influences cloud morphology is critical for evaluating cloud feedback in the western North Atlantic Ocean and beyond, where mesoscale air-sea interactions dominate. This study investigates the impact of altered mean sea surface temperature (SST) and SST gradients on post-frontal cloud characteristics during cold-air outbreaks, using the Weather Research and Forecasting (WRF) model. Three sensitivity experiments are conducted: a control simulation (default SST), Plus4 (uniform SST increase of 4 K), and Gradplus (SST gradient enhanced by 25 %, centered around mean SST). Results reveal distinctly different responses in boundary layer dynamics and cloud macro-physics. In Plus4, a warmer and moister boundary layer reduces total cloud cover but promotes larger cloud sizes and elongated cloud streets, with diminished liquid water and enhanced ice-phase hydrometeors. Conversely, Gradplus amplifies impacts in the upwind colder SST regions, yielding a drier, colder boundary layer, weaker energy transport, and higher liquid water path but reduced ice water content and cloud lines. Tracer analysis highlights that SST modifications alter airmass sources near cloud tops due to the entrainment of ambient air, with Plus4 amplifying boundary layer contributions to cloud-top regions. These findings underscore the spatially varying effects of SST gradients and mean SST on cloud organization and microphysics, emphasizing the need to resolve ocean-atmosphere coupling in global models to improve the prediction of marine cloud feedback under warming scenarios.

AIR-SEA INTERACTION↗
NASA NTRS2021

Air Pollution Scenario over Pakistan: Characterization and Ranking of Extremely Polluted Cities using Long-Term Concentrations of Aerosols and Trace Gases

Pakistan ranks third in the world in terms of mortality attributable to air pollution, with aerosol mass concentrations (PM2.5) consistently well above WHO (World Health Organization) air quality guidelines (AQG). However, regulation is dependent on a sparse network of air quality monitoring stations and insufficient ground data. This study utilizes long-term observations of aerosols and trace gases to characterize and rank the air pollution scenarios and pollution characteristics of 80 selected cities in Pakistan. Datasets used include (1) the Aqua and Terra (AquaTerra) MODIS (Moderate Resolution Imaging Spectroradiometer) Level 2 Collection 6.1 merged Dark Target and Deep Blue (DTB) aerosol optical depth (AOD) retrieval products; (2) the CAMS (Copernicus Atmosphere Monitoring Service) reanalysis PM1, PM2.5, and PM10 data; (3) the MERRA-2 (Modern-Era Retrospective analysis for Research and Applications, Version 2) reanalysis PM2.5 data, (4) the OMI (Ozone Monitoring Instrument) tropospheric vertical column density (TVCD) of nitrogen dioxide (NO2), and VCD of sulfur dioxide (SO2) in the Planetary Boundary Layer (PBL), (5) the VIIRS (Visible Infrared Imaging Radiometer Suite) Nighttime Lights data, (6) MODIS Collection 6 Version 2 global monthly fire location data (MCD14ML), (7) population density, (8) MODIS Level 3 Collection 6 land cover types, (9) AERONET (AErosol RObotic NETwork) Version 3 Level 2.0 data, and (10) ground-based PM2.5 concentrations from air quality monitoring stations. Potential Source Contribution Function (PSCF) analyses were performed by integrating with ground-based PM2.5 concentrations and the NOAA (National Oceanic and Atmospheric Administration) HYSPLIT (Hybrid Single-Particle Lagrangian Integrated Trajectory) air parcel back trajectories to identify potential pollution source areas which are responsible for extreme air pollution in Pakistan. Results show that the ranking of the top polluted cities depends on the type of pollutant considered and the metric used. For example, Jhang, Multan, and Vehari were characterized as the top three polluted cities in Pakistan when considering AquaTerra DTB AOD products; for PM1, PM2.5, and PM10 Lahore, Gujranwala, and Okara were the top three; for tropospheric NO2 VCD Lahore, Rawalpindi, and Islamabad and for PBL SO2 VCD Lahore, Mirpur, and Gujranwala. The results demonstrate that Pakistan’s entire population has been exposed to high PM2.5 concentrations for many years, with a mean annual value of 54.7 μg/cu. m, over all Pakistan from 2003 to 2020. This value exceeds Pakistan’s National Environmental Quality Standards (Pak-NEQS, i.e., <15 μg/cu. m annual mean) for ambient air defined by the Pakistan Environmental Protection Agency (Pak-EPA) as well as the WHO Interim Target-1 (i.e., mean annual PM2.5 <35 μg/cu. m). The spatial analyses of the concentrations of aerosols and trace gases in terms of population density, nighttime lights, land cover types, and fire location data, and the PSCF analysis indicate that Pakistan’s air quality is strongly affected by anthropogenic sources inside of Pakistan, with contributions from surrounding countries. Statistically significant positive (increasing) trends in PM1, PM2.5, PM10, tropospheric NO2 VCD, and SO2 VCD were observed in ~89%, ~67%, ~48%, 91%, and ~88% of the Pakistani cities (80 cities), respectively. This comprehensive analysis of aerosol and trace gas levels, their characteristics in spatio-temporal domains, and their trends over Pakistan, is the first of its kind. Results will be helpful to the Ministry of Climate Change (Government of Pakistan), Pak-EPA, SUPARCO (Pakistan Space and Upper Atmosphere Research Commission), policymakers, and the local research community to mitigate air pollution and its effects on human health.

Muhammad Bilal↗
NASA NTRS1995

Effects of Chronic 2.0% and 0.7% CO2 Exposures on the Well-Being, Growth and Renal Function of Rats

On the Space Shuttle and MIR, mean CO2 levels have been 0.3% which is ten times that of normal air. There have also been extended periods with levels of 0.7% CO2 with peak concentrations at 2.0%. The Space Station program had proposed that CO2 concentration levels be maintained, on average, at 0.7%, and not to exceed 1.0%. To ensure that these levels of CO2 would not compromise the integrity of the science performed on the Space Station, the effects of chronic exposure of rats to 2.0% and 0.7% CO2 were investigated. Ten male rats per group were placed in individual metabolic cages for monitoring of food and water consumption, as well as fecal and urine production. Cages were placed in a large (4W x 10L x 4H ft.) plexiglass chamber with a controlled atmospheric environment. Following 7 days of cage adaptation, animals were exposed to experimental (2.0% or 0.7% CO2) or control (ambient air) conditions for 30 days. Daily body weight, food and water intake, and fecal and urine excretions were measured for the last three days of adaptation and the first ten days of exposure and then every three to four days for the remaining three weeks. Urine was measured for pH and total CO2. During 2.0% and 0.7% CO2 exposures, animal growth, fecal production and food and water consumption were within normal ranges. Urine excretion was significantly (p less than 0.05) higher in both experimental groups compared to controls. Urine pH of animals exposed to 2.0% CO2 was decreased by 0.32 over the first 6 days of exposure, followed by a 0.63 increase by day 30. In animals exposed to 0.7% CO2, urine pH did not decrease early in the exposure period, but did increase by 0.37 by day 30. Urine CO2 excretion did not change the first 6 days of exposure, but significantly increased in both 2.0% and 0.7% CO2 by day 30 (897 and 402 mmol/day, respectively). These results of chronic exposure to 2.0% and 0.7% CO2 are consistent with renal compensation in response to an altered acid-base homeostasis. These findings may impact science conducted on the Space Shuttle or the Space Station if CO2 concentrations reach 0.7%.

Lang, C. K.↗
NASA NTRS2018

Exploring Li-Air Batteries for High Specific Energy and High Power Applications: A Simulation Study

Commercialization of lithium-air batteries face many challenges, such as electrolyte decomposition, short cycle life, low energy efficiency, low power density, etc. However, commercialization of Li-air batteries for mass sensitive applications such as electric vehicles, portable power source, and drones is more challenging due to additional constraints of safety, electrolyte evaporation, high specific energy requirements, and reliable discharge times. In this presentation, we will present our finite element simulation results comparing Li-O2 and Li-air batteries using power density, energy density, specific power, and discharge times as metrics to evaluate different electrolytes and electrode geometry to reduce total mass and maximize discharge current. We use a finite element model and a discharge product model developed in which is based on porous electrode and concentrated electrolyte theories and the discharge product is modeled using quantum tunneling; for reaction kinetics and oxygen diffusion, an improved model was used. The electrolyte properties such as ion conductivity and ion diffusion were obtained from Molecular Dynamics (MD) simulations while the other parameters for the finite element model were calibrated to match experiments at high discharge current densities (>1.5 mA/cm2). The mass densities of different electrolytes were computed using MD simulations as well. For this presentation, we examine the practical electrochemical mass of a system at different current ratings, the sensitivity of mass to the use of ambient air as compared to pure oxygen as well as the electrolyte, which affects maximum current density and the total mass associated with the electrolyte (which includes the mass of additional components), and, the optimization of battery geometry for total discharge time, average discharge voltage, maximum discharge current, and minimum electrochemical mass.

Mehta, M.↗
DOE OSTI2024

Bench-Scale Testing of Monolithic PPI Structured Contactors for Direct Air Capture of CO 2

The overall project objective was to develop, optimize and bench-scale test the integrated embodiment of a leading direct air capture (DAC) sorbent composition, linear-poly(propylenimine) (l-PPI), in a structured material system, specifically a monolithic contactor for achieving low pressure drop, to justify its further scale-up in a subsequent program. The project team was led by CORMETECH, a leading monolithic gas/solid contactor manufacturer for environmental applications, and included Global Thermostat, a well-known DAC start-up, and Georgia Tech, a prominent US academic institution in carbon capture and DAC. The monolithic contactor for l-PPI in this project employed an advanced, cost-effective fabrication technique from CORMETECH, namely a porous monolith substrate directly impregnated with the amine, an approach contrasting to the traditional wash-coating methods used for activating monoliths. The l-PPI monolithic contractor is targeted for use in DAC systems such as the Global Thermostat DAC process, which involves the cyclic operation of ambient air flow over a monolithic amine contactor followed by steam-mediated thermal desorption and CO 2 collection, maximizing volumetric productivity while reducing the auxiliary power required to capture CO 2 from air. The Global Thermostat DAC process currently utilizes poly(ethyleneimine) (PEI) materials as baseline sorbents, which are subject to oxidative degradation and slow capacity fade at the elevated temperature required for efficient CO 2 removal. Georgia Tech, with Global Thermostat, had discovered in lab-scale efforts that l-PPI had superior resistance to oxidative degradation compared to PEI, with similar CO 2 adsorption capacity. While the novel l-PPI sorbent offers significant advantages over PEI for DAC, including potential design simplification and increased process efficiency, it is not commercially available, and prior to this project, had not yet been evaluated on the bench-scale in a structured contactor.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Pre-Ionization Controlled Laser Plasma Formation for Ignition Applications (Final Scientific/Technical Report)

This report consists of three grand funded papers. Abstracts for each follow. 1) In this work, we present experimental and modeling studies of air pre-ionization using ultraviolet (UV) laser pulses and its effect on laser breakdown of an overlapped near-infrared (NIR) pulse. Experimental studies are conducted with a 266 nm beam (fourth harmonic of Nd:YAG) for UV pre-ionization and an overlapped 1064 nm NIR beam (fundamental of Nd:YAG), both having pulse duration of 10 ns. Results show that the UV beam produces a pre-ionized volume which assists in breakdown of the NIR beam, leading to reduction in NIR breakdown threshold by factor of >2. Numerical modeling is performed to examine the ionization and breakdown of both beams. The modeled breakdown threshold of the NIR, including assist by pre-ionization, is in reasonable agreement with the experimental results. 2) The present contribution compares the energy absorption, optical emission, temperature, and fluid dynamics of ultraviolet (UV) λ = 266 nm and near infrared (NIR) λ = 1064 nm nanosecond laser induced plasmas in ambient air. For UV pulses at the conditions studied, energy absorption by the plasmas increases relatively gradually with laser pulse energy starting at delivered energy of E~8 mJ. Corresponding measurements of plasma luminosity show that the absorption of UV radiation does not necessarily result in visible plasma emission. For the NIR induced plasmas, the energy absorption profile is far more abrupt and begins at ~55 mJ. In contrast with UV, the absorption of NIR radiation is always accompanied by intense optical emission. The temperatures of both types of plasma have been measured with Rayleigh scattering thermometry (at times after the Thomson signal sufficiently diminishes). The UV plasmas can attain a wider range of temperatures, including lower temperatures, depending on the pulse energy (e.g., T ~400–2000K for E ~7–35 mJ at Δt = 10 μs after the pulse) while the NIR plasmas show only hotter temperatures (e.g., T ~ 12 000 K for E = 75 mJ at Δt = 10 μs after the pulse) as is consistent with the literature. Differences in the fluid dynamics for UV versus NIR pulses are shown with Schlieren imaging. In this work, the contrast in the UV and NIR plasma threshold behavior is attributed to differing roles of avalanche ionization and multiphoton ionization as is also illustrated by a simple numerical model. 3) The present contribution examines the impact of plasma dynamics and plasma-driven fluid dynamics on the flame growth of laser ignited mixtures and shows that a new dual-pulse scheme can be used to control the kernel formation process in ways that extend the lean ignition limit. We perform a comparative study between (conventional) single-pulse laser ignition (λ = 1064 nm) and a novel dual-pulse method based on combining an ultraviolet (UV) pre-ionization pulse (λ = 266 nm) with an overlapped near-infrared (NIR) energy addition pulse (λ = 1064 nm). We employ OH* chemiluminescence to visualize the evolution of the early flame kernel. For single-pulse laser ignition at lean conditions, the flame kernel separates through third lobe detachment, corresponding to high strain rates that extinguish the flame. In this work, we investigate the capabilities of the dual-pulse to control the plasma-driven fluid dynamics by adjusting the axial offset of the two focal points. In particular, we find there exists a beam waist offset whereby the resulting vorticity suppresses formation of the third lobe, consequently reducing flame stretch. With this approach, we demonstrate that the dual-pulse method enables reduced flame speeds (at early times), an extended lean limit, increased combustion efficiency, and decreased laser energy requirements.

Mechanical engineering↗
DOE OSTI2024

Assessment of Amine-Based CO2BOLs for Direct Air Capture

Direct air capture (DAC) technologies extract CO 2 from the atmosphere for CO 2 storage, or utilization. Capturing CO 2 from the air is the most expensive application of carbon capture because CO 2 in the atmosphere is very dilute. There are limited number of CO 2 capture technologies for DAC application. This project aims at developing an energy efficient technology for DAC, leveraging two PNNL’s chemistries (solid and liquid CO 2 capture). Three CO 2 capture sorbents consisting of amine based CO 2 BOLs immobilized in mesoporous silica were designed, synthesized, and tested. These sorbents had ~ 19-23 wt.% amine loadings which is lower than typical amine-based silica sorbents. The surface area and pore volumes of these solid supported CO 2 BOLs are lower compared to those of the pristine silica support. The CO 2 capture performance of these materials was significantly lower than the typical silica supported amines due to low amine loading and higher molecular weight with low amine density. These results show that immobilize CO 2 BOLs in silica are not viable materials for removing CO 2 from ambient air. This project also designed, synthesized at tested liquid solvents for DAC application. Solvent properties that is vapor pressure, CO 2 uptake capacity, kinetics, and viscosity for three novel solvents were evaluated. The CO 2 uptake capacity for one of the most promising amine-based solvent BEPBEGDA was the highest at 13.2 wt% corresponding to 97 mol%. The vapor pressure of the BEPBEGDA solvents were very low at 80 °C compared to other solvents making them suitable for DAC application. The effect of humidity on the CO 2 capture performance of these solvents was evaluated which shows that presence of moisture doesn’t have a negative effect on the CO 2 uptake performance but makes it slightly better. The performances of these solvents were slightly below that of the 0.1M NaOH solution tested under similar conditions. Despite of the slightly lower CO 2 uptake, it is expected that these liquid solvents will have lower regeneration temperature and minimum evaporative losses due their low vapor pressure. Future work will focus on optimization of the liquid solvents for DAC application to improve both CO 2 capture efficiency and capacity without viscosity and vapor pressure increase. Testing of these solvents under DAC conditions using a gas liquid contactor that mimic industrial applications is needed. Solvent cost projection, techno-economic analysis and life cycle analysis are required to evaluate economic viability of this technology.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗