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All sourcesNASA NTRSDOE OSTI
NASA NTRSDate not supplied

Utilizing Radiocarbon and Thermo-optical Measurements to Quantify Source Contributions for Aircraft Engine Particulate Emissions

Recent technological advancements in aircraft engine technology and fuel sources have promising potential for reducing particulate emissions from aircraft engines. During the 2022 Boeing ecoDemonstrator ground-based field campaign, particle and trace gas emissions were sampled for four different fuels, including 100% sustainable aviation fuel (SAF), petroleum-based Jet A fuel, petroleum-based Jet A low sulfur fuel, and a SAF blend. Particulate emissions were collected on quartz microfiber filters and analysed for their radiocarbon content and their elemental carbon (EC) and organic carbon (OC) concentrations. In addition, the radiocarbon content of Jet A fuel, SAF, and aircraft engine oil was also measured. We used the radiocarbon content of the particulate emissions samples and source end members to quantify the relative contribution from engine oil and fuel to carbonaceous aerosol emissions. The results from this study can be used to understand how the implementation of technological advancements in aircraft engine technology and fuel sources will likely impact future aircraft particulate emissions.

Liz Wiggins↗
NASA NTRSDate not supplied

Preliminary Results from the Saffire VI Experiment

Preliminary results are presented for one test of the last flight of the Spacecraft Fire Experiment (Saffire VI) which was conducted on an orbiting Cygnus spacecraft. These experiments directly address the risks associated with our understanding of spacecraft fire behavior at practical length scales and geometries. The lack of this experimental data has forced spacecraft designers to base their designs and safety precautions on 1-g understanding of flame spread, flame self-extinguishment, fire detection, and suppression. The Saffire experiment was developed by an international team of investigators with the goal of addressing open issues in spacecraft fire safety. NASA’s Spacecraft Fire Safety Demonstration Project was formulated with the goal of conducting a series of large-scale experiments in spacecraft environments that represent practical spacecraft fires. These tests spanned 1.5 to 3.2 kW with free air volumes of 17 to 19 cubic meters. The final flight in the series of six experiments examined concurrent spread over large samples (all 41 cm wide) including a thin sheet of flammable fuel (cotton/fiberglass 50 cm long); 2-sided spread over 1 cm thick polymethyl methacrylate (PMMA) (18 cm long); 1-sided spread over 0.5 cm thick (18 cm long); and Nomex fabric (7 cm long). Results are presented for the PMMA samples, the SIBAL sample, and the thin cotton samples from Saffire IV and V. The flame heat release is determined and compared to the overall temperature rise in the spacecraft and the change in the concentration of carbon dioxide and carbon monoxide in the spacecraft. Overall, the temperature and pressure rise in the spacecraft were found to be less significant than the increase in carbon dioxide and carbon monoxide.

fire↗
NASA NTRSDate not supplied

Preliminary Results from the Saffire VI Experiment

The preliminary results are presented for one test of the last flight of the Spacecraft Fire Experiment (Saffire VI) which was conducted on an orbiting Cygnus spacecraft. These experiments directly address the risks associated with our understanding of spacecraft fire behavior at practical length scales and geometries. The lack of this experimental data has forced spacecraft designers to base their designs and safety precautions on 1-g understanding of flame spread, flame self-extinguishment, fire detection, and suppression. The Saffire experiment was developed by an international team of investigators with the goal of addressing open issues in spacecraft fire safety. NASA’s Spacecraft Fire Safety Demonstration Project was designed with the goal of conducting a series of large-scale experiments in spacecraft environments that represent practical spacecraft fires. The final flight examined concurrent spread over large samples (all 41 cm wide) including a thin sheet of flammable fuel (cotton/fiberglass 50 cm long); 2-sided spread over 1 cm thick polymethyl methacrylate (PMMA) (18 cm long) ; 1-sided spread over 0.5 cm thick (18 cm long); and Nomex fabric (7 cm long). This paper focusses on the two-sided PMMA sample. The flame heat release is determined and is compared to the overall temperature rise in the spacecraft and the change in the concentration of carbon dioxide and carbon monoxide in the spacecraft.

fire↗
DOE OSTI2026

Influence of Operating Conditions on Ethanol Passive Prechamber Cold-start Operation

Cold-start operation in spark ignition engines is characterized by many drawbacks such as poor fuel vaporization, substantial wall film formation, and weak ignition which can result in unstable combustion and high concentrations of carbon monoxide (CO), nitrogen oxides (NOx), and unburnt hydrocarbons (UHC) prior to catalyst light-off. These challenges are particularly important for ethanol as the fuel’s high latent heat of vaporization and low vapor pressure can hinder reliable ignition during cold-start. In this context, passive prechamber ignition systems offer a viable pathway to improve ignitability by producing hot turbulent jets that can promote combustion in the main chamber. In this study, the influence of operating conditions on jet formation and combustion characteristics in an ethanol-fueled passive prechamber spark ignition engine is investigated. Two intake pressures (40 kPa and 60 kPa) and two engine speeds (450 and 600 rpm) are studied to represent various stages of the cold-start ramp-up. Results indicate that lower intake pressures lead to delayed and asymmetric turbulent jet formation, and lower peak heat release rates. Lower engine speeds, on the other hand, produced higher peak heat release and faster combustion due to greater residence time in the engine. This greater residence time also increases the likelihood of autoignition in the main chamber, potentially promoting quicker heat release for lower engine speeds. These results provide insight into the role of operating conditions on cold-start ramp-up of passive prechamber engines.

Banagiri, Shrikar [ORNL] (ORCID:0000000239745099)↗
DOE OSTI2025

Colloidal Behavior of Plutonium Oxide in Concentrated Electrolyte Solutions

The Hanford Site in Washington State manages legacy high-level radioactive waste streams that display major chemistry and engineering challenges, including the high salt levels and pH values that correspond to conditions under which many classical concepts describing chemical reactivity cannot be applied. One particular challenge that needs to be tackled at Hanford is that Pu concentrations, [Pu], in the soluble phases of the tank wastes are higher than expected based on the solubility of crystalline PuO2, which is widely accepted to be caused by the formation of PuO2 colloid, consisting of nano- to submicron-sized particles (PuO2 NPs). Fundamental research underpinning the behavior of PuO2 NPs under conditions not only relevant to the Hanford tank waste but at high ionic strength in general is needed to reliably predict the chemical reactivity of PuO2 NPs and develop engineering solutions to safely and efficiently process high-level radioactive waste into forms suitable for long-term storage. In this work, we study the behavior of PuO2 NPs (particle size ~100 nm) under high ionic strength conditions by reacting it with highly concentrated (up to 5 M) salt solutions. We explore different electrolyte compositions to elucidate the impact of different anions (NO3-, Cl-, ClO4-, SO42-, C2O42-, CO32-) on the stability of PuO2 NP in the acidic and alkaline pH regime. PuO2 NP aggregation and precipitation as function electrolyte concentration is tracked by a combination of liquid scintillation counting, dynamic light scattering for determination of particle size distributions, and zeta potentials as a proxy for particle charge. At acidic pH, electrolytes containing non-coordinating anions, such as NaNO3, NaCl, and NaClO4 mostly stabilize PuO2 NPs over a large electrolyte concentration range, showing only subtle differences in their reactivity. Other electrolyte anions show a more pronounced effect on the PuO2 NP stability: SO42-, binds directly to the particles’ surface, reverses the particle charge, and precipitates the PuO2 NPs efficiently even at intermediate sulfate concentrations (>0.1 M). In contrast, C2O42- is found to lead to high [Pu] in solution, in the milli-molar range, even at mildly acidic pH (~4). Thermodynamic modeling of the dissolved Pu concentrations using PHREEQC is unable to predict the observed [Pu] in the acidic pH regime, supporting the influence of colloids in maintaining elevated [Pu]. It is noteworthy that the current thermodynamic databases do not include constants for colloidal Pu phases and cannot accurately predict many of the high ionic strength solutions relevant to this work. The mechanisms and models responsible for these observations will need further investigation in the future. At high pH values (~12), PuO2 NPs exhibits classical sol-gel chemistry, meaning that upon destabilization of the colloidal sol, for example by addition of concentrated NaOH, highly porous and viscid PuO2 coagulates are formed that consist of a three-dimensional network likely held together by physical interactions. The PuO2 NP coagulate shows no significant reversibility of the aggregation when contacted with concentrated brines; however, PuO2 NPs can be efficiently resuspended in solution by addition of diluted electrolytes, alkaline solutions containing high amounts of carbonate, or simple addition of water. Especially carbonate is shown to stabilize PuO2 NPs in solution at high pH, characterized by stable colloidal suspensions that are resistant against sedimentation during centrifugation. Thermodynamic modeling of the carbonate system was able to predict an increasing dissolved Pu concentration with increasing carbonate concentration. However, the model was profoundly sensitive to the fixed redox potential and does not include any thermodynamic constants for colloidal Pu species.

Neumann, Julia↗
NASA NTRS1982

The concentration and isotopic composition of hydrogen, carbon and nitrogen in carbonaceous meteorites

Stepwise pyrolysis was used to extract H2, N2 and C from powdered meteorites and from meteorite residues resulting from partial dissolution in aqueous HF or from reaction with HF-HCl solutions. Concentrations and isotopic compositions were determined for the cases of the carbonaceous chondrites Orgueil, Murray, Murchison, Renazzo and Cold Bokkeveld. Acidification of the meteorites removed the organic sources of H2, so that H2 in the HF-HCl acid residues came mostly from the insoluble organic matter making up 70-80% of the total carbon in carbonaceous meteorites. Good correlation is found between delta-D and the concentration of H2 in the acid residues, but no correlation exists between the delta-D, delta-C-13 and delta-N-15 in them. A model is proposed for both the high delta-D values and the relationship between those values and the H2 concentration.

Robert, F.↗
NASA NTRS1998

Satellite Investigations of Fire, Smoke, and Carbon Monoxide during April 1994 MAPS Mission: Case Studies over Tropical Asia

During April 9-19, 1994, the Measurement of Air Pollution from Satellites (MAPS) measured free tropospheric carbon monoxide (CO) concentrations on a near-global basis. For these eleven days the global lkm advanced very high resolution radiometer (AVHRR) Pathfinder data are used to detect fires and smoke over the Indo-Burma region (85 degrees E - 110 degrees E; 10 degrees N -30 degrees N). The fire activities are categorized for four major ecosystems that include (1) cropland/natural vegetation mosaic (CNVM), (2) evergreen broadleaf forest (EBF), (3) mixed forest (MFD), and (4) grassland (GL). Using published emission rates between particulate matter and carbon monoxide concentrations from temperate areas, the fire counts along with other information are used to obtain estimates of CO concentrations from the AVERR data. More than 7000 fires are detected during the study period with 23%, 43%, 24%, and 10% fires in the CNVM, EBF, MFD, and GL ecosystems, respectively. The enhanced CO concentrations over the area of study are either over or downwind of the fires detected by the AVHRR. The preliminary AVHRR estimates of CO concentrations are smaller than the MAPS-measured values by a factor of 4 to 5 for fire counts areater than 200. The differences are attributed to the lack of transport mechanisms and other assumptions in the current model. However, these results show a good potential for usino the AVHRR measurements to detect fires and smoke and also to estimate CO concentrations.

Christopher, Sundar A.↗
DOE OSTI2020

A meta-analysis of global cropland soil carbon changes due to cover cropping

Including cover crops within agricultural rotations may increase soil organic carbon (SOC). However, contradictory findings generated by on-site experiments make it necessary to perform a comprehensive assessment of interactions between cover crops, environmental and management factors, and changes in SOC. In this study, we collected data from studies that compared agricultural production with and without cover crops, and then analyzed those data using meta-analysis and regression. Our results showed that including cover crops into rotations significantly increased SOC, with an overall mean change of 15.5% (95% confidence interval of 13.8% to 17.3%). Whereas medium-textured soils had highest SOC stocks with (mean = 39 Mg ha-1) and without (mean = 37 Mg ha-1) cover crops, fine-textured soils showed the greatest increase in SOC after the inclusion of cover crops (mean change of 39.5%). Coarse-textured (11.4%) and medium-textured soils (10.3%) had comparatively smaller changes in SOC. Cover crop mixtures resulted in greater increases in SOC compared to mono-species cover crops, and using legumes resulted in greater SOC increases than grasses and broadleaf species. Cover cropping was associated with significant SOC increases in shallow soils (= 30 cm), but not in subsurface soils (> 30 cm). The regression analysis revealed that SOC changes from cover cropping were correlated with improvements in soil quality, specifically decreased runoff and erosion and increased mineralizable carbon, mineralizable nitrogen, and soil nitrogen. Soil carbon change was also affected by annual temperature, number of years after start of cover crop usage, latitude, and initial SOC concentrations. Finally, the mean rate of carbon sequestration from cover cropping across all studies was 0.56 Mg ha-1 yr-1. If 15% of current global cropland were to adopt cover crops, this value would translate to 0.17 Pg of carbon sequestered per year or ~1-2% of current fossil fuels emissions. Altogether, these results indicated that inclusion of cover crops into agricultural rotations can enhance soil carbon concentrations, improve many soil quality parameters, and serve as a potential sink for atmosphere CO2.

Cover crop, soil organic carbon, soil quality, soi↗
DOE OSTI2024

Acid–base concentration swing for direct air capture of carbon dioxide

This work demonstrates the first experimental evidence of the acid–base concentration swing (ABCS) for direct air capture of CO 2 . This process is based on the effect that concentrating particular acid–base chemical reactants will strongly acidify solution, through Le Chatelier's principle, and result in outgassing absorbed CO 2 . After collecting the outgassed CO 2 , diluting the solution will result in a reversal of the acid–base reaction, basifying the solution and allowing for atmospheric CO 2 absorption. The experimental study examines a system that includes sodium cation as the alkalinity carrier, boric acid, and a polyol complexing agent that reversibly reacts with boric acid to strongly acidify solution upon concentration. Though the tested experimental system faces absorption rate and water capacity limitations, the ABCS process described here provides a basis for further process optimization. A generalized theoretical ABCS reaction framework is developed and different reaction orders and conditions are studied mathematically. Higher order reactions yield favorable cycle output results, reaching volumetric cycle capacity above 50 mM for third-order and 80 mM for fourth-order reactions. Optimal equilibrium constants are determined in order to guide alternative chemical searches and synthetic chemistry design targets. There is a substantial energetic benefit for reaction orders above the first, with second- and third-order ABCS cycles exhibiting a thermodynamic minimum work for the concentrating and outgassing steps around 150 kJ per mole of CO 2 . A significant advantage of the ABCS is that it can be driven through well-developed and widely-deployed desalination technologies, such as reverse osmosis, with opportunities for energy recovery when recombining the concentrated and diluted streams, and extraction can occur directly from the liquid phase upon vacuum application.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Improving Conversion of Captured CO 2 on Mixed-Oxide Dual-Function Materials by Low-Concentration Metal Promotion

Reactive carbon capture (RCC) is a promising nascent approach to harness the untapped resource of waste CO 2 to produce fuels and platform chemicals. However, process economics relies on the design of dual-function materials (DFMs) that exhibit maximal conversion of captured CO 2 and high selectivity toward valuable carbon products (e.g., CO). Herein, we report the use of low-concentration (ca. 0.5 wt %) metal promotors (Pt and Au) to improve the conversion of captured CO 2 on a Zn-Al mixed-oxide DFM by >30%, while also more than doubling per-cycle CO yield due to enhanced retention of captured CO 2 and H 2 activation. In situ DRIFTS of bound CO 2 on the DFMs showed distinctions in surface carbonate formation for the Pt- and Au-modified materials that were correlated with product evolution during the reactive desorption step of RCC. Particularly, Pt afforded superior H 2 activation but formed irreversibly-bound bicarbonates, compromising overall productivity, while the Na/Au/ZA DFM predominantly adsorbed CO 2 on Na sites, resulting in polydentate carbonates that are retained until higher temperatures before conversion to CO. In conclusion, these results indicate that adding a low concentration of oxidation-resistant noble metals, especially Au, is an effective strategy for improving key performance metrics of Zn-Al mixed-oxide DFMs to further advance the development of scalable RCC technologies.

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

The contribution of black carbon to global ice nucleating particle concentrations relevant to mixed-phase clouds

Significance The Earth’s climate is affected by the radiative properties of clouds. In clouds containing both supercooled water droplets and ice particles (mixed-phase clouds), cloud lifetime and albedo are affected by the presence of ice nucleating particles (INP). After decades of research, the importance of black carbon (BC) as an INP remains unresolved. In this work, we determined the contribution of BC to INP concentrations ([INP]) from real-world wildfires and prescribed burns. We found that BC does not contribute significantly to [INP] in near-field biomass burning plumes. These results were applied as parameterizations to global climate model output. Combined with previous work on diesel-engine exhaust, we find that BC does not contribute significantly to global [INP] relevant to mixed-phase clouds.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2010

The Use of Remote Sensing Data for Advancing America's Energy Policy

After briefly reviewing America's Energy Policy laid out by the Obama Administration, we outline how a Global Carbon Observing System designed to monitor Carbon from space can provide the necessary data and tools to equip decision makers with the knowledge necessary to formulate effective energy use and practices policy. To stabilize greenhouse gas emissions in the atmosphere in a manner that it does not interfere with the Earth's climate system (which is one of the goals of United Nations Framework for Convention on Climate Change) requires vastly improved prediction of the atmospheric carbon dioxide (CO2) concentrations. This in torn requires a robust understanding of the carbon exchange mechanisms between atmosphere, land, and oceans and a clear understanding of the sources and sinks (i.e. uptake and storage) of CO2. We discuss how the Carbon Observing System from space aids in better understanding of the connection between the carbon cycle and climate change and provides more accurate predictions of atmospheric CO2 concentration. It also enables implementation of greenhouse gas (GHG) mitigation policies such as cap and trade programs, international climate treaties, as well as formulation of effective energy use policies.

Valinia, Azita↗
NASA NTRS1985

Electrochemical CO2 concentration for the Space Station Program

Under the sponsorship of NASA, Electrochemical Carbon Dioxide (CO2) Concentration EDC technology has been developed that removes CO2 continuously or cyclically from low CO2 partial pressure (400 Pa) atmospheres with the performance and operating characteristics required for Space Station applications. The most recent advancement of this technology is the development of an advanced preprototype subsystem, the CS-3A, to remove the metabolic CO2 produced by three persons from the projected Space Station atmosphere. This paper provides an overview of EDC technology, shows how it is ideally suited for Space Station application, and presents technology enhancements that will be demonstrated by the CS-3A subsystem development program.

Lance, N.↗
DOE OSTI2021

Effects of salinity and nutrients on metabolism and growth of Ulva lactuca : Implications for bioremediation of coastal watersheds

We studied Ulva lactuca to determine its potential for bioremediation of coastal watersheds. We cultured Ulva in orthogonal combinations of two salinities and three nutrient concentrations for six weeks, and then measured its growth, photosynthesis, chlorophyll fluorescence, nitrogen, carbon and phosphorus tissue concentrations, and carbon and nitrogen uptake pathways. Our findings show that Ulva was negatively affected by decreased salinity but these effects were ameliorated by the addition of nutrients to the water, such as would be expected from freshwater runoff during heavy rain events. Also, increased nutrients resulted in altered nitrogen (NH$_4^ +$ vs. NO$_3^-$) and carbon (HCO$_3^-$ vs. CO 2 ) uptake pathways, which can allow Ulva to retain its bloom potential even under reduced salinities. Together, our study suggests that Ulva is an ideal species to grow for the purpose of bioremediation of coastal bays and estuaries, even during storms that freshen the surface waters and increase nutrients.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Probing pH-Dependent Dehydration Dynamics of Mg and Ca Cations in Aqueous Solutions with Multi-Level Quantum Mechanics/Molecular Dynamics Simulations

The dehydration of aqueous calcium and magnesium cations is the most fundamental process controlling their reactivity in chemical and biological phenomena, such as the formation of ionic solids or passing through ion channels. It holds particular relevance in light of recent advancements in the development of carbon capture techniques that rely on mineralization for long-term carbon storage. Specifically, dehydration of Ca 2+ and Mg 2+ is a key step in proposed carbon capture processes aiming to exploit the relatively high concentration of dissolved carbon dioxide in seawater via the formation of carbonate minerals from solvated Ca 2+ and Mg 2+ cations for sequestration and storage. Nevertheless, atomic-scale understanding of the dehydration of aqueous Ca 2+ and Mg 2+ cations remains limited. Here, we utilize rare event sampling via density functional theory molecular dynamics and embedded wavefunction theory calculations to elucidate the dehydration dynamics of aqueous Ca 2+ and Mg 2+ . Emphasis is placed on the investigation of the effect pH has on the stability of the different coordination environments. Here, our results reveal significant differences in the dehydration dynamics of the two cations and provide insight into how they may be modulated by pH changes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2004

The Water-Wheel IR (WIR): A Contact Survey Experiment for Water and Carbonates on Mars

Minimum requirements for life include water and accessible carbon. Mars has both in its polar caps and atmosphere. Water (or water-equivalent hydrogen) is present at shallow depths (approx. 10-20 cm) at latitudes =60 and is heterogeneously distributed in other parts of Mars [1]. Mars may have once had surface water that could plausibly have produced carbonate deposits [2-5]. Mars shows signs of hydrothermal activity [6-8] that may have affected soil composition [9, 10]. The Thermal Emission Spectrometer on the Mars Global Surveyor found large and small patches of hematite that may have been water-borne or water-derived [11, 12]. Current orbiting spacecraft (MGS & Odyssey) have not found massive carbonate deposits, however [13]. Shales and limestones, which we associate with moist and benign environments on Earth, are apparently not abundant on Mars. Both carbonate and organic carbon occur as alteration products in Martian meteorites of igneous origin [14]. One study of MGS-TES data suggests 2-5 wt% carbonates (mainly MgCO3) in surface dust, but found no concentrated source [15]. Carbonates and H2O/OH bearing minerals will be sought by the mini-TES and Mossbauer experiments on the Mars Exploration Rovers, one of which landed successfully on Mars on January 3.

Wang, Alian↗