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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 109 records · Page 6
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

The effect of non-redox promoters (AlO x , PO x , SiO x and ZrO x ) and surface sulfates on supported V 2 O 5 -WO 3 /TiO 2 catalysts in selective catalytic reduction of NO with NH 3

The SCR activity of MO x (M=Al, P, Si, Zr) promoted V 2 O 5 -WO 3 /TiO 2 was investigated before and after sulfation. In situ IR spectroscopy indicated that the VO x active sites preferentially anchor on promoter generated surface hydroxyl. In situ Raman spectroscopy confirmed that all oxides are completely dispersed on the TiO 2 surface. In situ NH 3 -IR spectroscopy showed that the oxides can increase the Lewis (AlO x and ZrO x ) and Brønsted (PO x , SiO x , VO x , WO x and SO x ) acid site concentrations. The SiO x and ZrO x promoters had little effect on NO conversion, while the AlO x and PO x promoters and surface sulfation generally inhibited it. The SiO x promoted catalyst was highly SCR active despite lacking Lewis acid sites, indicating that they are not vital for SCR. Finally, the N 2 O formation activity of the catalyst was inhibited by surface sulfation and the promoters, correlating with the promoter and SO x induced increase in the Brønsted acid sites’ strength.

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

Dissolution and initial hydration behavior of tricalcium aluminate in low activity sulfate solutions

Influences of alkali or alkaline earth sulfates on the hydration of cubic tricalcium aluminate (C 3 A) were evaluated by in situ dissolution rate measurements, by ex situ near-surface composition measurements with secondary ion mass spectrometry, and by in situ synchrotron X-ray diffraction to monitor precipitation of hydration products. Both slight reductions in dissolution rate and cation-specific interactions with the solid were observed. The near-surface Ca/Al ratio is significantly lower after some dissolution and the electrolyte cations are incorporated within the surface with different affinities (Mg 2+ > K + > Na + ). An interfacial dissolution-reprecipitation mechanism may explain the observations as well as, or better than, a simple cation exchange. The sulfate concentration in solution affects the rates of both C 3 A dissolution and precipitation of hydration products. Aditionally, sulfate ions likely adsorb at the hydrous Al-rich surface layer, thereby reducing the dissolution rate of aluminates and delaying the precipitation of aluminate hydration products.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Carbon Mineralization of Sulfate Wastes Containing Pb: Synchrotron Pb M3-Edge XANES Analysis of Simultaneous Heavy Metal and Carbon Sequestration

Sulfate wastes are produced in large quantities and contain toxic heavy metals such as lead (Pb), posing environmental risks. Because of favorable solubility differences, these wastes can be repurposed for engineered carbon dioxide (CO 2 ) sequestration. Understanding the fate and mobility of heavy metals during this process is important. This study focuses on Pb and the effect of zinc (Zn) on Pb in carbon mineralization. Synthesized gypsum was treated with a carbonate-rich solution at pH 11.5 to convert the sulfates to carbonates. Aqueous solutions and mineral solids were analyzed. Synchrotron-based micro-X-ray fluorescence and a novel application of Pb M3-edge X-ray absorption near-edge structure provided detailed insights into Pb distribution and mineral forms. Results showed significant reductions in aqueous Pb and Zn concentrations, indicating effective metal sequestration. Carbon mineralization transformed Pb from soluble anglesite (PbSO 4 ) into insoluble cerussite (PbCO 3 ) and hydrocerussite (Pb 3 (CO 3 ) 2 (OH) 2 ). Pb primarily precipitated onto calcium carbonate surfaces through surface-mediated precipitation reactions. While the presence of Zn modified crystallization dynamics, it did not impede Pb sequestration and potentially enhanced surface reactivity, facilitating greater Pb immobilization. These findings highlight carbon mineralization as a sustainable approach to immobilize toxic metals in sulfate wastes while advancing CO 2 sequestration efforts.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Metal–Oxo Cluster Formation Using Ammonium and Sulfate to Differentiate M IV (Th, U, Ce) Chemistries

Isolating isostructural compounds of tetravalent metals M IV (Zr, Hf, Ce, Th, U, Pu, Np) improves our understanding of metal hydrolysis and coordination behavior across the periodic table. These metals form polynuclear clusters typified by the hexamer [M IV 6 O 4 (OH) 4 ] 12+ . Exploiting the ammonium M IV -sulfate (Ce IV , Th IV , and U IV ) phase space targeting rapid crystallization, we isolate the common hexamer [M IV 6 (OH) 4 (O) 4 ] 12+ but with different numbers of capping sulfates and water molecules for Ce IV , Th IV , and U IV . Furthermore, these phases allowed a direct comparison of bonding trends across the series. Upon cocrystallization with the hexamers, higher complex structures can be identified. Thorium features assemblies with monomer-linked hexamer chains. Uranium features assemblies with sulfate-bridged hexamers and the supramolecular assembly of 14 hexamers into the U 84 , [U 6 (OH) 4 (O) 4 ) 14 (SO 4 ) 120 (H 2 O) 42 ] 72– . Last, cerium showcases the isolation from monomers to the Ce 62 , [Ce 62 (OH) 30 (O) 58 (SO 4 ) 71 (H 2 O) 33.25 ] 41– . Furthermore, small-angle X-ray scattering (room temperature) shows ammonium-induced cluster assembly for Ce IV but minimal reactivity for U IV and Th IV . In this study, because the phases crystallized at elevated temperature demonstrates favorable cluster assembly, these solution phase results were surprising and suggest some other characteristics such as Ce’s facile redox behavior, contributes to its solution-phase speciation.

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

Cu(II) Stability and UV-Induced Electron Transfer in a Metal–Organic Hybrid: An EPR, DFT, and Crystallographic Characterization of Copper-Doped Zinc Creatininium Sulfate

Single-crystal X-ray diffraction and electron paramagnetic resonance (EPR) spectroscopic experiments, complemented by quantum chemical DFT calculations, were carried out on the copper-doped metal–organic hybrid and Tutton salt analogue zinc creatininium sulfate to determine its crystal structure, to characterize the electronic structure of the doped Cu(II) binding site, and to propose a pathway for an excited-state, proton-coupled electron transfer (PCET) process in UV-exposed crystals. The crystal structure is isomorphous to that of cadmium creatininium sulfate, which has the transition ion, not in direct coordination with the creatinine, but forming a hexahydrate complex, which is bridged to a creatininium through an intervening sulfate ion. The EPR g (2.446, 2.112, 2.082) and copper hyperfine (A Cu : -327, -59.6, 10.8 MHz) tensor parameters are consistent with doped copper replacing host zinc in the metal–hexahydrate complex. These parameters are similar to those observed for copper hexahydrate in doped Tutton salt systems at low temperature, where the unpaired electron occupies mainly the copper 3d x 2 –y 2 orbital. At room temperature in the Tutton systems, vibration couplings stemming from a dynamic Jahn–Teller effect cause tensor averaging which results in a reduction in their maximum g-tensor and hyperfine tensor values. However, like for the doped isomorphous Cd creatinine crystal, the Cu(II) EPR exhibits little, or no room temperature averaging compared to its low temperature pattern. Samples exposed to 254 nm UV light generate a carbon-centered free radical species, characterized by an isotropic g-tensor (g = 2.0029) and an alpha-proton hyperfine coupling (-24 -14 +4 G). These parameters identify it as a creatinine radical cation formed by the oxidative release of one of its C2 methylene hydrogens. DFT calculations confirm the unpaired electronic structures of both the Cu(II) site and free radical. The growth in radical concentration with an increase in the UV exposure time coincides with a decrease in the copper EPR signal, indicating a coupled light-induced oxidation reduction process. A comparison of the crystal structure with the EPR parameters and DFT results provides evidence for a UV-induced PCET.

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

Increased Asian Sulfate Aerosol Emissions Remarkably Enhance Sahel Summer Precipitation

Observational evidence shows that Sahel summer precipitation has experienced a considerable increase since the 1980s, coinciding with significant diverging trends of increased sulfate emissions in Asia and decreased emissions in Europe (dipole pattern of aerosols between Asia and Europe). The decrease in European sulfate aerosols has substantial effects on the Sahel summer precipitation increase, but the corresponding effect of increased Asian sulfate is unknown. Multi-model simulations in the Precipitation Driver and Response Model Intercomparison Project (PDRMIP) show, compared to decreased European aerosols, that increased Asian aerosols similarly enhance the Sahel summer precipitation but with different large-scale atmospheric circulation changes. Further analysis of the Sixth Coupled Model Intercomparison Project (CMIP6) simulations under historical attribution and various emission scenarios reinforces the results about the climate impacts of anthropogenic aerosols and suggests that in future scenarios with strong international cooperation and rapid climate mitigations (SSP2-45), the Sahel drought will be intensified likely due to the decline in Asian aerosol emissions. Our results suggest that Asian anthropogenic aerosols are likely a non-negligible driver of the recent recovery in Sahel precipitation amounts

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Subsurface hydrocarbon degradation strategies in low- and high-sulfate coal seam communities identified with activity-based metagenomics

Environmentally relevant metagenomes and BONCAT-FACS derived translationally active metagenomes from Powder River Basin coal seams were investigated to elucidate potential genes and functional groups involved in hydrocarbon degradation to methane in coal seams with high- and low-sulfate levels. An advanced subsurface environmental sampler allowed the establishment of coal-associated microbial communities under in situ conditions for metagenomic analyses from environmental and translationally active populations. Metagenomic sequencing demonstrated that biosurfactants, aerobic dioxygenases, and anaerobic phenol degradation pathways were present in active populations across the sampled coal seams. In particular, results suggested the importance of anaerobic degradation pathways under high-sulfate conditions with an emphasis on fumarate addition. Under low-sulfate conditions, a mixture of both aerobic and anaerobic pathways was observed but with a predominance of aerobic dioxygenases. The putative low-molecular-weight biosurfactant, lichysein, appeared to play a more important role compared to rhamnolipids. The methods used in this study—subsurface environmental samplers in combination with metagenomic sequencing of both total and translationally active metagenomes—offer a deeper and environmentally relevant perspective on community genetic potential from coal seams poised at different redox conditions broadening the understanding of degradation strategies for subsurface carbon.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2022

Anthropogenic sulfate aerosol pollution in South and East Asia induces increased summer precipitation over arid Central Asia

Precipitation has increased across the arid Central Asia region over recent decades. However, the underlying mechanisms of this trend are poorly understood. Here, we analyze multi-model simulations from the Precipitation Driver and Response Model Intercomparison Project (PDRMIP) to investigate potential drivers of the observed precipitation trend. We find that anthropogenic sulfate aerosols over remote polluted regions in South and East Asia lead to increased summer precipitation, especially convective and extreme precipitation, in arid Central Asia. Elevated concentrations of sulfate aerosols over remote polluted Asia cause an equatorward shift of the Asian Westerly Jet Stream through a fast response to cooling of the local atmosphere at mid-latitudes. This shift favours moisture supply from low-latitudes and moisture flux convergence over arid Central Asia, which is confirmed by a moisture budget analysis. High levels of absorbing black carbon lead to opposing changes in the Asian Westerly Jet Stream and reduced local precipitation, which can mask the impact of sulfate aerosols. This teleconnection between arid Central Asia precipitation and anthropogenic aerosols in remote Asian polluted regions highlights long-range impacts of anthropogenic aerosols on atmospheric circulations and the hydrological cycle.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Anthropogenic sulfate-climate interactions suppress dust activity over East Asia

Observational evidences indicate a significant decline in dust storm frequencies over the East Asian arid-semiarid region during recent decades, which creates a strong contrast with a great increase in sulfate emissions over monsoonal Asia. However, the causes for decline of dust activities are still controversial. Through conducting a set of idealized sensitivity experiments of regional aerosol perturbations, here we show that anthropogenic sulfate aerosols over monsoonal Asia remarkably suppress the regional dust activities over East Asia. Southward shift of Asian westerly jet stream induced by sulfate aerosols results in increasing precipitation and weakening surface wind speeds over the arid-semiarid region, thereby suppressing local dust emission fluxes. Further, the latest Sixth Coupled Model Intercomparison Project simulations indicate that anthropogenic aerosols partly drive the recent weakening in regional dust activities and that future change of regional dust activities will likely depend on emissions scenarios of Asian anthropogenic aerosols and greenhouse gases.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Bis[squaramido]ferrocenes as electrochemical sulfate receptors

1,1′-Bis[squaramido]ferrocenes (FcSq 2 ) are introduced as electrochemically active scaffolds for sulfate recognition. FcSq 2 display high sulfate-binding affinity and selectivity in aqueous DMSO mixtures. Among tested anions, sulfate elicits a unique electrochemical response in FcSq 2 , enabling selective detection.

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

Laminarin stimulates single cell rates of sulfate reduction whereas oxygen inhibits transcriptomic activity in coastal marine sediment

Abstract The chemical cycles carried out by bacteria and archaea living in coastal sediments are vital aspects of benthic ecology. These ecosystems are subject to physical disruption, which may allow for increased respiration and complex carbon consumption—impacting chemical cycling in this environment often thought to be a terminal place of deposition. We use the redox-enzyme sensitive probe RedoxSensor Green to measure rates of electron transfer physiology in individual sulfate reducer cells residing in anoxic sediment, subjected to transient exposure of oxygen and laminarin. We use index fluorescence activated cell sorting and single cell genomics sequencing to link those measurements to genomes of respiring cells. We measure per-cell sulfate reduction rates in marine sediments (0.01–4.7 fmol SO42− cell−1 h−1) and determine that cells within the Chloroflexota phylum are the most active in respiration. Chloroflexota respiration activity is also stimulated with the addition of laminarin, even in marine sediments already rich in organic matter. Evaluating metatranscriptomic data alongside this respiration-based technique, Chloroflexota genomes encode laminarinases indicating a likely ability to degrade laminarin. We also provide evidence that abundant Patescibacteria cells do not use electron transport pathways for energy, and instead likely carry out fermentation of polysaccharides. There is a decoupling of respiration-related activity rates from transcription, as respiration rates increase while transcription decreases with oxygen exposure. Overall, we reveal an active community of respiring Chloroflexota that cycles sulfate at potential rates of 23–40 nmol h−1 per cm3 sediment in incubation settings, and non-respiratory Patescibacteria that can cycle complex polysaccharides.

Lindsay, Melody R.↗
DOE OSTI2020

Conversion of Uranium Metal to Uranyl Sulfate Solution

Experiments involving conversion of uranium (U) metal to U 3 O 8 , followed by dissolution to form uranyl sulfate solution, were performed with batches of up to 300 g of U metal. The focus was to identify major U species formed during the oxidation process, determine the particle size distribution of the uranium oxide product, and identify the size of the dissolution vessel needed to accommodate the exothermic reaction during the conversion of U 3 O 8 to uranyl sulfate using 30% hydrogen peroxide and H 2 SO 4 . The information obtained in this study will be used for designing full-scale processes to convert kilogram quantities of U metal to uranyl sulfate solution with a concentration of 300 g U/L.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2025

Development of Calcined Clay/Calcium Sulfate Blends for Robust Performance of LC3 Concrete

This report documents the development of robust blends of calcined clays (CCs) with calcium sulfate (gypsum) for application in limestone calcined clay cement (LC3) systems. The U.S. cement industry faces supply chain constraints and high energy intensity, motivating the need for alternative supplementary cementitious materials. Calcined clays are abundant and highly reactive when properly processed, but their variable physical and chemical characteristics can negatively impact hydration balance, rheology, and admixture demand in LC3 concretes. To address this, five calcined clays, two Portland cements, ground limestone, gypsum, and a polycarboxylate dispersant were procured. Isothermal calorimetry and mini-cone flow tests were used to determine sulfate and dispersant demand. Results show that the addition of approximately 6.7% gypsum, relative to the calcined clay weight, consistently balanced sulfate consumption across the LC3 systems studied. Dispersant demand, however, varied significantly with clay source, demonstrating the need for tailored admixture strategies. These findings confirm that supplying CC–gypsum blends directly to concrete producers is a viable approach to overcoming current manufacturing constraints, enabling reliable fresh and hardened performance of LC3 concretes, and supporting broader adoption of calcined clays in the U.S. market.

36 MATERIALS SCIENCE↗
DOE OSTI2020

On Aerosol Liquid Water and Sulfate Associations: The Potential for Fine Particulate Matter Biases

In humid locations of the Eastern U.S., sulfate is a surrogate for aerosol liquid water (ALW), a poorly measured particle constituent. Regional and seasonal variation in ALW–sulfate relationships offers a potential explanation to reconcile epidemiology and toxicology studies regarding particulate sulfur and health endpoints. ALW facilitates transfer of polar species from the gas phase to the particle phase and affects particle pH and metal oxidation state. Though abundant and a potential indicator of adverse health endpoints, ALW is largely removed in most particulate matter measurement techniques, including in routine particulate matter (PM 2.5 ) networks that use federal reference method (FRM) monitors, which are used in epidemiology studies. We find that in 2004, a typical year in the available record, ambient ALW mass is removed during sampling and filter equilibration to standard laboratory conditions at most (94%) sites, up to 85% of the ambient water mass. The removal of ALW can induce the evaporation of other semi-volatile compounds present in PM 2.5 , such as ammonium nitrate and numerous organics. This produces an artifact in the PM mass measurements that is, importantly, not uniform in space or time. This suggests that PM 2.5 epidemiology studies that exclude ALW are biased. This work provides a plausible explanation to resolve multi-decade discrepancies regarding ambient sulfate and health impacts in some epidemiological and toxicological studies

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

An approach to sulfate geoengineering with surface emissions of carbonyl sulfide

Sulfate geoengineering (SG) methods based on lower stratospheric tropical injection of sulfur dioxide (SO 2 ) have been widely discussed in recent years, focusing on the direct and indirect effects they would have on the climate system. Here a potential alternative method is discussed, where sulfur emissions are located at the surface or in the troposphere in the form of carbonyl sulfide (COS) gas. There are two time-dependent chemistry–climate model experiments designed from the years 2021 to 2055, assuming a 40 Tg-Syr -1 artificial global flux of COS, which is geographically distributed following the present-day anthropogenic COS surface emissions (SG-COS-SRF) or a 6 Tg-Syr -1 injection of COS in the tropical upper troposphere (SG-COS-TTL). The budget of COS and sulfur species is discussed, as are the effects of both SG-COS strategies on the stratospheric sulfate aerosol optical depth (~Δτ=0.080 in the years 2046–2055), aerosol effective radius (0.46 µm), surface SO x deposition (+8.9 % for SG-COS-SRF; +3.3 % for SG-COS-TTL), and tropopause radiative forcing (RF; ~-1.5 W m –2 in all-sky conditions in both SG-COS experiments). Indirect effects on ozone, methane and stratospheric water vapour are also considered, along with the COS direct contribution. According to our model results, the resulting net RF is –1.3 W m –2 , for SG-COS-SRF, and –1.5 W m –2 , for SG-COS-TTL, and it is comparable to the corresponding RF of –1.7 W m –2 obtained with a sustained injection of 4 Tg-Syr -1 in the tropical lower stratosphere in the form of SO 2 (SG-SO2, which is able to produce a comparable increase of the sulfate aerosol optical depth). Significant changes in the stratospheric ozone response are found in both SG-COS experiments with respect to SG-SO2 (~5 DU versus +1.4 DU globally). According to the model results, the resulting ultraviolet B (UVB) perturbation at the surface accounts for –4.3 % as a global and annual average (versus –2.4 % in the SG-SO2 case), with a springtime Antarctic decrease of –2.7 % (versus a +5.8 % increase in the SG-SO2 experiment). Overall, we find that an increase in COS emissions may be feasible and produce a more latitudinally uniform forcing without the need for the deployment of stratospheric aircraft. However, our assumption that the rate of COS uptake by soils and plants does not vary with increasing COS concentrations will need to be investigated in future work, and more studies are needed on the prolonged exposure effects to higher COS values in humans and ecosystems.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Understanding the Role of Zinc Hydroxide Sulfate and its Analogues in Mildly Acidic Aqueous Zinc Batteries: A Review

Abstract Mildly acidic aqueous zinc batteries (AZBs) have attracted tremendous attention for grid storage applications with the expectation to tackle the issues of Li‐ion batteries on high cost and poor safety. However, the performance, particularly energy density and cycle stability of AZBs are still unsatisfactory when compared with LIBs. To help the development of AZBs, a lot of effort have been made to understand the battery reaction mechanisms and precedent microscopic and spectroscopic analyses have shown flake‐like large particles of zinc hydroxide sulfate (ZHS) and its analogues formed on the surfaces of cathodes and anodes in sulfate and other electrolyte systems during cycling. However, because of the complexity of the thermodynamics and kinetics of aqueous reactions to understand different battery conditions, controversies still exist. This article will review the roles of ZHS discussed in recent representative references aiming to shine light on the fundamental mechanisms of AZBs and pave ways to further improve the battery performance.

25 ENERGY STORAGE↗
DOE OSTI2021

On the competitive antagonism effect in combined chloride-sulfate attack: A numerical exploration

Highlights: • A chemo-physical-mechanical method based on thermodynamic modelling is implemented. • The contradicting findings from reported experiments are numerically explored. • The competitive antagonism effect is time-dependent rather than a conclusive term. • The competitive antagonism effect is quantifiable with a novel assessment criterion. It is of tremendous difficulty to draw a conclusive verdict on the complex process of mutual interference regarding the combined chloride-sulfate attack on concrete, where many have explored the topic, but contradicting results have been reported. In this paper, by taking advantages of the chemo-physical-mechanical method, based on the robust technique of thermodynamic modelling, the competitive antagonism effect in combined chloride-sulfate attack is investigated. Firstly, a range of reported tests are numerically modelled to demonstrate the effectiveness of the employed method in interpreting those opposing and diverse experimental outcomes. More importantly, a fresh conjecture incorporating a novel assessment criterion for the competitive antagonism effect is proposed and supported through a carefully designed illustrative example. Based on the numerical exploration, unique findings and implications for future engineering practices are revealed.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Options for the Removal of Cesium and Strontium from Acidic Uranyl Sulfate Solutions from Molybdenum-99 Production

A small laboratory-scale column process aimed at removing fission products from prototypical acidic sulfate solution wastes from a prototypical Mo-99 recovery process has been operated in a radioactive materials hood at Savannah River National Laboratory. This equipment has been operated with realistic concentrations of uranium (0.4 wt % 235 U), plutonium ( 239 Pu), neptunium ( 237 Np), non-radioactive surrogates of common fission products (including Cs and Sr) and two promising absorbents AMP-PAN and CST R91290-B. The goal of this work was to demonstrate the removal and concentration of high specific activity isotopes which are expected to dominate the classification of the low-level waste from the production of 99 Mo. Both AMP-PAN and CST R9120-B are attractive absorbents for the removal of 137 Cs from an acidic sulfate waste stream. They do not provide a solution for the removal of 90 Sr from the acidic solutions, but CST should be investigated at a higher pH. Limited removal of transuranic species and almost no removal of uranium was observed in this testing. This could be important due to the relatively large amount of uranium expected to be present in such waste streams. The capacity of these absorbents for 137 Cs will likely be dependent on the Cs concentration in the solutions processed but loading in the range of 0.2 to 5 mg Cs per gram of absorbent appears to be achievable.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗