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At least 613 records · Page 34
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Methanol adsorption and dissociation on GaP(110) studied by ambient pressure X-ray photoelectron spectroscopy

Ambient pressure X-ray photoelectron spectroscopy (AP-XPS) was used to investigate methanol (CH 3 OH) adsorption and reaction on the GaP(110) surface. Exposure of CH 3 OH to GaP(110) at room temperature led to the formation of at least four different surface species as indicated by analysis of C 1s and O 1s XPS features. By combining AP-XPS data with density functional theory calculations, the surface species were identified as methoxy (CH 3 O*), formaldehyde (CH 2 O*), and paired methanol (p-CH 3 O*H) and methoxy (p-CH 3 O*) species, where “paired” means that they belong to a hydrogen-bonded methoxy-methanol complex. Asterisk * here indicates an adsite. The formation of CH 2 O* via the dehydrogenation of CH 3 O* was shown to be limited by the availability of vacant phosphorus (P) sites on GaP(110). With an increase in CH 3 OH pressure, the fractional coverage of CH 3 O* species reached 0.55, and the surface P sites were completely saturated with hydrogen. Under a constant CH 3 OH pressure of 0.5 Torr, the surface concentration of the paired species and of CH 2 O* remained constant until 400 K. At higher temperatures, thermally driven reactions led to a significant increase in the concentration of surface CH x * species, which suggests that C-O bond cleavage of the CH 3 O group is the dominant decomposition mechanism on GaP(110). In conclusion, based on the reactivity of GaP(110) toward CH 3 OH dehydrogenation, elevated temperatures and CH 3 OH pressures may be used to functionalize this surface.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Mineral nutrient signaling controls photosynthesis: focus on iron deficiency-induced chlorosis

Photosynthetic organisms convert light energy into chemical energy stored in carbohydrates. To perform this process, an adequate supply of essential mineral elements, such as iron, is required in the chloroplast. Because iron plays a crucial role during electron transport and chlorophyll formation, iron deficiency alters photosynthesis and promotes chlorosis, or the yellowing of leaves. Intriguingly, iron deficiency-induced chlorosis can be reverted by the depletion of other micronutrients [i.e., manganese (Mn)] or macronutrients [i.e., sulfur (S) or phosphorus (P)], raising the question of how plants integrate nutrient status to control photosynthesis. Here, in this work, we review how improving our understanding of the complex relationship between nutrient homeostasis and photosynthesis has great potential for crop improvement.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2023

Detailed investigation of electrical and optical properties of textured n-type and roughened p-type tunnel oxide passivated contacts for screen-printed double-side passivated contact silicon solar cell application

Here, this paper presents detailed characterization and analyses of the optical, electrical, and contact properties of a 35 nm phosphorus-doped (n-type) polysilicon (poly-Si) and a 250 nm boron-doped (p-type) poly-Si deposited respectively on textured and roughed surface. These layers could be applied respectively to the front and rear sides of an n-type Si to produce back junction bifacial screen-printed double-side tunnel oxide passivated contacts (DS-TOPCon) solar cells. Optical and device modeling revealed a short circuit current density loss of 1.5 mA/cm 2 and 0.5 mA/cm 2 due to absorption in the front n-TOPCon and rear side p-TOPCon layers, respectively. The passivation and contact properties including metalized and unmetallized recombination current density (J 0 ), as well as contact resistivity, were determined as a function of contact firing temperature in the range of 700~800°C. The passivation quality of the front thin n-TOPCon was found to deteriorate with increased firing temperature while the rear thick p-TOPCon improved. The study showed that the simulated contact firing at 730°C resulted in the best unmetallized double-side TOPCon precursor, with an excellent implied open-circuit voltage of 730 mV and implied fill factor of ~86 %. However, the metalized J0 increased and contact resistivity decreased monotonically with the increase in the firing temperature. The 2D device simulations revealed that these layers can produce screen-printed DS-TOPCon cells with an efficiency of ~22.5 %. Solar cell modeling also showed that the DS-TOPCon solar cell efficiency can reach 24.1 % by decreasing the n-TOPCon thickness to 20 nm and lowering the full area metalized J 0 to ~100 mA/cm 2 .

14 SOLAR ENERGY↗
DOE OSTI2022

A novel sub-pilot-scale direct-contact ultrasonic dehydration technology for sustainable production of distillers dried grains (DDG)

DDG is a major source of protein, calcium, phosphorus, and sulfur is arguably the most important byproduct of the bioethanol industry with increasing demand over the past few years. Reducing energy consumption in the DDG production process and energy recovery from DDG is vital for sustainable bioethanol productions. In this paper, a novel direct-contact multi-frequency, multimode, and modulated (MMM) ultrasonic dryer (US) was developed for the first time and has been applied in dehydration of wet distillers' grain (WDG). Ultrasonic drying (US) was combined with a convective airflow (HA) at different temperatures of 25 (room temperature), 50 and 70 °C to evaluate the impact of US, HA, and US + HA on drying kinetics, activation energy, chemical compositions, microstructure, and color of DDG. Semi-empirical kinetic models were developed and evaluating drying performances showed that the application of ultrasound significantly enhanced the drying rate and decreased the drying time (by 46%), especially at low drying temperatures. The activation energy for moisture removal in the presence of ultrasound was about 50% of that without ultrasound. The final dried distillers' grains product processed by ultrasonic drying had a brighter color, a higher available protein, a higher digestible protein (the lowest acid detergent insoluble crude protein), and a better surface profile with no compromise on minerals and fiber contents.

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

Electro-assisted regeneration of pH-sensitive ion exchangers for sustainable phosphate removal and recovery

Removal and recovery of phosphate from wastewater can minimize deleterious environmental impacts and supplement fertilizer supply. Hybrid anion exchangers (HAIX, with doped ferric oxide nanoparticles (FeOnp)) can remove phosphate from complex wastewaters and recover concentrated phosphate solutions. Here, we integrate HAIX with a weak acid cation exchanger (WAC) to enrich phosphate and calcium in mild regenerants and precipitate both elements for recovery. We demonstrated an electro-assisted regeneration approach to avoid strong acid and base input. Based on demonstrated pH sensitivities of both materials, electrochemically produced mild electrolytes (pH 3 and pH 11), which are 100–1000 times less concentrated than typical regenerants, preserved 80% WAC and 50% HAIX capacities over five batch adsorption-regeneration cycles. FeOnp in HAIX facilitated regeneration due to pH sensitivity and their likely distribution on the resin particle surface, which reduced intraparticle diffusion path length. In column tests, repeatable phosphate removal (> 95%) from synthetic wastewater (3 mg P/L) was achieved with 20 kWh/kg P specific energy consumption. After removal, a similar 50% HAIX regeneration efficiency as batch experiments was achieved. In spent regenerant, more than 95% phosphorus was recovered as hydroxyapatite. This novel approach enhances ion exchange by minimizing chemical inputs.

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

Interactions between phosphate and arsenic in iron/biochar-treated groundwater: Corrosion control insights from column experiments

An increasing number of studies have reported the coexistence of arsenic (As) and phosphorus at high concentrations in groundwater, which threatens human health and increases the complexity of groundwater remediation. However, limited work has been done regarding As interception in the presence of phosphate in flowing systems. In this study, a series of experiments were conducted to evaluate the interactions between phosphate and As during As removal by iron (Fe)-based biochar (FeBC). The addition of phosphate promoted As removal by FeBC in the batch and column experiments. X-ray absorption near edge structure (XANES) analysis provided evidence of simultaneous oxidation and reduction of trivalent arsenic in the FeBC column experiment, accompanied by corrosive Fe oxidation. However, the addition of phosphate enhanced As stabilization, attributed to the As-incorporated Fe-Ca-phosphates precipitates. The involvement of phosphate decelerated the Fe corrosion and the formation of secondary minerals in the column, mediating the risk of passivation and clogging. The As retained by Fe-Ca-phosphate precipitates was more readily oxidized, resulting in higher proportions of pentavalent arsenic. In conclusion, the results of this work identify the corrosion control and sustained-release roles of phosphate in FeBC application, informing the perspective of FeBC in As-contaminated groundwater remediation and providing new insights into the interactions between phosphate and As.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Improvised Field Expedient Method for Renal Replacement Therapy in a Porcine Model of Acute Kidney Injury

ABSTRACT Objective: Dialysis patients may not have access to conventional renal replacement therapy (RRT) following disasters. We hypothesized that improvised renal replacement therapy (ImpRRT) would be comparable to continuous renal replacement therapy (CRRT) in a porcine acute kidney injury model. Methods: Following bilateral nephrectomies and 2 hours of caudal aortic occlusion, 12 pigs were randomized to 4 hours of ImpRRT or CRRT. In the ImpRRT group, blood was circulated through a dialysis filter using a rapid infuser to collect the ultrafiltrate. Improvised replacement fluid, made with stock solutions, was infused pre-pump. In the CRRT group, commercial replacement fluid was used. During RRT, animals received isotonic crystalloids and norepinephrine. Results: There were no differences in serum creatinine, calcium, magnesium, or phosphorus concentrations. While there was a difference between groups in serum potassium concentration over time ( P < 0.001), significance was lost in pairwise comparison at specific time points. Replacement fluids or ultrafiltrate flows did not differ between groups. There were no differences in lactate concentration, isotonic crystalloid requirement, or norepinephrine doses. No difference was found in electrolyte concentrations between the commercial and improvised replacement solutions. Conclusion: The ImpRRT system achieved similar performance to CRRT and may represent a potential option for temporary RRT following disasters.

Public, Environmental & Occupational Health↗
DOE OSTI2022

Molecular Characterization of Organophosphorus Compounds in Wildfire Smoke Using 21-T Fourier Transform-Ion Cyclotron Resonance Mass Spectrometry

Here, we present a detailed molecular characterization of organophosphorus compounds in ambient organic aerosol influenced by wildfire smoke. Biomass burning organic aerosol (BBOA) is an important source of phosphorus (P) to surface waters, where even a small imbalance in the P flux can lead to substantial effects on water quality, such as eutrophication, algal blooms, and oxygen depletion. We aimed to exploit the ultrahigh resolving power, mass accuracy, and sensitivity of Fourier transform-ion cyclotron resonance mass spectrometry (FT-ICR MS) to explore the molecular composition of an ambient BBOA sample collected downwind of Pacific Northwest wildfires. The 21-T FT-ICR MS yielded 10533 distinct formulae, which included molecular species comprising C, H, O, and P with or without N, i.e., organophosphorus compounds that have long been quantified in wildfire smoke but have not yet been characterized at the molecular level. The lack of detailed molecular characterization of organophosphorus compounds in BBOA is primarily due to their inherently low concentrations in aerosols and poor ionization efficiency in complex mixtures. We demonstrate that the exceptional sensitivity of the 21-T FT-ICR MS allows qualitative analysis of a previously uncharacterized fraction of BBOA without its selective concentration from the organic matrix, exemplifying the need for ultrahigh-resolution tools for a more detailed and accurate molecular depiction of such complex mixtures.

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

Recycling of Nutrients from Dairy Wastewater by Extremophilic Microalgae with High Ammonia Tolerance

This study explored the possibility of incorporating extremophilic algal cultivation into dairy wastewater treatment by characterizing a unique algal strain. Results showed that extremophilic microalgae Chlorella vulgaris CA1 newly isolated from dairy wastewater tolerated a high level of ammonia nitrogen (2.7 g/L), which was over 20 times the ammonia nitrogen that regular Chlorella sp. could tolerate. The isolate was mixotrophically cultured in dairy effluent treated by anaerobic digestion (AD) for recycling nutrients and polishing the wastewater. The highest biomass content of 13.3 g/L and protein content of 43.4% were achieved in the culture in AD effluent. Up to 96% of the total nitrogen and 79% of the total phosphorus were removed from the dairy AD effluent. The ability of the algae to tolerate a high level of ammonia nitrogen suggests the potential for direct nutrient recycling from dairy wastewater while producing algal biomass and high value bioproducts.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Adsorption Mechanisms of Glyphosate on Ferrihydrite: Effects of Al Substitution and Aggregation State

Ferrihydrite is one of the most reactive iron (Fe) (oxyhydr)oxides in soils, but the adsorption mechanisms of glyphosate, the most widely used herbicide, on ferrihydrite remain unknown. Here, we determined the adsorption mechanisms of glyphosate on pristine and Al-substituted ferrihydrites with aggregated and dispersed states using macroscopic adsorption experiments, zeta potential, phosphorus K-edge X-ray absorption near-edge structure spectroscopy, in situ attenuated total reflectance Fourier transform infrared spectroscopy coupled with two-dimensional correlation spectroscopy, and multivariate curve resolution analyses. Aggregation of ferrihydrite decreases the glyphosate adsorption capacity. The partial substitution of Al in ferrihydrite inhibits glyphosate adsorption on aggregated ferrihydrite due to the decrease of external specific surface area, while it promotes glyphosate adsorption on dispersed ferrihydrite, which is ascribed to the increase of surface positive charge. Glyphosate predominately forms protonated and deprotonated, depending on the sorption pH, monodentate-mononuclear complexes (MMH 1 /MMH 0 , 77-90%) on ferrihydrites, besides minor deprotonated bidentate-binuclear complexes (BBH 0 , 23-10%). Both Al incorporation and a low pH favor the formation of the BB complex. The adsorbed glyphosate preferentially forms the MM complex on ferrihydrite and preferentially bonds with the Al-OH sites on Al-substituted ferrihydrite. In conclusion, these new insights are expected to be useful in predicting the environmental fate of glyphosate in ferrihydrite-rich environments.

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

Speciation and Aqueous Dissolution of Macronutrients in Fire Ash: Variation across Ecosystems and the Effects on Nutrient Cycling

This study investigated the speciation and aqueous dissolution of macronutrients in fire ash from diverse ecosystems and speciation of ash and smoke from laboratory burning, exploring the variations and their causes. The speciation of phosphorus (P), calcium (Ca), and potassium (K) in fire ash from five globally distributed ecosystems was characterized by using X-ray absorption spectroscopy and sequential fractionation. Aqueous dissolution of the macronutrients was measured by batch experiments at acidic and alkaline pHs. The results showed that P existed mainly as Ca phosphates, Ca as double carbonates, calcite, and sulfates, and most K was associated with Ca carbonates. Mineralogy and the relative abundance of the species were primarily controlled by elemental stoichiometry and fire temperature. Differences in Ca and P speciation existed between ash and smoke from laboratory burning, possibly caused by the temperature difference and/or mass fractionation during burning. The rates, extents, and pH dependencies of macronutrient dissolution differed among macronutrients and depended on their speciation, with K being highly soluble and the P and Ca regulated by solution pH. The variability in ash macronutrient chemistry and ecosystemspecific fire ash loads resulted in varying loads and availability of individual macronutrient from fire among ecosystems. This study provides a mechanistic understanding of how fires transform the chemistry of macronutrients and affect macronutrient returns to soils across different ecosystems, which is essential for evaluating the disturbance to ecosystem nutrient cycling by fires.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Ion Clusters Reveal the Sources, Impacts, and Drivers of Freshwater Salinization

Population growth, land use change, climate change, and natural resource extraction are driving the salinization of freshwater resources worldwide. Reversing these trends will require data-centric approaches that identify salt sources, environmental drivers, and ecosystem responses. In this study, we applied principal component analysis and hierarchical clustering to identify ion covariance patterns, or “ion clusters,” in Broad Run, an urban stream in the Mid-Atlantic United States. These clusters correspond to distinct hydrologic regimes and reveal specific salinization risks: (1) phosphorus pollution mobilized during summer storms (Cluster 1); (2) elevated concentrations of sulfate and bicarbonate during baseflow (Cluster 2), likely reflecting groundwater discharge; and (3) elevated specific conductance and sodium, chloride, and potassium ion concentrations during snowmelt and rain-on-snow events (Cluster 3), driven by deicer and anti-icer wash-off. These ion fingerprints offer a transferable framework for diagnosing salt sources, assessing ecological risk, and identifying management targets. Our findings underscore the need for next-generation stormwater infrastructure and smart growth policies to protect aquatic life in rapidly urbanizing watersheds.

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

The Effect of Core-Hole Shape on Attosecond Valence Electron Dynamics

Rapid X-ray ionization of a core electron is known to induce the attosecond motion of valence electrons; however, the effect of core-hole shape on the triggered dynamics remains relatively unknown. In this work, the sub-four fs response of prototypical functionalized/heterocyclic/polycyclic molecules was simulated using real-time time-dependent density functional theory (RT-TDDFT), a sudden approximation core-hole, and phenomenologically Auger–Meitner (AM) decay. These molecules included fluorobenzene, chlorobenzene, bromobenzene, phenol, thiophenol, pyridine, phosphorus, and azulene. It is observed that the valence electron dynamics are essentially independent of the core-hole created, provided that it is ionized from an inner-shell orbital and not an inner-valence orbital. This has broad implications for free-electron laser studies of X-ray pumped attosecond processes since the flexibility in edge allows for a wide range of experimental modalities, core-holes with longer AM lifetimes, and molecular targets.

aromatic compounds↗
DOE OSTI2023

Quantifying the Variation in the Number of Donors in Quantum Dots Created Using Atomic Precision Advanced Manufacturing

Atomic-precision advanced manufacturing enables unique silicon quantum electronics built on quantum dots fabricated from small numbers of phosphorus dopants. The number of dopant atoms comprising a dot plays a central role in determining the behavior of charge and spin confined to the dots and thus overall device performance. Here in this work, we use both theoretical and experimental techniques to explore the combined impact of lithographic variation and stochastic kinetics on the number of P incorporations in quantum dots made using these techniques and how this variation changes as a function of the size of the dot. Using a kinetic model of PH3 dissociation augmented with novel reaction barriers, we demonstrate that for a 2 × 3 silicon dimer window the probability that no donor incorporates goes to zero, allowing for certainty in the placement of at least one donor. However, this still comes with some uncertainty in the precise number of incorporated donors (either one or two), and this variability may still impact certain applications. We also examine the impact of the size of the initial lithographic window, finding that the incorporation fraction saturates to δ-layer-like coverage as the circumference-to-area ratio decreases. We predict that this incorporation fraction depends strongly on the dosage of the precursor and that the standard deviation of the number of incorporations scales as ~√n, as would be expected for a sequence of largely independent incorporation events. Finally, we characterize an array of 36 experimentally prepared multidonor 3 × 3 nm lithographic windows with scanning tunneling microscopy, measuring the fidelity of the lithography to the desired array and the final location of PH x fragments within these lithographic windows. We use our kinetic model to examine the expected variability due to the observed lithographic error, predicting a negligible impact on incorporation statistics. We find good agreement between our model and the inferred incorporation locations in these windows from scanning tunneling microscope measurements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Transient Mesoscopic Immiscibility, Viscosity Anomaly, and High Internal Pressure at the Semiconductor–Metal Transition in Liquid Ga 2 Te 3

Gallium tellurides appear to be promising phase-change materials (PCMs) of the next generation for brain-inspired computing and reconfigurable optical metasurfaces. They are different from the benchmark PCMs because of sp 3 gallium hybridization in both cubic Ga 2 Te 3 and amorphous pulsed laser deposition (PLD) films. Liquid Ga 2 Te 3 also shows a viscosity η(T) anomaly just above melting when η(T) first increases and only then starts decreasing. We used high-energy X-ray diffraction to observe a transient mesoscopic immiscibility that suggested dense metallic liquid droplets in a semiconducting melt. The η(T) shape was consistent with this finding. A vanishing first sharp diffraction peak that also shifts to a higher Q indicates a high internal pressure in the metallic melt, which produces a remarkable asymmetry of the Ga–Te nearest neighbor distances and is reminiscent of high-pressure rhombohedral Ga 2 Te 3 . Finally, the observed phenomena provide a realistic scenario for a fast, multilevel SET–RESET response, which also unravels similar trends in the purported density-driven liquid polyamorphism of water, phosphorus, sulfur, and other materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Understanding the Adsorption of Rare-Earth Elements in Oligo-Grafted Mesoporous Carbon

Rare-earth elements (REEs) are 17 elements of the periodic table primarily consisting of lanthanides. In modern society, the usage of REEs is ubiquitous in almost all modern gadgets and therefore efficient recovery and separation of REEs are of high importance. Selective adsorption and chelation of REEs in solid sorbents is a unique and sustainable process for their recovery. In this work, single-stranded oligos with 100 units of thymine were grafted onto carboxylated mesoporous carbon to synthesize a sorbent with phosphorus and oxygen functionalities. Additionally, the sorbent was characterized by X-ray photoelectron spectroscopy, Fourier-transform infrared spectroscopy, and scanning electron microscopy-energy-dispersive X-ray spectroscopy. Three different REEs with varying atomic radii and densities, Lu, Dy, and La, were adsorbed onto the carbon from aqueous solutions. It was observed that the adsorbed amounts increased with the increase in the atomic radius or decrease in the atomic density. Calculation of the distribution coefficients for all the equilibrium adsorption amounts suggested that adsorption is more effective in the lower concentration region. The L 3 -edge X-ray absorption near-edge structure confirmed a 3+ oxidation state of REEs in the adsorbed phase. Extended X-ray absorption fine structure (EXAFS) confirmed the binding of REEs with oxygen functionalities in the adsorbed phase. The radial distribution functions calculated from the EXAFS data suggest a longer RE–O distance for La compared to those for Lu and Dy. The coordination numbers and Debye–Waller factors have typical values of about 8–9 atoms and 0.01–0.02 Å 2 , respectively.

36 MATERIALS SCIENCE↗
DOE OSTI2021

High-Temperature-Performance Cyanate Ester Composites with Carboranes

Cyanate ester (CE) is an important class of materials among high-temperature performance thermosets. It is used in aerospace launch vehicles, heat sinks, booms, and trusses of satellites etc. due to its high glass transition temperatures (>220°C), excellent thermal stability, and low flammability. Current approaches to improve the thermal stability of CE include incorporation of siloxanes or phosphorus- based flame retardants (PFRs). In this work, we have explored boron-based hydroxy (PD) and epoxy (EP) functionalized carborane additives to improve the thermal properties of CE. Carborane fillers were solvent blended at various mass loadings in the resin and cured to study their effect on thermal properties. PD and EP carboranes react with CE to form iminocarbonate and oxazolidinone linkages respectively. Cure kinetics studies at different wt% loadings explained that carboranes catalyze the curing reaction by reducing curing activation energy by about 54% and 26% for 10 wt% loadings of PD and EP carboranes respectively. In addition, carborane-filled cyanate ester (CE) nanocomposites demonstrate an exceptionally high thermal stability as compared to the pristine resin in air and inert environment. Our thermogravimetric analysis (TGA) experiments show that the ultimate char yield of the resin can be increased from 0% to as high as 76% and 82% with 30 wt% PD and EP carborane loading respectively at 1000 °C in air. The initial degradation temperature T d;5 of the composites decreased with increasing carborane loadings in both air and argon. For instance, T d;5 for CE was 465 and 471.6 °C in argon and air while that for P20 was 437.4 and 452.1 °C. Modulated TGA studies gave evidence of the effect of carboranes on degradation kinetics and the mechanism of the resin in air and inert environment. The effect of bonding between carboranes and CE at various loadings on the thermal expansion of the matrix was also studied using Thermomechanical Analyzer (TMA). PD carborane reduced the T g for P20 to about 225 °C while CE had T g >350 °C.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗