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DOE OSTI2020

Increased replication of dissimilatory nitrate-reducing bacteria leads to decreased anammox bioreactor performance

Background: Anaerobic ammonium oxidation (anammox) is a biological process employed to remove reactive nitrogen from wastewater. While a substantial body of literature describes the performance of anammox bioreactors under various operational conditions and perturbations, few studies have resolved the metabolic roles of their core microbial community members. Results: Here, we used metagenomics to study the microbial community of a laboratory-scale anammox bioreactor from inoculation, through a performance destabilization event, to robust steady-state performance. Metabolic analyses revealed that nutrient acquisition from the environment is selected for in the anammox community. Dissimilatory nitrate reduction to ammonium (DNRA) was the primary nitrogen removal pathway that competed with anammox. Increased replication of bacteria capable of DNRA led to the out-competition of anammox bacteria, and the loss of the bioreactor's nitrogen removal capacity. These bacteria were highly associated with the anammox bacterium and considered part of the core microbial community. Conclusions: Our findings highlight the importance of metabolic interdependencies related to nitrogen- and carbon-cycling within anammox bioreactors and the potentially detrimental effects of bacteria that are otherwise considered core microbial community members.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2025

Manganese concentration influences nitrogen cycling in agricultural soil

Manganese (Mn) can modulate nitrogen (N) transformations in soil, yet its role in agroecosystems remains understudied. We conducted a 51-day microcosm incubation with agricultural soils differing in long-term N history (N 0 , no added N; N 1 , added 225 kg N ha −1 for a duration of 27 years) and amended with soluble Mn at 0 (M 0 ), 50 (M 1 ), or 250 (M 2 ) mg kg −1 and Glyceria striata (Lam.) residue. In N 1 soils, Mn additions (both M 1 and M 2 ) lowered total mineral N by 25 % relative to N 1 M 0 at day 51 and reduced 51-day cumulative N₂O by 32 % (N 1 M 1 ) and 42 % (N 1 M 2 ) vs. N 1 M 0 , whereas effects in N 0 were negligible. Mn also depressed ammonia-oxidizing bacterial amoA gene transcripts at day 15 in N 1 M 2 vs. N 1 M 0 (2.5 fold change). This reduction was likely due to increased N loss via complete denitrification to N₂ through microbial pathways such as nitrate/nitrite-dependent manganese oxidation (NDMO), where bacteria directly used the added Mn 2+ to reduce nitrate (NO 3 − ) and nitrite (NO 2 − ) to N 2 or as Mn dependent-ammonia oxidation (Mnammox) where bacteria oxidized ammonium (NH 4 + ) to N 2 , using Mn oxides as electron acceptors that formed from the oxidation of the added Mn. Other contributing mechanisms may include Mn-induced N immobilization, toxicity, and changes in the microbial community. These mechanistic results indicate that background Mn availability and redox dynamics can shape nitrification–denitrification pathways under N-rich conditions. In conclusion, we highlight how native Mn pools and redox state may help explain observed variability in N losses and greenhouse gas production across agricultural soils.

Decomposition↗

DOE OSTI2026

Engineering diamond interfaces free of dark spins

Nitrogen-vacancy (NV) centers in diamond are utilized extensively as quantum sensors for imaging fields at the nanoscale. The ultrahigh sensitivity of NV magnetometers has enabled the detection and spectroscopy of individual electron spins, with potentially far-reaching applications in condensed matter physics, spintronics, and molecular biology. However, the surfaces of these diamond sensors naturally contain electron spins, which create a background signal that can be hard to differentiate from the signal of the target spins. In this study, we develop a surface modification approach that eliminates the unwanted signal of these so-called dark electron spins. Our surface passivation technique, based on coating diamond surfaces with a thin titanium oxide (Ti⁢O 2 ) layer, reduces the dark spin density. The observed reduction in dark spin density aligns with our findings on the electronic structure of the diamond-Ti⁢O 2 interface. The reduction, from a typical value of 2000 μm −2 to a value below that set by the detection limit of our NV sensors (200 μm −2 ), results in a twofold increase in Hahn-echo coherence time of near surface NV centers. Furthermore, we derive a comprehensive spin model that connects dark spin relaxation with NV coherence, providing additional insights into the mechanisms behind the observed spin dynamics. Our findings are directly transferable to other quantum platforms, including nanoscale solid-state qubits and superconducting qubits.

74 ATOMIC AND MOLECULAR PHYSICS↗

NASA NTRS1973

Effects of prevaporized fuel on exhaust emissions of an experimental gas turbine combustor

Effects of fuel vaporization on the exhaust emission levels of oxides of nitrogen (NOX), carbon monoxide, total hydrocarbons, and smoke number were obtained in an experimental turbojet combustor segment. Two fuel injector types were used in which liquid ASTM A-1 jet fuel and vapor propane fuel were independently controlled to simulate varying degrees of vaporization. Tests were conducted over a range of inlet-air temperatures from 478 to 700 K (860 to 1260 R), pressures from 4 to 20 atmospheres, and combustor reference velocities from 15.3 to 27.4 m/sec (50 to 90 ft/sec). Converting from liquid to complete vapor fuel resulted in NOX reductions as much as 22 percent and smoke number reductions up to 51 percent.

Norgren, C. T.↗

DOE OSTI2026

Sub-Nanometer Nanoclusters of Copper Atop Single-Atom Copper Moieties toward Electrochemical CO 2 Hydrogenation to Methane

The electrochemical CO 2 reduction (eCO 2 R) offers a compelling route for converting CO 2 into value-added fuels and chemicals. Among CO 2 -derived products, methane (CH 4 ) occupies a distinct position, serving both as a key intermediate for emerging cascade electro-oxidation to oxygenates and as a strategically important extraterrestrial fuel that can be generated in situ from off-planet CO 2 resources. Although Cu-based catalysts capable of selectively producing CH 4 have been reported, they seldom sustain high selectivity at practically relevant current densities. Here, we created a single-step co-pyrolysis strategy toward generating and anchoring Cu sub-nanometer clusters (Cu SNC ) atop Cu-N x single-atom (SA) motifs embedded within N-doped carbon (NC), with controllable nanostructures through tuning of the synthesis parameters. Complementary spectroscopic analyses and density functional theory (DFT) calculations help reveal a structure−activity correlation that could guide the catalyst design. The Cu SNC @NC sample synthesized at 550 °C pyrolysis temperature (best described and modeled as Cu 3 -CuN 4 domains) represents the most effective combination of cluster size, metal-nitrogen coordination, and adsorption energetics needed to selectively promote CH 4 generation versus other eCO 2 R products. Incorporating pulsed electrolysis and hydrophobicity-modulated transport tuning at the triple-phase boundary (TPB) further enhanced CH 4 production achieving a partial CH 4 current density of ∼321 mA cm −2 , 53% Faradaic efficiency (FECH 4 ), and less than 4% combined FE for other eCO 2 R products, simplifying downstream CH 4 purification or upgrading. This work establishes generalizable principles for controlling Cu cluster atomicity and metal−nitrogen coordination, both of which are recognized determinants of CH 4 -efficient eCO 2 R.

CH4 production↗

DOE OSTI2026

Critical transverse compressive stresses of straight and bent CORC® wires with and without impregnation

CORC® wires are a promising superconductor for accelerator magnet applications. While their excellent uniaxial tensile properties have been well established, potential degradation under transverse compression remains a concern for accelerator magnets, in which transverse compression is a primary stress experienced by superconductors. To evaluate the critical transverse compressive stresses of rare-earth barium copper oxide conductors, we developed an experimental system that enables testing of samples both with and without impregnation in liquid nitrogen. Furthermore, because bending strain induced during coil winding may influence the critical compressive response of CORC® wires, the apparatus was also modified to allow testing under the bending condition. In this study wires were tested for five configurations: (1) straight, non-impregnated, (2) bent, non-impregnated, (3) straight, Stycast 2850 FT-impregnated, (4) bent, Stycast 2850 FT-impregnated, and (5) bent, paraffin wax-impregnated. The transverse pressures corresponding to 3% and 5% reductions in the critical current are reported. In conclusion, the effects of wire bending and impregnation on the critical transverse pressure are analyzed, and the implications for transverse stress levels in accelerator magnet conductors are discussed.

CORC® wire↗

NASA NTRS1984

Terrestrial nitrous oxide cycles and atmospheric effects

The basic processes that cause N2O emission from soils are briefly discussed, and the rate of the processes is shown to vary widely in space and time, depending on soil, climate, and agrotechnical conditions. Although significant amounts of N2O are indeed emitted from the land, the complexity of the soil processes involved and the wide variation of measured rates still prevents the quantitative evaluation, global budgeting, and reliable prediction of atmospheric N2O. Increased atmospheric N2O abundance increases the levels of odd-nitrogen in the stratosphere, which, in turn, decreases the stratospheric ozone density via a catalytic cycle. Using appropriate atmospheric models and current chemical kinetic data, it has been found that the dependence of ozone reduction on N2O increase is nearly linear; a simulated doubling of N2O leads to a predicted decrease of about 14 percent in total ozone column density. A 10 percent increase in N2O yields a predicted increase in nonmelanoma skin cancer of several percent, and a possible raising of surface temperature of 0.03 K.

Whitten, R. C.↗

NASA NTRS1990

Advanced air revitalization system modeling and testing

To support manned lunar and Martian exploration, an extensive evaluation of air revitalization subsystems (ARS) is being conducted. The major operations under study include carbon dioxide removal and reduction; oxygen and nitrogen production, storage, and distribution; humidity and temperature control; and trace contaminant control. A comprehensive analysis program based on a generalized block flow model was developed to facilitate the evaluation of various processes and their interaction. ASPEN PLUS was used in modelling carbon dioxide removal and reduction. Several life support test stands were developed to test new and existing technologies for their potential applicability in space. The goal was to identify processes which use compact, lightweight equipment and maximize the recovery of oxygen and water. The carbon dioxide removal test stands include solid amine/vacuum desorption (SAVD), regenerative silver oxide chemisorption, and electrochemical carbon dioxide concentration (EDC). Membrane-based carbon dioxide removal and humidity control, catalytic reduction of carbon dioxide, and catalytic oxidation of trace contaminants were also investigated.

Dall-Baumann, Liese↗

DOE OSTI2025

Direct Conversion of MnO2 into Atomic Mn Sites for Oxygen Reduction

Development of platinum group metal (PGM)-free catalysts has been investigated to replace the platinum group metal catalyst in future inexpensive polymer electrolyte membrane (PEM) fuel cells. Usually, synthetic methods for these PGM-free catalysts involve introducing transition-metal salts or molecules. Herein, we demonstrate a facile synthetic method to prepare PGM-free Mn-N-C catalysts by directly converting manganese oxides into highly active MnN4 sites. Typically, MnO2 is used as a Mn source. Ammonium chloride and benzimidazole are introduced during high-temperature treatment to enhance catalytic activity and stability further. Ammonia generated from the decomposition of ammonium chloride can improve the intrinsic ORR activity of MnNx moieties through chemical or electronic effects by introducing additional nitrogen groups. The Mn-N-C catalyst exhibits promising ORR activity, achieving a half-wave potential of 0.83 V in 0.5 M H2SO4, outperforming most PGM-free ORR catalysts. The robust carbon structure resulting from organic-molecule treatment is also verified by electrochemical and physical characterization, thereby improving the catalyst's durability.

Yang, Xiaoxuan↗

NASA NTRS2023

Tracking NO2 Pollution Changes Over Texas: Synthesis of In Situ and Satellite Observations

Nitrogen oxides (NO x ) are major air pollutants that play a crucial role in atmospheric chemistry. We compare Ozone Measuring Instrument's (OMI) NO 2 records with the in situ surface measurements from the Air Quality System of the US Environmental Protection Agency and the Texas Commission on Environmental Quality network in the state of Texas with the goal of understanding the correspondence of satellite and in situ surface observations and identifying the potential synergies between the two observing systems. Our analysis of over 40 in situ daily surface site observations, mostly from urban areas, and OMI daily observed data suggests a correlation ( r ) ranging between 0.2 and 0.8. The correlation improves considerably ( r > 0.5) for monthly average data. Weekly variation of surface NO 2 with a Sunday minimum is well captured by OMI tropospheric NO 2 column observations with similar weekend reductions. NO 2 trend in Texas during 2005–2019 is characterized by significant reductions of 20%–36% in highly populated cities and urban centers. However, a significant (up to 80%) increase was observed in oil and gas producing regions of the Permian and Eagle Ford Basins over the same period. In March–April of 2020, like the other US and global cities, Texas experienced up to 60% reduction in NO 2 levels in major cities due to travel restrictions imposed at local and national levels to contain the spread of COVID-19. Though such reduction is temporary, these reductions were significantly larger than those achieved in the past 16 years of OMI record suggesting that technological advancement can curtail NO x emissions.

Nitrogen dioxide (NO2)↗

NASA NTRS1994

Impact of stratospheric aircraft emissions on ozone: A two dimensional model study

Atmospheric perturbations caused by the emission of nitrogen oxides from a projected fleet of stratospheric aircraft are studied with a two dimensional chemistry, transport model. Photochemistry of the lower stratosphere, the region where these aircraft may fly, is now known to be influenced by heterogeneous reactions involving sulfuric acid aerosols. This study examines the sensitivity of the atmospheric effects of aircraft to heterogeneous reactions. Information of background aerosols based on the SAGE 2 measurements have been used in the parameterization of the heterogeneous conversion rates. It is found that heterogeneous reactions make the lower stratospheric ozone less sensitive to perturbations in the odd nitrogen level. The calculated reduction in global ozone due to NO(x) injection from a fleet of Mach 2.4 aircraft is 1.28 percent if gas phase reactions only are considered in the model, and 0.06 percent if heterogeneous reactions are included.

Natarajan, M.↗

DOE OSTI2022

On the provenance of GEMS, a quarter century post discovery

The provenance of GEMS (glass with embedded metal and sulfides) in cometary type interplanetary dust particles is investigated using analytical scanning transmission electron microscopy and secondary ion mass spectrometry. We review the current state of knowledge and closely examine the densities, elemental compositions and distributions, iron oxidation states, and isotopic compositions of a subset of GEMS in chondritic porous interplanetary dust. We find that GEMS are underdense with estimated densities that are 35–65% of compositionally equivalent crystalline aggregates. GEMS low densities result in a lower contribution to the bulk compositions of IDPs than has been assumed based on their volume fraction. We also find that element/Si ratios, assumed to be primary (indigenous), are instead perturbed by contamination and secondary alteration, including pulse heating during atmospheric entry. Fe in pyrrhotite inclusions was oxidized and Mg, S, Ca, and Fe were depleted relative to lithophile Al and Si, resulting in reduction in element/Si ratios. Because they trap outgassing elements, Fe-rich oxide rims that formed on the surface of GEMS are serendipitous “witness plates” to the changes in composition that accompany atmospheric entry. As a result of alteration, GEMS elemental compositions cannot reliably inform about their provenance. Except for highly anomalous oxygen isotope ratios measured in some large GEMS grains that indicate a contribution from circumstellar dust, oxygen isotope compositions are generally poor indicators of provenance. Prior work indicates that most GEMS fall close to the terrestrial oxygen isotope composition, which, however, does not exclude a presolar interstellar origin. Nitrogen isotopic compositions are more diagnostic. Elevated 15 N/ 14 N ratios indicate that GEMS accreted in conjunction with formation of organic matter by ion–molecule reactions in a cold (<50 K) presolar environment like the extreme outer nebula or interstellar medium. Considering all observations, we conclude that GEMS are most likely processed interstellar silicates.

79 ASTRONOMY AND ASTROPHYSICS↗

NASA NTRS2011

Polymer Electrolyte-Based Ambient Temperature Oxygen Microsensors for Environmental Monitoring

An ambient temperature oxygen microsensor, based on a Nafion polymer electrolyte, has been developed and was microfabricated using thin-film technologies. A challenge in the operation of Nafion-based sensor systems is that the conductivity of Nafion film depends on the humidity in the film. Nafion film loses conductivity when the moisture content in the film is too low, which can affect sensor operation. The advancement here is the identification of a method to retain the operation of the Nafion films in lower humidity environments. Certain salts can hold water molecules in the Nafion film structure at room temperature. By mixing salts with the Nafion solution, water molecules can be homogeneously distributed in the Nafion film increasing the film s hydration to prevent Nafion film from being dried out in low-humidity environment. The presence of organics provides extra sites in the Nafion film to promote proton (H+) mobility and thus improving Nafion film conductivity and sensor performance. The fabrication of ambient temperature oxygen microsensors includes depositing basic electrodes using noble metals, and metal oxides layer on one of the electrode as a reference electrode. The use of noble metals for electrodes is due to their strong catalytic properties for oxygen reduction. A conducting polymer Nafion, doped with water-retaining components and extra sites facilitating proton movement, was used as the electrolyte material, making the design adequate for low humidity environment applications. The Nafion solution was coated on the electrodes and air-dried. The sensor operates at room temperature in potentiometric mode, which measures voltage differences between working and reference electrodes in different gases. Repeat able responses to 21-percent oxygen in nitrogen were achieved using nitrogen as a baseline gas. Detection of oxygen from 7 to 21 percent has also been demonstrated. The room-temperature oxygen micro sensor developed has extremely low power consumption (no heating for operation, no voltage applied to the sensor, only a voltmeter is needed to measure the output), is small in size, is simple to batch-fabricate, and is high in sensor yield. It is applicable in a wide humidity range, with improved operation in low humidity after the additives were added to the Nafion film. Through further improvement and development, the sensor can be used for aerospace applications such as fuel leak detection, fire detection, and environmental monitoring.

Hunter, Gary W.↗

DOE OSTI2022

In-Use Passenger Vessel Emission Rates of Black Carbon and Nitrogen Oxides

This study quantified emission factors of black carbon (BC) and nitrogen oxides (NO x ) from 21 engines on in-use excursion vessels and ferries operating in California's San Francisco Bay, including EPA uncertified and Tier 1-4 engines and across engine operating modes. On average, ~60 fuel-based emission factors per engine were measured using a novel combination of exhaust plume capture combined with GPS location and speed data that can be more readily deployed than common portable emissions measurement systems. Here, BC and NO x emission factors (g kg -1 ) were lowest and least variable during fast cruising and highest during maneuvering and docked operation. Selective catalytic reduction (SCR) reduced NO x emissions by ~80% when functional. However, elevated NO x emissions that exceeded corresponding exhaust standards were measured on most Tier 3 and Tier 4 engines sampled, which can be attributed to inactive SCR during frequent low engine load operation. In contrast, BC emissions exceeded the PM emission standard for only one engine, and SCR systems employed as a NO x reduction technology also reduced emitted BC. Using these measured emission factors to compare commuting options, we show that the CO 2 -equivalent emissions per passenger-kilometer are comparable when commuting by car and ferry, but BC and NO x emissions can be several to more than ten times larger when commuting by ferry.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Metal Oxynitrides for the Electrocatalytic Reduction of Nitrogen to Ammonia

The successful deployment of technologies for the electrocatalytic nitrogen reduction reaction (e-NRR) to synthesize ammonia would enable distributed ammonia production with lower greenhouse gas emissions compared to the Haber–Bosch process. However, electrocatalysts that can readily activate N 2 , promote selective ammonia formation over the competing hydrogen evolution reaction, and maintain stability under reaction conditions are needed to enable this technology. Herein, we give our perspective on metal oxynitrides (A x B y O w N z ) as an emerging and underexplored materials class for e-NRR. Furthermore, we contrast the activity, selectivity, and stability of metal oxynitrides with those of their metal nitride and metal oxide counterparts. We discuss the different possible e-NRR reaction mechanisms on metal oxynitrides, emphasize challenges related to using metal oxynitrides for e-NRR, and provide an outlook for future research. Ultimately, the huge design space of metal oxynitrides is ripe for exploration to find catalyst formulations that overcome some of the limitations of traditional metal oxides and metal nitrides for e-NRR.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Deinococcus radiodurans UWO298 Dependence on Background Radiation for Optimal Growth

Ionizing radiation is a major environmental variable for cells on Earth, and so organisms have adapted to either prevent or to repair damages caused by it, primarily from the appearance and accumulation of reactive oxygen species (ROS). In this study, we measured the differential gene expression in Deinococcus radiodurans UWO298 cultures deprived of background ionizing radiation (IR) while growing 605 m underground at the Waste Isolation Pilot Plant (WIPP), reducing the dose rate from 72.1 to 0.9 nGy h –1 from control to treatment, respectively. This reduction in IR dose rate delayed the entry into the exponential phase of the IR-shielded cultures, resulting in a lower biomass accumulation for the duration of the experiment. The RNASeq-based transcriptome analysis showed the differential expression of 0.2 and 2.7% of the D. radiodurans genome after 24 and 34 h of growth in liquid culture, respectively. Gene expression regulation after 34 h was characterized by the downregulation of genes involved in folding newly synthesized and denatured/misfolded proteins, in the assimilation of nitrogen for amino acid synthesis and in the control of copper transport and homeostasis to prevent oxidative stress. We also observed the upregulation of genes coding for proteins with transport and cell wall assembly roles. These results show that D. radiodurans is sensitive to the absence of background levels of ionizing radiation and suggest that its transcriptional response is insufficient to maintain optimal growth.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2025

1,10-Phenanthroline-Iron Complex-Derived Fe-N-C Electrocatalysts: Enhanced Oxygen Reduction Activity and Stability Through Synthesis Tuning

The development of electrocatalysts composed of earth-abundant elements is essential for advancing the commercial application of Proton Exchange Membrane Fuel Cells (PEMFC). Among these, single-atom electrocatalysts, such as Fe-N-C, show great promise for the oxygen reduction reaction (ORR). This study aims to improve the ORR activity and stability of Fe-N-C electrocatalysts by fine-tuning the straightforward 1,10-phenanthroline-iron complexation synthesis method. Key parameters, including iron-to-phenanthroline ratio, carbon powder surface area, and pyrolysis temperature were systematically varied to evaluate their influence on the resulting electrocatalysts. The findings of this study revealed that the electrocatalysts synthesized with 1,10-phenanthroline (Phen) and high-surface-area Black Pearls (BP) possessed much better ORR activity than electrocatalysts prepared by using Vulcan carbon (lower surface area). Interestingly, electrocatalysts prepared with BP, but with a non-bidentate nitrogen-containing ligand molecule, such as imidazole, showed a much poorer activity, as the resulting material predominantly consisted of inactive structures, such as encapsulated iron nanoparticles and iron oxide, as evidenced by HR-TEM, EXAFS, and XRD. Therefore, the results suggest that only the synergistic combination of the bidentate ligand phenanthroline (Phen) and the high-surface-area carbon support (BP) favored the formation of ORR-active Fe-N-C single-atom species upon pyrolysis. The study also unveiled a significant enhancement in electrocatalyst stability during accelerated durability tests (and air storage) as the pyrolysis temperature was increased from 700 to 1300 °C, albeit at the expense of ORR activity, likely resulting from the generation of iron particles. Pyrolysis at 1050 °C yielded the electrocatalyst with the most favorable balance of activity and stability in rotating disk measurements, while maintaining moderate durability under PEM fuel cell operation. The insights obtained in this study may guide the development of more active efficient and durable electrocatalysts, synthesized via a simple method using earth-abundant elements, for application in PEMFC cathodes.

30 DIRECT ENERGY CONVERSION↗

NASA NTRS1976

Experimental clean combustor program, phase 2

Combustor pollution reduction technology for commercial CTOL engines was generated and this technology was demonstrated in a full-scale JT9D engine in 1976. Component rig refinement of the two best combustor concepts were tested. These concepts are the vorbix combustor, and a hybrid combustor which combines the pilot zone of the staged premix combustor and the main zone of the swirl-can combustor. Both concepts significantly reduced all pollutant emissions relative to the JT9D-7 engine combustor. However, neither concept met all program goals. The hybrid combustor met pollution goals for unburned hydrocarbons and carbon monoxide but did not achieve the oxides of nitrogen goal. This combustor had significant performance deficiencies. The Vorbix combustor met goals for unburned hydrocarbons and oxides of nitrogen but did not achieve the carbon monoxide goal. Performance of the vorbix combustor approached the engine requirements. On the basis of these results, the vorbix combustor was selected for the engine demonstration program. A control study was conducted to establish fuel control requirements imposed by the low-emission combustor concepts and to identify conceptual control system designs. Concurrent efforts were also completed on two addendums: an alternate fuels addendum and a combustion noise addendum.

Roberts, R.↗