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All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Coordination and activation of nitrous oxide by iron zeolites

Iron-containing zeolites are heterogeneous catalysts that exhibit remarkable activity in the selective oxidation of inert hydrocarbons and catalytic decomposition of nitrous oxide (N 2 O). The reduction of N 2 O is critical to both these functions, but experimental data tracking the iron active sites during N 2 O binding and activation are limited. Here, the N 2 O-ligated Fe(ii) active site in iron-exchanged zeolite beta is isolated and characterized by variable-temperature Mössbauer, diffuse reflectance UV-vis-NIR and Fourier transform infrared spectroscopy. N 2 O binds through the terminal nitrogen atom with substantial backbonding from the Fe(ii) centre at low temperature. At higher temperatures, the Fe–N 2 O interaction is weakened, facilitating isomerization to the O-bound form, which is competent in O-atom transfer. Density functional theory calculations show the geometric and electronic structure requirements for N 2 O binding and activation. A geometric distortion imposed by the zeolite lattice plays an important role in activating N 2 O. As a result, this highlights a mechanism for structural control over function in Fe-zeolite catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1998

Advanced Low Emissions Subsonic Combustor Study

Recent advances in commercial and military aircraft gas turbines have yielded significant improvements in fuel efficiency and thrust-to-weight ratio, due in large part to increased combustor operating pressures and temperatures. However, the higher operating conditions have increased the emission of oxides of nitrogen (NOx), which is a pollutant with adverse impact on the atmosphere and environment. Since commercial and military aircraft are the only important direct source of NOx emissions at high altitudes, there is a growing consensus that considerably more stringent limits on NOx emissions will be required in the future for all aircraft. In fact, the regulatory communities have recently agreed to reduce NOx limits by 20 percent from current requirements effective in 1996. Further reductions at low altitude, together with introduction of limits on NOx at altitude, are virtual certainties. In addition, the U.S. Government recently conducted hearings on the introduction of federal fees on the local emission of pollutants from all sources, including aircraft. While no action was taken regarding aircraft in this instance, the threat of future action clearly remains. In these times of intense and growing international competition, the U.S. le-ad in aerospace can only be maintained through a clear technological dominance that leads to a product line of maximum value to the global airline customer. Development of a very low NOx combustor will be essential to meet the future needs of both the commercial and military transport markets, if additional economic burdens and/or operational restrictions are to be avoided. In this report, Pratt & Whitney (P&W) presents the study results with the following specific objectives: Development of low-emissions combustor technologies for advances engines that will enter into service circa 2005, while producing a goal of 70 percent lower NOx emissions, compared to 1996 regulatory levels. Identification of solution approaches to barriers to the productization and economic viability of the low-emissions technologies. Preparation of these technologies to facilitate an annular rig high-pressure demonstration.

Smith, Reid↗
NASA NTRS2004

Workshop on Oxygen in the Terrestrial Planets

This volume contains abstracts that have been accepted for presentation at the Workshop on Oxygen in the Terrestrial Planets, July 20-23,2004, Santa Fe, New Mexico. The contents include: 1) Experimental Constraints on Oxygen and Other Light Element Partitioning During Planetary Core Formation; 2) In Situ Determination of Fe(3+)/SigmaFe of Spinels by Electron Microprobe: An Evaluation of the Flank Method; 3) The Effect of Oxygen Fugacity on Large-Strain Deformation and Recrystallization of Olivine; 4) Plagioclase-Liquid Trace Element Oxygen Barometry and Oxygen Behaviour in Closed and Open System Magmatic Processes; 5) Core Formation in the Earth: Constraints from Ni and Co; 6) Oxygen Isotopic Compositions of the Terrestrial Planets; 7) The Effect of Oxygen Fugacity on Electrical Conduction of Olivine and Implications for Earth s Mantle; 8) Redox Chemical Diffusion in Silicate Melts: The Impact of the Semiconductor Condition; 9) Ultra-High Temperature Effects in Earth s Magma Ocean: Pt and W Partitioning; 10) Terrestrial Oxygen and Hydrogen Isotope Variations: Primordial Values, Systematics, Subsolidus Effects, Planetary Comparisons, and the Role of Water; 11) Redox State of the Moon s Interior; 12) How did the Terrestrial Planets Acquire Their Water?; 13) Molecular Oxygen Mixing Ratio and Its Seasonal Variability in the Martian Atmosphere; 14) Exchange Between the Atmosphere and the Regolith of Mars: Discussion of Oxygen and Sulfur Isotope Evidence; 15) Oxygen and Hydrogen Isotope Systematics of Atmospheric Water Vapor and Meteoric Waters: Evidence from North Texas; 16) Implications of Isotopic and Redox Heterogeneities in Silicate Reservoirs on Mars; 17) Oxygen Isotopic Variation of the Terrestrial Planets; 18) Redox Exchanges in Hydrous Magma; 19) Hydrothermal Systems on Terrestrial Planets: Lessons from Earth; 20) Oxygen in Martian Meteorites: A Review of Results from Mineral Equilibria Oxybarometers; 21) Non-Linear Fractionation of Oxygen Isotopes Implanted in Lunar Metal Grains: Solar, Lunar or Terrestrial Origin? 22) Isotopic Zoning in the Inner Solar System; 23) Redox Conditions on Small Bodies; 24) Determining the Oxygen Fugacity of Lunar Pyroclastic Glasses Using Vanadium Valence - An Update; 25) Mantle Redox Evolution and the Rise of Atmospheric O2; 26) Variation of Kd for Fe-Mg Exchange Between Olivine and Melt for Compositions Ranging from Alkaline Basalt to Rhyolite; 27) Determining the Partial Pressure of Oxygen (PO,) in Solutions on Mars; 28) The Influence of Oxygen Environment on Kinetic Properties of Silicate Rocks and Minerals; 29) Redox Evolution of Magmatic Systems; 30) The Constancy of Upper Mantlefo, Through Time Inferred from V/Sc Ratios in Basalts: Implications for the Rise in Atmospheric 0 2; 31) Nitrogen Solubility in Basaltic Melt. Effects of Oxygen Fugacity, Melt Composition and Gas Speciation; 32) Oxygen Isotope Anomalies in the Atmospheres of Earth and Mars; 33) The Effect of Oxygen Fugacity on Interdiffusion of Iron and Magnesium in Magnesiowiistite 34) The Calibration of the Pyroxene Eu-Oxybarometer for the Martian Meteorites; 35) The Europium Oxybarometer: Power and Pitfalls; 36) Oxygen Fugacity of the Martian Mantle from PigeoniteMelt Partitioning of Samarium, Europium and Gadolinium; 37) Oxidation-Reduction Processes on the Moon: Experimental Verification of Graphite Oxidation in the Apollo 17 Orange Glasses; 38) Oxygen and Core Formation in the Earth; 39) Geologic Record of the Atmospheric Sulfur Chemistry Before the Oxygenation of the Early Earth s Atmosphere; 40) Comparative Planetary Mineralogy: V/(CrCAl) Systematics in Chromite as an Indicator of Relative Oxygen Fugacity; 41) How Well do Sulfur Isotopes Constrain Oxygen Abundance in the Ancient Atmospheres? 42) Experimental Constraints on the Oxygen Isotope (O-18/ O-16) Fractionation in the Ice vapor and Adsorbant vapor Systems of CO2 at Conditions Relevant to the Surface of Mars; 43) Micro-XANES Measurements on Experimental Spinels andhe Oxidation State of Vanadium in Spinel-Melt Pairs; 44) Testing the Magma Ocean Hypothesis Using Metal-Silicate Partitioning of Te, Se and S; 45) Solubility of Oxygen in Liquid Iron at High Pressure and Consequences for the Early Differentiation of Earth and Mars Metallic Liquid Segregation in Planetesimals; 46) Oxygen Fugacity of Lunar Basalts and the Lunar Mantle. Range of fo2 and the Effectiveness of Oxybarometers; 47) Thermodynamic Study of Dissociation Processes of Molecular Oxygen in Vapor over Oxide Compounds; 48) Oxygen Profile of a Thermo-Haliophilic Community in the Badwater Salt Flat; 49) Oxygen Barometry Using Synchrotron MicroXANES of Vanadium; 50) Mass-Independent Isotopic Fractionation of Sulfur from Sulfides in the Huronian Supergroup, Canada; 51) Mass Independent Isotopes and Applications to Planetary Atmospheres; 52) Electrical Conductivity, Oxygen Fugacity, and Mantle Materials; 53) Crustal Evolution and Maturation on Earth: Oxygen Isotope Evidence; 54) The Oxygen Isotope Composition of the Moon: Implications for Planet Formation; 55) Oxygen Isotope Composition of Eucrites and Implications for the Formation of Crust on the HED Parent Body; and 56) The Role of Water in Determining the Oxygen Isotopic Composition of Planets.

Source record↗
NASA NTRS2007

In Situ Multi-Species (O2, N2, Fuel, Other) Fiber Optic Sensor for Fuel Tank Ullage

A rugged and compact fiber optic sensor system for in situ real-time measurement of nitrogen (N2), oxygen (O2), hydrocarbon (HC) fuel vapors, and other gases has been developed over the past several years at Glenn Research Center. The intrinsically-safe, solid-state fiber optic sensor system provides a 1% precision measurement (by volume) of multiple gases in a 5-sec time window. The sensor has no consumable parts to wear out and requires less than 25 W of electrical power to operate. The sensor head is rugged and compact and is ideal for use in harsh environments such as inside an aircraft fuel tank, or as a feedback sensor in the vent-box of an on-board inert gas generation system (OBIGGS). Multiple sensor heads can be monitored with a single optical detection unit for a cost-effective multi-point sensor system. The present sensor technology is unique in its ability to measure N2 concentration directly, and in its ability to differentiate different types of HC fuels. The present sensor system provides value-added aircraft safety information by simultaneously and directly measuring the nitrogen-oxygen-fuel triplet, which provides the following advantages: (1) information regarding the extent of inerting by N2, (2) information regarding the chemical equivalence ratio, (3) information regarding the composition of the aircraft fuel, and (4) by providing a self-consistent calibration by utilizing a singular sensor for all species. Using the extra information made available by this sensor permits the ignitability of a fuel-oxidizer mixture to be more accurately characterized, which may permit a reduction in the amount of inerting required on a real-time basis, and yet still maintain a fire-safe fuel tank. This translates to an increase in fuel tank fire-safety through a better understanding of the physics of fuel ignition, and at the same time, a reduction in compressed bleed air usage and concomitant aircraft operational costs over the long-run. The present fiber optic sensor can also be used as a false-alarm-free engine/hidden/cargo space fire detector (by measuring increased CO2 and CO, and decreased O2), a multi-point in situ measurement and certification system for halogenated-compound fire protection systems, and for the testing and certification of other aircraft safety sensor systems. The technology (LEW-17826-1) developed in the present sensor system is patent pending.

Nguyen, Quang-Viet↗
DOE OSTI2021

Reduction of Ultrafine Hematite for a Spouting Bed Chemical Looping Process - Presentation

Chemical looping combustion research has been a topic of great interest since the mid-1990s, although the concept can be traced much further back. It is a combustion technology for fuel utilization that uses a two-reactor system to produce a carbon free effluent stream from the air reactor and a carbon dioxide rich stream from the fuel reactor with oxygen shuttled between the reactors with an oxygen carrier. Chemical looping combustion has been studied extensively because of this inherent separation of the carbon dioxide combustion product from the atmospheric nitrogen over that past 25 years with hundreds of research papers and tens of books. The oxygen carrier is, in general, a solid such as naturally occurring hematite or an engineered carrier like a copper and iron oxide supported on alumina. System technical and economic research activities conducted at the National Energy Technology Laboratory have shown that the costs associated with the carrier, initial and replacement, are a significant factor in the economic viability of the technology. To overcome this economic challenge, the work reported on in this paper investigates the use of a waste iron oxide as the chemical looping oxygen carrier. This waste material is quite unique as it has a particle size of 0.7 um. Given the particle size, the reactions are quite fast. However, the development of a contactor reactor to mix the fuel with the carrier is a fluidization challenge as the material is a Geldart group C material and highly cohesive. Normally, Geldart group C materials are fluidized with either a vibrating bed. This technique is acceptable for low temperature pharmaceuticals production but does not lend itself to much larger reactors used for power production or operation at temperatures in the order of 1100 to 1200 C. Therefore, a hydrodynamic solution was needed to break up the cohesive structures to replace the vibration. In this instance, it was hypothesized that a spouting bed of large Geldart group B or Geldart group D particles could provide the necessary energy to break up the cohesive structures of the Geldart group C material. This paper presents the reduction performance for this novel carrier material in a laboratory spouting bed reactor.

Breault, Ronald↗
NASA NTRS1976

The NASA Pollution-Reduction Technology Program for small jet aircraft engines - A status report

A three-phase experimental program is described which has the objective of enabling EPA Class T1 jet engines to meet the 1979 EPA emissions standards. In Phase I, three advanced combustor concepts, designed for the AiResearch TFE 731-2 turbofan engine, were evaluated in screening tests. Goals for carbon monoxide and unburned hydrocarbons were met or closely approached with two of the concepts with relatively modest departures from conventional combustor design practices. A more advanced premixing/prevaporizing combustor, while appearing to have the potential for meeting the oxides of nitrogen goal as well, will require extensive development to make it a practical combustion system. Smoke numbers for the two combustor concepts which will be carried forward into Phase II of the program were well within the EPA smoke standard. Phase II, Combustor-Engine Compatibility Testing, which is in its early stages, and planned Phase III, Combustor-Engine Demonstration Testing, are also described.

Fear, J. S.↗
NASA NTRS1992

Electron beam fluorescence measurements in the Boeing hypersonic shock tunnel

The Calspan electron beam fluorescence (EBF) measurement system is described along with the results of measurements made in hypersonic flow. Numerous self-emitting metallic species were identified, many of which may be associated with an aging/erosion process within the B30HST. Because there were only 16 tunnel runs, it was only possible to obtain spectral measurements over a limited range of wavelengths and time sampling periods. Many spectral features of the flow remain uninvestigated. Because flow self-emission is important to all optical diagnostic techniques, it is recommended that additional spectral studies by performed. The three electron beam-excited species that were identified are nitrogen, helium, and nitric oxide. The high metallic radiation background interfered with attempts to obtain the time-wise variation of N2 density and He radiation with the optical fiber/PMT channels. In the case of the N2 density measurements the result of interference was increased uncertainty. Unfortunately, the interference caused the time-wise He measurements to fail completely. It is recommended that the electron beam be modulated to provide discrimination against the background radiation in future N2 density measurements. Careful data reduction produced useful measurements of N2 vibrational temperature, even though the high background from metallic species significantly increased measurement uncertainty. Perhaps the recommended additional spectral studies would reveal N2(+) First Negative System band-pair regions having less background. Detection of the He arrival was easily accomplished with the spectrometer/array detector system. Because of this, it is recommended that this means of detecting He arrival be used in the future. With proper calibrations of the system an He number density could be obtained. Although the flow conditions were out of limits for the run in which the NO spectrum was recorded, the usefulness of the NO spectrum for determination of free-stream rotational temperature was demonstrated and should be exploited in future experiments. Indeed, based on the strong NO signals, it is recommended that lower resolution NO spectra be obtained to provide a measure of NO vibrational temperature in the same manner that the N2 temperature was obtained.

Price, Linwood L.↗
DOE OSTI2020

Milestone 2.7: Evaluation of Techniques for the Measurement of Molecular Hydrogen Gas in Helium Matrices

Published data by Task 2 (Oxyhydroxide Layer Radiolytic Gas Generation Resolution) for Technical Considerations and Challenges for Extended (>50 yrs) Dry Storage of Aluminum Cladded Spent Nuclear Fuel (ASNF), demonstrated that radiolytic molecular hydrogen (H2) production from gamma irradiated aluminum alloy 1100 (Al-1100) coupons exhibited significant dependence on backfill gaseous environment conditions: air, due to the presence of oxygen, completely inhibited H2 production; nitrogen promoted H2 production; and argon yielded more H2 than nitrogen environments. The concern here is that helium has been proposed as the backfill gas for extended storage and is more inert than argon, which may translate into significantly more H2 production than current Task 3 argon-based models predict. However, the measurement of H2 in helium media was not possible using the previously establish gas chromatography (GC) flame ionization detector, due to similarities in thermal conductivity. This milestone was initiated to evaluate an alternative GC approach that employed a mercuric oxide (HgO) reduction gas detector (RGD). Using the HgO RGD setup, H2 was successfully calibrated in the presence of a helium carrier gas, and then subsequently measured in control and irradiated crush-tube sample vials, consistent with previous sample measurements. Overall, the HgO RGD approach was found to be sufficient for future helium environment irradiations.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2020

Future impacts of ozone driven damages on agricultural systems

Current ozone (O 3 ) concentration levels entail significant damages in crop yields around the world. The reaction of the emitted precursors (mostly methane and nitrogen oxides) with solar radiation contribute to O 3 levels that exceed established thresholds for crop damage. This paper shows current and projected (up to 2080) relative yield losses (RYLs) driven by O 3 exposure for different crops and the associated economic damages applying dynamic crop production and prices that are calculated per region and period. We adjust future crop yields in the Global Change Assessment Model (GCAM) to reflect the RYLs and analyze the effects on agricultural markets. We find that the changes (generally reductions) in O 3 precursor emissions in a reference scenario would reduce the agricultural damages, compared to present, for most of the regions, with a few exceptions including India, where higher future O3 concentrations have large negative impacts on crop yields. The annual economic impact of O3 driven losses from 2010-2080 are, in billion US dollars at 2015 prices ($B), 5.0-6.0, 9.8-18.8, 6.7-10.6 and 10.4-12.5 for corn, soybeans, rice and wheat, respectively, with the large losses for wheat and soybeans driven by their comparatively high responses to O 3 . When O 3 effects are explicitly modelled as exogenous yield shocks in future periods, there is a direct impact in future agricultural markets. Therefore, the aggregated net present value (NPV) of crop production would be reduced around by $90.8B at a global level. However, these changes are not distributed evenly across regions, and the net present market value of the crops would increase by up to $118.2B (India) or decrease by up to $59.2B (China).

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1973

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

Effect 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, pressures from 4 to 20 atmospheres, and combustor reference velocities from 15.3 to 27.4 m/sec. Converting from liquid to complete vapor fuel resulted in NOx reductions as much as 22% and smoke number reductions up to 51%.

Norgren, C. T.↗
NASA NTRS2019

Mid-21st Century Ozone Air Quality and Health Burden in China Under Emissions Scenarios and Climate Change

Despite modest emissions reductions of air pollutants in recent years, China still suffers from poor air quality, and the outlook for future air quality in China is uncertain. We explore the impact of two disparate 2050 emissions scenarios relative to 2015 in the context of a changing climate with the Geophysical Fluid Dynamics Laboratory Atmospheric Model version 3 (GFDL-AM3) chemistry-climate model. We impose the same near-term climate change for both emission scenarios by setting global sea surface temperature (SST) and sea ice cover (SIC) to the average over 2010–2019 and 2046–2055, respectively, from a three-member ensemble of GFDL coupled climate model simulations under the RCP8.5 (Representative Concentration Pathway) scenario. By the 2050s, annual mean surface ozone increases throughout China by up to 8 ppbv from climate change alone (estimated by holding air pollutants at 2015 levels while setting SIC and SST to 2050 conditions in the model) and by 8–12 ppbv in a scenario in which emissions of ozone precursors nitrogen oxides (NO (sub x) ) and anthropogenic volatile organic compounds (VOCs) increase by ~10%. In a scenario in which NO (sub x) and anthropogenic VOC emissions decline by 60%, annual mean surface ozone over China decreases by 16–20 ppbv in the 2050s relative to the 2010s. The ozone increase from climate change alone results in an additional 62 000 premature deaths in China as compared to 330 000 fewer premature deaths by the 2050s under a strong emissions mitigation scenario. In springtime over Southwestern China in the 2050s, the model projects 9–12 ppbv enhancements to surface ozone from the stratosphere (diagnosed with a model tracer) and from international anthropogenic emissions (diagnosed by differencing AM3 simulations with the same emissions within China but higher versus lower emissions in the rest of the world). Our findings highlight the effectiveness of emissions controls in reducing the health burden in China due to air pollution, and also the potential for climate change and rising global emissions to offset, at least partially, some of the ozone decreases attained with regional emission reductions in China.

Westervelt, D. M.↗
DOE OSTI2020

Atomically Dispersed Iron–Nitrogen Sites on Hierarchically Mesoporous Carbon Nanotube and Graphene Nanoribbon Networks for CO 2 Reduction

Atomically dispersed metal and nitrogen co-doped carbon (M-N/C) catalysts hold great promise for electrochemical CO 2 conversion. However, there is a lack of cost-effective synthesis approaches to meet the goal of economic mass production of single-atom M-N/C with desirable carbon support architecture for efficient CO 2 reduction. Herein, we report facile transformation of commercial carbon nanotube (CNT) into isolated Fe-N 4 sites anchored on carbon nanotube and graphene nanoribbon (GNR) networks (Fe-N/CNT@GNR). The oxidization-induced partial unzipping of CNT results in the generation of GNR nanolayers attached to the remaining fibrous CNT frameworks, which reticulates a hierarchically mesoporous complex and thus enables a high electrochemical active surface area and smooth mass transport. The Fe residues originating from CNT growth seeds serve as Fe sources to form isolated Fe-N-4 moieties located at the CNT and GNR basal plane and edges with high intrinsic capability of activating CO 2 and suppressing hydrogen evolution. The Fe-N/CNT@GNR delivers a stable CO Faradaic efficiency of 96% with a partial current density of 22.6 mA cm -2 at a low overpotential of 650 mV, making it one of the most active M-N/C catalysts reported. This work presents an effective strategy to fabricate advanced atomistic catalysts and highlights the key roles of support architecture in single-atom electrocatalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1979

Novel approaches for alleviation of electrical hazards of graphite-fiber composites

Four basically different approaches were considered: gasification of fibers, retention in the matrix, clumping to prevent entrainment, and electrical insulation of fibers. The techniques used to achieve them are described in some detail. These involved surface treatment of fibers to improve the wettability of fibers and coating the fibers with the selected substances before laying them up for composite fabrication. Thermogravimetric analyses were performed on the plain and treated fibers in inert (nitrogen, argon) and reactive (air) atmospheres. The treated fibers embedded in epoxy were ignited in a Bunsen flame to determine the efficiency of these treatments. A simple apparatus was assembled to detect the time for the first short circuit (in a typical electrical circuit) when exposed to the combustion products from a graphite fiber composite fire. The state-of-the-art and treated fibers cast in typical epoxy were burned and ranked for potential success. It was inferred that the gasification schemes appear promising when reduction or oxidation is tried. It was also found that some very promising candidates were available for the clumping and for the electrical insulation of fibers.

Ramohalli, K.↗
NASA NTRS1990

The effect of nitrogen on xenon ion engine erosion

Erosion studies were performed on a 30-cm diameter J-series ion engine modified for operation on xenon propellant. The erosion rates of molybdenum and tantalum badges placed at different locations within the discharge chamber were measured as a function of the percentage of nitrogen (by mass) added to the xenon propellant. Reductions in the erosion rates of these badges of a factor of 8 to 50 were observed at nitrogen addition fractions between 0.5 to 2.0 percent. Reductions in cathode-side baffle erosion were achieved by adding nitrogen to the xenon propellant or by increasing the cathode orifice diameter. Analyses show that no significant degradation in ion engine performance should be expected at these nitrogen mass fractions. XRD, XPS and Auger analyses indicate the existence of nitrogen and nitrides in the surface of some but not all of the badges used in the tests where nitrogen was added to the xenon. Difficulty in identifying surface nitrides in the samples may be due to the existence of surface oxides and contaminants, or to the small thicknesses of the nitride layers.

Garner, Charles E.↗
DOE OSTI2026

Active site design enables industrial scale H 2 O 2 electrosynthesis with metal-free catalysts

The electrosynthesis of hydrogen peroxide (H 2 O 2 ) via a two-electron oxygen reduction reaction enables decentralized H 2 O 2 production. While metal-free carbon catalysts are sustainable and low-cost, their performance is hindered by poorly defined active sites and uncontrolled defect states. Here, we resolve these challenges through active site design and catalyst screening using fluorine (F) and nitrogen (N) codoped carbons as model materials. Statistical analysis combined with density functional theoretical calculations reveals that F-induced structural modification and defect passivation optimize OOH* binding, with F-doping and adjacent F atoms predominantly lowering abs ΔG(OOH*). Experimental results confirm that semi-ionic C–F bonds passivate defects in nitrogen-doped carbon, enhancing catalytic activity and durability. The resulting (N, F)-codoped carbon achieves nearly 100% H 2 O 2 selectivity at 0.5–0.65 V versus the reversible hydrogen electrode and maintains > 95% across 0.01–0.65 V versus the reversible hydrogen electrode. In an electrolyzer, (N, F)-codoped carbon exhibits an H 2 O 2 yield rate of 74.35 mol g cat. −1 h -1 and sustains 300 mA cm -2 for 105 hours with ~95% faradaic efficiency. Coupling the two-electron oxygen reduction reaction with methanol oxidation further reduces cell voltage and enhances productivity. This work provides a means to design efficient catalysts for industrial H 2 O 2 electrosynthesis.

H2O2 electrosynthesis↗
DOE OSTI2025

Poly-Si Passivating Contacts Hydrogenation by Microwave Annealing

Hydrogenation is a crucial step in the fabrication of high-efficiency silicon solar cells. In this study, we demonstrate the for the first time effectiveness of hydrogen activation via microwave annealing of hydrogen-rich dielectrics coated on poly-Si passivating contacts. This method is compared with conventional hydrogenation techniques, such as annealing in N2 in the presence of a hydrogen-rich source (such as hydrogenated aluminum oxide (AlOx:H), hydrogenated silicon nitride (SiNy:H), or a AlOx:H/SiNy:H stack). Key improvements observed include a reduction in J0 from 30 to <5 fA/cm2, an increase in iVoc from 690 to >730 mV, and an enhancement in effective lifetime (teff) from 0.6 to ~3.5 milliseconds on phosphorus-doped poly-Si/SiO2 passivating contact samples. With a very short annealing time of ~1-2 minutes, the samples passivated by AlOx:H, SiNy:H, or the stack show similar performance to samples subjected to 30 minutes of nitrogen annealing. Photoluminescence (PL) spectra corroborate our findings regarding the hydrogenation of the poly-Si layer and the c-Si substrate, with an increase in PL intensity after microwave annealing. Ultimately, our work suggests that microwave annealing could be a promising addition, offering flexibility to traditional firing hydrogenation processes.

14 SOLAR ENERGY↗
NASA NTRS1996

Effects of Hydrodynamics of Soot Formation in Laminar Opposed-Jet Diffusion Flames

Effects of flow (hydrodynamic properties on the presence of soot in hydrocarbon-fueled laminar opposed-jet diffusion flames were studied experimentally at atmospheric pressure, emphasizing effects of velocities normal to the Rom sheet. These velocities were varied for conditions corresponding to combustion in air by transferring nitrogen from the oxidizer stream to the fuel stream which increases the stoichiometric mixture fraction of the flame and causes the stagnation plane of the flow to shift toward the fuel-rich side of the flame sheet. Fuels considered included acetylene, ethylene, ethane, propylene, propane, and 1-3 butadiene. Present measurements consisted of the critical strain rates for the flames to contain soot (the soot extinction limit) and for the flames to extinguish (the flame extinction limit) It was found that increasing the stoichiometric mixture fraction causes a progressive reduction of the critical strain rates for both flame and soot extinction; however, their ratio increases, and even becomes unbounded in most instances to yield a permanently-blue-flame regime. The results suggest that soot formation in nonpremixed flames can be controlled by varying velocities normal to the flame sheet. Nevertheless, definitive conclusions along these lines require evaluation of effects of corresponding variations of fuel and oxygen concentrations on soot formation when velocities normal to the flame sheet are changed by varying stoichiometric mixture fractions for laminar opposed-jet diffusion flames.

Lin, K.-C.↗
DOE OSTI2025

Microwave Annealing for Fast and Effective Hydrogen Activation in Polycrystalline Silicon Passivating Contacts

Hydrogenation is a crucial step in the fabrication of high-efficiency silicon solar cells. In this study, the effectiveness of hydrogen activation is demonstrated via microwave annealing of hydrogen-rich dielectrics coated on poly-Si passivating contacts. This method is compared with conventional hydrogenation techniques, such as annealing in N2 in the presence of a hydrogen-rich source (such as hydrogenated aluminum oxide (AlOx:H), hydrogenated silicon nitride (SiNy:H), or a AlOx:H/SiNy:H stack). Key improvements observed include a reduction in J0 from 30 to <5 fA cm-2, an increase in iVoc from 690 to >730 mV, and an enhancement in effective lifetime (teff) from 0.6 to ~3.5 milliseconds on phosphorus-doped poly-Si/SiO2 passivating contact samples. With a very short annealing time of ~1-2 min, the samples passivated by AlOx:H, SiNy:H, or the stack show similar performance to samples subjected to 30 min of nitrogen annealing. Photoluminescence (PL) spectra corroborate the findings regarding the hydrogenation of the poly-Si layer and the c-Si substrate, with an increase in PL intensity after microwave annealing. Ultimately, this work suggests that microwave annealing could be a promising addition, offering flexibility to traditional firing hydrogenation processes.

hydrogenation↗