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At least 703 records · Page 39

CW nuclear pumped lasing of 3He-Ne

The results of a study on the CW nuclear pumped lasing of the He-Ne system are presented. Preliminary experiments measured single pass gain for the 6328.2A laser transition at neutron fluxes up to 1 x 10 to the 14th power neutrons/sq cm sec. Peak gain for a 300 torr (He-3)-Ne (5:1 mixture) was found to be 8.84 dB/meter at a 2 x 10 to the 12th power neutrons/sq cm sec neutron flux. Further experiments measured the gain in the flux region from one million to 2 x 10 to the 12th power neutrons/sq cm sec. In addition, gain vs. probe laser intensity at various neutron fluxes was measured. These measurements resulted in the construction of a laser cavity and the subsequent CW nuclear pumped lasing at 6328.2A in (He-3)-Ne. Experiments were also carried out on the 3.39 micrometer superradiant line in (He-3)-Ne. On three separate occasions, at two different facilities, lasing was observed. Although (He-3)-Ne was found to have the lowest threshold for lasing found so far, it also had the lowest output power on the order of tens of microwatts.

Carter, B. D.↗

A neutron-gamma pulse shape discrimination method based on pure and mixed sources

We present a novel trainable approach to distinguish neutrons from gammas using a particle detector. Traditionally, Pulse Shape Discrimination (PSD) methods for this problem utilize an ad-hoc computation of tail signal energy to perform the detection. Our first contribution is a rigorous analysis of the performance of this existing approach on gold standard Time of Flight (TOF) data. While this approach performs well for high energy pulses, its accuracy drops dramatically as the pulse energy decreases. Our second contribution is a novel data driven classifier that is trained from two readily available sources: one that emits gamma particles (Cs-137), and another that emits a mixture of gamma and neutron particles (Cf-252). We test our approach using TOF experiments and show a marked improvement in accuracy over the traditional method for low false positive rates and low energies.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

A study of laser induced ignition of methane–air mixtures inside a Rapid Compression Machine

We present herein a fundamental study of laser ignition of methane/air mixtures at temperatures and pressures representative of an internal combustion engine. An Nd:YAG laser operating at λ = 1064 nm was used to ignite methane/air mixtures at equivalence ratios of 0.4 ≤ Φ ≤ 1 in a Rapid Compression Machine (RCM). Experiments were conducted to study the lean limit, minimum spark energy (MSE), and minimum ignition energy (MIE). The results show that laser ignition exhibits a stochastic behavior which must be interpreted statistically. A 90% probability of occurrence was used to evaluate the MSE and MIE, which resulted in MSE 90 =2.3 mJ and MIE 90 =7.2 mJ at an equivalence ratio Φ = 0.4 at compressed pressure and temperature of P comp = 29 bar and T comp = 750 K, respectively. The lean limit was characterized based on the fraction of chemical energy converted into thermal energy, which was determined by calculating the apparent rate of heat release as derived from RCM high speed pressure data. A lean limit for 90% chemical energy conversion was found to correspond to an equivalence ratio of 0.47 (T comp = 782 K). Schlieren photography was employed as a diagnostics tool to visualize the flame initiation and propagation inside the RCM.

42 ENGINEERING↗

Effects of dilution and pressure on combustion characteristics within externally heated micro-tubes

Here this study investigates the impact of pressure and dilution on combustion behavior of of C 2H6/air/N2 mixtures within an externally heated micro-tube using both experimental and analytical techniques. Experiments are conducted for pressures up to 10 bar at multiple dilution levels and document three flame regimes, i.e. weak flames, FREI and normal flames. Characteristic temperatures for flame stabilization, as well as and ignition and extinction are obtained by applying a novel thin filament pyrometry method (TFP), which uses a thin silicon carbide (SiC) filament that enables temperature measurements for both reacting and non-reacting cases. Results show a decrease of characteristic temperatures with increasing pressure, which can be which can be partially compensated by a decrease of O2 content. Further, regime transitions occur at lower velocity as the pressure increases, whereas weak flame positions are insensitive to dilution at a given pressure. Predictions from the analytical model compare favorably with experimental results. The most prominent finding is that as dilution increases, the transition from weak flame to FREI becomes less abrupt and is completely lost for high dilution levels (i.e. low O2 content). Both experimental and analytical results indicate that the unstable FREI combustion regime does not exist at high dilution levels, i.e. weak flame and normal flame regimes are no longer clearly separated. As FREI are interpreted as a cyclic transition from an ignition zone to a propagating flame, results for highly diluted conditions are interpreted as a combustion regime where classical flame propagation ceases to exist.

42 ENGINEERING↗

Enhancement of CO 2 Uptake and Selectivity in a Metal–Organic Framework by the Incorporation of Thiophene Functionality

The complex [Zn 2 (tdc) 2 dabco] (H 2 tdc = thiophene-2,5-dicarboxylic acid; dabco = 1,4-diazabicyclooctane) shows a remarkable increase in carbon dioxide (CO 2 ) uptake and CO 2 /dinitrogen (N 2 ) selectivity compared to the nonthiophene analogue [Zn 2 (bdc) 2 dabco] (H 2 bdc = benzene-1,4-dicarboxylic acid; terephthalic acid). CO 2 adsorption at 1 bar for [Zn 2 (tdc) 2 dabco] is 67.4 cm 3 ·g -1 (13.2 wt %) at 298 K and 153 cm 3 ·g -1 (30.0 wt %) at 273 K. For [Zn 2 (bdc) 2 dabco], the equivalent values are 46 cm 3 ·g -1 (9.0 wt %) and 122 cm 3 ·g -1 (23.9 wt %), respectively. The isosteric heat of adsorption for CO 2 in [Zn 2 (tdc) 2 dabco] at zero coverage is low (23.65 kJ·mol -1 ), ensuring facile regeneration of the porous material. Enhancement by the thiophene group on the separation of CO 2 /N 2 gas mixtures has been confirmed by both ideal adsorbate solution theory calculations and dynamic breakthrough experiments. The preferred binding sites of adsorbed CO 2 in [Zn 2 (tdc) 2 dabco] have been unambiguously determined by in situ single-crystal diffraction studies on CO 2 -loaded [Zn 2 (tdc) 2 dabco], coupled with quantum-chemical calculations. These studies unveil the role of the thiophene moieties in the specific CO 2 binding via an induced dipole interaction between CO 2 and the sulfur center, confirming that an enhanced CO 2 capacity in [Zn 2 (tdc) 2 dabco] is achieved without the presence of open metal sites. The experimental data and theoretical insight suggest a viable strategy for improvement of the adsorption properties of already known materials through the incorporation of sulfur-based heterocycles within their porous structures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Influence of cluster–support interactions on reactivity of size-selected Nb x O y clusters

Size-selected niobium oxide nanoclusters (Nb 3 O 5 , Nb 3 O 7 , Nb 4 O 7 , and Nb 4 O 10 ) were deposited at room temperature onto a Cu(111) surface and a thin film of Cu 2 O on Cu(111), and their interfacial electronic interactions and reactivity toward water dissociation were examined. These clusters were specifically chosen to elucidate the effects of the oxidation state of the metal centers; Nb 3 O 5 and Nb 4 O 7 are the reduced counterparts of Nb 3 O 7 and Nb 4 O 10 , respectively. From two-photon photoemission spectroscopy (2PPE) measurements, we found that the work function increases upon cluster adsorption in all cases, indicating a negative interfacial dipole moment with the positive end pointing into the surface. The amount of increase was greater for the clusters with more metal centers and higher oxidation state. Additional analysis with DFT calculations of the clusters on Cu(111) indicated that the reduced clusters donate electrons to the substrate, indicating that the intrinsic cluster dipole moment makes a larger contribution to the overall interfacial dipole moment than charge transfer. X-ray photoelectron spectroscopy (XPS) measurements showed that the Nb atoms of Nb 3 O 7 and Nb 4 O 10 are primarily Nb 5+ on Cu(111), while for the reduced Nb 3 O 5 and Nb 4 O 7 clusters, a mixture of oxidation states was observed on Cu(111). Temperature-programmed desorption (TPD) experiments with D 2 O showed that water dissociation occurred on all systems except for the oxidized Nb 3 O 7 and Nb 4 O 10 clusters on the Cu 2 O film. A comparison of our XPS and TPD results suggests that Nb 5+ cations associated with Nb=O terminal groups act as Lewis acid sites which are key for water binding and subsequent dissociation. TPD measurements of 2-propanol dehydration also show that the clusters active toward water dissociation are indeed acidic. DFT calculations of water dissociation on Nb 3 O 7 support our TPD results, but the use of bulk Cu 2 O(111) as a model for the Cu 2 O film merits future scrutiny in terms of interfacial charge transfer. The combination of our experimental and theoretical results suggests that both Lewis acidity and metal reducibility are important for water dissociation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Conserved and reproducible bacterial communities associate with extraradical hyphae of arbuscular mycorrhizal fungi

Abstract Extraradical hyphae (ERH) of arbuscular mycorrhizal fungi (AMF) extend from plant roots into the soil environment and interact with soil microbial communities. Evidence of positive and negative interactions between AMF and soil bacteria point to functionally important ERH-associated communities. To characterize communities associated with ERH and test controls on their establishment and composition, we utilized an in-growth core system containing a live soil–sand mixture that allowed manual extraction of ERH for 16S rRNA gene amplicon profiling. Across experiments and soils, consistent enrichment of members of the Betaproteobacteriales, Myxococcales, Fibrobacterales, Cytophagales, Chloroflexales, and Cellvibrionales was observed on ERH samples, while variation among samples from different soils was observed primarily at lower taxonomic ranks. The ERH-associated community was conserved between two fungal species assayed, Glomus versiforme and Rhizophagus irregularis, though R. irregularis exerted a stronger selection and showed greater enrichment for taxa in the Alphaproteobacteria and Gammaproteobacteria. A distinct community established within 14 days of hyphal access to the soil, while temporal patterns of establishment and turnover varied between taxonomic groups. Identification of a conserved ERH-associated community is consistent with the concept of an AMF microbiome and can aid the characterization of facilitative and antagonistic interactions influencing the plant-fungal symbiosis.

59 BASIC BIOLOGICAL SCIENCES↗

Observation of shock-front separation in multi-ion-species collisional plasma shocks

We observe shock-front separation and species-dependent shock widths in multi-ion-species collisional plasma shocks, which are produced by obliquely merging plasma jets of a He/Ar mixture (97% He and 3% Ar by initial number density) on the plasma liner experiment. Visible plasma emission near the He-I 587.6-nm and Ar-II 476.5–514.5-nm lines is simultaneously recorded by splitting a single visible image of the shock into two different fast-framing cameras with different narrow bandpass filters (589 ± 5 nm for observing the He-I line and 500 ± 25 nm for the Ar-II lines). For conditions in these experiments (pre-shock ion and electron densities ≈5×10 14 cm –3 , ion and electron temperatures of ≈2.2 eV, and relative plasma-merging speed of 22 km/s), the observationally inferred magnitude of He/Ar shock-front separation and the shock widths themselves are <1 cm, which correspond to ~50 post-shock thermal ion–ion mean free paths. These experimental length scales are in reasonable qualitative and quantitative agreement with results from 1D multi-fluid simulations using the CHICAGO code. However, we note there are differences between the experimentally inferred and simulation-predicted ionization states and line emission intensities, particularly in the post-shock region. Overall, the experimental and simulation results are consistent with theoretical predictions that the lighter He ions diffuse farther ahead within the overall shock front than the heavier Ar ions.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Nitrogen Fertilization Effects on Productivity and Nitrogen Loss in Three Grass-Based Perennial Bioenergy Cropping Systems

Nitrogen (N) fertilization can greatly improve plant productivity but needs to be carefully managed to avoid harmful environmental impacts. Nutrient management guidelines aimed at reducing harmful forms of N loss such as nitrous oxide (N 2 O) emissions and nitrate (NO 3 - ) leaching have been tailored for many cropping systems. The developing bioenergy industry is likely to make use of novel cropping systems, such as polycultures of perennial species, for which we have limited nutrient management experience. We studied how a switchgrass (Panicum virgatum) monoculture, a 5-species native grass mixture and an 18- species restored prairie responded to annual fertilizer applications of 56 kg N ha -1 in a fieldscale agronomic trial in south-central Wisconsin over a 2-year period.We observed greater fertilizer-induced N 2 O emissions and sub-rooting zone NO 3 - concentrations in the switchgrass monoculture than in either polyculture. Fertilization increased aboveground net primary productivity in the polycultures, but not in the switchgrass monoculture. Switchgrass was generally more productive, while the two polycultures did not differ from each other in productivity or N loss. In conclusion, our results highlight differences between polycultures and a switchgrass monoculture in responding to N fertilization.

54 ENVIRONMENTAL SCIENCES↗

ChemoMechanical Controls on Induced Seismicity

In recent years, seismicity rates in the US have dramatically risen due to increased activity in onshore oil and gas production. This project attempts to tie observations about induced seismicity to dehydration reactions in laumontite, a common mineral found in fault gouge in crystalline basement formations. It is the hypothesis of this study that in addition to pressurerelated changes in the in situ stress state, the injection of wastewater pushes new fluids into crystalline fault fracture networks that are not in chemical equilibrium with the mineral assemblages, particularly laumontite in fault gouge. Experiments were conducted under hydrothermal conditions where samples of laumontite were exposed to NaC1 brines at different pH values. After exposure to different fluid chemistries for 8 weeks at 90° C, we did not observe substantial alteration of laumontite. In hydrostatic compaction experiments, all samples deformed similarly in the presence of different fluids. Pore pressure decreases were observed at the start of a 1 week hold at 85° C in a 1M NaC1 pH 3 solution, suggesting that acidic fluids might stabilize pore pressures in basement fault networks. Friction experiments on laumontite and kaolinite powders showed both materials have similar coefficients of friction. Mixtures with partial kaolinite content showed a slight decrease in the coefficient of friction, which could be sufficient to trigger slip on critically stressed basement faults.

58 GEOSCIENCES↗

Improved Creep Testing Approach for Bentonite EBS

In the United States, the nuclear reactor contributes 18.7 percent of the nation’s total electricity generation and produces a significant amount of spent nuclear fuel (SNF) and high-level waste. Because SNF is being stored for longer periods than initially envisioned, the U.S. Department of Energy Office of Nuclear Energy, Office of Spent Fuel and Waste Science and Technology is assessing the technical performance of the SNF storage systems after extended durations. The concept of a sustainable geologic repository for SNF disposal relies heavily on the safety provided by multiple barriers, such as repository host rock, overlying rock formation, and human-made engineered barrier systems (EBS). One of the major components of EBS is bentonite-based buffer materials that isolate the nuclear-waste canisters from the host rock and fill the void left in the horizontally drilled boreholes. The resaturated bentonite has a swelling characteristic, which is useful for self-sealing the microcracks in the host rock and supporting the canister’s heavy weight. However, factors such as nonuniformity in the saturation, swelling pressure of bentonite, and the high temperature at the canister-bentonite interface may lead to instability of the waste canister inside the borehole. Therefore, evaluating the long-term deformation of bentonite-based material is necessary. RESPEC Company, LLC recently completed a preliminary study for the U.S. Department of Energy (DE SC0022804) that is attempting to understand the time-dependent deformation in the consolidated sand/bentonite (SB) specimens through triaxial creep experiments and improve the understanding of EBS performance under anticipated repository conditions. The project included developing a standard testing procedure for preparing the consolidated core specimen from a mixture of sand and bentonite in a 50:50 ratio by weight, fabricating a new pressure vessel in-house, modifying existing creep equipment to perform triaxial creep experiments on consolidated SB specimens, and performing six long-term triaxial creep experiments under low-deviatoric stress at two different temperature conditions, which is representative of hypothetical conditions that might be encountered in a geologic repository within a reasonable rate of success in completing creep experiments. The consolidated SB specimen was prepared using the novel specimen preparation procedure and had physical characteristics (e.g., moisture content and bulk density) reasonably comparable with the properties of bentonite-based buffer, which is proposed to be used in the EBS in the Swedish KBS-3H design and the Swiss design of SNF disposal in the horizontal drifts. The newly fabricated pressure vessel could withstand the confining pressure of up to 15 megapascals (MPa) while maintaining the test temperature of up to 90 degrees Celsius (°C) for long-term creep experiments. The preliminary results from the triaxial creep experiments suggested that the consolidated SB specimen may experience time-dependent deformation at a low-deviatoric stress state and room temperature condition. Based on the deformation recorded in the SB specimen from axial and radial linear variable differential transformers (LVDTs) and physical characteristic changes, it is apparent that the time-dependent deformation is a combination of consolidation and creep, which is influenced by the level of deviatoric stresses and temperature. The systematic creep testing of bentonite-based specimens helped develop a standard testing procedure applicable for analyzing the similar characteristics of shale or clay-like materials in different geologic conditions outside repository science, including in civil engineering and infrastructure projects, underground and open pit mining, and deep drilling.

58 GEOSCIENCES↗

Renewable Aromatics from Syngas

This study focuses on developing a catalytic process for the aromatization of mixed olefin (comprised of C 2 -C 6 ) over various metal doped zeolites towards the formation of large aromatics (preferably C 8 -C 16 ) compliance to the sustainable aviation fuel (SAF). Experiments were carried out using model olefin feedstocks containing either ethylene (C 2 ) or mixture of C 2 and C 3+ olefins. Both the catalyst composition and process parameters were evaluated in detail to identify their impact on the formation large aromatics. We specifically focus on the aromatization of ethylene as the model reaction and evaluated the impact of C 2+ olefins and paraffins that may present in the real feedstock. In all the reaction condition, aromatization of ethylene was used as the baseline to evaluate the effect of larger olefins or paraffins. Our results show that at this reaction condition paraffins remained either inert or show positive impact on the formation of large aromatics. While C 2 and C 3 olefins are highly reactive towards aromatization during reaction condition, large olefins are less reactive and thus, strategy was developed to oligomerize these large olefins (C 4+ ) alongside the aromatization of smaller olefins (C 2 /C 3 ).

10 SYNTHETIC FUELS↗

Evaluating Impacts of CO2 and CH4 Gas Intrusion into an Unconsolidated Aquifer: Fate of As and Cd

Abstract The sequestration of carbon dioxide (CO2) in deep underground reservoirs has been identified as an important strategy to decrease atmospheric CO2 levels and mitigate global warming, but potential risks on overlying aquifers currently lack a complete evaluation. In addition to CO2, other gases such as methane (CH4) may be present in storage reservoirs. This paper explores for the first time the combined effect of leaking CO2 and CH4 gasses on the fate of major, minor and trace elements in an aquifer overlying a potential sequestration site. Emphasis is placed on the fate of arsenic (As) and cadmium (Cd) released from the sediments or present as soluble constituents in the leaking brine. Results from macroscopic batch and column experiments show that the presence of CH4 (at a concentration of 1 % in the mixture CO2/CH4) does not have a significant effect on solution pH or the concentrations of most major elements (such as Ca, Ba, and Mg). However, the concentrations of Mn, Mo, Si and Na are inconsistently affected by the presence of CH4 (i.e., in at least one sediment tested in this study). Cd is not released from the sediments and spiked Cd is mostly removed from the aqueous phase most likely via adsorption. The fate of sediment associated As [mainly sorbed arsenite or As(III) in minerals] and spiked As [i.e., As5+] is complex. Possible mechanisms that control the As behavior in this system are discussed in this paper. Results are significant for CO2 sequestration risk evaluation and site selection and demonstrate the importance of evaluating reservoir brine and gas stream composition during site selection to ensure the safest site is being chosen.

CO2 sequestration↗

Effect of Cooling Rate on Nano-Eutectic Formation in Laser Surface Remelted and Rare Earth Modified Hypereutectic Al-20Si Alloys

Laser Surface Remelting (LSR) was applied to arc-melted Al-20Si-0.2Sr, Al-20Si-0.2Ce, and Al-20Si hypereutectic alloys to refine microstructures. Experiments revealed that microstructures in the melt pool varied from fully eutectic to a mixture of Al dendrites and inter-dendritic eutectic. We calculated cooling rates using the Eagar-Tsai model and correlated cooling rates with characteristic microstructures, revealing that a cooling rate on the order of 104 K/s could lead to maximized fully eutectic microstructure morphology. Due to rapid solidification, the Si composition in the LSR eutectic was measured at 18.2 wt.%, higher than the equilibrium eutectic composition of 12.6 wt.%Si. Compared to Al-20Si, Ce addition had no significant effect on the volume fraction of the fully eutectic structure but refined Si fibers to approximately 30 nm in diameter. Sr addition did not further refine the diameter of eutectic Si fibers compared to Al-20Si but increased the volume fraction of the fully eutectic microstructure morphology. The refinement ratio (φ) of the Si fiber diameter from the bottom of the melt pool to the surface for the three alloys was similar, at around 28%. The established correlation between the cooling rate and the size and morphology of the microstructure within the melt pool will enable tailoring of the microstructure in laser-processed as well as deposited alloys for high strength and plasticity.

36 MATERIALS SCIENCE↗

In the search for extraterrestrial life

The study of stellar, planetary and galactic evolution leads to the conclusion that the phenomenon of life must be coursing through the universe. It is estimated, by means of telescopic sampling, that there are billions of stars capable of having those photochemical reactions necessary for the origin of life. One approach in the search for other life would be to deploy men and instruments in spacecraft. Radio contact with other civilizations is another approach. Finally, the question might be approached by considering life as an inevitable consequence of the evolution of matter. A survey of Martian characteristics shows the possibility of life there to be dubious. The possibility of life in other parts of the galaxy is supported by a fundamental conclusion of living matter that all organisms have a common chemical ancestry. The experiment of Urey and Miller, wherein four amino acids were obtained by subjecting a mixture of methane, ammonia, and water to an electric arc, is believed to duplicate the initial organic syntheses which led to the emergence of life on earth.

Ponnamperuma, C.↗

Gaseous sodium sulfate formation in flames and flowing gas environments

Formation of Na2SO4(g) in flames and hot flowing gas systems was studied by high pressure, free-jet expansion, modulated molecular beam mass spectrometric sampling. Fuel-lean CH4-O2 flames doped with SO2, H2O and NaCl yielded the gaseous Na2SO4 molecule in residence times of less than one millisecond. Intermediate species NaSO2(g) and NaSO3(g) were also observed and measured. Composition profiles were obtained for all reaction products. Nonflame flowing gas experiments showed that Na2SO4 and NaSO3 gaseous molecules were formed at 1140 C in mixtures of O2, H2O(g), SO2 and NaCl(g). Experimental results are compared with calculated equilibrium thermodynamic predictions.

Stearns, C. A.↗

Gaseous sodium sulfate formation in flames and flowing gas environments

Formation of Na2SO4(g) in flames and hot flowing gas systems was studied by high pressure, free-jet expansion, modulated molecular beam mass spectrometric sampling. Fuel-lean CH4-O2 flames doped with SO2, H2O and NaCl yielded the gaseous Na2SO4 molecule in residence times of less than one millisecond. Intermediate species NaSO2(g) and NaSO3(g) were also observed and measured. Composition profiles were obtained for all reaction products. Non-flame flowing gas experiments showed that Na2SO4 and NaSO3 gaseous molecules were formed at 1140 C in mixtures of O2, H2O(g), SO2 and and NaCl(g). Experimental results are compared with calculated equilibrium thermodynamic predictions.

Stearns, C. A.↗

Thermophysical property data: Who needs them?

Specific examples are cited to illustrate the universal needs and demands for thermophysical property data. Applications of the principle of similarity in fluid mechanics and heat transfer and extensions of the principle to fluid mixtures are discussed. It becomes quite clear that no matter how eloquent theories (or experiments) in fluid mechanics or heat transfer are, results of their application can be no more accurate than the thermophysical properties required to transform these theories into practice - or in the case of an experiment, to reduce the data. Present day projects take place on such a scale that the need for international standards groups and mutual cooperation is evident.

Hendricks, R. C.↗