Dendrite-free Li deposition using trace-amounts of water as an electrolyte additive
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Qian, Jiangfeng↗
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Ultrasonication-assisted trace amount solvent synthesis of Cs 4 PbBr 6 crystal with ultra-bright green light emission
Cs 4 PbBr 6 crystals have been synthesized by an ultrasonication-assisted trace amount polar solvent method. The prepared green Cs 4 PbBr 6 material was found to have high photoluminescence (PL) brightness and 10 ns PL lifetime. The prepared green light emitting device can achieve the maximum brightness of 3.8 × 10 9 cd/m 2 , which is nearly 100 times higher than a wick. The white light emitting device based on Cs 4 PbBr 6 crystals has better performance than commercial products, which can cover 32.3% of the color gamut and achieves 107.3% coverage for International Commission on Illumination (CIE)1931 and 84.8% coverage for CIE1976.
36 MATERIALS SCIENCE↗
Enhanced electrocatalytic activity and stability of Pd 3 V/C nanoparticles with a trace amount of Pt decoration for the oxygen reduction reaction
In this study, carbon supported Pd 3 V bimetallic alloy nanoparticles (Pd 3 V/C) have been successfully synthesized via a simple impregnation–reduction method, followed by high temperature treatment under a H 2 atmosphere. Electrochemical tests reveal that the half-wave potential of Pd 3 V/C-500 shifts positively 40 mV compared with Pd/C. However, the catalytic activity of Pd 3 V/C-500 suffers from serious degradation after 1k cycles. By a spontaneous displacement reaction or co-reduction method, a trace amount of Pt was decorated on the surface or inside of the Pd 3 V/C nanoparticles. The catalytic activity and stability of the Pd 3 V@Pt/C and Pt-Pd 3 V/C catalysts for the oxygen reduction reaction (ORR) are enhanced significantly, and are comparable to commercial Pt/C. In addition, the Pt mass activity of Pd 3 V@Pt/C and Pt-Pd 3 V/C improves by factors of 10.9 and 6.5 at 0.80 V relative to Pt/C. Moreover, Pt-decorated Pd 3 V/C nanoparticles show almost no obvious morphology change after durability tests, because the Pt-rich shell plays an important role in preventing degradation.
36 MATERIALS SCIENCE↗
Suppressing ion migration in metal halide perovskite via interstitial doping with a trace amount of multivalent cations
Cations with suitable sizes to occupy an interstitial site of perovskite crystals have been widely used to inhibit ion migration and promote the performance and stability of perovskite optoelectronics. However, such interstitial doping inevitably leads to lattice microstrain that impairs the long-range ordering and stability of the crystals, causing a sacrificial trade-off. Here, we unravel the evident influence of the valence states of the interstitial cations on their efficacy to suppress the ion migration. Incorporation of a trivalent neodymium cation (Nd 3+ ) effectively mitigates the ion migration in the perovskite lattice with a reduced dosage (0.08%) compared to a widely used monovalent cation dopant (Na + , 0.45%). As a result, the photovoltaic performances and operational stability of the prototypical perovskite solar cells are enhanced with a trace amount of Nd 3+ doping while minimizing the sacrificial trade-off.
36 MATERIALS SCIENCE↗
Removal of Trace Amounts of Co-60 from NPP Waste Water Using UV-C Irradiation, TiO{sub 2} and Co-Treat Inorganic Ion Exchange Media - 16025
The removal of Co-60 from an aqueous nuclear liquid waste obtained from a BWR NPP was tested using a two-step process. In the first phase the liquid waste was oxidized with ultraviolet irradiation at 254 nm (UV-C irradiation) together with a photo-catalyst, TiO{sub 2} P25 AEROXIDE, to degrade the organic complexing agents present in the solution. During some of the experiments it was noticed that TiO{sub 2} P25 AEROXIDE also removed Co-60 from the solution. In the second phase the UV-C irradiated solution was mixed with inorganic ion exchange media, Co-Treat, to remove the rest of Co-60 from the solution. The effect of pH and contact time with UV-C irradiation were evaluated and both had a noticeable effect on the results. Best results were attained when pH of the initial test solution was lowered to 3.5 ± 0.2 before the UV-C irradiation. From the initial Co-60 activity, 2.2 Bq/ml, the activity decreased to 0.03 ± 0.01 Bq/ml after 24 hours of UV-C irradiation together with the photo-catalyst and mixing with Co-Treat. (authors)
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
Effect of trace amounts of added Sc on microstructure and mechanical properties of 2055 aluminum alloy
Highlights: • Effect of trace Sc on microstructure and mechanical properties in 2055 Al-alloy was investigated. • T{sub 1} is the main strengthening phase in Sc free and Sc added 2055 alloy at the aging temperature of 175°C and 200°C. • The refinement of T{sub 1} by Sc addition depends on the aging temperature. • Mechanical properties were deteriorated by Sc at the aging temperature of 175°C and improved at 200°C aging treatment. - Abstract: The effects of Sc additions and isothermal aging on the microstructure and mechanical properties of 2055 aluminum alloy have been investigated. The isothermal aging temperatures investigated were 175 °C and 200 °C. Results show that the aging temperature does not affect the type of precipitates in both Sc-free and Sc-added 2055 Al alloys. While remarkable changes in the size and number density of T{sub 1} (Al{sub 2}CuLi) precipitates have been observed. For samples aged at 175 °C for 8 h, the average length of T{sub 1} precipitates was increased from 39.9 nm to 45.6 nm, the number density decreased from 5.77 × 10{sup 22} m{sup −3} to 3.68 × 10{sup 22} m{sup −3} after Sc addition. On the contrary, when samples were aged at 200 °C for 8 h, the length decreased from 59.89 nm to 43.32 nm and number density increased from 2.13 × 10{sup 22} m{sup −3} to 3.00 × 10{sup 22} m{sup −3} by adding trace Sc. Slight deterioration of tensile strength and yield strength with higher ductility was founded at the aging temperature of 175 °C for 8 h due to the larger size and lower number density of T{sub 1} precipitates along with the formation of a W (AlCuSc) phase during the casting or homogenization processes. When aging temperature increased to 200 °C, tensile strength and yield strength were significantly improved by Sc addition without losing ductility. Highly dense fine T{sub 1} precipitates take responsible for the strength improvement, and to some extent it compensated the strength loss caused by the formation of W phase. A “vacancy-prison” mechanism was adopted to explain the effect of Sc additions on the precipitation of T{sub 1} phase as a function of aging temperature.
36 MATERIALS SCIENCE↗
Atomic rearrangement from disordered to ordered Pd-Fe nanocatalysts with trace amount of Pt decoration for efficient electrocatalysis
The structure-activity relationship between the ORR performance and the surface electronic structure of Pd is constructed and the ORR performance are rationally modified via the structural transition from disordered face centered cubic phase (fcc, D-PdFe/C) to ordered intermetallic tetragonal phase (fct, O-PdFe/C). When the small amount of Pt atoms decorated on O-PdFe/C surface forming O-PdFe@Pt/C core-shell structure, the sublayer of Pd and Fe atoms may cause the lattice contraction of surface Pt and then weak the bonding energy on O-PdFe@Pt/C catalyst relative to bulk Pt/C, which is further illustrated by density functional theory (DFT) calculation. The weakened oxygen affinity results in the enhancement of ORR performance on O-PdFe@Pt/C. Here, for a practical application, the well-constructed O-PdFe@Pt/C exhibits higher voltage and peak power density than D-PdFe@Pt/C and Pt/C when applied as the air-breathing cathode material in Zn-air battery.
25 ENERGY STORAGE↗
Inhibition of Reaction Layer Formation on MgO(100) by Doping with Trace Amounts of Iron
Despite extensive research on MgO’s reactivity in the presence of CO 2 under various conditions, little is known about whether impurities incorporated into the solid, such as iron, enhance or impede hydroxylation and carbonation reactions. The purity of the MgO required for the successful implementation of MgO looping as a direct air capture technology affects the deployment costs. With this motivation, we tested how incorporated iron impacts MgO (100) reactivity and passivation layer formation under ambient conditions by using atomic force microscopy, electron microscopy, and synchrotron-based X-ray scattering. Based on electron microprobe analysis, our MgO samples were 0.5 wt % iron, and Mössbauer spectroscopy results indicated that 70% of the iron is present as Fe(II). We find that even these low levels of iron dopants impeded both the hydroxylation at various relative humidities (10%, 33%, 75%, and >95%) and carbonation in CO 2 (33%, 75%, and >95%) on the (100) surface. Crystalline reaction products were formed. Reaction layers on the sample were easily removed by exposing the sample to deionized water for 2 min. Overall, our findings demonstrate that the presence of iron dopants slows the reaction rate of MgO, indicating that MgO without incorporated iron is preferable for mineral looping applications.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
A new highly enriched 233 U reference material for improved simultaneous determination of uranium amount and isotope amount ratios in trace level samples
A highly-enriched 233 U reference material (>0.99987 n( 233 U)/n(U)) has been prepared and characterized for use as an isotope dilution mass spectrometry spike. An ion exchange separation was performed on 1 g of high purity 233 U to further reduce trace amounts of contaminant Pu in the material. The purified 233 U was then prepared as a master solution which was analyzed for molality of uranium by modified Davies and Gray titration. A portion of the master solution was quantitatively diluted and dispensed for reference material units. Selected units were analyzed for verification of uranium amount and to characterize uranium isotope amount ratios by multi-collector inductively couple plasma mass spectrometry. Furthermore, modelling of spike-corrected isotopic data show that the new spike will enable simultaneous measurements of uranium amount and isotope amount ratios with resulting uncertainties that are substantially less sensitive to over spiking than widely used 233 U certified reference materials.
233U↗
Electronic and Steric Influences of Pendant Amine Groups on the Protonation of Molybdenum Bis(dinitrogen) Complexes
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bio-inspired↗
Competitive grain boundary segregation of phosphorus and carbon governs delamination crack in a ferritic steel
Highlights: • Trace amounts of P in the steel cause delamination in case of Lt-high Temp. holding. • Anisotropic microstructure did not affect the delamination in this study. • Crack-linked GBs in Lt-high Temp. steel had higher P and lower C segregation. • Crack-interrupt GBs in St-high Temp. steel had lower P and higher C segregation. • Competitive segregation controlled by high Temp. holding time affects delamination. - Abstract: The present study aims at unveiling the influence of trace amounts of phosphorus on the macro-scale delamination in a ferritic steel. Two different steels with trace amounts of phosphorus were examined to reveal the cause: One was made by long-time high temperature holding to maximize the phosphorus segregation, and the other one was made by short-time high temperature holding to minimize the phosphorus segregation. The atom probe results at the grain boundaries ahead of the delamination-related cracks provide a strong evidence that phosphorus-enrichment and carbon-depletion for the long-time high temperature holding induces a larger degree of delamination as compared to the short-time high temperature holding. Reasons for the different segregation tendency were discussed by correlating the isothermal holding time at high temperature and the competitive segregation between phosphorus and carbon.
36 MATERIALS SCIENCE↗
Optimizing detector geometry for trace element mapping by X-ray fluorescence
Trace metals play critical roles in a variety of systems, ranging from cells to photovoltaics. X-Ray Fluorescence (XRF) microscopy using X-ray excitation provides one of the highest sensitivities available for imaging the distribution of trace metals at sub-100 nm resolution. With the growing availability and increasing performance of synchrotron light source based instruments and X-ray nanofocusing optics, and with improvements in energy-dispersive XRF detectors, what are the factors that limit trace element detectability? To address this question, we describe an analytical model for the total signal incident on XRF detectors with various geometries, including the spectral response of energy dispersive detectors. This model agrees well with experimentally recorded X-ray fluorescence spectra, and involves much shorter calculation times than with Monte Carlo simulations. With such a model, one can estimate the signal when a trace element is illuminated with an X-ray beam, and when just the surrounding non-fluorescent material is illuminated. From this signal difference, a contrast parameter can be calculated and this can in turn be used to calculate the signal-to-noise ratio (S/N) for detecting a certain elemental concentration. We apply this model to the detection of trace amounts of zinc in biological materials, and to the detection of small quantities of arsenic in semiconductors. We conclude that increased detector collection solid angle is (nearly) always advantageous even when considering the scattered signal. However, given the choice between a smaller detector at 90° to the beam versus a larger detector at 180° (in a backscatter-like geometry), the 90° detector is better for trace element detection in thick samples, while the larger detector in 180° geometry is better suited to trace element detection in thin samples.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
WIPP - February 2014 operational events and the compliance re-certification application (CRA) 2014 - 15293
On Wednesday, February 5, 2014, an underground mine fire involving a salt haul truck occurred at the Waste Isolation Pilot Plant (WIPP). There were 86 workers in the mine when the fire occurred. All workers were evacuated. Nine days later, on Friday, February 14, 2014, there was an incident in the underground repository at WIPP which resulted in the release of americium and plutonium from one or more transuranic (TRU) waste containers into the environment. The release was detected by an underground continuous air monitor and then directed through high-efficiency particulate air (HEPA) filter banks located in the surface exhaust building. However, a measurable portion bypassed the HEPA filters via leakage through two ventilation system dampers and was discharged directly to the environment from an exhaust duct. No personnel were determined to have received external contamination; however, some individuals that were on site were identified through bioassay to have initially tested positive for low level amounts of internal contamination. Trace amounts of americium and plutonium were detected off-site.While significant to day-to-day operations, these events have no impact to the long-term performance of the repository. Because WIPP's re-certification is based solely on the post-closure performance of the repository (40 CFR 191, Subparts B and C), these recent events do not affect the long-term performance predictions or its technical and scientific basis. In this paper we will further explore the requirements for WIPP's re-certification, and the basis for our contention that the recent WIPP operational events do not impact long-term repository performance or have any implications on salt as a geologic disposal media, and that re-certification efforts should continue uninterrupted. (authors)
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
LINE IDENTIFICATIONS OF TYPE I SUPERNOVAE: ON THE DETECTION OF Si II FOR THESE HYDROGEN-POOR EVENTS
Here we revisit line identifications of type I supernovae (SNe I) and highlight trace amounts of unburned hydrogen as an important free parameter for the composition of the progenitor. Most one-dimensional stripped-envelope models of supernovae indicate that observed features near 6000–6400 Å in type I spectra are due to more than Si ii λ6355. However, while an interpretation of conspicuous Si ii λ6355 can approximate 6150 Å absorption features for all SNe Ia during the first month of free expansion, similar identifications applied to 6250 Å features of SNe Ib and Ic have not been as successful. When the corresponding synthetic spectra are compared with high-quality timeseries observations, the computed spectra are frequently too blue in wavelength. Some improvement can be achieved with Fe ii lines that contribute redward of 6150 Å; however, the computed spectra either remain too blue or the spectrum only reaches a fair agreement when the rise-time to peak brightness of the model conflicts with observations by a factor of two. This degree of disagreement brings into question the proposed explosion scenario. Similarly, a detection of strong Si ii λ6355 in the spectra of broadlined Ic and super-luminous events of type I/R is less convincing despite numerous model spectra used to show otherwise. Alternatively, we suggest 6000–6400 Å features are possibly influenced by either trace amounts of hydrogen or blueshifted absorption and emission in Hα, the latter being an effect which is frequently observed in the spectra of hydrogen-rich, SNe II.
79 ASTRONOMY AND ASTROPHYSICS↗
Development of an in situ temperature stage for synchrotron X-ray spectromicroscopy
In situ characterization of micro- and nanoscale defects in polycrystalline thin-film materials is required to elucidate the physics governing defect formation and evolution during photovoltaic device fabrication and operation. X-ray fluorescence spectromicroscopy is particularly well-suited to study defects in compound semiconductors, as it has a large information depth appropriate to study thick and complex materials, is sensitive to trace amounts of atomic species, and provides quantitative elemental information, non-destructively. Current in situ methods using this technique typically require extensive sample preparation. In this work, we design and build an in situ temperature stage to study defect kinetics in thin-film solar cells under actual processing conditions, requiring minimal sample preparation. Careful selection of construction materials also enables controlled non-oxidizing atmospheres inside the sample chamber such as H 2 Se and H 2 S. Temperature ramp rates of up to 300 °C/min are achieved, with a maximum sample temperature of 600 °C. As a case study, we use the stage for synchrotron X-ray fluorescence spectromicroscopy of CuIn x Ga 1–x Se 2 (CIGS) thin-films and demonstrate predictable sample thermal drift for temperatures 25–400°C, allowing features on the order of the resolution of the measurement technique (125 nm) to be tracked while heating. As a result, the stage enables previously unattainable in situ studies of nanoscale defect kinetics under industrially relevant processing conditions, allowing a deeper understanding of the relationship between material processing parameters, materials properties, and device performance.
47 OTHER INSTRUMENTATION↗
Probing the Effects of NO x and SO x Impurities on Oxy-Fuel Combustion in Supercritical CO 2 : Shock Tube Experiments and Chemical Kinetic Modeling
The direct-fired supercritical carbon dioxide cycles are one of the most promising power generation methods in terms of their efficiency and environmental friendliness. Two important challenges in implementing these cycles are the high pressure (300 bar) and high CO 2 dilution (>80%) in the combustor. The design and development of supercritical oxy-combustors for natural gas require accurate reaction kinetic models to predict the combustion outcomes. The presence of a small amount of impurities in natural gas and other feed streams to oxy-combustors makes these predictions even more complex. During oxy-combustion, trace amounts of nitrogen present in the oxidizer is converted to NO x and gets into the combustion chamber along with the recirculated CO 2 . Similarly, natural gas can contain a trace amount of ammonia and sulfurous impurities that get converted to NO x and SO x and get back into the combustion chamber with recirculated CO 2 . In this work, a reaction model is developed for predicting the effect of impurities such as NO x and SO x on supercritical methane combustion. The base mechanism used in this work is GRI Mech 3.0. H 2 S combustion chemistry is obtained from Bongartz et al. while NOx chemistry is from Konnov. The reaction model is then optimized for a pressure range of 30–300 bar using high-pressure shock tube data from the literature. It is then validated with data obtained from the literature for methane combustion, H 2 S oxidation, and NO x effects on ignition delay. The effect of impurities on CH 4 combustion up to 16 atm is validated using NO x -doped methane studies obtained from the literature. In order to validate the model for high-pressure conditions, experiments are conducted at the UCF shock tube facility using natural gas identical mixtures with N 2 O as an impurity at ~100 bar. Current results show that there is a significant change in ignition delay with the presence of impurities. A comparison is made with experimental data using the developed model and predictions are found to be in good agreement. The model developed was used to study the effect of impurities on CO formation from sCO 2 combustors. It was found that NO x helps in reducing CO formation while the presence of H 2 S results in the formation of more CO. The reaction mechanism developed herein can also be used as a base mechanism to develop reduced mechanisms for use in CFD simulations.
Energy & Fuels↗
Nuclear Considerations for the Application of Lanthanum Telluride in Future Radioisotope Power Systems
Thermoelectric-based radioisotope power systems (RPSs) produced in the United States convert the heat generated by the radioactive emission of alpha particles from plutonium dioxide ( 238 puO 2 ) into electricity by means of the Seebeck effect [1]. Certain designs for thermoelectric convertors propose the use of lanthanum telluride (La 3 Te 4 ) materials due to their significant conversion capabilities [2]. The generation of neutrons from spontaneous fission and alpha-neutron (α,n) reactions is also associated with the decay of 238 PuO 2 . A portion of these neutrons will interact with the thermoelectric materials and induce trace amounts of transmutation reactions in various lanthanum and tellurium isotopes. While very small quantities of several transmutation products are predicted, the most significant reaction channels are expected to produce trace amounts of iodine which will accumulate over time. Although iodine is classified as a halogen, it is the least reactive of the halogens, and as such, it is the most likely to be able to chemically convert back into the molecule I 2 . Since I 2 is a gas at RPS temperatures, it may be possible for iodine to attack other components in the thermoelectric cavity of an RPS system. Iodine reacts easily with metals to produce a wide variety of salts. This behavior could affect the performance of La 3 Te 4 thermoelectric devices, particularly the segmented architectures that include multiple sets of bonding and metallization layers. In this type of architecture, several segments of different thermoelectric materials are joined to increase the average thermoelectric figure of merit over a relatively large temperature gradient. It is plausible that sophisticated bonding/metallization layers could be required to join the segment interfaces to each other and to the cold- and hot-shoe materials. The long-term stability and performance of these segmented material combinations could degrade as a result of the potential formation and reactions of metal-iodide compounds at the segment interfaces. This paper (1) investigates the degree to which, if any, this process may threaten potential La 3 Te 4 thermoelectric technologies, (2) presents calculations of the amount of iodine generated over the operational life of a radioisotope thermoelectric generator design, and (3) discusses the potential effects of the resulting material's chemical reactions in a segmented couple-level architecture containing La 3 Te 4 . Conclusions drawn from combined particle transport, transmutation, and thermochemical calculations for La 3 Te 4 thermoelectric materials undergoing a notional 20-year mission scenario suggest that there is no significant potential for transmutation-induced thermoelectric (TE) performance degradation.
Smith, Michael↗