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At least 19 records

Low temperature dry reforming of methane using Ru-Ni-Mg/ceria-zirconia catalysts: Effect of Ru loading and reduction temperature

Dry reforming catalysts, especially those with activity at moderate temperatures, have been intensely investigated to enhance the conversion of biogas. Here, Ru is evaluated as a promoter for Ni-Mg based catalysts. Catalysts based on 1.4 wt%Ni-1.0 wt%Mg-Ce 0.6 Zr 0.4 O 2 with Ru (0.02–0.32 wt%) were prepared using incipient wetness. The reducibility of the catalysts and conversions increased with increasing Ru content. Increases in conversions with increasing Ru loading was attributed to the additional active sites and synergistic effect between Ru and Ni, which weakened Ni-Mg interactions. Samples showed dry reforming activity at low temperatures (450–510 °C). Reaction rates and activation energies of higher loading Ru samples (1.4 wt%Ni-1.0 wt%Mg/Ce 0.6 Zr 0.4 O 2 with 0.16 and 0.32 wt%Ru) decreased when the reduction temperature was raised from 300 to 400 °C. A 20 h TOS study showed stable catalytic activity with minimal coke deposition. Furthermore, the results suggest that Ru is an alternative to Pt in promoting low temperature dry reforming of methane.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Imaging the oblique propagation of electrons in germanium crystals at low temperature and low electric field

Excited electrons in the conduction band of germanium collect into four energy minima, or valleys, in momentum space. These local minima have highly anisotropic mass tensors which cause the electrons to travel in directions which are oblique to an applied electric field at sub-Kelvin temperatures and low electric fields, in contrast to the more isotropic behavior of the holes. This experiment produces a full two-dimensional image of the oblique electron and hole propagation and the quantum transitions of electrons between valleys for electric fields oriented along the [0,0,1] direction. Charge carriers are excited with a focused laser pulse on one face of a germanium crystal and then drifted through the crystal by a uniform electric field of strength between 0.5 and 6 V/cm. The pattern of charge density arriving on the opposite face is used to reconstruct the trajectories of the carriers. Measurements of the two-dimensional pattern of charge density are compared in detail with Monte Carlo simulations developed for the Cryogenic Dark Matter Search (SuperCDMS) to model the transport of charge carriers in high-purity germanium detectors.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Technetium-99 Behavior in Low-Temperature, Low-Pressure Evaporation Systems at the Hanford Site - 18461

This paper seeks to provide a technical basis for predicting the behavior of Technetium-99 (Tc-99) in the Effluent Management Facility (EMF) evaporator during the Direct Feed Low-Activity Waste (DFLAW) mission at the Hanford Site. This is done by using the 242-A Evaporator and the DM10 Melter System evaporator as analogues for the predicted design and operating strategy of the EMF evaporator. The focus of this investigation is to establish how Tc-99 behavior coincides with the behavior of several process variables (e.g. feed Tc-99 concentrations, feed sources, extent of evaporative concentration) associated with low-temperature, low-pressure evaporator operations. The primary measure of Tc-99 behavior was the partitioning of Tc-99 from the feed stream into the condensate stream (i.e. boil-off) of the evaporators. Analysis of 242-A and DM10 Melter System evaporator data allowed for the identification of the following trends regarding Tc-99 behavior in low-temperature, low-pressure evaporator systems: Tc-99 partitions minimally from the feed to the condensate stream and Tc-99 partitions consistently across a variety of operating and feed conditions. Given the similarities in design and operating strategies between the studied evaporator systems and the EMF evaporator, it is reasonable to suggest that these trends can be used to aid in planning for future EMF operations. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Mainstream nitrogen removal from low temperature and low ammonium strength municipal wastewater using hydrogel-encapsulated comammox and anammox

Application of partial nitritation (PN)-anammox to mainstream wastewater treatment faces challenges in low water temperature and low ammonium strength. In this study, a continuous flow PN-anammox reactor with hydrogel-encapsulated comammox and anammox was designed and operated for nitrogen removal from mainstream wastewater with low temperature. Long-term operation with synthetic and real wastewater as the feed demonstrated nearly complete ammonium and total inorganic nitrogen (TIN) removal by the reactor at temperatures as low as 10 °C. A significantly decreased nitrogen removal performance and biomass activity was observed in the reactor at 4 °C before a selective heating strategy was employed. A novel heating technology using radiation to heat carbon black co-encapsulated in the hydrogel matrix with biomass was used to selectively heat biomass but not water in the treatment system. This selective heating technology enabled nearly complete ammonium removal and 89.4 ± 4.3 % TIN removal at influent temperature of 4 °C and reactor temperature 5 °C. Activity tests suggested selective heating brought the biomass activity at influent temperatures of 4 °C and reactor temperature 5 °C to a level comparable to that at 10 °C. Comammox and anammox were consistently present in the system and spatially organized in the hydrogel beads as revealed by qPCR and fluorescence in-situ hybridization (FISH). The abundance of comammox largely decreased by 3 orders of magnitude during the operation at 4 °C, and rapidly recovered after the application of selective heating. The anammox-comammox technology tested in this study essentially enabled mainstream shortcut nitrogen removal, and the selective heating ensured good performance of the technology at temperature as low as 5 °C.

54 ENVIRONMENTAL SCIENCES↗

Defect evolution in single crystalline tungsten following low temperature and low dose neutron irradiation

The tungsten plasma-facing components of fusion reactors will experience an extreme environment including high temperature, intense particle fluxes of gas atoms, high-energy neutron irradiation, and significant cyclic stress loading. Irradiation-induced defect accumulation resulting in severe thermo-mechanical property degradation is expected. For this reason, and because of the lack of relevant fusion neutron sources, the fundamentals of tungsten radiation damage must be understood through coordinated mixed-spectrum fission reactor irradiation experiments and modeling. In this study, high-purity (110) single-crystal tungsten was examined by positron annihilation spectroscopy and transmission electron microscopy following low-temperature (~90 °C) and low-dose (0.006 and 0.03 dpa) mixed-spectrum neutron irradiation and subsequent isochronal annealing at 400, 500, 650, 800, 1000, 1150, and 1300 °C. The results provide insights into microstructural and defect evolution, thus identifying the mechanisms of different annealing behavior. Following 1 h annealing, ex situ characterization of vacancy defects using positron lifetime spectroscopy and coincidence Doppler broadening was performed. The vacancy cluster size distributions indicated intense vacancy clustering at 400 °C with significant damage recovery around 1000 °C. Coincidence Doppler broadening measurements confirm the trend of the vacancy defect evolution, and the S–W plots indicate that only a single type of vacancy cluster is present. Furthermore, transmission electron microscopy observations at selected annealing conditions provide supplemental information on dislocation loop populations and visible void formation. This microstructural information is consistent with the measured irradiation-induced hardening at each annealing stage. This provides insight into tungsten hardening and embrittlement due to irradiation-induced matrix defects.

Hu, Xunxiang↗

Progress Towards the Reality of Low-Temperature Critical Experiments with Low-Temperature TEX

Integral benchmarks for criticality safety do not exist below room temperature. Incredible support for below room temperature benchmarks is present across the international community. Validation of low-temperature neutron cross sections is necessary to verify any operation at temperatures below room temperature which is typically observed in environments far from the equator. For example, a fissile material transportation truck may routinely observe ambient temperatures down to -40°C, which is the lower temperature bound of the normal conditions of transportation defined in the United States Title 10 Code of Federal Regulations §71.71c2. Similarly, the IAEA, which contains 176 member states, has the same requirement for subcriticality for fissile material transportation. Additionally, sub-room temperature benchmarks can validate newly produced cross sections, that include novel thermal scattering laws, from North Carolina State University. A six-case experiment designed based off the TEX-HEU baseline experiments has been proposed utilizing a chilled vacuum chamber capable of cooling the HEU stack down to -50°C. The six proposed configurations span the entire neutron fission energy range and can be tested at intermediate temperatures between room temperature and -40°C. Of the six configurations, the fastest case utilizes nearly 135 kg of HEU. Understanding the system is required prior to critical experiment operations. In order to test the functionality of the system, testing with surrogate fuel materials has been conducted. The following discusses the design of the low temperature TEX (LT-TEX) experiment as well as the progress made via surrogate testing towards a reality in which low-temperature integral benchmarks exist in the International Criticality Safety Benchmark Evaluation Project (ICSBEP).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Low-temperature heat capacity and localized vibrational modes in natural and synthetic tetrahedrites

The heat capacity of natural (Cu{sub 12−x} (Fe, Zn, Ag){sub x}(Sb, As){sub 4}S{sub 13}) and synthetic (Cu{sub 12−x}Zn{sub x}Sb{sub 4}S{sub 13} with x = 0, 1, 2) tetrahedrite compounds was measured between 2 K and 380 K. It was found that the temperature dependence of the heat capacity can be described using a Debye term and three Einstein oscillators with characteristic temperatures that correspond to energies of ∼1.0 meV, ∼2.8 meV, and ∼8.4 meV. The existence of localized vibrational modes, which are assigned to the displacements of the trigonally coordinated Cu atoms in the structure, is discussed in the context of anharmonicity and its effect on the low lattice thermal conductivity exhibited by these compounds.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Carbon capture turned upside down: high-temperature adsorption & low-temperature desorption (HALD)

Carbon capture & sequestration (CCS) could reduce CO 2 emissions from large fossil-fuel power plants on the short term, but the high energy penalty of the process hinders its industrial deployment. Moreover, the utility of nanoporous materials, known to be selective for the CO 2 /N 2 separation, is drastically reduced due to the competitive adsorption with H 2 O. Taking advantage of the power plant's waste heat to perform CCS while at the same time surmounting the negative effect of H 2 O is therefore an attractive idea. We propose an upside-down approach for CCS in nanoporous materials, high-temperature adsorption & low-temperature desorption (HALD), that exploits the temperature-dependent competitive adsorption of CO 2 and H 2 O. First, we provide a theoretical background for this entropy-driven behavior and demonstrate under what conditions competitive adsorption can be in favor of CO 2 at high temperature and in favor of H 2 O at low temperature. Then, molecular simulations in all-silica MFI provide a proof of concept. The International Zeolite Association database is subsequently screened for potential candidates and finally, the most promising materials are selected using a post-Pareto search algorithm. The proposed post-Pareto approach is able to select the material that shows an optimal combination of multiple criteria, such as CO 2 /H 2 O selectivity, CO 2 /N 2 selectivity, CO 2 uptake and H 2 O uptake. As a conclusion, this work provides new perspectives to reduce the energy requirement for CCS and to overcome the competitive adsorption of H 2 O.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Signature of Ferromagnetic Phase at Low Temperature in Low-Doped La{sub 0.88}Ca{sub 0.12}MnO{sub 3} Single Crystal

The confirmation of ferromagnetism at low temperature in a low-doped manganites system is always debatable. It is for the first time, electrical, magnetic, and thermal properties have been measured for manganites single crystal of La{sub 0.88}Ca{sub 0.12}MnO{sub 3} by using a floating-zone method. The electrical resistivity shows a perceptible change of resistance at a low temperature which can be viewed as a signature of the ferromagnetic phase. The ferromagnetic phase of the investigated La{sub 0.88}Ca{sub 0.12}MnO{sub 3} single crystal with Curie temperature of T{sub C} = 120 K which is in closed agreement with ac-susceptibility measurement. An analysis of the specific heat suggests the transition peak (T{sub P}) coincides with the T{sub C} and attains 1.2 J mol{sup −1} K at 116 K. The magnetoresistance (MR) and temperature coefficient of resistance (TCR) were found to be 69% and 10% respectively, which expands its subtle potential for applications in spintronics and thermistor.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Characterisation of ODS Fe-14Cr-2W-0.3Ti before and after high temperature triple and low temperature single ion irradiations

Highlights: • Nanoparticles stable after high temperature triple-beam and low temperature single-beam irradiation • Samples appear to have maintained the composition after both irradiations. • Slight decrease of the nanoparticle sizes below 5 nm after both irradiations • There appears to be incomplete dissolution of smaller nanoparticles after both irradiations. - Abstract: Oxide dispersion strengthened reduced activation ferritic steels are being considered as structural materials for future fusion reactors and Gen IV fission reactors. In this work, the stability of the nanometric oxides after being irradiated at different conditions and temperatures has been investigated. A Fe-14Cr-2W-0.3Ti-0.3Y{sub 2}O{sub 3} alloy was simultaneously triple-beam irradiated at 600 °C with Fe, He and H ions. The same alloy was irradiated with Fe ions at − 80 °C. The microstructure of this alloy was investigated using Transmission Electron Microscopy, Atom Probe Tomography and nanoindentation before and after the irradiations. There were no significant changes in the morphology and chemical composition of the nanoparticles after the irradiations, although the size of the smaller ones tends to decrease for both irradiation conditions. Small irradiation-induced bubbles were present after the triple simultaneous irradiation at high temperature. Nanoindentation also shows no significant differences with a slight increase in hardness for the sample irradiated at low temperature, while softening appears in the high temperature irradiation.

36 MATERIALS SCIENCE↗

Low temperature oxidation of plutonium

The initial oxidation of gallium stabilized {delta}-plutonium metal at 193 K has been followed using x-ray photoelectron spectroscopy. On exposure to Langmuir quantities of oxygen, plutonium rapidly forms a trivalent oxide followed by a tetravalent plutonium oxide. The growth modes of both oxides have been determined. Warming the sample in vacuum, the tetravalent oxide reduces to the trivalent oxide. The kinetics of this reduction reaction have followed and the activation energy has been determined to be 38.8 kJ mol{sup -1}.

36 MATERIALS SCIENCE↗

Advancing a Low-Temperature, Low-Cost Direct Air Capture System Based on Organic Chemistry

Holocene Climate Corporation (Holocene) partnered with Oak Ridge National Laboratory (ORNL) to conduct bench-scale testing of a new optimized Direct Air Capture (DAC) process to assist the U.S. Department of Energy (DOE) in achieving the Carbon Negative Shot target of under $\$$100/net tonne CO₂ removed by 2031. Holocene’s DAC process for carbon dioxide (CO₂) removal uses amino acids and guanidine compounds, an ORNL-invented chemical process and licensed by Holocene. Holocene will use this novel chemistry to develop a new process and deploy the technology commercially.

36 MATERIALS SCIENCE↗