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At least 73 records · Page 4

Microwave-Mediated ammonia synthesis over Co 2 Mo 3 N catalysts at low pressures

The Haber-Bosch process for ammonia (NH 3 ) synthesis is a major contributor to greenhouse gas emissions and is responsible for > 2 % of the world’s energy consumption each year encouraging the need for alternative renewable-based options. Here, this study investigates an earth-abundant ternary metal nitride (i.e., Co 2 Mo 3 N) catalyst to develop a renewable-based NH 3 synthesis approach, utilizing an energy-efficient microwave-assisted route. Using a combination of spectroscopic and catalytic measurements coupled with surface analysis techniques, Co 2 Mo 3 N was evaluated as a stable and efficient NH 3 synthesis catalyst. Results presented here demonstrate NH 3 synthesis on Co 2 Mo 3 N at ~420 °C and ambient pressure yield ~0.7 mmolNH3.g cat -1 .h -1 and up to ~12 mmol NH3 .g cat -1 .h -1 at 28 bar under microwave irradiation. Co 2 Mo 3 N displayed an activation energy of ~72 kJ.mol -1 and yielded NH 3 following first-order kinetics with respect to both H 2 and N 2 . These studies illustrate the potential of using this catalyst for a sustainable, cost-effective, and environmentally friendly approach to producing NH 3 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Low-pressure methanol synthesis from CO 2 over metal-promoted Ni-Ga intermetallic catalysts

Ni-Ga and M-Ni-Ga (M = Au, Co, Cu) catalysts were evaluated for methanol synthesis from CO 2 at 10 bar and 200-270°C. The following trend in turnover frequency (TOF) for CO 2 hydrogenation was observed: AuNiGa > CuNiGa > NiGa > CoNiGa, where TOF increased with decreasing catalyst affinity for CO. The presence of a third metal was found to influence both the formation of the Ni-Ga intermetallic phase as well as the number of available sites for CO chemisorption. Phase formation, catalyst composition and stability were evaluated using therm ogravimetric analysis (TGA), X-ray diffraction (XRD), X-ray fluorescence (XRF), scanning transmission electron microscopy and energy dispersive X-ray spectroscopy (STEM-EDX). Au-Ni-Ga, which showed a nearly 4-fold improvement in TOF at 263°C and 10 bar compared to Ni-Ga, consisted of Ni 3 Ga particles decorated with Au, as evidenced by post catalysis characterization.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Metastability exchange optical pumping of 3 He at low pressure and high magnetic field

We report systematic studies on metastability exchange optical pumping of 3 He nuclei have been performed at Jefferson Lab using a 1-torr sealed cell at magnetic fields from 2 to 4 T. The effects of the discharge intensity, pump laser power and pumping transition schemes on achievable nuclear polarization and pumping rate have been investigated. A maximum steady-state nuclear polarization of about 75% has been obtained. This work provides a baseline for the development of the novel polarized 3 He target for CLAS12 at Jefferson Lab.

47 OTHER INSTRUMENTATION↗

A characterization of plasma properties of a heterogeneous magnetized low pressure discharge column

An approach is presented for characterizing heterogeneous magnetized plasma discharge tubes through the scattering of electromagnetic plane waves. Here, we formulate the analytical problem of electromagnetic scattering from a gyrotropic plasma column. The scattering accounts for the heterogeneous composition of the cylindrical discharge plasma and facilitates determining its propensity for gyrotropic scattering, particularly when electron collisional damping may be prevalent. The analytical results are validated using computational simulations. Scattered fields from the magnetized plasma are measured experimentally, and, by comparing the analytical and experimental results, the unknown parameters of the discharge, i.e., characteristic plasma and electron collisional damping frequencies, are determined. The technique is relatively straight-forward to use and removes the need for commercial computational electromagnetic simulations when experimental data on scattering characteristics of such cylindrical discharge plasmas are available.

36 MATERIALS SCIENCE↗

Low-Pressure Electrochemical Synthesis of Complex High-Pressure Superconducting Superhydrides

There is great current interest in multicomponent superhydrides due to their unique quantum properties under pressure. A remarkable example is the ternary superhydride Li 2 MgH 16 computationally identified to have an unprecedented high superconducting critical temperature T c of ~470 K at 250 GPa. However, the very high synthesis pressures required remains a significant hurdle for detailed study and potential applications. In this Letter, we evaluate the feasibility of synthesizing ternary Li-Mg superhydrides by the recently proposed pressure-potential (P 2 ) method that uniquely combines electrochemistry and applied pressure to control synthesis and stability. Furthermore, the results indicate that it is possible to synthesize Li-Mg superhydrides at modest pressures by applying suitable electrode potentials. Using pressure alone, no Li-Mg ternary hydrides are predicted to be thermodynamically stable, but in the presence of electrode potentials, both Li 2 MgH 16 and Li 4 MgH 24 can be stabilized at modest pressures. Three polymorphs are predicted as ground states of Li 2 MgH 16 below 300 GPa, with transitions at 33 and 160 GPa. The highest pressure phase is superconducting, while the two at lower pressures are not. Our findings point out the potentially important role of the P 2 method in controlling phase stability of complex multicomponent superhydrides.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

High-temperature oxidation behavior of the SiC layer of TRISO particles in low-pressure oxygen

Surrogate tristructural-isotropic (TRISO)-coated fuel particles were oxidized in 0.2 kPa O 2 at 1200–1600°C to examine the behavior of the SiC layer and understand the mechanisms. The thickness and microstructure of the resultant SiO 2 layers were analyzed using scanning electron microscopy, focused ion beam, and transmission electron microscopy. The majority of the surface comprised smooth, amorphous SiO 2 with a constant thickness indicative of passive oxidation. The apparent activation energy for oxide growth was 188 ± 8 kJ/mol and consistent across all temperatures in 0.2 kPa O 2 . The relationship between activation energy and oxidation mechanism is discussed. Raised nodules of porous, crystalline SiO 2 were dispersed across the surface, suggesting that active oxidation and redeposition occurred in those locations. These nodules were correlated with clusters of nanocrystalline SiC grains, which may facilitate active oxidation. So these findings suggest that microstructural inhomogeneities such as irregular grain size influence the oxidation response of the SiC layer of TRISO particles and may influence their accident tolerance.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Preliminary results from Low Pressure Steam Oxidation Testing of ALD ZrN and ZrO2 Coating Deposited over UCN Fuel Kernels

Steam oxidation testing was used to investigate as-developed 100 nm ALD ZrN and 1000 nm ZrO 2 coatings deposited over UC1-xNx fuel kernels. The results of these tests were compared against oxidation of uncoated kernels. This work was performed to support development of coatings which both provide high temperature Zr metal diffusion barrier and also provide resistance against oxidation, especially against high temperature steam and/or air. This work was performed in collaboration with Oak Ridge National Laboratory (ORNL), using ORNL-provided samples. The oxidation tests yielded valuable information, including relative differences in performance of different coating materials and coating thicknesses.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗