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At least 271 records · Page 15

M4SF-22LL010302062-NEA-TDB and Sorption DataBase Development

This progress report (Level 4 Milestone Number M4SF-22LL010302062) summarizes research conducted at Lawrence Livermore National Laboratory (LLNL) within the Crystalline International Collaborations Activity Number SF-22LL01030206. The activity is focused on our long-term commitment of engaging our partners in international nuclear waste repository research. This includes participation in the Nuclear Energy Agency Thermochemical Database (NEA-TDB) Project (Cindy Atkins-Duffin, Mavrik Zavarin) and development of methodologies for integrating US and international thermodynamic databases for use in SFWST Generic Disposal System Assessment (GDSA) efforts.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

M3SF-24LL010302062-NEA-TDB Management and International Collaborations in Sorption and Thermodynamic Modeling

This progress report (Level 3 Milestone Number M3SF-24LL010302062) summarizes research conducted at Lawrence Livermore National Laboratory (LLNL) within the Crystalline International Collaborations Work Package Number SF-24LL01030206. The activity is focused on our long-term commitment to engaging our partners in international nuclear waste repository research. This includes participation in the Nuclear Energy Agency Thermochemical Database (NEA-TDB) Project and development of methodologies for integrating US and international thermodynamic databases for use in SFWST Generic Disposal System Assessment (GDSA) efforts. A continuing focus for FY24 efforts is to support the US participation in the NEA-TDB effort. The focus of FY24 activities was the development of an agreement for a Phase 7 activity that will start in Q1 of 2025. Mavrik Zavarin is now the US representative on both the Management Board and the Executive group to the NEA-TDB. He is also the POC for the Cements State of the Art Report that is undergoing peer review in FY24. In FY24, we used our position on the NEA-TDB MB and EG to facilitate the integration of NEA-TDB thermochemical data with LLNL’s SUPCRTNE thermodynamic database that supports the SFWST GDSA activities. This effort is coordinated with the Argillite work package SUPCRTNE database development efforts (Wolery, 2024). The goal is to provide a downloadable database that will be hosted on LLNL’s thermodynamics website which incorporates NEA-TDB data into the LLNL database where appropriate. We also began engagement with the EURAD2 program that was initiated in FY24 by our European collaborators at the Karlsruhe Institute of Technology (KIT), Germany. The primary focus of the engagement is with WP20: DITUSC Thermodynamic database evaluation program. A kickoff meeting for this activity is planned for early FY25. Finally, we have been selected to co-host (with Clemson University) the International Conference on Chemistry and Migration Behaviour of Actinides and Fission Products in the Geosphere in 2025 (Migration2025). The meeting will be held September 21-26, 2025, in New Orleans, Louisiana, and will focus on international efforts to understand the risks of radionuclide releases into the environment. This central focus of this conference is on international efforts to develop safe disposal options for nuclear wastes. As such, we are developing a theme focused on US underground nuclear waste repository science.

58 GEOSCIENCES↗

Water sorption equilibrium and dynamics on Epon 828-Epikure 3125

Epon 828-Epikure 3125 absorbs a significant amount of water (up to 4 weight percent), but diffusion of water into the material is slow. A one cm thick open slab may take 80 days to reach equilibrium at 70 °C and five years at 20 °C.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Sorption of noble gases by solids, with reference to meteorites. I - Magnetite and carbon

The trapping of meteoritic noble gases by solids is simulated through the synthesis of 18 Fe3O4 samples at 350-720 K in a noble gas atmosphere, by means of the reactions: (1) 3Fe + 4H2O yields Fe3O4 + 4H2, using Ne, Ar, Kr and Xe; and (2) 3Fe + 4CO yields Fe3O4 + 4C + carbides, using Xe. Etching experiments suggest an analogy with 'Phase Q' in meteorites. Adsorbed atmospheric gases are present in all samples, and dominate whenever the noble gas partial pressure in the atmosphere is greater than that in the synthesis. While many of the results of Lancet and Anders (1973) appear to have been dominated by such an atmospheric component, others are suspect. When the doubtful samples of Lancet and Anders are corrected or eliminated, the fractionation pattern no longer peaks at Ar, but rather, as in the present sample, rises monotonically from Ne to Xe. No evidence is found for the earlier study's claim of a strong temperature dependence.

Yang, J.↗

Sorption of noble gases by solids, with reference to meteorites. II - Chromite and carbon. III - Sulfides, spinels, and other substances; on the origin of planetary gases

The trapping of noble gases by chromite and carbon, two putative carriers of primordial noble gases in meteorites, was studied by synthesizing 19 samples in a Ne-Ar-Kr-Xe atmosphere at 440-720 K. Noble gas contents are found to approximately obey Henry's Law, but only slight correlations are found with composition, surface area, or adsorption temperature. Geometric mean distribution coefficients for bulk samples and HCl residues in 10 cu cm STP/g atm are: Xe 100, Kr 15, Ar 3.5, and Ne 0.62. Elemental fractionation data support the suggestion of Lewis et al. (1977) that chromite and carbon in C2 and C3 chondrites were formed by the reaction: Fe, Cr + 4CO yields (Fe, Cr)3O4 + 4C + carbides. In contrast to meteoritic minerals, the synthetic specimens show no isotopic fractionation of noble gases. In a subsequent study, attention is given to the cases of sulfides and spinels, on the way to consideration of the origin of planetary gases. Sulfides showed three distinctive trends relative to chromite or magnetite. The elemental fractionation pattern of Ar, Kr and Xe in meteorites, terrestrial rocks and planets resembles the adsorption patterns on the carbons, spinels, sulfides, and other solids studied. The high release temperature of meteoritic noble gases may be explained by transformation of the physisorbed or chemisorbed gas. The ready loss of meteoritic heavy gases on surficial oxidation is consistent with adsorption, as is the high abundance.

Yang, J.↗

Laboratory simulation of meteoritic noble gases. II - Sorption of xenon on carbon: Etching and heating experiments

The release of trapped Xe from amorphous-C phases of meteorites is simulated experimentally by HNO3 etching of carbon-black and pyrolyzed polyvinylidene chloride samples exposed to Xe-127 for 0.5-240 h at 100-1000 C and then degassed for 9 h or more at the same temperatures, as reported by Wacker et al. (1985). The results are presented in tables and graphs and characterized in detail. Samples exposed at 100-200 C are found to lose most of their Xe after etching to a depth of only about 20 pm, while those exposed at 800-1000 C exhibit a second more tightly bound component extending to a depth of 3 nm, indicative of diffusion of Xe during exposure and resembling planetary Xe. The higher noble-gas concentrations measured in meteorites are attributed to rate-controlled Xe uptake over a long period in the solar nebula.

Zadnik, M. G.↗

Improved heat switch for gas sorption compressor

Thermal conductivities of the charcoal bed and the copper matrix for the gas adsorption compressor were measured by the concentric-cylinder method. The presence of the copper matrix in the charcoal bed enhanced the bed conductance by at least an order of magnitude. Thermal capacities of the adsorbent cell and the heat leaks to two compressor designs were measured by the transient method. The new gas adsorption compressor had a heat switch that could transfer eight times more heat than the previous one. The cycle time for the new prototype compressor is also improved by a factor of eight to within the minute range.

Chan, C. K.↗

Design and performance analysis of gas sorption compressors

Compressor kinetics based on gas adsorption and desorption processes by charcoal and for gas absorption and desorption processes by LaNi5 were analyzed using a two-phase model and a three-component model, respectively. The assumption of the modeling involved thermal and mechanical equilibria between phases or among the components. The analyses predicted performance well for compressors which have heaters located outside the adsorbent or the absorbent bed. For the rapidly-cycled compressor, where the heater was centrally located, only the transient pressure compared well with the experimental data.

Chan, C. K.↗

Sorption cooler technology development at JPL

Simple heating and cooling of chemisorption and physisorption compressors provide high pressure gas, which, when expanded through a Joule-Thomson (J- T) valve, can provide cooling from 0.3 to 200 K depending on the sorbent/gas combination. System life tests are under way on Pr(1-n)Ce(n)O(x)/O2 (PCO/O2) chemisorption compressors for 65-80 K cooling and on carbon/krypton (C/Kr) physisorption compressors for 120-140 K cooling. Investigations have been initiated to examine reliability physics issues related to critical compressor components such as sorbents, container materials and electrical heaters.

Jones, J. A.↗

High-Suction Hydride Sorption Pump

Improved design provides high pumping speed at low pressure. Hydride-forming powder retained in thin layer in contact with inner surface of stainless-steel tube. Configuration provides large surface area and short path for efficient transfer of heat and small resistance to flow.

Bard, Steven↗

Fast, Low-Duty-Cycle Sorption Refrigerators

Metal hydride/hydrogen-sorption refrigerators developed to provide rapid, intermittent cooling at temperatures between 30 and 10 K. In original application, refrigerators cool infrared detectors aboard spacecraft, exhausting heat to outer space via radiators at 250 K. Modified to cool scientific instrumentation on Earth with some loss of efficiency. Require no power during quick cooldown and low heating power during relatively long recharge periods.

Johnson, AL↗