Selection and Characterization of Carbon Black and Surfactants for Development of Small Scale Uranium Oxicarbide Kernels

This report supports the effort for development of small scale fabrication of UCO (a mixture of UO{sub 2} and UC{sub 2}) fuel kernels for the generation IV high temperature gas reactor program. In particular, it is focused on optimization of dispersion conditions of carbon black in the broths from which carbon-containing (UO{sub 2} {center_dot} H{sub 2}O + C) gel spheres are prepared by internal gelation. The broth results from mixing a hexamethylenetetramine (HMTA) and urea solution with an acid-deficient uranyl nitrate (ADUN) solution. Carbon black, which is previously added to one or other of the components, must stay dispersed during gelation. The report provides a detailed description of characterization efforts and results, aimed at identification and testing carbon black and surfactant combinations that would produce stable dispersions, with carbon particle sizes below 1 {micro}m, in aqueous HMTA/urea and ADUN solutions. A battery of characterization methods was used to identify the properties affecting the water dispersability of carbon blacks, such as surface area, aggregate morphology, volatile content, and, most importantly, surface chemistry. The report introduces the basic principles for each physical or chemical method of carbon black characterization, lists the results obtained, and underlines cross-correlations between methods. Particular attention is given to a newly developed method for characterization of surface chemical groups on carbons in terms of their acid-base properties (pK{sub a} spectra) based on potentiometric titration. Fourier-transform infrared (FTIR) spectroscopy was used to confirm the identity of surfactants, both ionic and non-ionic. In addition, background information on carbon black properties and the mechanism by which surfactants disperse carbon black in water is also provided. A list of main physical and chemical properties characterized, samples analyzed, and results obtained, as well as information on the desired trend or range of values generally associated with better dispersability, is provided in the Appendix. Special attention was given to characterization of several surface-modified carbon blacks produced by Cabot Corporation through proprietary diazonium salts chemistry. As demonstrated in the report, these advanced carbons offer many advantages over traditional dispersions. They disperse very easily, do not require intensive mechanical shearing or sonication, and the particle size of the dispersed carbon black aggregates is in the target range of 0.15-0.20 {micro}m. The dispersions in water and HMTA/urea solutions are stable for at least 30 days; in conditions of simulated broth, the dispersions are stable for at least 6 hours. It is proposed that the optimization of the carbon black dispersing process is possible by replacing traditional carbon blacks and surfactants with surface-modified carbon blacks having suitable chemical groups attached on their surface. It is recognized that the method advanced in this report for optimizing the carbon black dispersion process is based on a limited number of tests made in aqueous and simulated broth conditions. The findings were corroborated by a limited number of tests carried out with ADUN solutions by the Nuclear Science and Technology Division at Oak Ridge National Laboratory (ORNL). More work is necessary, however, to confirm the overall recommendation based on the findings discussed in this report: namely, that the use of surface-modified carbon blacks in the uranium-containing broth will not adversely impact the chemistry of the gelation process, and that high quality uranium oxicarbide (UCO) kernels will be produced after calcination

Initial assessment of environmental effects on SiC/SiC composites in helium-cooled nuclear systems

This report summarized the information available in the literature on the chemical reactivity of SiC/SiC composites and of their components in contact with the helium coolant used in HTGR, VHTR and GFR designs. In normal operation conditions, ultra-high purity helium will have chemically controlled impurities (water, oxygen, carbon dioxide, carbon monoxide, methane, hydrogen) that will create a slightly oxidizing gas environment. Little is known from direct experiments on the reactivity of third generation (nuclear grade) SiC/SiC composites in contact with low concentrations of water or oxygen in inert gas, at high temperature. However, there is ample information about the oxidation in dry and moist air of SiC/SiC composites at high temperatures. This information is reviewed first in the next chapters. The emphasis is places on the improvement in material oxidation, thermal, and mechanical properties during three stages of development of SiC fibers and at least two stages of development of the fiber/matrix interphase. The chemical stability of SiC/SiC composites in contact with oxygen or steam at temperatures that may develop in off-normal reactor conditions supports the conclusion that most advanced composites (also known as nuclear grade SiC/SiC composites) have the chemical resistance that would allow them maintain mechanical properties at temperatures up to 1200 1300 oC in the extreme conditions of an air or water ingress accident scenario. Further research is needed to assess the long-term stability of advanced SiC/SiC composites in inert gas (helium) in presence of very low concentrations (traces) of water and oxygen at the temperatures of normal operation of helium-cooled reactors. Another aspect that needs to be investigated is the effect of fast neutron irradiation on the oxidation stability of advanced SiC/SiC composites in normal operation conditions

Use of Carbon Fiber Composite Molecular Sieves for Air Separation

A novel adsorbent material, 'carbon fiber composite molecular sieve' (CFCMS), has been developed by the Oak Ridge National Laboratory. Its features include high surface area, large pore volume, and a rigid, permeable carbon structure that exhibits significant electrical conductivity. The unique combination of high adsorptive capacity, permeability, good mechanical properties, and electrical conductivity represents an enabling technology for the development of novel gas separation and purification systems. In this context, it is proposed that a fast-cycle air separation process that exploits a kinetic separation of oxygen and nitrogen should be possible using a CFCMS material coupled with electrical swing adsorption (ESA). The adsorption of O{sub 2}, N{sub 2}, and CO{sub 2} on activated carbon fibers was investigated using static and dynamic techniques. Molecular sieving effects in the activated carbon fiber were highlighted by the adsorption of CO{sub 2}, a more sensitive probe molecule for the presence of microporosity in adsorbents. The kinetic studies revealed that O2 was more rapidly adsorbed on the carbon fiber than N{sub 2}, and with higher uptake under equilibrium conditions, providing the fiber contained a high proportion of very narrow micropores. The work indicated that CFCMS is capable of separating O{sub 2} and N{sub 2} from air on the basis of the different diffusion rates of the two molecules in the micropore network of the activated carbon fibers comprising the composite material. In response to recent enquires from several potential users of CFCMS materials, attention has been given to the development of a viable continuous process for the commercial production of CFCMS material. As part of this effort, work was implemented on characterizing the performance of lignin-based activated carbon fiber, a potentially lower cost fiber than the pitch-based fibers used for CFCMS production to date. Similarly, to address engineering issues, measurements were made to characterize the pressure drop of CFCMS as a function of carbon fiber dimensions and monolith density

Note on Graphite Oxidation by Oxygen and Moisture

Simplified equations of graphite oxidation are reviewed for semi-infinite slab, finite slab, and cylinder geometries, using the principal assumptions of linearized oxidation kinetics and quasi-steady state oxidation profile. All equations are coupled to a general surface mass transfer boundary condition. The equations include those for oxidant concentration distribution, surface oxidation rate, burnoff profile, and oxidation efficiency. This review also covers some areas that may not be well recognized. The key role of the effective diffusivity is highlighted, with a brief review of measured values. The temperature-dependence of the surface oxidation rate is shown to be more complex than usually shown for the diffusion-affected zone. Assumption of linear kinetics permits ready estimation of equilibration time for development of the quasi-steady burnoff profile. In addition, approximations for the time-steady hydrogen concentration profiles are developed for the case of oxidation by H2O. All cited methods can be readily evaluated by spreadsheet calculation

Activated Carbon Composites for Air Separation

In continuation of the development of composite materials for air separation based on molecular sieving properties and magnetic fields effects, several molecular sieve materials were tested in a flow system, and the effects of temperature, flow conditions, and magnetic fields were investigated. New carbon materials adsorbents, with and without pre-loaded super-paramagnetic nanoparticles of Fe3O4 were synthesized; all materials were packed in chromatographic type columns which were placed between the poles of a high intensity, water-cooled, magnet (1.5 Tesla). In order to verify the existence of magnetodesorption effect, separation tests were conducted by injecting controlled volumes of air in a flow of inert gas, while the magnetic field was switched on and off. Gas composition downstream the column was analyzed by gas chromatography and by mass spectrometry. Under the conditions employed, the tests confirmed that N2 - O2 separation occurred at various degrees, depending on material's intrinsic properties, temperature and flow rate. The effect of magnetic fields, reported previously for static conditions, was not confirmed in the flow system. The best separation was obtained for zeolite 13X at sub-ambient temperatures. Future directions for the project include evaluation of a combined system, comprising carbon and zeolite molecular sieves, and testing the effect of stronger magnetic fields produced by cryogenic magnets

Use of Carbon Fiber Composite Molecular Sieves for Air Separation

A novel adsorbent material, 'carbon fiber composite molecular sieve' (CFCMS), has been developed by the Oak Ridge National Laboratory. Its features include high surface area, large pore volume, and a rigid, permeable carbon structure that exhibits significant electrical conductivity. The unique combination of high adsorptive capacity, permeability, good mechanical properties, and electrical conductivity represents an enabling technology for the development of novel gas separation and purification systems. In this context, it is proposed that a fast-cycle air separation process that exploits a kinetic separation of oxygen and nitrogen should be possible using a CFCMS material coupled with electrical swing adsorption (ESA). The adsorption of O{sub 2}, N{sub 2}, and CO{sub 2} on activated carbon fibers was investigated using static and dynamic techniques. Molecular sieving effects in the activated carbon fiber were highlighted by the adsorption of CO{sub 2}, a more sensitive probe molecule for the presence of microporosity in adsorbents. The kinetic studies revealed that O2 was more rapidly adsorbed on the carbon fiber than N{sub 2}, and with higher uptake under equilibrium conditions, providing the fiber contained a high proportion of very narrow micropores. The work indicated that CFCMS is capable of separating O{sub 2} and N{sub 2} from air on the basis of the different diffusion rates of the two molecules in the micropore network of the activated carbon fibers comprising the composite material. In response to recent enquires from several potential users of CFCMS materials, attention has been given to the development of a viable continuous process for the commercial production of CFCMS material. As part of this effort, work was implemented on characterizing the performance of lignin-based activated carbon fiber, a potentially lower cost fiber than the pitch-based fibers used for CFCMS production to date. Similarly, to address engineering issues, measurements were made to characterize the pressure drop of CFCMS as a function of carbon fiber dimensions and monolith density

Operation of the CERN disk storage infrastructure during LHC Run-3

The CERN IT Storage group operates multiple distributed storage systems to support all CERN data storage requirements. The storage and distribution of physics data generated by LHC and non-LHC experiments is one of the biggest challenges the group has to take on during LHC Run-3.EOS [1], the CERN distributed disk storage system is playing a key role in LHC data-taking. During the first ten months of 2022, more than 440PB have been written by the experiments and 2.9EB have been read out. The data storage requirements of LHC Run-3 are higher than what was previously delivered. The storage operations team has started investigating multiple areas to upgrade and optimize the current storage resources. A new, dedicated and redundant EOS infrastructure based on 100Gbit servers was installed, commissioned and deployed for the ALICE Online and Offline (O2) project. This cluster can sustain high-throughput data transfer between the ALICE Event Processing Nodes (EPN) and the CERN’s data center.This paper will present the architecture, techniques and workflows in place allowing EOS to deliver fast, reliable and scalable data storage to meet experiment needs during LHC Run-3 and beyond

EOS workshop

Our team is in charge of providing storage and transfer services for the LHC and non-LHC experiments at CERN. In this presentation we are going to walk you through the activities of the EOS operations team at CERN in 2020. We are going to focus on the achievements, hurdles and lessons learned throughout the past year

EOS workshop

In this talk we will highlight the operational challenges we faced while bringing up a high-throughput EOS instance for the Run 3 ALICE data acquisition. The journey started in 2020 and we are still perfecting the instance to this day. During this time all storage nodes got migrated from CentOS 7 to CentOS 8 and, later on, CentOS Stream 8, and not without inherent challenges which we are going to detail in this talk