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The Skylab Trash Airlock (TAL) used throughout the Skylab mission to transfer trash materials that could support microbial growth from the pressurized cabin to the unpressurized waste tank is described. The TAL, which uses several basic mechanisms, was successfully operated daily for the 170 days of manned missions for a total of 637 cycles.
The cement industry is the most energy-intensive industry in the United States in terms of energy cost as a percentage of the total product cost. An assessment of gas-side fouling in cement plants with special emphasis on heat recovery applications is provided. In the present context, fouling is defined as the buildup of scale on a heat-transfer surface which retards the transfer of heat and includes the related problems of erosion and corrosion. Exhaust gases in the cement industry which are suitable for heat recovery range in temperature from about 100 to 1300 K, are generally dusty, may be highly abrasive, and are often heavily laden with alkalies, sulfates, and chlorides. Particulates in the exhaust streams range in size from molecular to about 100 micrometers in diameter and come from both the raw feed as well as the ash in the coal which is the primary fuel used in the cement industry. The major types of heat-transfer equipment used in the cement industry include preheaters, gas-to-air heat exchangers, waste heat boilers, and clinker coolers. At the present time, the trend in this country is toward suspension preheater systems, in which the raw feed is heated by direct contact with the hot kiln exit gases, and away from waste heat boilers as the principal method of heat recovery. The most important gas-side fouling mechanisms in the cement industry are those due to particulate, chemical reaction, and corrosion fouling.
The main aim of the PEBS project is to evaluate the sealing and barrier performance of the EBS over time, through development of a comprehensive approach involving experiments, model development, and consideration of the potential impacts on long-term safety functions. The experiments and models cover the full range of conditions, from initial emplacement of wastes (high heat generation and EBS re-saturation) through to later stage establishment of near steady state conditions, i.e. full re-saturation and thermal equilibrium with the host rock. These aspects will be integrated in a manner that will lead to greater certainty and thus greater confidence regarding the development from the initial transient state of the EBS to its long-term state, which provides the required isolation of the wastes. The work proposed within the project builds on existing knowledge and experience generated during recent years and supported by ongoing national and EC research programs. The project aims to provide a more complete description of the THM and THMC (thermo-hydro-mechanical- chemical) evolution of the EBS system, a more quantitative basis for relating the evolutionary behavior to the safety functions of the system, and a further clarification of the significance of residual uncertainties for long-term performance assessment. The importance of uncertainties arising from potential disagreement between the process models and the laboratory and in-situ experiments to be performed within PEBS, and their implications for an extrapolation of the results, will be reviewed, with particular emphasis on possible impacts on safety functions. In addition to the scientific-technical aims, the consortium will disseminate the basic findings to the broad scientific community within the EU, China and Japan, use expertise gained for public information purposes, and promote knowledge and technology transfer through training. (authors)
The Tank Closure Cesium Removal (TCCR) system is a Savannah River Site (SRS) demonstration 'at-tank' process designed to remove {sup 137}Cs from the high-level aqueous tank waste so that the decontaminated solution can be disposed as low-level waste. Cesium is removed by ion exchange (IX) columns using engineered IONSIV{sup TM} R9120-B form of the Crystalline Silicotitanate (CST) media. The TCCR system is deployed at Tanks 10 and Tank 11 in the SRS H Tank Farm. Water is added to the salt-cake in Tank 10 H to dissolve it. The dissolved salt solution waste is pumped out of Tank 10H (feed tank), through filters and IX columns. The decontaminated salt solution is transferred to Tank 11 (receipt tank), and on to Tank 50H for final disposal in the Saltstone Production Facility. The current TCCR can accommodate lead-lag (two-column) or lead-lag-guard (three-column) configurations to optimize media utilization and achieve the target decontamination. To assist the TCCR operations, a parametric study was conducted to evaluate the impact of different parameters (e.g., column configurations (single column, two columns or three columns in series), waste characteristics, operating temperature, process flow rate, CST average particle size) on the IX column performance including CST bed utilization. The initial results indicate that the IX column performance is improved at slower process flow rate, at lower operating temperature, and with smaller CST average particle size. Multi-column configurations are recommended, because the single-column configuration does not utilize CST bed effectively. This paper demonstrates the versatility of the ion exchange modeling to evaluate the effects of CST characteristics and operational parameters on IX column performances. (authors)
The simulation work presented in this report supports DOE-NE Used Fuel Disposition Campaign (UFDC) goals related to the development of drift scale in-situ field testing of heat-generating nuclear waste (HGNW) in salt formations. Numerical code verification and validation is an important part of the lead-up to field testing, allowing exploration of potential heater emplacement designs, monitoring locations, and perhaps most importantly the ability to predict heat and mass transfer around an evolving test. Such predictions are crucial for the design and location of sampling and monitoring that can be used to validate our understanding of a drift scale test that is likely to span several years.
A Saltstone waste form was prepared in the Savannah River National Laboratory (SRNL) from a Tank 50H sample and Z-Area premix material for the third quarter of calendar year 2011 (3QCY11). After the prescribed 32 day cure, samples of the saltstone were collected, and the waste form was shown to meet the South Carolina Hazardous Waste Management Regulations (SCHWMR) R.61-79.261.24 and R.61-79.268.48(a) requirements for a nonhazardous waste form with respect to RCRA metals and underlying hazardous constituents. These analyses met all quality assurance specifications of USEPA SW-846. The Saltstone Production Facility (SPF) receives waste from Tank 50H for treatment. In the third quarter of the 2011 calendar year (3QCY11), Tank 50H accepted transfers of approximately 20 kgal from the Effluent Treatment Project (ETP), approximately 236 kgal from the Actinide Removal Process/Modular Caustic Side Solvent Extraction Unit (ARP/MCU) Decontaminated Salt Solution Hold Tank (DSS-HT), and approximately 25 kgal from other sources. The Saltstone Grout Sampling plan provides the South Carolina Department of Health and Environmental Control (SCDHEC) with the chemical and physical characterization strategy for the salt solution which is to be disposed of in the Z-Area Solid Waste Landfill (SWLF). During operation, samples were collected from Tank 50H and grout samples prepared to determine the non-hazardous nature of the grout to meet the requirements of the South Carolina Hazardous Waste Management Regulations (SCHWMR) R.61-79.261.24(b) and R.61-79.268.48(a). Savannah River National Laboratory (SRNL) was asked to prepare saltstone from samples of Tank 50H obtained July 7, 2011 during 3QCY11 to determine the non-hazardous nature of the grout. The samples were cured and shipped to Babcock & Wilcox Technical Services Group-Radioisotope and Analytical Chemistry Laboratory (B&W TSG-RACL) to perform the Toxic Characteristic Leaching Procedure (TCLP) and subsequent extract analysis on saltstone samples for the analytes required for the quarterly analysis saltstone sample. In addition to the eight toxic metals - arsenic, barium, cadmium, chromium, mercury, lead, selenium and silver - analytes included the underlying hazardous constituents (UHC) antimony, beryllium, nickel, and thallium which could not be eliminated from analysis by process knowledge. B&W TSG-RACL provided subsamples to GEL Laboratories, LLC for analysis for the UHCs benzene, phenols and total and amenable cyanide.
We report to attain a basic understanding of the primary foam structure and behavior, which affects the heat and mass transfer and the efficiency of the glass melting process, we investigated the primary foam layer under the glass batch floating on molten glass. The primary foam affects mass transfer during batch melting, in turn affecting the melting process. The recently performed direct in-situ three-dimensional X-ray computed tomography of the batch melting in a laboratory-scale melter vessel allowed us to visualize the features of the reacting batch layer and the foam that develops at its bottom, though with an insufficient resolution of images. In this study, we obtained better temporal and spatial resolution using the two-dimensional X-ray radiography and visual observation of the structure and behavior of transient primary foam as it formed and decayed. As soon as the batch was charged onto the melt surface, foam bubbles began to evolve, grow, and coalesce, forming a primary foam layer, 5-10 mm thick, within tens of seconds. This foam layer was sustained by ongoing gas evolving reactions counterbalanced by bubble coalescence into cavities that moved sideways and escaped to the atmosphere. Eventually, the entire remaining batch turned into foam that gradually decayed at the melt surface. The decay rate agreed with literature observations of surface foam produced by secondary foaming.
The Saltstone Production Facility (SPF) receives waste from Tank 50H for treatment. In the fourth quarter of the 2011 calendar year (4QCY11), Tank 50H accepted transfers of approximately 10 kgal from the Effluent Treatment Project (ETP), approximately 4 kgal from 211H, approximately 573 kgal from the Actinide Removal Process/Modular Caustic Side Solvent Extraction Unit (ARP/MCU) Decontaminated Salt Solution Hold Tank (DSS-HT), and approximately 5 kgal from other sources. The Saltstone Grout Sampling plan provides the South Carolina Department of Health and Environmental Control (SCDHEC) with the chemical and physical characterization strategy for the salt solution which is to be disposed of in the Z-Area Solid Waste Landfill (SWLF). During operation, samples were collected from Tank 50H and grout samples prepared to determine the non-hazardous nature of the grout to meet the requirements of the South Carolina Hazardous Waste Management Regulations (SCHWMR) R.61-79.261.24(b) and R.61-79.268.48(a). Savannah River National Laboratory (SRNL) was asked to prepare saltstone from samples of Tank 50H obtained Oct. 12, 2011 during 4QCY11 to determine the non-hazardous nature of the grout. The samples were cured and shipped to Babcock & Wilcox Technical Services Group-Radioisotope and Analytical Chemistry Laboratory (B&W TSG-RACL) to perform the Toxic Characteristic Leaching Procedure (TCLP) and subsequent extract analysis on saltstone samples for the analytes required for the quarterly analysis saltstone sample. In addition to the eight toxic metals - arsenic, barium, cadmium, chromium, mercury, lead, selenium and silver - analytes included the underlying hazardous constituents (UHC) antimony, beryllium, nickel, and thallium which could not be eliminated from analysis by process knowledge. B&W TSG-RACL provided subsamples to GEL Laboratories, LLC for analysis for the UHCs benzene, phenols and total and amenable cyanide.
The new PIP-II superconducting linac will deliver a 2 mA average H⁻ beam to the existing Booster synchrotron. The injected beam is accumulated by charge exchange over approximately 300 turns; phase space painting is used to mitigate space charge effects. To limit the power load on the internal waste beam absorber from the transverse tails of the H⁻ distribution missing the foil, the beam will be collimated in both planes in the linac to Booster transfer line using compact collimators of a novel design. Both the number of parasitic hits and the fraction of the beam missing the foil are sensitive functions of the H⁻ beam centroid position with respect to the edge of the foil. The positioning of the collimation is constrained by the availability of suitable space in the transfer line lattice, by specifics of the collimator design, by the phase space orientation at the collimator, and by the betatron phase advance to the foil needed to achieve proper orientation of the spatial distribution at the injection point. In this contribution, we describe the procedure by which collimator positions were optimized. We then discuss the expected performance of the overall system.
Safety issues involved in the disposal of nuclear wastes in space as a complement to mined geologic repositories are examined as part of an assessment of the feasibility of nuclear waste disposal in space. General safety guidelines for space disposal developed in the areas of radiation exposure and shielding, containment, accident environments, criticality, post-accident recovery, monitoring systems and isolation are presented for a nuclear waste disposal in space mission employing conventional space technology such as the Space Shuttle. The current reference concept under consideration by NASA and DOE is then examined in detail, with attention given to the waste source and mix, the waste form, waste processing and payload fabrication, shipping casks and ground transport vehicles, launch site operations and facilities, Shuttle-derived launch vehicle, orbit transfer vehicle, orbital operations and space destination, and the system safety aspects of the concept are discussed for each component. It is pointed out that future work remains in the development of an improved basis for the safety guidelines and the determination of the possible benefits and costs of the space disposal option for nuclear wastes.
The project has made progress toward developing a comprehensive modeling capability for the capture of target species in off gas evolved during the reprocessing of nuclear fuel. The effort has integrated experimentation, model development, and computer code development for adsorption and absorption processes. For adsorption, a modeling library has been initiated to include (a) equilibrium models for uptake of off-gas components by adsorbents, (b) mass transfer models to describe mass transfer to a particle, diffusion through the pores of the particle and adsorption on the active sites of the particle, and (c) interconnection of these models to fixed bed adsorption modeling which includes advection through the bed. For single-component equilibria, a Generalized Statistical Thermodynamic Adsorption (GSTA) code was developed to represent experimental data from a broad range of isotherm types; this is equivalent to a Langmuir isotherm in the two-parameter case, and was demonstrated for Kr on INL-engineered sorbent HZ PAN, water sorption on molecular sieve A sorbent material (MS3A), and Kr and Xe capture on metal-organic framework (MOF) materials. The GSTA isotherm was extended to multicomponent systems through application of a modified spreading pressure surface activity model and generalized predictive adsorbed solution theory; the result is the capability to estimate multicomponent adsorption equilibria from single-component isotherms. This advance, which enhances the capability to simulate systems related to off-gas treatment, has been demonstrated for a range of real-gas systems in the literature and is ready for testing with data currently being collected for multicomponent systems of interest, including iodine and water on MS3A. A diffusion kinetic model for sorbent pellets involving pore and surface diffusion as well as external mass transfer has been established, and a methodology was developed for determining unknown diffusivity parameters from transient uptake data. Two parallel approaches have been explored for integrating the kernels described above into a mass-transport model for adsorption in fixed beds. In one, the GSTA isotherm kernel has been incorporated into the MOOSE framework; in the other approach, a focused finite-difference framework and PDE kernels have been developed. Issues, including oscillatory behavior in MOOSE solutions to advection-diffusion problems, and opportunities have been identified for each approach, and a path forward has been identified toward developing a stronger modeling platform. Experimental systems were established for collection of microscopic kinetics and equilibria data for single and multicomponent uptake of gaseous species on solid sorbents. The systems, which can operate at ambient temperature to 250°C and dew points from -69 to 17°C, are useful for collecting data needed for modeling performance of sorbents of interest. Experiments were conducted to determine applicable models and parameters for isotherms and mass transfer for water and/or iodine adsorption on MS3A. Validation experiments were also conducted for water adsorption on fixed beds of MS3A. For absorption, work involved modeling with supportive experimentation. A dynamic model was developed to simulate CO 2 absorption with chemical reaction using high alkaline content water solutions. A computer code was developed to implement the model based upon transient mass and energy balances. Experiments were conducted in a laboratory-scale column to determine model parameters. The influence of geometric parameters and operating variables on CO 2 absorption was studied over a wide range of conditions. This project has resulted in 7 publications, with 3 manuscripts in preparation. Also, 15 presentations were given at national meetings of ANS and AIChE and at Material Recovery and Waste Forms Campaign Working Group meetings.
A solvent extraction system for removal of cesium (Cs) from alkaline solutions was developed utilizing a novel solvent invented at the Oak Ridge National Laboratory (ORNL). This solvent consists of a calix[4]arene-crown-6 extractant dissolved in an inert hydrocarbon matrix. A Modifier is added to the solvent to enhance the extraction power of the calixarene and to prevent the formation of a third phase. An additional additive, called a suppressor, is used to improve stripping performance. The process that deploys this solvent system is known as Caustic Side Solvent Extraction (CSSX). The solvent system has been deployed at the Savannah River Site (SRS) in the Modular CSSX Unit (MCU) since 2008.
We report as glass batch is charged into an electric melter, a cold cap forms on the glass melt surface. Heat transfer to the cold cap from the molten glass below and the melter atmosphere above determines the melting rate. A mathematical model of the cold cap and the experimental kinetic data of the feed-to-glass conversion that were collected for several simulated low-activity and high-level waste melter feeds allowed us to develop relationships between the internal structure of the cold cap, its properties, its thickness, and the internal heat transfer. This contribution shows the distribution of major crystalline phases and the cumulative evolution of gases within the cold cap. It also examines the temperature, conversion degree, and heating rate the melter feed is experiencing during the passage through the cold cap and their effects on the cold-cap bottom temperature and morphology, which are important for the computational fluid dynamics simulations of melters.
Controlling ion desolvation, transport, and charge transfer at the electrode-electrolyte interface (EEI) is critical to enabling the rational design of efficient and selective separation of targeted heavy metals and decontamination of industrial waste water. One challenge is to sufficiently resolve and interrogate the intermediate transformation steps between solvated metal cations and bare cations for electroreduction at the EEI and establish pathways to modulate these steps to achieve efficient energy transfer for targeted reactive separations. Herein, we obtained a predictive understanding of the effect of adding a hydrophobic ionic liquid, 1-ethyl-3-methylimidazolium chloride (EMIMCl), to an aqueous electrolyte on modulating the desolvation and electrosorption of Pb 2+ cations using a combination of experimental and theoretical techniques. Here, we reveal formation of a compact interphase layer consisting of EMIMCl-Pb complex clusters under an applied electric field using operando electrochemical Raman spectroscopy, atomic force microscopy, and electrochemical impedance spectroscopy measurements combined with classical molecular dynamics simulations. The application of a larger negative potential is shown to result in formation of a well oriented layer with the positive imidazolium ring of the EMIMCl lying on the electrode and the long hydrophobic alkyl chain extending into the bulk electrolyte. This oriented layer is demonstrated to facilitate desolvation of incoming solvated Pb 2+ cations and decrease the charge transfer resistance for Pb electrodeposition, which has important implications for selective removal of Pb from contaminated mixtures. Overall, our studies open up new opportunities to modulate ion desolvation using hydrophobic ionic liquids in aqueous electrolytes for efficient heavy metal separation.
The degradation of organic matter by microorganisms provides a source of electrical potential or so-called 'self potential' (SP) that can be measured by using a voltmeter. During this process electrons are being produced as a waste-product and bacterial cells have to dispose of these to allow for the complete biodegradation of organic matter. Especially in anaerobic microbial communities, exo-cellular electron transfer is the most important driving force behind this process and organisms have developed different, but also similar, ways to transfer electrons to other microorganisms. Recently, it has been postulated that direct electron transfer from cell-to-cell is actually done by 'hard-wired' microorganisms. This shuttling of electrons is most likely done by certain c-type cytochromes that form the functional part of electrically conductive nanowires. In this study we investigated if nanowires can explain the geoelectrical (self potential and spectral induced polarization) signals observed at some biostimulated environments such as DOE sites. The objectives of our project are to: (1) investigate any temporal changes in the geophysical signatures (Self Potential (SP) and Induced Polarization (IP)) associated with nanowires of the bacterium Shewanella oneidensis MR-1, wild type and mtrc/omcA deletion mutant, (2) demonstrate that mutant strains of bacteria that produce nonconductive nanowires do not contribute to geoelectrical responses. We accomplished the following: (1) Provided training to students and a postdoctoral fellow that worked on the project, (2) Conducted several SP & IP measurements correlating the distribution of nanowires and SIP/SP signals in partial fulfillment of object No. 1 and 2. On the following we will report and discuss the results of our last experiment with some emphasis on the source mechanisms of both SP and IP associated with Shewanella oneidensis MR-1, wild type in sand columns.
Environmental concerns pose the biggest challenge for the development of the nuclear energy industry, often preventing or limiting the construction of new plants and radioactive waste disposal facilities. There are currently numerous sites in the world at which surface and groundwater are contaminated by nuclear weapon production and testing, as well as due to nuclear power plant accidents. Many of those sites remain unused or inhabited primarily due to public concern. Improving scientific and technical capabilities to develop environmental resiliency is critical not only to address existing contamination, but also to build public confidence and support for nuclear energy. One of the obstacles in remediation is to tackle a large volume of contaminated soil and groundwater with relatively low concentrations. Although many contaminant removal technologies have developed (e.g., pump-and-treat systems), they are often expensive and not cost-effective for low-concentration radionuclide contamination. Although soil removal is often the most effective, it produces a large amount of waste that has to be stored securely for a long period of time or treated at the special treatment facilities. Transporting a large amount of waste may also produce greenhouse gases and disrupt local communities. Recently, the concept of 'sustainable remediation' has been proposed to improve a remediation system as a whole, including the consideration of cost effectiveness, reduction of greenhouse emission, waste production and energy usage. Rather than just focusing on removing contaminants, the sustainable remediation highlights the use of passive remediation technologies to immobilize radionuclides along with the application of monitored natural attenuation and longer institutional control. However, such passive technologies and monitored natural attenuation require the increased burden of proof to ensure that those immobilized contaminants would not compromise the long-term public health. Although contaminant transport modeling and risk assessments are always performed, they sometimes fail due to the lack of understanding the contaminant transport proposes at the time of the risk assessment or due to some unexpected processes. Monitoring technologies are critical to ensure the long-term stability of such remediated sites, and also to address the public concerns. Recent advances in in situ sensor technologies and spatially-extensive mapping technologies (such as unmanned aerial vehicles, airborne mapping, geophysics) have improved monitoring of contamination over space and time. In addition to new sensing devices, data management and data analytics technologies have been expanded to manage and process large spatial and temporal datasets. Such technologies can be used to reduce monitoring cost significantly, and to facilitate long-term monitoring. In this study, we demonstrate our data analytics technologies for two nuclear-related contaminated sites: (1) air dose rate monitoring in Fukushima prefecture, and (2) groundwater monitoring at the Savannah River Site F-Area. We are developing the spatial and temporal data integration methodologies to integrate various spatially extensive data and time-series data for improving long-term monitoring. Such monitoring technologies and experiences at the existing contaminated sites can be transferred to build a better monitoring system for nuclear facilities, such as nuclear power plants or nuclear waste storages.
Cleaving inert SP3-SP3 carbon-carbon (C-C) bonds selectively remains a major challenge in organic chemistry and a main bottleneck in the chemical upcycling of recalcitrant polyolefin waste. Here, we present an electrochemical strategy using redox mediators to activate and break C-C bonds at room temperature and ambient pressure. Specifically, we use N-hydroxyphthalimide (NHPI) as a redox mediator that undergoes electrochemical oxidation to form the phthalimide-N-oxyl (PINO) radical to initiate hydrogen atom transfer (HAT) reactions with benzylic C-H bonds. The resulting benzylic carbon radical is readily captured by molecular oxygen to form a peroxy radical that decomposes into oxygenated C-C bond-scission fragments. This indirect, mediated approach for Csp3-Csp3 bond cleavage reduces the oxidation potential by > 1.2 V compared to the direct oxidation of the substrate, thereby eliminating deleterious side reactions, such as solvent oxidation, that may occur at high potentials. Studies with a bibenzyl model compound revealed a bifurcated reaction pathway following the initial HAT step. At a bibenzyl conversion of 61.0%, the C-C bond cleavage pathway generates benzaldehyde and benzoic acid products at 38.4% selectivity, and the C-H bond oxygenation pathway leads to 1,2-diphenylethanone and benzil products at 39.2% selectivity. Changes in reaction selectivity were investigated with various model compounds, including bibenzyl, 1,3-diphe-nylpropane, 1,4-diphenylbutane, and their derivatives. Product selectivity is correlated with the C-C bond strength of the reactant, with weaker C-C bonds favoring the C-C bond cleavage pathway. We also evaluated the mediated oxidation of oligo-meric styrene (Mn= 510 Da, OS510) which were converted into oxygenated products. Lastly, proof-of-concept depolymeriza-tion of polystyrene (PS, ~10,000 Da) into oxygenated monomers, dimers, and oligomers was demonstrated using NHPI-mediated oxidation.
Bioreactors are of interest for value‐upgrading of stranded or waste industrial gases. Reactor intensification requires development of low cost bioreactors with fast gas–liquid mass transfer rate. Here we assess published reactor technology in comparison with a novel downward bubble flow created by a micro‐jet array. Compared to known technology, the advanced design achieves higher volumetric gas transfer efficiency (k L a per power density) and can operate at higher k L a. We measure the effect of four reactor heights (height‐to‐diameter ratios of 12, 9, 6, and 3) on the gas transfer coefficient k L , total interfacial area a, liquid residence time distribution, energy consumption, and turbulent hydrodynamics. Leading models for predicting k L and a are appraised with experimental data. The results show k L is governed by “entrance effects” due to Higbie penetration dominate at short distances below the micro‐jet array, while turbulence dominates at intermediate distances, and finally terminal rise velocity dominates at large distances. © 2017 American Institute of Chemical Engineers AIChE J , 64: 1399–1411, 2018