This assessment seeks (1) to determine the most probable chemical compounds formed between fission products and actinides in urania fuels under normal and accident conditions and (2) to identify gaps in knowledge of these fission-product compounds. The ultimate goal of this effort is to develop predictive capability about the behavior of fission products under normal and accident conditions. The relevant thermochemical data have been organized by compound type, the chemical stability of resultant compounds determined, and data uncertainty evaluated. The assessment focused on fission-product and actinide oxides, halides, tellurides, and hydroxides. Free energy equations are given for those compounds for which data were available.

The use of radiotracer spiking as a method of measuring the leaching from simulated nuclear-waste glass is shown to give results comparable with other analytical detection methods. The leaching behavior of strontium-85, ruthenium-106, barium-133, cesium-137, cerium-141, europium-152, and other isotopes is measured for several defense waste glasses. These tests show that radiotracer spiking is a sensitive, multi-element technique that can provide leaching data, for actual waste elements, that are difficult to obtain by other methods. Additionally, a detailed procedure is described that allows spiked glass to be prepared with a suitable distribution of radionuclides.

This sixth symposium covers process control processes and issues involved in the conversion of fossil fuels into synthetic fuels.

Annual report of the Argonne National Laboratory Radiological and Environmental Research Division regarding activities related to atmospheric physics. This report discusses the section's participation in the Atmospheric Studies in COmplex Terrain (ASCOT) experiment.

A preliminary analysis is presented for a seasonal storage solar heating system for the Charlestown Navy Yard in Boston, Massachusetts. The area occupies a prominent location in the Boston Harbor and is being redeveloped for residential and commercial use. The system makes use of two large, buried concrete storage tanks totaling 5700 cubic meters as a water heat store. Other storage facilities, including a dry dock, offer additional solar opportunities for the navy Yard as the redevelopment progresses. The analysis makes extensive use of MINSUN, a computer performance and economic simulation routine written specifically for solar seasonal storage systems. The system performance and economics are analyzed for different collector types and areas, component costs, exogenous economic conditions, and optional inclusion of a heat pump. System cost-effectiveness is defined in relation to an economic break-even situation with respect to a conventional system, and is presented in terms of a solar premium, which is the incremental cost for the solar system per MWH of conventional fuel displaced. The additional analysis and design considerations necessary before an implementation phase are outlined. System implementation is discussed in terms of the roles of the various parties involved and funding/financing possibilities.

This report provides background and procedural information for the use of a general-purpose Stirling-engine analysis code developed at Argonne National Laboratory and available through the National Energy Software Center. Different engine configurations are easily specified, or the user may make use of provided data for existing engines, both kinematic and free piston. The code models heat transfer and fluid mechanics throughout the engine and accounts for system energy flows and losses. Good agreement is shown between code predictions and experimental measurements. The present analysis method was chosen for fast execution and useful information on energy flows in the system. A description is provided of the code structure that is intended to accept different analysis modules that can provide improved system modeling or optimization capability.

From Abstract: This report provides background and procedural information for the use of a general-purpose Stirling-engine analysis code developed at Argonne National Laboratory and available through the National Energy Software Center. Different engine configurations are easily specified, or the user may make use of provided data for existing engines, both kinematic and free piston. The code models heat transfer and fluid mechanics throughout the engine and accounts for system energy flows and losses. Good agreement is shown between code predictions and experimental measurements. The present analysis method was chosen for fast execution and useful information on energy flows in the system. A description is provided of the code structure that is intended to accept different analysis modules that can provide improved system modeling or optimization capability.

The U-Al-Si system was investigated in the composition range from U to U-80 at.% Al to U-75 at.% Si. More than 260 binary and ternary alloys were arc melted and studied by metallographic and x-ray powder diffraction techniques, in the as-cast condition and after thermal treatment at temperatures ranging from 700 to 1040 C. One or possibly two ternary compounds of undetermined crystal structure exist at or near U2AlSi2 The binary silicides U3Si, U3Si2, and USi can dissolve only small amounts of Al in solid solution, but the higher silicides U3Si5, USi2-x, and USi/sub 3/ dissolve increasingly larger amounts of Al. Of the three binary aluminides, UAl2 can dissolve more than 12 at.% Si in solid solution. UAl3 forms a continuous solid solution with USi3, and UAl4 is not present in alloys containing more than 3 at.% Si.

A variance-to-mean noise technique, modified to eliminate systematic errors from drifting of reactor power, has been used to infer integral values of effective beta for uranium and plutonium fueled fast reactor modk-ups. The measurement technique, including corrections for a finite detector-electrometer time response, is described together with preliminary beta measurement results.

This manual summarizes the numerical software contained in the Applied Mathematics Division Subroutine Library (AMDLIB), the International Mathematical and Statistical Libraries, Inc. (IMSL), and the Numerical Algorithms Group, Ltd. (NAG) mathematical libraries. Seventeen numerical analysis subjects are discussed, and the appropriate subroutines available in the three libraries for solving each type of problem are listed, with our recommendations for particular types of applications.

Quarterly report discussing fuel cell research and development work at Argonne National Laboratory (ANL). This report describes efforts directed toward understanding and improving components of molten carbonate fuel cells and have included operation of 10-cm square cells.

PART 1: The effectiveness of a neutron well correlation counter (NWCC) and a random driver (RD) for plutonium-containing item assay and loss detection has been studied. The items were 4 in. x 2 in. x 1/4 in. stainless steel-clad metal plates and 6 in. x 3/8 in. stainless steel-clad oxide rods, each in two types of containment. PART 2: A neutron-counting/fuel-weighting system has been developed to provide the capability to assay the ZPR-6 and -9 plutonium fuel canisters rapidly and accurately. This system makes feasible the inline monitoring of fuel transfer from the storage vault to the fuel loading hoods and vice-versa. To exploit fully the system's potential, the equipment is intended to be used in conjunction with an on-line computer having a fuel and fuel-canister data base.

Quarterly report of the Argonne National Laboratory Chemical Engineering Division regarding activities related to properties and handling of radioactive materials, operation of nuclear reactors, and other relevant research.

A modified Newton method for unconstrained minimization is presented and analyzed. The modification is based upon the model trust region approach. This report contains a thorough analysis of the locally constrained quadratic minimizations that arise as sub-problems in the modified Newton iteration. Several promising alternatives are presented for solving these sub-problems in ways that overcome certain theoretical difficulties exposed by this analysis. Very strong convergence results are presented concerning the minimization algorithm. In particular, the explicit use of second-order information is justified by demonstrating that the iterates converge to a point that satisfies the second-order necessary conditions for minimization. With the exception of very pathological cases this convergence occurs whenever the algorithm is applied to problems with continuous second partial derivatives.

Nuclear fuel cycles safeguards should be considered in the dynamic context of a world deployment of various reactor types and varying availability of fuel-cycle services. There will be a close interaction between thermal-reactor cycles and the future deployment of fast breeders. The quantities of plutonium and the reprocessing, conversion, fabrication, and storage methods of the fuel for the fast breeders will have a significant impact on safeguards techniques. The approach to the fast breeder fuel cycle safeguards follows the general safeguards system approach proposed by the IAEA. Objective of IAEA safeguards is the detection of diversion of nuclear material and deterrence of such diversion. To achieve independent verification of material balance accountancy requires the capability to monitor inventory status and verify material flows and quantities of all nuclear materials subject to safeguards. Containment and surveillance measures are applied to monitor key measurement points, maintain integrity of material balance, and complement material accountancy. The safeguards study attempts to develop a generic reference IAEA Safeguards System and explores various system options using containment/surveillance and material accountancy instrumentation and integrated systems designs.

Three types of metallic thermal insulation were investigated analytically and experimentally: multilayer reflective plates, multilayer honeycomb composite, and multilayer screens. Each type was subjected to evacuated and non-evacuated conditions, where thermal measurements were made to determine thermal-physical characteristics. A variation of the separation distance between adjacent reflective plates of multilayer reflective plates and multilayer screen insulation was also experimentally studied to reveal its significance. One configuration of the multilayer screen insulation was further selected to be examined in sodium and sodium oxide environments. The emissivity of Type 304 stainless steel used in comprising the insulation was measured by employing infrared technology. A comprehensive model was developed to describe the different proposed types of thermal insulation. Various modes of heat transfer inherent in each type of insulation were addressed and their relative importance compared. Provision was also made in the model to allow accurate simulation of possible sodium and sodium oxide contamination of the insulation. The thermal-radiation contribution to heat transfer in the temperature range of interest for LMFBR's was found to be moderate, and the suppression of natural convection within the insulation was vital in preserving its insulating properties. Experimental data were compared with the model and other published results. …

Quarterly report discussing fuel cell research and development work at Argonne National Laboratory (ANL). This report describes efforts directed toward understanding and improving the components of molten-carbonate-electrolyte fuel cells operated at temperatures near 925 K. The primary focus of this work has been the development of electrolyte structures that have good electrolyte retention and mechanical properties as well as long-term stability, and on developing methods of synthesis amendable to mass production.

Both 2F di-n-amyl-n-amylphosphonate in n-dodecane (DA(AP)-DD) and 0.77F tricaprylmethylammonium nitrate in Aromatic 100 (TCMA.NO/sub 3/-AR100) extract uranium and thorium into relatively concentrated organic solutions. Countercurrent-flow tests with each extractant have demonstrated effective uranium-thorium separations by selective stripping from the organic phase. Both extractants offer advantageous alternatives to tributylphosphate (Thorex) in reprocessing irradiated mixed ThO2-UO2 fuels. Formic acid is used for removing thorium from DA(AP)-DD; dilute HNO3 removes uranium from TCMA.NO3-AR100. Spectra of plutonium in formic acid are shown. The use of concentrated TCMA.NO3-AR100 at 50 to 65/sup 0/C avoids viscosity problems and suppresses third-phase formation. Thorium extracts into concentrated TCMA.NO/sub 3/-AR100 in greater amounts than would be predicted from stoichiometric assumptions.

A review was conducted during the period of mid-June to mid-August 1979, of the literature on spray combustion. Particular attention has been paid to theoretical and experimental work on droplet and spray combustion applicable to the use of alternate fuels, mainly liquid fuels derived from coal and shale.

Annual report of the Argonne National Laboratory Chemical Engineering Division regarding studies of nuclear waste migration in geologic media. This report discusses research regarding nuclide migration by fluid flow in rock.

Abstract: "The Environmental Working Level Monitor (EWLM) is an instrument used to automatically monitor airborne Rn-daughter concentrations and the Working Level (WL). It is an ac powered, microprocessor-based instrument with an external inverter provided for dc operation if desired. The microprocessor's control processor unit (CPU) controls the actuation of the detector assembly and processes its output signals to yield the measurements in the proper units. The detectors are fully automated and require no manual operations once the instrument is programmed. They detect and separate the alpha emitters of RaA and RaC' as well as detecting the beta emitters of RaB and RaC. The resultant pulses from these detected radioisotopes are transmitted to the CPU. The programmed microprocessor performs the mathematical manipulations necessary to output accurate Rn-daughter concentrations and the WL. A special subroutine within the system program enables the EWLM to run a calibration procedure on command which yields calibration data. This data can then be processed in a separate program on most computers capable of BASIC programming. This calibration program results in the derivation of coefficients and beta efficiencies which provides the calibrated coefficients and beta efficiencies required by the main system program to assure proper calibration of the …

Operation of liquid-metal-cooled fast breeder reactors (LMFBRs) will result in production of various quantities of radioactive sodium waste. Two methods have been developed and tested on a small scale for converting this sodium waste to inert compounds suitable for disposal. The first method is direct oxidation of the sodium after dispersal in a silica matrix. The sodium is mixed with silica and oxidized in a rotary drum reactor. The product is suitable for making glass when other stabilizing compounds are added. The second method is reaction of elemental sodium with molten sodium hydroxide at 450 degrees C and subsequent injection of steam into the melt to convert the reaction products (Na2O and NaH) to additional sodium hydroxide. The reactions are smooth and easily controlled with little danger of run-away reactions. The end product is molten sodium hydroxide which can be cast into drums for further treatment or disposal. The advantages of these two methods over more conventional aqueous processes are the elimination of aqueous wastes and the elimination of minimization of gaseous effluents.

The domain and surface structures of metallic sodium tungsten bronzes, NaxWO₃, 0.4 < x < 1, were studied using optical microscopy, supplemented by chemical methods, photoelectron spectroscopy, electron microscopy, etc. The birefringent, multidomain structure of the bronze is exhibited by a sodium-deficient, epitaxial surface film and hence is not, as reported elsewhere, a bulk property. The film can be synthesized by anodic electrolysis in alkaline solution and can exist only epitaxially with the substrate. It is chemically inert, translucent, and often laminated to a multilayered film. The film domain is hypersensitive to lateral stress and to thermal change, and appears to be modulated by minute structural changes of the substrate. This epitaxial modulation of the film is strikingly large at the phase transitions of the substrate induced by slightly different tiltings of the oxygen octahedra. The domain-wall movement is often slow enough to be visible, and that by thermal effect is occasionally accompanied by an audible, high-pitched, snapping sound.

Commercial refractories were tested for up to 500 h in both basic and acidic slags. The slag compositions typify those expected in slagging coal gasifiers. The slag temperatures ranged up to 1600 degrees C. Compositions tested have included silicon carbides, chrome-alumina-magnesia spinels, and alumina and magnesia-based refractories with various amounts of chromia and silica. In some tests, the cold faces were water cooled. With water cooling, the silicon carbides showed virtually no attack after 500 h. In the absence of water cooling, the chrome-alumina-magnesia spinels were the most resistant to slag attack but were subject to thermal-shock cracking. Alumina-chrome refractories performed well in acid slags when water cooled, are probably more stable than silicon carbide in coal-gasification atmospheres, and, in the form of ramming mixes, showed excellent thermal-shock resistances. Plans for future testing are described.