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DOE OSTI2011

Production of Actinium-225 via High Energy Proton Induced Spallation of Thorium-232

The science of cancer research is currently expanding its use of alpha particle emitting radioisotopes. Coupled with the discovery and proliferation of molecular species that seek out and attach to tumors, new therapy and diagnostics are being developed to enhance the treatment of cancer and other diseases. This latest technology is commonly referred to as Alpha Immunotherapy (AIT). Actinium-225/Bismuth-213 is a parent/daughter alpha-emitting radioisotope pair that is highly sought after because of the potential for treating numerous diseases and its ability to be chemically compatible with many known and widely used carrier molecules (such as monoclonal antibodies and proteins/peptides). Unfortunately, the worldwide supply of actinium-225 is limited to about 1,000mCi annually and most of that is currently spoken for, thus limiting the ability of this radioisotope pair to enter into research and subsequently clinical trials. The route proposed herein utilizes high energy protons to produce actinium-225 via spallation of a thorium-232 target. As part of previous R and D efforts carried out at Argonne National Laboratory recently in support of the proposed US FRIB facility, it was shown that a very effective production mechanism for actinium-225 is spallation of thorium-232 by high energy proton beams. The base-line simulation for the production rate of actinium-225 by this reaction mechanism is 8E12 atoms per second at 200 MeV proton beam energy with 50 g/cm2 thorium target and 100 kW beam power. An irradiation of one actinium-225 half-life (10 days) produces {approx}100 Ci of actinium-225. For a given beam current the reaction cross section increases slightly with energy to about 400 MeV and then decreases slightly for beam energies in the several GeV regime. The object of this effort is to refine the simulations at proton beam energies of 400 MeV and above up to about 8 GeV. Once completed, the simulations will be experimentally verified using 400 MeV and 8 GeV protons available at Fermi National Accelerator Laboratory. Targets will be processed at Argonne National Laboratory to separate and purify the actinium-225 that will subsequently be transferred to NorthStar laboratory facilities for product quality testing and comparison to the product quality of ORNL produced actinium-225, which is currently the industry standard. The test irradiations at FNAL will produce 1-20 mCi per day which is more than sufficient for quantitative evaluation of the proposed production process. The beneficial outcome of this effort will be a new production route for actinium-225 that does not use or require any uranium-233 materials owned by DOE or use any radium-226 as an irradiation target but can supply the medical community's needs for actinium-225 now and in the future.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2012

V5 and V10 Contactor Testing with the Next Generation (CSSX) Solvent for the Savannah River Site Integrated Salt Disposition Process

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.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2012

Next Generation Solvent – Materials Compatibility with Polymer Components within Modular CausticSide Solvent Extraction Unit (Final Report)

The Office of Waste Processing, within the Office of Technology Innovation and Development, is funding the development of an enhanced solvent for deployment at the Savannah River Site for removal of cesium from High Level Waste. The technical effort is collaboration between Oak Ridge National Laboratory (ORNL), Savannah River National Laboratory (SRNL), and Argonne National Laboratory. The first deployment target for the technology is within the Modular Caustic-Side Solvent Extraction Unit (MCU). Deployment of a new chemical within an existing facility requires verification that the chemical components are compatible with the installed equipment. In the instance of a new organic solvent, the primary focus is on compatibility of the solvent with organic polymers used in the facility. This report provides the data from exposing these polymers to the Next Generation Solvent (NGS). The test was conducted over six months. An assessment of the dimensional stability of polymers present in MCU (i.e., PEEK, Grafoil, Tefzel and Isolast) in the modified NGS (where the concentration of LIX®79 and MaxCalix was varied systematically) showed that LIX®79 selectively affected Tefzel and its different grades (by an increase in size and lowering its density). The copolymer structure of Tefzel and possibly its porosity allows for the easier diffusion of LIX®79. Tefzel is used as the seat material in some of the valves at MCU. Long term exposure to LIX®79, may make the valves hard to operate over time due to the seat material (Tefzel) increasing in size. However, since the physical changes of Tefzel in the improved solvent are comparable to the changes in the CSSX baseline solvent, no design changes are needed with respect to the Tefzel seating material. PEEK, Grafoil and Isolast were not affected by LIX®79 and MaxCalix within six months of exposure. The initial rapid weight gain observed in every polymer is assigned to the finite and limited uptake of Isopar® L/Modifier by the polymers probably due to the polymers porosity and rough surfaces. Spectroscopic data on the organic liquid and the polymer surfaces showed no preferential adsorption of any component in the NGS to the polymers and with the exception of CPVC, no leachate was observed in the NGS from any of the polymers studied. The testing shows no major concerns for compatibility over the short duration of these tests but does indicate that longer duration exposure studies are warranted, especially for Tefzel. However, the physical changes experienced by Tefzel in the improved solvent were comparable to the physical changes obtained when Tefzel is placed in CSSX baseline solvent. Therefore, there is no effect of the improved solvent beyond those observed in CSSX baseline solvent.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2011

FY11 annual Report: PHEV Engine Control and Energy Management Strategy

Objectives are to: (1) Investigate novel engine control strategies targeted at rapid engine/catalyst warming for the purpose of mitigating tailpipe emissions from plug-in hybrid electric vehicles (PHEV) exposed to multiple engine cold start events; and (2) Validate and optimize hybrid supervisory control techniques developed during previous and on-going research projects by integrating them into the vehicle level control system and complementing them with the modified engine control strategies in order to further reduce emissions during both cold start and engine re-starts. Approach used are: (1) Perform a literature search of engine control strategies used in conventional powertrains to reduce cold start emissions; (2) Develop an open source engine controller providing full access to engine control strategies in order to implement new engine/catalyst warm-up behaviors; (3) Modify engine cold start control algorithms and characterize impact on cold start behavior; and (4) Develop an experimental Engine-In-the-Loop test stand in order to validate control methodologies and verify transient thermal behavior and emissions of the real engine when combined with a virtual hybrid powertrain. Some major accomplishments are: (1) Commissioned a prototype engine controller on a GM Ecotec 2.4l direct injected gasoline engine on an engine test cell at the University of Tennessee. (2) Obtained from Bosch (with GM's approval) an open calibration engine controller for a GM Ecotec LNF 2.0l Gasoline Turbocharged Direct Injection engine. Bosch will support the bypass of cold start strategies if calibration access proves insufficient. The LNF engine and its open controller were commissioned on an engine test cell at ORNL. (3) Completed a literature search to identify key engine cold start control parameters and characterized their impact on the real engine using the Bosch engine controller to calibrate them. (4) Ported virtual hybrid vehicle model from offline simulation environment to real-time Hardware-In-the-Loop platform.

33 ADVANCED PROPULSION SYSTEMS↗
DOE OSTI2012

High Performance Computing Facility Operational Assessment, CY 2011 Oak Ridge Leadership Computing Facility

Oak Ridge National Laboratory's Leadership Computing Facility (OLCF) continues to deliver the most powerful resources in the U.S. for open science. At 2.33 petaflops peak performance, the Cray XT Jaguar delivered more than 1.4 billion core hours in calendar year (CY) 2011 to researchers around the world for computational simulations relevant to national and energy security; advancing the frontiers of knowledge in physical sciences and areas of biological, medical, environmental, and computer sciences; and providing world-class research facilities for the nation's science enterprise. Users reported more than 670 publications this year arising from their use of OLCF resources. Of these we report the 300 in this review that are consistent with guidance provided. Scientific achievements by OLCF users cut across all range scales from atomic to molecular to large-scale structures. At the atomic scale, researchers discovered that the anomalously long half-life of Carbon-14 can be explained by calculating, for the first time, the very complex three-body interactions between all the neutrons and protons in the nucleus. At the molecular scale, researchers combined experimental results from LBL's light source and simulations on Jaguar to discover how DNA replication continues past a damaged site so a mutation can be repaired later. Other researchers combined experimental results from ORNL's Spallation Neutron Source and simulations on Jaguar to reveal the molecular structure of ligno-cellulosic material used in bioethanol production. This year, Jaguar has been used to do billion-cell CFD calculations to develop shock wave compression turbo machinery as a means to meet DOE goals for reducing carbon sequestration costs. General Electric used Jaguar to calculate the unsteady flow through turbo machinery to learn what efficiencies the traditional steady flow assumption is hiding from designers. Even a 1% improvement in turbine design can save the nation billions of gallons of fuel.

99 GENERAL AND MISCELLANEOUS↗
DOE OSTI2012

NMIS with Imaging and Gamma Ray Spectrometry for Pu, HEU, HE and Other Materials

The Nuclear Material Identification System (NMIS) has been under development at ORNL and the National Nuclear Security Administration (NNSA) Y-12 National Security Complex since 1984. In the mid-1990s, what is now the US Department of Energy (DOE) Office of Nuclear Verification (ONV) realized that it was a useful technology for future arms control treaty applications and supported further development of the system. In 2004, fast-neutron imaging was incorporated into the system. In 2007, the ONV decided to develop a fieldable version of the system, designated as FNMIS, for potential use in future treaties. The FNMIS is being developed to be compatible with the eventual incorporation of gamma-ray spectrometry and an information barrier. This report addresses how and what attributes could be determined by the FNMIS system with gamma-ray spectrometry. The NMIS is a time-dependent coincidence system that incorporates tomographic imaging (including mapping of the fission sites) and gamma-ray spectrometry. It utilizes a small, lightweight (30 lb), portable deuterium-tritium (DT) neutron (14.1 MeV) generator (4 x 10 7 neutrons/second) for active interrogation and can also perform passive interrogation. A high-purity germanium (HPGe) gamma-ray detector with multichannel analysis can be utilized in conjunction with the source for active interrogation or passively. The system uses proton recoil scintillators: 32 small 2.5 x 2.5 x 10.2-cm-thick plastic scintillators for imaging and at least two 2 x 2 arrays of 27 x 27 x 10-cm-thick plastic scintillators that detect induced fission radiation. The DT generator contains an alpha detector that time and directionally tags a fan beam of some of the neutrons emitted and subdivides it into pixels. A fast (1 GHz) time correlation processor measures the time-dependent coincidence among all detectors in the system. A computer-controlled scanner moves the small detectors and the source appropriately for scanning a target object for imaging. The system is based on detection of transmitted 14.1 MeV neutrons, fission neutrons, and gamma rays from spontaneous, inherent source fission of the target, fission neutrons and gamma rays induced by the external DT source, gamma rays from natural emissions of uranium and plutonium, and induced gamma-ray emission by the interaction of the 14.1 MeV neutrons from the DT source. The NMIS can and has been used with a time-tagged californium spontaneous fission source. It has also been used with pulsed interrogation sources such as LINACs, DT, and deuterium-deuterium (DD) sources. This system is uniquely suited for detection of shielded highly enriched uranium (HEU), plutonium, and other special nuclear materials and detection of high explosives (HE) and chemical agents. The NMIS will be adapted to utilize a trusted processor that incorporates information barrier and authentication techniques using open software and then be useful in some international applications for materials whose characteristics may be classified. The proposed information barrier version of the NMIS system would consist of detectors and cables, the red (classified side) computer system, which processes the data, and the black (unclassified side) computer, which handles the computer interface. The system could use the 'IB wrapper' concept proposed by Los Alamos National Laboratory and the software integrity (digital signatures) system proposed by Sandia. Since it is based entirely on commercially available components, the entire system, including NMIS data acquisition boards, can be built with commercial off-the-shelf components. This system is being developed into a fieldable system (FNMIS) for potential arms control treaties by the ONV. The system will be modularly constructed with the RF shielded modules connected to the processor by appropriate control and signal cable in metal conduit. The FNMIS is presently being designed for eventual incorporation of gamma-ray spectrometry and an information barrier to protect classified information. The system hardware and software can be configured to obtain the following: plutonium presence, plutonium mass, Pu-240/239 ratio, plutonium geometry, plutonium metal vs non-metallic (absence of metal), time (age) since processing for plutonium (or last purification), uranium presence, uranium mass, uranium enrichment, uranium geometry, uranium metal vs non-metallic compound (absence of metal), beryllium presence and mass, tritium and deuterium gas bottle presence, HE, and chemical weapons. A matrix of the quantities determined, the method of determination, whether active (external neutron source) or passive, and the measurement equipment involved is given in the Tables 1-4. Some of these attributes can be obtained by multiple data analysis methods. The gamma-ray spectrometry methods for HEU, plutonium, and HE have been developed by other laboratories, are well known, and will be incorporated.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2012

High-rate, Low-cost Process for High-Efficiency Flexible c-Si PV

The film c-Si based photovoltaics on RABiTS substrates would be capable of achieving efficiency above 15%, but at costs comparable to thin films. Utilizing a uniquely-textured and flexible metal substrate developed at the superconducting materials program at ORNL, coupled to an NREL breakthrough in hotwire chemical vapor deposition (HWCVD) processes, silicon heteroepitaxy is for the first time being directly-deposited out of silane gas, into a silicon structure that is less than 5 microns thick, crystallographically-oriented, and large-grained – ideal for solar PV power generation. We have recently overcome the problem of Ni and Cu diffusion into Si forming NiSi/CuSi towers through buffer development. Due to the lattice mismatch between the oxide cap layer and Si, recombination-active threading dislocation defects form in the silicon layer. We can lattice match the buffer with silicon by alloying with germanium, which can subsequently be graded out for the actual device layer. The main goal of this project is to develop a physical vapor deposition process for the growth Silicon, Germanium, or Silicon-Germanium alloy films.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2012

An Assessment of Energy Potential at Non-Powered Dams in the United States

The United States has produced clean, renewable electricity from hydropower for more than 100 years, but hydropower-producing facilities represent only a fraction of the infrastructure development that has taken place on the nation’s waterways. In contrast to the roughly 2,500 dams that provide 78 gigawatts (GW) 1 of conventional and 22 GW of pumped-storage hydropower, the United States has more than 80,000 non-powered dams (NPDs)—dams that do not produce electricity—providing a variety of services ranging from water supply to inland navigation. Importantly, many of the monetary costs and environmental impacts of dam construction have already been incurred at NPDs, so adding power to the existing dam structure can often be achieved at lower cost, with less risk, and in a shorter timeframe than development requiring new dam construction. The abundance, cost, and environmental favorability of NPDs, combined with the reliability and predictability of hydropower, make these dams a highly attractive source for expanding the nation’s renewable energy supply. To better characterize this unique national resource, the U.S. Department of Energy (DOE) Wind and Water Power Program has undertaken a national-scale analysis of U.S. dams to determine the ability of NPDs to provide hydroelectric power. DOE’s Oak Ridge National Laboratory (ORNL), with input from DOE’s Idaho National Laboratory, quantified the potential capacity and generation available from adding power production capability to U.S. NPDs. Of the more than 80,000 NPDs throughout the U.S., 54,391 dams were analyzed, with remaining dams eliminated from consideration due to erroneous geographic information, or erroneous flow or drainage area attributes that could not be resolved and corrected through independent investigation of maps and records. Anecdotal information suggests that these dams with missing or erroneous information are likely to be relatively small or have low potential to produce hydroelectric energy. Dams with a reported height of less than five feet were also excluded from analysis. A thorough quality control and review process ensured that the 54,391 remaining NPDs were analyzed and characterized as accurately as possible. Figure ES-1 demonstrates the spatial and capacity potential distribution of the nation’s NPDs. Electric generating capacities included in the report were calculated using the assumption that all water passing a facility would be available for conversion into electrical energy and that hydraulic head at the facility would remain constant. The analysis did not consider the economic feasibility of developing each unpowered facility. The assessment provides preliminary information for stakeholders (such as developers, municipal planners, and policymakers), who can further evaluate the potential to increase hydropower production at NPD sites. Developers could use the information provided in this assessment to focus on more detailed analysis of sites that demonstrate a reasonable potential for being developed. Adding power to U.S. NPDs has the potential to add up to 12 GW (12,000 megawatts or MW) of new renewable capacity—a potential equivalent to increasing the size of the existing conventional hydropower fleet by 15%. A majority of this potential is concentrated in just 100 NPDs, which could contribute approximately 8 GW of clean, reliable hydropower; the top 10 facilities alone could add up to 3 GW of new hydropower. Eighty-one of the 100 top NPDs are U.S. Army Corps of Engineers (USACE) facilities, many of which, including all of the top 10, are navigation locks on the Ohio River, Mississippi River, Alabama River, and Arkansas River, as well as their major tributaries. This study also shows that dams owned by the U.S. Bureau of Reclamation hold the potential to add approximately 260 MW of capacity; the Bureau has also engaged in an effort to conduct a more detailed evaluation of its own facilities.

13 HYDRO ENERGY↗
DOE OSTI2012

Code Qualification of Structural Materials for AFCI Advanced Recycling Reactors

This report summarizes the further findings from the assessments of current status and future needs in code qualification and licensing of reference structural materials and new advanced alloys for advanced recycling reactors (ARRs) in support of Advanced Fuel Cycle Initiative (AFCI). The work is a combined effort between Argonne National Laboratory (ANL) and Oak Ridge National Laboratory (ORNL) with ANL as the technical lead, as part of Advanced Structural Materials Program for AFCI Reactor Campaign. The report is the second deliverable in FY08 (M505011401) under the work package 'Advanced Materials Code Qualification'. The overall objective of the Advanced Materials Code Qualification project is to evaluate key requirements for the ASME Code qualification and the Nuclear Regulatory Commission (NRC) approval of structural materials in support of the design and licensing of the ARR. Advanced materials are a critical element in the development of sodium reactor technologies. Enhanced materials performance not only improves safety margins and provides design flexibility, but also is essential for the economics of future advanced sodium reactors. Code qualification and licensing of advanced materials are prominent needs for developing and implementing advanced sodium reactor technologies. Nuclear structural component design in the U.S. must comply with the ASME Boiler and Pressure Vessel Code Section III (Rules for Construction of Nuclear Facility Components) and the NRC grants the operational license. As the ARR will operate at higher temperatures than the current light water reactors (LWRs), the design of elevated-temperature components must comply with ASME Subsection NH (Class 1 Components in Elevated Temperature Service). However, the NRC has not approved the use of Subsection NH for reactor components, and this puts additional burdens on materials qualification of the ARR. In the past licensing review for the Clinch River Breeder Reactor Project (CRBRP) and the Power Reactor Innovative Small Module (PRISM), the NRC/Advisory Committee on Reactor Safeguards (ACRS) raised numerous safety-related issues regarding elevated-temperature structural integrity criteria. Most of these issues remained unresolved today. These critical licensing reviews provide a basis for the evaluation of underlying technical issues for future advanced sodium-cooled reactors. Major materials performance issues and high temperature design methodology issues pertinent to the ARR are addressed in the report. The report is organized as follows: the ARR reference design concepts proposed by the Argonne National Laboratory and four industrial consortia were reviewed first, followed by a summary of the major code qualification and licensing issues for the ARR structural materials. The available database is presented for the ASME Code-qualified structural alloys (e.g. 304, 316 stainless steels, 2.25Cr-1Mo, and mod.9Cr-1Mo), including physical properties, tensile properties, impact properties and fracture toughness, creep, fatigue, creep-fatigue interaction, microstructural stability during long-term thermal aging, material degradation in sodium environments and effects of neutron irradiation for both base metals and weld metals. An assessment of modified versions of Type 316 SS, i.e. Type 316LN and its Japanese version, 316FR, was conducted to provide a perspective for codification of 316LN or 316FR in Subsection NH. Current status and data availability of four new advanced alloys, i.e. NF616, NF616+TMT, NF709, and HT-UPS, are also addressed to identify the R&D needs for their code qualification for ARR applications. For both conventional and new alloys, issues related to high temperature design methodology are described to address the needs for improvements for the ARR design and licensing. Assessments have shown that there are significant data gaps for the full qualification and licensing of the ARR structural materials. Development and evaluation of structural materials require a variety of experimental facilities that have been seriously degraded in the past. The availability and additional needs for the key experimental facilities are summarized at the end of the report. Detailed information covered in each Chapter is given.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2012

Lab-Based Measurement of Remediation Techniques for Radiation Portal Monitors (Initial Report)

Radiation Portal Monitors (RPM) deployed by the Second Line of Defense (SLD) are known to be sensitive to the natural environmental radioactive background. There are several techniques used to mitigate the effects of background on the monitors, but since the installation environments can vary significantly from one another the need for a standardized, systematic, study of remediation techniques was proposed and carried out. This study is not meant to serve as the absolute last word on the subject. The data collected are, however, intelligible and useful. Some compromises were made, each of which will be described in detail. The hope of this initial report is to familiarize the SLD science teams with ORNL's effort to model the effect of various remediation techniques on simple, static backgrounds. This study provides a good start toward benchmarking the model, and each additional increment of data will serve to make the model more robust. The scope of this initial study is limited to a few basic cases. Its purpose is to prove the utility of lab-based study of remediation techniques and serve as a standard data set for future use. This importance of this first step of standardization will become obvious when science teams are working in parallel on issues of remediation; having a common starting point will do away with one category of difference, thereby making easier the task of determining the sources of disagreement. Further measurements will augment this data set, allowing for further constraint of the universe of possible situations. As will be discussed in the 'Going Forward' section, more data will be included in the final report of this work. Of particular interest will be the data taken with the official TSA lead collimators, which will provide more direct results for comparison with installation data.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2012

Fuel Cycle Research & Development Technical Monthly – May 2012

Management and Integration LANL - Initial coordination meetings with NE and NA-20 were held the first week of May. Additional meetings, to include NA-82 and the new Proliferation and Terrorism Risk Assessment task are scheduled for June. Work package planning as part of the NTD transition is ongoing. Microcalorimetry LANL - Some parts to attempt repair of a malfunctioning water chiller that has been holding up work on the current detector array have arrived. We will attempt to begin running the compressor/cryostat next week to resume work on commissioning the detector array. We have also been working on a backup plan to temporarily move our system to a different lab space. Completed data analysis and prepared a paper summarizing Pu measurements for peer-review journal. Two members of our team presented work at the SORMA West 2012 conference. Completed data analysis and prepared a milestone report summarizing the development of Monte Carlo tools to study systematic errors. Electrochemical Sensor INL - The second sensor test was stopped short due to the work stand-down. Some activities related to this work have resumed, but not all. The sensor used during the second test was removed from the furnace and it showed cracks and later crumbled when being rinsed for sample preparation. The sensor material will be submitted to SEM analysis once work is resumed in the facilities where analysis is performed. A third sensor test has started. Tests with different arrangements will continue and will be oriented based on post-test analysis of the first three sensor tests. Materials with different annealing temperatures will also be prepared for analysis. Lead slowing down spectrometer LANL - Continued work on perturbation method for LSDS analysis. We are running simulations to delineate issues and are checking additional data libraries to see whether there are differences in simulation results. Electrochemical sensor INL - The second sensor test was stopped short due to the work stand-down. Some activities related to this work have resumed, but not all. The sensor used during the second test was removed from the furnace and it showed cracks and later crumbled when being rinsed for sample preparation. The sensor material will be submitted to SEM analysis once work is resumed in the facilities where analysis is performed. A third sensor test has started. Tests with different arrangements will continue and will be oriented based on post-test analysis of the first three sensor tests. Materials with different annealing temperatures will also be prepared for analysis. Fast Neutron Multiplicity analysis INL - The University of Michigan team continues its work on the post-experiment analysis of the validation data from JRC ISPRA, as well as scoping studies using the simulation tool MCNPX-PoliMi. At INL, our new staff member working on this project is now working to model performance capabilities for the fast-neutrons scintillator design concepts. At INL our primary analysis approach is focused on the Feynman mean-to-variance approach. At the University of Michigan, the primary analysis approach is multiplicity coincidence analysis. Fast Neutron Imaging to Quantify Nuclear Materials ORNL - Completed additional measurements of the two 'trainer' configurations as well as calibration measurements with sources on an x-y stage. The imager was shipped to Pantex for an NA-22 obligation at the end of May. Lead Slowing Down Spectrometer LANL - Continued to look into He4 detector. A Swiss company was located that makes He4 detectors and associated electronics. Had a teleconference with them to assess the possible help we can get from them. We are also looking in to constructing one locally. Ongoing perturbation calculations are providing information on the fundamental systematic error limits of LSDS. In order to achieve separating the contribution of Pu and 235U to the signal, there will need to be tight controls on systematic errors. Multi-isotope Process Monitor PNNL - Attended a training call in advanced multivariate classification and analysis methods. These methods were applied to the multivariate analysis of fuel characteristics based on simulated gamma. Work continued on a computational framework to quantify the impact of gamma-ray counting statistical precision on principal component regression (PCR) analysis of a multi-component (i.e. multi-isotope) gammaray spectrum. Tests of the simulation framework are anticipated to begin in early June. Development of a proposal to instrument H-Canyon is being prepared in conjunction with SRNL and the NNSA's NGSI program is ongoing.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2012

Evaluating the Effects of the Kingston Fly Ash Release on Fish Reproduction: Spring 2009 – 2010 Studies

On December 22, 2008, a dike containing fly ash and bottom ash at the Tennessee Valley Authority's (TVA) Kingston Fossil Plant in East Tennessee failed and released a large quantity of ash into the adjacent Emory River. Ash deposits from the spill extended 4 miles upstream of the facility to Emory River mile 6 and downstream to Tennessee River mile 564 ({approx}8.5 miles downstream of the confluence of the Emory River with the Clinch River, and {approx}4 miles downstream of the confluence of the Clinch River with the Tennessee River). A byproduct of coal combustion, fly ash contains a variety of metals and other elements which, at sufficient concentrations and in specific forms, can be harmful to biological systems. The ecological effects of fly ash contamination on exposed fish populations depend on the magnitude and duration of exposure, with the most significant risk considered to come from elevated levels of certain metals in the ash, particularly selenium, on fish reproduction and fish early life stages (Lemly 1993; Besser and others 1996). The ovaries of adult female fish in a lake contaminated by coal ash were reported to have an increased frequency of atretic oocytes (dead or damaged immature eggs) and reductions in the overall numbers of developing oocytes (Sorensen 1988) associated with elevated body burdens of selenium. Larval fish exposed to selenium through maternal transfer of contaminants to developing eggs in either contaminated bodies of water (Lemly 1999) or in experimental laboratory exposures (Woock and others 1987, Jezierska and others 2009) have significantly increased incidences of developmental abnormalities. Contact of fertilized eggs and developing embryos to ash in water and sediments may also pose an additional risk to the early life stages of exposed fish populations through direct uptake of metals and other ash constituents (Jezierska and others 2009). The establishment and maintenance of fish populations is intimately associated with the ability of individuals within a population to reproduce. Reproduction is thus generally considered to be the most critical life function affected by environmental contamination. From a regulatory perspective, the issue of potential contaminant-related effects on fish reproduction from the Kingston fly ash spill has particular significance because the growth and propagation of fish and other aquatic life is a specific classified use of the affected river systems. To address the potential effects of fly ash from the Kingston spill on the reproductive health of exposed fish populations, ORNL has undertaken a series of studies in collaboration with TVA that include: (1) a combined field study of metal bioaccumulation in ovaries and other fish tissues (Adams and others 2012) and the reproductive condition of sentinel fish species in reaches of the Emory and Clinch Rivers affected by the fly ash spill (the current report); (2) laboratory tests of the potential toxicity of fly ash from the spill area on fish embryonic and larval development (Greeley and others 2012); (3) additional laboratory experimentation focused on the potential effects of long-term exposures to fly ash on fish survival and reproductive competence (unpublished); and (4) a combined field and laboratory study examining the in vitro developmental success of embryos and larvae obtained from fish exposed in vivo for over two years to fly ash in the Emory and Clinch Rivers (unpublished). The current report focuses on the reproductive condition of adult female fish in reaches of the Emory and Clinch Rivers influenced by the fly ash spill at the beginning of the spring 2009 breeding season - the first breeding season immediately following the fly ash release - and during the subsequent spring 2010 breeding season. Data generated from this and related reproductive/early life stage studies provide direct input to ecological risk assessment efforts and complement and support other phases of the overall biomonitoring program associated with the fly ash spill.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2012

Evaluating the Effects of Fly Ash Exposure on Fish Early Life Stages: Fathead Minnow Embryo-Larval Tests

On December 22, 2008, a dike containing fly ash and bottom ash in an 84-acre complex of the Tennessee Valley Authority's (TVA) Kingston Steam Plant in East Tennessee failed and released a large quantity of ash into the adjacent Emory River. Ash deposits extended as far as 4 miles upstream (Emory River mile 6) of the Plant, and some ash was carried as far downstream as Tennessee River mile 564 ({approx}4 miles downstream of the Tennessee River confluence with the Clinch River). A byproduct of coal burning power plants, fly ash contains a variety of metals and other elements which, at sufficient concentrations and in specific forms, can be toxic to biological systems. The effects of fly ash contamination on exposed fish populations depend on the magnitude and duration of exposure, with the most significant risk considered to be the effects of specific ash constituents, especially selenium, on fish early life stages. Uptake by adult female fish of fly ash constituents through the food chain and subsequent maternal transfer of contaminants to the developing eggs is thought to be the primary route of selenium exposure to larval fish (Woock and others 1987, Coyle and others 1993, Lemly 1999, Moscatello and others 2006), but direct contact of the fertilized eggs and developing embryos to ash constituents in river water and sediments is also a potential risk factor (Woock and others 1987, Coyle and others 1993, Jezierska and others 2009). To address the risk of fly ash from the Kingston spill to the reproductive health of downstream fish populations, ORNL has undertaken a series of studies in collaboration with TVA including: (1) a field study of the bioaccumulation of fly ash constituents in fish ovaries and the reproductive condition of sentinel fish species in reaches of the Emory and Clinch Rivers affected by the fly ash spill; (2) laboratory tests of the potential toxicity of fly ash from the spill area on fish embryonic and larval development (reported in the current technical manuscript); (3) additional laboratory experimentation focused on the potential effects of long-term exposures to fly ash on fish survival and reproductive competence; and (4) a combined field and laboratory study examining the in vitro developmental success of embryos and larvae obtained from fish exposed in vivo for over two years to fly ash in the Emory and Clinch Rivers. These fish reproduction and early life-stage studies are being conducted in conjunction with a broader biological monitoring program administered by TVA that includes a field study of the condition of larval fish in the Emory and Clinch Rivers along with assessments of water quality, sediment composition, ecotoxicological studies, terrestrial wildlife studies, and human and ecological risk assessment. Information and data generated from these studies will provide direct input into risk assessment efforts and will also complement and help support other phases of the overall biomonitoring program. Fish eggs, in general, are known to be capable of concentrating heavy metals and other environmental contaminants from water-borne exposures during embryonic development (Jezierska and others 2009), and fathead minnow embryos in particular have been shown to concentrate methylmercury (Devlin 2006) as well as other chemical toxicants. This technical report focuses on the responses of fathead minnow embryos to simple contact exposures to fly ash in laboratory toxicity tests adapted from a standard fathead minnow (Pimephales promelas) 7-d embryo-larval survival and teratogenicity test (method 1001.0 in EPA 2002) with mortality, hatching success, and the incidences of developmental abnormalities as measured endpoints.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2012

Fuel Cycle Research & Development: Technical Monthly – June 2012

Topics are: (1) MPACT Campaign - (a) Management and Integration • Coordination meetings between NE and NA-22, NA-24, and NA-82 were conducted the week of June 11th. Preparations are being made for the next MPACT working group meeting, scheduled for Aug 28-30 at Idaho Falls. In addition to covering accomplishments and discussing future plans, a site tour of INL facilities (MFC, EBR, ATR, INTEC) is being organized. (2) Accounting and Control Technologies - (a) Microcalorimetry • Now operating 256-pixel array at LANL. We are in the process of tuning detector parameters to improve and optimize performance. Preliminary measurements show approximate number of live pixels is similar to that observed previously at NIST. Continuing to study contribution to systematic error from uncertainties in tabulated gamma-ray energies. (b) Electrochemical Sensor • Testing of sensors fashioned from different precursor materials continued. SEM analysis of all used sensors has been or will be performed. (c) Lead Slowing Down Spectrometer • Ongoing perturbation calculations are providing information on the fundamental systematic error limits of LSDS. In order to achieve separating the contribution of Pu and 235U to the signal, there will need to be tight controls on systematic errors. Continuing to look into a He4 detector. Research into local construction of a He4 detector continued. We have started to apply the algorithm to test the LSDS using experimental data from previous RPI measurements. PNNL also developed a plan to address the lack of statistics in the MCNP modeling of the NGSI 64 assemblies. The ISU graduate student built and tested a fission chamber to gain experience with them. (d) Fast Neutron Imaging to Quantify Nuclear Materials • The imaging detector design was modified for each pixel to have an 8 x 8 pixel array. Quotations and purchasing process for components, including the new PSD scintillator are in progress. (e) Fast Neutron Multiplicity Analysis • The team submitted two papers to the upcoming INMM meeting that are related to the fast neutron multiplicity R&D effort. Progress was made on the project's main goal of designing a concept for a prototype fast-neutron multiplicity counter. We started laying out the outline for the final report. We have been working with our ORNL collaborators to develop a new digitizer system to support our experimental campaign planned for next year. (3) MPACT Analysis Tools - (a) Multi-isotope Process Monitor • Fuel characterization framework development continued during June. A report describing the methodologies is being completed. Kenneth Dayman, from University of Texas, spent a week at PNNL wrapping up his master's research and working on a journal submission covering that work. The target journal is the IEEE transactions on Nuclear Science; submission is planned for the end of July. A proposal to instrument H-Canyon is being prepared in conjunction with SRNL and the NNSA's NGSI program. The impact of gamma-ray spectrum counting statistics on the precision of relative radioisotope component intensities as reconstructed via Principal Component Regression (PCR) continued in June with Monte Carlo simulations of a two-component (i.e., two radioisotope) system. This work generalizes earlier studies in FY12 in which Poisson counting variations of only a single spectrum component were simulated. (b) Modeling and Simulation for Analysis of Safeguards Performance (Electrochemical) • Preliminary insights into safeguards challenges and the initial design for an electrochemical plant have been written up into an INMM paper and will be presented at the INMM Summer Meeting. Work is currently adding a new visualization capability for integrating materials accountancy with physical protection. (c) Material Control including Process Monitoring (Pattern Recognition, Sensors) • Fabrication of quartz chips continued at an external foundry. Awaiting delivery of the heat exchange manifold and chip holder. (d) MPACT System Integration and Technical Support • The initial report on cost-basis metrics for nuclear material security risk and proliferation risk was completed as scheduled. (4) Safeguards and Security by Design - (a) Used fuels storage security analysis, guidance and best practices • RFP was finalized and sent out. Awaiting response from World Institute for Nuclear Security. Coordinated with Scott Demuth on joint report • LANL milestone on best practices. Attended Nuclear Energy Institute National Nuclear Security Conference. Developed plan for soliciting input on prioritized issues for used fuel storage security. Worked on setting up a meeting with the Nuclear Regulatory Commission. Worked on FY2013 work package planning.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2012

Efficiency of TTAC's ORTEC IDM

ORNL's Technical Testing and Analysis Center (TTAC) acquired a High Purity Germanium Detector (HPGe) from ORTEC - a variant called an Interchangeable Detection Module (IDM). This detector has excellent energy resolution as well as high intrinsic efficiency. The purpose of this report is to detail the determination of the efficiency curve of the IDM, so future measurements can quantify the (otherwise unknown) activity of sources. Without such a curve, the activity cannot be directly reported by use of the IDM alone - a separate device such as an ion chamber would be required. This builds upon the capability of TTAC. The method for determining the energy-dependent intrinsic efficiency is laid-out in this report. It's noteworthy that this basic technique can be applied to any spectroscopic radiation detector, independent of the specific type (e.g. NaI, CzT, ClYC).

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2012

Novel refractory materials for high alkali, high temperature environments

A project was led by Oak Ridge National Laboratory (ORNL) in collaboration with a research team comprised of the academic institution Missouri University of Science and Technology (MS&T), and the industrial company MINTEQ International, Inc. (MINTEQ), along with representatives from the aluminum, chemical, glass, and forest products industries. The project was to address the need for new innovative refractory compositions by developing a family of novel MgO-Al 2O3, MgAl2O4, or other similar spinel structured or alumina-based unshaped refractory compositions (castables, gunnables, shotcretes, etc.) utilizing new aggregate materials, bond systems, protective coatings, and phase formation techniques (in-situ phase formation, altered conversion temperatures, accelerated reactions, etc). This family of refractory compositions would then be tailored for use in high-temperature, high-alkaline industrial environments like those found in the aluminum, chemical, forest products, glass, and steel industries. Both practical refractory development experience and computer modeling techniques were used to aid in the design of this new family of materials.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2012

Mesoscale Benchmark Demonstration, Problem 1: Mesoscale Simulations of Intra-granular Fission Gas Bubbles in UO 2 under Post-irradiation Thermal Annealing

A study was conducted to evaluate the capabilities of different numerical methods used to represent microstructure behavior at the mesoscale for irradiated material using an idealized benchmark problem. The purpose of the mesoscale benchmark problem was to provide a common basis to assess several mesoscale methods with the objective of identifying the strengths and areas of improvement in the predictive modeling of microstructure evolution. In this work, mesoscale models (phase-field, Potts, and kinetic Monte Carlo) developed by PNNL, INL, SNL, and ORNL were used to calculate the evolution kinetics of intra-granular fission gas bubbles in UO 2 fuel under post-irradiation thermal annealing conditions. The benchmark problem was constructed to include important microstructural evolution mechanisms on the kinetics of intra-granular fission gas bubble behavior such as the atomic diffusion of Xe atoms, U vacancies, and O vacancies, the effect of vacancy capture and emission from defects, and the elastic interaction of non-equilibrium gas bubbles. An idealized set of assumptions was imposed on the benchmark problem to simplify the mechanisms considered. The capability and numerical efficiency of different models are compared against selected experimental and simulation results. These comparisons find that the phase-field methods, by the nature of the free energy formulation, are able to represent a larger subset of the mechanisms influencing the intra-granular bubble growth and coarsening mechanisms in the idealized benchmark problem as compared to the Potts and kinetic Monte Carlo methods. It is recognized that the mesoscale benchmark problem as formulated does not specifically highlight the strengths of the discrete particle modeling used in the Potts and kinetic Monte Carlo methods. Future efforts are recommended to construct increasingly more complex mesoscale benchmark problems to further verify and validate the predictive capabilities of the mesoscale modeling methods used in this study.

99 GENERAL AND MISCELLANEOUS↗
DOE OSTI2011

Biomass Energy Data Book: Edition 4

The Biomass Energy Data Book is a statistical compendium prepared and published by Oak Ridge National Laboratory (ORNL) under contract with the Biomass Program in the Energy Efficiency and Renewable Energy (EERE) program of the Department of Energy (DOE). Designed for use as a convenient reference, the book represents an assembly and display of statistics and information that characterize the biomass industry, from the production of biomass feedstocks to their end use, including discussions on sustainability. This is the fourth edition of the Biomass Energy Data Book which is only available online in electronic format. There are five main sections to this book. The first section is an introduction which provides an overview of biomass resources and consumption. Following the introduction to biomass, is a section on biofuels which covers ethanol, biodiesel and bio-oil. The biopower section focuses on the use of biomass for electrical power generation and heating. The fourth section is on the developing area of biorefineries, and the fifth section covers feedstocks that are produced and used in the biomass industry. The sources used represent the latest available data. There are also two appendices which include frequently needed conversion factors, a table of selected biomass feedstock characteristics, and discussions on sustainability. A glossary of terms and a list of acronyms are also included for the reader's convenience.

Boundy, Robert Gary↗