National Security Posters

Nanoparticles, Superabsorbent Gel Used to Clean Radioactivity from Porous Structures Nondestructively

M. D. Kaminski, M. R. Finch, C. J. Mertz, M. Kalensky, N. Kivenas, and J. L. Jerden

Argonne researchers are designing a system to safely capture and dispose of radioactive elements in porous structures outdoors, such as buildings and monuments, using a spray-on, superabsorbent gel and engineered nanoparticles. Such a system would help the nation be more prepared in the event of a terrorist attack with a “dirty bomb” or other radioactive dispersal device.

Contact Mike Kaminski (630-252-4777, kaminski@cmt.anl.gov). View Poster

Functionalized Nanoparticle Development for Impacting a Wide Range of Biomedical Applications

C. J. Mertz, M. R. Finck, Y. Xie, and M. D. Kaminski

Tiny engineered nanoparticles are the key to revolutionary technology that could help detoxify humans following exposure to biological, chemical or radiological weapons; provide earlier diagnosis of medical conditions and better-targeted drug delivery; and selectively remove toxins that result from trauma or auto-immune disease.

Contact Carol Mertz (630-252-4394, mertz@cmt.anl.gov). View Poster

Analytical Chemistry Laboratory: Analytical Services and Research

Vivian Sullivan, Delbert Bowers, Nancy Dietz, Donald Graczyk, Michael Kalensky, Susan Lopykinski, Seema Naik, Yifen Tsai, and Mark Vander Pol

The Analytical Chemistry Laboratory (ACL) is a full-cost-recovery service center, with the primary mission of providing a broad range of analytical chemistry support services to the scientific and engineering programs at Argonne. In addition, the ACL conducts a research program in analytical chemistry, works on instrumental and methods development, and provides analytical services for governmental, educational, and industrial organizations. The ACL handles a wide range of analytical problems, from routine standard analyses to unique problems that require significant development of methods and techniques. Facilities exist for inorganic or organic analysis of radioactive samples.

• The Inorganic Analysis Group uses wet-chemical and instrumental methods for elemental, compositional, and isotopic analyses of solid, liquid, and gaseous samples and provides specialized analytical services.
• The Radiochemical Analysis Group uses nuclear counting techniques in radiochemical analyses over a wide range of sample types, from environmental samples with low radioactivity to samples with high radioactivity that require containment. Other types of analyses use X-ray diffraction, scanning electron microscopy, or transmission electron microscopy instruments.
• The Organic Analysis Group uses a number of complementary techniques to separate and to quantitatively and qualitatively analyze, at the trace level, complex organic mixtures and compounds, including toxic substances, fossil-fuel residues and emissions, environmental pollutants, pesticides, potentially hazardous wastes, and drugs.

Contact Vivian Sullivan (630-252-1890, sullivan@cmt.anl.gov). View Poster

Application of MARLAP to Validation and Verification of Existing Data

Vivian Sullivan

MARLAP (Multi-Agency Radiological Laboratory Analytical Protocols Manual) is a guidance document for the use of radiological data. This poster will show an application of MARLAP to data packages collected under a specific Quality Assurance Project Plan (QAPP) for application to environmental cleanup of sites. The use of MARLAP and the QAPP to develop an Excel worksheet for easy and consistent data verification and validation will also be presented. An overview of MARLAP and radiological data collection, verification and validation through Directed Project Planning will also be provided. This project was funded by the U.S. Army Corps of Engineers, Buffalo District.

Contact Vivian Sullivan (630-252-1890, sullivan@cmt.anl.gov). View Poster

Determination of Actinide and Fission Product Isotopes in High-Burnup Spent Nuclear Fuel

Delbert L. Bowers, Mark A. Clark, Donald G. Graczyk, Vivian S. Sullivan, Yifen Tsai, and Mark H. Vander Pol, and Michael C. Billone

Interest among nuclear power producers has grown over the past few decades in higher utilization of nuclear fuel, which translates to achieving higher burnup (a measure of the number of atoms that underwent fission). Computer codes that predict the time-dependent nuclide inventory in spent nuclear fuels, as needed for safety and licensing evaluations, have been validated for burnup levels up to about 40 GWd/MTU. Experimental isotope-assay data for higher-burnup fuels are relatively rare but are of considerable interest for benchmarking code performance beyond this range, particularly in relation to the concept of “burnup credit,” an allowance in safety analysis calculations for decreased reactivity in the fuel as a result of actinide depletion and a presence of neutron-absorbing irradiation products (poisons) that reduce the fuel’s ability to achieve criticality. This poster describes our determination of a wide array of actinide and fission-product isotopes in light-water-reactor fuel specimens having >70 GWd/MTU burnup. Uranium, plutonium, and neodymium isotopes were measured with isotope-dilution methods to provide high accuracy for these key nuclides. Solutions of the raw fuel and separated fractions were also analyzed by thermal-ionization and inductively-coupled-plasma mass spectrometry, alpha counting, and gamma counting. With relatively few operations, data were made available for 75 isotopes. Some of the burnup-credit isotopes we measured (¹⁰³Rh, ⁹⁵Mo, ¹⁰¹Ru) have not been reported previously for high-burnup fuels.

This work was funded by the U.S. Nuclear Regulatory Commission (through the Energy Technology Division), and by the U.S. Department of Energy, Office of Civilian Radioactive Waste Management, through Argonne’s Energy Technology Division.

Contact Del Bowers (630-252-4354, bowers@cmt.anl.gov). View Poster

Electron Microscopy of Materials

Nancy L. Dietz

Electron microscopy methods are an important part of materials research and development in the Chemical Engineering Division. With ever increasing demands on materials performance, it is essential to relate microstructure and composition to materials properties. Scanning and transmission electron microscopy (SEM and TEM) methods allow for the observation and characterization of materials at this level. This display demonstrates the application of SEM/TEM methods in solving problems of current scientific and technological importance.

Contact Nancy Dietz (630-252-9798, dietz@cmt.anl.gov). View poster

Inductively Coupled Plasma-Mass Spectrometry (ICP-MS) Capabilities and Applications

Yifen Tsai

Inductively coupled plasma-mass spectrometry (ICP-MS) is the most powerful technique for the analysis and quantification of trace elements and isotopes in both liquid and solid samples. There are two ICP-MS systems available in the Chemical Engineering Division. One is the Fisons/VG PQII+ with a quadrupole mass spectrometer, and the other is the VG Elemental Axiom high-resolution ICP-MS with a high-resolution magnetic sector mass spectrometer. Their capabilities for applications in various programs funded by the Department of Energy are presented in this poster.

Contact Yifen Tsai (630-252-7732, tsai@cmt.anl.gov). View Poster

Inductively Coupled Plasma-Optical Emission Spectrometry Method for Material Accountancy Measurements

Susan J. Lopykinski, Donald G.Graczyk, Seema R. Naik, and Alice M. Essling

Spent-fuel-treatment processes being developed for conceptual advanced nuclear-fuel-cycle applications need accurate chemical analysis data to track inventories of the actinide elements (uranium and plutonium) and satisfy material accountancy requirements. Presently, actinide accountancy measurements are done by isotope dilution mass spectrometry (IDMS), which provides high accuracy (± 0.25 % of the value) but requires several days to complete. As a result, processes capable of providing high-throughput separation of spent fuel constituents are hampered by anticipated long measurement delays. In recent years, we have gained experience in using an unconventional inductively coupled plasma-optical emission spectrometry (ICP-OES) approach for precise (0.1% RSD) measurements, which promised faster analysis. The pertinent methodology was conceived at the National Institute of Standards and Technology (NIST) and has been applied there to certification of NIST Standard Reference Materials. In past work, we applied the method for highly precise assays of lithium and aluminum in lithium aluminate ceramics used in tritium production. The present work focused on implementing and evaluating the method to measure uranium. Necessary steps included choosing an appropriate internal standard, selecting analysis wavelengths, establishing a useful range of working concentrations, and optimizing plasma operating conditions. Some effects of sample matrix were evaluated during measurements made with samples of electrolyte salt from a test-scale electrorefiner. Using scandium internal standard, a relative precision better than 0.1% RSD was achieved when matrix-matched standards were used. The ICP-OES method provides data as accurate as that from IDMS but with simpler sample preparation and faster turnaround.

Contact Susan Lopykinski (630-252-7521, lopykinski@cmt.anl.gov). View poster

Use of the ORIGEN2 Code to Determine Isobaric Compositions in the Analysis of Spent Fuel by ICP-MS

Mark H. Vander Pol, Delbert L. Bowers, Candido Pereira

Determining the elements contained in spent fuel is a daunting task not only because of the inherent radiation levels involved, but also the overwhelming number of isotopes present in the fuel. ICP-MS is a useful analytical tool for many types of samples, but the large number of isobaric interferences (isotopes of the same mass) among the elements present in spent fuel makes direct measurement of the concentrations of many elements impossible. Using the fuel composition calculated using ORIGEN2 computer code, we were able to determine those mass numbers where there were no (or very slight) isobaric interferences, and then ratio that mass to the other isotopes of that particular element. This method allowed us to get concentrations for all of the elements from atomic number 38 through 96. Thermal ionization mass spectroscopy was also used in conjunction with ORIGEN as a forensic tool to identify the fuel rod from which the sample was obtained.

This work is supported by the U.S. Department of Energy, Office of Nuclear Energy, Science and Technology.

Contact Mark Vander Pol (630-252-1552, vanderpol@cmt.anl.gov). View Poster