Chemical aspects of actinides in the geosphere: towards a rational nuclear materials management
A complete understanding of actinide interactions in the geosphere is paramount for developing a rational Nuclear and Environmental Materials Management Policy. One of the key challenges towards understanding the fate and transport of actinides is determining their speciation (i.e., oxidation state and structure). Since an element's speciation directly dictates physical properties such as toxicity and solubility, this information is critical for evaluating and controlling the evolution of an actinide element through the environment. Specific areas within nuclear and environmental management programs where speciation is important are (1) waste processing and separations; (2) wasteform materials for long-term disposition; and (3) aqueous geochemistry. The goal of this project was to develop Actinide X-ray Absorption Spectroscopy ( U S ) as a core capability at LLNL and integrate it with existing facilities, providing a multi-technique approach to actinide speciation. XAS is an element-specific structural probe which determines the oxidation state and structure for most atoms. XAS can be more incisive than other spectroscopies because it originates from an atomic process and the information is always attainable, regardless of an element's speciation. Despite the utility, XAS is relatively complex due to the need for synchrotron radiation and significant expertise with data acquisition and analysis. The coupling of these technical hurdles with the safe handling of actinides at a general user synchrotron facility such as the Stanford Synchrotron Radiation Facility (SSRL) make such experiments even more difficult. As a result, XAS has been underutilized by programs that could benefit by its application. We achieved our project goals by implementing key state-of-the-art Actinide XAS instrumentation at SSRL (Ge detector and remote positioning equipment), and by determining the chemical speciation of actinides (Th, U, and Np) in aqueous solutions, wasteform cements, and with geologic materials. The results provide a rational scientific basis for ongoing DOE projects involving nuclear and environmental materials challenges. Future LLNL projects will utilize the Actinide XAS expertise to characterize actinides in important chemical systems, while continuing to improve the XAS capabilities to study metallic alloys, cryogenic sample conditions, and lower analyte concentrations.
- Research Organization:
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Sponsoring Organization:
- US Department of Energy (US)
- DOE Contract Number:
- W-7405-ENG-48
- OSTI ID:
- 15005560
- Report Number(s):
- UCRL-ID-142414; TRN: US0305545
- Resource Relation:
- Other Information: PBD: 9 Feb 2001
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
12 MANAGEMENT OF RADIOACTIVE WASTES, AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES
36 MATERIALS SCIENCE
43 PARTICLE ACCELERATORS
42 ENGINEERING
ABSORPTION SPECTROSCOPY
ACTINIDES
AQUEOUS SOLUTIONS
DATA ACQUISITION
ENVIRONMENTAL MATERIALS
LAWRENCE LIVERMORE NATIONAL LABORATORY
MANAGEMENT
NUCLEAR MATERIALS MANAGEMENT
PHYSICAL PROPERTIES
SYNCHROTRON RADIATION
VALENCE
WASTE FORMS
WASTE PROCESSING