Abstract
A key component to closing the nuclear fuel cycle is the storage and disposition of nuclear waste in geologic systems. Multiphase ceramic waste forms have been studied extensively as a potential host matrix for nuclear waste. Understanding the speciation, partitioning, and release behavior of radionuclides immobilized in multiphase ceramic waste forms is a critical aspect of developing the scientific and technical basis for nuclear waste management. In this study, we evaluated a sodalite-bearing multiphase ceramic waste form (i.e., fluidized-bed steam reform sodium aluminosilicate [FBSR NAS] product) as a potential host matrix for long-lived radionuclides, such as technetium (99Tc). The FBSR NAS material consists primarily of nepheline (ideally NaAlSiO4), anion-bearing sodalites (ideally M8[Al6Si6O24]X2, where M refers to alkali and alkaline earth cations and X refers to monovalent anions), and nosean (ideally Na8[AlSiO4]6SO4). Bulk X-ray absorption fine structure analysis of the multiphase ceramic waste form, suggest rhenium (Re) is in the Re(VII) oxidation state and has partitioned to a Re-bearing sodalite phase (most likely a perrhenate sodalite Na8[Al6Si6O24](ReO4)2). Rhenium was added as a chemical surrogate for 99Tc during the FBSR NAS synthesis process. The weathering behavior of the FBSR NAS material was evaluated under hydraulically unsaturated conditions with deionized water at 90°C. The steady-state Al, Na, and Si concentrations suggests the weathering mechanisms are consistent with what has been observed for other aluminosilicate minerals and include a combination of ion exchange, network hydrolysis, and the formation of an enriched-silica surface layer or phase. The steady-state S and Re concentrations are within an order of magnitude of the nosean and perrhenate sodalite solubility, respectively. The order of magnitude difference between the observed and predicted concentration for Re and S may be associated with the fact that the anion-bearing sodalites contained in the multiphase ceramic matrix are present as mixed-anion sodalite phases. These results suggest the multiphase FBSR NAS material may be a viable host matrix for long-lived, highly mobilie radionuclides which is a critical aspect in the management of nuclear waste.
| Original language | English |
|---|---|
| Pages (from-to) | 47-59 |
| Number of pages | 13 |
| Journal | Applied Geochemistry |
| Volume | 42 |
| DOIs | |
| State | Published - Mar 2014 |
Funding
This research was supported by the U.S. Department of Energy’s (DOE) Environmental Management (EM) Tank Waste Management program and DOE EMs Office of River Protection, Immobilization of Low-Activity Waste Program. Portions of this research was performed at Oak Ridge National Laboratory (ORNL), Pacific Northwest National Laboratory (PNNL), Lawrence Berkeley National Laboratory (LBNL), Savannah River National Laboratory (SRNL), and Brookhaven National Laboratory (BNL). ORNL is operated by UT-Battelle, LLC for DOE under Contract No. DE-AC05-00OR22725. PNNL is operated by Battelle for DOE under Contract No. DE-AC05-76RL0-1830. LBNL is managed by the University of California for DOE under Contract No. DE-AC02-05CH11231. SRNL is managed by Savannah River Nuclear Solutions for DOE. A portion of this research was carried out with the use of the National Synchrotron Light Source an Office of Science, Office of Basic Energy Sciences, User Facility operated by BNL for DOE under Contract No. DE-AC02-98CH10886. Portions of this research were carried out at the Stanford Synchrotron Radiation Lightsource, a Directorate of SLAC National Accelerator Laboratory and an Office of Science User Facility operated for DOE Office of Science by Stanford University. The SSRL Structural Molecular Biology Program is supported by the DOE Office of Biological and Environmental Research, and by the National Institutes of Health, National Center for Research Resources, Biomedical Technology Program (P41RR001209).