Dissimilar behavior of technetium and rhenium in borosilicatewaste glass as determined by X-ray absorption spectroscopy

Journal Article · Thu Nov 09 04:00:00 EST 2006 · Chemistry of Materials

OSTI ID:901526

Lukens, Wayne W; McKeown, David A; Buechele, Andrew C; Muller, Isabelle S; Shuh, David K; Pegg, Ian L

Technetium-99 is an abundant, long-lived (t1/2 = 213,000 yr)fission product that creates challenges for the safe, long-term disposalof nuclear waste. While 99Tc receives attention largely due to its highenvironmental mobility, it also causes problems during its incorporationinto nuclear waste glass due to the volatility of Tc(VII) compounds. Thisvolatility decreases the amount of 99Tc stabilized in the waste glass andcauses contamination of the waste glass melter and off-gas system. Theapproach to decrease the volatility of 99Tc that has received the mostattention is reduction of the volatile Tc(VII) species to less volatileTc(IV) species in the glass melt. On engineering scale experiments,rhenium is often used as a non-radioactive surrogate for 99Tc to avoidthe radioactive contamination problems caused by volatile 99Tc compounds.However, Re(VII) is more stable towards reduction than Tc(VII), so morereducing conditions would be required in the glass melt to produceRe(IV). To better understand the redox behavior of Tc and Re in nuclearwaste glass, a series of glasses were prepared under different redoxconditions. The speciation of Tc and Re in the resulting glasses wasdetermined by X-ray absorption fine structure spectroscopy. Surprisingly,Re and Tc do not behave similarly in the glass melt. Although Tc(0),Tc(IV), and Tc(VII) were observed in these samples, only Re(0) andRe(VII) were found. In no case was Re(IV) (or Re(VI))observed.

• Research Organization: Ernest Orlando Lawrence Berkeley NationalLaboratory, Berkeley, CA (US)
• Sponsoring Organization: USDOE Director. Office of Science. Office of AdvancedScientific Computing Research. Office of Biological and EnvironmentalResearch. Environmental Remediation Sciences Division
• DOE Contract Number: AC02-05CH11231
• OSTI ID: 901526
• Report Number(s): LBNL--61959; BnR: KP1302000
• Journal Information: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 3 Vol. 19; ISSN CMATEX; ISSN 0897-4756
• Country of Publication: United States
• Language: English

Related Subjects

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS
ABSORPTION
ABSORPTION SPECTROSCOPY
BOROSILICATE GLASS
CERAMIC MELTERS
CONTAMINATION
FINE STRUCTURE
FISSION PRODUCTS
GLASS
OFF-GAS SYSTEMS
RADIOACTIVE WASTES
RHENIUM
SPECTROSCOPY
TECHNETIUM
TECHNETIUM 99
Technetium rhenium nuclear waste glass
VOLATILITY
WASTES