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Title: Single phase melt processed powellite (Ba,Ca)MoO 4 for the immobilization of Mo-rich nuclear waste

Abstract

Crystalline and glass composite materials are currently being investigated for the immobilization of combined High Level Waste (HLW) streams resulting from potential commercial fuel reprocessing scenarios. Several of these potential waste streams contain elevated levels of transition metal elements such as molybdenum (Mo). Molybdenum has limited solubility in typical silicate glasses used for nuclear waste immobilization. Under certain chemical and controlled cooling conditions, a powellite (Ba,Ca)MoO 4 crystalline structure can be formed by reaction with alkaline earth elements. In this study, single phase BaMoO 4 and CaMoO 4 were formed from carbonate and oxide precursors demonstrating the viability of Mo incorporation into glass, crystalline or glass composite materials by a melt and crystallization process. X-ray diffraction, photoluminescence, and Raman spectroscopy indicated a long range ordered crystalline structure. In situ electron irradiation studies indicated that both CaMoO4 and BaMoO 4 powellite phases exhibit radiation stability up to 1000 years at anticipated doses with a crystalline to amorphous transition observed after 1 x 10 13 Gy. Aqueous durability determined from product consistency tests (PCT) showed low normalized release rates for Ba, Ca, and Mo (<0.05 g/m2).

Authors:
 [1];  [1];  [1];  [1];  [2];  [3]
  1. Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1158504
Report Number(s):
PNNL-SA-94806
Journal ID: ISSN 0925-8388
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Journal of Alloys and Compounds
Additional Journal Information:
Journal Volume: 551; Journal ID: ISSN 0925-8388
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; waste form; nuclear materials; radiation damage; chemical durability

Citation Formats

Brinkman, Kyle, Fox, Kevin M., Marra, James C., Reppert, Jason, Crum, Jarrod V., and Tang, Ming. Single phase melt processed powellite (Ba,Ca)MoO4 for the immobilization of Mo-rich nuclear waste. United States: N. p., 2012. Web. doi:10.1016/j.jallcom.2012.09.049.
Brinkman, Kyle, Fox, Kevin M., Marra, James C., Reppert, Jason, Crum, Jarrod V., & Tang, Ming. Single phase melt processed powellite (Ba,Ca)MoO4 for the immobilization of Mo-rich nuclear waste. United States. doi:10.1016/j.jallcom.2012.09.049.
Brinkman, Kyle, Fox, Kevin M., Marra, James C., Reppert, Jason, Crum, Jarrod V., and Tang, Ming. Tue . "Single phase melt processed powellite (Ba,Ca)MoO4 for the immobilization of Mo-rich nuclear waste". United States. doi:10.1016/j.jallcom.2012.09.049.
@article{osti_1158504,
title = {Single phase melt processed powellite (Ba,Ca)MoO4 for the immobilization of Mo-rich nuclear waste},
author = {Brinkman, Kyle and Fox, Kevin M. and Marra, James C. and Reppert, Jason and Crum, Jarrod V. and Tang, Ming},
abstractNote = {Crystalline and glass composite materials are currently being investigated for the immobilization of combined High Level Waste (HLW) streams resulting from potential commercial fuel reprocessing scenarios. Several of these potential waste streams contain elevated levels of transition metal elements such as molybdenum (Mo). Molybdenum has limited solubility in typical silicate glasses used for nuclear waste immobilization. Under certain chemical and controlled cooling conditions, a powellite (Ba,Ca)MoO4 crystalline structure can be formed by reaction with alkaline earth elements. In this study, single phase BaMoO4 and CaMoO4 were formed from carbonate and oxide precursors demonstrating the viability of Mo incorporation into glass, crystalline or glass composite materials by a melt and crystallization process. X-ray diffraction, photoluminescence, and Raman spectroscopy indicated a long range ordered crystalline structure. In situ electron irradiation studies indicated that both CaMoO4 and BaMoO4 powellite phases exhibit radiation stability up to 1000 years at anticipated doses with a crystalline to amorphous transition observed after 1 x 1013 Gy. Aqueous durability determined from product consistency tests (PCT) showed low normalized release rates for Ba, Ca, and Mo (<0.05 g/m2).},
doi = {10.1016/j.jallcom.2012.09.049},
journal = {Journal of Alloys and Compounds},
issn = {0925-8388},
number = ,
volume = 551,
place = {United States},
year = {2012},
month = {10}
}