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Title: Single Phase Melt Processed Powellite (Ba,Ca) MoO{sub 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{sub 4} crystalline structure can be formed by reaction with alkaline earth elements. In this study, single phase BaMoO{sub 4} and CaMoO{sub 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 CaMoO{sub 4} and BaMoO{sub 4} powellite phases exhibit radiation stability up to 1000 years at anticipated doses with a crystalline to amorphous transition observed after 1 X 10{sup 13} Gy. Aqueous durability determined from product consistency tests (PCT) showed low normalized release rates for Ba, Ca, and Mo (<0.05 g/m{sup 2}).

Authors:
 [1];  [1];  [1];  [1];  [2];  [3]
  1. Savannah River Site (SRS), Aiken, SC (United States)
  2. Paci fic Northwest National Laboratory , Richland, WA (United States)
  3. Los Alamos National Laboratory , Los Alamos, NM (United States)
Publication Date:
Research Org.:
Savannah River Site (SRS), Aiken, SC (United States)
Sponsoring Org.:
USDOE (United States)
OSTI Identifier:
1053795
Report Number(s):
SRNL-STI-2012-00569
Journal ID: ISSN 0925-8388; TRN: US1300246
DOE Contract Number:  
DE-AC09-08SR22470
Resource Type:
Journal Article
Journal Name:
Journal of Alloys and Compounds
Additional Journal Information:
Journal Name: Journal of Alloys and Compounds; Journal ID: ISSN 0925-8388
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, Marra, James, Fox, Kevin, Reppert, Jason, Crum, Jarrod, and Tang, Ming. Single Phase Melt Processed Powellite (Ba,Ca) MoO{sub 4} For The Immobilization Of Mo-Rich Nuclear Waste. United States: N. p., 2012. Web. doi:10.1016/j.jallcom.2012.09.049.
Brinkman, Kyle, Marra, James, Fox, Kevin, Reppert, Jason, Crum, Jarrod, & Tang, Ming. Single Phase Melt Processed Powellite (Ba,Ca) MoO{sub 4} For The Immobilization Of Mo-Rich Nuclear Waste. United States. doi:10.1016/j.jallcom.2012.09.049.
Brinkman, Kyle, Marra, James, Fox, Kevin, Reppert, Jason, Crum, Jarrod, and Tang, Ming. Mon . "Single Phase Melt Processed Powellite (Ba,Ca) MoO{sub 4} For The Immobilization Of Mo-Rich Nuclear Waste". United States. doi:10.1016/j.jallcom.2012.09.049. https://www.osti.gov/servlets/purl/1053795.
@article{osti_1053795,
title = {Single Phase Melt Processed Powellite (Ba,Ca) MoO{sub 4} For The Immobilization Of Mo-Rich Nuclear Waste},
author = {Brinkman, Kyle and Marra, James and Fox, Kevin and Reppert, Jason and Crum, Jarrod 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)MoO{sub 4} crystalline structure can be formed by reaction with alkaline earth elements. In this study, single phase BaMoO{sub 4} and CaMoO{sub 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 CaMoO{sub 4} and BaMoO{sub 4} powellite phases exhibit radiation stability up to 1000 years at anticipated doses with a crystalline to amorphous transition observed after 1 X 10{sup 13} Gy. Aqueous durability determined from product consistency tests (PCT) showed low normalized release rates for Ba, Ca, and Mo (<0.05 g/m{sup 2}).},
doi = {10.1016/j.jallcom.2012.09.049},
journal = {Journal of Alloys and Compounds},
issn = {0925-8388},
number = ,
volume = ,
place = {United States},
year = {2012},
month = {9}
}