DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Synergy in Materials: Leveraging Phosphosilicate Waste Forms for Electrochemical Salt Waste

Journal Article · · ACS Sustainable Resource Management
ORCiD logo [1]; ORCiD logo [2];  [3];  [4];  [2];  [3];  [3]; ORCiD logo [2]; ORCiD logo [1]
  1. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Washington State University, Pullman, WA (United States)
  2. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
  3. Missouri University of Science and Technology, Rolla, MO (United States)
  4. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Colorado State University, Fort Collins, CO (United States)

Here, waste forms containing glassy and crystalline phosphate and silicate phases were produced to immobilize salt waste simulants from pyroprocessing and characterized by using Raman spectroscopy, Mössbauer spectroscopy, X-ray diffraction, scanning electron microscopy, heat capacity, and chemical durability measurements. In this work, a phosphosilicate waste form is presented to leverage the benefits of both borosilicate glasses and iron phosphate glasses. To improve waste loading, prior to immobilization, salt simulants were successfully dechlorinated using ammonium dihydrogen phosphate, mixed with a borosilicate frit (5–30 wt %) and Fe2O3, and vitrified. Additions of 2.5–15 wt % borosilicate glass (NBS3) improved normalized release rates for Cs relative to iron-phosphates without NBS3, resulting in chemical durabilities similar to high-level waste borosilicate glass reference materials. The release rates of the alkalis (i.e., Li, Na, K, Cs) were the lowest with the addition of 5 wt % NBS3. Although Sr was not specifically targeted in this study, evidence exists that it preferentially partitioned with Si to form an amorphous droplet phase within the iron phosphate glass matrix.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE Office of Nuclear Energy (NE), Nuclear Fuel Cycle and Supply Chain
Grant/Contract Number:
AC05-76RL01830
OSTI ID:
2549292
Report Number(s):
PNNL-SA--206446
Journal Information:
ACS Sustainable Resource Management, Journal Name: ACS Sustainable Resource Management Journal Issue: 3 Vol. 2; ISSN 2837-1445
Publisher:
ACS PublicationsCopyright Statement
Country of Publication:
United States
Language:
English

References (47)

Encyclopedia of Glass Science, Technology, History, and Culture book February 2021
A study on chlorination of uranium metal using ammonium chloride journal July 2017
Dechlorination of molten chloride waste salt from electrorefining via ion-exchange using pelletized ultra-stable H-Y zeolite in a fluidized particle reactor journal March 2019
Chlorination of uranium metal to uranium trichloride using ammonium chloride journal April 2022
De-chlorination and solidification of radioactive LiCl waste salt by using SiO2-Al2O3-P2O5 (SAP) inorganic composite including B2O3 component journal June 2017
The structure of high-silica alkali-silicate glasses. A Raman spectroscopic investigation journal November 1983
Chloride and water solubility in basalt and andesite melts and implications for magmatic degassing journal March 1999
Properties and structure of sodium-iron phosphate glasses journal July 1997
Raman spectroscopy study of the structure of lithium and sodium ultraphosphate glasses journal January 1998
Chemically durable iron phosphate glass wasteforms journal November 1998
Effect of melting temperature and time on iron valence and crystallization of iron phosphate glasses journal July 1999
Properties of mixed Na2O and K2O iron phosphate glasses journal March 2000
World energy outlook and state of renewable energy: 10-Year evaluation journal December 2023
Structural study of Na2O–FeO–Fe2O3–P2O5 glasses by Raman and Mössbauer spectroscopy journal October 2014
Structure and thermochemical study of strontium sodium phosphate glasses journal September 2016
Redox effects on the structure and properties of Na-Mo-Fe-phosphate glasses journal April 2021
Iodine solubility in a low-activity waste borosilicate glass at 1000°C journal September 2014
Glass binder development for a glass-bonded sodalite ceramic waste form journal June 2017
Investigation of physical and chemical properties for upgraded SAP (SiO2Al2O3P2O5) waste form to immobilize radioactive waste salt journal March 2019
Dehalogenation of electrochemical processing salt simulants with ammonium phosphates and immobilization of salt cations in an iron phosphate glass waste form journal February 2020
Synthesis and characterization of uranium trichloride in alkali-metal chloride media journal July 2022
Dechlorination and vitrification of electrochemical processing salt waste journal August 2022
Compositional effects on the chemical durabilities of aluminophosphate glasses: A review journal March 2024
Heated goethite and natural hematite: Can Raman spectroscopy be used to differentiate them? journal November 2007
Insight into the Partitioning and Clustering Mechanism of Rare-Earth Cations in Alkali Aluminoborosilicate Glasses journal October 2021
Electrochemical Salt Wasteform Development: A Review of Salt Treatment and Immobilization Options journal May 2020
Kinetics of Dechlorination of Molten Chloride Salt Using Protonated Ultrastable Y Zeolite journal July 2019
Dechlorination Apparatus for Treating Chloride Salt Wastes: System Evaluation and Scale-Up journal November 2021
Phosphate-Based Dechlorination of Electrorefiner Salt Waste using a Phosphoric Acid Precursor journal April 2024
Characteristics of Solidified Products Containing Radioactive Molten Salt Waste journal November 2007
Stabilization/Solidification of Radioactive Salt Waste by Using x SiO 2y Al 2 O 3z P 2 O 5 (SAP) Material at Molten Salt State journal December 2008
Electrochemical processing in molten salts – a nuclear perspective journal January 2023
Raman spectroscopic investigation of the structure of silicate glasses. III. Raman intensities and structural units in sodium silicate glasses journal October 1981
Control of Radioactive Waste Glass Melters: I, Preliminary General Limits at Savannah River journal October 1990
A Raman Study of Iron-Phosphate Crystalline Compounds and Glasses: Raman Study of Iron Phosphates journal April 2011
The Future of Nuclear Energy: Electrochemical Reprocessing of Fuel Takes Center Stage journal September 2021
Improving the Integral Fast Reactor's Proposed Salt Waste Management System journal June 2012
Advances in Raman Spectroscopy Applied to Earth and Material Sciences journal January 2014
Road Map for Developing Iron Phosphate Waste Forms for Salt Wastes report February 2021
Evaluating Geologic Disposal Pathways for Advanced Reactor Spent Fuels.
  • Sassani, David; Price, Laura; Park, Heeho
  • Proposed for presentation at the INTERNATIONAL HIGH-LEVEL RADIOACTIVE WASTE MANAGEMENT CONFERENCE held November 13-17, 2022 in phoenix, AZ US https://doi.org/10.2172/2005981
conference November 2022
Crystalline versus Glassy Nature of Iron Phosphate Waste Forms Subjected to Different Slow Cooling Curves report September 2023
Tank waste remediation system high-level waste feed processability assessment report report December 1994
Glass Property Data and Models for Estimating High-Level Waste Glass Volume report October 2009
Retention of Halogens in Waste Glass report May 2010
Development of Electrorefiner Waste salt Disposal Process for the ebr- ii Spent fuel Treatment Project journal April 2008
Pyroprocessing Flowsheets for Recycling used Nuclear fuel journal August 2011
Vitrification of wastes: from unwanted to controlled crystallization, a review journal December 2022