Electrochemical Salt Wasteform Development: A Review of Salt Treatment and Immobilization Options

Riley, Brian J.

doi:10.1021/acs.iecr.0c01357

Title: Electrochemical Salt Wasteform Development: A Review of Salt Treatment and Immobilization Options

Journal Article · Thu May 14 00:00:00 EDT 2020 · Industrial and Engineering Chemistry Research

DOI:https://doi.org/10.1021/acs.iecr.0c01357· OSTI ID:1638741

^[1]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Electrochemical reprocessing, also referred to as pyroprocessing, is a technique for recycling actinides from used nuclear fuel (UNF) to produce fuel for future reactors. Here, UNF is dissolved in a molten salt (e.g., LiCl-KCl eutectic) within an electrorefiner. After UNF dissolution, fission products are released into the electrolyte salt and converted to chlorides. This paper discusses wasteform options for processing the base electrolyte salt with the fission product salts as well as just the rare-earth fission products (as RECl₃, REOCl, or REO_x) with the intent of finding optimal methods for reducing total waste salt volumes or partitioning the salt for alternate wasteform options. Furthermore, two of the more detailed partitioning options discussed herein include halide removal from the salt (dehalogenation), which accounts for more than half of the salt on a molar basis, and RE fission product removal for wasteforms with high-RE loadings. Wasteform properties are compared with emphasis on wasteform volume starting from a given amount of (1) total salt cations or (2) RE cations. Comparisons are also made of wasteform chemical durabilities, with the data available from like testing methods. A main conclusion from this work is the justification of subsequent salt processing after electrorefiner operations for achieving significant wasteform volume reduction.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1638741

Report Number(s):: PNNL-SA-151993

Journal Information:: Industrial and Engineering Chemistry Research, Vol. 59, Issue 21; ISSN 0888-5885

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 13 works

Citation information provided by
Web of Science

References (48)

Stabilization/Solidification of Radioactive Salt Waste by Using x SiO ₂ − y Al ₂ O ₃ − z P ₂ O ₅ (SAP) Material at Molten Salt State Park, Hwan-Seo; Kim, In-Tae; Cho, Yong-Zun Environmental Science & Technology, Vol. 42, Issue 24 https://doi.org/10.1021/es802012x	journal	December 2008
Stability of lanthanide oxides in LiCl–KCl eutectic melt Hayashi, Hirokazu; Minato, Kazuo Journal of Physics and Chemistry of Solids, Vol. 66, Issue 2-4 https://doi.org/10.1016/j.jpcs.2004.06.054	journal	February 2005
On the Development of a Distillation Process for the Electrometallurgical Treatment of Irradiated Spent Nuclear fuel Westphal, Brian R.; Marsden, Kenneth C.; Price, John C. Nuclear Engineering and Technology, Vol. 40, Issue 3 https://doi.org/10.5516/NET.2008.40.3.163	journal	April 2008
Thermal Conversion of Heavy Metal Chlorides (PbCl ₂ , CdCl ₂ ) and Alkaline Chlorides (NaCl, KCl) into Phosphate Glasses Donze, Sébastien; Montagne, Lionel; Palavit, Gérard Chemistry of Materials, Vol. 12, Issue 7 https://doi.org/10.1021/cm991205d	journal	July 2000
Immobilizationof LanthanideOxides Waste fromPyrochemical Process Ahn, B. G.; Park, H. S.; Kim, I. T. Energy Procedia, Vol. 7 https://doi.org/10.1016/j.egypro.2011.06.073	journal	January 2011
Melt Crystallization Process Treatment of LiCl Salt Waste Generated from Electrolytic Reduction Process of Spent Oxide Fuel Cho, Yung-Zun; Ahn, Byung-Gil; Eun, Hee-Chul Energy Procedia, Vol. 7 https://doi.org/10.1016/j.egypro.2011.06.072	journal	January 2011
Dehalogenation of electrochemical processing salt simulants with ammonium phosphates and immobilization of salt cations in an iron phosphate glass waste form Riley, Brian J.; Peterson, Jacob A.; Vienna, John D. Journal of Nuclear Materials, Vol. 529 https://doi.org/10.1016/j.jnucmat.2019.151949	journal	February 2020
SEPARATION OF CsCl FROM LiCl-CsCl MOLTEN SALT BY COLD FINGER MELT CRYSTALLIZATION Versey, Joshua R.; Phongikaroon, Supathorn; Simpson, Michael F. Nuclear Engineering and Technology, Vol. 46, Issue 3 https://doi.org/10.5516/NET.06.2013.082	journal	June 2014
Molten salt reactor waste and effluent management strategies: A review Riley, Brian J.; McFarlane, Joanna; DelCul, Guillermo D. Nuclear Engineering and Design, Vol. 345 https://doi.org/10.1016/j.nucengdes.2019.02.002	journal	April 2019
Iodine solubility in a low-activity waste borosilicate glass at 1000°C Riley, Brian J.; Schweiger, Michael J.; Kim, Dong-Sang Journal of Nuclear Materials, Vol. 452, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2014.04.027	journal	September 2014
Synthesis and characterization of sintered H–Y zeolite-derived waste forms for dehalogenated electrorefiner salt Gardner, Levi D.; Wasnik, Manish S.; Riley, Brian J. Ceramics International, Vol. 46, Issue 11 https://doi.org/10.1016/j.ceramint.2020.04.075	journal	August 2020
Retention of Halogens in Waste Glass Hrma, Pavel R. https://doi.org/10.2172/981571	report	May 2010
Chemical basis for pyrochemical reprocessing of nuclear fuel Ackerman, John P. Industrial & Engineering Chemistry Research, Vol. 30, Issue 1 https://doi.org/10.1021/ie00049a022	journal	January 1991
Improving the Integral Fast Reactor's Proposed Salt Waste Management System Siemer, Darryl D. Nuclear Technology, Vol. 178, Issue 3 https://doi.org/10.13182/NT12-A13599	journal	June 2012
Assessment of lead tellurite glass for immobilizing electrochemical salt wastes from used nuclear fuel reprocessing Riley, Brian J.; Kroll, Jared O.; Peterson, Jacob A. Journal of Nuclear Materials, Vol. 495 https://doi.org/10.1016/j.jnucmat.2017.08.037	journal	November 2017
Characteristics of Solidified Products Containing Radioactive Molten Salt Waste Park, Hwan-Seo; Kim, In-Tae; Cho, Yong-Zun Environmental Science & Technology, Vol. 41, Issue 21 https://doi.org/10.1021/es0712524	journal	November 2007
Synthesis of nuclear waste monazites, ideal actinide hosts for geologic disposal McCarthy, Gregory J.; White, William B.; Pfoertsch, Diane E. Materials Research Bulletin, Vol. 13, Issue 11 https://doi.org/10.1016/0025-5408(78)90215-5	journal	November 1978
Dechlorination of molten chloride waste salt from electrorefining via ion-exchange using pelletized ultra-stable H-Y zeolite in a fluidized particle reactor Wasnik, M. S.; Grant, A. K.; Carlson, K. Journal of Radioanalytical and Nuclear Chemistry, Vol. 320, Issue 2 https://doi.org/10.1007/s10967-019-06476-y	journal	March 2019
Kinetics of Dechlorination of Molten Chloride Salt Using Protonated Ultrastable Y Zeolite Wasnik, Manish S.; Livingston, Tanner C.; Carlson, Krista Industrial & Engineering Chemistry Research, Vol. 58, Issue 33 https://doi.org/10.1021/acs.iecr.9b02577	journal	July 2019
Structure and Chemistry in Halide Lead–Tellurite Glasses McCloy, John S.; Riley, Brian J.; Lipton, Andrew S. The Journal of Physical Chemistry C, Vol. 117, Issue 7 https://doi.org/10.1021/jp310820t	journal	February 2013
Viscosities and working region predictions for bismuth aluminoborosilicate glasses Gardner, Levi D.; Riley, Brian J.; Elliott, Casey International Journal of Applied Glass Science, Vol. 10, Issue 2 https://doi.org/10.1111/ijag.12973	journal	October 2018
Inclusion behavior of Cs, Sr, and Ba impurities in LiCl crystal formed by layer-melt crystallization: Combined first-principles calculation and experimental study Choi, Jung-Hoon; Cho, Yung-Zun; Lee, Tae-Kyo Journal of Crystal Growth, Vol. 371 https://doi.org/10.1016/j.jcrysgro.2013.02.013	journal	May 2013
Pyroprocessing Flowsheets for Recycling used Nuclear fuel Williamson, M. A.; Willit, J. L. Nuclear Engineering and Technology, Vol. 43, Issue 4 https://doi.org/10.5516/NET.2011.43.4.329	journal	August 2011
separation of strontium and cesium from ternary and quaternary lithium chloride-potassium chloride salts via melt crystallization Williams, Ammon N.; Pack, Michael; Phongikaroon, Supathorn Nuclear Engineering and Technology, Vol. 47, Issue 7 https://doi.org/10.1016/j.net.2015.08.006	journal	December 2015
Baseline Glass Development for Combined Fission Products Waste Streams Crum, Jarrod V.; Billings, Amanda Y.; Lang, Jesse B. https://doi.org/10.2172/1048019	report	June 2009
Tellurite glasses for vitrification of technetium-99 from pyrochemical processing Pyo, Jae-Young; Lee, Cheong Won; Park, Hwan-Seo Journal of Nuclear Materials, Vol. 493 https://doi.org/10.1016/j.jnucmat.2017.05.052	journal	September 2017
Treatment of a waste salt delivered from an electrorefining process by an oxidative precipitation of the rare earth elements Cho, Yung-Zun; Yang, Hee-Chul; Park, Gil-Ho Journal of Nuclear Materials, Vol. 384, Issue 3 https://doi.org/10.1016/j.jnucmat.2008.11.020	journal	February 2009
Synthesis and characterization of iodosodalite Chong, Saehwa; Peterson, Jacob; Nam, Junghune Journal of the American Ceramic Society, Vol. 100, Issue 5 https://doi.org/10.1111/jace.14772	journal	March 2017
Separation of CsCl from a ternary CsCl–LiCl–KCl salt via a melt crystallization technique for pyroprocessing waste minimization Williams, Ammon N.; Phongikaroon, Supathorn; Simpson, Michael F. Chemical Engineering Science, Vol. 89 https://doi.org/10.1016/j.ces.2012.12.012	journal	February 2013
A study on chlorination of uranium metal using ammonium chloride Eun, H. C.; Kim, T. J.; Jang, J. H. Journal of Radioanalytical and Nuclear Chemistry, Vol. 314, Issue 1 https://doi.org/10.1007/s10967-017-5359-y	journal	July 2017
Use of electrochemical techniques for the study of solubilization processes of cerium–oxide compounds and recovery of the metal from molten chlorides Castrillejo, Y.; Bermejo, M. R.; Pardo, R. Journal of Electroanalytical Chemistry, Vol. 522, Issue 2 https://doi.org/10.1016/S0022-0728(02)00717-9	journal	April 2002
Characteristics of Wasteform Composing of Phosphate and Silicate To Immobilize Radioactive Waste Salts Park, Hwan-Seo; Cho, In-Hak; Eun, Hee Chul Environmental Science & Technology, Vol. 45, Issue 5 https://doi.org/10.1021/es1029975	journal	March 2011
EUTECTIC(LiCl-KCl) WASTE SALT TREATMENT BY SEQUENCIAL SEPARATION PROCESS Cho, Yung-Zun; Lee, Tae-Kyo; Choi, Jung-Hun Nuclear Engineering and Technology, Vol. 45, Issue 5 https://doi.org/10.5516/NET.06.2013.022	journal	October 2013
Glass waste form options for rare-earth fission products from electrochemical reprocessing Riley, Brian J.; Chong, Saehwa Journal of Non-Crystalline Solids, Vol. 545 https://doi.org/10.1016/j.jnoncrysol.2020.120161	journal	October 2020
Liquidus temperature and chemical durability of selected glasses to immobilize rare earth oxides waste Mohd Fadzil, Syazwani; Hrma, Pavel; Schweiger, Michael J. Journal of Nuclear Materials, Vol. 465 https://doi.org/10.1016/j.jnucmat.2015.06.050	journal	October 2015
Waste form evaluation for RECl3 and REO fission products separated from used electrochemical salt Riley, Brian J.; Pierce, David A.; Crum, Jarrod V. Progress in Nuclear Energy, Vol. 104 https://doi.org/10.1016/j.pnucene.2017.09.005	journal	April 2018
Candidate waste forms for immobilisation of waste chloride salt from pyroprocessing of spent nuclear fuel Vance, E. R.; Davis, J.; Olufson, K. Journal of Nuclear Materials, Vol. 420, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2011.09.020	journal	January 2012
Component effects on crystallization of RE-containing aluminoborosilicate glass Mohd Fadzil, Syazwani; Hrma, Pavel; Schweiger, Michael J. Journal of Nuclear Materials, Vol. 478 https://doi.org/10.1016/j.jnucmat.2016.06.018	journal	September 2016
Tellurite glass as a waste form for mixed alkali–chloride waste streams: Candidate materials selection and initial testing Riley, Brian J.; Rieck, Bennett T.; McCloy, John S. Journal of Nuclear Materials, Vol. 424, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2012.01.024	journal	May 2012
Concentration of Cesium and Strontium Elements Involved in a LiCl Waste Salt by a Melt Crystallization Process Cho, Yung-Zun; Park, Gil-Ho; Lee, Han-Su Nuclear Technology, Vol. 171, Issue 3 https://doi.org/10.13182/NT09-7	journal	September 2010
Properties and structure of sodium-iron phosphate glasses Yu, Xiaoyan; Day, Delbert E.; Long, Gary J. Journal of Non-Crystalline Solids, Vol. 215, Issue 1 https://doi.org/10.1016/S0022-3093(97)00022-7	journal	July 1997
Purification of LiCl–KCl eutectic waste salt containing rare earth chlorides delivered from the pyrochemical process of used nuclear fuel using a reactive distillation process Eun, H. C.; Choi, J. H.; Cho, I. H. Journal of Radioanalytical and Nuclear Chemistry, Vol. 307, Issue 2 https://doi.org/10.1007/s10967-015-4231-1	journal	June 2015
Stabilization/Solidification of Radioactive Molten Salt Waste via Gel-Route Pretreatment Park, Hwan-Seo; Kim, In-Tae; Kim, Hwan-Young Environmental Science & Technology, Vol. 41, Issue 4 https://doi.org/10.1021/es0615472	journal	February 2007
Investigation of physical and chemical properties for upgraded SAP (SiO2Al2O3P2O5) waste form to immobilize radioactive waste salt Lee, Ki Rak; Riley, Brian J.; Park, Hwan-Seo Journal of Nuclear Materials, Vol. 515 https://doi.org/10.1016/j.jnucmat.2019.01.004	journal	March 2019
Characteristics of Oxidation Reaction of Rare-earth Chlorides for Precipitation in LiCl-KCl Molten Salt by Oxygen Sparging Cho, Yong-Jun; Yang, Hee-Chul; Eun, Hee-Chul Journal of Nuclear Science and Technology, Vol. 43, Issue 10 https://doi.org/10.1080/18811248.2006.9711221	journal	October 2006
Glass binder development for a glass-bonded sodalite ceramic waste form Riley, Brian J.; Vienna, John D.; Frank, Steven M. Journal of Nuclear Materials, Vol. 489 https://doi.org/10.1016/j.jnucmat.2017.03.041	journal	June 2017
Precipitation of Rare Earth Compounds in LiCl ‐ KCl Eutectic Katayama, Yasushi; Hagiwara, Rika; Ito, Yasuhiko Journal of The Electrochemical Society, Vol. 142, Issue 7 https://doi.org/10.1149/1.2044271	journal	July 1995
Occlusion and Ion Exchange of Eutectic LiCl-KCl in H-Y Zeolite Bagri, Prashant; Simpson, Michael F. Journal of Nuclear Fuel Cycle and Waste Technology, Vol. 13, Issue Special https://doi.org/10.7733/jnfcwt.2015.13.S.45	journal	November 2015

Similar Records

Waste form evaluation for RECl₃ and REO_x fission products separated from used electrochemical salt

Journal Article · Fri Sep 22 00:00:00 EDT 2017 · Progress in Nuclear Energy · OSTI ID:1638741

Riley, Brian J.; Pierce, David A.; Crum, Jarrod V.; +3 more

Management of Alkali and Alkaline Earth Fission Products in Used Pyroprocessing Salt

Technical Report · Sat Sep 09 00:00:00 EDT 2023 · OSTI ID:1638741

Rose, M. A.; Thomas, S.

Liquidus temperature and chemical durability of selected glasses to immobilize rare earth oxides waste

Journal Article · Tue Jun 30 00:00:00 EDT 2015 · Journal of Nuclear Materials, 465:657-663 · OSTI ID:1638741

Mohd Fadzil, Syazwani Binti; Hrma, Pavel R.; Schweiger, Michael J.; +1 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
electrochemical
pyroprocessing
wasteform
separations technologies
mixtures
salts
wastes
amorphous materials
halogens

Title: Electrochemical Salt Wasteform Development: A Review of Salt Treatment and Immobilization Options

Citation Formats

References (48)

Similar Records

Related Subjects