The simultaneous removal of technetium and iodine from Hanford tank waste

Asmussen, Robert Matthew; Westesen, Amy M.; Alvarez, Christian; Peterson, Reid A.; Cordova, Elsa; Cho, Herman; Branch, Shirmir D.; Walter, Eric D.; Hall, Gabriel B.; Orgnic, Andrew L.; Carney, Andrew M.

doi:10.1016/j.cej.2024.151449

Title: The simultaneous removal of technetium and iodine from Hanford tank waste

Journal Article · 22 April 2024 · Chemical Engineering Journal

DOI: https://doi.org/10.1016/j.cej.2024.151449 · OSTI ID:2458236

^[1];

^[1]; Alvarez, Christian ^[1];

^[1];

^[1]; Branch, Shirmir D. ^[1];

^[1];

^[1]; Orgnic, Andrew L. ^[1]; Carney, Andrew M. ^[1]

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

The simultaneous removal of radionuclides technetium-99 and iodine-129 from an actual decontaminated Hanford tank waste sample (a mixture of decontaminated waste from tanks 241-AP-105 and 241-AP-107) was demonstrated for the first time in this work. A series of commercially available ion exchange resins were evaluated in batch contact tests in the tank waste, and all showed removal of both Tc and I. The highest Tc removal was observed for Purolite A530e while the highest iodine removal was observed for ResinTech SIR-110-MP. Batch tests in simulated tank waste with these two resins showed that the SIR-110-HP-MP had consistently higher K_d for both pertechnetate and iodide and much higher K_d than previous works on Tc removal from Hanford waste. As such, the SIR-110-MP was evaluated in a dual -column (lead/lag) test processing 5.2L of the tank waste mixture showing 60% breakthrough of Tc on the lead column and no significant breakthrough on the lag after 625 bed volumes (BV, 6 mL size) while significant iodine breakthrough (>50%) occurred after 28 BV. The limited iodine uptake was attributed to the column conditions generating mass transfer limitations. A fraction of the Tc and I was not captured by the resin (<10%) in either the batch tests or column tests. The iodine fraction was identified to be an iodide, likely organo-iodide. The fraction of the Tc was identified as a non-pertechnetate species, which is the first time non-pertechnetate has been identified in AP-105 and AP-107 tanks, although the exact species is still unknown.

View Accepted Manuscript (DOE)

Cite

Export

Save

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

Sponsoring Organization:: USDOE Office of Environmental Management (EM); USDOE Office of Environmental Management (EM), Technology Development

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2458236

Report Number(s):: PNNL-SA-189635

Journal Information:: Chemical Engineering Journal, Journal Name: Chemical Engineering Journal Vol. 490; ISSN 1385-8947

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (66)

A history of Hanford tank waste, implications for waste treatment, and disposal Colburn, Heather A.; Peterson, Reid A. Environmental Progress & Sustainable Energy, Vol. 40, Issue 1 https://doi.org/10.1002/ep.13567	journal	December 2020
Behavior of technetium in nuclear waste vitrification processes Pegg, Ian L. Journal of Radioanalytical and Nuclear Chemistry, Vol. 305, Issue 1 https://doi.org/10.1007/s10967-014-3900-9	journal	January 2015
Evaluation of iodine speciation and 129I/127I ratios at low concentrations in environmental samples using IC-ICP-MS Kimmig, Sara R.; Thompson, Christopher; Baum, Steven Journal of Radioanalytical and Nuclear Chemistry, Vol. 327, Issue 2 https://doi.org/10.1007/s10967-020-07537-3	journal	January 2021
Efficient removal of iodide/iodate from aqueous solutions by Purolite A530E resin Zhao, Yuting; Li, Jie; Chen, Long Journal of Radioanalytical and Nuclear Chemistry, Vol. 332, Issue 4 https://doi.org/10.1007/s10967-023-08786-8	journal	January 2023
99Tc NMR Spectroscopy Mikhalev, V. A. Radiochemistry, Vol. 47, Issue 4 https://doi.org/10.1007/s11137-005-0097-3	journal	July 2005
The removal of the pertechnetate ion and actinides from radioactive waste streams at Hanford, Washington, USA and Sellafield, Cumbria, UK: the role of iron-sulfide-containing adsorbent materials Watson, J. H. P.; Ellwood, D. C. Nuclear Engineering and Design, Vol. 226, Issue 3 https://doi.org/10.1016/S0029-5493(03)00194-8	journal	December 2003
Surface functionalized nanofibers for the removal of chromium(VI) from aqueous solutions Avila, M.; Burks, T.; Akhtar, F. Chemical Engineering Journal, Vol. 245 https://doi.org/10.1016/j.cej.2014.02.034	journal	June 2014
Analysis of technetium immobilization and its molecular retention mechanisms by Fe(II)-Al(III)-Cl layered double hydroxide Mayordomo, Natalia; Rodríguez, Diana M.; Rossberg, André Chemical Engineering Journal, Vol. 408 https://doi.org/10.1016/j.cej.2020.127265	journal	March 2021
Technetium-99 decontamination from radioactive wastewater by modified bentonite: batch, column experiment and mechanism investigation Yang, Junqiang; Shi, Keliang; Wu, Fei Chemical Engineering Journal, Vol. 428 https://doi.org/10.1016/j.cej.2021.131333	journal	January 2022
Highly selective removal of Technetium-99 using imidazolium-based macroporous anion exchange resins Hu, Tingwei; Hao, Wenfeng; Zou, Haifeng Chemical Engineering Journal, Vol. 465 https://doi.org/10.1016/j.cej.2023.142951	journal	June 2023
Reductive immobilization of pertechnetate in soil and groundwater using synthetic pyrite nanoparticles Huo, Lijuan; Xie, Wenbo; Qian, Tianwei Chemosphere, Vol. 174 https://doi.org/10.1016/j.chemosphere.2017.02.018	journal	May 2017
Effects of hydrated lime on radionuclides stabilization of Hanford tank residual waste Wang, Guohui; Um, Wooyong; Cantrell, Kirk J. Chemosphere, Vol. 185 https://doi.org/10.1016/j.chemosphere.2017.06.103	journal	October 2017
Decontamination of radioactive wastewater: State of the art and challenges forward Zhang, Xiaoyuan; Gu, Ping; Liu, Yu Chemosphere, Vol. 215 https://doi.org/10.1016/j.chemosphere.2018.10.029	journal	January 2019
Review of intermediate-scale field tests in support of disposal of waste forms Neeway, James J.; Emerson, Hilary P.; Asmussen, R. Matthew Chemosphere, Vol. 347 https://doi.org/10.1016/j.chemosphere.2023.140625	journal	January 2024
Risk to ecological resources following remediation can be due mainly to increased resource value of successful restoration: A case study from the Department of Energy's Hanford Site Burger, Joanna; Gochfeld, Michael; Kosson, David S. Environmental Research, Vol. 186 https://doi.org/10.1016/j.envres.2020.109536	journal	July 2020
Effects of speciation on partitioning of iodine in aqueous biphasic systems and onto ABEC® resins Griffin, S.; Spear, S.; Rogers, R. Journal of Chromatography B, Vol. 807, Issue 1 https://doi.org/10.1016/j.jchromb.2004.01.051	journal	July 2004
Characterization of spent Purolite A530E resin with implications for long-term radioactive contaminant removal Levitskaia, Tatiana G.; Campbell, Emily L.; Hall, Gabriel B. Journal of Environmental Chemical Engineering, Vol. 8, Issue 5 https://doi.org/10.1016/j.jece.2020.104155	journal	October 2020
Radioiodine sorption/desorption and speciation transformation by subsurface sediments from the Hanford Site Xu, Chen; Kaplan, Daniel I.; Zhang, Saijin Journal of Environmental Radioactivity, Vol. 139 https://doi.org/10.1016/j.jenvrad.2014.09.012	journal	January 2015
Bioregeneration of perchlorate-laden gel-type anion-exchange resin in a fluidized bed reactor Venkatesan, Arjun K.; Sharbatmaleki, Mohamadali; Batista, Jacimaria R. Journal of Hazardous Materials, Vol. 177, Issue 1-3 https://doi.org/10.1016/j.jhazmat.2009.12.092	journal	May 2010
Getters for improved technetium containment in cementitious waste forms Asmussen, R. Matthew; Pearce, Carolyn I.; Miller, Brian W. Journal of Hazardous Materials, Vol. 341 https://doi.org/10.1016/j.jhazmat.2017.07.055	journal	January 2018
Impact of oxidation and carbonation on the release rates of iodine, selenium, technetium, and nitrogen from a cementitious waste form Chen, Zhiliang; Zhang, Peng; Brown, Kevin G. Journal of Hazardous Materials, Vol. 449 https://doi.org/10.1016/j.jhazmat.2023.131004	journal	May 2023
Accumulation mechanisms for contaminants on weak-base hybrid ion exchange resins Saslow, Sarah A.; Cordova, Elsa A.; Escobedo, Nancy M. Journal of Hazardous Materials, Vol. 459 https://doi.org/10.1016/j.jhazmat.2023.132165	journal	October 2023
Volatile species of technetium and rhenium during waste vitrification Kim, Dongsang; Kruger, Albert A. Journal of Non-Crystalline Solids, Vol. 481 https://doi.org/10.1016/j.jnoncrysol.2017.10.013	journal	February 2018
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
The function of Sn(II)-apatite as a Tc immobilizing agent Asmussen, R. Matthew; Neeway, James J.; Lawter, Amanda R. Journal of Nuclear Materials, Vol. 480 https://doi.org/10.1016/j.jnucmat.2016.09.002	journal	November 2016
A short history of waste management at the Hanford Site Gephart, Roy E. Physics and Chemistry of the Earth, Parts A/B/C, Vol. 35, Issue 6-8 https://doi.org/10.1016/j.pce.2010.03.032	journal	January 2010
Iodine immobilization by materials through sorption and redox-driven processes: A literature review Moore, Robert C.; Pearce, Carolyn I.; Morad, Joseph W. Science of The Total Environment, Vol. 716 https://doi.org/10.1016/j.scitotenv.2019.06.166	journal	May 2020
Removing nitrate from water using iron-modified Dowex 21K XLT ion exchange resin: Batch and fluidised-bed adsorption studies Kalaruban, Mahatheva; Loganathan, Paripurnanda; Shim, W. G. Separation and Purification Technology, Vol. 158 https://doi.org/10.1016/j.seppur.2015.12.022	journal	January 2016
Identification and Quantification of Technetium Species in Hanford Waste Tank AN-102 Chatterjee, Sayandev; Holfeltz, Vanessa E.; Hall, Gabriel B. Analytical Chemistry, Vol. 92, Issue 20 https://doi.org/10.1021/acs.analchem.0c02864	journal	September 2020
Removal of TcO ₄ ^– from Representative Nuclear Waste Streams with Layered Potassium Metal Sulfide Materials Neeway, James J.; Asmussen, R. Matthew; Lawter, Amanda R. Chemistry of Materials, Vol. 28, Issue 11 https://doi.org/10.1021/acs.chemmater.6b01296	journal	May 2016
Reduction and Simultaneous Removal of ⁹⁹ Tc and Cr by Fe(OH) ₂ (s) Mineral Transformation Saslow, Sarah A.; Um, Wooyong; Pearce, Carolyn I. Environmental Science & Technology, Vol. 51, Issue 15 https://doi.org/10.1021/acs.est.7b02278	journal	July 2017
Review of the Scientific Understanding of Radioactive Waste at the U.S. DOE Hanford Site Peterson, Reid A.; Buck, Edgar C.; Chun, Jaehun Environmental Science & Technology, Vol. 52, Issue 2 https://doi.org/10.1021/acs.est.7b04077	journal	January 2018
Iodine Removal from Carbonate-Containing Alkaline Liquids Using Strong Base Resins, Hybrid Resins, and Silver Precipitation Asmussen, R. Matthew; Westesen, Amy; Cordova, Elsa A. Industrial & Engineering Chemistry Research, Vol. 62, Issue 7 https://doi.org/10.1021/acs.iecr.2c03527	journal	February 2023
Hybrid Sorbents for ¹²⁹ I Capture from Contaminated Groundwater Cordova, Elsa A.; Garayburu-Caruso, Vanessa; Pearce, Carolyn I. ACS Applied Materials & Interfaces, Vol. 12, Issue 23 https://doi.org/10.1021/acsami.0c01527	journal	May 2020
Task-Specific Tailored Cationic Polymeric Network with High Base-Resistance for Unprecedented ⁹⁹TcO₄^– Cleanup from Alkaline Nuclear Waste Li, Jie; Li, Baoyu; Shen, Nannan ACS Central Science, Vol. 7, Issue 8 https://doi.org/10.1021/acscentsci.1c00847	journal	August 2021
Removal of Pertechnetate from Simulated Nuclear Waste Streams Using Supported Zerovalent Iron Darab, John G.; Amonette, Alexandra B.; Burke, Deborah S. D. Chemistry of Materials, Vol. 19, Issue 23 https://doi.org/10.1021/cm0607379	journal	November 2007
Identification of the Non-Pertechnetate Species in Hanford Waste Tanks, Tc(I)−Carbonyl Complexes Lukens, Wayne W.; Shuh, David K.; Schroeder, Norman C. Environmental Science & Technology, Vol. 38, Issue 1 https://doi.org/10.1021/es034318d	journal	January 2004
Anion Exchange Resins for the Selective Separation of Technetium from Uranium in Carbonate Solutions Long, Kristy M.; Goff, George S.; Ware, Stuart D. Industrial & Engineering Chemistry Research, Vol. 51, Issue 31 https://doi.org/10.1021/ie300534e	journal	July 2012
Design, Synthesis, and Uptake Performance of ABEC Resins for the Removal of Pertechnetate from Alkaline Radioactive Wastes Bond, Andrew H.; Chang, Frank W. K.; Thakkar, Anil H. Industrial & Engineering Chemistry Research, Vol. 38, Issue 4 https://doi.org/10.1021/ie980072n	journal	April 1999
Temperature and Isotope Substitution Effects on the Structure and NMR Properties of the Pertechnetate Ion in Water Cho, Herman; de Jong, Wibe A.; McNamara, Bruce K. Journal of the American Chemical Society, Vol. 126, Issue 37 https://doi.org/10.1021/ja047447i	journal	September 2004
Removal of TcO ₄ ⁻ ions from solution: materials and future outlook Banerjee, Debasis; Kim, Dongsang; Schweiger, Michael J. Chemical Society Reviews, Vol. 45, Issue 10 https://doi.org/10.1039/C5CS00330J	journal	January 2016
Removal of hexavalent chromium by anion exchange: non-target anion behavior and practical implications Flint, Leah C.; Arias-Paić, Miguel S.; Korak, Julie A. Environmental Science: Water Research & Technology, Vol. 7, Issue 12 https://doi.org/10.1039/D1EW00382H	journal	January 2021
Characterization of SuperLig ^® 639 Rhenium and Technetium Resin with Batch Contact and Column Tests Nash, Charles; Musall, Benjamin; Morse, Megan Separation Science and Technology, Vol. 50, Issue 18 https://doi.org/10.1080/01496395.2015.1085410	journal	December 2015
Tc removal from the waste treatment and immobilization plant low-activity waste vitrification off-gas recycle Taylor-Pashow, Kathryn M. L.; McCabe, Daniel J.; Nash, Charles A. Separation Science and Technology, Vol. 53, Issue 12 https://doi.org/10.1080/01496395.2017.1302952	journal	May 2017
Impact of feed variability on cesium removal with multiple actual waste samples from the Hanford site Westesen, A. M.; Campbell, E. L.; Fiskum, S. K. Separation Science and Technology, Vol. 57, Issue 15 https://doi.org/10.1080/01496395.2022.2059378	journal	March 2022
Extraction of Technetium From Simulated Hanford Tank Wastes Chaiko, D. J.; Vojta, Y.; Takeuchi, M. Separation Science and Technology, Vol. 30, Issue 7-9 https://doi.org/10.1080/01496399508010336	journal	April 1995
Review: Waste-Pretreatment Technologies for Remediation of Legacy Defense Nuclear Wastes Wilmarth, William R.; Lumetta, Gregg J.; Johnson, Michael E. Solvent Extraction and Ion Exchange, Vol. 29, Issue 1 https://doi.org/10.1080/07366299.2011.539134	journal	January 2011
Aqueous Biphasic Extraction Chromatography (Abec™): Uptake of Pertechnetate from Simulated Hanford tank Wastes Rogers, Robin D.; Griffin, Scott T.; Philip Horwitz, E. Solvent Extraction and Ion Exchange, Vol. 15, Issue 4 https://doi.org/10.1080/07366299708934493	journal	July 1997
Superlig® 639 Equilibrium Sorption data for Technetium from Hanford tank Waste Supernates Hassan, N. M.; King, W. D.; McCabe, D. J. Solvent Extraction and Ion Exchange, Vol. 20, Issue 2 https://doi.org/10.1081/SEI-120003022	journal	April 2002
Multiple Ion Exchange Column Tests for Technetium Removal from Hanford Site Tank 241‐AW‐101 with Superlig^®639 Resin Hassan, Neguib M.; Adu‐Wusu, Kofi; Nash, Charles A. Solvent Extraction and Ion Exchange, Vol. 22, Issue 4 https://doi.org/10.1081/SEI-120039636	journal	December 2004
Technetium Removal from Hanford and Savannah River Site Actual Tank Waste Supernates with Superlig ^® 639 Resin King, William D.; Hassan, Neguib M.; McCabe, Daniel J. Separation Science and Technology, Vol. 38, Issue 12-13 https://doi.org/10.1081/SS-120022588	journal	January 2003
Removal of Technetium from Hanford Tank Waste Supernates Burgeson, I. E.; Deschane, J. R.; Blanchard, D. L. Separation Science and Technology, Vol. 40, Issue 1-3 https://doi.org/10.1081/SS-200041916	journal	January 2005
Column Performance Testing of SuperLig^® 639 Resin with Simulated Hanford Waste Supernates: Identification of the Primary Sorbing Species and Detailed Characterization of Their Desorption Profiles King, William D.; Spencer, William A.; Hamm, L. Larry Separation Science and Technology, Vol. 40, Issue 1-3 https://doi.org/10.1081/SS-200042472	journal	February 2005
From legacy contamination to watershed systems science: a review of scientific insights and technologies developed through DOE-supported research in water and energy security Dwivedi, Dipankar; Steefel, Carl I.; Arora, Bhavna Environmental Research Letters, Vol. 17, Issue 4 https://doi.org/10.1088/1748-9326/ac59a9	journal	March 2022
An Integrated Framework for Evaluating Leaching in Waste Management and Utilization of Secondary Materials Kosson, D. S.; van der Sloot, H. A.; Sanchez, F. Environmental Engineering Science, Vol. 19, Issue 3 https://doi.org/10.1089/109287502760079188	journal	May 2002
NMR nomenclature. Nuclear spin properties and conventions for chemical shifts(IUPAC Recommendations 2001) Harris, Robin K.; Becker, Edwin D.; Cabral de Menezes, Sonia M. Pure and Applied Chemistry, Vol. 73, Issue 11 https://doi.org/10.1351/pac200173111795	journal	January 2001
Silver-based getters for 129I removal from low-activity waste Asmussen, R. Matthew; Neeway, James J.; Lawter, Amanda R. Radiochimica Acta, Vol. 104, Issue 12 https://doi.org/10.1515/ract-2016-2598	journal	January 2016
Marine Sediment Toxicity Identification Evaluation Methods for the Anionic Metals Arsenic and Chromium Burgess, Robert M.; Perron, Monique M.; Cantwell, Mark G. Environmental Toxicology and Chemistry, Vol. 26, Issue 1 https://doi.org/10.1897/06-014R.1	journal	January 2007
Distributions of 14 elements on 63 absorbers from three simulant solutions (acid-dissolved sludge, acidified supernate, and alkaline supernate) for Hanford HLW Tank 102-SY Marsh, S. F.; Svitra, Z. V.; Bowen, S. M. https://doi.org/10.2172/10177119	report	August 1994
Evaluation of Ammonium and Iodine Decontamination Factors for Hanford's Waste Treatment and Immobilization Plant Feed in the Effluent Treatment Facility Siegfried, Matthew; McCabe, Daniel; Stone, Michael https://doi.org/10.2172/1804665	report	June 2021
Follow-on Report of Analysis of Approaches to Supplemental Treatment of Low-Activity Waste at the Hanford Nuclear Reservation (Supporting Information Vol. II) Bates, William F. https://doi.org/10.2172/1863801	report	April 2022
Measurement of Iodine, Iodide, and Iodate in Hanford Tank Waste: Technology Transfer from PNNL to Hanford 222-S Laboratory Soderquist, Chuck; Branch, Shirmir; Gartman, Brandy https://doi.org/10.2172/1963872	report	September 2021
Technetium in alkaline, high-salt, radioactive tank waste supernate: Preliminary characterization and removal Blanchard, D. L. Jr.; Brown, G. N.; Conradson, S. D. https://doi.org/10.2172/475671 PNNL--11386	report	January 1997
Electrochemical reduction removal of technetium-99 from Hanford tank wastes Lawrence, W. E.; Blanchard, Jr., D. L.; Kurath, D. E. https://doi.org/10.2172/567517	report	September 1997
Removal of technetium from alkaline nuclear-waste media by a solvent-extraction process using crown ethers Bonnesen, P. V.; Presley, D. J.; Haverlock, T. J. https://doi.org/10.2172/86950	report	July 1995
Review of recent developments in iodine wasteform production Asmussen, R. Matthew; Turner, Joshua; Chong, Saehwa Frontiers in Chemistry, Vol. 10 https://doi.org/10.3389/fchem.2022.1043653	journal	December 2022

Similar Records

Cesium Ion Exchange Testing Using Crystalline Silicotitanate with Hanford Tank Waste 241-AP-107

Technical Report · 2021 · OSTI ID:1814008

Westesen, Amy M.; Fiskum, Sandra K.; Colburn, Heather A.; +3 more

Ion Exchange Processing of AW-105 Hanford Tank Waste through Crystalline Silicotitanate in a Staged 2- then 3-Column System

Technical Report · 2025 · OSTI ID:2998070

Westesen, Amy M.; Bachman, Austin A.; Carney, Andrew M.; +3 more

Cesium Ion Exchange Testing Using a Three-Column System with Crystalline Silicotitanate and Hanford Tank Waste 241-AP-107

Technical Report · 2019 · OSTI ID:1645027

Fiskum, Sandra K.; Rovira, Amy M.; Colburn, Heather A.; +2 more

Related Subjects

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES
129-I removal
Hanford waste
Radioioddine
Technetium
ion exchange
nuclear waste
tank waste
technetium removal

Title: The simultaneous removal of technetium and iodine from Hanford tank waste

Citation Formats

References (66)

Similar Records

Related Subjects