Hybrid Sorbents for 129I Capture from Contaminated Groundwater

Cordova, Elsa A.; Garayburu-Caruso, Vanessa; Pearce, Carolyn I.; Cantrell, Kirk J.; Morad, Joseph W.; Gillispie, Elizabeth C.; Riley, Brian J.; Colon, Ferdinan Cintron; Levitskaia, Tatiana G.; Saslow, Sarah A.; Qafoku, Odeta; Resch, Charles T.; Rigali, Mark J.; Szecsody, Jim E.; Heald, Steve M.; Balasubramanian, Mahalingam; Meyers, Peter; Freedman, Vicky L.

doi:10.1021/acsami.0c01527

Hybrid Sorbents for ¹²⁹I Capture from Contaminated Groundwater

Journal Article · Mon May 18 00:00:00 EDT 2020 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.0c01527· OSTI ID:1660393

^[1]; ^[1]; ^[1]; Cantrell, Kirk J. ^[1]; ^[1]; ^[1]; ^[1]; Colon, Ferdinan Cintron ^[1]; ^[1]; ^[1]; ^[1]; ^[1]; Rigali, Mark J. ^[2]; Szecsody, Jim E. ^[1]; ^[3]; ^[3]; Meyers, Peter ^[4]; Freedman, Vicky L. ^[1]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Resin Tech, West Berlin, NJ (United States)

Radioiodine (¹²⁹I) poses a risk to the environment due to its long half-life, toxicity, and mobility. It is found at the U.S. Department of Energy Hanford Site due to legacy releases of nuclear wastes to the subsurface where ¹²⁹I is predominantly present as iodate (IO₃^–). To date, a cost-effective and scalable cleanup technology for ¹²⁹I has not been identified, with hydraulic containment implemented as the remedial approach. Here, novel high-performing sorbents for ¹²⁹I remediation with the capacity to reduce ¹²⁹I concentrations to or below the US Environmental Protection Agency (EPA) drinking water standard and procedures to deploy them in an ex-situ pump and treat (P&T) system are introduced. Furthermore, this includes implementation of hybridized polyacrylonitrile (PAN) beads for ex-situ remediation of IO₃^–-contaminated groundwater for the first time. Iron (Fe) oxyhydroxide and bismuth (Bi) oxyhydroxide sorbents were deployed on silica substrates or encapsulated in porous PAN beads. In addition, Fe–, cerium (Ce)–, and Bi–oxyhydroxides were encapsulated with anion-exchange resins. The PAN–bismuth oxyhydroxide and PAN–ferrihydrite composites along with Fe- and Ce-based hybrid anion-exchange resins performed well in batch sorption experiments with distribution coefficients for IO₃^– of >1000 mL/g and rapid removal kinetics. Of the tested materials, the Ce-based hybrid anion-exchange resin was the most efficient for removal of IO₃^– from Hanford groundwater in a column system, with 50% breakthrough occurring at 324 pore volumes. The functional amine groups on the parent resin and amount of active sorbent in the resin can be customized to improve the iodine loading capacity. These results highlight the potential for IO₃^– remediation by hybrid sorbents and represent a benchmark for the implementation of commercially available materials to meet EPA standards for cleanup of ¹²⁹I in a large-scale P&T system.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Environmental Management (EM); USDOE Office of Science (SC), Office of Basic Energy Sciences (BES) Scientific User Facilities Division; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC02-06CH11357; AC05-76RL01830; NA0003525

OSTI ID:: 1660393

Alternate ID(s):: OSTI ID: 1638588
OSTI ID: 1778043

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 23 Vol. 12; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (26)

The geochemistry of iodine — a review Fuge, Ronald; Johnson, Christopher C. Environmental Geochemistry and Health, Vol. 8, Issue 2 https://doi.org/10.1007/BF02311063	journal	June 1986
Cesium removal from solution using PAN-based potassium nickel hexacyanoferrate (II) composite spheres Du, Zhihui; Jia, Mingchun; Wang, Xiaowei Journal of Radioanalytical and Nuclear Chemistry, Vol. 298, Issue 1 https://doi.org/10.1007/s10967-012-2396-4	journal	December 2012
Geochemical controls of iodine uptake and transport in Savannah River Site subsurface sediments Emerson, Hilary P.; Xu, Chen; Ho, Yi-Fang Applied Geochemistry, Vol. 45 https://doi.org/10.1016/j.apgeochem.2014.03.002	journal	June 2014
Is soil natural organic matter a sink or source for mobile radioiodine (129I) at the Savannah River Site? Xu, Chen; Zhang, Saijin; Ho, Yi-Fang Geochimica et Cosmochimica Acta, Vol. 75, Issue 19 https://doi.org/10.1016/j.gca.2011.07.011	journal	October 2011
Iodine dynamics in soils Shetaya, W. H.; Young, S. D.; Watts, M. J. Geochimica et Cosmochimica Acta, Vol. 77 https://doi.org/10.1016/j.gca.2011.10.034	journal	January 2012
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
Silica-based waste form for immobilization of iodine from reprocessing plant off-gas streams Matyáš, Josef; Canfield, Nathan; Sulaiman, Sannoh Journal of Nuclear Materials, Vol. 476 https://doi.org/10.1016/j.jnucmat.2016.04.047	journal	August 2016
Speciation of iodine isotopes inside and outside of a contaminant plume at the Savannah River Site Schwehr, Kathleen A.; Otosaka, Shigeyoshi; Merchel, Silke Science of The Total Environment, Vol. 497-498 https://doi.org/10.1016/j.scitotenv.2014.07.006	journal	November 2014
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
A review of the behavior of radioiodine in the subsurface at two DOE sites Neeway, James J.; Kaplan, Daniel I.; Bagwell, Christopher E. Science of The Total Environment, Vol. 691 https://doi.org/10.1016/j.scitotenv.2019.07.146	journal	November 2019
Evaluation of materials for iodine and technetium immobilization through sorption and redox-driven processes Pearce, Carolyn I.; Cordova, Elsa A.; Garcia, Whitney L. Science of The Total Environment, Vol. 716 https://doi.org/10.1016/j.scitotenv.2019.136167	journal	May 2020
Separation of Cerium from Rare Earths by Precipitation as Iodate from Homogeneous Solution Willard, H. H.; Yu, S. T. Analytical Chemistry, Vol. 25, Issue 11 https://doi.org/10.1021/ac60083a048	journal	November 1953
Evidence for Hydroxamate Siderophores and Other N-Containing Organic Compounds Controlling ^239,240 Pu Immobilization and Remobilization in a Wetland Sediment Xu, Chen; Zhang, Saijin; Kaplan, Daniel I. Environmental Science & Technology, Vol. 49, Issue 19 https://doi.org/10.1021/acs.est.5b02310	journal	September 2015
Novel Long-Term Immobilization Method for Radioactive Iodine-129 Using a Zeolite/Apatite Composite Sintered Body Watanabe, Yujiro; Ikoma, Toshiyuki; Yamada, Hirohisa ACS Applied Materials & Interfaces, Vol. 1, Issue 7 https://doi.org/10.1021/am900251m	journal	June 2009
Concentration-Dependent Mobility, Retardation, and Speciation of Iodine in Surface Sediment from the Savannah River Site Zhang, S.; Du, J.; Xu, C. Environmental Science & Technology, Vol. 45, Issue 13 https://doi.org/10.1021/es1040442	journal	July 2011
Iodine-129 and Iodine-127 Speciation in Groundwater at the Hanford Site, U.S.: Iodate Incorporation into Calcite Zhang, Saijin; Xu, Chen; Creeley, Danielle Environmental Science & Technology, Vol. 47, Issue 17 https://doi.org/10.1021/es401816e	journal	August 2013
Polyacrylonitrile-Chalcogel Hybrid Sorbents for Radioiodine Capture Riley, Brian J.; Pierce, David A.; Chun, Jaehun Environmental Science & Technology, Vol. 48, Issue 10 https://doi.org/10.1021/es405807w	journal	April 2014
Temporal Variation of Iodine Concentration and Speciation ( ¹²⁷ I and ¹²⁹ I) in Wetland Groundwater from the Savannah River Site, USA Zhang, Saijin; Ho, Yi-Fang; Creeley, Danielle Environmental Science & Technology, Vol. 48, Issue 19 https://doi.org/10.1021/es502003q	journal	September 2014
Organo-Iodine Formation in Soils and Aquifer Sediments at Ambient Concentrations Schwehr, K. A.; Santschi, P. H.; Kaplan, D. I. Environmental Science & Technology, Vol. 43, Issue 19 https://doi.org/10.1021/es900795k	journal	October 2009
Redox Transformations and Transport of Cesium and Iodine (−1, 0, +5) in Oxidizing and Reducing Zones of a Sand and Gravel Aquifer Fox, Patricia M.; Kent, Douglas B.; Davis, James A. Environmental Science & Technology, Vol. 44, Issue 6 https://doi.org/10.1021/es902865s	journal	March 2010
Capture of iodine and organic iodides using silica zeolites and the semiconductor behaviour of iodine in a silica zeolite Pham, Tung Cao Thanh; Docao, Son; Hwang, In Chul Energy & Environmental Science, Vol. 9, Issue 3 https://doi.org/10.1039/C5EE02843D	journal	January 2016
Granulous KMS-1/PAN composite for Cs ⁺ removal Wang, Yun-Xia; Li, Jian-Rong; Yang, Jia-Cheng E. RSC Advances, Vol. 5, Issue 111 https://doi.org/10.1039/C5RA16205J	journal	January 2015
Porous sorbents for the capture of radioactive iodine compounds: a review Huve, Joffrey; Ryzhikov, Andrey; Nouali, Habiba RSC Advances, Vol. 8, Issue 51 https://doi.org/10.1039/C8RA04775H	journal	January 2018
Multi-tests for pore structure characterization-A case study using lamprophyre Li, Zhen; Feng, Guorui; Luo, Yi AIP Advances, Vol. 7, Issue 8 https://doi.org/10.1063/1.4997749	journal	August 2017
Evaluation of PAN–TiO ₂ Composite Adsorbent for Removal of Pb(II) Ion in Aqueous Solution Kim, Hyung-Tae; Lee, Chang-Ha; Shul, Yong-Gun Separation Science and Technology, Vol. 38, Issue 3 https://doi.org/10.1081/SS-120016660	journal	January 2003
A Mass-Production Process of a Highly Pure Medical Use 99mTc from Natural Isotopic Mo(n, γ) 99Mo without Using Uranium Tatenuma, Katsuyoshi; Ishikawa, Koji; Tsuguchi, Akira RADIOISOTOPES, Vol. 63, Issue 11 https://doi.org/10.3769/radioisotopes.63.501	journal	January 2014

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
bismuth oxyhydroxide
cerium oxide/oxyhydroxide
ferrihydrite
groundwater remediation
ion-exchange resins
polyacrylonitrile beads
radioiodine
silica substrates

Hybrid Sorbents for 129I Capture from Contaminated Groundwater

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References (26)

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Hybrid Sorbents for ¹²⁹I Capture from Contaminated Groundwater