Hybrid Sorbents for 129I Capture from Contaminated Groundwater

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

doi:10.1021/acsami.0c01527

Hybrid Sorbents for ¹²⁹I Capture from Contaminated Groundwater

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

Emerging and Solid-State Batteries

Research output: Contribution to journal › Article › peer-review

33 Scopus citations

Abstract

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. 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.

Original language	English
Pages (from-to)	26113-26126
Number of pages	14
Journal	ACS Applied Materials and Interfaces
Volume	12
Issue number	23
DOIs	https://doi.org/10.1021/acsami.0c01527
State	Published - Jun 10 2020

Funding

This document was prepared under the Deep Vadose Zone–Applied Field Research Initiative at Pacific Northwest National Laboratory. The authors express thanks to Dr. Christian Herbert from Dralon for providing the samples of PAN fibers. SEM measurements were performed in the Environmental Molecular Science Laboratory, a national user facility supported by the DOE Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. Use of the Advanced Photon Source, an Office of Science User Facility operated by Argonne National Laboratory, was supported by the U.S. DOE under Contract No. DE-AC02-06CH11357. The authors acknowledge Steven Baum and Ian Leavy for ICP-MS measurements. The authors greatly appreciate the technical review provided by Mike Truex and Chris Johnson and technical editing provided by Matt Wilburn. The Pacific Northwest National Laboratory is operated by Battelle Memorial Institute for the DOE under Contract DE-AC05-76RL01830. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-NA0003525. This technology is patent pending.

Keywords

bismuth oxyhydroxide
cerium oxide/oxyhydroxide
ferrihydrite
groundwater remediation
ion-exchange resins
polyacrylonitrile beads
radioiodine
silica substrates

Access to Document

10.1021/acsami.0c01527

Cite this

Cordova, E. A., Garayburu-Caruso, V., Pearce, C. I., Cantrell, K. J., Morad, J. W., Gillispie, E. C., Riley, B. J., Colon, F. C., Levitskaia, T. G., Saslow, S. A., Qafoku, O., Resch, C. T., Rigali, M. J., Szecsody, J. E., Heald, S. M., Balasubramanian, M., Meyers, P., & Freedman, V. L. (2020). Hybrid Sorbents for ¹²⁹I Capture from Contaminated Groundwater. ACS Applied Materials and Interfaces, 12(23), 26113-26126. https://doi.org/10.1021/acsami.0c01527

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title = "Hybrid Sorbents for 129I Capture from Contaminated Groundwater",

abstract = "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. 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.",

keywords = "bismuth oxyhydroxide, cerium oxide/oxyhydroxide, ferrihydrite, groundwater remediation, ion-exchange resins, polyacrylonitrile beads, radioiodine, silica substrates",

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

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year = "2020",

month = jun,

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doi = "10.1021/acsami.0c01527",

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Cordova, EA, Garayburu-Caruso, V, Pearce, CI, Cantrell, KJ, Morad, JW, Gillispie, EC, Riley, BJ, Colon, FC, Levitskaia, TG, Saslow, SA, Qafoku, O, Resch, CT, Rigali, MJ, Szecsody, JE, Heald, SM, Balasubramanian, M, Meyers, P & Freedman, VL 2020, 'Hybrid Sorbents for ¹²⁹I Capture from Contaminated Groundwater', ACS Applied Materials and Interfaces, vol. 12, no. 23, pp. 26113-26126. https://doi.org/10.1021/acsami.0c01527

TY - JOUR

T1 - Hybrid Sorbents for 129I Capture from Contaminated Groundwater

AU - Cordova, Elsa A.

AU - Garayburu-Caruso, Vanessa

AU - Pearce, Carolyn I.

AU - Cantrell, Kirk J.

AU - Morad, Joseph W.

AU - Gillispie, Elizabeth C.

AU - Riley, Brian J.

AU - Colon, Ferdinan Cintron

AU - Levitskaia, Tatiana G.

AU - Saslow, Sarah A.

AU - Qafoku, Odeta

AU - Resch, Charles T.

AU - Rigali, Mark J.

AU - Szecsody, Jim E.

AU - Heald, Steve M.

AU - Balasubramanian, Mahalingam

AU - Meyers, Peter

AU - Freedman, Vicky L.

PY - 2020/6/10

Y1 - 2020/6/10

N2 - 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. 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.

AB - 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. 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.

KW - bismuth oxyhydroxide

KW - cerium oxide/oxyhydroxide

KW - ferrihydrite

KW - groundwater remediation

KW - ion-exchange resins

KW - polyacrylonitrile beads

KW - radioiodine

KW - silica substrates

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U2 - 10.1021/acsami.0c01527

DO - 10.1021/acsami.0c01527

M3 - Article

C2 - 32421326

AN - SCOPUS:85086346372

SN - 1944-8244

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EP - 26126

JO - ACS Applied Materials and Interfaces

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