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Title: Evaluation of materials for iodine and technetium immobilization through sorption and redox-driven processes

Abstract

Radioactive iodine-129 (129I) and technetium-99 (99Tc) pose a risk to groundwater due to their long half-lives, toxicity, and high environmental mobility. Based on literature reviewed in Moore et al. (2019) and Pearce et al. (2019), natural and engineered materials, including iron oxides, low-solubility sulfides, tin-based materials, bismuth-based materials, organoclays, and metal organic frameworks, were tested for potential use as a deployed technology for the treatment of 129I and 99Tc to reduce environmental mobility. Materials were evaluated with metrics including capacity for IO3 and TcO4 uptake, selectivity and long-term immobilization potential. Batch testing was used to determine IO3 and TcO4 sorption under aerobic conditions for each material in synthetic groundwater at different solution to solid ratios. Material association with IO3 and TcO4 was spatially resolved using scanning electron microscopy and X-ray microprobe mapping. The potential for redox reactions was assessed using X-ray absorption near edge structure spectroscopy. Of the materials tested, we report bismuth oxy(hydroxide) and ferrihydrite performed the best for IO3. The commercial Purolite A530E anion-exchange resin outperformed all materials in its sorption capacity for TcO4. Tin-based materials had high capacity for TcO4, but immobilized TcO4 via reductive precipitation. Bismuth-based materials had high capacity for TcO4, though slightly lower thanmore » the tin-based materials, but did not immobilize TcO4 by a redox-drive process, mitigating potential negative re-oxidation effects over longer time periods under oxic conditions. Cationic metal organic frameworks and polymer networks had high Tc removal capacity, with TcO4 trapped within the framework of the sorbent material. Although organoclays did not have the highest capacity for IO3 and TcO4 removal in batch experiments, they are available commercially in large quantities, are relatively low cost and have low environmental impact, so were investigated in column experiments, demonstrating scale-up and removal of IO3 and TcO4 via sorption, and reductive immobilization with iron- and sulfur-based species.« less

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1];  [1];  [1];  [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [1];  [2];  [1];  [3];  [3];  [4];  [5];  [5] more »;  [6];  [1];  [1] « less
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  4. Soochow Univ., Suzhou (China)
  5. Lab. for Functional Inorganic Materials (EPFL), Sion (Switzerland)
  6. Monrovia, CA (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL); Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1638579
Alternate Identifier(s):
OSTI ID: 1632288
Report Number(s):
PNNL-SA-138462
Journal ID: ISSN 0048-9697
Grant/Contract Number:  
AC05-76RL01830; AC02-06CH11357; NA0003525
Resource Type:
Accepted Manuscript
Journal Name:
Science of the Total Environment
Additional Journal Information:
Journal Volume: 716; Journal Issue: C; Journal ID: ISSN 0048-9697
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; bismuth-based materials; iodate; iron oxides; layered double hydroxides; metal organic frameworks; pertechnetate

Citation Formats

Pearce, Carolyn I., Cordova, Elsa A., Garcia, Whitney L., Saslow, Sarah A., Cantrell, Kirk J., Morad, Joseph W., Qafoku, Odeta, Matyáš, Josef, Plymale, Andrew E., Chatterjee, Sayandev, Kang, Jaehyuk, Colon, Ferdinan Cintron, Levitskaia, Tatiana G., Rigali, Mark J., Szecsody, Jim E., Heald, Steve M., Balasubramanian, Mahalingam, Wang, Shuao, Sun, Daniel T., Queen, Wendy L., Bontchev, Ranko, Moore, Robert C., and Freedman, Vicky L.. Evaluation of materials for iodine and technetium immobilization through sorption and redox-driven processes. United States: N. p., 2019. Web. https://doi.org/10.1016/j.scitotenv.2019.136167.
Pearce, Carolyn I., Cordova, Elsa A., Garcia, Whitney L., Saslow, Sarah A., Cantrell, Kirk J., Morad, Joseph W., Qafoku, Odeta, Matyáš, Josef, Plymale, Andrew E., Chatterjee, Sayandev, Kang, Jaehyuk, Colon, Ferdinan Cintron, Levitskaia, Tatiana G., Rigali, Mark J., Szecsody, Jim E., Heald, Steve M., Balasubramanian, Mahalingam, Wang, Shuao, Sun, Daniel T., Queen, Wendy L., Bontchev, Ranko, Moore, Robert C., & Freedman, Vicky L.. Evaluation of materials for iodine and technetium immobilization through sorption and redox-driven processes. United States. https://doi.org/10.1016/j.scitotenv.2019.136167
Pearce, Carolyn I., Cordova, Elsa A., Garcia, Whitney L., Saslow, Sarah A., Cantrell, Kirk J., Morad, Joseph W., Qafoku, Odeta, Matyáš, Josef, Plymale, Andrew E., Chatterjee, Sayandev, Kang, Jaehyuk, Colon, Ferdinan Cintron, Levitskaia, Tatiana G., Rigali, Mark J., Szecsody, Jim E., Heald, Steve M., Balasubramanian, Mahalingam, Wang, Shuao, Sun, Daniel T., Queen, Wendy L., Bontchev, Ranko, Moore, Robert C., and Freedman, Vicky L.. Sun . "Evaluation of materials for iodine and technetium immobilization through sorption and redox-driven processes". United States. https://doi.org/10.1016/j.scitotenv.2019.136167. https://www.osti.gov/servlets/purl/1638579.
@article{osti_1638579,
title = {Evaluation of materials for iodine and technetium immobilization through sorption and redox-driven processes},
author = {Pearce, Carolyn I. and Cordova, Elsa A. and Garcia, Whitney L. and Saslow, Sarah A. and Cantrell, Kirk J. and Morad, Joseph W. and Qafoku, Odeta and Matyáš, Josef and Plymale, Andrew E. and Chatterjee, Sayandev and Kang, Jaehyuk and Colon, Ferdinan Cintron and Levitskaia, Tatiana G. and Rigali, Mark J. and Szecsody, Jim E. and Heald, Steve M. and Balasubramanian, Mahalingam and Wang, Shuao and Sun, Daniel T. and Queen, Wendy L. and Bontchev, Ranko and Moore, Robert C. and Freedman, Vicky L.},
abstractNote = {Radioactive iodine-129 (129I) and technetium-99 (99Tc) pose a risk to groundwater due to their long half-lives, toxicity, and high environmental mobility. Based on literature reviewed in Moore et al. (2019) and Pearce et al. (2019), natural and engineered materials, including iron oxides, low-solubility sulfides, tin-based materials, bismuth-based materials, organoclays, and metal organic frameworks, were tested for potential use as a deployed technology for the treatment of 129I and 99Tc to reduce environmental mobility. Materials were evaluated with metrics including capacity for IO3– and TcO4– uptake, selectivity and long-term immobilization potential. Batch testing was used to determine IO3– and TcO4– sorption under aerobic conditions for each material in synthetic groundwater at different solution to solid ratios. Material association with IO3– and TcO4– was spatially resolved using scanning electron microscopy and X-ray microprobe mapping. The potential for redox reactions was assessed using X-ray absorption near edge structure spectroscopy. Of the materials tested, we report bismuth oxy(hydroxide) and ferrihydrite performed the best for IO3–. The commercial Purolite A530E anion-exchange resin outperformed all materials in its sorption capacity for TcO4–. Tin-based materials had high capacity for TcO4–, but immobilized TcO4– via reductive precipitation. Bismuth-based materials had high capacity for TcO4–, though slightly lower than the tin-based materials, but did not immobilize TcO4– by a redox-drive process, mitigating potential negative re-oxidation effects over longer time periods under oxic conditions. Cationic metal organic frameworks and polymer networks had high Tc removal capacity, with TcO4– trapped within the framework of the sorbent material. Although organoclays did not have the highest capacity for IO3– and TcO4– removal in batch experiments, they are available commercially in large quantities, are relatively low cost and have low environmental impact, so were investigated in column experiments, demonstrating scale-up and removal of IO3– and TcO4– via sorption, and reductive immobilization with iron- and sulfur-based species.},
doi = {10.1016/j.scitotenv.2019.136167},
journal = {Science of the Total Environment},
number = C,
volume = 716,
place = {United States},
year = {2019},
month = {12}
}

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