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Title: Reduction and Simultaneous Removal of 99Tc and Cr by Fe(OH)2(s) Mineral Transformation

Abstract

Technetium (Tc) remains a priority remediation concern due to persistent challenges, including mobilization due to rapid reoxidation of immobilized Tc, and competing comingled contaminants, e.g., Cr(VI), that inhibit Tc(VII) reduction and incorporation into stable mineral phases. Here Fe(OH)2(s) is investigated as a comprehensive solution for overcoming these challenges, by serving as both the reductant, (Fe(II)), and the immobilization agent to form Tc-incorporated magnetite (Fe3O4). Trace metal analysis suggests removal of Tc(VII) and Cr(VI) from solution occurs simultaneously; however, complete removal and reduction of Cr(VI) is achieved earlier than the removal/reduction of comingled Tc(VII). Bulk oxidation state analysis of the final magnetite solid phase by XANES shows that the majority of Tc is Tc(IV), which is corroborated by XPS measurements. Furthermore, EXAFS results show successful, albeit partial, Tc(IV) incorporation into magnetite octahedral sites. Cr XPS analysis indicates reduction to Cr(III) and the formation of a Cr-incorporated spinel, Cr2O3, and Cr(OH)3 phases. Spinel (modeled as Fe3O4), goethite (α-FeOOH), and feroxyhyte (δ-FeOOH) are detected in all reacted final solid phase samples analyzed by XRD. Incorporation of Tc(IV) has little effect on the spinel lattice structure. Reaction of Fe(OH)2(s) in the presence of Cr(III) results in the formation of a spinel phase that ismore » a solid solution between magnetite (Fe3O4) and chromite (FeCr2O4).« less

Authors:
 [1]; ORCiD logo [1];  [1];  [1];  [1]; ORCiD logo [2];  [1]; ORCiD logo [1];  [1];  [1];  [3]
+ Show Author Affiliations
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  3. Dept. of Energy (DOE), Richland, WA (United States). Office of River Protection
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1482521
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Environmental Science and Technology
Additional Journal Information:
Journal Volume: 51; Journal Issue: 15; Journal ID: ISSN 0013-936X
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Saslow, Sarah A., Um, Wooyong, Pearce, Carolyn I., Engelhard, Mark H., Bowden, Mark E., Lukens, Wayne, Leavy, Ian I., Riley, Brian J., Kim, Dong-Sang, Schweiger, Michael J., and Kruger, Albert A. Reduction and Simultaneous Removal of 99Tc and Cr by Fe(OH)2(s) Mineral Transformation. United States: N. p., 2017. Web. doi:10.1021/acs.est.7b02278.
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Saslow, Sarah A., Um, Wooyong, Pearce, Carolyn I., Engelhard, Mark H., Bowden, Mark E., Lukens, Wayne, Leavy, Ian I., Riley, Brian J., Kim, Dong-Sang, Schweiger, Michael J., & Kruger, Albert A. Reduction and Simultaneous Removal of 99Tc and Cr by Fe(OH)2(s) Mineral Transformation. United States. https://doi.org/10.1021/acs.est.7b02278
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Saslow, Sarah A., Um, Wooyong, Pearce, Carolyn I., Engelhard, Mark H., Bowden, Mark E., Lukens, Wayne, Leavy, Ian I., Riley, Brian J., Kim, Dong-Sang, Schweiger, Michael J., and Kruger, Albert A. Tue . "Reduction and Simultaneous Removal of 99Tc and Cr by Fe(OH)2(s) Mineral Transformation". United States. https://doi.org/10.1021/acs.est.7b02278. https://www.osti.gov/servlets/purl/1482521.
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@article{osti_1482521,
title = {Reduction and Simultaneous Removal of 99Tc and Cr by Fe(OH)2(s) Mineral Transformation},
author = {Saslow, Sarah A. and Um, Wooyong and Pearce, Carolyn I. and Engelhard, Mark H. and Bowden, Mark E. and Lukens, Wayne and Leavy, Ian I. and Riley, Brian J. and Kim, Dong-Sang and Schweiger, Michael J. and Kruger, Albert A.},
abstractNote = {Technetium (Tc) remains a priority remediation concern due to persistent challenges, including mobilization due to rapid reoxidation of immobilized Tc, and competing comingled contaminants, e.g., Cr(VI), that inhibit Tc(VII) reduction and incorporation into stable mineral phases. Here Fe(OH)2(s) is investigated as a comprehensive solution for overcoming these challenges, by serving as both the reductant, (Fe(II)), and the immobilization agent to form Tc-incorporated magnetite (Fe3O4). Trace metal analysis suggests removal of Tc(VII) and Cr(VI) from solution occurs simultaneously; however, complete removal and reduction of Cr(VI) is achieved earlier than the removal/reduction of comingled Tc(VII). Bulk oxidation state analysis of the final magnetite solid phase by XANES shows that the majority of Tc is Tc(IV), which is corroborated by XPS measurements. Furthermore, EXAFS results show successful, albeit partial, Tc(IV) incorporation into magnetite octahedral sites. Cr XPS analysis indicates reduction to Cr(III) and the formation of a Cr-incorporated spinel, Cr2O3, and Cr(OH)3 phases. Spinel (modeled as Fe3O4), goethite (α-FeOOH), and feroxyhyte (δ-FeOOH) are detected in all reacted final solid phase samples analyzed by XRD. Incorporation of Tc(IV) has little effect on the spinel lattice structure. Reaction of Fe(OH)2(s) in the presence of Cr(III) results in the formation of a spinel phase that is a solid solution between magnetite (Fe3O4) and chromite (FeCr2O4).},
doi = {10.1021/acs.est.7b02278},
journal = {Environmental Science and Technology},
number = 15,
volume = 51,
place = {United States},
year = {Tue Jul 11 00:00:00 EDT 2017},
month = {Tue Jul 11 00:00:00 EDT 2017}
}
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https://doi.org/10.1021/acs.est.7b02278
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    Works referencing / citing this record:

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