Anion-exchanged and quaternary ammonium functionalized MIL-101-Cr metal-organic framework (MOF) for ReO4–/TcO4– sequestration from groundwater
Abstract
There are few effective technologies for the sequestration of highly water-soluble pertechnetate (TcO4–) from contaminated water despite the urgency of environmental and public health concerns. Here, anion exchanged and cetyltrimethylammonium bromide (CTAB) functionalized MIL-101-Cr-NO3 were investigated for perrhenate (ReO4–), a surrogate of TcO4–, sequestration from artificial groundwater. Cl–, I–, and CF3SO3– exchanged MIL-101-Cr proved more effective at ReO4– removal than the parent MIL-101-Cr-F. Compared to the parent framework, CTAB functionalized MIL-101-Cr-NO3 increased ReO4– removal capacity from 39 to 139 mg/g, improved the reaction kinetics from ~30 to <10 min to reach full adsorption capacity and the selectivity for ReO4– over competing NO3–, CO32–, SO42–, and Cl–. Spectroscopic data indicated that the chemical speciation of Re in the exchanged MIL-101-Cr remained ReO4–, indicating synergistic sequestration through both anion exchange and non-ion exchange binding with the positively charged ligand of CTAB. These studies foreshadow potential applications of MOFs for the remediation of 99TcO4– from contaminated environments.
- Authors:
-
- Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
- Univ. of South Carolina, Columbia, SC (United States)
- Savannah River Site (SRS), Aiken, SC (United States). Savannah River Ecology Lab. (SREL)
- Canadian Light Source, Saskatoon, SK (Canada)
- Publication Date:
- Research Org.:
- Savannah River Site (SRS), Aiken, SC (United States); Savannah River National Laboratory (SRNL), Aiken, SC (United States); Univ. of South Carolina, Columbia, SC (United States)
- Sponsoring Org.:
- USDOE Office of Environmental Management (EM); USDOE Laboratory Directed Research and Development (LDRD) Program; Univ. of Georgia Research Foundation; Natural Sciences and Engineering Research Council of Canada (NSERC); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1756606
- Alternate Identifier(s):
- OSTI ID: 1646539; OSTI ID: 1776555
- Report Number(s):
- SRNL-STI-2020-00352
Journal ID: ISSN 0265-931X; TRN: US2205652
- Grant/Contract Number:
- AC09-08SR22470; AC09-96SR18500; FC09-07-SR22506; SC0016574; LDRD-2018-00055
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Environmental Radioactivity
- Additional Journal Information:
- Journal Volume: 222; Journal ID: ISSN 0265-931X
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; pertechnetate; perrhenate; CTAB functionalization; MIL-101-Cr; sequestration
Citation Formats
Li, Dien, Shustova, Natalia B., Martin, Corey R., Taylor-Pashow, Kathryn, Seaman, John C., Kaplan, Daniel I., Amoroso, Jake W., and Chernikov, Roman. Anion-exchanged and quaternary ammonium functionalized MIL-101-Cr metal-organic framework (MOF) for ReO4–/TcO4– sequestration from groundwater. United States: N. p., 2020.
Web. doi:10.1016/j.jenvrad.2020.106372.
Li, Dien, Shustova, Natalia B., Martin, Corey R., Taylor-Pashow, Kathryn, Seaman, John C., Kaplan, Daniel I., Amoroso, Jake W., & Chernikov, Roman. Anion-exchanged and quaternary ammonium functionalized MIL-101-Cr metal-organic framework (MOF) for ReO4–/TcO4– sequestration from groundwater. United States. https://doi.org/10.1016/j.jenvrad.2020.106372
Li, Dien, Shustova, Natalia B., Martin, Corey R., Taylor-Pashow, Kathryn, Seaman, John C., Kaplan, Daniel I., Amoroso, Jake W., and Chernikov, Roman. Thu .
"Anion-exchanged and quaternary ammonium functionalized MIL-101-Cr metal-organic framework (MOF) for ReO4–/TcO4– sequestration from groundwater". United States. https://doi.org/10.1016/j.jenvrad.2020.106372. https://www.osti.gov/servlets/purl/1756606.
@article{osti_1756606,
title = {Anion-exchanged and quaternary ammonium functionalized MIL-101-Cr metal-organic framework (MOF) for ReO4–/TcO4– sequestration from groundwater},
author = {Li, Dien and Shustova, Natalia B. and Martin, Corey R. and Taylor-Pashow, Kathryn and Seaman, John C. and Kaplan, Daniel I. and Amoroso, Jake W. and Chernikov, Roman},
abstractNote = {There are few effective technologies for the sequestration of highly water-soluble pertechnetate (TcO4–) from contaminated water despite the urgency of environmental and public health concerns. Here, anion exchanged and cetyltrimethylammonium bromide (CTAB) functionalized MIL-101-Cr-NO3 were investigated for perrhenate (ReO4–), a surrogate of TcO4–, sequestration from artificial groundwater. Cl–, I–, and CF3SO3– exchanged MIL-101-Cr proved more effective at ReO4– removal than the parent MIL-101-Cr-F. Compared to the parent framework, CTAB functionalized MIL-101-Cr-NO3 increased ReO4– removal capacity from 39 to 139 mg/g, improved the reaction kinetics from ~30 to <10 min to reach full adsorption capacity and the selectivity for ReO4– over competing NO3–, CO32–, SO42–, and Cl–. Spectroscopic data indicated that the chemical speciation of Re in the exchanged MIL-101-Cr remained ReO4–, indicating synergistic sequestration through both anion exchange and non-ion exchange binding with the positively charged ligand of CTAB. These studies foreshadow potential applications of MOFs for the remediation of 99TcO4– from contaminated environments.},
doi = {10.1016/j.jenvrad.2020.106372},
journal = {Journal of Environmental Radioactivity},
number = ,
volume = 222,
place = {United States},
year = {Thu Aug 06 00:00:00 EDT 2020},
month = {Thu Aug 06 00:00:00 EDT 2020}
}
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