Optimizing radionuclide sequestration in anion nanotraps with record pertechnetate sorption
Abstract
The elimination of specific contaminants from high concentrations of competitors poses a significant challenge. Rather than relying on a single direct interaction, the cooperation of multiple functionalities is an emerging strategy for adsorptive materials design to achieve this requisite affinity. Here, we describe that the interaction with the analyte of interest can be altered by modifying the local environment of the direct contact site, as demonstrated by manipulating the affinity of pyridinium-based anion nanotraps toward pertechnetate. Systematic control of the substituent effect allows the resulting anion nanotraps to combine multiple features as ideal pertechnetate scavengers with exceptional performances, substantially overcoming the long-term challenge of TcO4- segregation under extreme conditions of super acidity and basicity, strong irradiation field, and high ionic strength. The top material exhibits the highest sorption capacity together with unprecedented extraction efficiencies after a single treatment from conditions relevant to the used nuclear fuel (Hanford tank wastes, 95%) and legacy nuclear wastes (Savannah River Sites, 80%) among materials reported thus far.
- Authors:
-
[1];
[1];
[1]
- Univ. of South Florida, Tampa, FL (United States)
- Soochow University, Suzhou (China); Southwest University of Science and Technology, Mianyang, Sichuan (China)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Tsinghua University, Beijing (China)
- Soochow University, Suzhou (China)
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE; National Science Foundation (NSF); Univ. of South Florida, Tampa, FL (United States)
- OSTI Identifier:
- 1510295
- Report Number(s):
- PNNL-SA-141179
Journal ID: ISSN 2041-1723
- Grant/Contract Number:
- AC05-76RL01830; CBET-1706025
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Sun, Qi, Zhu, Lin, Aguila, Briana, Thallapally, Praveen K., Xu, Chao, Chen, Jing, Wang, Shuao, Rogers, David, and Ma, Shengqian. Optimizing radionuclide sequestration in anion nanotraps with record pertechnetate sorption. United States: N. p., 2019.
Web. doi:10.1038/s41467-019-09630-y.
Sun, Qi, Zhu, Lin, Aguila, Briana, Thallapally, Praveen K., Xu, Chao, Chen, Jing, Wang, Shuao, Rogers, David, & Ma, Shengqian. Optimizing radionuclide sequestration in anion nanotraps with record pertechnetate sorption. United States. https://doi.org/10.1038/s41467-019-09630-y
Sun, Qi, Zhu, Lin, Aguila, Briana, Thallapally, Praveen K., Xu, Chao, Chen, Jing, Wang, Shuao, Rogers, David, and Ma, Shengqian. Tue .
"Optimizing radionuclide sequestration in anion nanotraps with record pertechnetate sorption". United States. https://doi.org/10.1038/s41467-019-09630-y. https://www.osti.gov/servlets/purl/1510295.
@article{osti_1510295,
title = {Optimizing radionuclide sequestration in anion nanotraps with record pertechnetate sorption},
author = {Sun, Qi and Zhu, Lin and Aguila, Briana and Thallapally, Praveen K. and Xu, Chao and Chen, Jing and Wang, Shuao and Rogers, David and Ma, Shengqian},
abstractNote = {The elimination of specific contaminants from high concentrations of competitors poses a significant challenge. Rather than relying on a single direct interaction, the cooperation of multiple functionalities is an emerging strategy for adsorptive materials design to achieve this requisite affinity. Here, we describe that the interaction with the analyte of interest can be altered by modifying the local environment of the direct contact site, as demonstrated by manipulating the affinity of pyridinium-based anion nanotraps toward pertechnetate. Systematic control of the substituent effect allows the resulting anion nanotraps to combine multiple features as ideal pertechnetate scavengers with exceptional performances, substantially overcoming the long-term challenge of TcO4- segregation under extreme conditions of super acidity and basicity, strong irradiation field, and high ionic strength. The top material exhibits the highest sorption capacity together with unprecedented extraction efficiencies after a single treatment from conditions relevant to the used nuclear fuel (Hanford tank wastes, 95%) and legacy nuclear wastes (Savannah River Sites, 80%) among materials reported thus far.},
doi = {10.1038/s41467-019-09630-y},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {Tue Apr 09 00:00:00 EDT 2019},
month = {Tue Apr 09 00:00:00 EDT 2019}
}
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Figures / Tables:
Fig. 1: Anion nanotraps for TcO4− removal. Illustration of optimizing pyridinium based anion nanotraps for TcO4− recognition inspired by supramolecular technology
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99TcO4− remediation by a cationic polymeric network
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Emerging opportunities for nanotechnology to enhance water security
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Gas storage in porous aromatic frameworks (PAFs)
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