skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: 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 TcO 4- 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];  [2]; ORCiD logo [1];  [3];  [4];  [4];  [5]; ORCiD logo [1]; ORCiD logo [1]
  1. Univ. of South Florida, Tampa, FL (United States)
  2. Soochow University, Suzhou (China); Southwest University of Science and Technology, Mianyang, Sichuan (China)
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  4. Tsinghua University, Beijing (China)
  5. Soochow University, Suzhou (China)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (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. doi: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. doi: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 = {2019},
month = {4}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Save / Share: