Optimizing radionuclide sequestration in anion nanotraps with record pertechnetate sorption

Sun, Qi; Zhu, Lin; Aguila, Briana; Thallapally, Praveen K.; Xu, Chao; Chen, Jing; Wang, Shuao; Rogers, David; Ma, Shengqian

doi:10.1038/s41467-019-09630-y

Title: Optimizing radionuclide sequestration in anion nanotraps with record pertechnetate sorption

Journal Article · 09 April 2019 · Nature Communications

DOI: https://doi.org/10.1038/s41467-019-09630-y · OSTI ID:1510295

Sun, Qi ^[1]; Zhu, Lin ^[2];

^[1]; Thallapally, Praveen K. ^[3]; Xu, Chao ^[4]; Chen, Jing ^[4]; Wang, Shuao ^[5];

^[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)

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.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE; National Science Foundation (NSF); Univ. of South Florida, Tampa, FL (United States)

Grant/Contract Number:: AC05-76RL01830; CBET-1706025

OSTI ID:: 1510295

Report Number(s):: PNNL-SA-141179

Journal Information:: Nature Communications, Vol. 10, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 124 works

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Alternative energy technologies Dresselhaus, M. S.; Thomas, I. L. Nature, Vol. 414, Issue 6861 https://doi.org/10.1038/35104599	journal	November 2001
Charge-specific size-dependent separation of water-soluble organic molecules by fluorinated nanoporous networks Byun, Jeehye; Patel, Hasmukh A.; Thirion, Damien Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms13377	journal	November 2016
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Gas storage in porous aromatic frameworks (PAFs) Ben, Teng; Pei, Cuiying; Zhang, Daliang Energy & Environmental Science, Vol. 4, Issue 10 https://doi.org/10.1039/c1ee01222c	journal	January 2011
Conjugated microporous polymers: design, synthesis and application Xu, Yanhong; Jin, Shangbin; Xu, Hong Chemical Society Reviews, Vol. 42, Issue 20 https://doi.org/10.1039/c3cs60160a	journal	January 2013
Technetium-99 Removal from Process Solutions and Contaminated Groundwater del Cul, G. D.; Bostick, W. D.; Trotter, D. R. Separation Science and Technology, Vol. 28, Issue 1-3 https://doi.org/10.1080/01496399308019506	journal	January 1993

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