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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 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];  [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:
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Cited by: 14 works
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Figures / Tables:

Fig. 1 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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Works referenced in this record:

Conjugated microporous polymers: design, synthesis and application
journal, January 2013

  • Xu, Yanhong; Jin, Shangbin; Xu, Hong
  • Chemical Society Reviews, Vol. 42, Issue 20
  • DOI: 10.1039/c3cs60160a

Selective Anion Extraction and Recovery Using a Fe II 4 L 4 Cage
journal, February 2018

  • Zhang, Dawei; Ronson, Tanya K.; Mosquera, Jesús
  • Angewandte Chemie International Edition, Vol. 57, Issue 14
  • DOI: 10.1002/anie.201800459

NDTB-1: A Supertetrahedral Cationic Framework That Removes TcO 4 from Solution
journal, February 2010

  • Wang, Shuao; Alekseev, Evgeny V.; Diwu, Juan
  • Angewandte Chemie International Edition, Vol. 49, Issue 6
  • DOI: 10.1002/anie.200906397

Design and Preparation of Porous Polymers
journal, April 2012

  • Wu, Dingcai; Xu, Fei; Sun, Bin
  • Chemical Reviews, Vol. 112, Issue 7
  • DOI: 10.1021/cr200440z

Technetium-99 Removal from Process Solutions and Contaminated Groundwater
journal, January 1993

  • del Cul, G. D.; Bostick, W. D.; Trotter, D. R.
  • Separation Science and Technology, Vol. 28, Issue 1-3
  • DOI: 10.1080/01496399308019506

Identifying the Recognition Site for Selective Trapping of 99 TcO 4 in a Hydrolytically Stable and Radiation Resistant Cationic Metal–Organic Framework
journal, October 2017

  • Zhu, Lin; Sheng, Daopeng; Xu, Chao
  • Journal of the American Chemical Society, Vol. 139, Issue 42
  • DOI: 10.1021/jacs.7b08632

Exceptional Iodine Capture in 2D Covalent Organic Frameworks
journal, May 2018


Sensing Uranyl(VI) Ions by Coordination and Energy Transfer to a Luminescent Europium(III) Complex
journal, June 2018

  • Harvey, Peter; Nonat, Aline; Platas-Iglesias, Carlos
  • Angewandte Chemie International Edition, Vol. 57, Issue 31
  • DOI: 10.1002/anie.201805316

A hierarchical porous ionic organic polymer as a new platform for heterogeneous phase transfer catalysis
journal, January 2015

  • Sun, Qi; Ma, Shengqian; Dai, Zhifeng
  • Journal of Materials Chemistry A, Vol. 3, Issue 47
  • DOI: 10.1039/C5TA07267K

Preparation of Polymer-Coated, Scintillating Ion-Exchange Resins for Monitoring of 99 Tc in Groundwater
journal, June 2011

  • Seliman, Ayman F.; Samadi, Azadeh; Husson, Scott M.
  • Analytical Chemistry, Vol. 83, Issue 12
  • DOI: 10.1021/ac103311p

Metal–organic framework-based materials: superior adsorbents for the capture of toxic and radioactive metal ions
journal, January 2018

  • Li, Jie; Wang, Xiangxue; Zhao, Guixia
  • Chemical Society Reviews, Vol. 47, Issue 7
  • DOI: 10.1039/C7CS00543A

Impeding 99Tc(IV) mobility in novel waste forms
journal, June 2016

  • Lee, Mal-Soon; Um, Wooyong; Wang, Guohui
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms12067

99TcO4− remediation by a cationic polymeric network
journal, August 2018


Alternative energy technologies
journal, November 2001

  • Dresselhaus, M. S.; Thomas, I. L.
  • Nature, Vol. 414, Issue 6861
  • DOI: 10.1038/35104599

Materials for the Recovery of Uranium from Seawater
journal, June 2017


Fluorescent sensing of 99 Tc pertechnetate in water
journal, January 2014

  • Amendola, Valeria; Bergamaschi, Greta; Boiocchi, Massimo
  • Chem. Sci., Vol. 5, Issue 5
  • DOI: 10.1039/C3SC53504E

Chemical Trends in Solid Alkali Pertechnetates
journal, February 2017


Emerging opportunities for nanotechnology to enhance water security
journal, August 2018

  • Alvarez, Pedro J. J.; Chan, Candace K.; Elimelech, Menachem
  • Nature Nanotechnology, Vol. 13, Issue 8
  • DOI: 10.1038/s41565-018-0203-2

Highly Efficient Enrichment of Volatile Iodine by Charged Porous Aromatic Frameworks with Three Sorption Sites
journal, August 2015

  • Yan, Zhuojun; Yuan, Ye; Tian, Yuyang
  • Angewandte Chemie International Edition, Vol. 54, Issue 43
  • DOI: 10.1002/anie.201503362

Mercury nano-trap for effective and efficient removal of mercury(II) from aqueous solution
journal, November 2014

  • Li, Baiyan; Zhang, Yiming; Ma, Dingxuan
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms6537

Selectivity, Kinetics, and Efficiency of Reversible Anion Exchange with TcO4− in a Supertetrahedral Cationic Framework
journal, March 2012

  • Wang, Shuao; Yu, Ping; Purse, Bryant A.
  • Advanced Functional Materials, Vol. 22, Issue 11
  • DOI: 10.1002/adfm.201103081

Role of nanomaterials in water treatment applications: A review
journal, December 2016

  • Santhosh, Chella; Velmurugan, Venugopal; Jacob, George
  • Chemical Engineering Journal, Vol. 306
  • DOI: 10.1016/j.cej.2016.08.053

Stable Covalent Organic Frameworks for Exceptional Mercury Removal from Aqueous Solutions
journal, February 2017

  • Huang, Ning; Zhai, Lipeng; Xu, Hong
  • Journal of the American Chemical Society, Vol. 139, Issue 6
  • DOI: 10.1021/jacs.6b12328

Bio-inspired nano-traps for uranium extraction from seawater and recovery from nuclear waste
journal, April 2018


Function-led design of new porous materials
journal, May 2015


Thioether-Based Fluorescent Covalent Organic Framework for Selective Detection and Facile Removal of Mercury(II)
journal, February 2016

  • Ding, San-Yuan; Dong, Ming; Wang, Ya-Wen
  • Journal of the American Chemical Society, Vol. 138, Issue 9
  • DOI: 10.1021/jacs.5b10754

Opportunities of Porous Organic Polymers for Radionuclide Sequestration
journal, June 2019


Topotactic Transformations of Metal–Organic Frameworks to Highly Porous and Stable Inorganic Sorbents for Efficient Radionuclide Sequestration
journal, September 2014

  • Abney, Carter W.; Taylor-Pashow, Kathryn M. L.; Russell, Shane R.
  • Chemistry of Materials, Vol. 26, Issue 18
  • DOI: 10.1021/cm501894h

Molecularly Imprinted Porous Aromatic Frameworks and Their Composite Components for Selective Extraction of Uranium Ions
journal, February 2018


Removal of Pertechnetate from Simulated Nuclear Waste Streams Using Supported Zerovalent Iron
journal, November 2007

  • Darab, John G.; Amonette, Alexandra B.; Burke, Deborah S. D.
  • Chemistry of Materials, Vol. 19, Issue 23
  • DOI: 10.1021/cm0607379

Rapid removal of organic micropollutants from water by a porous β-cyclodextrin polymer
journal, December 2015

  • Alsbaiee, Alaaeddin; Smith, Brian J.; Xiao, Leilei
  • Nature, Vol. 529, Issue 7585
  • DOI: 10.1038/nature16185

Rapid, Selective Heavy Metal Removal from Water by a Metal–Organic Framework/Polydopamine Composite
journal, March 2018


Porous Organic Materials: Strategic Design and Structure–Function Correlation
journal, December 2016


Hierarchical Materials as Tailored Nuclear Waste Forms: A Perspective
journal, June 2018


Efficient and Selective Uptake of TcO 4 by a Cationic Metal–Organic Framework Material with Open Ag + Sites
journal, March 2017

  • Sheng, Daopeng; Zhu, Lin; Xu, Chao
  • Environmental Science & Technology, Vol. 51, Issue 6
  • DOI: 10.1021/acs.est.7b00339

Artificial Organic Host Molecules for Anions
journal, August 1997

  • Schmidtchen, Franz P.; Berger, Michael
  • Chemical Reviews, Vol. 97, Issue 5
  • DOI: 10.1021/cr9603845

Seawater Uranium Sorbents: Preparation from a Mesoporous Copolymer Initiator by Atom-Transfer Radical Polymerization
journal, October 2013

  • Yue, Yanfeng; Mayes, Richard T.; Kim, Jungseung
  • Angewandte Chemie International Edition, Vol. 52, Issue 50
  • DOI: 10.1002/anie.201307825

Physical Removal of Anions from Aqueous Media by Means of a Macrocycle-Containing Polymeric Network
journal, February 2018

  • Ji, Xiaofan; Wu, Ren-Tsung; Long, Lingliang
  • Journal of the American Chemical Society, Vol. 140, Issue 8
  • DOI: 10.1021/jacs.7b13656

Development of Bifunctional Anion-Exchange Resins with Improved Selectivity and Sorptive Kinetics for Pertechnetate:  Batch-Equilibrium Experiments
journal, September 2000

  • Bonnesen, Peter V.; Brown, Gilbert M.; Alexandratos, Spiro D.
  • Environmental Science & Technology, Vol. 34, Issue 17
  • DOI: 10.1021/es990858s

The Development of a Classical Force Field To Determine the Selectivity of an Aqueous Fe 3+ –EDA Complex for TcO 4 and SO 4 2–
journal, July 2014

  • Williams, Christopher D.; Burton, Neil A.; Travis, Karl P.
  • Journal of Chemical Theory and Computation, Vol. 10, Issue 8
  • DOI: 10.1021/ct500198c

Catalyst: Nuclear Power in the 21 st Century
journal, November 2016


Charge-specific size-dependent separation of water-soluble organic molecules by fluorinated nanoporous networks
journal, November 2016

  • Byun, Jeehye; Patel, Hasmukh A.; Thirion, Damien
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms13377

Efficient Capture of Perrhenate and Pertechnetate by a Mesoporous Zr Metal–Organic Framework and Examination of Anion Binding Motifs
journal, January 2018


A review of the radiation stability of ion exchange materials
journal, November 1986

  • Pillay, K. K. S.
  • Journal of Radioanalytical and Nuclear Chemistry Articles, Vol. 102, Issue 1
  • DOI: 10.1007/BF02037966

Three-Dimensional Ionic Covalent Organic Frameworks for Rapid, Reversible, and Selective Ion Exchange
journal, November 2017

  • Li, Zonglong; Li, Hui; Guan, Xinyu
  • Journal of the American Chemical Society, Vol. 139, Issue 49
  • DOI: 10.1021/jacs.7b11283

Ionic Liquids-Based Extraction: A Promising Strategy for the Advanced Nuclear Fuel Cycle
journal, December 2011

  • Sun, Xiaoqi; Luo, Huimin; Dai, Sheng
  • Chemical Reviews, Vol. 112, Issue 4
  • DOI: 10.1021/cr200193x

Removal of TcO 4 ions from solution: materials and future outlook
journal, January 2016

  • Banerjee, Debasis; Kim, Dongsang; Schweiger, Michael J.
  • Chemical Society Reviews, Vol. 45, Issue 10
  • DOI: 10.1039/C5CS00330J

Selective Solid-Liquid and Liquid-Liquid Extraction of Lithium Chloride Using Strapped Calix[4]pyrroles
journal, June 2018

  • He, Qing; Williams, Neil J.; Oh, Ju Hyun
  • Angewandte Chemie International Edition, Vol. 57, Issue 37
  • DOI: 10.1002/anie.201805127

Gas storage in porous aromatic frameworks (PAFs)
journal, January 2011

  • Ben, Teng; Pei, Cuiying; Zhang, Daliang
  • Energy & Environmental Science, Vol. 4, Issue 10
  • DOI: 10.1039/c1ee01222c

Highly Efficient Heterogeneous Hydroformylation over Rh-Metalated Porous Organic Polymers: Synergistic Effect of High Ligand Concentration and Flexible Framework
journal, April 2015

  • Sun, Qi; Dai, Zhifeng; Liu, Xiaolong
  • Journal of the American Chemical Society, Vol. 137, Issue 15
  • DOI: 10.1021/jacs.5b02122

Selective Solid-Liquid and Liquid-Liquid Extraction of Lithium Chloride Using Strapped Calix[4]pyrroles
journal, June 2018


Sensing Uranyl(VI) Ions by Coordination and Energy Transfer to a Luminescent Europium(III) Complex
journal, June 2018

  • Harvey, Peter; Nonat, Aline; Platas-Iglesias, Carlos
  • Angewandte Chemie, Vol. 130, Issue 31
  • DOI: 10.1002/ange.201805316

    Works referencing / citing this record:

    Spectroscopic characterization and in silico modelling of polyvinylpyrrolidone as an anion-responsive fluorescent polymer in aqueous media
    journal, June 2019


    Spectroscopic characterization and in silico modelling of polyvinylpyrrolidone as an anion-responsive fluorescent polymer in aqueous media
    journal, June 2019


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