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Title: Anion-adaptive crystalline cationic material for 99TcO 4 - trapping

Abstract

Efficient anion recognition is of great significance for radioactive 99TcO 4 - decontamination, but it remains a challenge for traditional sorbents. Herein, we put forward a tactic using soft crystalline cationic material with anion-adaptive dynamics for 99TcO 4 - sequestration. A cucurbit[8]uril-based supramolecular metal-organic material is produced through a multi-component assembly strategy and used as a sorbent for effective trapping of TcO 4 -. Excellent separation of TcO 4 -/ReO 4 - is demonstrated by fast removal kinetics, good sorption capacity and high distribution coefficient. Remarkably, the most superior selectivity among metal-organic materials reported so far, together with good hydrolytic stability, indicates potential for efficient TcO 4 - removal. The structure incorporating ReO 4 - reveals that the supramolecular framework undergoes adaptive reconstruction facilitating the effective accommodation of TcO 4 -/ReO 4 -. The results highlight opportunities for development of soft anion-adaptive sorbents for highly selective anion decontamination.

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [2];  [1];  [1];  [1]; ORCiD logo [1];  [3];  [2];  [4];  [1]
  1. Chinese Academy of Sciences (CAS), Beijing (China)
  2. Tsinghua Univ., Beijing (China)
  3. Chinese Academy of Sciences (CAS), Beijing (China); Chinese Academy of Sciences, Ningbo, Zhejiang (China)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Actinide Science & Technology (CAST); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1546668
Grant/Contract Number:  
AC02-05CH11231; SC0016568
Resource Type:
Journal Article: 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:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Mei, Lei, Li, Fei-ze, Lan, Jian-hui, Wang, Cong-zhi, Xu, Chao, Deng, Hao, Wu, Qun-yan, Hu, Kong-qiu, Wang, Lin, Chai, Zhi-fang, Chen, Jing, Gibson, John K., and Shi, Wei-qun. Anion-adaptive crystalline cationic material for 99TcO4- trapping. United States: N. p., 2019. Web. doi:10.1038/s41467-019-09504-3.
Mei, Lei, Li, Fei-ze, Lan, Jian-hui, Wang, Cong-zhi, Xu, Chao, Deng, Hao, Wu, Qun-yan, Hu, Kong-qiu, Wang, Lin, Chai, Zhi-fang, Chen, Jing, Gibson, John K., & Shi, Wei-qun. Anion-adaptive crystalline cationic material for 99TcO4- trapping. United States. doi:10.1038/s41467-019-09504-3.
Mei, Lei, Li, Fei-ze, Lan, Jian-hui, Wang, Cong-zhi, Xu, Chao, Deng, Hao, Wu, Qun-yan, Hu, Kong-qiu, Wang, Lin, Chai, Zhi-fang, Chen, Jing, Gibson, John K., and Shi, Wei-qun. Thu . "Anion-adaptive crystalline cationic material for 99TcO4- trapping". United States. doi:10.1038/s41467-019-09504-3. https://www.osti.gov/servlets/purl/1546668.
@article{osti_1546668,
title = {Anion-adaptive crystalline cationic material for 99TcO4- trapping},
author = {Mei, Lei and Li, Fei-ze and Lan, Jian-hui and Wang, Cong-zhi and Xu, Chao and Deng, Hao and Wu, Qun-yan and Hu, Kong-qiu and Wang, Lin and Chai, Zhi-fang and Chen, Jing and Gibson, John K. and Shi, Wei-qun},
abstractNote = {Efficient anion recognition is of great significance for radioactive 99TcO4- decontamination, but it remains a challenge for traditional sorbents. Herein, we put forward a tactic using soft crystalline cationic material with anion-adaptive dynamics for 99TcO4- sequestration. A cucurbit[8]uril-based supramolecular metal-organic material is produced through a multi-component assembly strategy and used as a sorbent for effective trapping of TcO4-. Excellent separation of TcO4-/ReO4- is demonstrated by fast removal kinetics, good sorption capacity and high distribution coefficient. Remarkably, the most superior selectivity among metal-organic materials reported so far, together with good hydrolytic stability, indicates potential for efficient TcO4- removal. The structure incorporating ReO4- reveals that the supramolecular framework undergoes adaptive reconstruction facilitating the effective accommodation of TcO4-/ReO4-. The results highlight opportunities for development of soft anion-adaptive sorbents for highly selective anion decontamination.},
doi = {10.1038/s41467-019-09504-3},
journal = {Nature Communications},
issn = {2041-1723},
number = 1,
volume = 10,
place = {United States},
year = {2019},
month = {4}
}

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    Works referencing / citing this record:

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    journal, March 2012

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

    NDTB-1: A Supertetrahedral Cationic Framework That Removes TcO 4 from Solution
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    • Wang, Shuao; Alekseev, Evgeny V.; Diwu, Juan
    • Angewandte Chemie International Edition, Vol. 49, Issue 6
    • DOI: 10.1002/anie.200906397

    Bambus[6]uril
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    • DOI: 10.1002/anie.201409895

    A Water-Stable Cationic Metal-Organic Framework as a Dual Adsorbent of Oxoanion Pollutants
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    • Desai, Aamod V.; Manna, Biplab; Karmakar, Avishek
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    • DOI: 10.1002/anie.201600185

    Selective Anion Extraction and Recovery Using a Fe II 4 L 4 Cage
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    • Zhang, Dawei; Ronson, Tanya K.; Mosquera, Jesús
    • Angewandte Chemie International Edition, Vol. 57, Issue 14
    • DOI: 10.1002/anie.201800459

    Removal of Pertechnetate-Related Oxyanions from Solution Using Functionalized Hierarchical Porous Frameworks
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    • Banerjee, Debasis; Elsaidi, Sameh K.; Aguila, Briana
    • Chemistry - A European Journal, Vol. 22, Issue 49
    • DOI: 10.1002/chem.201603908

    Anion encapsulation and complexation by cucurbit[n]urils and their derivatives
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    • Zhang, Mingli; Lin, Rui-Lian; Sun, Wen-Qi
    • Journal of Inclusion Phenomena and Macrocyclic Chemistry, Vol. 90, Issue 3-4
    • DOI: 10.1007/s10847-017-0777-6

    Synthesis and guest exchange reactions of inclusion compounds of cucurbit[8]uril with nickel(II) and copper(II) complexes
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    • Mitkina, T. V.; Naumov, D. Yu.; Kurat’eva, N. V.
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    • Derradji, Mehdi; Zegaoui, Abdeldjalil; Xu, Yi-Le
    • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 421
    • DOI: 10.1016/j.nimb.2018.02.017

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    Cucurbituril-Based Molecular Recognition
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    Reversible, Selective Trapping of Perchlorate from Water in Record Capacity by a Cationic Metal–Organic Framework
    journal, January 2016

    • Colinas, Ian R.; Silva, Rachel C.; Oliver, Scott R. J.
    • Environmental Science & Technology, Vol. 50, Issue 4
    • DOI: 10.1021/acs.est.5b03455

    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

    Zirconium-Based Metal–Organic Framework for Removal of Perrhenate from Water
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    Modular Chemistry: Secondary Building Units as a Basis for the Design of Highly Porous and Robust Metal−Organic Carboxylate Frameworks
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    • Eddaoudi, Mohamed; Moler, David B.; Li, Hailian
    • Accounts of Chemical Research, Vol. 34, Issue 4, p. 319-330
    • DOI: 10.1021/ar000034b

    Self-Assemblies Based on the “Outer-Surface Interactions” of Cucurbit[ n ]urils: New Opportunities for Supramolecular Architectures and Materials
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    • Ni, Xin-Long; Xiao, Xin; Cong, Hang
    • Accounts of Chemical Research, Vol. 47, Issue 4
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    Metal–Organic Frameworks for Separations
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    • Li, Jian-Rong; Sculley, Julian; Zhou, Hong-Cai
    • Chemical Reviews, Vol. 112, Issue 2, p. 869-932
    • DOI: 10.1021/cr200190s

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    • Koch, U.; Popelier, P. L. A.
    • The Journal of Physical Chemistry, Vol. 99, Issue 24
    • DOI: 10.1021/j100024a016

    Smart Molecular Helical Springs as Tunable Receptors
    journal, October 2000

    • Jung, Ok-Sang; Kim, Yun Ju; Lee, Young-A
    • Journal of the American Chemical Society, Vol. 122, Issue 41
    • DOI: 10.1021/ja001618b

    Revealing Noncovalent Interactions
    journal, May 2010

    • Johnson, Erin R.; Keinan, Shahar; Mori-Sánchez, Paula
    • Journal of the American Chemical Society, Vol. 132, Issue 18
    • DOI: 10.1021/ja100936w

    A New Paradigm for Anion Trapping in High Capacity and Selectivity: Crystal-to-Crystal Transformation of Cationic Materials
    journal, July 2011

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