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Title: Covalent Organic Frameworks as a Decorating Platform for Utilization and Affinity Enhancement of Chelating Sites for Radionuclide Sequestration

Abstract

The potential consequences of nuclear events and the complexity of nuclear waste management motivate the development of selective solid-phase sorbents to provide enhanced protection. In this paper, it is shown that 2D covalent organic frameworks (COFs) with unique structures possess all the traits to be well suited as a platform for the deployment of highly efficient sorbents such that they exhibit remarkable performance, as demonstrated by uranium capture. The chelating groups laced on the open 1D channels exhibit exceptional accessibility, allowing significantly higher utilization efficiency. In addition, the 2D extended polygons packed closely in an eclipsed fashion bring chelating groups in adjacent layers parallel to each other, which may facilitate their cooperation, thereby leading to high affinity toward specific ions. As a result, the amidoxime-functionalized COFs far outperform their corresponding amorphous analogs in terms of adsorption capacities, kinetics, and affinities. Specifically, COF-TpAb-AO is able to reduce various uranium contaminated water samples from 1 ppm to less than 0.1 ppb within several minutes, well below the drinking water limit (30 ppb), as well as mine uranium from spiked seawater with an exceptionally high uptake capacity of 127 mg g -1. Finally, these results delineate important synthetic advances toward the implementation ofmore » COFs in environmental remediation.« less

Authors:
 [1];  [1]; ORCiD logo [2]; ORCiD logo [2];  [1];  [3]; ORCiD logo [1]
  1. Univ. of South Florida, Tampa, FL (United States). Department of Chemistry
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Physical and Computational Science Directorate
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1435179
Alternate Identifier(s):
OSTI ID: 1430134
Grant/Contract Number:  
AC05-00OR22725; NE0008281; AC02‐76SF00515; AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Name: Advanced Materials; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 54 ENVIRONMENTAL SCIENCES; amidoxime chelating groups; covalent organic frameworks; environmental remediation; radionuclide sequestration; uranium capture

Citation Formats

Sun, Qi, Aguila, Briana, Earl, Lyndsey D., Abney, Carter W., Wojtas, Lukasz, Thallapally, Praveen K., and Ma, Shengqian. Covalent Organic Frameworks as a Decorating Platform for Utilization and Affinity Enhancement of Chelating Sites for Radionuclide Sequestration. United States: N. p., 2018. Web. doi:10.1002/adma.201705479.
Sun, Qi, Aguila, Briana, Earl, Lyndsey D., Abney, Carter W., Wojtas, Lukasz, Thallapally, Praveen K., & Ma, Shengqian. Covalent Organic Frameworks as a Decorating Platform for Utilization and Affinity Enhancement of Chelating Sites for Radionuclide Sequestration. United States. doi:10.1002/adma.201705479.
Sun, Qi, Aguila, Briana, Earl, Lyndsey D., Abney, Carter W., Wojtas, Lukasz, Thallapally, Praveen K., and Ma, Shengqian. Tue . "Covalent Organic Frameworks as a Decorating Platform for Utilization and Affinity Enhancement of Chelating Sites for Radionuclide Sequestration". United States. doi:10.1002/adma.201705479. https://www.osti.gov/servlets/purl/1435179.
@article{osti_1435179,
title = {Covalent Organic Frameworks as a Decorating Platform for Utilization and Affinity Enhancement of Chelating Sites for Radionuclide Sequestration},
author = {Sun, Qi and Aguila, Briana and Earl, Lyndsey D. and Abney, Carter W. and Wojtas, Lukasz and Thallapally, Praveen K. and Ma, Shengqian},
abstractNote = {The potential consequences of nuclear events and the complexity of nuclear waste management motivate the development of selective solid-phase sorbents to provide enhanced protection. In this paper, it is shown that 2D covalent organic frameworks (COFs) with unique structures possess all the traits to be well suited as a platform for the deployment of highly efficient sorbents such that they exhibit remarkable performance, as demonstrated by uranium capture. The chelating groups laced on the open 1D channels exhibit exceptional accessibility, allowing significantly higher utilization efficiency. In addition, the 2D extended polygons packed closely in an eclipsed fashion bring chelating groups in adjacent layers parallel to each other, which may facilitate their cooperation, thereby leading to high affinity toward specific ions. As a result, the amidoxime-functionalized COFs far outperform their corresponding amorphous analogs in terms of adsorption capacities, kinetics, and affinities. Specifically, COF-TpAb-AO is able to reduce various uranium contaminated water samples from 1 ppm to less than 0.1 ppb within several minutes, well below the drinking water limit (30 ppb), as well as mine uranium from spiked seawater with an exceptionally high uptake capacity of 127 mg g-1. Finally, these results delineate important synthetic advances toward the implementation of COFs in environmental remediation.},
doi = {10.1002/adma.201705479},
journal = {Advanced Materials},
number = ,
volume = ,
place = {United States},
year = {2018},
month = {3}
}

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Figures / Tables:

Figure 1 Figure 1: a) Synthetic scheme of COF-TpDb through the condensation of Tp (black) and Db (blue) and corresponding chemical transformation from the cyano to amidoxime group, yielding COF-TpDb-AO. b,c) Graphic view of the eclipsed AA stacking structure of COF-TpDb (blue, N; gray, C; red, O; hydrogen is omitted for clarity).more » d) Graphic view of COF-TpDb-AO (blue, N; gray, C; red, O; hydrogen is omitted for clarity).« less

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