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

Journal Article · · Advanced Materials
 [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

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. Herein, 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 . These results delineate important synthetic advances toward the implementation of COFs in environmental remediation.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Nuclear Energy (NE); USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC05-00OR22725; NE0008281; AC02‐76SF00515; DE‐NE0008281; DE‐AC02‐76SF00515
OSTI ID:
1435179
Alternate ID(s):
OSTI ID: 1430134
Journal Information:
Advanced Materials, Journal Name: Advanced Materials; ISSN 0935-9648
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 350 works
Citation information provided by
Web of Science

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Ammoniating Covalent Organic Framework (COF) for High‐Performance and Selective Extraction of Toxic and Radioactive Uranium Ions journal June 2019
Extraction and adsorption of U(VI) from aqueous solution using affinity ligand-based technologies: an overview journal July 2019
Opportunities of Covalent Organic Frameworks for Advanced Applications journal November 2018
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Figures / Tables (7)