Strategies toward the Synthesis of Advanced Functional Sorbent Performance for Uranium Uptake from Seawater
Abstract
A polymer fiber-based adsorbent (AF1) composed of acrylonitrile and itaconic acid functional groups was synthesized by a radiation-induced graft polymerization technique onto hollow-gear shaped polyethylene (PE) fibers. Investigation of the optimum reaction parameters for the conversion of grafted cyano moieties into amidoxime groups was conducted by the reaction with hydroxylamine at different temperatures and periods in a variety of aqueous and organic solvents. The 13C CP/MAS spectra of amidoximated AF1 adsorbent fibers from water–methanol and dimethyl sulfoxide (DMSO) revealed that both the cyclic imide dioxime and open-chain amidoxime were formed through the reaction. The conversion from amidoxime to imide dioxime was found to occur slowly and gradually with the increasing reaction time. The quicker diffusion of DMSO as compared to that of water–methanol, in the grafted trunk PE fiber, resulted in faster kinetics of the amidoximation reaction. The uranium adsorption capacity of the amidoximated AF1 samples was determined after (i) 24 h contact with sodium-based brine spiked with uranium and (ii) 56 days of exposure to filtered seawater (Sequim Bay, WA, USA) in flow-through columns. Finally, the uranium extraction performance of the adsorbents after exposure to filtered seawater was consistent with the laboratory screening results, and the amidoximated AF1 samplesmore »
- Authors:
-
[1];
[1];
[1];
[3]
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Office of Nuclear Energy (NE)
- OSTI Identifier:
- 1833942
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Industrial and Engineering Chemistry Research
- Additional Journal Information:
- Journal Volume: 60; Journal Issue: 42; Journal ID: ISSN 0888-5885
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; seawater; fibers; uranium; adsorption; solvents; fiber-based adsorbent; polyacrylonitrile; uranium adsorption; itaconic acid; amidoximation
Citation Formats
Das, Sadananda, Wang, Zongyu, Brown, Suree, Janke, Christopher, Mayes, Richard, A. Gill, Gary, and Dai, Sheng. Strategies toward the Synthesis of Advanced Functional Sorbent Performance for Uranium Uptake from Seawater. United States: N. p., 2021.
Web. doi:10.1021/acs.iecr.1c02920.
Das, Sadananda, Wang, Zongyu, Brown, Suree, Janke, Christopher, Mayes, Richard, A. Gill, Gary, & Dai, Sheng. Strategies toward the Synthesis of Advanced Functional Sorbent Performance for Uranium Uptake from Seawater. United States. https://doi.org/10.1021/acs.iecr.1c02920
Das, Sadananda, Wang, Zongyu, Brown, Suree, Janke, Christopher, Mayes, Richard, A. Gill, Gary, and Dai, Sheng. Wed .
"Strategies toward the Synthesis of Advanced Functional Sorbent Performance for Uranium Uptake from Seawater". United States. https://doi.org/10.1021/acs.iecr.1c02920. https://www.osti.gov/servlets/purl/1833942.
@article{osti_1833942,
title = {Strategies toward the Synthesis of Advanced Functional Sorbent Performance for Uranium Uptake from Seawater},
author = {Das, Sadananda and Wang, Zongyu and Brown, Suree and Janke, Christopher and Mayes, Richard and A. Gill, Gary and Dai, Sheng},
abstractNote = {A polymer fiber-based adsorbent (AF1) composed of acrylonitrile and itaconic acid functional groups was synthesized by a radiation-induced graft polymerization technique onto hollow-gear shaped polyethylene (PE) fibers. Investigation of the optimum reaction parameters for the conversion of grafted cyano moieties into amidoxime groups was conducted by the reaction with hydroxylamine at different temperatures and periods in a variety of aqueous and organic solvents. The 13C CP/MAS spectra of amidoximated AF1 adsorbent fibers from water–methanol and dimethyl sulfoxide (DMSO) revealed that both the cyclic imide dioxime and open-chain amidoxime were formed through the reaction. The conversion from amidoxime to imide dioxime was found to occur slowly and gradually with the increasing reaction time. The quicker diffusion of DMSO as compared to that of water–methanol, in the grafted trunk PE fiber, resulted in faster kinetics of the amidoximation reaction. The uranium adsorption capacity of the amidoximated AF1 samples was determined after (i) 24 h contact with sodium-based brine spiked with uranium and (ii) 56 days of exposure to filtered seawater (Sequim Bay, WA, USA) in flow-through columns. Finally, the uranium extraction performance of the adsorbents after exposure to filtered seawater was consistent with the laboratory screening results, and the amidoximated AF1 samples (in DMSO at 70 °C for 3 h) exhibited the highest 56 day uranium adsorption capacity (5.04 ± 0.15 g U/kg-ads) with faster adsorption kinetics compared to the pristine AF1 adsorbents.},
doi = {10.1021/acs.iecr.1c02920},
journal = {Industrial and Engineering Chemistry Research},
number = 42,
volume = 60,
place = {United States},
year = {Wed Oct 13 00:00:00 EDT 2021},
month = {Wed Oct 13 00:00:00 EDT 2021}
}
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