Strategies toward the Synthesis of Advanced Functional Sorbent Performance for Uranium Uptake from Seawater

Sadananda Das; Zongyu Wang; Suree Brown; Christopher J. Janke; Richard T. Mayes; Gary A. Gill; Sheng Dai

doi:10.1021/acs.iecr.1c02920

Strategies toward the Synthesis of Advanced Functional Sorbent Performance for Uranium Uptake from Seawater

Sadananda Das, Zongyu Wang, Suree Brown, Christopher J. Janke, Richard T. Mayes, Gary A. Gill, Sheng Dai

Research output: Contribution to journal › Article › peer-review

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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. The¹³C 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. 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.

Original language	English
Pages (from-to)	15037-15044
Number of pages	8
Journal	Industrial and Engineering Chemistry Research
Volume	60
Issue number	42
DOIs	https://doi.org/10.1021/acs.iecr.1c02920
State	Published - Oct 27 2021

Funding

This research was conducted at Oak Ridge National Laboratory (ORNL) and the Marine Sciences Laboratory of Pacific Northwest National Laboratory (PNNL). This work was supported by the U.S. Department of Energy, Office of Nuclear Energy. This manuscript has been authored by UT-Battelle, LLC under contract no. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research following the DOE Public Access Plan ( http://energy.gov/ downloads/doe-public-access-plan). We thank Dr. Venkata S. Neti for help with the construction, maintenance, and operation of the testing facility.

Funders	Funder number
U.S. Department of Energy
Office of Nuclear Energy	DE-AC05-00OR22725

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title = "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. The13C 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. 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.",

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AB - 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. The13C 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. 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.

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Strategies toward the Synthesis of Advanced Functional Sorbent Performance for Uranium Uptake from Seawater

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