A poly(acrylonitrile)-functionalized porous aromatic framework synthesized by atom-transfer radical polymerization for the extraction of uranium from seawater

Yanfeng Yue; Chenxi Zhang; Qing Tang; Richard T. Mayes; Wei Po Liao; Chen Liao; Costas Tsouris; Joseph J. Stankovich; Jihua Chen; Dale K. Hensley; Carter W. Abney; De En Jiang; Suree Brown; Sheng Dai

doi:10.1021/acs.iecr.5b03372

A poly(acrylonitrile)-functionalized porous aromatic framework synthesized by atom-transfer radical polymerization for the extraction of uranium from seawater

Yanfeng Yue, Chenxi Zhang, Qing Tang, Richard T. Mayes, Wei Po Liao, Chen Liao, Costas Tsouris, Joseph J. Stankovich, Jihua Chen, Dale K. Hensley, Carter W. Abney, De En Jiang, Suree Brown, Sheng Dai

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72 Scopus citations

Abstract

In order to ensure a sustainable reserve of fuel for nuclear power generation, tremendous research efforts have been devoted to developing advanced sorbent materials for extracting uranium from seawater. In this work, a porous aromatic framework (PAF) was surface-functionalized with poly(acrylonitrile) through atom-transfer radical polymerization (ATRP). Batches of this adsorbent were conditioned with potassium hydroxide (KOH) at room temperature or 80 °C prior to contact with a uranium-spiked seawater simulant, with minimal differences in uptake observed as a function of conditioning temperature. A maximum capacity of 4.81 g-U/kg-ads was obtained following 42 days contact with uranium-spiked filtered environmental seawater, which demonstrates a comparable adsorption rate. A kinetic investigation revealed extremely rapid uranyl uptake, with more than 80% saturation reached within 14 days. Relying on the semiordered structure of the PAF adsorbent, density functional theory (DFT) calculations reveal cooperative interactions between multiple adsorbent groups yield a strong driving force for uranium binding.

Original language	English
Pages (from-to)	4125-4129
Number of pages	5
Journal	Industrial and Engineering Chemistry Research
Volume	55
Issue number	15
DOIs	https://doi.org/10.1021/acs.iecr.5b03372
State	Published - Oct 30 2015

Funding

This work was sponsored by the U.S. Department of Energy, Office of Nuclear Energy, under Contract No. DE-AC05-00OR22725 with Oak Ridge National Laboratory, managed by UT-Battelle, LLC. This work was sponsored by the U.S. Department of Energy, Office of Nuclear Energy, under Contract No. DE-AC05-00OR22725 with Oak Ridge National Laboratory, managed by UT-Battelle, LLC. Electron microscopy (J.C. and D.K.H.) experiments were conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. DFT computation (Q.T. and D.J.) was supported by DOE Office of Nuclear Energy - Nuclear Energy University Programs (Grant No. DE-NE0008397) and resources of the National Energy Research Scientific Computing Center, which is a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy, under Contract No. DE-AC02-05CH11231.

Funders	Funder number
DOE Office of Nuclear Energy
DOE Office of Science
National Energy Research Scientific Computing Center
Nuclear Energy University Programs	DE-NE0008397
UT-Battelle
U.S. Department of Energy
Office of Science
Office of Nuclear Energy	DE-AC05-00OR22725
Oak Ridge National Laboratory

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10.1021/acs.iecr.5b03372

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Yue, Y., Zhang, C., Tang, Q., Mayes, R. T., Liao, W. P., Liao, C., Tsouris, C., Stankovich, J. J., Chen, J., Hensley, D. K., Abney, C. W., Jiang, D. E., Brown, S., & Dai, S. (2015). A poly(acrylonitrile)-functionalized porous aromatic framework synthesized by atom-transfer radical polymerization for the extraction of uranium from seawater. Industrial and Engineering Chemistry Research, 55(15), 4125-4129. https://doi.org/10.1021/acs.iecr.5b03372

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title = "A poly(acrylonitrile)-functionalized porous aromatic framework synthesized by atom-transfer radical polymerization for the extraction of uranium from seawater",

abstract = "In order to ensure a sustainable reserve of fuel for nuclear power generation, tremendous research efforts have been devoted to developing advanced sorbent materials for extracting uranium from seawater. In this work, a porous aromatic framework (PAF) was surface-functionalized with poly(acrylonitrile) through atom-transfer radical polymerization (ATRP). Batches of this adsorbent were conditioned with potassium hydroxide (KOH) at room temperature or 80 °C prior to contact with a uranium-spiked seawater simulant, with minimal differences in uptake observed as a function of conditioning temperature. A maximum capacity of 4.81 g-U/kg-ads was obtained following 42 days contact with uranium-spiked filtered environmental seawater, which demonstrates a comparable adsorption rate. A kinetic investigation revealed extremely rapid uranyl uptake, with more than 80% saturation reached within 14 days. Relying on the semiordered structure of the PAF adsorbent, density functional theory (DFT) calculations reveal cooperative interactions between multiple adsorbent groups yield a strong driving force for uranium binding.",

author = "Yanfeng Yue and Chenxi Zhang and Qing Tang and Mayes, {Richard T.} and Liao, {Wei Po} and Chen Liao and Costas Tsouris and Stankovich, {Joseph J.} and Jihua Chen and Hensley, {Dale K.} and Abney, {Carter W.} and Jiang, {De En} and Suree Brown and Sheng Dai",

note = "Publisher Copyright: {\textcopyright} 2015 American Chemical Society.",

year = "2015",

month = oct,

day = "30",

doi = "10.1021/acs.iecr.5b03372",

language = "English",

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Yue, Y, Zhang, C, Tang, Q, Mayes, RT, Liao, WP, Liao, C, Tsouris, C, Stankovich, JJ, Chen, J , Hensley, DK, Abney, CW, Jiang, DE, Brown, S & Dai, S 2015, 'A poly(acrylonitrile)-functionalized porous aromatic framework synthesized by atom-transfer radical polymerization for the extraction of uranium from seawater', Industrial and Engineering Chemistry Research, vol. 55, no. 15, pp. 4125-4129. https://doi.org/10.1021/acs.iecr.5b03372

A poly(acrylonitrile)-functionalized porous aromatic framework synthesized by atom-transfer radical polymerization for the extraction of uranium from seawater. / Yue, Yanfeng; Zhang, Chenxi; Tang, Qing et al.
In: Industrial and Engineering Chemistry Research, Vol. 55, No. 15, 30.10.2015, p. 4125-4129.

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

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T1 - A poly(acrylonitrile)-functionalized porous aromatic framework synthesized by atom-transfer radical polymerization for the extraction of uranium from seawater

AU - Yue, Yanfeng

AU - Zhang, Chenxi

AU - Tang, Qing

AU - Mayes, Richard T.

AU - Liao, Wei Po

AU - Liao, Chen

AU - Tsouris, Costas

AU - Stankovich, Joseph J.

AU - Chen, Jihua

AU - Hensley, Dale K.

AU - Abney, Carter W.

AU - Jiang, De En

AU - Brown, Suree

AU - Dai, Sheng

PY - 2015/10/30

Y1 - 2015/10/30

N2 - In order to ensure a sustainable reserve of fuel for nuclear power generation, tremendous research efforts have been devoted to developing advanced sorbent materials for extracting uranium from seawater. In this work, a porous aromatic framework (PAF) was surface-functionalized with poly(acrylonitrile) through atom-transfer radical polymerization (ATRP). Batches of this adsorbent were conditioned with potassium hydroxide (KOH) at room temperature or 80 °C prior to contact with a uranium-spiked seawater simulant, with minimal differences in uptake observed as a function of conditioning temperature. A maximum capacity of 4.81 g-U/kg-ads was obtained following 42 days contact with uranium-spiked filtered environmental seawater, which demonstrates a comparable adsorption rate. A kinetic investigation revealed extremely rapid uranyl uptake, with more than 80% saturation reached within 14 days. Relying on the semiordered structure of the PAF adsorbent, density functional theory (DFT) calculations reveal cooperative interactions between multiple adsorbent groups yield a strong driving force for uranium binding.

AB - In order to ensure a sustainable reserve of fuel for nuclear power generation, tremendous research efforts have been devoted to developing advanced sorbent materials for extracting uranium from seawater. In this work, a porous aromatic framework (PAF) was surface-functionalized with poly(acrylonitrile) through atom-transfer radical polymerization (ATRP). Batches of this adsorbent were conditioned with potassium hydroxide (KOH) at room temperature or 80 °C prior to contact with a uranium-spiked seawater simulant, with minimal differences in uptake observed as a function of conditioning temperature. A maximum capacity of 4.81 g-U/kg-ads was obtained following 42 days contact with uranium-spiked filtered environmental seawater, which demonstrates a comparable adsorption rate. A kinetic investigation revealed extremely rapid uranyl uptake, with more than 80% saturation reached within 14 days. Relying on the semiordered structure of the PAF adsorbent, density functional theory (DFT) calculations reveal cooperative interactions between multiple adsorbent groups yield a strong driving force for uranium binding.

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SN - 0888-5885

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JO - Industrial and Engineering Chemistry Research

JF - Industrial and Engineering Chemistry Research

IS - 15

ER -

A poly(acrylonitrile)-functionalized porous aromatic framework synthesized by atom-transfer radical polymerization for the extraction of uranium from seawater

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