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

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

78 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.

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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

@article{622fef5b217a413f93d303f8025c7327,

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

TY - JOUR

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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SP - 4125

EP - 4129

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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