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. Furthermore, 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.
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Sul Ross State Univ., Alpine, TX (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Univ. of California, Riverside, CA (United States)
- Univ. of Tennessee, Knoxville, TN (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 Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
- Sponsoring Org.:
- USDOE Office of Nuclear Energy (NE)
- OSTI Identifier:
- 1319227
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Industrial and Engineering Chemistry Research
- Additional Journal Information:
- Journal Volume: 55; Journal Issue: 15; Journal ID: ISSN 0888-5885
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS
Citation Formats
Yue, Yanfeng, Zhang, Chenxi, Tang, Qing, Mayes, Richard T., Liao, Wei -Po, Liao, Chen, Tsouris, Costas, Stankovich, Joseph J., Chen, Jihua, Hensley, Dale K., Abney, Carter W., Jiang, De-en, Brown, Suree, and Dai, Sheng. A poly(acrylonitrile)-functionalized porous aromatic framework synthesized by atom-transfer radical polymerization for the extraction of uranium from seawater. United States: N. p., 2015.
Web. doi:10.1021/acs.iecr.5b03372.
Yue, Yanfeng, Zhang, Chenxi, Tang, Qing, Mayes, Richard T., Liao, Wei -Po, Liao, Chen, Tsouris, Costas, Stankovich, Joseph J., Chen, Jihua, Hensley, Dale K., Abney, Carter W., Jiang, De-en, Brown, Suree, & Dai, Sheng. A poly(acrylonitrile)-functionalized porous aromatic framework synthesized by atom-transfer radical polymerization for the extraction of uranium from seawater. United States. https://doi.org/10.1021/acs.iecr.5b03372
Yue, Yanfeng, Zhang, Chenxi, Tang, Qing, Mayes, Richard T., Liao, Wei -Po, Liao, Chen, Tsouris, Costas, Stankovich, Joseph J., Chen, Jihua, Hensley, Dale K., Abney, Carter W., Jiang, De-en, Brown, Suree, and Dai, Sheng. Fri .
"A poly(acrylonitrile)-functionalized porous aromatic framework synthesized by atom-transfer radical polymerization for the extraction of uranium from seawater". United States. https://doi.org/10.1021/acs.iecr.5b03372. https://www.osti.gov/servlets/purl/1319227.
@article{osti_1319227,
title = {A poly(acrylonitrile)-functionalized porous aromatic framework synthesized by atom-transfer radical polymerization for the extraction of uranium from seawater},
author = {Yue, Yanfeng and Zhang, Chenxi and Tang, Qing and Mayes, Richard T. and Liao, Wei -Po and Liao, Chen and Tsouris, Costas and Stankovich, Joseph J. and Chen, Jihua and Hensley, Dale K. and Abney, Carter W. and Jiang, De-en and Brown, Suree and Dai, Sheng},
abstractNote = {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. Furthermore, 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.},
doi = {10.1021/acs.iecr.5b03372},
journal = {Industrial and Engineering Chemistry Research},
number = 15,
volume = 55,
place = {United States},
year = {Fri Oct 30 00:00:00 EDT 2015},
month = {Fri Oct 30 00:00:00 EDT 2015}
}
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