Effective Removal of Anionic Re(VII) by Surface-Modified Ti 2 CT x MXene Nanocomposites: Implications for Tc(VII) Sequestration
Abstract
Environmental contamination by 99Tc(VII) from radioactive wastewater streams is of particular concern due to the long half-life of 99Tc and high mobility of pertechnetate. Here in this paper, we report a novel MXene-polyelectrolyte nanocomposite with three-dimensional networks for enhanced removal of perrhenate, which is pertechnetate simulant. The introduction of poly(diallyldimethylammonium chloride) (PDDA) regulates the surface charge and improves the stability of Ti2CTx nanosheet, resulting in Re(VII) removal capacity of up to 363 mg g–1, and fast sorption kinetics. The Ti2CTx/PDDA nanocomposite furthermore exhibits good selectivity for ReO4– when competing anions (such as Cl– and SO42–) coexist at a concentration of 1800 times. The immobilization mechanism was confirmed as a sorption-reduction process by batch sorption experiments and X-ray photoelectron spectroscopy. The pH-dependent reducing activity of Ti2CTx/PDDA nanocomposite toward Re(VII) was clarified by X-ray absorption spectroscopy. As the pH increases, the local environment gradually changes from octahedral-coordinated Re(IV) to tetrahedral-coordinated Re(VII). The overall results suggest that Ti2CTx/PDDA nanocomposite may be a promising candidate for efficient elimination of Tc contamination. The reported surface modification strategy might result in applications of MXene-based materials in environmental remediation of other oxidized anion pollutants.
- Authors:
-
[1];
[1];
[3];
[1]
- Chinese Academy of Sciences (CAS), Beijing (China). Lab. of Nuclear Energy Chemistry and Key Lab. for Biomedical Effects of Nanomaterials and Nanosafety, Inst. of High Energy Physics
- Chinese Academy of Sciences (CAS), Beijing (China). Lab. of Nuclear Energy Chemistry and Key Lab. for Biomedical Effects of Nanomaterials and Nanosafety, Inst. of High Energy Physics; Univ. of South China, Hengyang (China). School of Chemistry and Chemical Engineering and Hunan Key Lab. for the Design and Application of Actinide Complexes
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
- Chinese Academy of Sciences (CAS), Beijing (China). Beijing Synchrotron Radiation Facility, Inst. of High Energy Physics
- Univ. of South China, Hengyang (China). School of Chemistry and Chemical Engineering and Hunan Key Lab. for the Design and Application of Actinide Complexes
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Actinide Science & Technology (CAST); Florida State Univ., Tallahassee, FL (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC)
- OSTI Identifier:
- 1566498
- Alternate Identifier(s):
- OSTI ID: 1656505
- Grant/Contract Number:
- SC0016568; 21577144; 11675192; 21790373; 21790370; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Environmental Science and Technology
- Additional Journal Information:
- Journal Volume: 53; Journal Issue: 7; Journal ID: ISSN 0013-936X
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; nuclear; defects; mechanical behavior; corrosion; charge transport; superconductivity; magnetism and spin physics; separations; geophysics/geochemistry; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly); synthesis (predictive); synthesis (scalable processing)
Citation Formats
Wang, Lin, Song, Huan, Yuan, Liyong, Li, Zijie, Zhang, Peng, Gibson, John K., Zheng, Lirong, Wang, Hongqing, Chai, Zhifang, and Shi, Weiqun. Effective Removal of Anionic Re(VII) by Surface-Modified Ti 2 CT x MXene Nanocomposites: Implications for Tc(VII) Sequestration. United States: N. p., 2019.
Web. doi:10.1021/acs.est.8b07083.
Wang, Lin, Song, Huan, Yuan, Liyong, Li, Zijie, Zhang, Peng, Gibson, John K., Zheng, Lirong, Wang, Hongqing, Chai, Zhifang, & Shi, Weiqun. Effective Removal of Anionic Re(VII) by Surface-Modified Ti 2 CT x MXene Nanocomposites: Implications for Tc(VII) Sequestration. United States. https://doi.org/10.1021/acs.est.8b07083
Wang, Lin, Song, Huan, Yuan, Liyong, Li, Zijie, Zhang, Peng, Gibson, John K., Zheng, Lirong, Wang, Hongqing, Chai, Zhifang, and Shi, Weiqun. Thu .
"Effective Removal of Anionic Re(VII) by Surface-Modified Ti 2 CT x MXene Nanocomposites: Implications for Tc(VII) Sequestration". United States. https://doi.org/10.1021/acs.est.8b07083. https://www.osti.gov/servlets/purl/1566498.
@article{osti_1566498,
title = {Effective Removal of Anionic Re(VII) by Surface-Modified Ti 2 CT x MXene Nanocomposites: Implications for Tc(VII) Sequestration},
author = {Wang, Lin and Song, Huan and Yuan, Liyong and Li, Zijie and Zhang, Peng and Gibson, John K. and Zheng, Lirong and Wang, Hongqing and Chai, Zhifang and Shi, Weiqun},
abstractNote = {Environmental contamination by 99Tc(VII) from radioactive wastewater streams is of particular concern due to the long half-life of 99Tc and high mobility of pertechnetate. Here in this paper, we report a novel MXene-polyelectrolyte nanocomposite with three-dimensional networks for enhanced removal of perrhenate, which is pertechnetate simulant. The introduction of poly(diallyldimethylammonium chloride) (PDDA) regulates the surface charge and improves the stability of Ti2CTx nanosheet, resulting in Re(VII) removal capacity of up to 363 mg g–1, and fast sorption kinetics. The Ti2CTx/PDDA nanocomposite furthermore exhibits good selectivity for ReO4– when competing anions (such as Cl– and SO42–) coexist at a concentration of 1800 times. The immobilization mechanism was confirmed as a sorption-reduction process by batch sorption experiments and X-ray photoelectron spectroscopy. The pH-dependent reducing activity of Ti2CTx/PDDA nanocomposite toward Re(VII) was clarified by X-ray absorption spectroscopy. As the pH increases, the local environment gradually changes from octahedral-coordinated Re(IV) to tetrahedral-coordinated Re(VII). The overall results suggest that Ti2CTx/PDDA nanocomposite may be a promising candidate for efficient elimination of Tc contamination. The reported surface modification strategy might result in applications of MXene-based materials in environmental remediation of other oxidized anion pollutants.},
doi = {10.1021/acs.est.8b07083},
journal = {Environmental Science and Technology},
number = 7,
volume = 53,
place = {United States},
year = {Thu Mar 07 00:00:00 EST 2019},
month = {Thu Mar 07 00:00:00 EST 2019}
}
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