Effective Removal of Anionic Re(VII) by Surface-Modified Ti 2 CT x MXene Nanocomposites: Implications for Tc(VII) Sequestration

Wang, Lin; Song, Huan; Yuan, Liyong; Li, Zijie; Zhang, Peng; Gibson, John K.; Zheng, Lirong; Wang, Hongqing; Chai, Zhifang; Shi, Weiqun

doi:10.1021/acs.est.8b07083

Effective Removal of Anionic Re(VII) by Surface-Modified Ti ₂ CT _x MXene Nanocomposites: Implications for Tc(VII) Sequestration

Journal Article · Thu Mar 07 00:00:00 EST 2019 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.8b07083· OSTI ID:1566498

^[1]; Song, Huan ^[2]; ^[1]; Li, Zijie ^[1]; Zhang, Peng ^[1]; ^[3]; Zheng, Lirong ^[4]; Wang, Hongqing ^[5]; Chai, Zhifang ^[1]; ^[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

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 Ti₂CT_x nanosheet, resulting in Re(VII) removal capacity of up to 363 mg g^–1, and fast sorption kinetics. The Ti₂CT_x/PDDA nanocomposite furthermore exhibits good selectivity for ReO₄– when competing anions (such as Cl^– and SO₄^2–) 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 Ti₂CT_x/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 Ti₂CT_x/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.

View Accepted Manuscript (DOE)

Research Organization:: 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 Organization:: National Natural Science Foundation of China (NNSFC); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; SC0016568

OSTI ID:: 1566498

Alternate ID(s):: OSTI ID: 1656505

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 7 Vol. 53; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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