Efficient U(VI) Reduction and Sequestration by Ti2CTx MXene

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

doi:10.1021/acs.est.8b03711

Efficient U(VI) Reduction and Sequestration by Ti₂CT_x MXene

Journal Article · Mon Aug 27 00:00:00 EDT 2018 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.8b03711· OSTI ID:1566346

^[1]; Song, Huan ^[2]; ^[1]; Li, Zijie ^[1]; Zhang, Yujuan ^[3]; ^[4]; Zheng, Lirong ^[1]; Chai, Zhifang ^[1]; ^[1]

Chinese Academy of Sciences (CAS), Beijing (China)
Chinese Academy of Sciences (CAS), Beijing (China); Univ. of South China, Hengyang (China)
Univ. of Science and Technology, Beijing (China)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Although reduction of highly mobile U(VI) to less soluble U(IV) has been long considered an effective approach to in situ environmental remediation of uranium, candidate reducing agents are largely limited to Fe-based materials and microbials. The importance of titanium-containing compounds in natural uranium ore deposits suggests a role for titanium in uranium migration. In this report, for the first time, a two-dimensional transition metal carbide, Ti₂CT_x, is shown to efficiently remove uranium via a sorption-reduction strategy. Batch experiments demonstrate that Ti₂CT_x exhibits excellent U(VI) removal over a wide pH range, with an uptake capacity of 470 mg g^–1 at pH 3.0. The mechanism for U(VI) to U(IV) reduction by Ti₂CT_x was deciphered by X-ray absorption spectroscopy and diffraction and photoelectron spectroscopy. The reduced U(IV) species at low pH is identified as mononuclear with bidendate binding to the MXene substrate. At near-neutral pH, nanoparticles of the UO_2+x phase adsorb to the substrate with some Ti₂CT_x transformed to amorphous TiO₂. A subsequent in-depth study suggests Ti₂CT_x materials may be potential candidates for permeable reactive barriers in the treatment of wastewaters from uranium mining. Finally, this work highlights reduction-induced immobilization of U(VI) by Ti₂CT_x MXene including a pH-dependent reduction mechanism that might promote applications of titanium-based materials in the elimination of other oxidized contaminants.

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)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0016568

OSTI ID:: 1566346

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 18 Vol. 52; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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