Efficient U(VI) Reduction and Sequestration by Ti 2 CT x MXene

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1 Supporting Information for Efficient U(VI) Reduction and Sequestration by Ti 2 CT x MXene Lin Wang, 1 Huan Song, 1,2 Liyong Yuan, 1 Zijie Li, 1 Yujuan Zhang, 3 John K. Gibson, 4 Lirong Zheng, 5 Zhifang Chai 1 and Weiqun Shi* 1 1. Laboratory of Nuclear Energy Chemistry and Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing , China. 2. School of Chemistry and Chemical Engineering, University of South China, Hengyang , China. 3. School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing , China. 4. Chemical Sciences Division, Lawrence Berkeley National Laboratory (LBNL), Berkeley, California 94720, United States. 5. Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing , China. *Corresponding Authors: shiwq@ihep.ac.cn Pages: 10 Figures: 10 Tables: 2 S-1

2 Sorption data fitting by kinetics models In order to clarify the sorption process of U(VI) by V 2 CT x, the pseudo-first-order kinetic model and the pseudo-second-order kinetic model were used to analyze the experimentally observed kinetic data. The linearized form of the two models are given as follows: 1,2 k1 log( qe qt ) log qe t (S1) t 1 t (S2) 2 q k q q t 2 e e where q e (mg/g) and q t (mg/g) are the quantities of the sorbed U(VI) at equilibrium at time t respectively, k l (1/min) and k 2 (g/(mg min)) are the pseudo-first-order and pseudo-second-order sorption rate constants. The plot of log(q e q t ) versus t and t/q t versus t give straight line, and k 1 and k 2 can be calculated from the slope. The model parameters and the correlation coefficient obtained by both the models are listed in Table S2. S-2

$U(IV) and U(VI) fractions in totally removed uranium by Ti 2$

3 Figures: Figure S1. XRD pattern (A) and SEM images (B-D) of S-Ti 2 CT x. Figure S2. U(IV) and U(VI) fractions in totally removed uranium by Ti 2 CT x at different time intervals. C 0 = 200 mg L -1, ph = 3.0±0.1, m sorbent /V solution = 0.4 g L -1. S-3

4 Figure S3. Competing removal experiments of U(VI) and Th(IV) as a function of contact time at different ambient conditions. C 0 [U] = C 0 [Th] = 200 mg L -1, ph = 3.0±0.1, m sorbent /V solution = 0.4 g L -1. S-4

5 Figure S4. Re(VII) removal from aqueous solution by multilayered Ti 2 CT x as a function of contact time. C 0 = 200 mg L -1, ph = 4.0±0.1, m sorbent /V solution = 0.4 g L -1. Figure S5. SEM image and EDS spectrum of multilayered Ti 2 CT x after Re(VII) removal. S-5

6 Figure S6. TEM images of M-Ti 2 CT x -ph5.0 (A, B) and M-Ti 2 CT x -ph8.0(c, D). S-6

7 Figure S7. High-resolution O 1s XPS spectra of multilayered Ti 2 CT x before and after U(VI) removal. Figure S8. Raman spectra of Ti 2 CT x samples before and after U(VI) reduction. The standard Raman spectrum of TiO 2 reference is also shown on the bottom. S-7

8 Figure S9. Removal of U(VI) from simulated acid mine waste water by Ti 2 CT x at different concentration of competing metal cations. C 0 = 20 mg L -1, m sorbent /V solution = 1 g L -1. C 1 =10.8 mmol L -1 Al 2 (SO 4 ) 3, 1.08 mmol L -1 Ca(NO 3 ) 2, 0.72 mmol L -1 MgSO 4, 2.88 mmol L -1 Na 2 SO 4 and 2.88 mmol L -1 (NH 4 ) 2 SO 4. [Fe 3+ ] = 0.8 mmol L -1. Figure S10. XRD pattern of oxidation product of Ti 2 CT x in simulated uranium-contaminated acid mine waste water after exposing to air for one month. S-8

9 Tables Table S1. Influence of Na 2 CO 3 on U(VI) removal efficiency by Ti 2 CT x. 1 mm Na 2 CO 3 a 10 mm Na 2 CO 3 a ph (U+Na2CO3) ph contacting with Ti2CTx ph final Removal percent (%) 99 7 a m sorbent /V solution = 0.1 g L -1, C 0 = 33.7 mg L -1. Table S2. Kinetics model constants and correlation coefficients for U(VI) removal by Ti 2 CT x. Kinetics model Pseudo-first-order Pseudo-second-order q e (mg/g) k 1 (h 1 ) R 2 q e (mg/g) k 2 (g mg -1 h -1 ) R 2 Saturation capacity from experiment (mg/g) S-9

10 References (1) Lagergren, S. About the Theory of So-called Adsorption of Soluble Substances; Kungl. Svenska Vetenskapsakademiens Handlingar 1898; Vol. 24. (2) Sureshkumar, M. K.; Das, D.; Mallia, M. B.; Gupta, P. C. Adsorption of Uranium from Aqueous Solution Using Chitosan-tripolyphosphate (CTPP) Beads. J. Hazard. Mater. 2010, 184, S-10

MOF-76: From Luminescent Probe to Highly Efficient U VI Sorption Material

MOF-76: From Luminescent Probe to Highly Efficient U VI Sorption Material Weiting Yang, a Zhi-Qiang Bai, b Wei-Qun Shi*, b Li-Yong Yuan, b Tao Tian, a Zhi-Fang Chai*, c Hao Wang, a and Zhong-Ming Sun*