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Appendix A. Supplementary data for Effective Capture of Aqueous Uranium from Saline Lake with Magnesium-based Binary and Ternary Layered Double Hydroxides Jingwei Tu a,b , Xiaoqian Peng a,b , Shuting Wang a,b , Chen Tian a,b,* , Hong Deng a,b , Zhi Dang a , Guining Lu a , Zhenqing Shi a , Zhang Lin a,b a School of Environment and Energy, The Key Laboratory of Pollution Control and Ecosystem Restoration in Industry Clusters (Ministry of Education), South China University of Technology, Guangzhou, Guangdong 510006, China b Guangdong Engineering and Technology Research Center for

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Page 1: ars.els-cdn.com · Web viewSynthesis of a hydrotalcite-like compound from oil shale ash and its application in uranium removal. Colloid Surf. A-Physicochem. Eng. …

Appendix A. Supplementary data for

Effective Capture of Aqueous Uranium from Saline Lake with Magnesium-based

Binary and Ternary Layered Double Hydroxides

Jingwei Tu a,b, Xiaoqian Peng a,b, Shuting Wang a,b , Chen Tian a,b,*, Hong Deng a,b, Zhi

Dang a, Guining Lu a, Zhenqing Shi a, Zhang Lin a,b

a School of Environment and Energy, The Key Laboratory of Pollution Control and

Ecosystem Restoration in Industry Clusters (Ministry of Education), South China

University of Technology, Guangzhou, Guangdong 510006, China

b Guangdong Engineering and Technology Research Center for Environmental

Nanomaterials, South China University of Technology, Guangzhou, Guangdong

510006, China

Submitted to Science of the Total Environment

*Corresponding author

E-mail: [email protected] (Dr. Chen Tian)

Content

Supplemental Materials and Experiments

12 pages, 7 figures, 5 tables

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Table S1

Isotherm parameters of U(VI) adsorption by MgAl-LDH and MgAlFe-LDH for

Freundlich simulation.

MgAl-LDH MgAlFe-LDH

U(VI)Kf

(mg g-1)

n R2Kf

(mg g-1)

n R2

Whole 126.43 2.81 0.945 186.94 2.09 0.932

part A 580.22 1.95 0.9569 976.42 1.33 0.992

part B 151.52 4.06 0.9348 169.03 3.50 0.931

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Table S2

Comparison of the distribution coefficient value (Kd) of MgAl-LDH and MgAlFe-

LDH with other adsorbents.

MaterialExperimental

conditionsKd (L g-1) References

MgFeAl LDH T = 298 K, pH = 5.0 96.63 (Song et al.,

2018)

NiFeAl LDH T = 298 K, pH = 5.0 3.00 (Song et al.,

2018)

rGO/LDH T = 298 K, pH = 5.0 234.67 (Tan et al.,

2015)

HTlca T = 298 K, pH = 4.0 53.23 (Zhang et al.,

2014)

Fe3O4@C@Ni-Al LDH T = 298 K, pH = 6.0 19.55 (Zhang et al.,

2013)

magnetic citrate MgAl LDH T = 298 K, pH = 6.0 4.88 (Zhang et al.,

2012)

clinoptilolite zeolite T = 298 K, pH = 6.0 62.50 (Camacho et

al., 2010)

Saccharomyces cerevisiae T = 298 K, pH = 6.0 13.23 (Bai et al.,

2016)

amidoximated silica T = 298 K, pH = 5.0 5.72 (Yin et al.,

2017)

Page 4: ars.els-cdn.com · Web viewSynthesis of a hydrotalcite-like compound from oil shale ash and its application in uranium removal. Colloid Surf. A-Physicochem. Eng. …

Oxime-mesoporous carbon T = 298 K, pH = 4.5 1.24 (Tian et al.,

2011)

talc T = 298 K, pH = 4.5 0.28 (Sprynskyy et

al., 2011)

POP-oNH2-AO T = 298 K, pH = 6.0 Around

8.36 × 106

(Sun et al.,

2018)

MgAl-LDH T = 298 K, pH = 6.0 377.31 This work

MgAlFe-LDH T = 298 K, pH = 6.0 434.78 This work

Page 5: ars.els-cdn.com · Web viewSynthesis of a hydrotalcite-like compound from oil shale ash and its application in uranium removal. Colloid Surf. A-Physicochem. Eng. …

Table S3

Kinetic parameters of U(VI) adsorption by MgAl-LDH and MgAlFe-LDH

sorbent

Pseudo-first-order model Pseudo-second-order model

Qe

(mg g−1 )

k1

(min−1)R2

Qe

(mg g−1)

k2

(g mg−1 min−1)R2

MgAl-LDHs 4.849 0.01168 0.9723 22.13 0.008540 0.9995

MgAlFe-LDHs 3.813 0.008797 0.8330 23.07 0.01032 0.9996

Table S4

Specific surface areas and pore parameters of MgAl-LDH and MgAlFe-LDH

samples

Surface

area(m2/g)a

Pore diameter

(nm)b

Pore volume

(cm3/g)b

MgAl-LDH 90.0114 36.74247 0.826810

MgAlFe-LDH 132.1487 30.25010 0.999378

a Performed by multipoint BET method.

b Cumulative desorption pore volume and average pore diameter performed by BJH method.

Page 6: ars.els-cdn.com · Web viewSynthesis of a hydrotalcite-like compound from oil shale ash and its application in uranium removal. Colloid Surf. A-Physicochem. Eng. …

Table S5

Desorption yields of some desorptive solutions.

EluantConcentration

(mol L-1)

Desorption efficiency for

MgAl-LDH

(%)

Desorption efficiency for

MgAlFe-LDH

(%)

H2O - 6.35 5.15

NaOH 0.5 23.29 23.19

Na2CO3 0.5 41.59 52.99

HCl 0.5 87.4 93.81

Page 7: ars.els-cdn.com · Web viewSynthesis of a hydrotalcite-like compound from oil shale ash and its application in uranium removal. Colloid Surf. A-Physicochem. Eng. …

Fig. S1 TGA curves of as-prepared MgAl-LDH and MgAlFe-LDH samples.

100 200 300 400 500 600 700 800 90050

60

70

80

90

100

110M

ass (

%)

Temperature ( )℃

MgAlFe-LDH MgAl-LDH

Page 8: ars.els-cdn.com · Web viewSynthesis of a hydrotalcite-like compound from oil shale ash and its application in uranium removal. Colloid Surf. A-Physicochem. Eng. …

Fig. S2 The Fredundlich fitting for U(VI) adsorption in part A (C0=0.2 mg L-1 to 5 mg

L-1) , part B (C0=5 mg L-1 to 30 mg L-1).

Page 9: ars.els-cdn.com · Web viewSynthesis of a hydrotalcite-like compound from oil shale ash and its application in uranium removal. Colloid Surf. A-Physicochem. Eng. …
Page 10: ars.els-cdn.com · Web viewSynthesis of a hydrotalcite-like compound from oil shale ash and its application in uranium removal. Colloid Surf. A-Physicochem. Eng. …

Fig. S3 U(VI) adsorption and desorption percentages in 5 consecutive cycles for

MgAl-LDH and MgAlFe-LDH.

90

92

94

96

98

100

102

54321

uran

ium

rem

oval

rat

e (%

)

cycles

MgAl-LDH MgAlFe-LDH

Page 11: ars.els-cdn.com · Web viewSynthesis of a hydrotalcite-like compound from oil shale ash and its application in uranium removal. Colloid Surf. A-Physicochem. Eng. …

Fig. S4 Effect of initial pH on adsorption property of MgAl-LDH and MgAlFe-LDH.

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Fig. S5 Species distribution of U(VI) species without precipitation as a function of

Page 13: ars.els-cdn.com · Web viewSynthesis of a hydrotalcite-like compound from oil shale ash and its application in uranium removal. Colloid Surf. A-Physicochem. Eng. …

pH. C0 = 0.5 mg L-1, T = 25 .℃

Fig. S6 Zeta potentials of LDHs at pH= 6-9.

Fig. S7 FT-IR spectra of MgAl-LDH and MgAlFe-LDH samples after U(VI) sorption.

Page 14: ars.els-cdn.com · Web viewSynthesis of a hydrotalcite-like compound from oil shale ash and its application in uranium removal. Colloid Surf. A-Physicochem. Eng. …

ReferencesBai, J., Yin, X., Zhu, Y., Fan, F., Wu, X., Tian, W., Tan, C., Zhang, X., Wang, Y., Cao, S., Fan, F., Qin, Z., Guo, J., 2016. Selective uranium sorption from salt lake brines by amidoximated Saccharomyces cerevisiae. Chem. Eng. J. 283, 889-895.Camacho, L.M., Deng, S., Parra, R.R., 2010. Uranium removal from groundwater by natural clinoptilolite zeolite: Effects of pH and initial feed concentration. J. Hazard. Mater. 175, 393-398.Song, S., Yin, L., Wang, X., Liu, L., Huang, S., Zhang, R., Wen, T., Yu, S., Fu, D., Hayat, T., Wang, X., 2018. Interaction of U(VI) with ternary layered double hydroxides by combined batch experiments and spectroscopy study. Chem. Eng. J. 338, 579-590.Sprynskyy, M., Kowalkowski, T., Tutu, H., Cukrowska, E.M., Buszewski, B., 2011. Adsorption performance of talc for uranium removal from aqueous solution. Chem. Eng. J. 171, 1185-1193.Sun, Q., Aguila, B., Perman, J., Ivanov, A.S., Bryantsev, V.S., Earl, L.D., Abney, C.W., Wojtas, L., Ma, S., 2018. Bio-inspired nano-traps for uranium extraction from seawater and recovery from nuclear waste. Nat. Commun. 9, 1644.Tan, L., Wang, Y., Liu, Q., Wang, J., Jing, X., Liu, L., Liu, J., Song, D., 2015. Enhanced adsorption of uranium (VI) using a three-dimensional layered double hydroxide/graphene hybrid material. Chem. Eng. J. 259, 752-760.Tian, G., Geng, J., Jin, Y., Wang, C., Li, S., Chen, Z., Wang, H., Zhao, Y., Li, S., 2011. Sorption of uranium(VI) using oxime-grafted ordered mesoporous carbon CMK-5. J. Hazard. Mater. 190, 442-450.Yin, X., Bai, J., Tian, W., Li, S., Wang, J., Wu, X., Wang, Y., Fan, F., Huang, Q., Qin, Z., 2017. Uranium sorption from saline lake brine by amidoximated silica. J. Radioanal. Nucl. Ch. 313, 113-121.Zhang, H., Wang, J., Zhang, B., Liu, Q., Li, S., Yan, H., Liu, L., 2014. Synthesis of a hydrotalcite-like compound from oil shale ash and its application in uranium removal. Colloid Surf. A-Physicochem. Eng. Asp. 444, 129-137.Zhang, X., Ji, L., Wang, J., Li, R., Liu, Q., Zhang, M., Liu, L., 2012. Removal of uranium(VI) from aqueous solutions by magnetic Mg–Al layered double hydroxide intercalated with citrate: Kinetic and thermodynamic investigation. Colloid Surf. A-Physicochem. Eng. Asp. 414, 220-227.Zhang, X., Wang, J., Li, R., Dai, Q., Gao, R., Liu, Q., Zhang, M., 2013. Preparation of Fe3

O4@C@Layered Double Hydroxide Composite for Magnetic Separation of Uranium. Ind. Eng. Chem. Res. 52, 10152-10159.