Eu(Ⅲ)在蒙脱石上的吸附及碳酸根和磷酸根对其吸附的影响

doi:10.3866/PKU.WHXB202003031

Abstract

Abstract:

The environmental behaviours of actinides and fission products have been highly concerned due to their potential risks to human beings after entering the body through inhalation or food chains. The chemical reactions of actinides and fission products at mineral-water interface are the most important factors influencing the sorption, diffusion, migration and other processes of actinides and fission products in natural environments. Therefore, it is of great importance to investigate the chemical behaviours of these radioactive elements or nuclides in terms of environmental safety, especially in the area of safety assessment for geological disposal of high level radioactive wastes. However, the chemical behaviours of nuclides at mineral-water interface are complex and the investigations at a molecular level are challenging. To understand the chemical behaviours of trivalent actinides An(Ⅲ) in depth, non-radioactive Eu(Ⅲ) is used as an analogue of An(Ⅲ) due to their similar ionic sizes and chemical characteristics. In this study, batch sorption experiments and spectroscopic characterization methods were used to study the surface sorption species of Eu(Ⅲ) on montmorillonite and possible sorption mechanisms. We studied the effects of solid-liquid ratio, contacting time, ionic strength, pH, carbonate and phosphate on Eu(Ⅲ) sorption on montmorillonite. Our results indicated that the sorption percentage of Eu(Ⅲ) on montmorillonite was low in the range of pH 3.0 to 6.0, and much higher in the range of pH 7.0 to 10.0. The increase of ionic strength inhibited the sorption of Eu(Ⅲ) at low pH values, suggesting that the sorption of Eu(Ⅲ) on montmorillonite was mainly outer-sphere complexation in low pH conditions. Based on the results of fluorescence analysis, we can conclude that the sorption of Eu(Ⅲ) on montmorillonite is mainly outer-sphere complexation in low pH conditions, inner-sphere complexation in neutral pH conditions and surface induced precipitations in high pH conditions. Furthermore, we studied the sorption behaviours of Eu(Ⅲ) not only in montmorillonite/Eu(Ⅲ) binary system but also in montmorillonite/Eu(Ⅲ)/anion ternary system. Our results indicated that carbonate and phosphate could also influence the sorption of Eu(Ⅲ). Carbonate did not have an obvious influence on the sorption amount of Eu(Ⅲ), but it helped to change the surface sorption species of Eu(Ⅲ) on montmorillonite in high pH conditions. As for phosphate, although the sorption of phosphate onto montmorillonite was very weak, it could significantly enhance the sorption of Eu(Ⅲ) on montmorillonite. Because there were no reference data about fluorescence lifetime of Eu(Ⅲ)-phosphate species, we did XPS measurements and phosphate sorption experiments to find out the reason for phosphate enhancing effect. Our results proved that Eu(Ⅲ) precipitated as EuPO₄ on the surface of montmorillonite resulting in the enhancement of Eu(Ⅲ) sorption. This work is expected to provide a deeper understanding of the chemical behaviours of trivalent actinides An(Ⅲ) at mineral-water interface and predict the migration of An(Ⅲ) in the environment.

Key words: Mineral-water interface, Sorption, Fluorescence, Surface complexation, Precipitation

MSC2000:

O647

Mingkai Chang, Na Hu, Yao Li, Dongfan Xian, Wanqiang Zhou, Jingyi Wang, Yanlin Shi, Chunli Liu. Sorption of Eu(Ⅲ) on Montmorillonite and Effects of Carbonate and Phosphate on Its Sorption[J].Acta Phys. -Chim. Sin., 2022, 38(3): 2003031.

Figures/Tables 17

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References 35

1	Tian W. Y. ; Li C. ; Liu X. Y. ; Wang L. H. ; Zheng Z. ; Wang X. Y. ; Liu C. L. J. Radioanal. Nucl. Chem. 2013, 295, 1423. doi: 10.1007/s10967-012-2284-y
2	Dong Y. H. ; Liu Z. J. ; Li Y. Y. J. Radioanal. Nucl. Chem. 2011, 289, 257. doi: 10.1007/s10967-011-1072-4
3	Qi L. Y. ; Yang X. Y. ; Wang C. L. ; Zhou W. Q. ; Liu C. L. J. Nucl. Radiochem. 2018, 40, 112.
	齐立也; 杨小雨; 王春丽; 周万强; 刘春立. 核化学与放射化学, 2018, 40, 112. doi: 10.7538/hhx.2017.YX.2017016
4	Bruno J. ; Ewing R. C. Elements 2006, 2, 343. doi: 10.2113/gselements.2.6.343
5	Seaborg G. T. Radiochim. Acta 1993, 61, 115. doi: 10.1524/ract.1993.61.34.115
6	Rabung T. ; Stumpf T. ; Geckeis H. ; Klenze R. ; Kim J. I. Radiochim. Acta 2000, 88, 711. doi: 10.1524/ract.2000.88.9-11.711
7	McCarthy J. F. ; Sanford W. E. ; Stafford P. L. Environ. Sci. Technol. 1998, 32, 3901. doi: 10.1021/es971004f
8	Liatsou I. ; Efstathiou M. ; Pashalidis I. J. Radioanal. Nucl. Chem. 2015, 304, 41. doi: 10.1007/s10967-014-3448-8
9	Fan Q. H. ; Tan X. L. ; Li J. X. ; Wang X. K. ; Wu W. S. ; Montavon G. Environ. Sci. Technol. 2009, 43, 5776. doi: 10.1021/es901241f
10	Jin Q. ; Wang G. ; Ge M. T. ; Chen Z. Y. ; Wu W. S. ; Guo Z. J. Appl. Geochem. 2014, 47, 17. doi: 10.1016/j.apgeochem.2014.05.004
11	Bradbury M. H. ; Baeyens B. ; Geckeis H. ; Rabung T. Geochim. Cosmochim. Acta 2005, 69, 5403. doi: 10.1016/j.gca.2005.06.031
12	Geckeis H. ; Lutzenkirchen J. ; Polly R. ; Rabung T. ; Schmidt M. Chem. Rev. 2013, 113, 1016. doi: 10.1021/cr300370h
13	Xu X. Y. ; Liao Y. Q. ; Sun J. C. ; Wang X. H. ; Chen S. Q. ; Lv Z. ; Song J. Q. Acta Phys. -Chim. Sin. 2019, 35, 317.
	徐向宇; 廖艳清; 孙建川; 王旭辉; 陈帅奇; 吕志; 宋家庆. 物理化学学报, 2019, 35, 317. doi: 10.3866/PKU.WHXB201805021
14	Chen Z. Y. ; Zhang R. ; Yang X. L. ; Wu W. S. ; Guo Z. J. ; Liu C. L. Acta Phys. -Chim. Sin. 2013, 29, 2019.
	陈宗元; 张瑞; 杨兴龙; 吴王锁; 郭治军; 刘春立. 物理化学学报, 2013, 29, 2019. doi: 10.3866/PKU.WHXB201306271
15	Wen X. ; Wu Y. ; Su J. ; Zhang Y. ; Liu F. Environ. Geol. 2005, 48, 665. doi: 10.1007/s00254-005-0001-7
16	Wu P. ; Tang C. ; Zhu L. ; Liu C. ; Cha X. ; Tao X. Hydrol. Processes 2009, 23, 2012. doi: 10.1002/hyp.7332
17	Pernet-Coudrier B. ; Qi W. ; Liu H. ; Mueller B. ; Berg M. Environ. Sci. Technol. 2012, 46, 5294. doi: 10.1021/es3004415
18	Zhou Q. X. ; Gibson C. E. ; Zhu Y. M. Chemosphere 2001, 42, 221. doi: 10.1016/s0045-6535(00)00129-6
19	Dejneka M. ; Snitzer E. ; Riman R. E. J. Lumin. 1995, 65, 227. doi: 10.1016/0022-2313(95)00073-9
20	Zhang B. B. ; Miao M. Y. ; Bai J. ; Yuan G. J. ; Jia Y. Y. ; Han Z. X. ; Zhao Z. G. ; Su H. Q. Adv. Mater. Res. 2014, 962, 809. doi: 10.4028/www.scientific.net/AMR.962-965.809
21	Myllykyla E. ; Tanhua-Tyrkko M. ; Bouchet A. ; Tiljander M. Clay Miner. 2013, 48, 295. doi: 10.1180/claymin.2013.048.2.11
22	Kinniburgh, D.; Cooper, D. PhreePlot, version 1; Phreeplot Inc.: Bangor, Gwynedd, UK, 2011.
23	Plancque G. ; Maurice Y. ; Moulin V. ; Toulhoat P. ; Moulin C. Appl. Spectrosc. 2005, 59, 432. doi: 10.1366/0003702053641540
24	Pan D. Q. ; Fan F. Y. ; Wang Y. C. ; Li P. ; Hu P. Z. ; Fan Q. H. ; Wu W. S. Chem. Eng. J. 2017, 330, 559. doi: 10.1016/j.cej.2017.07.184
25	Tertre E. ; Berger G. ; Simoni E. ; Castet S. ; Giffaut E. ; Loubet M. ; Catalette H. Geochim. Cosmochim. Acta 2006, 70, 4563. doi: 10.1016/j.gca.2006.06.1568
26	Rabung T. ; Pierret M. C. ; Bauer A. ; Geckeis H. ; Bradbury M. H. ; Baeyens B. Geochim. Cosmochim. Acta 2005, 69, 5393. doi: 10.1016/j.gca.2005.06.030
27	Horrocks W. D. ; Sudnick D. R. J. Am. Chem. Soc. 1979, 101, 334. doi: 10.1021/ja00496a010
28	Plancque G. ; Moulin V. ; Toulhoat P. ; Moulin C. Anal. Chim. Acta 2003, 478, 11. doi: 10.1016/s0003-2670(02)01486-1
29	Kowal-Fouchard A. ; Drot R. ; Simoni E. ; Marmier N. ; Fromage F. ; Ehrhardt J. J. New J. Chem. 2004, 28, 864. doi: 10.1039/b400306c
30	Hartmann E. ; Baeyens B. ; Bradbury M. H. ; Geckeis H. ; Stumpft T. Environ. Sci. Technol. 2008, 42, 7601. doi: 10.1021/es801092f
31	Ishida K. ; Saito T. ; Aoyagi N. ; Kimura T. ; Nagaishi R. ; Nagasaki S. ; Tanaka S. J. Colloid Interface Sci. 2012, 374, 258. doi: 10.1016/j.jcis.2012.01.060
32	Takahashi Y. ; Kimura T. ; Kato Y. ; Minai Y. ; Tominaga T. Radiochim. Acta 1998, 82, 227.
33	Lochhead M. J. ; Bray K. L. Chem. Mater. 1995, 7, 572. doi: 10.1021/cm00051a019
34	Ford R. G. ; Scheinost A. C. ; Sparks D. L. Adv. Agron. 2001, 74, 41. doi: 10.1016/s0065-2113(01)74030-8
35	Oday P. A. ; ChisholmBrause C. J. ; Towle S. N. ; Parks G. A. ; Brown G. E. Geochim. Cosmochim. Acta 1996, 60, 2515. doi: 10.1016/0016-7037(96)00114-7

Composition	SiO₂	Al₂O₃	Fe₂O₃	CO₂	MgO	Na₂O	CaO	K₂O	SO₃	P₂O₅
w/%	61.3	21.4	5.45	3.93	2.34	2.00	1.81	0.679	0.550	0.201

pH	Lifetime/μs
5.0	65.0 ± 0.6 *
6.0	76.1 ± 1.0
7.0	139.6 ± 1.6
8.0	117.8 ± 3.0; 22.8 ± 0.3
9.0	18.2 ± 0.2
10.0	12.3 ± 0.2

pH	Lifetime/μs
6.0	66.1 ± 0.6 *
7.0	267.5 ± 0.7
8.0	161.7 ± 2.8; 47.7 ± 0.7
9.0	46.3 ± 0.2
10.0	53.1 ± 1.6

pH	Lifetime/μs
5.0	199.3 ± 1.7 *
6.0	215.1 ± 1.6
7.0	267.6 ± 1.3
8.0	269.0 ± 1.2
9.0	279.7 ± 1.1
10.0	284.9 ± 1.3

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Sorption of Eu(Ⅲ) on Montmorillonite and Effects of Carbonate and Phosphate on Its Sorption

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