In cooperation with the Iranian Nuclear Society

Document Type : Research Paper

Authors

Nuclear Fuel Cycle Research School, Nuclear Science and Technology Research Institute, AEOI, P.O.Box: 11365-8486, Tehran-Iran

Abstract

In the present study, the uranium recovery by utilizing the bulk liquid membrane which contains Alamine 336 has been investigated. The effect of uranium and sulfuric acid concentration in the donor phase, carrier concentration in the liquid membrane phase, and ammonium carbonate concentration in the acceptor phase and transport kinetics were studied. The optimum conditions of uranium transport were obtained at 0.15 mol.L-1 H2SO4 in donor phase, 0.5 mol.L-1 (NH4)2CO3 in the acceptor phase, 0.0125 mol.L-1 Alamine 336 in kerosene. The results demonstrated that by increasing the concentration of sulfuric acid up to 0.15 mol.L-1  and the Alamine 336 concentration to 0.0125 mol.L-1, the uranium transfer will increase and then decrease. The uranium transfer was decreased with an increment in initial uranium concentration. Studying the effect of time on the uranium transfer showed that the cause of rate-controlling is the release of uranyl from the liquid membrane phase to the acceptor phase. The kinetics of uranium transport was modeled assuming consecutive irreversible pseudo-first-order reactions. The extraction rate constant of 0.0061 min-1 and 0.0107 min-1 and the stripping rate constant of 5.56×10-4 and 12× 10-4 min-1 were obtained for liquid membrane containing Alamine 336 and sulfated Alamine 336, respectively.

Highlights

1.  M.E. Nasab, Solvent extraction separation of uranium (VI) and thorium (IV) with neutral organophosphorus and amine ligands, Fuel‌ 116 (2014) 595-600.

 

2.     V.‌Opratko, Purification of yellow cake, U.S. Patent No. (1965) 174-821.

 

3.    K.‌Chakrabarty, Liquid membrane based technology for removal of pollutants from wastewater, Doctor of philosophy thesis from IIT Guwahati (2010).

 

4.   ‌I. Diaconu et al. Analytical applicationsof transport through bulk liquid membranes, Cri. Rev. Anal. Chem. 46 (2016) 332-341.

 

5.     G. Muthuraman et al. Use of bulk liquid membrane for the removal of chromium (VI) from aqueous acidic solution with tri-n-butyl phosphate as a carrier, Desalination 249 (2009) 884-890.

 

6.     G. León and M.A. Guzmán, Facilitated transport of cobalt through bulk liquid membranes containing D2EHPA as carrier. Kinetic study of the influence of some operational variables, Des. Water Treat. 13 (2010) 267-273.

 

7.   A. Dinkar et al. Carrier mediated transport of thorium from nitric acid medium using 2-ethyl hexyl hydrogen 2-ethyl hexyl phosphonate (PC88A)/N-dodecane as carrier, Sep. Sci. Tech. 48 (2013) 728-735.

 

8.    S. Tarahomi et al. Selective transport of silver (I) cation across a bulk liquid membrane containing bis-β-enamino ester as ion carrier, J. Braz. Chem. Soc. 28 (2017) 68-75.

 

9.   T.T. Teng et al. Bulk liquid membrane and its applications in wastewater treatment, Wast. Eng. Adv. Wast. Treat. Sys. (2014) 158.

 

10.    M.M. Zahedi and S.M. Ghasemi, Separation study of Mg+2 from seawater and RO brine through a facilitated bulk liquid membrane transport using 18-Crown-6, J. Wat. Reu. Desalination (2016) 468-475.

 

11.  V. Ghaffari et al. The competitive and selective transport of metal cations through bulk liquid membrane by 5, 6,11,12-tetraphenyl-1,2,4,7, 8,10-hexa azo-cyclododeca-4,6,10,12-tetra-N-9,4-ditione and new synthesized phosphorus-nitrogen compound,(CF3C(O)NH)(C6H11NH)P(O)[NHCH2C‌(CH3)2CH2NH]P(O)(NHC6H11)(NHC(O)CF3), 19th Iranian Seminar of Analytical Chemistry (ISAC 19) (2013).

 

12.  M. Shamsipur, R. Davarkhah, and A.R. Khanchi, Facilitated transport of uranium (VI) across a bulk liquid membrane containing thenoyltrifluoroacetone in the presence of crown ethers as synergistic agents, Sep. Pur. Tech. 71 (2010) 63-69.

 

13.   M. Shamsipur et al. Selective facilitated transport of uranium (VI) across a bulk liquid membrane containing benzoyltrifluoroacetone as extractant-carrier, Sep. Sci. Tech 44 (2009) 2645-2660.

 

 

14.  R.‌Davarkhah et al. Kinetic studies on the extraction of uranium (VI) from phosphoric acid medium by bulk liquid membrane containing di-2-ethylhexyl phosphoric acid, J. Rad. Nuc. Chem. 298 (2013).

 

15.   J. Ramkumar, S. Nayak, and B. Maiti, Transport of uranyl ion across a bulk liquid membrane using calixarene and synergistic agents as carriers, J. mem. sci. 196 (2002) 203-210.

 

16.  D. Nanda et al. Selective and uphill transport of uranyl ion in the presence of some base metals and thorium across bulk liquid membrane by di (2-ethylhexyl) phosphoric acid, Sep. Sci. Tech. 37 (2002) 3357-3367.

 

17.   K. Južnič and Š. Fedina, The extraction of uranium (IV) from sulphuric acid by tri-octylamine in benzene, Micr. Acta 62 (1974) 39-44.

 

18.   S.J. Lyle and M. Tamizi, A study of equilibria in the extraction of uranium (VI) from aqueous sulphate solution by tri-n-octylamine in benzene or petroleum spirit, Hydrometallurgy 11 (1983) 1-11.

 

19.  J.R. Kumar  et al. Solvent extraction of uranium (VI) and separation of vanadium (V) from sulfate solutions using Alamine 336, J. Rad. Nuc. Chem. 285 (2010) 301-308.

 

20. J.R. Kumar et al. A brief review on solvent extraction of uranium from acidic solutions, Sep. Pur. Rev. 40 (2011) 77-125.

 

21.  F. Khanramaki et al. Equilibrium and kinetic of uranium (VI) extraction from a sulfate leach liquor solution by Alamine 336 using single drop technique, Chem. Eng. Res. Des. (2017).

 

22. F. Khanramaki et al. Investigation of liquid extraction and thermodynamic studies on uranium from sulfate solution by Alamine 336 as an extractant, Int.  J. Env.  Sci. Tech. (2017) 1-10.

 

23.   G. Ramadevi et al. Solvent extraction of uranium from lean grade acidic sulfate leach liquor with alamine 336 reagent, J. Rad. Nuc. Chem. 294 (2012) 13-18.

 

24.  C.-J. Kim et al. Solvent extraction studies on uranium using amine based extractants and recovery from low grade ore leach liquors, J.Braz. Chem. Soc. 23 (2012) 1254-1264.

 

25.  C. Morais et al. Uranium stripping from tertiary amine by sulfuric acid solution and its precipitation as uranium peroxide, Min. eng. 18 (2005) 1331-1333.

 

26. J. Rydberg, Solvent extraction principles and practice, revised and expanded, CRC Press (2004).

 

27.  ‌F. Hurst, and D. Crouse, Recovery of uranium from amine extractants with ammonium carbonate, in, Oak Ridge National Lab., Tenn (1961).

 

28. V. Pandey, A. Chakraborty, and N. Maity, Preparation of nuclear grade uranium oxide from Jaduguda leach liquor, (1991).

 

29. D.J. Crouse and K. Brown, Amine extraction processes for uranium recovery from sulfate liquors, Oak Ridge National Laboratory (1956).

 

30.   D. Crouse and  K. Brown, Amine extract processes for uranium recovery from sulfate liquors. VOL. I, Oak Ridge National Lab., Tenn. (1955).

 

31.  F. Zahakifar et al. Solvent extraction of uranium (VI) from leach liquor solution of Bandar Abbas Gachin ore using Alamine 336, Nuc. Sci. Tech. in Press (2017).

 

32.   É. Avelar et al. modeling of the solvent extraction equilibrium of uranium sulfate with Alamine 336, Braz. J. Chem. Eng. 34 (2017) 355-362.

 

33.  N. Yakubu and A. Dudeney, A study of uranium solvent extraction equilibria with alamine 336 in kerosene, Hydrometallurgy 18 (1987) 93-104.

 

34.   A. Yilmaz, et al. Kinetic analysis of chromium (VI) ions transport through a bulk liquid membrane containing p-tert-butylcalix [4] arene dioxaoctylamide derivative, Sep. Pur. Tech. 59 (2008) 1-8.

 

35.  I.H. Gubbuk et al. Kinetic study of mercury (II) transport through a liquid membrane containing calix [4] arene nitrile derivatives as a carrier in chloroform, Desalination 261 (2010) 157-161.

 

36.  W. Zhang et al. Kinetic study of chromium (VI) facilitated transport through a bulk liquid membrane using tri-n-butyl phosphate as carrier, Chem. Eng. J. 150 (2009) 83-89.

 

37.  A.Ö. Saf, S. Alpaydin, and A. Sirit, Transport kinetics of chromium (VI) ions through a bulk liquid membrane containing p-tert-butyl calix [4] arene 3-morpholino propyl diamide derivative, J. mem. sci. 283 (2006) 448-455.

 

38.   D. He, M. Ma, and Z. Zhao, Transport of cadmium ions through a liquid membrane containing amine extractants as carriers, J.  Mem. Sci. 169 (2000) 53-59.

 

39.  D. He and M. Ma, Kinetics of cadmium (II) transport through a liquid membrane containing tricapryl amine in xylene, Sep. Sci. Tech. 35 (2000) 1573-1585

 

40.   M. Ma et al. Kinetics of europium (III) transport through a liquid membrane containing HEH (EHP) in kerosene, Talanta 55 (2001) 1109-1117.

 

41.  C. Wilke and P. Chang, Correlation of diffusion coefficients in dilute solutions, AIChE J. 1 (1955) 264-270.

 

 

42.  W. Zhang et al. Simultaneous removal and recovery of copper (II) from acidic wastewater by hollow fiber renewal liquid membrane with LIX984N as carrier, Chem. Eng. J. 157 (2010) 230-237.

 

43.  S. Dadfarnia and M. Shamsipur, Highly selective membrane transport of Zn2+ ion by a cooperative carrier composed of 1, 10-diaza-18-crown-6 and palmitic acid, Bull. Chem. Soc. Jap. 65 (1992) 2779-2783.

Keywords

1.  M.E. Nasab, Solvent extraction separation of uranium (VI) and thorium (IV) with neutral organophosphorus and amine ligands, Fuel‌ 116 (2014) 595-600.
 
2.     V.‌Opratko, Purification of yellow cake, U.S. Patent No. (1965) 174-821.
 
3.    K.‌Chakrabarty, Liquid membrane based technology for removal of pollutants from wastewater, Doctor of philosophy thesis from IIT Guwahati (2010).
 
4.   ‌I. Diaconu et al. Analytical applicationsof transport through bulk liquid membranes, Cri. Rev. Anal. Chem. 46 (2016) 332-341.
 
5.     G. Muthuraman et al. Use of bulk liquid membrane for the removal of chromium (VI) from aqueous acidic solution with tri-n-butyl phosphate as a carrier, Desalination 249 (2009) 884-890.
 
6.     G. León and M.A. Guzmán, Facilitated transport of cobalt through bulk liquid membranes containing D2EHPA as carrier. Kinetic study of the influence of some operational variables, Des. Water Treat. 13 (2010) 267-273.
 
7.   A. Dinkar et al. Carrier mediated transport of thorium from nitric acid medium using 2-ethyl hexyl hydrogen 2-ethyl hexyl phosphonate (PC88A)/N-dodecane as carrier, Sep. Sci. Tech. 48 (2013) 728-735.
 
8.    S. Tarahomi et al. Selective transport of silver (I) cation across a bulk liquid membrane containing bis-β-enamino ester as ion carrier, J. Braz. Chem. Soc. 28 (2017) 68-75.
 
9.   T.T. Teng et al. Bulk liquid membrane and its applications in wastewater treatment, Wast. Eng. Adv. Wast. Treat. Sys. (2014) 158.
 
10.    M.M. Zahedi and S.M. Ghasemi, Separation study of Mg+2 from seawater and RO brine through a facilitated bulk liquid membrane transport using 18-Crown-6, J. Wat. Reu. Desalination (2016) 468-475.
 
11.  V. Ghaffari et al. The competitive and selective transport of metal cations through bulk liquid membrane by 5, 6,11,12-tetraphenyl-1,2,4,7, 8,10-hexa azo-cyclododeca-4,6,10,12-tetra-N-9,4-ditione and new synthesized phosphorus-nitrogen compound,(CF3C(O)NH)(C6H11NH)P(O)[NHCH2C‌(CH3)2CH2NH]P(O)(NHC6H11)(NHC(O)CF3), 19th Iranian Seminar of Analytical Chemistry (ISAC 19) (2013).
 
12.  M. Shamsipur, R. Davarkhah, and A.R. Khanchi, Facilitated transport of uranium (VI) across a bulk liquid membrane containing thenoyltrifluoroacetone in the presence of crown ethers as synergistic agents, Sep. Pur. Tech. 71 (2010) 63-69.
 
13.   M. Shamsipur et al. Selective facilitated transport of uranium (VI) across a bulk liquid membrane containing benzoyltrifluoroacetone as extractant-carrier, Sep. Sci. Tech 44 (2009) 2645-2660.
 
 
14.  R.‌Davarkhah et al. Kinetic studies on the extraction of uranium (VI) from phosphoric acid medium by bulk liquid membrane containing di-2-ethylhexyl phosphoric acid, J. Rad. Nuc. Chem. 298 (2013).
 
15.   J. Ramkumar, S. Nayak, and B. Maiti, Transport of uranyl ion across a bulk liquid membrane using calixarene and synergistic agents as carriers, J. mem. sci. 196 (2002) 203-210.
 
16.  D. Nanda et al. Selective and uphill transport of uranyl ion in the presence of some base metals and thorium across bulk liquid membrane by di (2-ethylhexyl) phosphoric acid, Sep. Sci. Tech. 37 (2002) 3357-3367.
 
17.   K. Južnič and Š. Fedina, The extraction of uranium (IV) from sulphuric acid by tri-octylamine in benzene, Micr. Acta 62 (1974) 39-44.
 
18.   S.J. Lyle and M. Tamizi, A study of equilibria in the extraction of uranium (VI) from aqueous sulphate solution by tri-n-octylamine in benzene or petroleum spirit, Hydrometallurgy 11 (1983) 1-11.
 
19.  J.R. Kumar  et al. Solvent extraction of uranium (VI) and separation of vanadium (V) from sulfate solutions using Alamine 336, J. Rad. Nuc. Chem. 285 (2010) 301-308.
 
20. J.R. Kumar et al. A brief review on solvent extraction of uranium from acidic solutions, Sep. Pur. Rev. 40 (2011) 77-125.
 
21.  F. Khanramaki et al. Equilibrium and kinetic of uranium (VI) extraction from a sulfate leach liquor solution by Alamine 336 using single drop technique, Chem. Eng. Res. Des. (2017).
 
22. F. Khanramaki et al. Investigation of liquid extraction and thermodynamic studies on uranium from sulfate solution by Alamine 336 as an extractant, Int.  J. Env.  Sci. Tech. (2017) 1-10.
 
23.   G. Ramadevi et al. Solvent extraction of uranium from lean grade acidic sulfate leach liquor with alamine 336 reagent, J. Rad. Nuc. Chem. 294 (2012) 13-18.
 
24.  C.-J. Kim et al. Solvent extraction studies on uranium using amine based extractants and recovery from low grade ore leach liquors, J.Braz. Chem. Soc. 23 (2012) 1254-1264.
 
25.  C. Morais et al. Uranium stripping from tertiary amine by sulfuric acid solution and its precipitation as uranium peroxide, Min. eng. 18 (2005) 1331-1333.
 
26. J. Rydberg, Solvent extraction principles and practice, revised and expanded, CRC Press (2004).
 
27.  ‌F. Hurst, and D. Crouse, Recovery of uranium from amine extractants with ammonium carbonate, in, Oak Ridge National Lab., Tenn (1961).
 
28. V. Pandey, A. Chakraborty, and N. Maity, Preparation of nuclear grade uranium oxide from Jaduguda leach liquor, (1991).
 
29. D.J. Crouse and K. Brown, Amine extraction processes for uranium recovery from sulfate liquors, Oak Ridge National Laboratory (1956).
 
30.   D. Crouse and  K. Brown, Amine extract processes for uranium recovery from sulfate liquors. VOL. I, Oak Ridge National Lab., Tenn. (1955).
 
31.  F. Zahakifar et al. Solvent extraction of uranium (VI) from leach liquor solution of Bandar Abbas Gachin ore using Alamine 336, Nuc. Sci. Tech. in Press (2017).
 
32.   É. Avelar et al. modeling of the solvent extraction equilibrium of uranium sulfate with Alamine 336, Braz. J. Chem. Eng. 34 (2017) 355-362.
 
33.  N. Yakubu and A. Dudeney, A study of uranium solvent extraction equilibria with alamine 336 in kerosene, Hydrometallurgy 18 (1987) 93-104.
 
34.   A. Yilmaz, et al. Kinetic analysis of chromium (VI) ions transport through a bulk liquid membrane containing p-tert-butylcalix [4] arene dioxaoctylamide derivative, Sep. Pur. Tech. 59 (2008) 1-8.
 
35.  I.H. Gubbuk et al. Kinetic study of mercury (II) transport through a liquid membrane containing calix [4] arene nitrile derivatives as a carrier in chloroform, Desalination 261 (2010) 157-161.
 
36.  W. Zhang et al. Kinetic study of chromium (VI) facilitated transport through a bulk liquid membrane using tri-n-butyl phosphate as carrier, Chem. Eng. J. 150 (2009) 83-89.
 
37.  A.Ö. Saf, S. Alpaydin, and A. Sirit, Transport kinetics of chromium (VI) ions through a bulk liquid membrane containing p-tert-butyl calix [4] arene 3-morpholino propyl diamide derivative, J. mem. sci. 283 (2006) 448-455.
 
38.   D. He, M. Ma, and Z. Zhao, Transport of cadmium ions through a liquid membrane containing amine extractants as carriers, J.  Mem. Sci. 169 (2000) 53-59.
 
39.  D. He and M. Ma, Kinetics of cadmium (II) transport through a liquid membrane containing tricapryl amine in xylene, Sep. Sci. Tech. 35 (2000) 1573-1585
 
40.   M. Ma et al. Kinetics of europium (III) transport through a liquid membrane containing HEH (EHP) in kerosene, Talanta 55 (2001) 1109-1117.
 
41.  C. Wilke and P. Chang, Correlation of diffusion coefficients in dilute solutions, AIChE J. 1 (1955) 264-270.
 
 
42.  W. Zhang et al. Simultaneous removal and recovery of copper (II) from acidic wastewater by hollow fiber renewal liquid membrane with LIX984N as carrier, Chem. Eng. J. 157 (2010) 230-237.
 
43.  S. Dadfarnia and M. Shamsipur, Highly selective membrane transport of Zn2+ ion by a cooperative carrier composed of 1, 10-diaza-18-crown-6 and palmitic acid, Bull. Chem. Soc. Jap. 65 (1992) 2779-2783.