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Separation of Uranium(VI) and Vanadium(V) from Sulfuric Acid Media by Amine Based Extractants through Liquid-liquid Extraction Technique

황산 용액으로부터 아민계 추출제의 액-액 추출법에 의한 우라늄(VI)과 바나듐(V)의 분리

  • Jeon, Jong-Hyuk (Korea Institute of Geoscience and Mineral Resources (KIGAM)) ;
  • Lee, Jin-Young (Korea Institute of Geoscience and Mineral Resources (KIGAM)) ;
  • Kim, Joon Soo (Institute of Research and Development, Wongwang Electric Power Corporation) ;
  • Yoon, Ho-Sung (Korea Institute of Geoscience and Mineral Resources (KIGAM)) ;
  • Jyothi, Rajesh Kumar (Korea Institute of Geoscience and Mineral Resources (KIGAM))
  • Received : 2021.07.28
  • Accepted : 2021.08.12
  • Published : 2021.08.31

Abstract

The importance of uranium metal is growing day by day in light of its increasing global demand for fulfilling societal needs through atomic power programs. Considering the high demand for uranium, it is necessary to find innovative hydrometallurgical techniques to separate uranium from other associated elements, especially vanadium. This study deals with the separation of uranium(VI) and vanadium(V) from sulfuric acid solutions using commercial amine-based extractants diluted in kerosene. The concentrations of the sulfuric acid solutions ranged from 0.005 to 5.0 mol/L. The effect of extractant concentration ranging from 0.005 to 0.2 mol/L was studied. The temperature was maintained at 25℃ and the experiment was performed for 30 min at an aqueous: organic phase ratio of 1 (A:O = 1:1). The calculated separation factors (SFs) are presented and comparisons are made among all the experiments.

원자력 발전 프로그램에 의해 세계 우라늄 메탈의 수요가 증가함에 따라 우라늄 메탈의 중요도는 날로 증가하고 있다. 이러한 우라늄 수요의 높은 증가로 인해 주로 바나듐을 비롯한 다른 원소들로부터 우라늄을 회수하고자 하는 새로운 추출법들이 더욱 중요하게 되었다. 본 연구에서는 kerosene에 희석된 상업용 아민 기반 추출제를 사용하여 황산 용액에서 우라늄(VI)과 바나듐(V)을 분리하는 방법을 다루었다. 0.005 ~ 5.0 mol/L농도의 황산 용액과 0.005 ~ 0.2 mol/L농도의 추출제를 사용하였다. 모든 실험은 25℃에서 30분동안 동일한 수상과 유기상의 비율(A:O = 1:1)로 수행하였다. 실험 결과 값으로부터 계산된 분리 계수(SF's)를 제시하고 모든 실험 값과 비교하였다.

Keywords

Acknowledgement

This work was supported by the Energy Efficiency and Resources (Physical and Chemical mineral dressing/refining of low grade uranium ore) of the Korea Institute of Energy Technology Evaluation and Planning (KETEP) grant funded by the Korea Government Ministry of Knowledge Economy. This work was supported by the National Research Council of Science & Technology (NST) grant by the Korean government (MSIT) (No.CRC-15-06-KIGAM). Thanks are also for Cognis Company, USA for providing all amine based extractants as gift samples. Authors are very much thankful to EMC 2011 for accepted the present data as oral presentation.

References

  1. Nigond, L., Musikas, C., Cuillerdier, C., 1994 : Extraction By N,N,N',N'-Tetraalkyl-2 Alkyl Propane-1,3 Diamides. I. H2O, HNO3 And HClO4, Solvent Extraction and Ion Exchange, 12(2), pp.261-296. https://doi.org/10.1080/07366299408918211
  2. Nair, G.M., Mahajan, G.R., Prabhu, D.R., 1995 : Extraction of uranium(VI) and plutonium(IV) with some high molecular weight aliphatic monoamides from nitric acid medium, Journal of Radioanalytical and Nuclear Chemistry, 191(2), pp.323-330. https://doi.org/10.1007/BF02038228
  3. Nair, G.M., Prabhu, D.R., Mahajan, G.R., 1994 : Methyl-butylmalonamide as an extractant for U(VI), Pu(IV) and Am(III), Journal of Radioanalytical and Nuclear Chemistry, 186(1), pp.47-55. https://doi.org/10.1007/BF02163241
  4. Nakamura, T., Miyake, C., 1995 : Extraction Of Lanthanide (III) And Uranyl(VI) From Nitric Acid Solution By N,N'-Dimethyl-N,N'-Dibutylmalonamide, Solvent Extraction and Ion Exchange, 13(2), pp.253-273. https://doi.org/10.1080/07366299508918273
  5. Preston, J.S., du Preez, A.C., 1995 : Solvent extraction of uranium(VI) and thorium(IV) from nitrate media by carboxylic acid amides, Solvent Extraction and Ion Exchange, 13(3), pp.391-413. https://doi.org/10.1080/07366299508918282
  6. Ruikar, P.B., Nagar, M.S., Subramanian, M.S., et al., 1995 : Extraction behavior of uranium(VI), plutonium(IV) and some fission products with gamma pre-irradiated n-dodecane solutions of N,N'-dihexyl substituted amides, Journal of Radioanalytical and Nuclear Chemistr, 196(1), pp.171-178. https://doi.org/10.1007/BF02036302
  7. Moore, F.L., 1958 : Liquid-Liquid Extraction of Uranium and Plutonium from Hydrochloric Acid Solution with Tri(iso-octyl)amine: Separation from Thorium and Fission Products, Analytical Chemistry, 30(5), pp.908-911. https://doi.org/10.1021/ac60137a012
  8. Juznic, K., Fedina, S., 1974 : The extraction of uranium (IV) from sulphuric acid by tri-octylamine in benzene, Microchimica Acta, 62(1), pp.39-44. https://doi.org/10.1007/BF01271414
  9. Goldenberg, J.F., Abbruzzese, C., 1983 : Extraction of uranium from heap leach liquor with tri-n-octylamine: Equilibrium data and flow-sheet calculations, International Journal of Mineral Processing, 10(4), pp.241-254. https://doi.org/10.1016/0301-7516(83)90015-7
  10. Lyle, S.J., Tamizi, M., 1983 : 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(1), pp.1-11. https://doi.org/10.1016/0304-386X(83)90012-9
  11. Ito, K., 1993 : Extraction of technetium(VII) from uranium (VI) in nitric acid system by primary amine - n-heptane solution, Journal of Radioanalytical and Nuclear Chemistry, 171(2), pp.371-382. https://doi.org/10.1007/BF02219861
  12. Behera, P., Mishra, R., Chakravortty, V., 1993 : Solvent extraction of uranium(VI) and molybdenium(VI) by Alamine 310 and its mixtures from aqueous H3PO4 solution, Journal of Radioanalytical and Nuclear Chemistry, 173(1), pp.161-169. https://doi.org/10.1007/BF02102708
  13. El-Nadi, Y.A., Awwad, N.S., Nayl, A.A., 2009 : A comparative study of vanadium extraction by Aliquat-336 from acidic and alkaline media with application to spent catalyst, International Journal of Mineral Processing, 92(3-4), pp.115-120. https://doi.org/10.1016/j.minpro.2009.03.005
  14. Lozano, L.J., Godinez, C., 2003 : Comparative study of solvent extraction of vanadium from sulphate solutions by primene 81R and alamine 336, Minerals Engineering, 16(3), pp.291-294. https://doi.org/10.1016/S0892-6875(03)00009-8
  15. Cosar, T., Ziyadanogullari, R., 1998 : Separation of molybdenum, vanadium and nickel by liquid-liquid extraction, Turkish Journal of Chemistry, 22(4), pp.379-386.
  16. Biswas, S., Hareendran, K.N., Singh, D.K., et al., 2010 : Extraction of U(VI) and Th(IV) from nitric acid medium using tri(butoxyethyl) phosphate (TBEP) in n -paraffin, Journal of Radioanalytical and Nuclear Chemistry, 283(3), pp.665-668. https://doi.org/10.1007/s10967-010-0453-4
  17. Cueva Sola, A.B., Parhi, P.K., Lee, J.Y., et al., 2020 : Environmentally friendly approach to recover vanadium and tungsten from spent SCR catalyst leach liquors using Aliquat 336, RSC Advances, 10(34), pp.19736-19746. https://doi.org/10.1039/d0ra02229b
  18. Cueva Sola, A.B., Jeon, J., Lee, J.Y., et al., 2020 : Spent SCR Catalyst Leach Liquor Processed for Valuable Metals Extraction by Solvent Extraction Technique, Journal of Korean Institute of Resources Recycling, 29(2), pp.55-61. https://doi.org/10.7844/KIRR.2020.29.2.55
  19. Gamare, J.S., Chetty, K. V., Mukerjee, S.K., et al., 2009 : Extraction studies of Uranium(VI), Plutonium(IV) and Americium(III) from nitric acid using the Bi-functional carbamoyl methyl sulfoxide ligands, Analytical Sciences, 25(9), pp.1167-1170. https://doi.org/10.2116/analsci.25.1167
  20. Takahashi, Y., Hotokezaka, H., Noda, K., et al., 2009 : Extraction of uranium(VI) from nitric acid solution using pyrrolidone derivatives, Journal of Nuclear Science and Technology, 46(8), pp.787-792. https://doi.org/10.3327/jnst.46.787
  21. Lapka, J.L., Paulenova, A., Alyapyshev, M.Y. et al., 2009 : Extraction of uranium(VI) with diamides of dipicolinic acid from nitric acid solutions, Radiochimica Acta, 97(6), pp.291-296.
  22. Singh, S.K., Dhami, P.S., Tripathi, S.C., et al., 2009 : Studies on the recovery of uranium from phosphoric acid medium using synergistic mixture of (2-Ethyl hexyl) Phosphonic acid, mono (2-ethyl hexyl) ester (PC88A) and Tri-n-butyl phosphate (TBP), Hydrometallurgy, 95(1-2), pp.170-174. https://doi.org/10.1016/j.hydromet.2008.04.006
  23. Jha, R.K., Gupta, K.K., Kulkarni, P.G., et al., 2008 : Third phase formation studies in the extraction of Th(IV) and U(VI) by N,N-dialkyl aliphatic amides, Desalination 232 (1-3), pp.225-233. https://doi.org/10.1016/j.desal.2007.11.054
  24. Egorova, N.S., Belova, V. V., Voshkin, A.A., et al., 2008 : Extraction of uranyl nitrate with a binary extractant based on di(2,4,4-trimethylpentyl)phosphinic acid, Theoretical Foundations of Chemical Engineering, 42(5), pp.708-713. https://doi.org/10.1134/S0040579508050394
  25. SATO, T., TAKAYANAGI, T., SATO, K., 2010 : Liquid-Liquid Extraction of Palladium(II) from Hydrochloric Acid Solutions by High Molecular Weight Amines, Solvent Extraction Research and Development, Japan, 17, pp.95-110. https://doi.org/10.15261/serdj.17.95
  26. Alibrahim, M., Shlewit, H., Alike, S., 2008 : Solvent extraction of Vanadium(IV) with di(2-ethylhexyl) phosphoric acid and tributyl phosphate, Periodica Polytechnica Chemical Engineering, 52(1), pp.29-33. https://doi.org/10.3311/pp.ch.2008-1.06
  27. Kurbatova, L.D., Kurbatov, D.I., 2008 : Vanadium(V) extraction from sulfuric acid solutions, Russian Journal of Inorganic Chemistry, 53(7), pp.1154-1157. https://doi.org/10.1134/S0036023608070292
  28. Elizalde, M.P., Garcia Pavon, E., Almela, A., et al., 2008 : Vanadium extraction from phosphoric acid solutions by LIX 860-I. Application to industrial phosphoric acid, Solvent Extraction and Ion Exchange, 26(3), pp.180-191. https://doi.org/10.1080/07366290802053520
  29. Langade, A.D., Shinde, V.M., 1980 : Liquid-liquid extraction and separation studies of uranium(VI), Mikrochimica Acta, 74(1-2), pp.93-98. https://doi.org/10.1007/BF01196490
  30. Kim, C.J., Kumar, J.R., Kim, J.S., et al., 2012 : Solvent extraction studies on uranium using amine based extractants and recovery from low grade ore leach liquors, Journal of the Brazilian Chemical Society, 23, pp.1254-1264. https://doi.org/10.1590/S0103-50532012000700009
  31. Kumar, J.R., Kim, J.S., Lee, J.Y., et al., 2010 : Solvent extraction of uranium(VI) and separation of vanadium(V) from sulfate solutions using Alamine 336, Journal of Radioanalytical and Nuclear Chemistry, 285(2), pp.301-308. https://doi.org/10.1007/s10967-010-0552-2
  32. Kim, J.-S., Kim, S.-D., Lee, H.-I., et al., 2013 : Process development for uranium and vanadium recovery from Korean Okcheon black shale ore leach liquor, Monatshefte fur chemie-Chemical Monthly, 144(11), pp.1589-1596. https://doi.org/10.1007/s00706-013-1061-0
  33. Kim, J.S., Chung, K.W., Lee, H.I., et al., 2014 : Leaching behavior of uranium and vanadium using strong sulfuric acid from Korean black shale ore, Journal of Radio-analytical and Nuclear Chemistry, 299(1), pp.81-87. https://doi.org/10.1007/s10967-013-2732-3
  34. Janardhan Reddy, K., Rajesh Kumar, J., Reddy, M.L.P., et al., 2009 : Synergistic enhancement and separation of zirconium(IV) and hafnium(IV) with 3-Phenyl-4-benzoyl-5-isoxazolone in the presence of crown ethers, Separation Science and Technology, 44(9), pp.2022-2040. https://doi.org/10.1080/01496390902885882
  35. Kumar, J.R., Lee, H.I., Lee, J.Y., et al., 2008 : Comparison of liquid-liquid extraction studies on platinum(IV) from acidic solutions using bis(2,4,4-trimethylpentyl) monothio-phosphinic acid, Separation and Purification Technology, 63(1), pp.184-190. https://doi.org/10.1016/j.seppur.2008.04.014
  36. Joon-Soo Kim, J. Rajesh Kumar, Jin-Young Lee, et al., 2011 : Extraction and Separation of U(VI) and V(V) from Sulfate Solutions using Alamine Extractants, Proceedings of European Metallurgical Conference (EMC), Germany, Dusseldorf, 26-29 June 2011, pp.1149-1160.