Recovery of Uranium and Plutonium from Waste Matrices Using Supercritical Fluid Extraction

Krishnamurthy Sujatha, Kancharlapalli Chinaraga Pitchaiah, Nagarajan Sivaraman, Thandankorai Ganapathi Srinivasan, Polur Ranga Rao Vasudeva Rao

Chemistry Group, Indira Gandhi Centre for Atomic Research, Kalpakkam, India.

DOI: 10.4236/ajac.2012.312A121                

Abstract

Supercritical fluid extraction (SFE) of plutonium in its nitrate form from actual waste, i.e. plutonium bearing cellulose matrix was demonstrated using 0.1 litre capacity extraction vessel. Complete recovery of plutonium was demonstrated using modified supercritical carbon dioxide (Sc-CO₂), i.e. Sc-CO₂ containing octylphenyl-N, N-diisobutyl-carbamoyl- methylphosphine oxide (φCMPO). Near complete recovery of uranium was demonstrated from simulated waste matri- ces, i.e. uranium bearing teflon, glass and cellulose matrices using preparative scale SFE, i.e. from 1 litre capacity ex- traction vessel. The recovery of uranium was established using Sc-CO₂ modified with acetyl acetone.

Keywords

Supercritical CO₂; SFE; Uranium; Plutonium; φCMPO; Cellulose Matrix

Conflicts of Interest

The authors declare no conflicts of interest.

References

[1]	M. Caude and D. Thiebaut, “Practical Supercritical Fluid Chromatography and Extraction,” Harwood Academic Publishers, Switzerland, 1999.
[2]	M. A. Mc-Hugh and V. J. Krukonis, “Supercritical Fluid Extraction: Principle and Practice,” 2nd Edition, Butter-worth-Heinamann, Boston, 1994.
[3]	C. Erkey, “Supercritical Carbon Dioxide Extraction of Metals from Aqueous Solutions: A Review,” Journal of Supercritical Fluids, Vol. 17, No. 3, 2000, pp. 259-287. doi:10.1016/S0896-8446(99)00047-9
[4]	K. E. Laintz, C. M. Wai, C. R. Yonker and R. D. Smith, “Extraction of Metal Ions from Liquid and Solid Materials by Supercritical Carbon Dioxide,” Analitical Chemistry, Vol. 64, No. 22, 1992, pp. 2875-2878. doi:10.1021/ac00046a039
[5]	Y. Lin, N. G. Smart and C. M. Wai, “Supercritical Fluid Extraction and Chromatography of Metal Chelates and Organometallic Compounds,” Trend Analitical Chemistry, Vol. 14, No. 3, 1995, pp. 123-133. doi:10.1016/0165-9936(95)94045-G
[6]	C .M. Wai, “Supercritical Fluid Extraction of Trace Metals from Solid and Liquid Materials for Analytical Applications,” Analitical Sciences, Vol. 11, No. 1, 1995, pp. 165-167. doi:10.2116/analsci.11.165
[7]	Y. Lin, R. D. Brauer, K. E. Laintz and C. M. Wai, “Supercritical Fluid Extraction of Lanthanides and Actinides from Solid Materials with a Fluorinated β-Diketone,” Analitical Chemistry, Vol. 65, No. 18, 1993, pp. 2549-2551. doi:10.1021/ac00066a027
[8]	S. Iso, S. Uno, Y. Meguro, T. Sasaki and Z. Yoshida, “Pressure Dependence of Extraction Behaviour of Plutonium (IV) and Uranium (VI) from Nitric Acid Solution to Supercritical Carbon Dioxide Containing Tributylphosphate,” Progress in Nuclear Energy, Vol. 37, No. 1-4, 2000, pp. 423-428. doi:10.1016/S0149-1970(00)00082-2
[9]	O. Tomioka, Y. Meguro, Y. Enokida, I. Yamamoto and Z. Yoshida, “Dissolution Behaviour of Uranium Oxides with Supercritical CO2 Using HNO3-TBP Complex as a Reactant,” Journal of Nuclear Science and Technology, Vol. 38, No. 12, 2001, pp. 1097-1102. doi:10.1080/18811248.2001.9715141
[10]	Y. Meguro, S. Iso, Z. Yoshida, O. Tomioka, Y. Enokida and I. Yamamoto, “Decontamination of Uranium Oxides from Solid Wastes by Supercritical CO2 Fluid Leaching Method Using HNO3-TBP Complex as a Reactant,” Journal of Supercritical Fluids, Vol. 31, No. 2, 2004, pp. 141-147. doi:10.1016/j.supflu.2003.10.005
[11]	T. I. Trofimov, M. D. Samsonov, Y. M. Kulyako and B. F. Myasoedov, “Dissolution and Extraction of Actinide Oxides in Supercritical Carbon Dioxide Containing the Complex of Tri-n-Butylphosphate with Nitric Acid,” Comptes Rendus Chimie, Vol. 7, No. 12, 2004, pp. 1209-1213. doi:10.1016/j.crci.2004.04.010
[12]	B. J. Mincher, R. V. Fox, R. G. G. Holmes, R. A. Robbins and C. Boardman, “Supercritical Fluid Extraction of Plutonium and Americium from Soil Using Theonytrifluoroacetone and Tributylphosphate Complexation,” Radiochimica Acta, Vol. 89, No. 10, 2001, pp. 613-617. doi:10.1524/ract.2001.89.10.613
[13]	A. A. Murzin, V. A. Babain, A. Yu. Shadrin, V. A. Kamachev, V. N. Romanovskii, V. A. Starchenko, S. V. Podoinitsyn, Yu. A. Revenko, M. V. Logunov and N. G. Smart, “Deactivation in Sub and Supercritical Carbon Dioxide,” Radiochemistry, Vol. 44, No. 4, 2002, pp. 410-415. doi:10.1023/A:1020641431291
[14]	M. Shamsipur, A. R. Ghiasvand and Y. Yamini, “Extraction of Uranium from Solid Matrices Using Modified Supercritical Fluid CO2,” Journal of Supercritical Fluids, Vol. 20, No. 2, 2001, pp. 163-169. doi:10.1016/S0896-8446(01)00052-3
[15]	Y. Lin, C. M. Wai, F. M. Jean and R. D. Brauer, “Supercritical Fluid Extraction of Thorium and Uranium Ions from Solid and Liquid Materials with Fluorinated beta-Diketones and Tributyl Phosphate,” Environmental Science and Technology, Vol. 28, No. 6, 1994, pp. 1190-1193. doi:10.1021/es00055a034
[16]	P. Kumar, A. Pal, M. K. Saxena and K. L. Ramakumar, “Supercritical Fluid Extraction of Uranium and Thorium from Solid Matrices,” Desalination, Vol. 232, No. 1-3, 2008, pp. 71-79. doi:10.1016/j.desal.2007.08.022
[17]	A. Rao, P. Kumar and K. L. Ramakumar, “Separation of Uranium from Different Uranium Oxide Matrices Employing Supercritical Carbon Dioxide Extraction,” Journal of Radioanalytical Nuclear Chemistry, Vol. 285, No. 2, 2010, pp. 247-257. doi:10.1007/s10967-010-0568-7
[18]	R. Kumar, N. Sivaraman, E. Senthil Vadivu, T. G. Srinivasan and P. R. Vasudeva Rao, “Complete Removal of Uranyl Nitrate from Tissue Matrix Using Supercritical Fluid Extraction,” Radiochimica Acta, Vol. 91, No. 4, 2003, pp. 197-201. doi:10.1524/ract.91.4.197.19966
[19]	R. Kumar, N. Sivaraman, K. Sujatha, T. G. Srinivasan and P. R. Vasudeva Rao, “Removal of Plutonium and Americium from Waste Matrices by Supercritical Carbon Dioxide Extraction,” Radiochimica Acta, Vol. 95, No. 10, 2007, pp. 577-584. doi:10.1524/ract.2007.95.10.577
[20]	V. Suresh Kumar, R. Kumar, N. Sivaraman, G. Ravisankar and P. R. Vasudeva Rao, “Design and Adaptation of a Novel Supercritical Extraction Facility for Operation in a Glove Box for Recovery of Radioactive Elements,” Review of Scientific Instruments, Vol. 81, No. 9, 2010, Article ID: 094101. doi:10.1063/1.3484190
[21]	A. Datta, N. Sivaraman, T. G. Srinivasan and P. R. Vasudeva Rao, “Liquid Chromatographic Behaviour of Actinides and Lanthanides on Monolith Supports,” Radiochimica Acta, Vol. 99, No. 5, 2011, pp. 275-283.
[22]	R. Kumar, N. Sivaraman, K. Sujatha, T. G. Srinivasan and P. R. Vasudeva Rao, “A Novel Technique for Modifier Free Delivery of Ligands for Supercritical Fluid Extraction,” Radiochimica Acta, Vol. 97, No. 8, 2009, pp. 443-451. doi:10.1524/ract.2009.1633