Simultaneous Separation of Pd, Rh, and Ru from Simulated Radwaste Using Tin as the Solvent Metal prior to Final Vitrification into Borosilicate Glass: An Attempt to Recover Wealth from Waste
Publication: Journal of Hazardous, Toxic, and Radioactive Waste
Volume 25, Issue 3
Abstract
Platinum group metals (PGMs), namely, Ru, Rh, and Pd, were removed simultaneously from molten borosilicate glass containing simulated high-level waste (HLW), using Sn as the solvent metal. The metal and glass phases were separated from each other after the melting was completed. The metal and glass phases were examined using X-ray diffraction and scanning electron microscopy (SEM) with energy dispersive X-ray (EDX) analysis; the composition of alloy phase was analyzed using inductively coupled plasma optical emission spectroscopy (ICP-OES). The percentage of recovery of the metal phase was 80%–87%. The metallic tin phase was found to contain PdSn4, Ru2Sn3, Ru3Sn7, and Pd0.15Rh0.15Ru0.70 intermetallic compounds, which crystallize in orthorhombic, tetragonal, cubic, and hexagonal structures, respectively. On dissolving the alloy in aqua regia, Ru3Sn7 and Pd0.15Rh0.15Ru0.70 were found to remain as an insoluble residue. The insoluble character of Ru3Sn7 and Pd0.15Rh0.15Ru0.70 affects the material balance of each element in the glass and metal alloy phases. The PGMs were separated to the metal alloy phase along with significant quantities of Fe, Te, Ni, and Mo, leaving behind Cs, Sr, and Zr in the glass phase. The recovery of PGMs has dual benefits; the removal of PGMs facilitates smooth vitrification of the waste by Joule heating. The other benefit is that of recycling PGMs (which are rare precious metals) from the waste.
Get full access to this article
View all available purchase options and get full access to this article.
Acknowledgments
The authors are grateful to Dr. Binaya Kumar Panigrahi, former Director, MC&MFCG, IGCAR Dr. N. Sivaraman, Director, MC&MFCG, Dr. V. Jayaraman, Associate Director, FMCG, and Dr. Rajesh Ganesan, Head of the Materials Chemistry Division, for their support and encouragement. Dr. R. Kumar, Head, ACSD and Dr. S. Vijayalakshmi, Head of the Analytical Chemistry Section/ACSD/MC and MFCG, IGCAR are duly acknowledged for extending their support and expertise for analyzing the alloy samples to determine the elemental composition of the metal buttons. We thank Dr. Manish Chandra, MC and MFCG for examining the metal and glass samples by SEM-EDX.
References
Advocat, T., P. Jollivet, J. L. Crovisier, and M. del Nero. 2001. “Long-term alteration mechanisms in water for SON68 radioactive borosilicate glass.” J. Nucl. Mater. 298 (1–2): 55–62. https://doi.org/10.1016/S0022-3115(01)00621-3.
Barin, I. 1995. Thermochemical data of pure substances. 3rd ed. Weinheim, Germany: VCH Weinheim.
Barin, I., and O. Knacke. 1973. Thermochemical properties of inorganic substances. Berlin: Springer.
Chapman, C. C., J. M. Pope, and S. M. Barnes. 1986. “Electric melting of nuclear waste glasses state of the art.” J. Non-Cryst. Solids 84 (1–3): 226–240. https://doi.org/10.1016/0022-3093(86)90781-7.
Chase, M. W., C. A. Davies, J. R. Downey, Jr., D. J. Fruip, R. A. McDonald, and A. N. Syverud. 1985. “JANAF thermochemical tables, 3rd edition, parts I and II. Supplement.” J. Phys. Chem. Ref. Data 14 (S1): 1–1896.
Clarke, F. W., and H. S. Washington. 1924. The composition of the Earth’s crust. Dept. of the Interior, US Geological Survey, Professional paper 127. Seattle: Washington Government Printing Office.
Ellingham, H. J. T. 1944. “Reducibility of oxides and sulphides in metallurgical processes.” J. Soc. Chem. Ind. 63 (5): 125–160.
Igarashi, H., and T. Takahashi. 1991. “The draining of noble metals in vitrified nuclear waste by a melter with a sloping floor.” Glass Technol. 32 (2): 46–50.
Jena, H., K. V. G. Kutty, and P. R. V. Rao. 2011. “Effect of temperature on the extraction of Pd by liquid tin from molten borosilicate glass containing simulated radwaste.” J. Non-Cryst. Solids 357 (15): 2911–2919. https://doi.org/10.1016/j.jnoncrysol.2011.03.033.
Jena, H., R. R. Madhavan, K. V. G. Kutty, and P. R. V. Rao. 2015. “Feasibility studies on Pd removal from molten BSG containing simulated nuclear waste using lead or aluminum as a solvent metal.” J. Hazard. Toxic Radioact. Waste 19 (2): 04014024. https://doi.org/10.1061/(ASCE)HZ.2153-5515.0000228.
Jena, H., R. Sudha, P. Venkatesh, B. P. Reddy, and K. V. G. Kutty. 2018. “Removal of Ru from simulated high-level waste prior to the final vitrification into borosilicate glass using tin as the alloying element: Feasibility study.” J. Hazard. Toxic Radioact. Waste 22 (4): 04018018. https://doi.org/10.1061/(ASCE)HZ.2153-5515.0000408.
Jensen, G. A., A. M. Platt, G. B. Mellinger, and W. J. Bjorklund. 1984. “Recovery of noble metals from fission products.” Nucl. Technol. 65 (2): 305–324. https://doi.org/10.13182/NT84-A33413.
Kolarik, Z., and E. V. Renard. 2003b. “Recovery of value fission platinoids from spent nuclear fuel.” Platinum Met. Rev. 47 (2): 74–87.
Kolarik, Z., and E. V. Renard. 2003a. “Recovery of value fission platinoids from spent nuclear fuel.” Platinum Met. Rev. 47 (3): 123–131.
Kolarik, Z., and E. V. Renard. 2005. “Potential applications of fission platinoids in industry.” Platinum Met. Rev. 49 (2): 79–90. https://doi.org/10.1595/147106705X35263.
Luckscheiter, B., and M. Nesovic. 1996. “Development of glasses for the vitrification of high level liquid waste (HLLW) in a joule heated ceramic melter.” Waste Manage. (Oxford) 16 (7): 571–578. https://doi.org/10.1016/S0956-053X(97)88231-1.
Lutze, W., and R. C. Ewing. 1988. Radioactive waste forms for the future. Amsterdam, Netherlands: North-Holland.
Naito, K., T. Matsui, and Y. Tanaka. 1986. “Recovery of noble metals from insoluble residue of spent fuel.” J. Nucl. Sci. Technol. 23 (6): 540–549. https://doi.org/10.1080/18811248.1986.9735017.
Pflieger, R., M. Malki, Y. Guari, J. Larionova, and A. Grandjean. 2009. “Electrical conductivity of RuO2-borosilicate glasses: Effect of the synthesis route.” J. Am. Ceram. Soc. 92 (7): 1560–1566. https://doi.org/10.1111/j.1551-2916.2009.03088.x.
Poirot, R., D. Bourgeois, and D. Meyer. 2014. “Palladium extraction by a malonamide derivative (DMDOHEMA) from nitrate media: Extraction behavior and third phase characterization.” Solvent Extr. Ion Exch. 32 (5): 529–542. https://doi.org/10.1080/07366299.2014.908587.
Rindone, G. E., and J. L. Rhoads. 1956. “The colors of platinum, palladium and rhodium in simple glasses.” J. Am. Ceram. Soc. 39 (5): 173–180. https://doi.org/10.1111/j.1151-2916.1956.tb15640.x.
Ronneau, C., J. Cara, and A. Rimski-Korsakov. 1995. “Oxidation-enhanced emission of ruthenium from nuclear fuel.” J. Environ. Radioact. 26 (1): 63–70. https://doi.org/10.1016/0265-931X(95)91633-F.
Schreiber, H. D. 1986. “Redox processes in glass-forming melts.” J. Non-Cryst. Solids 84 (1–3): 129–141. https://doi.org/10.1016/0022-3093(86)90770-2.
Schreiber, H. D., T. R. Harville, and G. N. Damron. 1990. “Redox-Controlled solubility of palladium in a borosilicate glass melt.” J. Am. Ceram. Soc. 73 (5): 1435–1437. https://doi.org/10.1111/j.1151-2916.1990.tb05220.x.
Schreiber, H. D., and A. L. Hockman. 1987. “Redox chemistry in candidate glasses for nuclear waste immobilization.” J. Am. Ceram. Soc. 70 (8): 591–594. https://doi.org/10.1111/j.1151-2916.1987.tb05712.x.
Schreiber, H. D., F. A. Settle, P. L. Jamison, J. P. Eckenrode, and G. W. Headley. 1986. “Ruthenium in glass-forming borosilicate melts.” J. Less-Common Met. 115 (1): 145–154. https://doi.org/10.1016/0022-5088(86)90379-6.
Tooley, F. V. 1984. Vols. 1–2 of The handbook of glass manufacture: A book of reference for the plant executive and engineer. 3rd ed. New York: Ashlee Publishing Company.
Uruga, K., K. Sawada, Y. Arita, Y. Enokida, and I. Yamamoto. 2007. “Removal of platinum group metals contained in molten glass using copper.” J. Nucl. Sci. Technol. 44 (7): 1024–1031. https://doi.org/10.1080/18811248.2007.9711342.
Uruga, K., K. Sawada, Y. Enokida, and Y. Yamamoto. 2008. “Liquid metal extraction for removal of molybdenum from molten glass containing simulated nuclear waste elements.” J. Nucl. Sci. Technol. 45 (10): 1063–1071. https://doi.org/10.1080/18811248.2008.9711893.
Information & Authors
Information
Published In
Copyright
© 2021 American Society of Civil Engineers.
History
Received: Oct 20, 2020
Accepted: Mar 1, 2021
Published online: May 12, 2021
Published in print: Jul 1, 2021
Discussion open until: Oct 12, 2021
Authors
Metrics & Citations
Metrics
Citations
Download citation
If you have the appropriate software installed, you can download article citation data to the citation manager of your choice. Simply select your manager software from the list below and click Download.