Solubilization of Cs and K from Tetraphenylborate Precipitates in Highly Alkaline Environments
Publication: Journal of Hazardous, Toxic, and Radioactive Waste
Volume 22, Issue 1
Abstract
Precipitated Cs tetraphenylborate, along with K tetraphenylborate and aqueous alkaline supernate, is present in certain high-level waste tanks at the Savannah River Site. Two possible processes for transferring the (and ) into the aqueous phase are described. One consists of displacement of the heavy alkalis from the solid tetraphenylborate by adding a tetraalkylammonium hydroxide. Almost 100% solubilization is obtained at ambient temperature using tetra--butylammonium hydroxide. The other consists of oxidative decomposition of the tetraphenylborate using persulfate. The extent of solubilization is found to increase with increasing temperature and persulfate:tetraphenylborate ratio. High yields of tetraphenylborate decomposition are obtained at elevated temperatures (55–90°C), and these yields increase with rising persulfate:tetraphenylborate ratios. The decomposition yields are lowered in the presence of nitrite, which is a component of the alkaline supernate, but are still significant, especially at elevated temperatures and high persulfate:tetraphenylborate ratios. The adverse effect of nitrite can be greatly reduced by lowering the pH.
Get full access to this article
View all available purchase options and get full access to this article.
References
Anotai, J., Masomboon, N., Chuang, C.-L., and Lu, M.-C. (2011). “Persulfate oxidation for the aniline degradation in aqueous systems.” Water Sci. Technol., 63(7), 1434–1440.
Block, P. A., Brown, R. A., and Robinson, D. (2004). “Novel activation technologies for sodium persulfate in situ chemical oxidation.” Proc., 4th Int. Conf. on the Remediation of Chlorinated and Recalcitrant Compounds, Battelle Press, Columbus, OH.
Burger, K. (1973). Organic reagents in metal analysis, Elsevier, Amsterdam, Netherlands.
Crimi, M. L., and Taylor, J. (2007). “Experimental evaluation of catalyzed hydrogen peroxide and sodium persulfate for destruction of BTEX contaminants.” Soil Sediment Contam., 16(1), 29–45.
Cuypers, C., Grotenhuis, T., Joziasse, J., and Rulkens, W. (2000). “Rapid persulfate oxidation predicts PAH bioavailability in soils and sediments.” Environ. Sci. Technol., 34(10), 2057–2063.
Devine, J. C., Jr., et al. (2006). “Independent technical review (ITR) path forward for Savannah River Site Tank 48.”, U.S. Dept. of Energy Office of Environmental Management, Washington, DC.
Eberson, L. (1987). Electron transfer reactions in organic chemistry, Springer, Berlin.
Engelbrecht, R. M., and McCoy, F. A. (1956). “Determination of potassium by tetraphenylborate method.” Anal. Chem., 28(11), 1772–1773.
Flores, R., Blass, G., and Domínguez, V. (2007). “Soil remediation by an advanced oxidative method assisted with ultrasonic energy.” J. Hazard. Mater., 140(1–2), 399–402.
Gau, B. C., Chen, H., Zhang, Y., and Gross, M. L. (2010). “Sulfate radical anion as a new reagent for fast photochemical oxidation of proteins.” Anal. Chem., 82(18), 7821–7827.
House, D. A. (1962). “Kinetics and mechanism of oxidation by peroxydisulfate.” Chem. Rev., 62(3), 185–203.
Huang, K.-C., Zhao, Z., Hoag, G. E., Dahmani, A., and Block, P. A. (2005). “Degradation of volatile organic compounds with thermally activated persulfate oxidation.” Chemosphere, 61(4), 551–560.
Kronholm, J., Jyske, P., and Riekkola, M. L. (2000). “Oxidation efficiencies of potassium persulfate and hydrogen peroxide in pressurized hot water with and without preheating.” Ind. Eng. Chem. Res., 39(7), 2207–2213.
Lambert, D., Peters, T. B., and Fink, S. D. (2006). “Copper-catalyzed peroxide oxidation testing for tetraphenylborate decomposition.” Sep. Sci. Technol., 41(11), 2299–2312.
Lambert, D. P., Fink, S. D., and Peters, T. B. (2007). “Processing alternatives for destruction of tetraphenylborate.” IT3’07 Conf., Westinghouse Savannah River Company, Aiken, SC.
Lambert, D. P., Peters, T. B., and Fink, S. D. (2005). “In-tank peroxide oxidation process for the decomposition of tetraphenylborate in Tank 48H.”, Westinghouse Savannah River Company, Aiken, SC.
Lambert, D. P., Peters, T. B., Stallings, M. E., and Fink, S. D. (2004). “Process development for oxidative destruction of tetraphenylborate in Savannah River Site Tank 48H.”, Westinghouse Savannah River Company, Aiken, SC.
Latimer, W. M. (1952). Oxidation potentials, Prentice-Hall, Englewood Cliffs, NJ.
Li, Y., Liu, L.-D., Lu, L., Liu, Y., Zhang, H.-W., and Han, X. (2016). “Efficient oxidation of phenol by persulfate using manganite as a catalyst.” J. Mol. Catal. A Chem., 411, 264–271.
Liang, C., Bruell, C. J., Marley, M. C., and Sperry, K. L. (2004). “Persulfate oxidation for in situ remediation of TCE. I: Activated by ferrous ion with and without a persulfate-thiosulfate redox couple.” Chemosphere, 55(9), 1213–1223.
Liang, C., Chen, Y.-J., and Chang, K.-J. (2009a). “Evaluation of persulfate oxidative wet scrubber for removing BTEX gases.” J. Hazard. Mater., 164(2–3), 571–579.
Liang, C., Huang, C.-F., and Chen, Y.-J. (2008). “Potential for activated persulfate degradation of BTEX contamination.” Water Res., 42(15), 4091–4100.
Liang, C., Lin, Y.-T., and Shih, W.-H. (2009b). “Treatment of trichloroethylene by adsorption and persulfate oxidation in batch studies.” Ind. Eng. Chem. Res., 48(18), 8373–8380.
Lin, Y.-T., Liang, C., and Chen, J.-H. (2011). “Feasibility study of ultraviolet activated persulfate oxidation of phenol.” Chemosphere, 82(8), 1108–1172.
Nadim, F., Huang, K.-C., and Dahmani, A. M. (2006). “Remediation of soil and ground water contaminated with PAH using heat and Fe(II)-EDTA catalyzed persulfate oxidation.” Water Air Soil Pollut. Focus, 6(1–2), 227–232.
National Research Council. (2000). Alternatives for high-level waste salt processing at the Savannah River Site, National Academies Press, Washington, DC.
Nerud, F., Baldrian, P., Gabriel, J., and Ogbeifun, D. (2001). “Decolorization of synthetic dyes by the Fenton reagent and the system.” Chemosphere, 44(5), 957–961.
Popovych, O. (1981). Solubility data series. Vol. 18: Ttetraphenylborates, Pergamon Press, Oxford, U.K.
Sperry, K. L., Marley, M. C., Bruell, C. J., Liang, C., and Hochreiter, J. (2002). “Iron catalyzed persulfate oxidation of chlorinated solvents.” Proc., 3rd Int. Conf. on Remediation of Chlorinated and Recalcitrant Compounds, Battelle Press, Columbus, OH, 1158–1165.
Thomas, J. L. (2006). “Tank 48 best estimate chemical characterization.”, Westinghouse Savannah River Company, Aiken, SC.
Information & Authors
Information
Published In
Journal of Hazardous, Toxic, and Radioactive Waste
Volume 22 • Issue 1 • January 2018
Copyright
©2017 American Society of Civil Engineers.
History
Received: Jan 20, 2017
Accepted: May 9, 2017
Published online: Sep 13, 2017
Published in print: Jan 1, 2018
Discussion open until: Feb 13, 2018
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.