Aspects of the Fundamental Chemistry of Cesium Extraction from Acidic Media by HCCD

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The unique extraction properties of univalent polyhedral borate anions, are well known and have been extensively studied over the past three decades. This is particularly true of the hexachlorinated derivative of the chloro-protected cobalt bis(dicarbollide) anion [(8, 9, 12-Cl3-C2B9H8)2-3-Co]-, (CCD-), typically in the acid form (HCCD) and dissolved in a suitably polar diluent, such as nitrobenzene, which is known to have a high affinity for selective extraction of the Cs+ cation. Recent collaborations between Russian and USA researchers expanded the use of HCCD in the Universal Extraction (UNEX) process where Cs, Sr, actinides (An) and lanthanides (Ln) are all extracted ... continued below

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Herbst, R. Scott; Delmau, Laetitia H.; Peterman, Dean R. & Tillotson, Richard D. April 1, 2006.

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The unique extraction properties of univalent polyhedral borate anions, are well known and have been extensively studied over the past three decades. This is particularly true of the hexachlorinated derivative of the chloro-protected cobalt bis(dicarbollide) anion [(8, 9, 12-Cl3-C2B9H8)2-3-Co]-, (CCD-), typically in the acid form (HCCD) and dissolved in a suitably polar diluent, such as nitrobenzene, which is known to have a high affinity for selective extraction of the Cs+ cation. Recent collaborations between Russian and USA researchers expanded the use of HCCD in the Universal Extraction (UNEX) process where Cs, Sr, actinides (An) and lanthanides (Ln) are all extracted simultaneously by incorporating a neutral extractant (specifically diphenyl-N,N-di-n-butylcarbamoylmethyl phosphine oxide, CMPO) with HCCD and PEG-400 in the organic diluent phenyl trifluoromethyl sulfone (FS-13). In recent efforts to understand the complicated and unique synergistic chemical phenomena associated with simultaneous radionuclide (Cs, Sr, An, Ln) in the UNEX process, additional insight into Cs extraction by the HCCD system has been obtained. Four data sets with 25 experimental measurements of Cs distribution ratios, DCs [Cs]org/[Cs]aq, at a variety of initial conditions (various [HCCD] and [HNO3]) have been modeled using the SXLSQI computer program developed at ORNL. The SXLSQI program was used in this analysis to help elucidate the general chemical equilibria operative in the extraction of Cs+ into an organic phase comprised of HCCD in FS-13. The experimental data is best modeled with the following (simplified) chemical equilibria and the associated equilibrium constants (T = 25°C): (1) (2) (3) Where the over bar represents species formed in the organic phase. The equilibrium constant for the primary exchange reaction (1) of log Keq = 3.07 is in excellent agreement with values reported in the literature of log K = 3.00 for the dicarbollide/ nitrobenzene system. In general, the equilibria representing the mechanism of Cs extraction by HCCD is consistent with earlier works reported in the literature, albeit derived by different experimental and modeling schemes. The details of the experimental and modeling efforts are summarized in this work.

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  • 15th Radiochemical Conference,Czech Republic,04/23/2006,04/28/2006

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  • Report No.: INL/CON-05-00783
  • Grant Number: DE-AC07-99ID-13727
  • Office of Scientific & Technical Information Report Number: 911883
  • Archival Resource Key: ark:/67531/metadc885716

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  • April 1, 2006

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  • Sept. 22, 2016, 2:13 a.m.

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  • Nov. 7, 2016, 7:20 p.m.

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Herbst, R. Scott; Delmau, Laetitia H.; Peterman, Dean R. & Tillotson, Richard D. Aspects of the Fundamental Chemistry of Cesium Extraction from Acidic Media by HCCD, article, April 1, 2006; [Idaho Falls, Idaho]. (digital.library.unt.edu/ark:/67531/metadc885716/: accessed August 16, 2017), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.