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Interfacial Complexation Reactions of Sr 2+ with Octyl(phenyl)‐ N , N ‐diisobutylcarbamoylmethylphosphine Oxide for Understanding Its Extraction in Reprocessing Spent Nuclear Fuels
Author(s) -
Stockmann T. Jane,
Lu Yu,
Zhang Jing,
Girault Hubert H.,
Ding Zhifeng
Publication year - 2011
Publication title -
chemistry – a european journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.687
H-Index - 242
eISSN - 1521-3765
pISSN - 0947-6539
DOI - 10.1002/chem.201102491
Subject(s) - stoichiometry , aqueous solution , chemistry , oxide , extraction (chemistry) , nuclear chemistry , metal , analytical chemistry (journal) , organic chemistry
The complexation reactions between strontium (Sr 2+ ) and octyl(phenyl)‐ N , N ‐diisobutylcarbamoylmethylphosphine oxide (CMPO) were studied at the aqueous|1,2‐dichloroethane (w|DCE) and aqueous|room‐temperature ionic liquid (w|RTIL) microinterfaces, in order to understand its extraction in reprocessing spent nuclear fuels, remediation of environmental contamination, and potential radiological isotope feed stock for 90 Y from its isotope 90 Sr in fission byproducts. The stoichiometry (or metal to ligand ratios) and overall complexation constant ( β ) for these reactions at these two interfaces are described herein. Two stoichiometries at the w|DCE interface were discovered, that is, [Sr(CMPO) 2 ] 2+ and [Sr(CMPO) 3 ] 2+ with β values of 4.5×10 19 and 5.5×10 25 , respectively. Only one stoichiometry was observed at the w|RTIL interface: [Sr(CMPO) 3 ] 2+ with β equal to 1.5×10 34 . The larger complexation constant for [Sr(CMPO) 3 ] 2+ at the w|RTIL interface than those found at the w|DCE interface supported the previous observation of a greater distribution ratio in the aqueous–RTIL metal extraction than that in the aqueous–alkane processing. The kinetics of the reactions at the w|RTIL interface was slow. The stoichiometries at the w|DCE interface were confirmed using biphasic electrospray ionization mass spectrometry (BESI‐MS) as well as direct injection of Sr 2+ and CMPO mixture by means of a “shaking flask” experiment to conventional ESI‐MS.