Title: Enhancing f-Element Separations with ADAAM-EH: The Impact of Phase Modifiers and a DGA Aqueous Complexant

Journal Article · · Industrial and Engineering Chemistry Research
ORCiD logo [1];  [1]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Colorado School of Mines, Golden, CO (United States)
  2. Argonne National Laboratory (ANL), Argonne, IL (United States)
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Recent investigations have used a 2-ethylhexyl diamide amine (ADAAM-EH) for Am/Cm separations in combination with N,N,N ',N '-tetraethyldiglycolamide as an aqueous complexant to achieve an unprecedented separation factor of 41. The aim of this research effort is to understand the speciation of trivalent lanthanide (Ln) and actinide (An) ions in the organic phase of an ADAAM-EH extraction system, both with and without phase modifiers (PM) (1-octanol and tri-n-butyl phosphate (TBP)). Leveraging spectroscopic techniques in combination with distribution ratio measurements provides an understanding of organic phase f-element ligand complexation. In the absence of PM, Ln is extracted in a stoichiometric 1:1 [M(ADAAM-EH)1(NO3)x(H2O)1](NO3)3-x complex. The addition of 1-octanol at 20 vol % results in multiple species present. One of the species is the same as the no PM case, and the other species results in an increased -OH coordination to the inner sphere, potentially displacing some NO3. In the case of TBP, increasing concentration results in additional red-shifted bands in the UV-visible spectra, suggesting the complexation of additional ligands of either ADAAM-EH or TBP. Finally, the new system knowledge obtained by and spectroscopic experiments will provide benchmarking information for computational studies of the inner- and outer-sphere coordination environments of f-element cations and insights into ADAAM-EH adduct formation with PM, like 1-octanol and TBP.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
2497711
Journal Information:
Industrial and Engineering Chemistry Research, Journal Name: Industrial and Engineering Chemistry Research Journal Issue: 20 Vol. 63; ISSN 0888-5885
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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