Complexation of High-Valency Mid-Actinides by a Lipophilic Schiff Base Ligand: Synthesis, Structural Characterization, and Progress toward Selective Extraction

Bustillos, Christian G.; Hawkins, Cory A.; Copping, Roy; Reilly, Sean Douglas; Scott, Brian Lindley; May, Iain; Nilsson, Mikael

doi:10.1021/acs.inorgchem.8b02849

Complexation of High-Valency Mid-Actinides by a Lipophilic Schiff Base Ligand: Synthesis, Structural Characterization, and Progress toward Selective Extraction

Journal Article · Tue Feb 26 00:00:00 EST 2019 · Inorganic Chemistry

DOI:https://doi.org/10.1021/acs.inorgchem.8b02849· OSTI ID:1499366

Bustillos, Christian G. ^[1]; Hawkins, Cory A. ^[2]; Copping, Roy ^[3]; ^[3]; ^[3]; ^[3]; ^[4]

Univ. of California, Irvine, CA (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Tennessee Technological Univ., Cookeville, TN (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Univ. of California, Irvine, CA (United States)

We report that separation of U, Np, and Pu from used nuclear fuel (UNF) would result in lower long-term radiotoxicity, alleviating constraints on the storage and handling of the material. The complexity of UNF requires several industrial-scale processes with multiple waste streams. A one-step solution to the group removal of the elements, U–Pu, is desirable. Here we present a possible solution to group actinide separation utilizing the unique dioxy conformation of An(V/VI) cations and demonstrate the ability of a tetradentate lipophilic Schiff base ligand (L) to yield isostructural complexes of the general formula [(An^VIO₂)(L)(CH₃CN)] (where An = U, Np, or Pu). Extraction of An(VI) with the ligand follows the order U > Pu > Np, likely reflecting the decreased stability of the hexavalent actinide across the series. Lastly, while the results indicate a promising path toward a one-step process, further improvement in the ligand stability and control of the redox chemistry is required.

View Accepted Manuscript (DOE)

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: Laboratory Directed Research and Development (LDRD); USDOE

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 1499366

Report Number(s):: LA-UR--19-21331

Journal Information:: Inorganic Chemistry, Journal Name: Inorganic Chemistry Journal Issue: 6 Vol. 58; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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