skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

This content will become publicly available on February 26, 2020

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

Abstract

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 VIO 2)(L)(CH 3CN)] (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.

Authors:
 [1];  [2];  [3]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [4]
  1. Univ. of California, Irvine, CA (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Tennessee Technological Univ., Cookeville, TN (United States)
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  4. Univ. of California, Irvine, CA (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1499366
Report Number(s):
LA-UR-19-21331
Journal ID: ISSN 0020-1669
Grant/Contract Number:  
89233218CNA000001
Resource Type:
Accepted Manuscript
Journal Name:
Inorganic Chemistry
Additional Journal Information:
Journal Volume: 58; Journal Issue: 6; Journal ID: ISSN 0020-1669
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Bustillos, Christian G., Hawkins, Cory A., Copping, Roy, Reilly, Sean Douglas, Scott, Brian Lindley, May, Iain, and Nilsson, Mikael. Complexation of High-Valency Mid-Actinides by a Lipophilic Schiff Base Ligand: Synthesis, Structural Characterization, and Progress toward Selective Extraction. United States: N. p., 2019. Web. doi:10.1021/acs.inorgchem.8b02849.
Bustillos, Christian G., Hawkins, Cory A., Copping, Roy, Reilly, Sean Douglas, Scott, Brian Lindley, May, Iain, & Nilsson, Mikael. Complexation of High-Valency Mid-Actinides by a Lipophilic Schiff Base Ligand: Synthesis, Structural Characterization, and Progress toward Selective Extraction. United States. doi:10.1021/acs.inorgchem.8b02849.
Bustillos, Christian G., Hawkins, Cory A., Copping, Roy, Reilly, Sean Douglas, Scott, Brian Lindley, May, Iain, and Nilsson, Mikael. Tue . "Complexation of High-Valency Mid-Actinides by a Lipophilic Schiff Base Ligand: Synthesis, Structural Characterization, and Progress toward Selective Extraction". United States. doi:10.1021/acs.inorgchem.8b02849.
@article{osti_1499366,
title = {Complexation of High-Valency Mid-Actinides by a Lipophilic Schiff Base Ligand: Synthesis, Structural Characterization, and Progress toward Selective Extraction},
author = {Bustillos, Christian G. and Hawkins, Cory A. and Copping, Roy and Reilly, Sean Douglas and Scott, Brian Lindley and May, Iain and Nilsson, Mikael},
abstractNote = {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 [(AnVIO2)(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.},
doi = {10.1021/acs.inorgchem.8b02849},
journal = {Inorganic Chemistry},
number = 6,
volume = 58,
place = {United States},
year = {2019},
month = {2}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on February 26, 2020
Publisher's Version of Record

Save / Share: