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Title: Synthesis and radiometric evaluation of diglycolamide functionalized mesoporous silica for the chromatographic separation of actinides Th, Pa and U

Abstract

The separation of Th, Pa, and U is of critical importance in many applications including nuclear power, nuclear waste, environmental and geochemistry, nuclear forensics and nuclear medicine. Diglycolamide (DGA)-based resins have shown the ability to separate many elements, yet, these resins consist of non-covalent impregnation of the DGA molecules on the resin backbone resulting in co-elution of the extraction molecule during separation cycles, therefore limiting their long-term and repeated use. Covalently binding the DGA molecules onto silica is one way to overcome this issue. Herein, measured equilibrium distribution coefficients of normal extraction chromatographic DGA resin and a covalently bound form (KIT-6-N-DGA sorbent) are reported. Several differences are observed between the two systems, the most significant being observed for uranium, which demonstrated significantly lower sorption behavior on KIT-6-N-DGA. These results indicate that U can effectively be separated from Th and Pa using KIT-6-N-DGA, a task that could not be completed with the use of normal DGA alone.

Authors:
 [1]; ORCiD logo [1]; ORCiD logo [2];  [3];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Univ. of Vienna (Austria)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC). Nuclear Physics (NP) (SC-26); USDOE
OSTI Identifier:
1523235
Alternate Identifier(s):
OSTI ID: 1434126
Report Number(s):
LA-UR-17-29815
Journal ID: ISSN 1477-9226; ICHBD9
Grant/Contract Number:  
89233218CNA000001; AC52-06NA253996; FOA LAB 14-1099
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Dalton Transactions
Additional Journal Information:
Journal Volume: 47; Journal Issue: 15; Journal ID: ISSN 1477-9226
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English

Citation Formats

Hopkins, Philip D., Mastren, Tara, Florek, Justyna, Copping, Roy, Brugh, Mark, John, Kevin Dale, Meiring Nortier, Francois, Birnbaum, Eva R., Kleitz, Freddy, and Fassbender, Michael E. Synthesis and radiometric evaluation of diglycolamide functionalized mesoporous silica for the chromatographic separation of actinides Th, Pa and U. United States: N. p., 2018. Web. doi:10.1039/C8DT00404H.
Hopkins, Philip D., Mastren, Tara, Florek, Justyna, Copping, Roy, Brugh, Mark, John, Kevin Dale, Meiring Nortier, Francois, Birnbaum, Eva R., Kleitz, Freddy, & Fassbender, Michael E. Synthesis and radiometric evaluation of diglycolamide functionalized mesoporous silica for the chromatographic separation of actinides Th, Pa and U. United States. doi:10.1039/C8DT00404H.
Hopkins, Philip D., Mastren, Tara, Florek, Justyna, Copping, Roy, Brugh, Mark, John, Kevin Dale, Meiring Nortier, Francois, Birnbaum, Eva R., Kleitz, Freddy, and Fassbender, Michael E. Fri . "Synthesis and radiometric evaluation of diglycolamide functionalized mesoporous silica for the chromatographic separation of actinides Th, Pa and U". United States. doi:10.1039/C8DT00404H. https://www.osti.gov/servlets/purl/1523235.
@article{osti_1523235,
title = {Synthesis and radiometric evaluation of diglycolamide functionalized mesoporous silica for the chromatographic separation of actinides Th, Pa and U},
author = {Hopkins, Philip D. and Mastren, Tara and Florek, Justyna and Copping, Roy and Brugh, Mark and John, Kevin Dale and Meiring Nortier, Francois and Birnbaum, Eva R. and Kleitz, Freddy and Fassbender, Michael E.},
abstractNote = {The separation of Th, Pa, and U is of critical importance in many applications including nuclear power, nuclear waste, environmental and geochemistry, nuclear forensics and nuclear medicine. Diglycolamide (DGA)-based resins have shown the ability to separate many elements, yet, these resins consist of non-covalent impregnation of the DGA molecules on the resin backbone resulting in co-elution of the extraction molecule during separation cycles, therefore limiting their long-term and repeated use. Covalently binding the DGA molecules onto silica is one way to overcome this issue. Herein, measured equilibrium distribution coefficients of normal extraction chromatographic DGA resin and a covalently bound form (KIT-6-N-DGA sorbent) are reported. Several differences are observed between the two systems, the most significant being observed for uranium, which demonstrated significantly lower sorption behavior on KIT-6-N-DGA. These results indicate that U can effectively be separated from Th and Pa using KIT-6-N-DGA, a task that could not be completed with the use of normal DGA alone.},
doi = {10.1039/C8DT00404H},
journal = {Dalton Transactions},
issn = {1477-9226},
number = 15,
volume = 47,
place = {United States},
year = {2018},
month = {3}
}

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Works referenced in this record:

Adsorption of Gases in Multimolecular Layers
journal, February 1938

  • Brunauer, Stephen; Emmett, P. H.; Teller, Edward
  • Journal of the American Chemical Society, Vol. 60, Issue 2, p. 309-319
  • DOI: 10.1021/ja01269a023

Application of ion exchange and extraction chromatography to the separation of actinium from proton-irradiated thorium metal for analytical purposes
journal, February 2015