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Title: Development and Testing of Diglycolamide Functionalized Mesoporous Silica for Sorption of Trivalent Actinides and Lanthanides

Abstract

Sequestration of trivalent actinides and lanthanides present in used nuclear fuel and legacy wastes is necessary for appropriate long-term stewardship of these metals, particularly to prevent their release into the environment. Organically modified mesoporous silica is an efficient material for recovery and potential subsequent separation of actinides and lanthanides because of its high surface area, tunable ligand selection, and chemically robust substrate. Here, we have synthesized the first novel hybrid material composed of SBA-15 type mesoporous silica functionalized with diglycolamide ligands (DGA-SBA). Because of the high surface area substrate, the DGA-SBA was found to have the highest Eu capacity reported so far in the literature of all DGA solid-phase extractants. The sorption behavior of europium and americium on DGA-SBA in nitric and hydrochloric acid media was tested in batch contact experiments. DGA-SBA was found to have high sorption of Am and Eu in pH 1, 1 M, and 3 M nitric and hydrochloric acid concentrations, which makes it promising for sequestration of these metals from used nuclear fuel or legacy waste. The kinetics of Eu sorption were found to be two times slower than that for Am in 1 M HNO3. Additionally, the short-term susceptibility of DGA-SBA to degradation inmore » the presence of acid was probed using 29Si and 13C solid-state NMR spectroscopy. Finally, the material was found to be relatively stable under these conditions, with the ligand remaining intact after 24 h of contact with 1 M HNO3, an important consideration in use of the DGA-SBA as an extractant from acidic media.« less

Authors:
 [1];  [2];  [1];  [1];  [1];  [2];  [1]
+ Show Author Affiliations
  1. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
  2. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Glenn T. Seaborg Inst., Physical and Life Sciences Directorate
Publication Date:
Research Org.:
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF)
OSTI Identifier:
1234610
Report Number(s):
LLNL-JRNL-667351
Journal ID: ISSN 1944-8244
Grant/Contract Number:  
AC52-07NA27344; NA0002135; NA0001978; DGE 1106400
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 7; Journal Issue: 37; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND RUEL MATERIALS; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; americium; diglycolamide; europium; mesoporous silica; separations; solid-state NMR

Citation Formats

Shusterman, Jennifer A., Mason, Harris E., Bowers, Jon, Bruchet, Anthony, Uribe, Eva C., Kersting, Annie B., and Nitsche, Heino. Development and Testing of Diglycolamide Functionalized Mesoporous Silica for Sorption of Trivalent Actinides and Lanthanides. United States: N. p., 2015. Web. doi:10.1021/acsami.5b04481.
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Shusterman, Jennifer A., Mason, Harris E., Bowers, Jon, Bruchet, Anthony, Uribe, Eva C., Kersting, Annie B., & Nitsche, Heino. Development and Testing of Diglycolamide Functionalized Mesoporous Silica for Sorption of Trivalent Actinides and Lanthanides. United States. https://doi.org/10.1021/acsami.5b04481
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Shusterman, Jennifer A., Mason, Harris E., Bowers, Jon, Bruchet, Anthony, Uribe, Eva C., Kersting, Annie B., and Nitsche, Heino. Thu . "Development and Testing of Diglycolamide Functionalized Mesoporous Silica for Sorption of Trivalent Actinides and Lanthanides". United States. https://doi.org/10.1021/acsami.5b04481. https://www.osti.gov/servlets/purl/1234610.
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@article{osti_1234610,
title = {Development and Testing of Diglycolamide Functionalized Mesoporous Silica for Sorption of Trivalent Actinides and Lanthanides},
author = {Shusterman, Jennifer A. and Mason, Harris E. and Bowers, Jon and Bruchet, Anthony and Uribe, Eva C. and Kersting, Annie B. and Nitsche, Heino},
abstractNote = {Sequestration of trivalent actinides and lanthanides present in used nuclear fuel and legacy wastes is necessary for appropriate long-term stewardship of these metals, particularly to prevent their release into the environment. Organically modified mesoporous silica is an efficient material for recovery and potential subsequent separation of actinides and lanthanides because of its high surface area, tunable ligand selection, and chemically robust substrate. Here, we have synthesized the first novel hybrid material composed of SBA-15 type mesoporous silica functionalized with diglycolamide ligands (DGA-SBA). Because of the high surface area substrate, the DGA-SBA was found to have the highest Eu capacity reported so far in the literature of all DGA solid-phase extractants. The sorption behavior of europium and americium on DGA-SBA in nitric and hydrochloric acid media was tested in batch contact experiments. DGA-SBA was found to have high sorption of Am and Eu in pH 1, 1 M, and 3 M nitric and hydrochloric acid concentrations, which makes it promising for sequestration of these metals from used nuclear fuel or legacy waste. The kinetics of Eu sorption were found to be two times slower than that for Am in 1 M HNO3. Additionally, the short-term susceptibility of DGA-SBA to degradation in the presence of acid was probed using 29Si and 13C solid-state NMR spectroscopy. Finally, the material was found to be relatively stable under these conditions, with the ligand remaining intact after 24 h of contact with 1 M HNO3, an important consideration in use of the DGA-SBA as an extractant from acidic media.},
doi = {10.1021/acsami.5b04481},
journal = {ACS Applied Materials and Interfaces},
number = 37,
volume = 7,
place = {United States},
year = {Thu Sep 03 00:00:00 EDT 2015},
month = {Thu Sep 03 00:00:00 EDT 2015}
}
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https://doi.org/10.1021/acsami.5b04481
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