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

Shusterman, Jennifer A.; Mason, Harris E.; Bowers, Jon; Bruchet, Anthony; Uribe, Eva C.; Kersting, Annie B.; Nitsche, Heino

doi:10.1021/acsami.5b04481

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

Journal Article · Thu Sep 03 00:00:00 EDT 2015 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.5b04481· OSTI ID:1234610

Shusterman, Jennifer A. ^[1]; Mason, Harris E. ^[2]; Bowers, Jon ^[1]; Bruchet, Anthony ^[1]; Uribe, Eva C. ^[1]; Kersting, Annie B. ^[2]; Nitsche, Heino ^[1]

Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Glenn T. Seaborg Inst., Physical and Life Sciences Directorate

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.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF)

Grant/Contract Number:: AC52-07NA27344; NA0002135; NA0001978; DGE 1106400

OSTI ID:: 1234610

Report Number(s):: LLNL-JRNL-667351

Journal Information:: ACS Applied Materials and Interfaces, Vol. 7, Issue 37; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 41 works

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

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