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

Journal Article · · ACS Applied Materials and Interfaces
 [1];  [2];  [1];  [1];  [1];  [2];  [1]
  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
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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.
Research Organization:
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
Grant/Contract Number:
AC52-07NA27344; NA0001978; NA0002135
OSTI ID:
1234610
Report Number(s):
LLNL-JRNL--667351
Journal Information:
ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 37 Vol. 7; ISSN 1944-8244
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (56)

Solid-State NMR Spectroscopic Studies of Propylphosphonic Acid Functionalized SBA-15 Mesoporous Silica: Characterization of Hydrogen-Bonding Interactions journal March 2013
Luminescence study on determination of the hydration number of Cm(III) journal October 1994
Europium speciation by time-resolved laser-induced fluorescence journal February 2003
Synthesis of ordered large pore SBA-15 spherical particles for adsorption of biomolecules journal July 2006
Two novel extraction chromatography resins containing multiple diglycolamide-functionalized ligands: Preparation, characterization and actinide uptake properties journal March 2014
Extraction chromatography of lanthanides using N,N,N′,N′-tetraoctyl diglycolamide (TODGA) as the stationary phase journal September 2008
Design and synthesis of chelating diamide sorbents for the separation of lanthanides journal June 2011
Separation of trivalent actinides from lanthanides by using R-BTP resins and stability of R-BTP resin journal February 2006
Diglycolamic acid modified silica gel for the separation of hazardous trivalent metal ions from aqueous solution journal January 2015
Complexation of Ln(III) and Am(III) with the Hydrosoluble TEDGA: Speciation and Thermodynamics Studies journal January 2012
Assembled diglycolamide for f-element ions sequestration at high acidity journal January 2014
Synthesis and infrared and fluorescence spectra of new europium and terbium polynuclear complexes with an amide-based 1,10-phenanthroline derivative journal July 2004
Extraction chromatographic studies of metal ions using N,N,N′,N′-tetraoctyl diglycolamide as the stationary phase journal February 2006
Preorganization of diglycolamides on the calix[4]arene platform and its effect on the extraction of Am(III)/Eu(III) journal September 2012
Introduction of Bifunctional Groups into Mesoporous Silica for Enhancing Uptake of Thorium(IV) from Aqueous Solution journal March 2014
Tailoring of Organically Modified Silicas for the Solid−Liquid Extraction of Actinides journal February 2001
Actinide Sequestration Using Self-Assembled Monolayers on Mesoporous Supports journal March 2005
Probing the Surface Structure of Divalent Transition Metals Using Surface Specific Solid-State NMR Spectroscopy journal February 2012
Americium(III) Capture Using Phosphonic Acid-Functionalized Silicas with Different Mesoporous Morphologies: Adsorption Behavior Study and Mechanism Investigation by EXAFS/XPS journal May 2014
Preparation of Malonamide−MCM-41 Materials for the Heterogeneous Extraction of Radionuclides journal October 2002
Surface Modified, Collapsible Controlled Pore Glass Materials for Sequestration and Immobilization of Trivalent Metal Ions journal April 2011
Actinide Lanthanide Separation Process—ALSEP journal January 2014
Carbon CP-mass NMR and x-ray crystal structure of paramagnetic lanthanide acetates journal June 1986
Silicon-29 CP/MAS NMR studies of methylchlorosilane reactions on silica gel journal July 1981
A Novel Europium(III)-Based MRI Contrast Agent journal February 2001
Comparison of Covalency in the Complexes of Trivalent Actinide and Lanthanide Cations journal August 2002
Impact of Pore Size and Pore Surface Composition on the Dynamics of Confined Water in Highly Ordered Porous Silica journal March 2012
Understanding Nitric Acid-Induced Changes in the Arrangement of Monomeric and Polymeric Methacryloyl Diglycolamides on Their Affinity toward f-Element Ions journal December 2014
Reverse-Micelle Formation in the Partitioning of Trivalent f-Element Cations by Biphasic Systems Containing a Tetraalkyldiglycolamide journal April 2007
Separation of actinides from Low Level Liquid Wastes (LLLW) by extraction chromatography using novel DMDOHEMA and TODGA impregnated resins journal January 2004
An europium( iii ) diglycolamide complex: insights into the coordination chemistry of lanthanides in solvent extraction journal January 2015
Analysis of trivalent cation complexation to functionalized mesoporous silica using solid-state NMR spectroscopy journal January 2014
Lanthanide selective sorbents: self-assembled monolayers on mesoporous supports (SAMMS) journal January 2004
Design and synthesis of self-assembled monolayers on mesoporous supports (SAMMS): The importance of ligand posture in functional nanomaterials journal January 2007
A well-defined mesoporous amine silica surface via a selective treatment of SBA-15 with ammonia journal January 2012
First example of diglycolamide-grafted resins: synthesis, characterization, and actinide uptake studies journal January 2014
Development of Highly Selective Ligands for Separations of Actinides from Lanthanides in the Nuclear Fuel Cycle journal October 2011
Carrier Facilitated Transport of Europium(III) Across Supported Liquid Membranes Containing N,N,N ′, N ′-tetra-2-ethylhexyl-3-oxapentane-diamide (T2EHDGA) as the Extractant journal July 2011
A Novel Extraction Chromatography Resin for Trivalent Actinides Using 2,6-bis(5,6-diisobutyl-1,2,4-triazine-3-yl)pyridine journal November 2013
Comparison of Extraction Behaviour and Basicity of some Substituted Malonamides journal January 2000
Extraction Behavior of Americium and Curium on Selected Extraction Chromatography Resins from Pure Acidic Matrices journal May 2014
THE NOVEL EXTRACTANTS, DIGLYCOLAMIDES, FOR THE EXTRACTION OF LANTHANIDES AND ACTINIDES IN HNO 3 – n -DODECANE SYSTEM journal January 2001
Extraction of Actinides(Iii), (Iv), (v), (Vi), and Lanthanides(Iii) by Structurally Tailored Diamides journal February 2002
A Novel Bicyclic Diamide with High Binding Affinity for Trivalent f‐Block Elements journal January 2003
Influence of Extractant Aggregation on the Extraction of Trivalent f‐Element Cations by a Tetraalkyldiglycolamide journal December 2004
Novel Extraction of Chromatographic Resins Based on Tetraalkyldiglycolamides: Characterization and Potential Applications journal May 2005
Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides journal September 1976
Functionalized Monolayers on Ordered Mesoporous Supports journal May 1997
Triblock Copolymer Syntheses of Mesoporous Silica with Periodic 50 to 300 Angstrom Pores journal January 1998
Preparation and Properties of SiO2 Thin Films by the Sol-Gel Method Using Photoirradiation and Its Application to Surface Coating for Display book July 2005
Preparation of a Novel Macroporous Silica-based Diglycolamide Derivative-impregnated Polymeric Composite and its Adsorption Mechanism for Rare Earth Metal Ions journal June 2007
Studies on the Separation of Minor Actinides from High-Level Wastes by Extraction Chromatography Using Novel Silica-Based Extraction Resins journal December 2000
Evaluation study on a macroporous silica-based isohexyl-BTP adsorbent for minor actinides separation from nitric acid medium journal January 2014
Sorption of americium(III) and europium(III) from nitric acid solutions by a novel diglycolamide-grafted silica-based resins: Part 2. Sorption isotherms, column and radiolytic stability studies journal January 2014
Recovery of actinides and lanthanides from high-level liquid waste by extraction chromatography using TODGA+TBP impregnated resins journal January 2007
Extraction and separation of Am(III) and Sr(II) by N,N,N´,N´-tetraoctyl-3-oxapentanediamide (TODGA) journal January 2004

Cited By (5)

Preparation of diglycolamide polymer modified silica and its application as adsorbent for rare earth ions text January 2019
Investigation of U(VI), Th(IV), and Eu(III) ions’ sorption behavior onto silica gel modified with anhydride journal July 2019
Functionalization of mesoporous materials for lanthanide and actinide extraction journal January 2016
Preparation of a mesocellular siliceous foam supported lanthanide-sensitive polymer for the selective adsorption of lanthanides journal January 2018
Preparation of diglycolamide polymer modified silica and its application as adsorbent for rare earth ions journal January 2019

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americium
diglycolamide
europium
mesoporous silica
separations
solid-state NMR