DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Technetium immobilization by materials through sorption and redox-driven processes: A literature review

Journal Article · · Science of the Total Environment

The purpose of this review is to evaluate materials for use as a barrier or other deployed technology to treat technetium-99 (Tc) in the subsurface. To achieve this, Tc interactions with different materials are considered within the context of remediation strategies. Several naturally occurring materials are considered for Tc immobilization, including iron oxides and low solubility sulfide phases. Synthetic materials are also considered, and include tin-based materials, sorbents (resins, activated carbon, modified clays), layered double hydroxides, metal organic frameworks, cationic polymeric networks and aerogels. All of the materials were evaluated for their potential in-situ and ex-situ performance with respect to long-term Tc uptake and immobilization, environmental impacts and deployability. Other factors such as the technology maturity, cost and availability were also considered. Given the difficulty of evaluating materials under different experimental conditions (e.g., solution chemistry, redox conditions, solution to solid ratio, Tc concentration etc.), a subset of these materials will be selected, on the basis of this review, for subsequent standardized batch loading tests.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC05-76RL01830
OSTI ID:
1601144
Alternate ID(s):
OSTI ID: 1638577
Report Number(s):
PNNL-SA-138464
Journal Information:
Science of the Total Environment, Vol. 716, Issue 10; ISSN 0048-9697
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

References (90)

Synthesis and characterization of MgO-B2O3 mixed oxides prepared by coprecipitation; selective dehydrogenation of propan-2-ol journal January 1999
Synthesis and characterization of a novel Mg/In layered double hydroxide journal January 1999
The function of Sn(II)-apatite as a Tc immobilizing agent journal November 2016
Removal of Pertechnetate-Related Oxyanions from Solution Using Functionalized Hierarchical Porous Frameworks journal October 2016
Removal of TcO 4 ions from solution: materials and future outlook journal January 2016
New hydrotalcite-type anionic clays containing noble metals journal January 1996
Development of Bifunctional Anion-Exchange Resins with Improved Selectivity and Sorptive Kinetics for Pertechnetate:  Batch-Equilibrium Experiments journal September 2000
The identification of FeS2 as a sorption sink for Tc(IV) journal January 2007
Catalysts for low-temperature methanol synthesis. Preparation of Cu$z.dbnd;Zn$z.dbnd;Al mixed oxides via hydrotalcite-like precursors journal January 1984
Layered double hydroxides (LDHs) journal March 1988
Hydrotalcite-type anionic clays: Preparation, properties and applications. journal December 1991
Low-Temperature Synthesis of Mg x Co 1 - x Co 2 O 4 Spinel Catalysts for N 2 O Decomposition journal March 2000
Adsorption of phosphate by layered double hydroxides in aqueous solutions journal May 2006
Technetium-99 Removal from Process Solutions and Contaminated Groundwater journal January 1993
Behaviour of 99Tc in aqueous solutions in the presence of iron oxides and microorganisms journal July 2014
Ion exchange behaviour of hydrous tin oxide: Kinetics of anion exchange journal June 1992
Electrosorption and Reduction of Pertechnetate by Anodically Polarized Magnetite journal April 1999
Preparation and thermal stability of manganese-containing hydrotalcite, [Mg 0.75 Mn II 0.04 Mn III 0.21 (OH) 2 ](CO 3 ) 0.11 ·nH 2 O journal January 1994
Application of layered double hydroxides for removal of oxyanions: A review journal March 2008
Efficient separation and recovery of technetium-99 from contaminated groundwater journal April 1996
Direct Extraction of Ag + and Hg 2+ from Cyanide Complexes and Mode of Binding by the Layered K 2 MgSn 2 S 6 (KMS-2) journal March 2015
XAFS Study of the Chemical and Structural States of Technetium in Fe(III) Oxide Co-Precipitates
  • Heald, Steve M.; Zachara, John M.; Jeon, Byong-Hun
  • X-RAY ABSORPTION FINE STRUCTURE - XAFS13: 13th International Conference, AIP Conference Proceedings https://doi.org/10.1063/1.2644465
conference January 2007
Incorporation of pertechnetate and perrhenate into corroded steel surfaces studied by X-ray absorption fine structure spectroscopy journal April 2012
The biogeochemistry of technetium: A review of the behavior of an artificial element in the natural environment journal October 2010
Sorption of MO4- (M = Tc, Re) on Mg/Al Layered Double Hydroxide by Anion Exchange journal January 1996
Functional Monolithic Polymeric Organic Framework Aerogel as Reducing and Hosting Media for Ag nanoparticles and Application in Capturing of Iodine Vapors journal May 2012
Sorption of Tungsten(Vi) and Rhenium(Vii) on Various Ion-Exchange Materials journal December 2001
Selective Sorption of Technetium on Antimony-Doped Tin Dioxide journal December 2010
Synthesis and Characterization of Hydrotalcite-like Compounds Containing V 3+ in the Layers and of Their Calcination Products journal January 1996
The crystal structure of some rhenium and technetium dichalcogenides journal August 1996
Inorganic tin aluminophosphate nanocomposite for reductive separation of pertechnetate journal January 2016
Sorption coefficients and molecular mechanisms of Pu, U, Np, Am and Tc to Fe (hydr)oxides: A review journal December 2012
Aqueous 99Tc, 129I and 137Cs removal from contaminated groundwater and sediments using highly effective low-cost sorbents journal October 2014
99TcO4− remediation by a cationic polymeric network journal August 2018
Technetium in the Hydrosphere and in the Geosphere journal January 1987
Pertechnetate immobilization with amorphous iron sulfide journal January 2008
Tc(VII) reduction kinetics by titanomagnetite (Fe3−xTixO4) nanoparticles journal September 2012
X-ray absorption spectroscopy studies of reactions of technetium, uranium and neptunium with mackinawite journal January 2004
Incorporation of Technetium into Spinel Ferrites journal November 2016
Incorporating technetium in minerals and other solids: A review journal November 2015
Layered Metal Sulfides Capture Uranium from Seawater journal September 2012
Incorporation and Retention of 99-Tc(IV) in Magnetite under High pH Conditions journal October 2014
Functionalized Silica Aerogels: Advanced Materials to Capture and Immobilize Radioactive Iodine book September 2011
Silica-based waste form for immobilization of iodine from reprocessing plant off-gas streams journal August 2016
Selective Removal of Cs + , Sr 2+ , and Ni 2+ by K 2 x Mg x Sn 3– x S 6 ( x = 0.5–1) (KMS-2) Relevant to Nuclear Waste Remediation journal May 2013
Anion-exchange reactions of layered double hydroxides journal December 1990
Synthesis of new Hydrotalcite-Like Compounds and Their Physico-Chemical Properties journal August 1973
Size-Driven Structural and Thermodynamic Complexity in Iron Oxides journal March 2008
Removal of TcO 4 from Representative Nuclear Waste Streams with Layered Potassium Metal Sulfide Materials journal May 2016
Zn, Al, Rh-mixed oxides derived from hydrotalcite-like compound and their catalytic properties for N2O decomposition journal November 1997
Synthesis and properties of titanomagnetite (Fe3−xTixO4) nanoparticles: A tunable solid-state Fe(II/III) redox system journal December 2012
Technetium Stabilization in Low-Solubility Sulfide Phases: A Review journal April 2018
Treatment of radioactive wastes: An X-ray absorption spectroscopy study of the reaction of technetium with green rust journal December 2003
Heterogeneous reduction of Tc(VII) by Fe(II) at the solid–water interface journal March 2008
Reduction of Tc(VII) by Fe(II) Sorbed on Al (hydr)oxides journal August 2008
Structural promotion and stabilizing effect of Mg in the catalytic decomposition of nitrous oxide over calcined hydrotalcite-like compounds journal October 1999
Chalcogen-Based Aerogels As Sorbents for Radionuclide Remediation journal June 2013
A new hydrotalcite-like compound containing vanadium(3+) ions in the layers journal November 1993
The effect of interlayer anion on the reactivity of Mg–Al layered double hydroxides: Improving and extending the customization capacity of anionic clays journal July 2011
Insights on the Structural Chemistry of Hydrocalumite and Hydrotalcite-like Materials: Investigation of the Series Ca2M3+(OH)6Cl·2H2O (M3+: Al3+, Ga3+, Fe3+, and Sc3+) by X-Ray Powder Diffraction journal August 2002
Reduction and Simultaneous Removal of 99 Tc and Cr by Fe(OH) 2 (s) Mineral Transformation journal July 2017
Extraction and Reductive Stripping of Pertechnetate from Spent Nuclear Fuel Waste Streams journal February 2011
Technetium Incorporation into Hematite (α-Fe 2 O 3 ) journal August 2010
Technetium Incorporation into Goethite (α-FeOOH): An Atomic-Scale Investigation journal October 2015
Computational Investigation of Technetium(IV) Incorporation into Inverse Spinels: Magnetite (Fe 3 O 4 ) and Trevorite (NiFe 2 O 4 ) journal April 2016
Radioactive Iodine and Krypton Control for Nuclear Fuel Reprocessing Facilities journal January 2013
The Sorption of Technetium and Iodine Radioisotopes by Various Minerals journal July 1980
The rapid formation of crystalline double hydroxy salts and other compounds by controlled hydrolysis journal September 1984
Tc removal from the waste treatment and immobilization plant low-activity waste vitrification off-gas recycle journal May 2017
Immobilization of 99-Technetium (VII) by Fe(II)-Goethite and Limited Reoxidation journal June 2011
Iron oxide waste form for stabilizing 99Tc journal October 2012
Uranium and technetium interactions with wüstite [Fe 1–x O] and portlandite [Ca(OH) 2 ] surfaces under geological disposal facility conditions journal October 2014
New hydrotalcite-like anionic clays containing Zr4+ in the layers journal January 1997
New Hydrotalcite-like Anionic Clays Containing Zr 4+ in the Layers:  Synthesis and Physicochemical Properties journal November 1998
Synthesis of New Sn-Incorporated Layered Double Hydroxides and Their Thermal Evolution to Mixed Oxides journal August 1999
An Injectable Apatite Permeable Reactive Barrier for In Situ 90 Sr Immobilization journal April 2014
Preparation of Cd/Al layered double hydroxides and their intercalation reactions with phosphonic acids journal January 1997
Compositional and structural control on anion sorption capability of layered double hydroxides (LDHs) journal September 2006
NDTB-1: A Supertetrahedral Cationic Framework That Removes TcO 4 from Solution journal February 2010
Selectivity, Kinetics, and Efficiency of Reversible Anion Exchange with TcO4− in a Supertetrahedral Cationic Framework journal March 2012
Synthesis of Organically Templated Nanoporous Tin(II/IV) Phosphate for Radionuclide and Metal Sequestration journal March 2006
An X-ray absorption spectroscopy study of the coprecipitation of Tc and Re with mackinawite (FeS) journal March 2000
The sorption of anionic species on hydrous tin dioxide journal February 1997
Control of Surface Area and Porosity of Co 3 O 4 via Intercalation of Oxidative or Nonoxidative Anions in Hydrotalcite-like Precursors journal November 2000
In-Situ Generation of Maximum Trivalent Cobalt in Synthesis of Hydrotalcite-like Compounds Mg x Co II 1 - x - y Co III y (OH) 2 (NO 3 ) y · n H 2 O journal August 2000
A new approach for design and synthesis of CoII and CoII,III hydroxide materials journal June 2000
Systematic XAS study on the reduction and uptake of Tc by magnetite and mackinawite journal January 2016
Geomaterials: their application to environmental remediation journal December 2011
Identifying the Recognition Site for Selective Trapping of 99 TcO 4 in a Hydrolytically Stable and Radiation Resistant Cationic Metal–Organic Framework journal October 2017
Retardation of Technetium and Iodine by Antimony- and Mercury-Containing Minerals journal January 1995

Cited By (1)

The abiotic reductive removal and subsequent incorporation of Tc( iv ) into iron oxides: a frontier review journal January 2019

Figures / Tables (11)