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Title: Multiscale Speciation of U and Pu at Chernobyl, Hanford, Los Alamos, McGuire AFB, Mayak, and Rocky Flats

Journal Article · · Environmental Science and Technology
DOI:https://doi.org/10.1021/es506145b· OSTI ID:1454610
 [1];  [2];  [3];  [1];  [4];  [1];  [5];  [6];  [7];  [8];  [6];  [9];  [1];  [6];  [1];  [10];  [11];  [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Synchrotron-SOLEIL, Saint-Auben (France)
  3. Ural Federal Univ., Ekaterinburg (Russian Federation)
  4. V.G. Khlopin Radium Inst., St. Petersburg (Russian Federation)
  5. Univ. of Nevada, Las Vegas, NV (United States)
  6. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  7. Stanford Univ., CA (United States)
  8. Moscow State Univ., Moscow (Russian Federation); Russian Academy of Sciences (RAS), Moscow (Russian Federation). Frumkin Inst. of Physical Chemistry and Electrochemistry
  9. Russian Academy of Sciences (RAS), Moscow (Russian Federation). Frumkin Inst. of Physical Chemistry and Electrochemistry
  10. Moscow State Univ., Moscow (Russian Federation)
  11. SLAC National Accelerator Lab., Menlo Park, CA (United States)
+ Show Author Affiliations

The speciation of U and Pu in soil and concrete from Rocky Flats and in particles from soils from Chernobyl, Hanford, Los Alamos, and McGuire Air Force Base and bottom sediments from Mayak was determined by a combination of X-ray absorption fine structure (XAFS) spectroscopy and X-ray fluorescence (XRF) element maps. These experiments identify four types of speciation that sometimes may and other times do not exhibit an association with the source terms and histories of these samples: relatively well ordered PuO2+x and UO2+x that had equilibrated with O2 and H2O under both ambient conditions and in fires or explosions; instances of small, isolated particles of U as UO2+x, U3O8, and U(VI) species coexisting in close proximity after decades in the environment; alteration phases of uranyl with other elements including ones that would not have come from soils; and mononuclear Pu–O species and novel PuO2+x-type compounds incorporating additional elements that may have occurred because the Pu was exposed to extreme chemical conditions such as acidic solutions released directly into soil or concrete. Our results therefore directly demonstrate instances of novel complexity in the Å and μm-scale chemical speciation and reactivity of U and Pu in their initial formation and after environmental exposure as well as occasions of unexpected behavior in the reaction pathways over short geological but significant sociological times. They also show that incorporating the actual disposal and site conditions and resultant novel materials such as those reported here may be necessary to develop the most accurate predictive models for Pu and U in the environment.

Research Organization:
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States). Nuclear Science and Security Consortium
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA)
DOE Contract Number:
NA0000979
OSTI ID:
1454610
Journal Information:
Environmental Science and Technology, Vol. 49, Issue 11; ISSN 0013-936X
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English

References (40)

Radiation-induced decomposition of U(VI) phases to nanocrystals of UO2 journal December 2005
Radioactive contamination in the environment of the nuclear enterprise ‘Mayak’ PA. Results from the joint Russian-Norwegian field work in 1994 journal August 1997
A new uranyl oxide hydrate phase derived from spent fuel alteration journal September 1997
High energy X-ray microscopy for characterisation of fuel particles
  • Salbu, B.; Krekling, T.; Lind, O. C.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 467-468 https://doi.org/10.1016/S0168-9002(01)00641-6
journal July 2001
Plutonium in groundwater at the 100K-Area of the U.S. DOE Hanford Site journal February 2005
Plutonium contamination issues in Hanford soils and sediments: Discharges from the Z-Plant (PFP) complex journal January 2010
Nuclear Fuel in a Reactor Accident journal March 2012
Uranium release and secondary phase formation during unsaturated testing of UO2 at 90°C journal August 1992
Speciation of Uranium in Fernald Soils by Molecular Spectroscopic Methods:  Characterization of Untreated Soils journal January 1996
The Behavior of Nuclear Fuel in First Days of the Chernobyl Accident journal January 1996
Alteration of UO2+x under oxidizing conditions, Marshall Pass, Colorado, USA journal October 2007
Morphology of actinide-rich particles released from the BOMARC accident and collected from soil post remediation journal September 2012
Uranium Speciation As a Function of Depth in Contaminated Hanford Sediments - A Micro-XRF, Micro-XRD, and Micro- And Bulk-XAFS Study journal February 2009
Up-to-date radioecological situation around the `Mayak' nuclear facility journal June 1998
Radionuclides released to the environment following nuclear events journal June 2011
Uranium minerals and their relevance to long term storage of nuclear fuels journal May 2014
Local and Nanoscale Structure and Speciation in the PuO 2+ x - y (OH) 2 y · z H 2 O System journal October 2004
Pu and U Atom Ratios and Concentration Factors in Reservoir 11 and Asanov Swamp, Mayak PA:  An Application of Accelerator Mass Spectrometry journal December 2004
Ten-year results from unsaturated drip tests with UO2 at 90°C: implications for the corrosion of spent nuclear fuel journal October 1996
Local Structure and Charge Distribution in the UO 2 −U 4 O 9 System journal November 2004
Characterization of transuranic solid wastes from a plutonium processing facility report June 1975
Speciation of radionuclides – analytical challenges within environmental impact and risk assessments journal July 2007
Chemical speciation of heterogeneously reduced Pu in synthetic brines journal May 2006
Colloid Formation in Hanford Sediments Reacted with Simulated Tank Waste journal November 2004
Sorption of Co(II) on Metal Oxide Surfaces journal September 1999
Oxidation-hydration weathering of uraninite: the current state-of-knowledge journal April 2014
Plutonium Transport in the Environment journal June 2012
Fuel corrosion processes under waste disposal conditions journal November 2000
Charge distribution and local structure and speciation in the UO2+x and PuO2+x binary oxides for x⩽0.25 journal February 2005
Rocky Flats closure: The role of models in facilitating scientific communication with stakeholder groups journal October 2007
Speciation and Unusual Reactivity in PuO 2+ x journal June 2003
The product of microbial uranium reduction includes multiple species with U(IV)–phosphate coordination journal April 2014
Hot particles — a challenge within radioecology journal April 2001
Rapid, quantitative analysis of americium, curium and plutonium isotopes in Hanford samples using extraction chromatography and precipitation plating journal July 1995
Local structure in solid solutions of stabilised zirconia with actinide dioxides (UO2, NpO2) journal April 2011
XANES identification of plutonium speciation in RFETS samples journal October 2007
Solid state speciation and potential bioavailability of depleted uranium particles from Kosovo and Kuwait journal April 2009
Local atomic structure in cubic stabilized zirconia journal August 2001
Uranium passivation by C+ implantation: A photoemission and secondary ion mass spectrometry study journal March 2006
Surface complexation of Pb(II) at oxide-water interfaces: II. XAFS and bond-valence determination of mononuclear Pb(II) sorption products and surface functional groups on iron oxides journal July 1997

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