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Title: Hydrothermal Testing of K Basin Sludge and N Reactor Fuel at Sludge Treatment Project Operating Conditions

Abstract

The Sludge Treatment Project (STP), managed for the U. S. DOE by Fluor Hanford (FH), was created to design and operate a process to eliminate uranium metal from K Basin sludge prior to packaging for Waste Isolation Pilot Plant (WIPP). The STP process uses high temperature liquid water to accelerate the reaction, produce uranium dioxide from the uranium metal, and safely discharge the hydrogen. Under nominal process conditions, the sludge will be heated in pressurized water at 185°C for as long as 72 hours to assure the complete reaction (corrosion) of up to 0.25-inch diameter uranium metal pieces. Under contract to FH, the Pacific Northwest National Laboratory (PNNL) conducted bench-scale testing of the STP hydrothermal process in November and December 2006. Five tests (~50 ml each) were conducted in sealed, un-agitated reaction vessels under the hydrothermal conditions (e.g., 7 to 72 h at 185°C) of the STP corrosion process using radioactive sludge samples collected from the K East Basin and particles/coupons of N Reactor fuel also taken from the K Basins. The tests were designed to evaluate and understand the chemical changes that may be occurring and the effects that any changes would have on sludge rheological properties. The testsmore » were not designed to evaluate engineering aspects of the process. The hydrothermal treatment affected the chemical and physical properties of the sludge. In each test, significant uranium compound phase changes were identified, resulting from dehydration and chemical reduction reactions. Physical properties of the sludge were significantly altered from their initial, as-settled sludge values, including, shear strength, settled density, weight percent water, and gas retention.« less

Authors:
; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
936766
Report Number(s):
PNNL-16496
830403000; TRN: US0806002
DOE Contract Number:
AC05-76RL01830
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN; 12 MANAGEMENT OF RADIOACTIVE WASTES, AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; CORROSION; DEHYDRATION; DESIGN; HYDROGEN; N-REACTOR; PACKAGING; PHOSPHORS; PHYSICAL PROPERTIES; RETENTION; SHEAR PROPERTIES; SLUDGES; TESTING; URANIUM; URANIUM COMPOUNDS; URANIUM DIOXIDE; WATER; WIPP; corrosion process; hydrothermal treatment; energy dispersive spectroscopy (EDS); K Basin; KE Basin, K East Basin; KW Basin; K West Basin; Sludge Treatment Project (STP); K Basin Closure (KBC); Hanford; spent nuclear fuel; sludge rheology; shear strength; X-ray diffraction (XRD); characterization; scanning electron microscopy (SEM); phase identification; unconfined compressive strength; uranium; uranium metal reaction; N Reactor Fuel; metaschoepite; dehydrated schoepite; soddyite; ianthinite

Citation Formats

Delegard, Calvin H., Schmidt, Andrew J., and Thornton, Brenda M. Hydrothermal Testing of K Basin Sludge and N Reactor Fuel at Sludge Treatment Project Operating Conditions. United States: N. p., 2007. Web. doi:10.2172/936766.
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Delegard, Calvin H., Schmidt, Andrew J., & Thornton, Brenda M. Hydrothermal Testing of K Basin Sludge and N Reactor Fuel at Sludge Treatment Project Operating Conditions. United States. doi:10.2172/936766.
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Delegard, Calvin H., Schmidt, Andrew J., and Thornton, Brenda M. Fri . "Hydrothermal Testing of K Basin Sludge and N Reactor Fuel at Sludge Treatment Project Operating Conditions". United States. doi:10.2172/936766. https://www.osti.gov/servlets/purl/936766.
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@article{osti_936766,
title = {Hydrothermal Testing of K Basin Sludge and N Reactor Fuel at Sludge Treatment Project Operating Conditions},
author = {Delegard, Calvin H. and Schmidt, Andrew J. and Thornton, Brenda M.},
abstractNote = {The Sludge Treatment Project (STP), managed for the U. S. DOE by Fluor Hanford (FH), was created to design and operate a process to eliminate uranium metal from K Basin sludge prior to packaging for Waste Isolation Pilot Plant (WIPP). The STP process uses high temperature liquid water to accelerate the reaction, produce uranium dioxide from the uranium metal, and safely discharge the hydrogen. Under nominal process conditions, the sludge will be heated in pressurized water at 185°C for as long as 72 hours to assure the complete reaction (corrosion) of up to 0.25-inch diameter uranium metal pieces. Under contract to FH, the Pacific Northwest National Laboratory (PNNL) conducted bench-scale testing of the STP hydrothermal process in November and December 2006. Five tests (~50 ml each) were conducted in sealed, un-agitated reaction vessels under the hydrothermal conditions (e.g., 7 to 72 h at 185°C) of the STP corrosion process using radioactive sludge samples collected from the K East Basin and particles/coupons of N Reactor fuel also taken from the K Basins. The tests were designed to evaluate and understand the chemical changes that may be occurring and the effects that any changes would have on sludge rheological properties. The tests were not designed to evaluate engineering aspects of the process. The hydrothermal treatment affected the chemical and physical properties of the sludge. In each test, significant uranium compound phase changes were identified, resulting from dehydration and chemical reduction reactions. Physical properties of the sludge were significantly altered from their initial, as-settled sludge values, including, shear strength, settled density, weight percent water, and gas retention.},
doi = {10.2172/936766},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Fri Mar 30 00:00:00 EDT 2007},
month = {Fri Mar 30 00:00:00 EDT 2007}
}
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DOI:  10.2172/936766
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  • ; ;
    This report establishes the technical bases for using a ''slow uptake'' instead of a ''moderate uptake'' transportability class for americium-241 (241Am) for the K Basin Sludge Treatment Project (STP) dose consequence analysis. Slow uptake classes are used for most uranium and plutonium oxides. A moderate uptake class has been used in prior STP analyses for 241Am based on the properties of separated 241Am and its associated oxide. However, when 241Am exists as an ingrown progeny (and as a small mass fraction) within plutonium mixtures, it is appropriate to assign transportability factors of the predominant plutonium mixtures (typically slow) to themore » Am241. It is argued that the transportability factor for 241Am in sludge likewise should be slow because it exists as a small mass fraction as the ingrown progeny within the uranium oxide in sludge. In this report, the transportability class assignment for 241Am is underpinned with radiochemical characterization data on K Basin sludge and with studies conducted with other irradiated fuel exposed to elevated temperatures and conditions similar to the STP. Key findings and conclusions from evaluation of the characterization data and published literature are summarized here. Plutonium and 241Am make up very small fractions of the uranium within the K Basin sludge matrix. Plutonium is present at about 1 atom per 500 atoms of uranium and 241Am at about 1 atom per 19000 of uranium. Plutonium and americium are found to remain with uranium in the solid phase in all of the {approx}60 samples taken and analyzed from various sources of K Basin sludge. The uranium-specific concentrations of plutonium and americium also remain approximately constant over a uranium concentration range (in the dry sludge solids) from 0.2 to 94 wt%, a factor of {approx}460. This invariability demonstrates that 241Am does not partition from the uranium or plutonium fraction for any characterized sludge matrix. Most of the K Basin sludge characterization data is derived spent nuclear fuel corroded within the K Basins at 10-15?C. The STP process will place water-laden sludges from the K Basin in process vessels at {approx}150-180 C. Therefore, published studies with other irradiated (uranium oxide) fuel were examined. From these studies, the affinity of plutonium and americium for uranium in irradiated UO2 also was demonstrated at hydrothermal conditions (150 C anoxic liquid water) approaching those proposed for the STP process and even for hydrothermal conditions outside of the STP operating envelope (e.g., 150 C oxic and 100 C oxic and anoxic liquid water). In summary, by demonstrating that the chemical and physical behavior of 241Am in the sludge matrix is similar to that of the predominant species (uranium and for the plutonium from which it originates), a technical basis is provided for using the slow uptake transportability factor for 241Am that is currently used for plutonium and uranium oxides. The change from moderate to slow uptake for 241Am could reduce the overall analyzed dose consequences for the STP by more than 30%.« less

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  • ; ;
    Approximately 2100 metric tons of irradiated N Reactor fuel are stored in the KE and KW Basins at the Hanford Site, Richland, Washington. Corrosion of the fuel has led to the formation of sludges, both within the storage canisters and on the basin floors. Concern about the degraded condition of the fuel and the potential for leakage from the basins in proximity to the Columbia River has resulted in DOE`s commitment in the Tri-Party Agreement (TPA) to Milestone M-34-00-T08 to remove the fuel and sludges by a December 2002 target date. To support the planning for this expedited removal action,more » the implications of sludge management under various scenarios are examined. Volume 1 of this two-volume report describes the regulatory options for managing the sludges, including schedule and cost impacts, and assesses strategies for establishing a preferred path.« less