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Title: FRACTIONAL CRYSTALLIZATION OF HANFORD SINGLE SHELL TANK (SST) WASTES A MODELING APPROACH

Abstract

The Hanford site has 149 underground single-shell tanks (SST) storing mostly soluble, multi-salt, mixed wastes resulting from Cold War era weapons material production. These wastes must be retrieved and the salts immobilized before the tanks can be closed to comply with an overall site closure consent order entered into by the U.S. Department of Energy (DOE), the Environmental Protection Agency, and Washington State. Water will be used to retrieve the wastes and the resulting solution will be pumped to the proposed treatment process where a high curie (primarily {sup 137}Cs) waste fraction will be separated from the other waste constituents. The separated waste streams will then be vitrified to allow for safe storage as an immobilized high level waste, or low level waste, borosilicate glass. Fractional crystallization, a common unit operation for production of industrial chemicals and pharmaceuticals, was proposed as the method to separate the salt wastes; it works by evaporating excess water until the solubilities of various species in the solution are exceeded (the solubility of a particular species depends on its concentration, temperature of the solution, and the presence of other ionic species in the solution). By establishing the proper conditions, selected pure salts can be crystallizedmore » and separated from the radioactive liquid phase.« less

Authors:
Publication Date:
Research Org.:
Hanford Site (HNF), Richland, WA
Sponsoring Org.:
USDOE - Office of Environmental Management (EM)
OSTI Identifier:
896896
Report Number(s):
RPP-30993-FP Rev 0
TRN: US0700825
DOE Contract Number:
DE-AC27-99RL14047
Resource Type:
Conference
Resource Relation:
Conference: WM07 WASTE MANAGEMENT SYPMPOSIA (DOE) 02/25/2007 THRU 03/01/2007 TUCSON AZ
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE WASTES, AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; BOROSILICATE GLASS; CRYSTALLIZATION; EVAPORATION; KINETICS; NUCLEATION; PILOT PLANTS; SEPARATION EQUIPMENT; SOLUBILITY; LIQUID WASTES; RADIOACTIVE WASTE PROCESSING; RADIOACTIVE WASTE FACILITIES; HANFORD RESERVATION

Citation Formats

HAMILTON, D.W. FRACTIONAL CRYSTALLIZATION OF HANFORD SINGLE SHELL TANK (SST) WASTES A MODELING APPROACH. United States: N. p., 2006. Web.
HAMILTON, D.W. FRACTIONAL CRYSTALLIZATION OF HANFORD SINGLE SHELL TANK (SST) WASTES A MODELING APPROACH. United States.
HAMILTON, D.W. Thu . "FRACTIONAL CRYSTALLIZATION OF HANFORD SINGLE SHELL TANK (SST) WASTES A MODELING APPROACH". United States. doi:. https://www.osti.gov/servlets/purl/896896.
@article{osti_896896,
title = {FRACTIONAL CRYSTALLIZATION OF HANFORD SINGLE SHELL TANK (SST) WASTES A MODELING APPROACH},
author = {HAMILTON, D.W.},
abstractNote = {The Hanford site has 149 underground single-shell tanks (SST) storing mostly soluble, multi-salt, mixed wastes resulting from Cold War era weapons material production. These wastes must be retrieved and the salts immobilized before the tanks can be closed to comply with an overall site closure consent order entered into by the U.S. Department of Energy (DOE), the Environmental Protection Agency, and Washington State. Water will be used to retrieve the wastes and the resulting solution will be pumped to the proposed treatment process where a high curie (primarily {sup 137}Cs) waste fraction will be separated from the other waste constituents. The separated waste streams will then be vitrified to allow for safe storage as an immobilized high level waste, or low level waste, borosilicate glass. Fractional crystallization, a common unit operation for production of industrial chemicals and pharmaceuticals, was proposed as the method to separate the salt wastes; it works by evaporating excess water until the solubilities of various species in the solution are exceeded (the solubility of a particular species depends on its concentration, temperature of the solution, and the presence of other ionic species in the solution). By establishing the proper conditions, selected pure salts can be crystallized and separated from the radioactive liquid phase.},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Thu Dec 21 00:00:00 EST 2006},
month = {Thu Dec 21 00:00:00 EST 2006}
}

Conference:
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  • Laboratory studies demonstrate that fractional crystallization is a viable process for separating Hanford medium-curie waste into high-curie and low-curie fractions. The product salt from the crystallization process qualifies as low-curie feed to a supplemental treatment system (e.g., bulk vitrification). The high-curie raffinate is returned to the double-shell tank system, eventually to be sent as feed to the Waste Treatment and Immobilization Plant. Process flowsheet tests were designed with the aid of thermodynamic chemical modeling. Laboratory equipment design and test procedures were developed using simulated tank waste samples. Proof-of-concept flowsheet tests were carried out in a shielded hot cell using actualmore » tank waste samples. Data from both simulated waste tests and actual tank waste tests demonstrate that the process exceeded all of the separation criteria established for the program.« less
  • The Hanford site has 149 underground single-shell tanks (SST) storing mostly soluble, multi-salt mixed wastes resulting from Cold War era weapons material production. These wastes must be retrieved and the salts immobilized before the tanks can be closed to comply with an overall site-closure consent order entered into by the US Department of Energy, the Environmental Protection Agency, and the State of Washington. Water will be used to retrieve the wastes and the resulting solution will be pumped to a proposed pretreatment process where a high-curie (primarily {sup 137}Cs) waste fraction will be separated from the other waste constituents. Themore » separated waste streams will then be vitrified to allow for safe storage as an immobilized high-level waste, or low-level waste, borosilicate glass. Fractional crystallization, a common unit operation for production of industrial chemicals and pharmaceuticals, was proposed as the method to separate the salt wastes; it works by evaporating excess water until the solubilities of various species in the solution are exceeded (the solubility of a particular species depends on its concentration, temperature of the solution, and the presence of other ionic species in the solution). By establishing the proper conditions, selected pure salts can be crystallized and separated from the radioactive liquid phase. The aforementioned parameters, along with evaporation rate, proper agitation, and residence time, determine nucleation and growth kinetics and the resulting habit and size distribution of the product crystals. These crystals properties are important considerations for designing the crystallizer and solid/liquid separation equipment. A structured program was developed to (a) demonstrate that fractional crystallization could be used to pre-treat Hanford tank wastes and (b) provide data to develop a pilot plant design.« less
  • The ''Initial Single-Shell Tank System Performance Assessment for the Hanford Site [1] (SST PA) presents the analysis of the long-term impacts of residual wastes assumed to remain after retrieval of tank waste and closure of the SST farms at the US Department of Energy (DOE) Hanford Site. The SST PA supports key elements of the closure process agreed upon in 2004 by DOE, the Washington State Department of Ecology (Ecology), and the US Environmental Protection Agency (EPA). The SST PA element is defined in Appendix I of the ''Hanford Federal Facility Agreement and Consent Order'' (HFFACO) (Ecology et al. 1989)more » [2], the document that establishes the overall closure process for the SST and double-shell tank (DST) systems. The approach incorporated in the SST PA integrates substantive features of both hazardous and radioactive waste management regulations into a single analysis. The defense-in-depth approach used in this analysis defined two major engineering barriers (a surface barrier and the grouted tank structure) and one natural barrier (the vadose zone) that will be relied on to control waste release into the accessible environment and attain expected performance metrics. The analysis evaluates specific barrier characteristics and other site features that influence contaminant migration by the various pathways. A ''reference'' case and a suite of sensitivity/uncertainty cases are considered. The ''reference case'' evaluates environmental impacts assuming central tendency estimates of site conditions. ''Reference'' case analysis results show residual tank waste impacts on nearby groundwater, air resources; or inadvertent intruders to be well below most important performance objectives. Conversely, past releases to the soil, from previous tank farm operations, are shown to have groundwater impacts that re significantly above most performance objectives. Sensitivity/uncertainty cases examine single and multiple parameter variability along with plausible alternatives to ''reference'' cases to judge how the proposed closure system performs when changes to important assumptions are made to the hydrogeologic and engineered systems. The estimated impacts from these cases are generally consistent with ''reference'' case results (i.e., performance objectives are exceeded by contaminants from past releases but not tank residuals). This document and its future iterations will play a critical role in the decision making process for the closure of the Hanford Tank Farms. It will support interim decisions related to tank retrievals and interim corrective measures, in addition to supporting the major closure decisions of tanks and tank farms. Hence, it is imperative that the review process of this document is inclusive of the decision makers as well as the Hanford Stakeholders.« less
  • To improve the understanding of the single-shell tanks (SSTs) integrity, Washington River Protection Solutions, LLC (WRPS), the USDOE Hanford Site tank contractor, developed an enhanced Single-Shell Tank Integrity Project in 2009. An expert panel on SST integrity, consisting of various subject matters experts in industry and academia, was created to provide recommendations supporting the development of the project. This panel developed 33 recommendations in four main areas of interest: structural integrity, liner degradation, leak integrity and prevention, and mitigation of contamination migration. Seventeen of these recommendations were used to develop the basis for the M-45-10-1 Change Package for the Hanfordmore » Federal Agreement and Compliance Order, which is also known as the Tri-Party Agreement. The structural integrity of the tanks is a key element in completing the cleanup mission at the Hanford Site. There are eight primary recommendations related to the structural integrity of Hanford SSTs. Six recommendations are being implemented through current and planned activities. The structural integrity of the Hanford SSTs is being evaluated through analysis, monitoring, inspection, materials testing, and construction document review. Structural evaluation in the form of analysis is performed using modern finite element models generated in ANSYS{reg_sign} The analyses consider in-situ, thermal, operating loads and natural phenomena such as earthquakes. Structural analysis of 108 of 149 Hanford SSTs has concluded that the tanks are structurally sound and meet current industry standards. Analyses of the remaining Hanford SSTs are scheduled for FY2013. Hanford SSTs are monitored through a dome deflection program. The program looks for deflections of the tank dome greater than 1/4 inch. No such deflections have been recorded. The tanks are also subjected to visual inspection. Digital cameras record the interior surface of the concrete tank domes, looking for cracks and other surface conditions that may indicate signs of structural distress. The condition of the concrete and rebar of the Hanford SSTs is currently being tested and planned for additional activities in the near future. Concrete and rebar removed from the dome of a 65-year-old tank is being tested for mechanics properties and condition. Results indicated stronger than designed concrete with additional Petrographic examination and rebar testing ongoing. Material properties determined from previous efforts combined with current testing and construction document review will help to generate a database that will provide continuing indication of Hanford SST structural integrity.« less