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Title: Literature review of the potential impact of glycolic acid on the technetium chemistry of srs tank waste

Abstract

This document presents a literature study of the impact of glycolate on technetium chemistry in the Savannah River Site (SRS) waste system and specifically Saltstone. A predominant portion of the Tc at SRS will be sent to the Saltstone Facility where it will be immobilized. The Tc in the tank waste is in the highly soluble chemical form of pertechnetate ion (TcO 4 -) which is reduced by blast furnace slag (BFS) in Saltstone, rendering it highly insoluble and resistant to leaching.

Authors:
 [1];  [1]
  1. Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
Publication Date:
Research Org.:
Savannah River Site (SRS), Aiken, SC (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1407927
Report Number(s):
SRNL-STI-2017-00382
TRN: US1800028
DOE Contract Number:
AC09-08SR22470
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; GLYCOLIC ACID; TECHNETIUM; WASTES; PERTECHNETATES; BLAST FURNACES; technetium; saltstone

Citation Formats

Nash, Charles A., and McCabe, Daniel J.. Literature review of the potential impact of glycolic acid on the technetium chemistry of srs tank waste. United States: N. p., 2017. Web. doi:10.2172/1407927.
Nash, Charles A., & McCabe, Daniel J.. Literature review of the potential impact of glycolic acid on the technetium chemistry of srs tank waste. United States. doi:10.2172/1407927.
Nash, Charles A., and McCabe, Daniel J.. 2017. "Literature review of the potential impact of glycolic acid on the technetium chemistry of srs tank waste". United States. doi:10.2172/1407927. https://www.osti.gov/servlets/purl/1407927.
@article{osti_1407927,
title = {Literature review of the potential impact of glycolic acid on the technetium chemistry of srs tank waste},
author = {Nash, Charles A. and McCabe, Daniel J.},
abstractNote = {This document presents a literature study of the impact of glycolate on technetium chemistry in the Savannah River Site (SRS) waste system and specifically Saltstone. A predominant portion of the Tc at SRS will be sent to the Saltstone Facility where it will be immobilized. The Tc in the tank waste is in the highly soluble chemical form of pertechnetate ion (TcO4 -) which is reduced by blast furnace slag (BFS) in Saltstone, rendering it highly insoluble and resistant to leaching.},
doi = {10.2172/1407927},
journal = {},
number = ,
volume = ,
place = {United States},
year = 2017,
month =
}

Technical Report:

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  • A potential for an uncontrollable exothermic reaction between nitrate and organic salts during preparation of a high level waste melter feed has been identified. In order to examine this potential more closely, the thermal behavior of simulated neutralized current acid waste (NCAW) treated with various organic reductants was studied. Differential scanning calorimetry (DSC) measurements were collected on simulated waste samples and their supernates treated with organics. Organic reductants used were formic acid, glycolic acid, and oxalic acid. For comparison, samples of untreated simulant and untreated simulant with added noble metals were tested. When heated, untreated simulant samples both with andmore » without noble metals showed no exothermic behavior. All of the treated waste simulant samples showed exothermic behavior. Onset temperatures of exothermic reactions were 120 C to 210 C. Many onset temperatures, particularly those for formic acid treated samples, are well below 181 C, the estimated maximum steam coil temperature (considered to be a worst case maximum temperature for chemical process tank contents). The enthalpies of the reactions were {minus}180 {times} 10{sup {minus}3} J/Kg supernate ({minus}181 J/g) for the oxalic acid treated simulant supernate to {minus}1,150 {times} 10{sup {minus}3} J/Kg supernate ({minus}1,153 J/g) for the formic acid treated simulant supernate.« less
  • The Savannah River Site (SRS) has conducted performance assessment (PA) calculations to determine the risk associated with closing liquid waste tanks. The PA estimates the risk associated with a number of scenarios, making various assumptions. Throughout all of these scenarios, it is assumed that the carbon-steel tank liners holding the liquid waste do not sorb the radionuclides. Tank liners have been shown to form corrosion products, such as Fe-oxyhydroxides (Wiersma and Subramanian 2002). Many corrosion products, including Fe-oxyhydroxides, at the high pH values of tank effluent, take on a very strong negative charge. Given that many radionuclides may have netmore » positive charges, either as free ions or complexed species, it is expected that many radionuclides will sorb to corrosion products associated with tank liners. The objective of this report was to conduct a literature review to investigate whether Pu, U, Np, Am and Tc would sorb to corrosion products on tank liners after they were filled with reducing grout (cementitious material containing slag to promote reducing conditions). The approach was to evaluate radionuclides sorption literature with iron oxyhydroxide phases, such as hematite ({alpha}-Fe{sub 2}O{sub 3}), magnetite (Fe{sub 3}O{sub 4}), goethite ({alpha}-FeOOH) and ferrihydrite (Fe{sub 2}O{sub 3} {center_dot} 0.5H{sub 2}O). The primary interest was the sorption behavior under tank closure conditions where the tanks will be filled with reducing cementitious materials. Because there were no laboratory studies conducted using site specific experimental conditions, (e.g., high pH and HLW tank aqueous and solid phase chemical conditions), it was necessary to extend the literature review to lower pH studies and noncementitious conditions. Consequently, this report relied on existing lower pH trends, existing geochemical modeling, and experimental spectroscopic evidence conducted at lower pH levels. The scope did not include evaluating the appropriateness of K{sub d} values for the Fe-oxyhydroxides, but instead to evaluate whether it is a conservative assumption to exclude this sorption process of radionuclides onto tank liner corrosion products in the PA model. This may identify another source for PA conservatism since the modeling did not consider any sorption by the tank liner.« less
  • Glycolic acid is being evaluated as an alternative for formic and nitric acid in the DWPF flowsheet. Demonstration testing and modeling for this new flowsheet has shown that glycolic acid and glycolate has a potential to remain in certain streams generated during the production of the nuclear waste glass. A literature review was conducted to assess the impact of glycolic acid on the corrosion of the materials of construction for the DWPF facility as well as facilities downstream which may have residual glycolic acid and glycolates present. The literature data was limited to solutions containing principally glycolic acid.
  • Glycolic acid is being evaluated as an alternative for formic and nitric acid in the DWPF flowsheet. Demonstration testing and modeling for this new flowsheet has shown that glycolic acid and glycolate has a potential to remain in certain streams generated during the production of the nuclear waste glass. A literature review was conducted to assess the impact of glycolic acid on the corrosion of the materials of construction for the DWPF facility as well as facilities downstream which may have residual glycolic acid and glycolates present. The literature data was limited to solutions containing principally glycolic acid. The reportedmore » corrosion rates and degradation characteristics have shown the following for the materials of construction.« less
  • - This survey includes 148 references from the report and published literature on the elements Ce, Eu, Mo, Pm, Tc, and Zr. Chemical Abstracts, Jan. 1923 through Sept. 1968, and Nuclear Science Abstracts, Jan. 1948 through Aug. 1958, were the sources. (J.E.D.)