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Title: Study of cesium volatility from sodium carbonate based melts

Abstract

Purpose of this study was to obtain thermodynamic data on cesium volatility from sodium carbonate-based molten salts for application to the Rockwell-ETEC molten salt oxidation process. At 1073 to 1373 K, volatility tests were conducted on a horizontal and a vertical transpiration apparatus using a carrier gas composed of CO{sub 2}(g) and H{sub 2}O(g) which was passed over or bubbled through a sodium carbonate bath containing cesium carbonate and various additives. The major vapor species was identified to be CsOH(g) except when greater than 3% chloride is present in the melt, then the major vapor species is CsCl(g). The decrease in volatility of cesium as a function of cesium concentration in Cs{sub 2}CO{sub 3{minus}}Na{sub 2}CO{sub 3} mixtures follows Raoult`s law very closely. Thus, this system exhibits close to ideal solution behavior. Addition of 22.5 wt % sodium sulfate decreases the cesium volatility by just under a factor of 2, and the addition of 10.0 wt % sodium chloride increases the cesium volatility about an order of magnitude. The addition of 2.0 wt % ash, molecular sieve, or silica show little or no effect. However, the data indicate that higher concentrations of ash will decrease the cesium volatility. For the additionmore » of 22.5 wt % sodium sulfate the activity coefficient, {gamma}(Cs{sub 2}CO{sub 3}){sup {1/2}}, is calculated to be 0.720 {plus_minus} 0.068, and for the addition of 10.0 wt % sodium chloride, the activity coefficient, {gamma}(CsCl), is calculated to be 8.118 {plus_minus} 2.317. Assuming that Henry`s law applies, these activity coefficients are used to extrapolate the effect on cesium retention in the molten salt oxidizer of sulfate and chloride at lower cesium concentrations.« less

Authors:
; ; ;
Publication Date:
Research Org.:
Lawrence Livermore National Lab., CA (United States)
Sponsoring Org.:
USDOE, Washington, DC (United States)
OSTI Identifier:
10154136
Report Number(s):
UCRL-ID-115768
ON: DE94012588
DOE Contract Number:  
W-7405-ENG-48
Resource Type:
Technical Report
Resource Relation:
Other Information: PBD: Dec 1993
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; CESIUM; VOLATILITY; SODIUM CARBONATES; MOLTEN SALTS; SODIUM SULFATES; SODIUM CHLORIDES; ASHES; MOLECULAR SIEVES; SILICA; OXIDATION; RADIOACTIVE WASTE PROCESSING; 052001; WASTE PROCESSING

Citation Formats

Ebbinghaus, B B, Krikorian, O H, Adamson, M G, and Fleming, D L. Study of cesium volatility from sodium carbonate based melts. United States: N. p., 1993. Web. doi:10.2172/10154136.
Ebbinghaus, B B, Krikorian, O H, Adamson, M G, & Fleming, D L. Study of cesium volatility from sodium carbonate based melts. United States. https://doi.org/10.2172/10154136
Ebbinghaus, B B, Krikorian, O H, Adamson, M G, and Fleming, D L. 1993. "Study of cesium volatility from sodium carbonate based melts". United States. https://doi.org/10.2172/10154136. https://www.osti.gov/servlets/purl/10154136.
@article{osti_10154136,
title = {Study of cesium volatility from sodium carbonate based melts},
author = {Ebbinghaus, B B and Krikorian, O H and Adamson, M G and Fleming, D L},
abstractNote = {Purpose of this study was to obtain thermodynamic data on cesium volatility from sodium carbonate-based molten salts for application to the Rockwell-ETEC molten salt oxidation process. At 1073 to 1373 K, volatility tests were conducted on a horizontal and a vertical transpiration apparatus using a carrier gas composed of CO{sub 2}(g) and H{sub 2}O(g) which was passed over or bubbled through a sodium carbonate bath containing cesium carbonate and various additives. The major vapor species was identified to be CsOH(g) except when greater than 3% chloride is present in the melt, then the major vapor species is CsCl(g). The decrease in volatility of cesium as a function of cesium concentration in Cs{sub 2}CO{sub 3{minus}}Na{sub 2}CO{sub 3} mixtures follows Raoult`s law very closely. Thus, this system exhibits close to ideal solution behavior. Addition of 22.5 wt % sodium sulfate decreases the cesium volatility by just under a factor of 2, and the addition of 10.0 wt % sodium chloride increases the cesium volatility about an order of magnitude. The addition of 2.0 wt % ash, molecular sieve, or silica show little or no effect. However, the data indicate that higher concentrations of ash will decrease the cesium volatility. For the addition of 22.5 wt % sodium sulfate the activity coefficient, {gamma}(Cs{sub 2}CO{sub 3}){sup {1/2}}, is calculated to be 0.720 {plus_minus} 0.068, and for the addition of 10.0 wt % sodium chloride, the activity coefficient, {gamma}(CsCl), is calculated to be 8.118 {plus_minus} 2.317. Assuming that Henry`s law applies, these activity coefficients are used to extrapolate the effect on cesium retention in the molten salt oxidizer of sulfate and chloride at lower cesium concentrations.},
doi = {10.2172/10154136},
url = {https://www.osti.gov/biblio/10154136}, journal = {},
number = ,
volume = ,
place = {United States},
year = {1993},
month = {12}
}