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Title: Evaluation of a Zirconium Recycle Scrubber System

Abstract

A hot-cell demonstration of the zirconium recycle process is planned as part of the Materials Recovery and Waste Forms Development (MRWFD) campaign. The process treats Zircaloy® cladding recovered from used nuclear fuel with chlorine gas to recover the zirconium as volatile ZrCl4. This releases radioactive tritium trapped in the alloy, converting it to volatile tritium chloride (TCl). To meet regulatory requirements governing radioactive emissions from nuclear fuel treatment operations, the capture and retention of a portion of this TCl may be required prior to discharge of the off-gas stream to the environment. In addition to demonstrating tritium removal from a synthetic zirconium recycle off-gas stream, the recovery and quantification of tritium may refine estimates of the amount of tritium present in the Zircaloy cladding of used nuclear fuel. To support these objectives, a bubbler-type scrubber was fabricated to remove the TCl from the zirconium recycle off-gas stream. The scrubber was fabricated from glass and polymer components that are resistant to chlorine and hydrochloric acid solutions. Because of concerns that the scrubber efficiency is not quantitative, tests were performed using DCl as a stand-in to experimentally measure the scrubbing efficiency of this unit. Scrubbing efficiency was ~108% ± 3% with watermore » as the scrubber solution. Variations were noted when 1 M NaOH scrub solution was used, values ranged from 64% to 130%. The reason for the variations is not known. It is recommended that the equipment be operated with water as the scrubbing solution. Scrubbing efficiency is estimated at 100%.« less

Authors:
 [1];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE)
OSTI Identifier:
1357987
Report Number(s):
ORNL/TM-2017/233
AF5805010; NEAF327; NTRD-MRWFD-2017-000307
DOE Contract Number:
AC05-00OR22725
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES

Citation Formats

Spencer, Barry B., and Bruffey, Stephanie H. Evaluation of a Zirconium Recycle Scrubber System. United States: N. p., 2017. Web. doi:10.2172/1357987.
Spencer, Barry B., & Bruffey, Stephanie H. Evaluation of a Zirconium Recycle Scrubber System. United States. doi:10.2172/1357987.
Spencer, Barry B., and Bruffey, Stephanie H. Sat . "Evaluation of a Zirconium Recycle Scrubber System". United States. doi:10.2172/1357987. https://www.osti.gov/servlets/purl/1357987.
@article{osti_1357987,
title = {Evaluation of a Zirconium Recycle Scrubber System},
author = {Spencer, Barry B. and Bruffey, Stephanie H.},
abstractNote = {A hot-cell demonstration of the zirconium recycle process is planned as part of the Materials Recovery and Waste Forms Development (MRWFD) campaign. The process treats Zircaloy® cladding recovered from used nuclear fuel with chlorine gas to recover the zirconium as volatile ZrCl4. This releases radioactive tritium trapped in the alloy, converting it to volatile tritium chloride (TCl). To meet regulatory requirements governing radioactive emissions from nuclear fuel treatment operations, the capture and retention of a portion of this TCl may be required prior to discharge of the off-gas stream to the environment. In addition to demonstrating tritium removal from a synthetic zirconium recycle off-gas stream, the recovery and quantification of tritium may refine estimates of the amount of tritium present in the Zircaloy cladding of used nuclear fuel. To support these objectives, a bubbler-type scrubber was fabricated to remove the TCl from the zirconium recycle off-gas stream. The scrubber was fabricated from glass and polymer components that are resistant to chlorine and hydrochloric acid solutions. Because of concerns that the scrubber efficiency is not quantitative, tests were performed using DCl as a stand-in to experimentally measure the scrubbing efficiency of this unit. Scrubbing efficiency was ~108% ± 3% with water as the scrubber solution. Variations were noted when 1 M NaOH scrub solution was used, values ranged from 64% to 130%. The reason for the variations is not known. It is recommended that the equipment be operated with water as the scrubbing solution. Scrubbing efficiency is estimated at 100%.},
doi = {10.2172/1357987},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Sat Apr 01 00:00:00 EDT 2017},
month = {Sat Apr 01 00:00:00 EDT 2017}
}

Technical Report:

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  • This report presents the results of 18 tests on the butane wash system of Process Development Unit P-99 performed during Runs P99-82 and -83 feeding Powhatan No. 6 Mine coal and during Run P99-85 processing Ireland Mine coal. The objective of this experimental program was to investigate butane as an absorbing liquid for removing pentanes and heavier hydrocarbons from hydrogen-rich SRC-II recycle gas. This experimental data was gathered to assist in determining the feasibility of implementing this system on the SRC-II Demonstration Plant, as a means of reducing heavy hydrocarbons in the feed to the cryogenic unit to an acceptablemore » level (200 ppM C/sub 5//sup +/). Operating conditions were identified which achieved essentially a complete removal of the C/sub 5//sup +/ components from the recycle gas on PDU P-99. Detailed component analyses for individual hydrocarbons and fixed gases were determined for all inlet and outlet streams. Correlations were developed which adequately fit the experimental data; however, these correlations reveal inconsistencies and indicate the need for more extensive tests. Overall operability of the system was judged satisfactory, provided column temperatures were above 45/sup 0/F, and a sufficient supply of butane was fed to offset the large quantity which flashed overhead.« less
  • The report gives results of an analysis of flue gas desulfurization by a turbulent contact absorber (TCA) employing lime slurry, including the development of performance equations for the scrubber-hold tank recycle system. Performance characteristics investigated include pressure drop of the scrubber, CO/sub 2/ and SO/sub 2/ absorptions, and lime utilization. Experimental data obtained from EPA/Research Triangle Park and TVA/Shawnee Power Station are used for the analysis and correlation. The analysis of CO2 absorption indicates that the overall mass transfer coefficient is a function of the pH of inlet and outlet scrubber liquor and is very sensitive to the liquor flowmore » rate. (The rate of SO/sub 2/ absorption in a TCA has been developed previously by McMichael et al., 1976.) The correlations developed are used to formulate a simulation procedure for predicting SO/sub 2/ scrubbing efficiency as a function of pH of slurry and gas and liquor flow rates. The result of simulation indicates that, for a given lime feed rate and a fixed inlet and outlet SO2 concentration, a maximum flue gas flow rate exists which the scrubber can treat by the recycling slurry. An example is shown for the design of a TCA capable of desulfurizing flue gas from a 50-MW power station.« less
  • A 10 MW test using a limestone system with thiosulfate additive, was funded by the TVA Office of Power and was conducted at the Shawnee Test Facility between May 5 and August 17, 1982 on train 100 (spray tower). The primary purpose of the test was to evaluate the effect of sodium thiosulfate additive on spray tower system performance under typical commercial scrubbing conditions. A secondary test purpose was to obtain engineering data on scrubber system components under test conditions that would permit the comparison of actual performance with design performance. For specific test conditions (pH = 5.8, liquid-to-gas (L/G)more » ratio = 65 gal/1000 acf flue gas), SO/sub 2/ removal was unaffected by thiosulfate ion concentration, and the effective slurry liquor thiosulfate ion concentration for scale-free scrubbing was approximately 100 ppM. Another important finding was the increase of up to 20% in solids content of horizontal belt filter cake at a thiosulfate ion concentration in the slurry liquid of 600 ppM compared with belt filter cake solids when no thiosulfate ion was in the slurry liquid. Overall mass transfer coefficients (K/sub g/a for SO/sub 2/ absorption into limestone slurry ranged from 9.8 to 10.4 lb moles/hr ft/sup 3/ ATM. Comparisons of test K/sub g/a values with previously published values suggest that the gas film component was of predominant importance during all tests. Capital investment costs for the limestone-sodium thiosulfate scrubber system at 500 MW are approximately 6% lower than for a comparable limestone forced-oxidation system. The operating costs for a 500 MW limestone-sodium thiosulfate scrubber system are 5% lower than for a limestone forced-oxidation system of comparable size.« less
  • The report gives results of a study of the styrene removal efficiency of a pilot-scale version of the QUAD Chemtact scrubber, quantified by continuously measuring the total hydrocarbon (THC) content of spray booth exhaust air entering and exiting the device with THC analyzers and, for some tests, by collecting EPA Method 18 samples (adsorption tube procedure) at the inlet and exit of the device. Average styrene removal efficiencies approached but were never >55%. The test was carried out at a facility (Eljer Plumbingware in Wilson, NC) that manufactures polyester bathtubs and shower stalls by spraying styrene-based resins onto molds inmore » vented, open spray booths. A side stream of air, exhausted from one of the spray booths in the gel coating part of the process, was used for the test.« less
  • An evaluation of the utilization of plutonium recycle fuel in the Obrigheim power reactor was performed in order to study the characteristics of typical large PWR's operated with plutonium recycle fuel. The evaluation included nuclear characteristics, fuel management, a thermal-hydraulic analysis, and an economic analysis. (JWR)