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Title: Computerized mathematical model for the anion exchange processing of plutonium(IV)

Abstract

A computerized mathematical model for anion exchange processing of plutonium(IV) was adopted from a previously written code. The model was verified to predict, within +-30 percent, a profile of plutonium breakthrough for the sorption process on Dowex 1-X4 anion exchange resin. The program was modified to incorporate column washing and elution logic. Experimental washing and elution data were in satisfactory agreement with predicted data. Provisions for changing the flow rate during the course of a run and for plotting capabilities to aid in better presentation of column breakthrough curves also were incorporated into the model.

Authors:
; ;
Publication Date:
Research Org.:
Atomics International Div., Golden, CO (USA). Rocky Flats Plant
Sponsoring Org.:
US Energy Research and Development Administration (ERDA)
OSTI Identifier:
7324542
Report Number(s):
RFP-2572
TRN: 77-011941
DOE Contract Number:
EY-76-C-04-3533
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; PLUTONIUM; ION EXCHANGE; EXTRACTION COLUMNS; LEACHING; MATHEMATICAL MODELS; ORGANIC ION EXCHANGERS; WASHING; ACTINIDES; CLEANING; DISSOLUTION; ELEMENTS; EXTRACTION APPARATUSES; ION EXCHANGE MATERIALS; METALS; SEPARATION PROCESSES; TRANSURANIUM ELEMENTS; 400105* - Separation Procedures

Citation Formats

Navratil, J. D., Proctor, S. G., and Kirkby, L. L.. Computerized mathematical model for the anion exchange processing of plutonium(IV). United States: N. p., 1977. Web. doi:10.2172/7324542.
Navratil, J. D., Proctor, S. G., & Kirkby, L. L.. Computerized mathematical model for the anion exchange processing of plutonium(IV). United States. doi:10.2172/7324542.
Navratil, J. D., Proctor, S. G., and Kirkby, L. L.. Mon . "Computerized mathematical model for the anion exchange processing of plutonium(IV)". United States. doi:10.2172/7324542. https://www.osti.gov/servlets/purl/7324542.
@article{osti_7324542,
title = {Computerized mathematical model for the anion exchange processing of plutonium(IV)},
author = {Navratil, J. D. and Proctor, S. G. and Kirkby, L. L.},
abstractNote = {A computerized mathematical model for anion exchange processing of plutonium(IV) was adopted from a previously written code. The model was verified to predict, within +-30 percent, a profile of plutonium breakthrough for the sorption process on Dowex 1-X4 anion exchange resin. The program was modified to incorporate column washing and elution logic. Experimental washing and elution data were in satisfactory agreement with predicted data. Provisions for changing the flow rate during the course of a run and for plotting capabilities to aid in better presentation of column breakthrough curves also were incorporated into the model.},
doi = {10.2172/7324542},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Mon May 09 00:00:00 EDT 1977},
month = {Mon May 09 00:00:00 EDT 1977}
}

Technical Report:

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  • The major aqueous process used to recover and purify plutonium at the Los Alamos Plutonium Facility is anion exchange in nitric acid. This process is highly selective for plutonium; however, all plutonium must be as Pu(IV) to form the strongly sorbed anionic nitrato complex. The previous ''full-reduction treatment'' used at Los Alamos to obtain Pu(IV) results in a three- to fourfold increase in the feed solution volume and the introduction of kilogram quantities of extraneous salts immediately before a process whose function is to remove such impurities. That treatment has been successfully replaced by a single reagent, hydrogen peroxide, whichmore » converts all plutonium to Pu(IV), minimally increases the feed volume, and introduces no residual impurities. Safety aspects of this revised chemical treatment are addressed.« less
  • H-Canyon and HB-Line are tasked with the production of PuO{sub 2} from a feed of plutonium metal. The PuO{sub 2} will provide feed material for the MOX Fuel Fabrication Facility. After dissolution of the Pu metal in H-Canyon, the solution will be transferred to HB-Line for purification by anion exchange. Subsequent unit operations include Pu(IV) oxalate precipitation, filtration and calcination to form PuO{sub 2}. This report details the results from SRNL anion exchange, precipitation, filtration, calcination, and characterization tests, as requested by HB-Line1 and described in the task plan. This study involved an 80-g batch of Pu and employed testmore » conditions prototypical of HB-Line conditions, wherever feasible. In addition, this study integrated lessons learned from earlier anion exchange and precipitation and calcination studies. H-Area Engineering selected direct strike Pu(IV) oxalate precipitation to produce a more dense PuO{sub 2} product than expected from Pu(III) oxalate precipitation. One benefit of the Pu(IV) approach is that it eliminates the need for reduction by ascorbic acid. The proposed HB-Line precipitation process involves a digestion time of 5 minutes after the time (44 min) required for oxalic acid addition. These were the conditions during HB-line production of neptunium oxide (NpO{sub 2}). In addition, a series of small Pu(IV) oxalate precipitation tests with different digestion times were conducted to better understand the effect of digestion time on particle size, filtration efficiency and other factors. To test the recommended process conditions, researchers performed two nearly-identical larger-scale precipitation and calcination tests. The calcined batches of PuO{sub 2} were characterized for density, specific surface area (SSA), particle size, moisture content, and impurities. Because the 3013 Standard requires that the calcination (or stabilization) process eliminate organics, characterization of PuO{sub 2} batches monitored the presence of oxalate by thermogravimetric analysis-mass spectrometry (TGA-MS). To use the TGA-MS for carbon or oxalate content, some method development will be required. However, the TGA-MS is already used for moisture measurements. Therefore, SRNL initiated method development for the TGA-MS to allow quantification of oxalate or total carbon. That work continues at this time and is not yet ready for use in this study. However, the collected test data can be reviewed later as those analysis tools are available.« less
  • A method for separation of Pu and Th on a plant scale using anion exchange from HCl solution is described. Data on effects of Pu and HCl concentrations, and a plant-scale flowhseet are included. (J.R.D.)