Mary Ann H. Reimus

Nitrate anion exchange in 238Pu aqueous scrap recovery operations

Strong base, nitrate anion exchange (IX) is crucial to the purification of 238Pu solution feedstocks with gross levels of impurities. This paper discusses the work involved in bench scale experiments to optimize the nitrate anion exchange process. In particular, results are presented of experiments conducted to a) demonstrate that high levels of impurities can be separated from 238Pu solutions via nitrate anion exchange and, b) work out chemical pretreatment methodology to adjust and maintain 238Pu in the IV oxidation state to optimize the Pu(IV)-hexanitrato anionic complex sorption to Reillex-HPQ resin. Additional experiments performed to determine the best chemical treatment methodology to enhance recovery of sorbed Pu from the resin and VIS-NIR absorption studies to determine the steady state equilibrium of Pu(IV), Pu(III), and Pu(VI) in nitric acid are discussed.

High-silicon 238PuO2 fuel characterization study: Half module impact tests

The General-Purpose Heat Source (GPHS) provides power for space missions by transmitting the heat of 238Pu decay to an array of thermoelectric elements. The modular GPHS design was developed to address both survivability during launch abort and return from orbit. Previous testing conducted in support of the Galileo and Ulysses missions documented the response of GPHSs to a variety of fragment-impact, aging, atmospheric reentry, and Earth-impact conditions. The evaluations documented in this report are part of an ongoing program to determine the effect of fuel impurities on the response of the heat source to conditions baselined during the Galileo/Ulysses test program. In the first two tests in this series, encapsulated GPHS fuel pellets containing high levels of silicon were aged, loaded into GPHS module halves, and impacted against steel plates. The results show no significant differences between the response of these capsules and the behavior of relatively low-silicon fuel pellets tested previously.

Development program for 238Pu aqueous recovery process

Aqueous processing is necessary for the removal of impurities from 238Pu dioxide (238PuO2) scrap due to unacceptable levels of 234U and other non-actinide impurities. 238PuO2 is used to supply the thermal energy in General Purpose Heat Sources (GPHS). Impurities at levels above GPHS fuel specifications may impair the performance of the heat source. Efforts at Los Alamos have focused on developing the bench scale methodology for the aqueous process steps which include comminution, dissolution, ion exchange, precipitation, and calcination. Recently, work has been performed to qualify the bench scale methodology, to show that the developed process produces 238PuO2 that meets GPHS fuel specifications. This work has also enabled us to determine how liquid waste may be minimized during fullscale processing. Results of process qualification for the bench scale aqueous recovery operation and waste minimization efforts will be presented.

Removal of Pu-238 from aqueous process streams using a polymer filtration process

A glovebox facility is under construction at Los Alamos that will recover a significant quantity of the impure Pu-238 that exists in scrap and residues from past production operations. The general flowsheet consists of milling, acid dissolution, ion exchange, precipitation, calcination, oxygen isotope exchange, and waste treatment operations. As part of the waste treatment operations we are using polymer filtration to remove Pu-238 to meet facility discharge limits. Polymer filtration (PF) technology uses water-soluble polymers prepared with selective receptor sites to sequester metal ions, organic molecules, and other species from dilute aqueous solutions. The water-soluble polymers have a sufficiently large molecular size that they can be separated and concentrated using ultrafiltration (UF) methods. Water and small, unbound components of the solution pass freely through the UF membrane while the polymer concentrates in the retentate. The permeate stream is “cleaned” of the components bound to the polym...

Process parameters optimization in ion exchange 238Pu aqueous processing

This paper describes bench-scale efforts (5–7 grams of 238Pu) to optimize the ion exchange process for 234U separation with minimal 238Pu losses to the effluent and wash liquids. The bench-scale experiments also determine the methodology to be used for the full-scale process: 5 kg238Pu annual throughput. Heat transfer calculations used to determine the thermal gradients expected during ion exchange processing are also described. The calculations were performed in collaboration with Westinghouse Savannah River Technology Center (WSRTC) and provide information for the design of the full-scale ion exchange equipment.

Materials compatibility for 238Pu-HNO3/HF solution containment: 238Pu aqueous processing

The Power Source Technologies Group at Los Alamos National Laboratory is building a 238Pu Aqueous Scrap Recovery Line at the Plutonium Facility. The process line incorporates several unit operations including dissolution, filtration, ion exchange, and precipitation. During 1997–1999, studies were carried out to determine the chemistry used in the full-scale process. Other studies focussed on the engineering design of the operation. Part of the engineering design was to determine, in compatibility studies, the materials for reaction and storage vessels which will contain corrosive 238Pu−HNO3/HF solutions. The full-scale line is to be operational by the end of year 2000.

Anlysis capabilities for plutonium-238 programs

In this presentation, an overview of analysis capabilities that support 238Pu programs will be discussed. These capabilities include neutron emission rate and calorimetric measurements, metallography/ceramography, ultrasonic examination, particle size determination, and chemical analyses. The data obtained from these measurements provide baseline parameters for fuel clad impact testing, fuel processing, product certifications, and waste disposal. Also several in-line analyses capabilities will be utilized for process control in the full-scale 238Pu Aqueous Scrap Recovery line in FY01.

Containment of Nitric Acid Solutions of Plutonium-238

The corrosion of various metals that could be used to contain nitric acid solutions of Pu-238 has been studied. Tantalum and tantalum/2.5% tungsten resisted the test solvent better than 304L stainless steel and several INCONEL alloys. The solvent used to imitate nitric acid solutions of Pu-238 contained 70% nitric acid, hydrofluoric acid, and ammonium hexanitratocerate.

Light-weight radioisotope heater unit (LWRHU) impact tests

The light-weight radioisotope heater unit (LWRHU) is a 238PuO2-fueled heat source designed to provide one thermal watt in each of various locations on a spacecraft. Los Alamos National Laboratory designed, fabricated, and safety tested the LWRHU. The heat source consists of a hot-pressed 238PuO2 fuel pellet, a Pt-30Rh vented capsule, a pyrolytic graphite insulator, and a fineweave-pierced fabric graphite aeroshell assembly. To compare the performance of the LWRHUs fabricated for the Cassini mission with the performance of those fabricated for the Galileo mission, and to determine a failure threshold, two types of impact tests were conducted. A post-reentry impact test was performed on one of 180 flight-quality units produced for the Cassini mission and a series of sequential impact tests using simulant-fueled LWRHU capsules were conducted respectively. The results showed that deformation and fuel containment of the impacted Cassini LWRHU was similar to that of a previously tested Galileo LWRHU. Both units...