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Mulford, Roberta Nancy

Publications and source records attributed to Mulford, Roberta Nancy.

Effects of 18 O Exchange on Neutron Emission Rates of Aging 238 PuO 2 LWRHUs

The Lightweight Radioisotope Heater Unit (LWRHU) provides about 1 Watt of thermal power to critical electrical and mechanical systems in the extreme temperatures of space, maintaining the operating temperature of the spacecraft’s scientific and general operating equipment. Los Alamos National Laboratory (LANL) designed and tested the LWRHU in the 1970s through early 1980s. The first production campaign at LANL was in the early 1980s in support of the Galileo mission in which over 100 LWRHUs were manufactured. In the mid-1990s, almost 200 LWRHUs were manufactured in support of the Cassini mission. After the primary Cassini manufacturing campaign, the Department of Energy (DOE) approved the fabrication of more than 10 additional LWRHUs as spares in 1998. The LWRHU assembly contains the following components: a fuel pellet, a vented capsule, a pyrolytic graphite insulator, and a fine-weave pierced fabric (FWPF) graphite aeroshell. The fuel pellet is a hot-pressed 238 PuO 2 cylindrical pellet that is sintered to create a ceramic pellet. The pellet is encapsulated in a platinum-rhodium encapsulation. The welded fueled clad is placed inside a pyrolytic graphite thermal insulation to protect the fuel from the heat produced in reentry events. The exterior layer of the LWRHU assembly is the FWPF aeroshell. Before sintering, PuO 2 granules are heated in a furnace at temperatures greater than or equal to 700°C under an enriched 16 O atmosphere in order to reduce trace quantities of 18 O. Because 18 O undergoes an (α,n) reaction, 18 O needs to be removed as much as possible to meet radiation emission requirements set by the Jet Propulsion Laboratory (JPL) and the National Aeronautics and Space Administration (NASA), as well as other agencies. The relative abundances of the oxygen isotopes are indicated by neutron emission rate (NER) measurements. LWRHUs are vented with a sintered platinum frit vent (George 1986). During extraterrestrial operation, the vent in the cladding allows helium from the decay of plutonium to escape and relieves pressure from the system while preventing the solids from escaping (Rinehart 1996, Tate 1982 & 1985). This vent is protected during manufacture by a platinum-30 rhodium cover. The capsule vent is activated by milling a 0.025-inch diameter hole through the protective cover to a nominal depth of 0.015 inches, generally immediately before the LWRHU is loaded into the aeroshell (George 1986). Prior to long-term storage, LWRHUs are vented and thus potentially allow infiltration of 18 O from the ambient atmosphere. Although NER decreases with age due to the reduction in emitted alpha particles, it might be expected that NER reduction is mitigated by the exchange of 18 O. However, this is not necessarily the case and no trend was observed relating NER to age other than the natural decay of 238 Pu (Mulford 2021). The most probable and dominant factor for determining specific NER was manufacturing discrepancies between individual units. It is important to understand the lack of observed 16 O- 18 O exchange and to compare LWRHU pellets as much as possible.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Distended clads gas pressurization and material failure timescales

This document presents timescales for additional failure modes, including pressurization of void space in the pellet to the estimated tensile strength of the pellet. Because helium is known to be captured in the fuel as well as evolved as gas, previous timescales are adjusted to account for the substantial dissolution of helium in the matrix of the fuel at normal fuel temperatures. Helium arises from the decay of the 238Pu in the fuel, and can appear as a gas, creating bubbles within the fuel. The majority of helium is known to be captured within the fuel matrix at the operating temperatures of an isolated clad.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Particle size of several plutonium-238 oxide fuel samples from oxalate precipitation processes

Particle size of 238 PuO 2 powders is an important factor in determining the structural integrity of fuel pellets hot-pressed from the oxide powder. Understanding the evolution of particle size during aqueous processing is a first step in assuring control of particle size throughout the pellet formation process. Measured particle sizes are reported here, and discussed in terms of measured particle size changes occurring during calcining, observed aggregation of particulate, and particle morphology. Morphology and aggregation are related to surface energy, which governs granule formation and hot pressing behavior. Results are discussed in terms of reported dependence of oxide morphology on process temperatures and reagent concentrations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Helium pressure increase inside GPHS clads: implications for formation of distended clads

Distension of GPHS clads has generally been attributed to gas buildup inside the clad. The bulging vent frit cover can be caused only by gas pressure, since the vent cover is isolated from the fuel by the vent frit. Gas generation is the only change expected as the oxide fuel ages. However, several data suggest that gas pressure is not the origin of the distension of the clad body. Gas pressure sufficient to distend the iridium body of the clad would be on the order of 1500 psi. This high pressure is very unlikely to be reached inside a GPHS clad, because the vent frit cover weld cannot sustain high pressures. Every distended clad that has been examined has an open vent frit, suggesting that the vent frit cover eventually opens on all distended GPHS clads. No gas pressure has been observed in any distended clad. In addition, the vent frit cover is sufficiently thin, about 2 grains thick, that diffusion of helium through the intact cover is possible and almost certainly occurs. Conversely, no clad has ever been definitively observed to distend after venting. Removal of the vent cover allows free escape of any radiolytically generated helium. However, there is little data on the behavior of vented GPHS. The vent cover is seldom removed at LANL, and vent covers are not removed on clads that will be stored. The vent covers are known to have been removed from the four clads residing in a module which was stored for 8 years. Expansion of the fuel is more likely to provide sufficient force on the iridium clad to distort the iridium metal. Radiographs indicate that the fuel inside a distended GPHS clad is also distended, filling all or most of the interior volume of the GPHS. No radiograph shows the fuel expanded and in contact with the weld shield and the distorted side of the GPHS clad without distension. However, radiography is infrequently done on stored clads unless they exhibit distension, so the dimensions of fuel in normal clads are not generally known.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Distended GPHS Clads: Characterization of Fuel Particle Size

GPHS Clads have been observed to distend or bulge slightly after aging or after storage in hot conditions. Configurations in which the fuel can reach a temperature above about 900°C appear to promote distension.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Calibration of the PT 3845 Electrical Tester, July 13, 2018

The PT3845 Electrical Tester, calibration file number 101921, is used to test the electrical properties of components for the Surveillance Program. The unit is located in PF-4 room 214, and is a custom construction provided by Sandia National Laboratory/Primecore.

47 OTHER INSTRUMENTATION↗

A systematic error affecting NER calculations

Factors that may affect the precision of Neutron Emission Rate (NER) measurements made in the Canberra 4 neutron counter have been examined and quantified. Measurements of sample NER are corrected for the efficiency of the counter. The efficiency is calculated by measuring a source of known intensity, and taking the ratio of the measured neutrons per second (n/s) to the known output of the source.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗