No CrossRef data available.
Published online by Cambridge University Press: 28 May 2012
Plutonium oxide heat sources are used to power space missions. The heat produced by alpha decay of the 238 isotope of Pu is converted to electricity in a thermopile, providing electricity during a substantial fraction of the 88 year half-life of the isotope. Decay of the Pu produces helium and uranium, and a fraction of the evolved helium is captured in the oxide matrix. All of the helium produced in decay can in principle be contained in the oxide lattice, where it occupies the tetrahedral sites. Some helium diffuses out at a rate that is somewhat dependent on the form and morphology of the fuel. Rates have previously been measured for oxide aged about 1 year. Current measurements on sealed heat sources as old as 34 years indicate that the rate of diffusion has changed only slightly over time. Possible mechanisms for helium release include bubble diffusion, point defect migration, agglomeration and movement of He at grain boundaries, and volume diffusion through the lattice sites. We observe primarily diffusion from site to site within the lattice, with an activation energy of 18.7 kcal/mole, independent of point defect movement, despite the rising concentration of helium in the lattice over time and the accumulation of radiation damage within the lattice. Because of the slow diffusion of helium from the fuel to the headspace, heat sources are anticipated to be stable over a long lifetime.