Determination of the helium diffusion coefficient in nuclear waste storage ceramics by a nuclear reaction analysis method

Host matrices for actinide immobilisation will undergo the formation of large helium quantities due to alpha decay. Helium diffusion rate has to be known in order to predict the long-term behaviour of the material, and particularly, the influence of helium accumulation on mechanical properties. A nuclear reaction analysis method, namely the He-3(d, p)He-4 reaction, has been used to analyse the evolution of He-3 profiles after ion implantations at 1 and 3 MeV in two materials, monoclinic ZrO2 (as a test material) and Ca9Nd(PO4)(5)(SiO4)F-1.5(OH)(0.5) britholite (envisaged for Am and Pu long-term storage). Two data processing methods are used: the classical excitation curve (proton yields versus deuteron energy) and second, the proton energy spectrum for a given deuteron energy. The characteristics of the He-3 profiles (depth, width) obtained by both methods are compared to SRIM estimations. Their evolution during subsequent annealings allows an estimation of the helium diffusion rate in the britholite: D (cm(2)/s) = (2.5 + 1.5) x 10(-4) exp(- (1.07 +/- 0.03 eV)/kT) in the temperature range 200-400 degreesC, in agreement with previous results on similar materials. Moreover, the shape of the proton energy spectra suggests channeling effects in britholite. (C) 2002 Elsevier Science B.V. All rights reserved.