Understanding the role of Fe, Cr and Ni in Zircaloy-2 with special focus on the role of Ni on hydrogen pickup

Ni as an alloying addition in Zircaloy leads to an increase in hydrogen pick-up fraction. Atomic scale simulations of tetragonal ZrO2, based on density functional theory, are used to identify a possible mechanism for this observation. First, defect formation energies associated with Ni but also Fe and Cr are used to predict relative defect cluster and defect charge concentrations using Brouwer diagrams. At low oxygen partial pressures (), expected in the vicinity of the oxide metal interface, a cluster consisting of an oxygen vacancy adjacent to a charge neutral Ni0 atom is identified as the most populous cluster. Further simulations show that a hydrogen molecule will dissociate in the vicinity of this cluster. No other cluster is both sufficiently populous and acts in this way. This differentiates Ni from the other alloying elements.