Toward a Better Understanding of Ni Coarsening in Solid Oxide Cells: NiH on Ni (111) Examined Using a Combined Theoretical Approach

The coarsening of the Ni particles in the hydrogen electrode of solid oxide cells (SOCs) is an important degradation mechanism. In this paper, density-functional theory and kinetic Monte Carlo methods are used to explore our recent hypothesis that the surface diffusion of NiH may cause faster Ni coarsening in electrolysis cell mode under an overpotential. Using both methods, the diffusion constant or diffusivity of NiH on Ni (111) is determined as the product of the surface coverage and single-molecule diffusivity for the first time considering all possible diffusion paths. It is then determined versus overpotential at the triple-phase boundary of the hydrogen electrode assuming a typical operating temperature of the SOC. Under a significant overpotential, the diffusivity of NiH is found to be sufficiently large to support the above hypothesis that NiH may promote Ni coarsening. However, based on the adsorption configurations identified, the dissociation and reformation of NiH on Ni (111) could occur. Thus, more work is needed to develop a model of Ni coarsening considering both molecular and dissociated forms of NiH.