Hydrogen permeation on defected {\alpha}-Al2O3 surfaces: DFT calculations

TL;DR

This study uses density functional theory to investigate how defects on { extalpha}-Al2O3 surfaces influence hydrogen permeation, revealing that surface defects significantly lower energy barriers and facilitate hydrogen entry, explaining reduced permeability after irradiation.

Contribution

The paper provides the first detailed DFT analysis of hydrogen permeation mechanisms on defected { extalpha}-Al2O3 surfaces, highlighting the impact of surface defects on permeability.

Findings

Surface defects lower hydrogen migration barriers.

Hydrogen preferentially permeates through defect sites.

Radiation-induced defects explain permeability decrease.

Abstract

One of the key challenges to realize controlled fusion energy is tritium self-sufficiency. The application of hydrogen permeation barrier (HPB) is considered to be necessary for tritium self-sufficiency. {\alpha}-Al2O3 is currently a candidate material for HPB. However, a crucial issue for {\alpha}-Al2O3 is that its permeability reduction factor (PRF) will dramatically drop after ion or neutron irradiations. At present, little is known about the relevant mechanism. In order to shed light on this issue, the kinetics and energetic changes of hydrogen on defected {\alpha}-Al2O3 surfaces in comparison with perfect {\alpha}-Al2O3 surfaces were studied by density functional theory. For perfect {\alpha}-Al2O3 surfaces, the results show that the barrier for hydrogen migration from the outermost layer into the subsurface layer is the highest, making this migration step to be a rate limiting process. In contrast, surface point defects dramatically reduce this maximum barrier. Consequently, hydrogen can preferentially permeate into the interior of the material through surface defects. The findings can help explain the possible mechanism of significant decrease of PRF under radiation.