Atomic-scale understanding of oxidation mechanisms of materials by computational approaches: A review

Abstract

The urgent requirement of minimising the worldwide cost of corrosion, accompanied by the increasingly pivotal role of advanced oxide materials, highlights the importance of understanding the mechanisms of material oxidation at the atomic level, which could help us to precisely control the oxidation processes. Nowadays, we are able to model and predict how the surface structures of materials evolve during oxidation based on the cross-fertilisation of various computational techniques. This review first overviews the state-of-the-art first-principles and force-field-based approaches for modelling surface reactions. Then, classical theories and recent advances in understanding the atomic-scale oxidation of bulk materials are introduced, from the initial solid-gas interactions to the subsequent oxide film growth. Defect-promoted oxidation mechanisms will be discussed in detail. Finally, distinct oxidation mechanisms of nanomaterials are discussed, including nanoparticles, nanowires, and two-dimensional materials, which are significantly different from their bulk counterparts and could result in novel oxide nanostructures with unique properties. This review provides a systematic overview of the central role of computational techniques in probing the atomic-scale oxidation mechanisms, which could further guide the synthesis of oxide-based cutting-edge materials such as ultra-thin oxide films and hollow oxide nanostructures.