The Big Problem in Surface Catalysis Modelling

The existence of native point defects in crystalline solids are inevitable during synthesis. Such native defects will usually strongly impact the device performance of materials in catalysis applications. In recent years, the ability of first-principles approaches to accurately predict defect behavior has seen major progress. The underlying issue, as one would have guessed, is that these predictions of defect behavior and catalytic efficiency are extremely sensitive to the atomic structure of defect. Therefore, the proper identification of possible defect sites, their ground-state and metastable structures, and the correction scheme is crucial to resolving our understanding and control of defects’ role on catalytic performance. In this Comment, we aim to highlight recent advances of first-principles prediction for defect behavior while proposing a protocol for rigorous computational modelling.