The age-old conundrum in the catalysis community emerged at the interface between the usually idealized computational model and the underlying complexities of the "catalyst in action" during realistic conditions, commonly coined as the material gap and pressure gap. The recent Perspective by Reece et al. represents a valuable resource for understanding the necessary considerations required in bridging the pressure gap in silico. In another recent account of common pitfalls related to the surface catalysis modelling, Vogt and Weckhuysen 6 underlines the strength of computational modelling used to guide and influence the design of active sites, but also highlights the notorious issue of contemporary surface model studies, namely, the reductionist criteria employed to construct the model. Fig. represents the standard procedure to determine defect properties a priori, where the host materials have a well-described crystalline structure, and the relative charge of each defect configuration is represented by the Kröger-Vink notation. Typically, most of the possible defect sites for simple materials (e.g., bulk Si, graphene, carbon nanorods) are identical.