摘要： Theoretical analysis of surface chemistry using Density Functional Theory (DFT) calculations has significantly contributed to our understanding of catalyzed processes related to energy production or consumption by providing performance descriptors, reaction mechanisms, and physical pictures of how electronic structure relates to catalytic reactivity. The identification of reactivity correlations within databases of DFT calculations has elucidated trends between active site composition (for metals, oxides, nitrides, phosphides, perovskites, etc.) or structure and catalytic reactivity or reactions including CO2 hydrogenation, NH3 synthesis, and the electrochemical oxygen evolution reaction (OER), among others. DFT calculations are now ubiquitously used in the analysis of catalytic processes due to the existence of easy to use software packages. It has become commonplace for publications to include combined experimental and theoretical treatment of a catalytic process, with the aim of providing a holistic picture of a reaction mechanism, an understanding of why materials exhibit their catalytic behaviors, or simply supporting inferences made from experimental measurements. While the combined approach is laudable, it is critical to recognize the challenges associated with using DFT calculations of model systems to understand experimental systems and how those challenges influence the conclusions derived from the calculations.