Fundamental knowledge of structure-activity correlations for heterogeneous single-atom catalysts (SACs) is essential in guiding catalytic design. While linear scaling relations are powerful for predicting the performance of traditional metal catalysts, they appear to fail with the involvement of SACs. Comparing the catalytic CO oxidation activity of different atomically dispersed metals (3d, 4d, and 5d) in conjunction with computational modeling enabled us to establish multiple scaling relations between the activity and simply calculated descriptors. Through these efforts, we found that the thermodynamic driving force for the oxygen vacancy formation needed to be considered in addition to the adsorption energies of substrates (in particular CO). Our approach was to reduce the computational requirements in determining better CO oxidation catalysts using a few key thermodynamic descriptors. This work presents one of the first successful approaches for re-establishing scaling relations for catalytic reactions by SACs with potentially broad implications for catalytic processes actively involving this support.

非均相单原子催化剂 (SAC) 的结构-活性相关性的基础知识对于指导催化设计至关重要。虽然线性比例关系对于预测传统金属催化剂的性能很有效，但在 SAC 的参与下，它们似乎失败了。结合计算模型比较不同原子分散金属（3d、4d 和 5d）的催化 CO 氧化活性，使我们能够在活性和简单计算的描述符之间建立多重比例关系。通过这些努力，我们发现除了底物（特别是 CO）的吸附能之外，还需要考虑氧空位形成的热力学驱动力。我们的方法是使用一些关键的热力学描述符来减少确定更好的 CO 氧化催化剂的计算要求。这项工作提出了第一个成功的方法之一，用于通过 SAC 重新建立催化反应的比例关系，对积极参与这种支持的催化过程具有潜在的广泛影响。