Single-atom catalyst (SAC) have received increasing attention in the field of CO oxidation due to their higher catalytic activity and greater atomic utilization. The CO oxidation by O₂ on the single Rh atom embeddedover Graphdiyne (Rh-GDY) is systematically studied by using the first principles simulation. It is found that Rh atom can be stably and isolated in the GDY as a single metal atom binding to the carbon atoms. Both of the Langmuir–Hinshelwood (LH) and the Trimolecular Eley-Rideal (TER) mechanisms are preferable due to the rather low reaction barrier of their rate-determining steps. Moreover, LH mechanism could be more preferable than the TER mechanism according to their reaction rate constants at various temperatures, indicating that Rh-GDY is a promising catalyst for CO oxidation. Our investigation would help to reveal the mechanisms of the CO oxidation on SAC and shed light on the design of SAC based on GDY sheets for the oxidation of the fuel gas.

单原子催化剂（SAC）由于具有更高的催化活性和更大的原子利用率而在CO氧化领域受到越来越多的关注。O ₂氧化CO利用第一性原理模拟，系统地研究了单Rh原子嵌入石墨二炔（Rh-GDY）的过程。发现Rh原子可以作为结合碳原子的单个金属原子在GDY中稳定和分离。Langmuir-Hinshelwood（LH）和三分子Eley-Rideal（TER）机理都是可取的，因为它们的速率决定步骤的反应势垒很低。此外，根据它们在各种温度下的反应速率常数，LH机理可能比TER机理更优选，这表明Rh-GDY是有希望的CO氧化催化剂。我们的研究将有助于揭示SAC上CO氧化的机理，并为基于GDY薄板对燃料气体进行氧化的SAC设计提供启示。