Hemilability is an important concept in homogeneous catalysis where both the reactant activation and the product formation can occur simultaneously through a reversible opening and closing of the metal-ligand coordination sphere. However, this effect has rarely been discussed in heterogeneous catalysis. Here, by employing a theoretical study on CO oxidation over substituted Cu₁/CeO₂ single atom catalysts, we show that dynamic evolution of metal-support coordination can significantly change the electronic structure of the active center. The evolution of the active center is shown to either strengthen or weaken the metal-adsorbate bonding as the reaction proceeds from reactants, through intermediates, to products. As a result, the activity of the catalyst can be increased. We explain our observations by extending hemilability effects to single atom heterogenous catalysts and anticipate that introducing this concept can offer a new insight into the important role active site dynamics have in catalysis toward the rational design of more sophisticated single atom catalyst materials.

Hemilability 是均相催化中的一个重要概念，其中反应物活化和产物形成可以通过金属-配体配位球的可逆打开和关闭同时发生。然而，这种效应在多相催化中很少被讨论。_{在这里，通过对取代的 Cu 1} /CeO ₂上的 CO 氧化进行理论研究单原子催化剂，我们表明金属-载体配位的动态演化可以显着改变活性中心的电子结构。随着反应从反应物、中间体到产物的进行，活性中心的演变被证明会加强或削弱金属-吸附物键合。结果，可以提高催化剂的活性。我们通过将 hemilability 效应扩展到单原子多相催化剂来解释我们的观察结果，并预计引入这一概念可以为活性位点动力学在催化更复杂的单原子催化剂材料的合理设计中的重要作用提供新的见解。