Alcoholysis of amides on the CeO₂ surface is investigated from density functional theory (DFT) computations, in situ FT-IR spectroscopy, and catalytic studies. The thermodynamically stable amide bonds are effectively activated by the CeO₂ catalyst under mild conditions in contrast to other metal oxide catalysts. DFT calculations demonstrated that acetamide adsorbed on the CeO₂ surface is attacked by lattice oxygen to give a tetrahedral intermediate in the rate-determining step of the most favorable pathway. This is consistent with the experimental finding that the activity of metal oxide catalysts increases with an increase of the base strength of the catalyst. The strong base sites of CeO₂ are the most important factor for the high reactivity. Interestingly, the nucleophilic attack of lattice oxygen is further assisted by the moderately strong Ce⁴⁺ Lewis acid sites. Our computational results show that the high reactivity is ascribed to a catalytic interplay between the Lewis base and acid pair sites on the CeO₂ surface.

根据密度泛函理论（DFT）计算，原位FT-IR光谱和催化研究，研究了CeO ₂表面酰胺的醇解。与其他金属氧化物催化剂相比，在温和条件下，CeO ₂催化剂可有效活化热力学稳定的酰胺键。DFT计算表明，吸附在CeO ₂表面上的乙酰胺在最有利途径的速率确定步骤中受到晶格氧的攻击而得到四面体中间体。这与实验发现一致，即金属氧化物催化剂的活性随催化剂的碱强度的增加而增加。CeO ₂的强大基地是高反应性的最重要因素。有趣的是，中等强度的Ce ⁴⁺ Lewis酸位点进一步协助了晶格氧的亲核攻击。我们的计算结果表明，高反应性归因于CeO ₂表面上的路易斯碱和酸对位点之间的催化相互作用。