A linear scaling relation for CO oxidation on CeO2-supported Pd,Journal of the American Chemical Society

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A linear scaling relation for CO oxidation on CeO2-supported Pd
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2018-03-02 , DOI: 10.1021/jacs.7b13624
Jin-Xun Liu ₁ , Yaqiong Su ₁ , Ivo A W Filot ₁ , Emiel J M Hensen ₁

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Resolving the structure and composition of supported nanoparticles under reaction conditions remains a challenge in heterogeneous catalysis. Advanced configurational sampling methods at the density functional theory level are used to identify stable structures of a Pd8 cluster on ceria (CeO2) in the absence and presence of O2. A Monte Carlo method in the Gibbs ensemble predicts Pd-oxide particles to be stable on CeO2 during CO oxidation. Computed potential energy diagrams for CO oxidation reaction cycles are used as input for microkinetics simulations. Pd-oxide exhibits a much higher CO oxidation activity than metallic Pd on CeO2. This work presents for the first time a scaling relation for a CeO2-supported metal nanoparticle catalyst in CO oxidation: a higher oxidation degree of the Pd cluster weakens CO binding and facilitates the rate-determining CO oxidation step with a ceria O atom. Our approach provides a new strategy to model supported nanoparticle catalysts.

中文翻译：

CeO2 负载 Pd 上 CO 氧化的线性比例关系

在反应条件下解析负载纳米粒子的结构和组成仍然是多相催化中的一个挑战。使用密度泛函理论水平的先进构型采样方法来识别在不存在和存在 O2 的情况下二氧化铈 (CeO2) 上 Pd8 簇的稳定结构。吉布斯系综中的蒙特卡罗方法预测氧化钯颗粒在 CO 氧化过程中在 CeO2 上保持稳定。计算出的 CO 氧化反应循环势能图用作微动力学模拟的输入。 Pd-氧化物比 CeO2 上的金属 Pd 表现出更高的 CO 氧化活性。这项工作首次提出了 CeO2 负载的金属纳米粒子催化剂在 CO 氧化中的比例关系：Pd 簇的较高氧化程度削弱了 CO 结合，并促进了二氧化铈 O 原子的决定速率的 CO 氧化步骤。我们的方法提供了一种新的策略来模拟支持的纳米颗粒催化剂。

更新日期：2018-03-02

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