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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Balance in Adsorption Energy of Reactants Steers CO Oxidation Mechanism of Ag13 and Ag12Pd1 Nanoparticles: Association Mechanism versus Carbonate-Mediated Mechanism
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Balance in Adsorption Energy of Reactants Steers CO Oxidation Mechanism of Ag13 and Ag12Pd1 Nanoparticles: Association Mechanism versus Carbonate-Mediated Mechanism

机译:反应物吸附能的平衡控制了Ag13和Ag12Pd1纳米颗粒的CO氧化机理:缔合机理与碳酸盐介导机理

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摘要

CO oxidation is a very useful reference reaction in catalysis by nanoparticles (NPs). Two reaction models-an association mechanism (AM) and a carbonate-mediated mechanism (CMM)-have been suggested for CO oxidation catalyzed by small NPs. It is still unclear, however, when and why these mechanisms preferentially operate. With the Ag13 crystalline NPs and the Ag12Pd1 core-shell NP, using a density functional theory calculation and a microkinetic reaction model, we found that the different reaction mechanisms can operate with different reaction intermediates accompanied by a balance in the adsorption energy of reactants. Variations in the adsorption energy of adsorbates can result from the interchange of two reaction mechanisms, even in a single NP. An AM operates when both reactants interact strongly with a NP, whereas the contribution of the CMM in CO oxidation increases when a CO molecule interacts weakly or not at all with a NP.
机译:CO氧化是纳米颗粒(NPs)催化中非常有用的参考反应。对于小NPs催化的CO氧化,已经提出了两种反应模型-缔合机理(AM)和碳酸盐介导的机理(CMM)。但是,尚不清楚何时以及为什么这些机制优先运行。对于Ag13晶体NP和Ag12Pd1核-壳NP,使用密度泛函理论计算和微动力学反应模型,我们发现不同的反应机理可以在不同的反应中间体之间进行,同时平衡了反应物的吸附能。即使在单个NP中,两种反应机理的互换也会导致被吸附物吸附能的变化。当两种反应物都与NP强烈相互作用时,AM起作用,而当CO分子与NP弱相互作用或完全不相互作用时,CMM在CO氧化中的贡献增加。

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