Synthese und Partialoxidation von Methanol an wohldefinierten Modellträgerkatalysatoren - Teilprojekt: Theoretische Untersuchungen an wohldefinierten getragenen Edelmetall-Modellkatalysatoren

该项目的目的是在原子水平上了解以氧化膜为载体的模型金属催化剂上甲醇氧化的机理。这是与三个实验项目(柏林弗里茨-哈伯研究所的Libua/Freund和柏林Fritz Haber-Institute的Rupprechter/Freund和不来梅大学的Bäumer)合作的优先计划“多相催化”中的一项集体赠款的量子化学部分。采用密度泛函模型研究了金属纳米颗粒及其与甲醇分解相关的各种金属络合物的结构和能量。在建立了一种新的基于三维模型纳米团簇的计算策略后，我们最近量化和合理化了项目合作伙伴实验研究的催化剂的结构和吸附性能。在本资助期间，我们将把衬底的范围扩大到双金属Pd-Co纳米颗粒。此外，我们将解决单金属纳米颗粒的反应性方面，这是由于固有的团簇表面属性或沉积的不规则性造成的。这些关于反应和活化能的理论数据将对理解正在进行实验工作的项目合作伙伴的观察结果至关重要。最后，将对模型催化剂的反应性进行一致的定量理论和实验描述。

The project aims at understanding, at the atomic level, the mechanism of methanol oxidation on model metal catalysts supported on oxide films. It is the quantum chemistry part of a group grant within the priority programme "Heterogeneous Catalysis" in collaboration with three experimental projects (Libuda/Freund and Rupprechter/Freund at Fritz-Haber-Institut, Berlin and Bäumer at Universität Bremen). Advanced density functional cluster models are used to explore structure and energetics of metal nanoparticles and their complexes with various deposits pertinent to methanol decomposition on such species. Having established a new computational strategy based on three-dimensional model nanoclusters, we recently quantified and rationalized structural and adsorption properties of catalysts investigated experimentally by the project partners. In this funding period, we will extend the scope of substrates to bimetallic Pd-Co nanoparticles. Furthermore, we will address reactivity aspects of monometallic nanoparticles, caused by inherent cluster surface properties or deposited irregularities. These theoretical data on reaction and activation energies will be crucial for understanding observations of the experimentally working project partners. Finally, a consistent quantitative theoretical and experimental description of the reactivity of the model catalysts under scrutiny will be developed.