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理解甲醇在氧化膜上支撑的模型金属催化剂上的氧化机理。它是优先计划“多相催化”中的一个小组资助的量子化学部分，与三个实验项目（柏林弗里茨-哈伯研究所的Lixons/Freund和Rupprechter/Freund以及不莱梅大学的Bäumer）合作。先进的密度泛函簇模型被用来探索金属纳米粒子及其与各种沉积物的复合物的结构和能量，这些沉积物与甲醇在这些物种上的分解有关。在建立了一种基于三维模型纳米团簇的新计算策略后，我们最近对项目合作伙伴实验研究的催化剂的结构和吸附特性进行了量化和合理化。在此资助期内，我们将把基板的范围扩大到Pd-Co纳米粒子。此外，我们将解决反应性方面的monoclonal纳米粒子，所造成的固有簇表面特性或沉积的不规则性。这些关于反应能和活化能的理论数据对于理解实验工作项目合作伙伴的观测结果至关重要。最后，一个一致的定量理论和实验描述下审查的模型催化剂的反应性将开发。

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.