Theoretical Investigation of the Structural Properties of Copper Clusters at Zinc Oxide

氧化物负载的金属团簇在非均相催化中起着重要的作用。一个突出的例子是甲醇合成，它是由分散的铜和氧化锌颗粒催化的。尽管研究深入，实验数据丰富，但催化剂的原子结构仍是未知的，迫切需要理论研究来解开催化剂的详细结构。不幸的是，如果使用密度泛函理论等方法，则由于系统的复杂性，计算机模拟催化剂的实际结构模型受到严重阻碍。在这个项目中，基于人工神经网络的非常有效的原子间势，其精度接近第一性原理计算，将被开发并用于详细表征催化剂的结构特性。获得的信息将与实验数据相结合，以提供对活性位点性质的新见解。这是未来研究催化过程的详细反应机理的必要条件，迄今为止只能使用大大简化的模型系统进行研究。

Oxide-supported metal clusters play an important role in heterogeneous catalysis. A prominent example is methanol synthesis, which is catalyzed by dispersed copper and zinc oxide particles. In spite of intensive research and a wealth of experimental data, the atomistic structure of the catalyst is still unknown, and theoretical studies are urgently needed to unravel the detailed structure of the catalyst. Unfortunately, computer simulations of realistic structural models of the catalyst are severely hampered by the complexity of the system if methods like density-functional theory are used. In this project very efficient interatomic potentials based on artificial neural networks with an accuracy close to first principles calculations will be developed and employed to characterize the structural properties of the catalyst in detail. The obtained information will be combined with experimental data to provide new insights into the nature of the active sites. This is a mandatory condition for future studies of the detailed reaction mechanism of the catalytic process, which to date could be investigated using drastically simplified model systems only.