Hakimioun Amir H, Vandegehuchte Bart D, Curulla-Ferre Daniel, Kaźmierczak Kamila, Plessow Philipp N, Studt Felix
Institute of Catalysis Research and Technology, Karlsruhe Institute of Technology, Hermann-von-Helmholtz Platz 1, 76344 Eggenstein-Leopoldshafen, Germany.
TotalEnergies OneTech Belgium, B-7181 Seneffe, Belgium.
ACS Omega. 2023 Mar 7;8(11):10591-10599. doi: 10.1021/acsomega.3c00502. eCollection 2023 Mar 21.
Oxide supports play an important role in enhancing the catalytic properties of transition metal nanoparticles in heterogeneous catalysis. How extensively interactions between the oxide support and the nanoparticles impact the electronic structure as well as the surface properties of the nanoparticles is hence of high interest. In this study, the influence of a magnesium oxide support on the properties of copper nanoparticles with different size, shape, and adsorption sites is investigated using density functional theory (DFT) calculations. By proposing simple models to reduce the cost of the calculations while maintaining the accuracy of the results, we show using the nonreducible oxide support MgO as an example that there is no significant influence of the MgO support on the electronic structure of the copper nanoparticles, with the exception of adsorption directly at the Cu-MgO interface. We also propose a simplified methodology that allows us to reduce the cost of the calculations, while the accuracy of the results is maintained. We demonstrate in addition that the Cu nanowire model corresponds well to the nanoparticle model, which reduces the computational cost even further.
氧化物载体在增强过渡金属纳米颗粒在多相催化中的催化性能方面起着重要作用。因此，氧化物载体与纳米颗粒之间的相互作用在多大程度上影响纳米颗粒的电子结构以及表面性质备受关注。在本研究中，使用密度泛函理论（DFT）计算研究了氧化镁载体对具有不同尺寸、形状和吸附位点的铜纳米颗粒性质的影响。通过提出简单模型以降低计算成本同时保持结果的准确性，我们以不可还原的氧化物载体MgO为例表明，除了直接吸附在Cu-MgO界面处外，MgO载体对铜纳米颗粒的电子结构没有显著影响。我们还提出了一种简化方法，该方法可以在保持结果准确性的同时降低计算成本。此外，我们证明铜纳米线模型与纳米颗粒模型非常吻合，这进一步降低了计算成本。
