Banu Rareṣ, Loxha Adea, Müller Nicole, Spyroglou Stylianos, Rosenberg Egon Erwin, Palomares A Eduardo, Rey Fernando, Marini Carlo, Barrabés Noelia
Institue of Materials Chemistry, TU Wien, Getreidemarkt 9/E165, 1060 Vienna, Austria.
Institute of Chemical, Environmental and Bioscience Engineering, TU Wien, Getreidemarkt 9/E166, 1060 Vienna, Austria.
Nanoscale. 2025 Feb 27;17(9):5098-5105. doi: 10.1039/d4nr03865g.
In the field of nanocluster catalysis, it is crucial to understand the interplay of different parameters, such as ligands, support and pretreatment and their effect on the catalytic process. In this study, we chose the selective hydrogenation of phenylacetylene as a model reaction and employed two gold nanoclusters as catalysts, the phosphine protected Au and the thiolate protected Au, each with different binding motifs. They were supported on MgO, AlO and a hydrotalcite (HT), chosen for their different acidity. We found that while in the case of the Au MgO was the preferred support and the pretreatment had a positive impact on the catalysis. For the Au the HT performed best and pretreating had negative effects, indicating that the bonding motif of the ligands and their interaction with the support is crucial for the catalytic process. Using X-ray absorption spectroscopy we could trace these phenomena to changes in the cluster-ligand interface, which seem to impact the stability of the catalysts.
在纳米团簇催化领域，理解不同参数（如配体、载体和预处理）之间的相互作用及其对催化过程的影响至关重要。在本研究中，我们选择苯乙炔的选择性加氢作为模型反应，并使用两种金纳米团簇作为催化剂，即膦保护的金和硫醇盐保护的金，它们各自具有不同的结合模式。它们负载在氧化镁、氧化铝和水滑石（HT）上，选择这些载体是因其具有不同的酸度。我们发现，对于金/氧化镁而言，氧化镁是首选载体，且预处理对催化有积极影响。对于金/水滑石，水滑石表现最佳，而预处理则有负面影响，这表明配体的键合模式及其与载体的相互作用对催化过程至关重要。利用X射线吸收光谱，我们可以将这些现象追溯到团簇 - 配体界面的变化，这些变化似乎会影响催化剂的稳定性。
