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Towards Atomically Precise Supported Catalysts from Monolayer-Protected Clusters: The Critical Role of the Support.
Chemistry - A European Journal ( IF 3.9 ) Pub Date : 2020-03-27 , DOI: 10.1002/chem.202000637 Alessandro Longo 1, 2 , Ewoud J J de Boed 3 , Nisha Mammen 4 , Marte van der Linden 3 , Karoliina Honkala 5 , Hannu Häkkinen 4, 5 , Petra E de Jongh 3 , Baira Donoeva 3
Chemistry - A European Journal ( IF 3.9 ) Pub Date : 2020-03-27 , DOI: 10.1002/chem.202000637 Alessandro Longo 1, 2 , Ewoud J J de Boed 3 , Nisha Mammen 4 , Marte van der Linden 3 , Karoliina Honkala 5 , Hannu Häkkinen 4, 5 , Petra E de Jongh 3 , Baira Donoeva 3
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Controlling the size and uniformity of metal clusters with atomic precision is essential for fine‐tuning their catalytic properties, however for clusters deposited on supports, such control is challenging. Here, by combining X‐ray absorption spectroscopy and density functional theory calculations, it is shown that supports play a crucial role in the evolution of monolayer‐protected clusters into catalysts. Based on the acidic nature of the support, cluster‐support interactions lead either to fragmentation of the cluster into isolated Au–ligand species or ligand‐free metallic Au0 clusters. On Lewis acidic supports that bind metals strongly, the latter transformation occurs while preserving the original size of the metal cluster, as demonstrated for various Aun sizes. These findings underline the role of the support in the design of supported catalysts and represent an important step toward the synthesis of atomically precise supported nanomaterials with tailored physico‐chemical properties.
中文翻译：
从单分子保护的簇向原子精确负载的催化剂：载体的关键作用。
以原子精度控制金属团簇的大小和均匀度对于微调其催化性能至关重要，但是对于沉积在载体上的团簇而言，这种控制具有挑战性。在此，通过结合X射线吸收光谱法和密度泛函理论计算，表明载体在单层保护簇向催化剂的演化中起着至关重要的作用。根据载体的酸性性质，簇与载体之间的相互作用导致簇断裂成孤立的Au-配体物种或无配体的金属Au 0簇。对Lewis酸性载体，虽然保留该金属簇的原始大小绑定金属强烈，后一种情况发生转化，这表现为各种金Ñ大小。这些发现强调了载体在负载型催化剂设计中的作用，代表了合成具有精确理化性质的原子精确负载型纳米材料的重要一步。
更新日期：2020-03-27
中文翻译：
从单分子保护的簇向原子精确负载的催化剂：载体的关键作用。
以原子精度控制金属团簇的大小和均匀度对于微调其催化性能至关重要，但是对于沉积在载体上的团簇而言，这种控制具有挑战性。在此，通过结合X射线吸收光谱法和密度泛函理论计算，表明载体在单层保护簇向催化剂的演化中起着至关重要的作用。根据载体的酸性性质，簇与载体之间的相互作用导致簇断裂成孤立的Au-配体物种或无配体的金属Au 0簇。对Lewis酸性载体，虽然保留该金属簇的原始大小绑定金属强烈，后一种情况发生转化，这表现为各种金Ñ大小。这些发现强调了载体在负载型催化剂设计中的作用，代表了合成具有精确理化性质的原子精确负载型纳米材料的重要一步。
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