Garcia Clara, Truttmann Vera, Lopez Irene, Haunold Thomas, Marini Carlo, Rameshan Christoph, Pittenauer Ernst, Kregsamer Peter, Dobrezberger Klaus, Stöger-Pollach Michael, Barrabés Noelia, Rupprechter Günther
Institute of Materials Chemistry, Technische Universität Wien, Getreidemarkt 9/BC/165, 1060 Vienna, Austria.
Instituto De Tecnología Química, Universitat Politecnica de Valencia - Consejo Superior de Investigaciones Científicas (UPV-CSIC), Av. de los Naranjos, s/n, 46022 Valencia, Spain.
J Phys Chem C Nanomater Interfaces. 2020 Oct 29;124(43):23626-23636. doi: 10.1021/acs.jpcc.0c05735. Epub 2020 Oct 20.
Doping gold nanoclusters with palladium has been reported to increase their catalytic activity and stability. PdAu nanoclusters, with the Pd dopant atom located at the center of the Au cluster core, were supported on titania and applied in catalytic CO oxidation, showing significantly higher activity than supported monometallic Au nanoclusters. After pretreatment, DRIFTS spectroscopy detected CO adsorbed on Pd during CO oxidation, indicating migration of the Pd dopant atom from the Au cluster core to the cluster surface. Increasing the number of Pd dopant atoms in the Au structure led to incorporation of Pd mostly in the S-(M-S) protecting staples, as evidenced by XAFS. A combination of oxidative and reductive thermal pretreatment resulted in the formation of isolated Pd surface sites within the Au surface. The combined analysis of XAFS, DRIFTS, and XPS thus revealed the structural evolution of bimetallic PdAu nanoclusters, yielding a Pd single-site catalyst of 2.7 nm average particle size with improved CO oxidation activity.
据报道，用钯掺杂金纳米团簇可提高其催化活性和稳定性。钯金纳米团簇中，钯掺杂原子位于金团簇核心的中心，负载在二氧化钛上并应用于催化一氧化碳氧化反应，其活性明显高于负载型单金属金纳米团簇。预处理后，漫反射红外傅里叶变换光谱（DRIFTS）检测到一氧化碳氧化过程中吸附在钯上的一氧化碳，表明钯掺杂原子从金团簇核心迁移到了团簇表面。增加金结构中钯掺杂原子的数量导致钯主要掺入到S-(M-S)保护钉中，这由X射线吸收精细结构光谱（XAFS）证实。氧化和还原热预处理相结合导致在金表面形成孤立的钯表面位点。因此，XAFS、DRIFTS和X射线光电子能谱（XPS）的综合分析揭示了双金属钯金纳米团簇的结构演变，得到了平均粒径为2.7纳米且一氧化碳氧化活性提高的钯单中心催化剂。
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