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1篇 您的检索式:作者名="David R.Mullins"
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1CO oxidation over ceria supported Au_(22) nanoclusters: Shape effect of the support显示文摘Gold(Au) nanoclusters have recently emerged as ideal models for understanding Au catalysis, because the nanosized Au particles have precise atomic numbers and uniform size. In this work, we studied for the first time the support shape effect on the catalysis of Au nanoclusters by using CO oxidation as a model reaction. Au_(22)(L^8)_6(L = 1,8-bis(diphenylphosphino) octane) nanoclusters were supported on CeO_2 rods or cubes, then pretreated at different temperatures(up to 673 K), allowing the gradual removal of the organic phosphine ligands. CO oxidation test over these differently pretreated samples shows that CeO_2 rods are much better supports than cubes for Au_(22) nanoclusters in enhancing the reaction rate. In situ IR spectroscopy coupled with CO adsorption indicates that the shape of CeO_2 support can impact the nature and quantity of exposed Au sites, as well as the efficiency of organic ligand removal. Although CeO_2 rods are helpful in exposing a greater percentage of total Au sites upon ligands removal, the percentage of active Au sites(denoted by Au d+, 0 < d < 1) is lower than that on CeO_2 cubes. The in situ extended X-ray absorption spectroscopy(EXAFS) and high-angle annular dark-field scanning transmission electron microscopy(HAADF-STEM) results show that the Au nanoclusters bound more strongly to the CeO_2 rods than to the cubes where the Au nanoclusters show more sintering. Considering the typical redox mechanism for CO oxidation over supported Au nanoclusters and nanoparticles, it is concluded that the reactivity of the lattice oxygen of CeO_2 is the determining factor for CO oxidation over Au_(22)/CeO_2. CeO_2 rods offer more reactive lattice oxygen and abundant oxygen vacancies than the cubes and thus make the rods a superior support for Au nanoclusters in catalyzing low temperature CO oxidation.Zili Wu David R.Mullins Lawrence F.Allard Qianfan Zhang Laisheng Wang 2018Chinese Chemical Letters2018,29,6:4
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