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Surfactant-Concentration-Dependent Shape Evolution of AuPd Alloy Nanocrystals from Rhombic Dodecahedron to Trisoctahedron and Hexoctahedron

机译:从菱形十二面体到三八面体和六面体的AuPd合金纳米晶体的表面活性剂浓度依赖性形状演变

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摘要

The surface structure-controlled synthesis of noble metal nanocrystals (NCs) bounded by high-index facets has become a hot research topic due to their potential to significantly improve catalytic performance. This study reports the preparation of monodisperse Au-Pd alloy NCs with systematic shape evolution from rhombic dodecahedral (RD) to trisoctahedral (TOH), and hexoctahedral (HOH) structures by varying the concentration of surfactant in the surfactant-mediated synthesis. The as-prepared three kinds of alloy NCs possess almost the same size and composition as each other. It is suggested that the surfactant containing long-chain octadecyltrimethyl ammonium (OTA(+)) ions plays a key role in the formation of high index facets, and the crystal growth kinetics may also have an effect on the formation of different nanocrystal morphologies. In addition, the catalytic activities of these NCs are evaluated by structure-sensitive reactions, including ethanol electro-oxidation and the catalytic reduction of 4-nitrophenol (4-NPh). These three types of Au-Pd alloy NCs exhibit different catalytic selectivities towards these two reactions. The catalytic activities toward electro-oxidation of ethanol are in the order of HOH > RD > TOH, which follows the order of their corresponding surface energies. However, the activities toward catalytic reduction of 4-NPh are in the order of RD > TOH > HOH, which should be related to the local structure of the surfaces.
机译:由于具有显着改善催化性能的潜力,由高折射率小晶面界定的贵金属纳米晶体(NCs)的表面结构控制合成已成为研究的热点。这项研究报告了通过改变表面活性剂介导的合成物中表面活性剂的浓度来制备具有系统形状从菱形十二面体(RD)到三八面体(TOH)和六面体(HOH)结构的单分散Au-Pd合金NCs的方法。所制备的三种合金NC具有几乎相同的尺寸和组成。建议表面活性剂包含长链十八烷基三甲基铵(OTA(+))离子在高折射率小面的形成中起关键作用,并且晶体生长动力学也可能对不同纳米晶体形态的形成有影响。此外,这些NC的催化活性通过结构敏感的反应进行评估,包括乙醇电氧化和4-硝基苯酚(4-NPh)的催化还原。这三种类型的Au-Pd合金NCs对这两个反应表现出不同的催化选择性。乙醇电氧化的催化活性为HOH> RD> TOH,其遵循的是其相应表面能的顺序。但是,对4-NPh催化还原的活性的顺序为RD> TOH> HOH,这与表面的局部结构有关。

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