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基于金纳米立方体制备具有四面体、凹八面体和八面体结构的金-钯核壳纳米晶体及其电催化活性。

Au nanocube-directed fabrication of Au-Pd core-shell nanocrystals with tetrahexahedral, concave octahedral, and octahedral structures and their electrocatalytic activity.

机构信息

Department of Chemistry, National Tsing Hua University, Hsinchu 30013, Taiwan.

出版信息

J Am Chem Soc. 2010 Oct 20;132(41):14546-53. doi: 10.1021/ja105401p.

Abstract

In this study, we have successfully developed a facile method for the high-yield fabrication of Au-Pd core-shell heterostructures with an unusual tetrahexahedral (THH) morphology using Au nanocubes as the structure-directing cores. The lattice orientations of the Au nanocubes match those of the Pd shells. Structural analysis establishes that the THH nanocrystals are bounded by high-index {730} facets. A substantial lattice mismatch between Au and Pd, oxidative etching in the presence of chloride and oxygen, the use of cetyltrimethylammonium chloride (CTAC) surfactant, and the reaction temperature (30-60 °C) were identified to be key factors facilitating the formation of the THH core-shell nanocrystals. Intermediate products have also been examined to follow the growth process. By selecting cubic gold cores with sizes of 30-70 nm and varying the volume of the gold core solution used, THH Au-Pd core-shell nanocrystals with continuously adjustable sizes from 56 to 124 nm can be readily obtained. Their UV-vis spectra display progressive red-shifted bands. Interestingly, novel concave octahedral and octahedral Au-Pd core-shell nanocrystals can be prepared by lowering the reaction temperature and prolonging the reaction time. The concave octahedra show depressions on all the {111} faces. Electrocatalytic activity of the three Au-Pd core-shell structures for the oxidation of ethanol has been investigated. The THH nanocrystals with entirely high-index {730} facets were found to exhibit the best electrocatalytic activity. These size-tunable THH Au-Pd core-shell nanocrystals may be valuable for catalyzing other organic reactions.

摘要

在这项研究中,我们成功地开发了一种简便的方法,使用 Au 纳米立方体作为结构导向核,高产率制备具有异常四面体(THH)形态的 Au-Pd 核壳异质结构。Au 纳米立方体的晶格取向与 Pd 壳匹配。结构分析确定,THH 纳米晶体由高指数{730}面构成。Au 和 Pd 之间存在大量的晶格失配、存在氯和氧的氧化蚀刻、使用十六烷基三甲基氯化铵(CTAC)表面活性剂以及反应温度(30-60°C)被确定为促进 THH 核壳纳米晶体形成的关键因素。还检查了中间产物以跟踪生长过程。通过选择尺寸为 30-70nm 的立方金核,并改变使用的金核溶液的体积,可以容易地获得尺寸从 56 到 124nm 且连续可调的 THH Au-Pd 核壳纳米晶体。它们的紫外-可见光谱显示出逐渐红移的带。有趣的是,通过降低反应温度和延长反应时间,可以制备新颖的凹八面体和八面体 Au-Pd 核壳纳米晶体。凹八面体在所有{111}面上都有凹陷。研究了三种 Au-Pd 核壳结构对乙醇氧化的电催化活性。具有完全高指数{730}面的 THH 纳米晶体表现出最佳的电催化活性。这些尺寸可调的 THH Au-Pd 核壳纳米晶体可能对催化其他有机反应具有重要价值。

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