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首页> 外文期刊>Catalysis science & technology >Sub-15 nm CeO2 nanowires as an efficient non-noble metal catalyst in the room-temperature oxidation of aniline
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Sub-15 nm CeO2 nanowires as an efficient non-noble metal catalyst in the room-temperature oxidation of aniline

机译:Sub-15 nm CeO2纳米线作为一种高效的非贵金属金属在室温氧化催化剂苯胺的

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We described herein the facile synthesis of sub-15 nm CeO2 nanowires based on a hydrothermal method without the use of any capping/stabilizing agent, in which an oriented attachment mechanism took place during the CeO2 nanowire formation. The synthesis of sub-15 nm CeO2 nanowires could be achieved on relatively large scales (similar to 2.6 grams of nanowires per batch), in high yields (94%), and at low cost. To date, there are only a limited number of successful attempts towards the synthesis of CeO2 nanowires with such small diameters, and the reported protocols are typically limited to low amounts. The nanowires displayed uniform shapes and sizes, high surface areas, an increased number of oxygen defects sites, and a high proportion of Ce3+/Ce4+ surface species. These features make them promising candidates for oxidation reactions. To this end, we employed the selective oxidation of aniline as a model transformation. The sub-15 nm CeO2 nanowires catalyzed the selective synthesis of nitrosobenzene (up to 98% selectivity) from aniline at room temperature using H2O2 as the oxidant. The effect of solvent and temperature during the catalytic reaction was investigated. We found that such parameters played an important role in the control of the selectivity. The improved catalytic activities observed for the sub-15 nm nanowires could be explained by: i) the uniform morphology with a typical dimension of 11 +/- 2 nm in width, which provides higher specific surface areas relative to those of conventional catalysts; ii) the significant concentration of oxygen vacancies and high proportion of Ce3+/Ce4+ species at the surface that represent highly active sites towards oxidation reactions; iii) the crystal growth along the (110) highly catalytically active crystallographic directions, and iv) the mesoporous surface which is easily accessible by liquid substrates. The results reported herein demonstrated high activities under ambient conditions, provided novel insights into selectivities, and may inspire novel metal oxide-based catalysts with desired performances.
机译:我们这里描述的简单合成sub-15基于水热方法纳米CeO2纳米线没有任何限制/稳定剂的使用,一个面向附件机制了在CeO2纳米线的形成。sub-15 nm CeO2纳米线的合成实现在较大尺度上(类似于2.6克每批纳米线),在高收益率(在94%),低成本。只有数量有限的成功尝试对CeO2纳米线的合成等小直径,和报告的协议通常仅限于少量。显示统一的形状和大小,表面高领域,增加氧缺陷的数量网站,高比例的Ce3 + / Ce4 +表面物种。候选人氧化反应。我们雇佣了苯胺的选择性氧化一个模型转换。纳米线催化选择性的合成亚硝基苯(选择性高达98%)苯胺在室温下使用过氧化氢作为氧化剂。在催化反应研究。我们发现这样的扮演了一个重要的参数在选择性的控制作用。改善催化活动的观察sub-15 nm纳米线可以解释为:我)统一的形态与一个典型的维11+ / - 2 nm宽,它提供了更高的特定相对于那些传统的表面区域催化剂;氧空位和高比例的Ce3 + / Ce4 +表示高度的物种在表面活跃的网站对氧化反应;晶体生长沿着(110)高度催化地活跃的结晶方向,(四)介孔表面很容易可通过液体基质。这里报道了高的活动在环境条件下,提供了新颖的见解选择性,可以激发新颖的金属氧化物催化剂与预期的表现。

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