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Shape dependence of nanoceria on complete catalytic oxidation of o-xylene

机译:纳米氧化铈的形状依赖性对邻二甲苯的完全催化氧化

摘要

BTX (benzene, toluene, and xylene) in atmosphere, mainly emitted from various industrial processes and transportation activities, are of particular concern due to their potentially highly toxic effects on human health. Catalytic oxidation of o-xylene was investigated on nanosized CeO2 particles, cubes, and rods, among which rods show the highest activity, which is comparable with those of traditional noble-metal catalysts. CeO2 nanorods also exhibit long durability for o-xylene oxidation, without deactivation during a 50 h time-on stream test. Over the CeO2 rods and particles, the presence of water vapor slightly decreased o-xylene conversion, while water vapor enhanced o-xylene oxidation on the CeO2 cubes. High-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, positron annihilation spectroscopy, and O-2 temperature-programmed desorption measurements revealed that ceria rods enclosed by (111) and (100) facets exhibit the highest concentration of oxygen vacancy clusters (VCs), the presence of which promoted the adsorption of molecular oxygen. The lower the temperature for desorption of chemisorbed O-2 species is, the higher is the activity for o-xylene oxidation, identifying the key role of VCs in t(h)is reaction via the activation of molecular oxygen over nanoceria. The finding may also be fundamental for designing ceria-based catalysts with better performance for catalytic oxidation of volatile organic compounds.
机译:大气中的BTX(苯,甲苯和二甲苯)主要来自各种工业过程和运输活动,由于其对人体健康的潜在剧毒影响,引起人们的特别关注。在纳米尺寸的CeO2颗粒,立方体和棒上研究了邻二甲苯的催化氧化,其中棒表现出最高的活性,这与传统的贵金属催化剂相当。 CeO2纳米棒对邻二甲苯的氧化也显示出长久的耐用性,在50小时的运行时间测试中不会失活。在CeO2棒和颗粒上,水蒸气的存在会稍微降低邻二甲苯的转化率,而水蒸气会增强CeO2立方体上的邻二甲苯氧化。高分辨率透射电子显微镜,X射线光电子能谱,正电子an没能谱和O-2温度编程的解吸测量表明,被(111)和(100)面包围的二氧化铈棒显示出最高的氧空位簇(VC)浓度)的存在促进了分子氧的吸附。化学吸附的O-2物质的解吸温度越低,邻二甲苯氧化的活性就越高,通过在纳米氧化铈上激活分子氧来确定VC在t(h)is反应中的关键作用。该发现对于设计具有更好的挥发性有机化合物催化氧化性能的二氧化铈基催化剂也可能是基础的。

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