用过氧化氢催化苯乙烯环氧化用各种前体制备的氧化钙催化剂

Qingming Gu, Dan Han, Lei Shi, Qi Sun
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引用次数: 21

摘要

以市售的醋酸钙、碳酸钙、氢氧化钙、草酸钙等钙盐前驱体为原料,经煅烧合成了一系列的CaO样品。发现CaO样品在乙腈存在下使用过氧化氢作为氧化剂对苯乙烯的环氧化是有效的。为了确定理化性质和表面碱度对催化活性的影响,采用热重(TG)、x射线衍射(XRD)、扫描电镜(SEM)、n2吸附和程序升温解吸CO2 (CO2- tpd)对制备的CaO样品进行了表征。结果表明,CaO样品上强碱性位点的数量和高碱性强度是其具有优异催化性能的关键因素。相比之下,CaO样品的表面积、孔隙度和表面结构对催化活性的影响相对较小。用氢氧化钠在乙二醇溶液中沉淀硝酸钙,得到由Ca(OH)2分解得到的CaO样品,其强碱性位点数量最多,碱性位点强度也更强,因此在CaO样品中催化苯乙烯环氧化反应的速率最高。在选定的反应条件下,对苯乙烯氧化物的选择性为97.5%,转化率超过99%。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Styrene epoxidation with hydrogen peroxide over calcium oxide catalysts prepared from various precursors

A series of CaO samples were prepared by calcination of commercially available and synthesis of calcium salt precursors such as calcium acetate, carbonate, hydroxide and oxalate etc. CaO samples were found to be effective for the epoxidation of styrene using hydrogen peroxide as an oxidant in the presence of acetonitrile. To determine the influence of the physicochemical properties and surface basicity on the catalytic activity, the prepared CaO samples were characterized using thermogravimetry (TG), X-ray diffraction (XRD), scanning electron microscopy (SEM), N2-adsorption and temperature-programmed desorption of CO2 (CO2-TPD). The results indicate that the amounts of very strong basic sites and high basicity strength on CaO sample are key factors for its excellent catalytic performance. In contrast, the surface area, porosity and the surface structure of CaO sample have a relatively minor effect on the catalytic activity. CaO sample, obtained by the decomposition of Ca(OH)2, prepared by precipitating calcium nitrate with sodium hydroxide in ethylene glycol solution, exhibits the highest amount of very strong basic sites and stronger strength of basic sites, and therefore it catalyses the epoxidation of styrene with the highest rate among the tested CaO samples. Under the selected reaction conditions, the selectivity of 97.5% to styrene oxide at a conversion in excess of 99% could be obtained.

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来源期刊
Journal of Natural Gas Chemistry
Journal of Natural Gas Chemistry 化学-工程:化工
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