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Oxidative dehydrogenation of ethane to ethylene over LiCl/SO42--ZrO2 catalyst

机译:LiCl / SO42-ZrO2催化剂上乙烷氧化脱氢制乙烯

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摘要

Sulfated zirconia (SO42--ZrO2) samples were prepared by a modified two-step method (refluxing ZrO(OH)(2) precursor in basic solution followed by drying and (NH4)(2)SO4 impregnation) and then impregnated with a LiCl solution to give the SO42--ZrO2-supported LICI catalysts with Li mass content of 0.5% similar to 15%. The catalysts were characterized by X-ray diffraction, scanning electron microscopy, N-2 adsorption, temperature-programmed desorption-mass spectrometry, and X-ray photoelectron spectroscopy. The results show that with increasing LiCl loading, the specific surface area and acidity of the catalysts as well as the volume fraction of tetragonal zirconia in the catalysts decrease, while the catalytic performance of the catalysts for oxidative dehydrogenation of ethane (ODHE) to ethylene increases. Over the LiCl/SO42--ZrO2 catalyst with a Li content of 15% ethylene yield of 77.8% with an ethane conversion of 90.6% is achieved at 650 degrees C, and the yield higher than 71% is maintained over a period of 24 h. The textural structure of ZrO? has little effect on the catalytic behavior of the LiCl/SO42--ZrO2 catalysts. The specific surface area of SO42--ZrO2 samples prepared by the fled two-step method is much bigger than that of the SO42--ZrO2 samples made by the method reported in literature, and therefore more LiCl call be loaded on unit mass of support. This is favorable to improve the catalyst stability and slow down catalyst deactivation during the ODHE reaction due to the loss of LiCl.
机译:通过改进的两步法(在碱性溶液中回流ZrO(OH)(2)前驱体,然后干燥和(NH4)(2)SO4浸渍)制备硫酸化氧化锆(SO42-ZrO2)样品,然后用LiCl浸渍溶液制得SO42-ZrO2负载的LICI催化剂,其Li质量含量为0.5%类似于15%。通过X射线衍射,扫描电子显微镜,N-2吸附,程序升温解吸质谱和X射线光电子能谱对催化剂进行了表征。结果表明,随着LiCl负载量的增加,催化剂的比表面积和酸度以及四方氧化锆的体积分数降低,而催化剂对乙烷(ODHE)氧化脱氢为乙烯的催化性能提高。 。在650℃下,Li含量为15%的LiCl / SO42-ZrO2催化剂的乙烯收率为77.8%,乙烷转化率为90.6%,并在24小时内保持高于71%的收率。 ZrO的组织结构?对LiCl / SO42-ZrO2催化剂的催化行为影响很小。通过两步法制备的SO42-ZrO2样品的比表面积要比文献报道的方法制备的SO42-ZrO2样品的比表面积大得多,因此在载体的单位质量上需要负载更多的LiCl。 。这有利于提高催化剂的稳定性并减慢在ODHE反应期间由于LiCl的损失而引起的催化剂失活。

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