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首页> 外文期刊>Catalysis science & technology >Dual catalyst system for selective vinyl chloride production via ethene oxychlorination
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Dual catalyst system for selective vinyl chloride production via ethene oxychlorination

机译：双重选择性氯化乙烯的催化剂体系通过乙烯氧氯化生产

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A dual system comprising two catalytic reactors connected in series was developed for the direct conversion of ethene to vinyl chloride monomer (VCM). The first reactor uses ZrO2-supported ceria (CeO2/ZrO2) to perform ethene oxychlorination to 1,2-dichloroethene (EDC) that is dehydrochlorinated to VCM in the second reactor over calcium-promoted gamma-Al2O3. The choice of carrier for ceria is of critical importance to maximize the EDC production by reducing combustion products. While MgO, SiO2, SiC, TiO2, ZSM-5, and gamma-Al2O3 carriers induced higher overoxidation compared to bulk ceria, ZrO2 was the only carrier that suppressed COx formation. Moreover, the latter carrier led to the highest oxychlorination activity. The unique performance of the CeO2/ZrO2 catalyst was rationalized by its ability to promote chlorine evolution and to suppress the combustion of chlorinated products, as inferred from the activity evaluation in HCl and VCM oxidation, respectively. The outstanding redox properties, enabling operation at low temperature and thus high selectivity, are associated with the formation of defective CeO2 nanoparticles, contrasting the low activity over Ce-Zr mixed oxide. In order to subsequently form VCM, an efficient EDC dehydrochlorination catalyst was designed by moderating the acidity of gamma-Al(2)O(3)via calcium doping and used in a reactor after CeO2/ZrO2. This dual catalyst system displayed 100% selectivity to VCM at 25% ethene conversion, surpassing the space time yield of the best ethene-to-VCM catalyst EuOCl by a factor of four, where the first step is operated at an elevated temperature of about 100-150 K with respect to cupric chloride benchmarks. In addition, the catalytic dehydrochlorination, operated at a lower temperature of 100 K than the current non-catalytic process, showed minimized coke formation. This developed system rendered stable after slight initial deactivation, offering promising potential to intensify VCM production.
机译：双系统包括两个催化反应器直接连接在系列开发转换对氯乙烯单体乙烯(VCM)。二氧化铈(CeO2 /锆)执行乙烯氧氯化1,2-dichloroethene (EDC)dehydrochlorinated VCM第二吗反应堆在calcium-promoted gamma-Al2O3。二氧化铈的载体选择的关键EDC最大化生产的重要性减少燃烧产品。原文如此,二氧化钛,ZSM-5 gamma-Al2O3运营商诱导高氧化过度而散装二氧化铈锆是唯一的载体,抑制考克斯的形成。最高的氯氧化活性。独特的CeO2 /锆催化剂的性能合理化的能力促进氯进化和压制的燃烧氯化产品,作为推断的活动评估在盐酸和VCM氧化,分别。在较低的温度下,从而启用操作选择性高,相关的有缺陷的CeO2纳米颗粒的形成,对比低活动Ce-Zr混合氧化物。高效的EDC脱氯化氢作用的催化剂设计的缓和的酸度gamma-Al (2) O(3)通过钙掺杂和中使用反应堆CeO2 /氧化锆。系统显示100%的选择性VCM为25%乙烯转换,超越时空产量的最佳ethene-to-VCM EuOCl的催化剂四倍,是第一步在温度升高100 - 150 K对氯化铜基准。脱氯化氢作用,以更低的操作比当前的温度100 K非催化过程,显示最小化可乐形成。轻微的初始失活后,祭有前途的潜在加强VCM生产。

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