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Supramolecular self-assembled molecules as organic directing agent for synthesis of zeolites

机译:超分子自组装分子作为合成沸石的有机指导剂

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摘要

Solid materials with uniform micropores, such as zeolites, can act as selective catalysts and adsorbents for molecular mixtures by separating those molecules small enough to enter their pores while leaving the larger molecules behind(1,2). Zeolite A is a microporous material with a high void volume. Despite its widespread industrial use in, for example, molecular separations and in detergency(3,4), its capability as a petroleum-refining material is limited owing to its poor acid-catalytic activity and hydrothermal stability, and its low hydrophobicity. These characteristics are ultimately a consequence of the low framework Si/Al ratio (normally around one) and the resulting high cationic fraction within the pores and cavities(1,2). Researchers have modified the properties of type-A zeolites by increasing the Si/Al compositions up to a ratio of three(5-9). Here we describe the synthesis of zeolite A structures exhibiting high Si/Al ratios up to infinity ( pure silica). We synthesize these materials, named ITQ-29, using a supramolecular organic structure-directing agent obtained by the self-assembly, through pi-pi type interactions, of two identical organic cationic moieties. The highly hydrophobic pure-silica zeolite A can be used for hydrocarbon separations that avoid oligomerization reactions, whereas materials with high Si/Al ratios give excellent shape-selective cracking additives for increasing propylene yield in fluid catalytic cracking operations. We have also extended the use of our supramolecular structure-directing agents to the synthesis of a range of other zeolites.
机译:具有均匀微孔的固体材料,例如沸石,可以通过分离那些小到足以进入其孔的分子而将大分子留在后面的分子,充当分子混合物的选择性催化剂和吸附剂(1,2)。沸石A是具有高空隙体积的微孔材料。尽管其在例如分子分离和去污力方面得到了广泛的工业应用(3,4),但由于其弱的酸催化活性和水热稳定性以及低的疏水性,其作为石油精制材料的能力受到限制。这些特征最终归因于低的骨架Si / Al比(通常约为1)和在孔和腔内产生的高阳离子分数(1,2)。研究人员通过将Si / Al组成提高到三(5-9)的比例来改变A型沸石的性能。在这里,我们描述了一种沸石A结构的合成,该结构展现出高达Si / Al的无限高比(纯二氧化硅)。我们使用超分子有机结构导向剂合成了这些材料,命名为ITQ-29,该分子是通过pi-pi型相互作用自组装的两个相同的有机阳离子部分而获得的。高疏水性的纯二氧化硅沸石A可用于避免低聚反应的烃分离,而具有高Si ​​/ Al比的材料可提供出色的形状选择裂化添加剂,以提高流化催化裂化操作中的丙烯收率。我们还将超分子结构导向剂的用途扩展到了其他沸石的合成中。

著录项

  • 来源
    《Nature》 |2004年第7006期|p. 287-290|共4页
  • 作者单位

    Univ Politecn Valencia, CSIC, Inst Tecnol Quim, Valencia 46022, Spain;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 自然科学总论;
  • 关键词

    PORES;

    机译:毛孔;

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