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Investigation of the hydrocarbon pool species responsible for methanol to olefin catalysis on acidic zeolite and zeotype catalysts.

机译：研究在酸性沸石和分子筛催化剂上负责甲醇催化烯烃合成的烃类物质。

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摘要

The main theme of this dissertation is the study of aromatic hydrocarbon pool in the catalysis of methanol conversion to light olefins on zeolite and zeotype materials through the usage of gas chromatography, mass spectrometry, and isotopic labeling. The goal was to identify and characterize the species responsible for the majority of ethylene produced in methanol-to-olefin catalysis. The mechanism for methanol to olefin catalysis was originally thought to only proceed through an aromatic hydrocarbon pool, but this was difficult to reconcile with product spectrums of different catalysts. From this developed a dual cycle mechanism consisting of two hydrocarbon pools.;Ethylene is the most valuable of the products produced from methanol to olefin catalysis. Modifying catalysts or reaction conditions to maximize ethylene selectivity requires an understanding of which hydrocarbon pool produces ethylene in the highest selectivity and just how selective that hydrocarbon pool is.;The first two chapters of this dissertation pertain to a general overview of zeolites, zeotypes, and the methanol to olefins reaction. An understanding of the methanol to olefins reaction and the catalysts that make it possible are necessary for the remaining two chapters. The latter two chapters focus on the aromatic hydrocarbon pool and its role in methanol to olefins catalysis. Chapter three focuses on determining the selectivity of the two most valuable products of methanol to olefin catalysis -- ethylene and propylene. This selectivity is determined for both the aromatic hydrocarbon pool and the olefinic hydrocarbon pool while minimizing the effects of the alternate hydrocarbon pool. In chapter four, the product spectrum of the reaction of several polymethylbenzenes are determined over a zeotype and zeolite that share the faujasite topology. Results confirm that methylated aromatic species are the best route to ethylene in methanol to olefins catalysis, and that a higher acid strength is more selective for ethylene.
机译：本论文的主要主题是通过气相色谱，质谱和同位素标记研究在沸石和分子筛材料上催化甲醇转化为轻烯烃的芳烃库。目的是鉴定和表征负责甲醇制烯烃催化过程中产生的大部分乙烯的物质。最初认为甲醇催化烯烃催化的机理仅通过芳烃池进行，但这很难与不同催化剂的产物光谱相协调。由此发展出了一个由两个碳氢化合物池组成的双循环机理。乙烯是甲醇到烯烃催化生产的最有价值的产品。修改催化剂或反应条件以最大程度地提高乙烯的选择性需要了解哪个烃池以最高的选择性产生乙烯，以及该烃池的选择性如何。本论文的前两章概述了沸石，分子筛类型和甲醇与烯烃反应。在剩下的两章中，必须了解甲醇与烯烃的反应以及使之成为可能的催化剂。后两章重点介绍芳族烃库及其在甲醇制烯烃催化中的作用。第三章着重于确定甲醇对烯烃催化的两种最有价值的产物-乙烯和丙烯的选择性。确定了芳香烃库和烯烃烃库的选择性，同时将备用烃库的影响降至最低。在第四章中，确定了几种具有八面沸石拓扑结构的沸石和沸石的反应产物谱。结果证实，甲基化的芳香族物质是甲醇中甲醇制烯烃的最佳途径，而较高的酸强度对乙烯更具选择性。

著录项

  • 作者

    Guenther, Darryl Roy.;

  • 作者单位

    University of Southern California.;

  • 授予单位 University of Southern California.;
  • 学科 Chemistry Inorganic.;Chemistry Organic.
  • 学位 Ph.D.
  • 年度 2010
  • 页码 129 p.
  • 总页数 129
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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