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Catalytic Activation of Lower Alkanes under Carbon Dioxide Atmosphere

二氧化碳气氛下低级烷烃的催化活化

基本信息

批准号：
07455321
负责人：
HATTORI Tadashi
金额：
$ 4.74万
依托单位：
Nagoya University
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (B)
财政年份：
1995
资助国家：
日本
起止时间：
1995 至 1996
项目状态：
已结题

项目摘要

The present research aims at examining the possibility of production of multi-branched higher aliphatic hydrocarbons from lower alkanes under carbon dioxide atmosphere, and the following results were obtained.(1) Acceleration of Ethane Aromatization by Carbon DioxideCarbon dioxide was confirmed to accelerate the aromatization of ethane over Ga-ZSM-5 catalysts, and its effect was clarified to be the kinetic effect to accelerate the oligomerization of ethylene, but not thermodynamic effect due to the consumption of hydrogen through reverse water gas shift reaction.(2) Factors Controlling Product Distribution of Propane AromatizationPropane aromatization was conducted by using various Ga-silicate with MFI structure to elucidate factors controlling product distribution of propane aromatization, and it was found that the catalytic activity and selectivity depend mainly on the acid amount due to framework Ga ions incorporated in silicate lattice and on the amount and the particle size of extra-framework Ga-oxide.A neural network was preliminarilly applied for the estimation of catalytic performance in order to develop a computer system for the analysis of factors controlling catalytic activity and selectivity of complicated catalytic reactions.(3) Structure Activity Relationship in Dehydrogenation of Propane on Ga-oxide Catalystvarious types of Ga-oxides were prepared and applied for the catalytic runs of propane dehydrogenation, and it was found that the propane dehydrogenation is a structure sensitive reaction demanding large Ga2O3 particles. The activity also depends on local structure of Ga ions in oxide.(4) Methane ActivationMethane was able to be converted at lower temperature such 450ﾟC in the presence of bromine compound on various oxide catalysts. A minor amount of aromatic compounds were formed at higher temperature by adding aromatization catalyst to this catalytic system.

本研究旨在考察在二氧化碳气氛下由低级烷烃制备多支链高级脂肪烃的可能性，并获得了以下结果。(1)二氧化碳促进乙烷芳构化研究证实了二氧化碳促进乙烷在Ga-ZSM-5催化剂上芳构化的作用，其作用是促进乙烯齐聚的动力学效应，而不是由于逆水煤气变换反应消耗氢气而引起的热力学效应。(2)丙烷芳构化产物分布的控制因素用不同MFI结构的硅酸镓进行丙烷芳构化反应，探讨丙烷芳构化产物分布的控制因素，发现催化剂的活性和选择性主要取决于骨架Ga离子进入硅酸盐晶格的酸量和骨架外Ga离子的量和粒径。将神经网络应用于催化剂性能的预测，以建立一个分析复杂催化反应活性和选择性控制因素的计算机系统。(3)丙烷脱氢反应中Ga氧化物催化剂的构效关系制备了不同类型的Ga氧化物，并将其用于丙烷脱氢反应中，发现丙烷脱氢反应是一个结构敏感反应，需要大尺寸的Ga_2 O_3颗粒。氧化物中Ga离子的局域结构也决定了其活性。(4)甲烷活化甲烷能够在较低的温度如450 ℃下在溴化合物存在下在各种氧化物催化剂上转化。在该催化体系中加入芳构化催化剂，在较高温度下生成少量芳香族化合物。