Development and Design of New Heat-resistant Zeolite

新型耐热沸石的开发设计

• 批准号: 06555241
• 负责人: MIYAMOTO Akira
• 金额: $ 9.02万
• 依托单位: Tohoku University
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Scientific Research (A)
• 财政年份: 1994
• 资助国家: 日本
• 起止时间: 1994 至 1996
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-06555241/
• 关键词: Zeolite; Heat Resistance; deactivation of Catalysts; X-ray Diffraction; Molecular Dynamics; High Resolution transmission electron microscopy; Computer Graphics; Density Functional Method; モンテカルロ法; X線回析; 結晶成長機構; コンピュータグラフィックス

Zeolite are industrially important catalysts because of their applications to cracking, hydrocarbon isomerization, alkylation, and meethanol-to-gasoline processing etc. However, many zeolites catalysts with high activity and high selectivity have not been commercialized because of their lack of heat-resistance and water-resistance. Since it is not easy to clarify the deactivation process of zeolite catalysts experimentally, theoretical methods are desirable in addition to elaborate experimental work. In this investigation we studied the deactivation process of zeolite catalysts by using experimental technique and theoretical method. Particularly we investigated in detail : (1) the dealumination mechanism of zeolite by high-resolution transmission electron microscopy (HRTEM), (2) the mechanism of crystal growth, (3) reproducing the thermal destruction of zeolites molecular dynamics (MD) and computer graphics, (4) the deactivation process by water by density functional (DF) methods. As results, it was clarified that : (1) detailed information of the dealumination mechanism of zeolite can be obtained, (2) the possibilities of the design of new novel zeolites, (3) the heat-resistance of new novel zeolites by MD method can be predicted, and (4) the order of water-resistance in a reaction by DF method can be predicted. So it is considered that out investigation progressed and was successful to obtain important and fruitful results. Furthermore we will try to extract more useful information assuming more diversified model system.

分子筛催化剂在裂解、烃类异构化、烷基化、甲醇制汽油等方面具有重要的工业应用价值，但许多高活性、高选择性的分子筛催化剂由于缺乏耐热性和耐水性而未能实现工业化。由于通过实验来阐明沸石催化剂的失活过程并不容易，因此除了精细的实验工作之外，理论方法也是可取的。本文采用实验和理论相结合的方法研究了分子筛催化剂的失活过程。（1）用高分辨透射电子显微镜（HRTEM）研究了沸石的脱铝机理;（2）沸石的晶体生长机理;（3）用分子动力学（MD）和计算机图形学再现了沸石的热破坏过程;（4）用密度泛函（DF）方法研究了水对沸石的失活过程。结果表明：（1）可以获得沸石脱铝机理的详细信息，（2）设计新型沸石的可能性，（3）可以用MD法预测新型沸石的耐热性，（4）可以用DF法预测反应中的耐水性顺序。因此，我们认为，我们的研究取得了进展，并取得了重要而丰硕的成果。此外，我们将尝试提取更多有用的信息，假设更多样化的模型系统。

项目成果

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E.BROCLAWIK 等人：“金属交换 ZSM-5 中镓位点上甲烷活化反应路径的密度泛函理论计算”化学物理杂志。

M.Yamadaya et al.: "Quantum Chemical Investigation of Reactats in Selictive Reduction of NOx on Ion Excbargel ZOM-5" Studies in Surface Science and Catalysis. 105. 1485-1492 (1997)

M.Yamadaya 等人：“离子 Excbargel ZOM-5 上氮氧化物选择性还原反应的量子化学研究”表面科学和催化研究。

A.Miyamoto et al.: "Structure and Dynamics of Ion-exchanged Zeolites as Investigated by Molecular Dynamics and Computer Graphics" Studies in Surface Science and Catalysis. 83. 117-124 (1994)

A.Miyamoto 等人：“通过分子动力学和计算机图形学研究离子交换沸石的结构和动力学”表面科学和催化研究。

O.Tarasaki et al.: "What can we observe in zeolite related materials by HRTEM?" Catalysis Today. 23. 201-218 (1995)

O.Tarasaki 等人：“我们可以通过 HRTEM 在沸石相关材料中观察到什么？”

O.Terasaki: "Fine Structures of Zeolites" J.Electron Microscopy. 43. 337-346 (1994)

O.Terasaki：“沸石的精细结构”J.电子显微镜。