Synthesis of New Types of Zeolite, and their Application to Catalysis

新型沸石的合成及其催化应用

基本信息

批准号：
10450303
负责人：
SUGI Yoshihiro
金额：
$ 1.92万
依托单位：
Faculty of Engineering, Gifu University
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (B).
财政年份：
1998
资助国家：
日本
起止时间：
1998 至 2000
项目状态：
已结题

来源：
https://kaken.nii.ac.jp/en/grant/KAKENHI-PROJECT-10450303/
关键词：
Zeolite Catalysis Shape-selective catalysis Isopropylation H-Mordenite Zeolite Synthesis SDA GON

项目摘要

Clean chemical processes are one of key technologies for sustainable growth of industry. Zeolites are the most important candidate for the purpose. It is important to find new types of zeolite with large pores to establish new era of the zeolite catalysis, . We devote to synthesize new types of zeolite and to understand the mechanism of zeolite catalysis.1) Shape-selective formation of 4,4'-diisopropylbiphenyl (4,4'-DIPB) was observed in the isopropylation of biphenyl over H-mordenite (HM). The shape-selectivity was governed by spatial restriction at transition states in HM pores. The selectivity for 4,4'-DIPB was influenced by many factors such as SiO_2/Al_2O_3 ratio, reaction temperature.2) The high selectivities for 4,4'-DIPB in encapsulated products were observed because of shape-selective catalysis inside HM pores. The decrease of the selectivity for 4,4'-DIPB occurred with the increase of temperature : The decrease was ascribed to the isomerization of 4,4'-DIPB at the external ac … More id sites.3) Two organic templates were used as SDA for the synthesis of all-silica MTW.These templates gives MTW crystals with different stacking sequences. This is ascribed to the difference in the properties related to organic-silica interaction as well as other inorganic factors.4) 1,1'-Butylenedi (4-aza-1-azonia-2,5-dimethylbicyclo [2.2.2] octane) was used as structure-directing agent (SDA) for zeolite synthesis. A new phase (GUS-1) within ZSM-12 phase is obtained from all-silica crystal. GUS-1 is indexed in the orthorhombic crystal class with refined lattice constants a=16.4206(4), b=20.0540(4), and c=5.0464(1) Å. Framework topology of GUS-1 was reported in the Database of Zeolite Structures by IZA under the code GON.5) Synthesis of high-silica [Al]-SSZ-31 zeolite by dry-gel conversion method was found to be dependent on the alkali concentration of the initial gel, and a phase change from BEA to SSZ-31 to MFI was observed with time course at optimum alkali concentration. A phase transformation from BEA to SSZ-31 was observed when the crystallization temperature was changed from 150→C to 175→C. Less

清洁化学工艺是工业可持续发展的关键技术之一，寻找新型大孔沸石对于开创沸石催化的新时代非常重要。新型沸石并了解沸石催化机理。1）4,4'-二异丙基联苯（4,4'-DIPB）的择形形成联苯在H-丝光沸石(HM)上的异丙基化反应中观察到形状选择性受HM孔内过渡态空间限制的影响。4,4'-DIPB的选择性受SiO_2/Al_2O_3等多种因素的影响。比例，反应温度。2）由于HM内部的择形催化作用，在封装产品中观察到4,4'-DIPB的高选择性随着温度的升高，4,4'-DIPB 的选择性降低：这种降低归因于 4,4'-DIPB 在外部 ac … More id 位点的异构化。3) 两种有机模板。用作合成全二氧化硅 MTW 的 SDA。这些模板使 MTW 晶体具有不同的堆积顺序，这是由于与有机-二氧化硅相互作用以及其他无机相互作用相关的特性差异。 4) 1,1'-丁烯二(4-aza-1-azonia-2,5-二甲基双环[2.2.2]辛烷)被用作沸石合成的结构导向剂(SDA)新相(GUS)。 -1) ZSM-12 相是从全二氧化硅晶体中获得的，属于具有精细晶格常数的斜方晶系。 a=16.4206(4)、b=20.0540(4) 和 c=5.0464(1) Å。IZA 的沸石结构数据库中报告了 GON 的框架拓扑。5) 高分子筛的合成通过干凝胶转化法发现二氧化硅[Al]-SSZ-31沸石取决于初始凝胶的碱浓度，并且相在最佳碱浓度下，观察到从 BEA 到 SSZ-31 到 MFI 的变化，当结晶温度从 150→C 变为 175→C 时，观察到从 BEA 到 SSZ-31 的相变。