Development of environmentlly benign chemical processes using specific catalytic functions of zeolites

利用沸石的特定催化功能开发环境友好的化学工艺

基本信息

批准号：
09305054
负责人：
YASHIMA Tatsuaki
金额：
$ 23.87万
依托单位：
Tokyo Institute of Technology
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (A)
财政年份：
1997
资助国家：
日本
起止时间：
1997 至 1999
项目状态：
已结题

项目摘要

In order to achieve environmentally benign chemical processes, specific functions of zeolite catalysts have been utilized in some synthesis reactions, which have significant environmental problems in industry.1. Titanosilicates with mordenite and MCM-22 structure were prepared to use as catalysts for the liquid-phase ammoximation of cyclohexanone. Characterization by UV, IR, XRD and CィイD116ィエD1OィイD22ィエD2-CィイD118ィエD1OィイD22ィエD2 exchange revealed that TiィイD14+ィエD1 was introduced into the framework of zeolite structure. These titanosilicates showed high activity and selectivity for the formation of cyclohexanone oxime.2. Ferrierite and Ca-A zeolite were found to have high selectivity to ε-caprolactam in the Beckmann rearrangement of cyclohexanone oxime. Based on the kinetic results, the reaction scheme and the effect of solvent were discussed.3. Zeolites having various acidity and structure were used as a bi-functional catalyst for the isomerization of heptane combined with Pt particles loaded on the surface of zeolites. Pt-β showed the highest activity for the isomerization into monomethyl hexane and dimethyl heptane.4. Pt-Ge intermetallic compounds were supported on H-ZSM-5 by chemical vapor deposition of GeClィイD22ィエD2(acac)ィイD22ィエD2 onto Pt loaded H-ZSM-5. This catalyst gave high activity, selectivity and stability for the formation of aromatic hydrocarbons from butane because of high dehydrogenation activity and low hydrogenolysis activity.5. Titanosilicate with MCM-22 structure was revealed to have high activity and selectivity for the formation of isobutenol from isobutene and formaldehyde. Its low acidity resulted in the long catalyst life compared with MCM-22 aluminosilicate zeolite.From the above results, the possibility to realize the environmentally benign chemical process was discussed.

为了实现环境良性的化学过程，在某些合成反应中使用了沸石催化剂的特定功能，这些反应在行业中存在重大环境问题。1。准备用麦迪林和MCM-22结构的钛硅酸盐用作环己酮的液相屈光度的催化剂。 UV，IR，XRD和CII D116 D1O D22 D2-CII D118 D1O D22 D2 D2 D2交换的表征表明，将TII D14+ D1引入到沸石结构的框架中。这些钛硅酸盐在形成环己酮的氧电时表现出很高的活性和选择性。2。发现在环己酮氧电的贝克曼重排中，发现对ε-丙二酰酰胺的选择性很高。基于动力学结果，讨论了反应方案和偿付能力的效果3。沸石具有多种酸度，结构用作六烷的异构化含己烷的双官能催化剂，并结合了载有沸石表面的Pt颗粒。 PT-β在单甲基己烷和二甲基二甲烷中的异构化表现出最高的活性。4。通过GECLII D22（ACAC）II D22的化学蒸气沉积在PT装载的H-ZSM-5上，在H-ZSM-5上支持了PT-GE的金属间化合物。由于脱氢活性高和低氢解活性，该催化剂给出了从丁烷形成芳基烃的高活性，选择性和稳定性。5。与MCM-22结构的钛硅酸盐相结合，从异丁烯和甲醛形成异丁醇具有很高的活性和选择性。与MCM-22铝氧化沸石相比，其低酸度导致催化剂寿命长。从上述结果，讨论了讨论环境良性化学过程的可能性。