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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.

为了实现环境友好的化学过程，沸石催化剂的特殊功能被用于一些合成反应中，这些反应在工业上具有显著的环境问题.制备了具有丝光沸石和MCM-22结构的钛硅酸盐催化剂，用于环己酮的液相氨肟化反应。通过UV、IR、XRD和C_（116）O_（10）D_（22）O_（10）D_（12）-C_（118）O_（10）D_（22）O_（10）D_（14）交换等手段对产物进行了表征，结果表明Ti_（10）D_（14）+Ti_（10）D_（11）被引入到沸石骨架中。这些钛硅酸盐对环己酮肟的生成具有较高的活性和选择性.在环己酮肟的贝克曼重排反应中，镁碱沸石和Ca-A沸石对ε-己内酰胺具有较高的选择性。在动力学研究的基础上，讨论了反应方案和溶剂的影响.以具有不同酸性和结构的沸石为载体，结合负载铂颗粒，制备了庚烷异构化双功能催化剂。Pt-β对单甲基己烷和二甲基庚烷的异构化反应活性最高.通过化学气相沉积法将GeCl_（22）Ge_（22）Pt_（22）Ge_（22）负载在H-ZSM-5上。该催化剂具有较高的脱氢活性和较低的氢解活性，对丁烷制芳烃反应具有较高的活性、选择性和稳定性.具有MCM-22结构的钛硅分子筛对异丁烯和甲醛合成异丁烯醇具有较高的催化活性和选择性。与MCM-22分子筛相比，该分子筛的酸性较低，催化剂的使用寿命较长。