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

• 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
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-09305054/
• 关键词: Zeloite; Metallosilicate; Catalyst; Beckmann rearrangement; Ammoximation; Aromatization; Isobutenol; Environmentally benign process; シクロヘキサノンオキシム; ε-カプロラクタム; チタノシリケート; モルデナイト; シリカライト; ヘプタン; 異性化; 白金; オキシム化

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，在综合催化剂中使用了沸石催化剂的特定功能，这是环境问题的重要作用。1。 IR，XRD和C D1O D22 Yi D118 II D22交换TII D14+EIE D1被引入沸石结构的框架中。在沸石表面上的Pt型六烷的二象催化剂显示出异构化的异构化。 D2上加载的H-ZSM-5。从异丁烯和甲醛中形成异丁醇的选择性。

项目成果

Zheng-Bao Wang: "Isomerization of *-heptane over Pt-loaded zeolite βcatalysts"Applied Catalysis A : General. 159. 119-132 (1997)

王正宝：“*-庚烷在 Pt 负载沸石 β 催化剂上的异构化”应用催化 A：综述 159. 119-132 (1997)

P.Wu: "Isomorphous substitution of Fe^<3+>in the framework of aluminosilicate mordenite by hydrothermal synthesis"Microporous and Mesoporous Materials. 20. 139-147 (1998)

P.Wu：“通过水热合成在铝硅酸盐丝光沸石骨架中Fe^3的同晶取代”微孔和介孔材料。

T.Komatsu: "Cu^<2+>-exchanged MFI-ferrisilicate catalysts for the reduction of nitric oxide with ammonia" J.Chem.Soc.,Faraday Trans.94. 949-953 (1998)

T.Komatsu：“Cu^2-交换的MFI-硅酸铁催化剂用于用氨还原一氧化氮”J.Chem.Soc.，Faraday Trans.94。

Takayuki Komatsu: "Shape-Selective Catalysis"American Chemical Society. 410 (2000)

Takayuki Komatsu：“择形催化”美国化学会。

T.Yashima: "Vapor phase Beckmann rearrangement of cyclohexanone oxime on the zeolite catalysts"Catalysis Today. 38. 249-253 (1997)

T.Yashima：“环己酮肟在沸石催化剂上的气相贝克曼重排”《今日催化》。