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C-C bond scission of carbocations in zeolite pore cavity showing enzyme-like recognition

沸石孔腔中碳正离子的 C-C 键断裂显示出类酶识别

基本信息

批准号：
23655122
负责人：
BABA Toshihide
金额：
$ 2.66万
依托单位：
Tokyo Institute of Technology
依托单位国家：
日本
项目类别：
Grant-in-Aid for Challenging Exploratory Research
财政年份：
2011
资助国家：
日本
起止时间：
2011 至 2012
项目状态：
已结题

项目摘要

The conversions of C_2H_4 , pentenes, and hexenes were examined. The catalytic performance was compared, in order to investigate the role of the pore volume of zeolites with8-, 10-, and 12-membered rings in the selective production of C_3H_6 . The selectivity for C_3H_6 was crucially dependent upon the pore volume of the zeolite. Highly selective production of C_3H_6 from olefins (C_2H_4,pentenes, and hexenes) can be accomplished by employing a new concept: adjusting the pore volume of a zeolite to accommodate the volume of an olefin and/or its carbenium cations, as opposed to a conventional molecular sieve approach. For example, an unimolecular cracking of pentenes into C_3H_6 and C_2H_4 involving primary cations can be controlled by the pore volume of a zeolite.Furthermore, the reaction mechanism for the production of C_3H_6 from C_2H_4 was also investigated. C_3H_6 was produced by the β-scission of the same specific octyl carbocations in the conversions of both butene and C_2H_4.

考察了C_2H_4、戊烯和己烯的转化率。比较了8元环、10元环和12元环分子筛的催化性能，考察了孔容对选择性生成C_3H_6的影响。C_3H_6的选择性主要取决于沸石的孔容。采用一种新的概念，即通过调节沸石的孔容来容纳烯烃和/或其正碳离子的体积，从而实现从烯烃（C_2H_4、戊烯和己烯）高选择性地生产C_3H_6，这与传统的分子筛方法不同。例如，在伯阳离子存在下，戊烯单分子裂解为C_3H_6和C_2H_4的反应可以通过沸石的孔容来控制，并对C_2H_4裂解制C_3H_6的反应机理进行了探讨。在丁烯和C_2H_4的转化过程中，C_3H_6是由相同的特定辛基碳正离子的β-断裂产生的。

项目成果

期刊论文数量（0）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Temperature Effect on 1H Chemical Shift of Hydroxyl Groups in Zeolites and Their Catalytic Activities as Solid Acids

DOI：
10.1021/jp3043945
发表时间：
2012-07-12
期刊：
JOURNAL OF PHYSICAL CHEMISTRY C
影响因子：
3.7
作者：
Munakata, Hajime;Koyama, To-ru;Baba, Toshihide
通讯作者：
Baba, Toshihide

Proton exchange reaction between hydroxyl groups in the supercage and those in the sodalitecage of Y zeolite as studied by variable temperature 1H MAS NMR

变温1H MAS NMR研究Y型沸石超级笼与方钠石笼羟基之间的质子交换反应

DOI：
发表时间：
2012
期刊：
The Journal of Physical Chemistry C
影响因子：
0
作者：
Krishna Reddy Jakkidi;Ken Motokura;To-ru Koyama;Akimitsu Miyaji;and Toshihide Baba;Naoki Asakawa,Ken Motokura,Tatsuaki Yashima,To-ru Koyama,Toshinori O-nuki,Akimitsu Miyaji,Toshihide Baba
通讯作者：
Naoki Asakawa,Ken Motokura,Tatsuaki Yashima,To-ru Koyama,Toshinori O-nuki,Akimitsu Miyaji,Toshihide Baba

Shape-selective catalysis determined by the volume of a zeolite cavity for propylene production by the conversion of lower olefins using a H+-exchanged zeolite

由沸石空腔体积决定的择形催化，用于通过使用 H 交换沸石转化低级烯烃来生产丙烯

DOI：
发表时间：
2012
期刊：
影响因子：
0
作者：
Yasuyoshi IWASE;Akinobu SHIGA;To-ru KOYAMA;Akimitsu MIYAJI;Ken MOTOKURA;Yasuharu SAKAMOTO and Toshihide BABA;Yasuyoshi Iwase,Akimitsu Miyaji,Ken Motokura,To-ru Koyama,Toshihide Baba
通讯作者：
Yasuyoshi Iwase,Akimitsu Miyaji,Ken Motokura,To-ru Koyama,Toshihide Baba

Concept of Shape-Selective Catalysis Determined by Volume of Zeolite Cavity and Reaction Mechanism for Propylene Production by the Conversions of Butene Using Proton Exchanged Zeolite

沸石空腔体积决定的择形催化概念及质子交换沸石转化丁烯制丙烯的反应机理

DOI：
发表时间：
2012
期刊：
Journal of Physical Chemistry C
影响因子：
3.7
作者：
Yasuyoshi IWASE;Akinobu SHIGA;To-ru KOYAMA;Akimitsu MIYAJI;Ken MOTOKURA;Yasuharu SAKAMOTO and Toshihide BABA
通讯作者：
Yasuharu SAKAMOTO and Toshihide BABA

Shape-Selective Catalysis Determined by the Volume of a Zeolite Cavity and the Reaction Mechanism for Propylene Production by the Conversion of Butene Using a Proton-Exchanged Zeolite