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沸石孔体积对烯烃选择性制备丙烯的关键作用。

Key role of the pore volume of zeolite for selective production of propylene from olefins.

机构信息

Department of Environmental Chemistry and Engineering, Interdisciplinary Graduate School of Science and Engineering, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama 226-8502, Japan.

出版信息

Phys Chem Chem Phys. 2010 Mar 20;12(11):2541-54. doi: 10.1039/b921927g. Epub 2010 Jan 25.

Abstract

A plausible reaction mechanism for propylene (C(3)H(6)) production from ethylene (C(2)H(4)) was investigated, based on the amounts of effluent hydrocarbons and hydrocarbons produced in the pores of SAPO-34. Propylene was produced via an oligomerization-cracking mechanism. On the basis of this mechanism, the conversions of C(2)H(4), pentenes, and hexenes were examined. The catalytic performance was compared, in order to investigate the role of the pore volume of zeolites with 8-, 10-, and 12-membered rings in the selective production of C(3)H(6). The selectivity for C(3)H(6) was crucially dependent upon the pore volume of the zeolite. Highly selective production of C(3)H(6) from olefins (C(2)H(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(3)H(6) and C(2)H(4) involving primary cations can be controlled by the pore volume of a zeolite.

摘要

基于 SAPO-34 孔道中流出的烃类和生成的烃类的量,研究了丙烯(C3H6)由乙烯(C2H4)生成的一个可能的反应机理。丙烯是通过齐聚-裂化机理生成的。根据这一机理,考察了 C2H4、戊烯和己烯的转化率。为了研究具有 8、10 和 12 元环的沸石的孔体积在 C3H6 选择性生成中的作用,对催化性能进行了比较。C3H6 的选择性主要取决于沸石的孔体积。通过采用新的概念,可以从烯烃(C2H4、戊烯和己烯)高度选择性地生成 C3H6:调整沸石的孔体积以适应烯烃及其碳正离子的体积,而不是采用传统的分子筛方法。例如,通过沸石的孔体积可以控制戊烯通过初级碳正离子转化为 C3H6 和 C2H4 的单分子裂化。

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