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芳氧基锆系催化剂催化乙烯齐聚与Friedel-Crafts烷基化的串联反应

秦一超 叶健 蒋斌波 王靖岱 阳永荣

高等学校化学学报Issue(9):1825-1831,7.
高等学校化学学报Issue(9):1825-1831,7.DOI:10.7503/cjcu20150312

芳氧基锆系催化剂催化乙烯齐聚与Friedel-Crafts烷基化的串联反应

Ethylene Oligomerization and Friedel-Crafts Alkylation Tandem Action Catalyzed by Aryloxy Zirconium Catalysts

秦一超 1叶健 1蒋斌波 1王靖岱 1阳永荣1

作者信息

  • 1. 浙江大学化学工程与生物工程学院,化学工程联合国家重点实验室,杭州310027
  • 折叠

摘要

Abstract

Linear α-olefins are currently produced predominantly by the oligomerization of ethylene. Among the most promising catalysts, zirconium catalysts are largely studied due to its mild reaction condition and well-distributed products. In this article, aryloxy zirconium catalysts, Zr( OAr) n Cl4-n ·mArOH, were synthesized via modifying the aryl ring structure. The influence of Zr/Phenol molar ratio and the free phenol content on ethylene oligomerization was studied. Among these catalytic systems, Zr(OPh)3Cl·mPhOH/TEA/EtAlCl2 was proved to be highly active with the activity up to 6. 8×104 g/(mol Zr·h), while the product consisted of mainly α-olefins( C4—C24 ) without polymers. In addition, a suitable amount of free phenol was found to be responsible for stabilizing the active species. It was also found that increasing the ethylene pressure or altering the substituents on the benzene ring could result in the formation of a tandem catalytic system, in which the obtained α-olefins were then mostly converted into the corresponding Friedel-Crafts alkylated-toluene products.

关键词

芳氧基锆催化剂/乙烯齐聚/Friedel-Crafts烷基化/串联反应/α-烯烃

Key words

Aryloxy zirconium catalyst/Ethylene oligomerization/Friedel-Crafts alkylated reaction/Tandem action/α-Olefin

分类

化学化工

引用本文复制引用

秦一超,叶健,蒋斌波,王靖岱,阳永荣..芳氧基锆系催化剂催化乙烯齐聚与Friedel-Crafts烷基化的串联反应[J].高等学校化学学报,2015,(9):1825-1831,7.

基金项目

国家自然科学基金(批准号:21176208)和上海市聚烯烃核心技术重点实验室开放基金(批准号:120DZ260400)资助 (批准号:21176208)

高等学校化学学报

OA北大核心CSCDCSTPCD

0251-0790

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