N-四氢糠基PNP配体/铬催化体系及其乙烯选择性齐聚性能

doi:10.6023/cjoc201703010

有机化学 ›› 2017, Vol. 37 ›› Issue (9): 2315-2321.DOI: 10.6023/cjoc201703010 上一篇下一篇

研究论文

N-四氢糠基PNP配体/铬催化体系及其乙烯选择性齐聚性能

刘睿^a, 钟向宏b^b, 刘振宇^b, 梁胜彪^b, 朱红平^a

a 厦门大学化学化工学院固体表面物理化学国家重点实验室厦门 361005;
b 中国石油化工股份有限公司茂名分公司茂名 525011

收稿日期:2017-03-03 修回日期:2017-05-05 发布日期:2017-05-17
通讯作者: 钟向宏, 朱红平 E-mail:zhongxh.mmsh@sinopec.com;hpzhu@xmu.edu.cn
基金资助:
国家自然科学基金面上（Nos.21473142，21673191）、创新群体基金（No.IRT_14R31）资助项目.

Selective Ethylene Oligomerization Catalyzed by the Chromium Complex Bearing N-Tetrahydrofurfuryl PNP Ligand

Liu Rui^a, Zhong Xianghong^b, Liu Zhenyu^b, Liang Shengbiao^b, Zhu Hongping^a

a State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University, Xiamen 361005;
b Maoming Branch R & D Institute, SINOPEC, Maoming 525011

Received:2017-03-03 Revised:2017-05-05 Published:2017-05-17
Contact: 10.6023/cjoc201703010 E-mail:zhongxh.mmsh@sinopec.com;hpzhu@xmu.edu.cn
Supported by:
Project supported by the National Natural Science Foundation of China (Nos. 21473142, 21673191) and the Innovative Research Team Program (No. IRT_14R31).

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摘要/Abstract

通过胺基锂盐分离的方法合成了一种未有报道过的N-四氢糠基PNP配体E.E分别与CrCl₃（THF）₃和Cr（CO）₆反应生成化合物[{Ph₂PN（CH₂OC₄H₇） PPh₂}CrCl₂（μ-Cl）]₂（1）和[Ph₂PN（CH₂OC₄H₇） PPh₂]Cr（CO）₄（2）.这三个化合物通过谱学和元素分析表征，化合物2进一步经过X射线单晶结构确认.在甲基铝氧烷（MAO）或其它助剂作用下，考察了1、2以及E/CrCl₃（THF）₃、E/Cr（acac）₃、E/CrCl₂（THF）₂催化体系催化乙烯齐聚的性能.这些体系高选择性地催化乙烯四聚，最高活性为15.9 kg（product）/g（Cr）·h，1-辛烯的选择性最高可达63.6%.

关键词: 铬配合物, 催化性能, 乙烯三聚联四聚, 催化反应条件

The N-tetrahydrofurfuryl diphoshinoamine (PNP) ligand (E) was synthesized by means of two-step salt elimination reactions where separation of the two kinds of the aminyl lithium salts for the respective reactions is necessary for obtaining a high yield of E. The ligand reacted with CrCl₃(THF)₃ and Cr(CO)₆ to give P,P-chelation complexes[{Ph₂PN(CH₂OC₄H₇)-PPh₂}CrCl₂(μ-Cl)]₂ (1) and[Ph₂PN(CH₂OC₄H₇)PPh₂]Cr(CO)₄ (2), respectively. Complexes E, 1 and 2 were characterized by spectroscopy and elemental analysis, of which complex 2 was further confirmed by X-ray crystallography. Upon activation with methylaluminoxane (MAO) or AlEt₃, the catalyst systems including 1, 2, E/CrCl₃(THF)₃, E/Cr(acac)₃ and E/CrCl₂(THF)₂ were investigated. The best catalytic activity was achieved by 15.9 kg (product)/g (Cr)·h in which a selectivity of 63.6% for 1-C₈ was obtained.

Key words: chromium complexes, catalytic property, ethylene tri-/tetramerization, catalytic reaction conditions

引用此文

刘睿, 钟向宏, 刘振宇, 梁胜彪, 朱红平. N-四氢糠基PNP配体/铬催化体系及其乙烯选择性齐聚性能[J]. 有机化学, 2017, 37(9): 2315-2321.

Liu Rui, Zhong Xianghong, Liu Zhenyu, Liang Shengbiao, Zhu Hongping. Selective Ethylene Oligomerization Catalyzed by the Chromium Complex Bearing N-Tetrahydrofurfuryl PNP Ligand[J]. Chin. J. Org. Chem., 2017, 37(9): 2315-2321.

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N-四氢糠基PNP配体/铬催化体系及其乙烯选择性齐聚性能

Selective Ethylene Oligomerization Catalyzed by the Chromium Complex Bearing N-Tetrahydrofurfuryl PNP Ligand

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