Synthesis and characterization of amine-functionalized supported phosphine catalysts and their application in ethylene oligomerization

IF 0.8 4区化学 Q4 CHEMISTRY, MULTIDISCIPLINARY

South African Journal of Chemistry-Suid-Afrikaanse Tydskrif Vir Chemie Pub Date : 2022-01-01 DOI:10.17159/0379-4350/2022/v76a02

Mzamo L. Shozi, Xolelwa Zulu, H. Friedrich

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引用次数: 0

Abstract

ABSTRACT A series of phosphorus and nitrogen-based ethylene oligomerization ligands of the type Ph2PN(X)PPh2 where X = i-propyl, n-butyl, ethylbenzene and cyclohexyl substituents are reported. These ligands were functionalized to enable tethering on amino-silica. The free ligands, amino-silica and the tethered ligands were characterized by BET, XRD, IR, TGA and NMR. The catalysts were tested for ethylene oligomerization using Cr(acac)3 (acac = acetylacetonate) as the precursor and MMAO (modified methylaluminoxane) as the activator. The activity and selectivity of these catalysts to 1-octene was monitored at 45 bar ethylene in the temperature range of45-100 °C. The activity of the supported catalysts was comparable to their homogeneous counterparts, surpassing them in some cases and selectivities to 1-octene in the C8 products were as high as 99 wt%. The steric effect of the substituent on the ligand as well as that of the support was found to influence the activity and product distribution. Keywords: 1-hexene, 1-octene, ethylene oligomerization, phosphine ligands, silica, supported catalysts

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胺功能化负载膦催化剂的合成、表征及其在乙烯低聚反应中的应用

摘要报道了一系列磷基和氮基的Ph2PN(X)PPh2型乙烯低聚配体，其中X = i-丙基、正丁基、乙苯和环己基取代基。这些配体被功能化，使其能够在氨基二氧化硅上系固。通过BET、XRD、IR、TGA和NMR等手段对游离配体、氨基二氧化硅和系链配体进行了表征。以Cr(acac)3 (acac =乙酰丙酮酸)为前驱体，MMAO(改性甲基铝氧烷)为活化剂，对催化剂进行了乙烯低聚反应试验。在45 bar乙烯条件下，在45 ~ 100℃的温度范围内监测了这些催化剂对1-辛烯的活性和选择性。负载型催化剂的活性与均相催化剂相当，在某些情况下甚至超过了它们，C8产物对1-辛烯的选择性高达99%。取代基对配体和载体的空间效应影响了活性和产物的分布。关键词:1-己烯，1-辛烯，乙烯低聚，膦配体，二氧化硅，负载催化剂

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来源期刊

South African Journal of Chemistry-Suid-Afrikaanse Tydskrif Vir Chemie 化学-化学综合

CiteScore

3.10

自引率

0.00%

发文量

审稿时长

>12 weeks

期刊介绍： Original work in all branches of chemistry is published in the South African Journal of Chemistry. Contributions in English may take the form of papers, short communications, or critical reviews.