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Selective Trimerization of α-Olefins with Triazacyclohexane Complexes of Chromium as Catalysts.
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Olefin oligomerization via metallacycles: dimerization, trimerization, tetramerization, and beyond.通过金属环进行的烯烃低聚反应：二聚、三聚、四聚及更高阶聚合。
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Influence of process parameters on the reaction kinetics of the chromium-catalyzed trimerization of ethylene.工艺参数对乙烯铬催化三聚反应动力学的影响。
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Ligand effects in chromium diphosphine catalysed olefin co-trimerisation and diene trimerisation.配体效应对铬双膦催化烯烃共三聚和二烯三聚的影响。
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PCNCP ligands in the chromium-catalyzed oligomerization of ethylene: tri- versus tetramerization.用于铬催化乙烯齐聚反应的PCNCP配体：三聚与四聚反应
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Mechanistic studies of olefin and alkyne trimerization with chromium catalysts: deuterium labeling and studies of regiochemistry using a model chromacyclopentane complex.铬催化剂催化烯烃和炔烃三聚反应的机理研究：氘标记及使用环铬戊烷配合物模型的区域化学研究
J Am Chem Soc. 2007 Nov 21;129(46):14281-95. doi: 10.1021/ja073493h. Epub 2007 Oct 31.
7
The selective trimerisation of isoprene with chromium N,N-bis(diarylphosphino)amine catalysts.异戊二烯与铬N,N-双（二芳基膦基）胺催化剂的选择性三聚反应。
Chem Commun (Camb). 2007 Jul 19(27):2835-7. doi: 10.1039/b702331f. Epub 2007 May 1.
8
Chromium-catalysed ethene trimerisation and tetramerisation--breaking the rules in olefin oligomerisation.铬催化乙烯三聚和四聚——打破烯烃齐聚规则
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9
An unprecedented alpha-olefin distribution arising from a homogeneous ethylene oligomerization catalyst.一种由均相乙烯齐聚催化剂产生的前所未有的α-烯烃分布。
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10
Highly selective chromium-based ethylene trimerisation catalysts with bulky diphosphinoamine ligands.具有庞大双膦基胺配体的高选择性铬基乙烯三聚催化剂。
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铬- PNP配合物催化乙烯与α-烯烃共聚的机理研究

Mechanistic Studies of Ethylene and α-Olefin Co-oligomerization Catalyzed by Chromium-PNP Complexes.

作者信息

Do Loi H, Labinger Jay A, Bercaw John E

机构信息

Arnold and Mabel Beckman Laboratories of Chemical Synthesis, California Institute of Technology, Pasadena, California 91125.

出版信息

Organometallics. 2012 Jul 23;31(14):5143-5149. doi: 10.1021/om300492r.

DOI:10.1021/om300492r
PMID:22904593
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC3418797/
Abstract

To explore the possibility of producing a narrow distribution of mid- to long-chain hydrocarbons from ethylene as a chemical feedstock, co-oligomerization of ethylene and linear α-olefins (LAOs) was investigated, using a previously reported chromium complex, [CrCl(3)(PNP(OMe))] (1, where PNP(OMe) = N,N-bis(bis(o-methoxyphenyl)phosphino)methylamine). Activation of 1 by treatment with modified methylaluminoxane (MMAO) in the presence of ethylene and 1-hexene afforded mostly C(6) and C(10) alkene products. The identities of the C(10) isomers, assigned by detailed gas chromatographic and mass spectrometric analyses, strongly support a mechanism that involves five- and seven-membered metallacyclic intermediates comprising of ethylene and LAO units. Using 1-heptene as a mechanistic probe, it was established that 1-hexene formation from ethylene is competitive with formation of ethylene/LAO co-trimers, and that co-trimers derived from one ethylene and two LAO molecules are also generated. Complex 1/MMAO is also capable of converting 1-hexene to C(12) dimers and C(18) trimers, albeit with poor efficiency. The mechanistic implications of these studies are discussed and compared to previous reports of olefin co-trimerization.

摘要

为了探索以乙烯作为化学原料生产窄分布的中长链烃的可能性，研究了乙烯与线性α-烯烃（LAOs）的共齐聚反应，使用先前报道的铬配合物[CrCl(3)(PNP(OMe))]（1，其中PNP(OMe)=N,N-双（双（邻甲氧基苯基）膦基）甲胺）。在乙烯和1-己烯存在下，用改性甲基铝氧烷（MMAO）处理1进行活化，主要得到C(6)和C(10)烯烃产物。通过详细的气相色谱和质谱分析确定的C(10)异构体的结构，有力地支持了一种涉及由乙烯和LAO单元组成的五元环和七元环金属环中间体的机理。使用1-庚烯作为机理探针，确定了乙烯生成1-己烯与乙烯/LAO共三聚体的生成相互竞争，并且还生成了由一个乙烯分子和两个LAO分子衍生的共三聚体。配合物1/MMAO也能够将1-己烯转化为C(12)二聚体和C(18)三聚体，尽管效率较低。讨论了这些研究的机理意义，并与先前烯烃共三聚反应的报道进行了比较。