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Live hard die young: Insight into the short life time of highly active vanadium(III) catalysts. The James Dean of alpha-olefin polymerization catalysts.

机译：活得早死：洞悉高活性钒（III）催化剂的使用寿命短。 α-烯烃聚合催化剂的James Dean。

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The effects of different donor atoms of the supporting ligands (i.e. oxygen and nitrogen donor ligands) are at the root of this study as well as an attempt to improve our understanding of the catalyst/co-catalyst interaction.; Simply based on the lack of knowledge in the area of vanadium polymerization mechanism our group has set out to investigate possible activation pathways through a series of alkylation reactions to assess the vanadium-carbon bond stability by using a variety of oxygen and nitrogen donor-based supporting ligands. Upon using alkylating agents such as the alkylaluminium co-catalysts, attempts to trap and crystallize the active intermediate were attempted only to elucidate the deactivation process.; Insight into the activation and deactivation pathways of vanadium-based catalysts and a few other metal congeners such as zirconium, chromium, and manganese will be investigated in the following thesis.; The second chapter will cover insight into the activation and deactivation pathways of the industrially used tris(acetylacetonato) vanadium complex in the copolymerization of ethylene and propylene forming a polymer used in the production of synthetic rubber.; In attempt to combine the migratory properties of the oxygen donor based ligands and the stabilization properties nitrogen donor based ligands, the reactivity of the acetylpyrrolide ligand system was investigated with V(III). Two novel organometallic complexes were synthesized where, in one case, vanadium(III) mediated an aldolic condensation of the acetylpyrrolide ligand and in a second case a vanadium(II) metal centre promoted a pinacolic coupling of the ligand (Chapter 5).; Chapter 6 in mainly focused on the vanadium/aluminium interaction and the role of the co-catalyst in the activation and deactivation of the vanadium metal centre. In this case the vanadium centre is supported by the bulky N,N,N, tris-trimethylsilyl diethylenediamidoamino ligand. Formation of novel vanadium/aluminium clusters were synthesized and have given great insight into the vanadium/aluminium interaction and have demonstrated involvement of the ligand as seen previously in the case of the bis(imino)pyridyl ligand system.; Preliminary reactivity of the meso-diphenyldipyrrolemethane ligand was investigated with Zr(IV), V(III), Cr(III), Cr(II) in Chapter 7. These reactions revealed the possible bonding modes of the pyrrolide moiety with the metal centre. Treatment of the V(III) meso-diphenyldipyrrolidemethane complex with a sterically demanding aryloxide led to an interesting deoxygenation reaction of the aryloxide to form an oxygen bridged vanadium dimer which exerted high polymerization activities upon activation with dimethylaluminiumchloride. (Abstract shortened by UMI.)

机译：支持配体的不同供体原子（即氧和氮供体配体）的影响是这项研究的根本，也是试图提高我们对催化剂/助催化剂相互作用的理解的尝试。仅仅基于对钒聚合机理领域知识的缺乏，我们小组着手通过一系列烷基化反应来研究可能的活化途径，从而通过使用多种基于氧和氮供体的支持物来评估钒-碳键的稳定性。配体。在使用烷基化剂如烷基铝助催化剂时，试图捕获和结晶活性中间体只是为了阐明失活过程。在接下来的论文中，将深入研究钒基催化剂和一些其他金属同类物（例如锆，铬和锰）的活化和失活途径。第二章将介绍在乙烯和丙烯共聚形成合成橡胶生产中使用的聚合物时，工业上使用的三（乙酰丙酮基）钒配合物的活化和失活途径。为了结合基于氧供体的配体的迁移特性和基于氮供体的配体的稳定特性，用V（III）研究了乙酰基吡咯化物配体体系的反应性。合成了两种新颖的有机金属配合物，在一种情况下，钒（III）介导了乙酰基吡咯化物配体的醛缩合，在第二种情况下，钒（II）的金属中心促进了配体的品醇偶联（第5章）。第6章主要集中在钒/铝的相互作用以及助催化剂在钒金属中心的活化和失活中的作用。在这种情况下，钒中心由庞大的N，N，N， tris -三甲基甲硅烷基二亚乙基二氨基氨基配体支撑。合成了新颖的钒/铝簇，并且对钒/铝的相互作用有了深入的了解，并证明了如先前在双（亚氨基）吡啶基配体系统中所见，该配体的参与。在第7章中用Zr（IV），V（III），Cr（III），Cr（II）研究了 meso -二苯基二吡咯甲烷配体的初步反应性。这些反应揭示了可能的键合方式吡咯部分与金属中心。用空间上需要的芳基氧化物处理V（III）的<斜体>间苯二胺-二苯基二吡咯烷甲烷配合物导致了该芳基氧化物的有趣的脱氧反应，形成了氧桥连的钒二聚体，该二聚体在被二甲基氯化铝活化后发挥了很高的聚合活性。（摘要由UMI缩短。）

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作者
Reardon, Damien Francis.;
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作者单位

University of Ottawa (Canada).;

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授予单位 University of Ottawa (Canada).;
学科 Chemistry Polymer.
学位 Ph.D.
年度 2002
页码 246 p.
总页数 246
原文格式 PDF
正文语种 eng
中图分类高分子化学（高聚物）;
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Live hard die young: Insight into the short life time of highly active vanadium(III) catalysts. The James Dean of alpha-olefin polymerization catalysts.

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