2-(-鄰?fù)檠趸交?-咪唑配體的合成及催化乙烯聚合

摘要
本論文以水楊醛、聯(lián)苯甲酰、乙酸銨等原料合成了多取代咪唑類(lèi)配體。將所得多取代咪唑類(lèi)配體與四氯化鈦于甲苯中合成了相應(yīng)的咪唑鈦配合物。然后在助催化劑MAO作用下，以所得鈦的咪唑配合物為催化劑前體，催化乙烯聚合反應(yīng)。系統(tǒng)的考察了Al/Ti比(50-800)、聚合反應(yīng)溫度(7.5-55oC)、催化劑用量等因素對(duì)催化劑活性的影響。實(shí)驗(yàn)結(jié)果表明：催化活性隨著溫度的升高有明顯的增大，但繼續(xù)升高反應(yīng)溫度活性呈下降趨勢(shì)，在25℃是活性最高；催化劑的活性隨Al/Ti比的增大而增大。在選定的優(yōu)化條件下催化劑活性可達(dá)148.0 Kg-PE•mol-M 1•h-1。

關(guān)鍵詞:  多取代咪唑配體，多取代咪唑鈦配合物，乙烯聚合，甲基鋁氧烷(MAO)

ABSTRACT
Multi-substituted imidazole ligands were synthesized by using aromatic aldehyde, benzil, ammonium acetate as starting materials. Their corresponding titanium complexes were synthesized in toluene from the reaction of the imidazole ligands and titanium tetrachloride. In the present of methylaluminoxane(MAO) co-catalysts, the obtained imidazole titanium complexes were used as catalyst precursor, ethylene polymerization properties were systematically studied. Ethylene polymerization experiments were carried out with Al/Ti ratio ranged from 50 to 800, in the reaction temperature 7.5, 15, 25, 35, 45, 55oC. The results show that the activities of the catalysts increased with the increasing of Al/Ti ratio. With the polymerization temperature increasing, the catalysts activities firstly increased, and then decreased. The highest activity was observed at 25oC. An optimum activities 148.0 Kg-PE • mol-M 1 • h-1 was obtained at 25oC with Al/Ti at 800.

Key words:   multi-substituted imidazole ligands
imidazole complexes of titanium
ethylene polymerization
methylaluminoxane(MAO)

目錄
第1章 前言 1
§1.1 課題的提出及研究的目的、意義 1
§1.2 過(guò)渡金屬化合物催化烯烴聚合的研究概況 2
§1.3 咪唑配體的研究概況 5
第2章 實(shí)驗(yàn)部分 8
§2.1 原料和試劑 8
§2.2 咪唑配體及配合物的合成 8
§2.2.1醛原料及配體合成 9
§2.2.2 鈦配合物的合成 11
§2.3 助催化劑MAO的合成 11
§2.4 催化乙烯聚合 12
第3章 結(jié)果與討論 13
§3.1 催化劑的合成影響因素 13
§3.2 溫度對(duì)催化劑聚合活性的影響 13
§3.3 Al/Ti比對(duì)催化劑聚合活性的影響 14
第4章 結(jié)論 16
參考文獻(xiàn) 17
致    謝 21