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硅甲基和硅乙基对位取代基对酚盐改性半茂钛催化乙烯共聚反应中高活性及羟基引入的影响

The Effect of SiMe and SiEt Para Substituents for High Activity and Introduction of a Hydroxy Group in Ethylene Copolymerization Catalyzed by Phenoxide-Modified Half-Titanocenes.

作者信息

Kitphaitun Suphitchaya, Yan Qing, Nomura Kotohiro

机构信息

Department of Chemistry, Graduate School of Science, Tokyo Metropolitan University, 1-1 Minami Osawa, Hachioji, Tokyo, 192-0376, Japan.

出版信息

Angew Chem Int Ed Engl. 2020 Dec 14;59(51):23072-23076. doi: 10.1002/anie.202010559. Epub 2020 Oct 7.

DOI:10.1002/anie.202010559
PMID:32886419
Abstract

Remarkable effects of SiMe and SiEt para-substituents in the phenoxide-modified half-titanocenes, Cp*TiCl (O-2,6- Pr -4-R-C H ) [R=SiMe (6), SiEt (7)], toward the catalytic activities in ethylene copolymerizations with 2-methyl-1-pentene, 1-decene, 1-dodecene and with 9-decen-1-ol (DC-OH) have been demonstrated. The activities by 6, 7 at 50 °C showed higher than those conducted at 25 °C in all cases in the presence of MAO cocatalyst. Efficient synthesis of high-molecular-weight (HMW) ethylene copolymers incorporating DC-OH (or 5-hexen-1-ol, HX-OH) has been attained in the copolymerization by 7, which showed better DC-OH (HX-OH) incorporation at 50 °C to afford the HMW copolymers, poly(ethylene-co-DC-OH)s, with high activities (activity 1.21-3.81×10  kg-polymer mol -Ti h, M =6.55-10.0×10 , DC-OH 2.3-3.6 mol %).

摘要

已证明，在苯氧基修饰的半钛茂化合物Cp*TiCl(O-2,6-Pr-4-R-C6H) [R = SiMe (6)，SiEt (7)]中，SiMe和SiEt对位取代基对与2-甲基-1-戊烯、1-癸烯、1-十二碳烯以及与9-癸烯-1-醇(DC-OH)进行乙烯共聚反应的催化活性具有显著影响。在MAO助催化剂存在下，6和7在50°C时的活性在所有情况下均高于25°C时的活性。通过7进行的共聚反应实现了高效合成包含DC-OH(或5-己烯-1-醇，HX-OH)的高分子量(HMW)乙烯共聚物，其在50°C时表现出更好的DC-OH(HX-OH)掺入率，从而以高活性(活性为1.21 - 3.81×10³ kg-聚合物·mol⁻¹-Ti·h，M = 6.55 - 10.0×10⁴，DC-OH 2.3 - 3.6 mol%)得到HMW共聚物聚(乙烯-co-DC-OH)s。

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