边臂策略在聚烯烃催化剂设计中的应用

孙秀丽; 唐勇

doi:10.11777/j.issn1000-3304.2017.17033

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边臂策略在聚烯烃催化剂设计中的应用

专论 | 更新时间：2021-01-26

- 边臂策略在聚烯烃催化剂设计中的应用
- Sidearm Approach to the Synthesis of Catalysts Used in Olefin Polymerization
- 高分子学报 2017年第7期页码：1019-1037
- 作者机构：
  
  中国科学院上海有机化学研究所上海 200032
- 作者简介：
  
  [ "唐勇, 男, 1964年9月生.博士, 中国科学院上海有机化学研究所研究员.1986年于四川师范大学获得学士学位, 1993年于中国科学院上海有机化学研究所获得硕士学位, 1996年于中国科学院上海有机化学研究所获得博士学位.主要从事有机合成与高分子化学中的选择性控制与催化的基本问题研究, 特别是不对称催化和烯烃催化剂的设计、合成及烯烃可控性聚合.2002年获国家杰出青年科学基金, 2012年获国家自然科学二等奖(第一完成人), 2015年增选为中国科学院院士" ]
- 基金信息：
  
  国家重点研发计划(项目号2016YFA0202900);国家自然科学基金(基金号21421091);中国科学院战略性先导科技专项（B类）(项目号XDB20000000)
- DOI：10.11777/j.issn1000-3304.2017.17033
  中图分类号：
- 纸质出版日期：2017-7，
  
  收稿日期：2017-2-28，
  
  修回日期：2017-3-26，
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孙秀丽, 唐勇. 边臂策略在聚烯烃催化剂设计中的应用[J]. 高分子学报, 2017,(7):1019-1037.

Sun Xiu-li, Tang Yong. Sidearm Approach to the Synthesis of Catalysts Used in Olefin Polymerization[J]. Acta Polymerica Sinica, 2017,(7):1019-1037.
孙秀丽, 唐勇. 边臂策略在聚烯烃催化剂设计中的应用[J]. 高分子学报, 2017,(7):1019-1037. DOI： 10.11777/j.issn1000-3304.2017.17033.

Sun Xiu-li, Tang Yong. Sidearm Approach to the Synthesis of Catalysts Used in Olefin Polymerization[J]. Acta Polymerica Sinica, 2017,(7):1019-1037. DOI： 10.11777/j.issn1000-3304.2017.17033.

摘要

提出用“边臂”策略设计和改造烯烃聚合催化剂，以钛、镍等配合物为模型，系统研究了边臂基团对配合物的配位模式、配合物的稳定性，对乙烯均聚活性以及乙烯与

-烯烃、环烯烃以及极性单体共聚合的活性和对聚烯烃的结构与性能的影响.研究结果表明通过边臂基团可以调节催化中心的空间形状和电子特性，实现对催化物种性质的控制与调节，调控烯烃聚合活性和聚烯烃的结构与性能.

Abstract

Catalyst design for single-site olefin polymerization is of great scientific and industrial importance

and has attracted much attention since the pioneering work of Ziegle-Natta. "Sidearm strategy" developed in the last decades has been used successfully for designing homogenous catalyst. By which

a "sidearm" group is introduced to a basic unit

and the performance of the active center could be improved readily by modulate its shape and/or the electronic properties. This review article discloses the application of sidearm strategy in olefin polymerization catalyst design. Modification of a simple bidentate salicylaldeminate by a coordination group (OR

SeR

PPh

) induced the coordination pattern variation. Of the newly-designed salicylaldiminato titanium trichlorides

both steric and electronic properties of the active species were proved to be readily tunable. Sidearm effect was obviously seen. For example

hard and small oxygen as a donor atom in sidearm induced moderate catalytic activity (10

gPE/mol(Ti)·h·atm) when it was used to polymerize ethylene in the presence of MMAO

whereas the complexes with soft and large S

and P atoms as donor atom showed much higher activity (10

gPE/mol(Ti)·h·atm). The sidearm effect on thermostability of the complexes was also observed. In addition

the capability of catalyzing ethylene/comonomers (

-olefin

cycloolefin) copolymerization was also sidearm dependent. Both the activity and the incorporation of a comonomer could be improved by replacing the sidearm from bulky-S

Pr to-S

Pr. The newly designed titanium trichloride complexes was proved to have good polar group tolerance. Consequently

-alkenol

-alkenoic acid

and

-alkenoic ester

etc

. could be incorporated into PE backbone efficiently. By this way

PPh

-and AsPh

-were zipped on polyethylene efficiently

which was proved to be efficient in catalytic[3 + 2] cycloaddition and Wittig reaction

separately. This is a simple way for the preparation of readily recovered and reused PE-supported organocatalyst. The strategy was also extended to the modification of SHOP-type catalysts

and nickel complexes bearing an alkyloxyl group as a sidearm were synthesized. The distance between Ni and O(R) is shorter than the sum of van der Waals radii of Ni and O (2.985 Å versus 3.15 Å)

indicating a weak interaction between O(R) and Ni atoms. Further studies showed that the introduction of alkoxyl group improved the activity and thermostability. Based on the optimized metal complex

heterogeneous titanium catalyst was developed and used in production of ultra-high molecular weight polyethylene (UHMWPE)

which is highly linear and readily processible.

关键词

边臂策略金属配合物聚烯烃催化剂乙烯聚合极性单体

Keywords

Sidearm strategyMetal complexesPolyolefin catalystEthylene polymerizationPolar comonomers

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