From Stereochemically Tunable Homopolymers to Stereomultiblock Copolymers: Lewis Base Regulates Stereochemistry in the Coordination Polymerization of 2-Vinylpyridine,Macromolecules

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From Stereochemically Tunable Homopolymers to Stereomultiblock Copolymers: Lewis Base Regulates Stereochemistry in the Coordination Polymerization of 2-Vinylpyridine
Macromolecules ( IF 5.1 ) Pub Date : 2018-03-08 00:00:00 , DOI: 10.1021/acs.macromol.8b00125
Chao Yan ₁ , Tie-Qi Xu ₁ , Xiao-Bing Lu ₁

Affiliation

Excellent isoselectivity (mmmm > 99%) and high activity (TOF > 4000 h^–1) were achieved for the first time in the polymerization of the polar 2-vinylpyridine by using the simple lutetium-based catalysts, Lu(CH₂SiMe₃)₃(THF)_x(Py)_2–x (x = 0, 1, 2). The isoselectivity (mm) of the polymer could be varied between 37% and 99% through simply altering the quantity of Lewis base (tetrahydrofuran, 1,4-diazabicyclo[2.2.2]octane, 3-bromopyridine, and pyridine) added. Moreover, a novel method for preparing isotactic–atactic stereomultiblock poly(2-vinylpyridine)s was developed by the addition and removal of THF during polymerization. The polymerization process including stereoselective control mechanism was deduced by DFT calculations.

中文翻译：

从立体化学可调谐均聚物到立体多嵌段共聚物：Lewis碱调节2-乙烯基吡啶配位聚合中的立体化学

使用简单的-基催化剂Lu（CH ₂ SiMe ₃），在极性2-乙烯基吡啶的聚合反应中，首次获得了出色的等选择性（mmmm > 99％）和高活性（TOF> 4000 h ^–1）。₃（THF）_x（Py）_2–_x（x = 0，1，2）。等选择性（mm通过简单地改变所添加的路易斯碱（四氢呋喃，1，4-二氮杂双环[2.2.2]辛烷，3-溴吡啶和吡啶）的量，可以使聚合物的聚合物的％在37％至99％之间变化。此外，通过在聚合过程中添加和去除THF，开发了一种制备等规-无规立体多嵌段聚（2-乙烯基吡啶）的新方法。通过DFT计算推导了包括立体选择性控制机理的聚合过程。

更新日期：2018-03-08

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