可再生的 3-亚甲基环戊烯与稀土金属前体的配位聚合。
Coordination Polymerization of Renewable 3-Methylenecyclopentene with Rare-Earth-Metal Precursors.
机构信息
State Key Laboratory of Polymer Physics and Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022, China.
Key Laboratory of Automobile Materials of Ministry of Education, Department of Materials Science and Engineering, Jilin University, Changchun, 130025, China.
出版信息
Angew Chem Int Ed Engl. 2017 Apr 10;56(16):4560-4564. doi: 10.1002/anie.201700546. Epub 2017 Mar 22.
Coordination polymerization of renewable 3-methylenecyclopentene has been investigated for the first time using rare-earth metal-based precursors bearing various bulky ligands. All the prepared complexes catalyze controllable polymerization of 3-methylenecyclopentene into high molecular weight polymers, of which the NPN- and NSN-tridentate non-Cp ligated lutetium-based catalytic systems exhibited extremely high activities up to 11 520 kg/(mol ⋅h) in a dilute toluene solution (3.2 g/100 mL) at room temperature. The resultant polymers have pure 1,4-regioregularity (>99 %) and tailorable number average molecular weights (1-20×10 ) with narrow molecular weight distributions (polydispersity index (PDI)=1.45-1.79). DFT simulations were employed to study the polymerization mechanism and stereoregularity control.
首次使用带有各种大位阻配体的稀土金属前体制备了可再生的 3-亚甲基环戊烯的配位聚合。所有制备的配合物都可以催化 3-亚甲基环戊烯的可控聚合，得到高分子量聚合物，其中 NPN 和 NSN 三齿非 Cp 配体镥基催化体系在室温下在稀甲苯溶液（3.2 g/100 mL）中表现出极高的活性，高达 11520 kg/（mol ⋅h）。所得聚合物具有纯 1,4-规则性（>99%）和可调节的数均分子量（1-20×10），分子量分布较窄（多分散指数（PDI）=1.45-1.79）。采用 DFT 模拟研究了聚合机理和立构规整性控制。
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