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Investigations of ligand backbone effects on bulky diarylmethyl-based nickel(II) and palladium(II) catalyzed ethylene polymerization and copolymerization
Journal of Organometallic Chemistry ( IF 2.1 ) Pub Date : 2021-08-21 , DOI: 10.1016/j.jorganchem.2021.122046
Lihua Guo 1 , Xueyan Hu 1 , Weiqing Lu 2 , Guoyong Xu 2 , Qin Liu 1 , Shengyu Dai 2
Affiliation  

Recently, the sterically hindered ortho-dibenzhydryl or diarylmethyl-derived (CHPh2 or CHAr2 on the N-aryl ring) α-diimine nickel(II) and palladium(II) catalysts have received much attention due to their unique catalytic properties for olefin (co)polymerization. In this work, the synthesis and characterization of bulky diarylmethyl-derived Ni(II) and Pd(II) ethylene (co)polymerization catalysts containing a series of backbone substituents (H, CH3 and acenaphthene) were described. Substituent effect of the backbone on catalyst activity and stability, polymer molecular weight, polymer branching density and polar monomer incorporation were investigated in detail. Overall, acenaphthene-based Ni3 showed the highest catalytic activity and produced the polymer with the highest molecular weight in Ni(II) system, while CH3-based Pd2 showed the best catalytic property in Pd(II) system. The H-substituted Ni(II) and Pd(II) catalyst was notable in its low activity or no activity compared to the other substituted Ni(II) and Pd(II) catalyst. Most interestingly, Pd2 demonstrated highest polymerization activities under gas-phase conditions through the self-supported catalytic mechanism.



中文翻译:

研究配体骨架对庞大的二芳基甲基镍(II)和钯(II)催化乙烯聚合和共聚的影响

近来,位阻二苯甲基或二芳基甲基衍生的(N-芳环上的CHPh 2或CHAR 2)α-二亚胺镍(II)和钯(II)催化剂因其对烯烃的独特催化性能而备受关注。 (共)聚合。在这项工作中,描述了含有一系列骨架取代基(H、CH 3和苊)的庞大的二芳基甲基衍生的 Ni(II) 和 Pd(II) 乙烯(共)聚合催化剂的合成和表征。详细研究了主链的取代基对催化剂活性和稳定性、聚合物分子量、聚合物支化密度和极性单体掺入的影响。总的来说,苊基Ni3在Ni(II)体系中表现出最高的催化活性并产生了最高分子量的聚合物,而CH 3Pd2在Pd(II)体系中表现出最好的催化性能。与其他取代的 Ni(II) 和 Pd(II) 催化剂相比,H 取代的 Ni(II) 和 Pd(II) 催化剂的显着特点是其低活性或无活性。最有趣的是,Pd2通过自支撑催化机制在气相条件下表现出最高的聚合活性。

更新日期:2021-08-29
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