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首页> 外文期刊>Catalysis science & technology >Combining hydrogen bonding interactions with steric and electronic modifications for thermally robust alpha-diimine palladium catalysts toward ethylene (co)polymerization
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Combining hydrogen bonding interactions with steric and electronic modifications for thermally robust alpha-diimine palladium catalysts toward ethylene (co)polymerization

机译：氢键相互作用结合立体和电子热的修改健壮的alpha-diimine钯催化剂的方向乙烯聚合(有限公司)

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摘要

Development of thermally robust palladium-based catalysts for (co)polymerization of ethylene and polar monomers with high activities is a continuing challenge. Combining hydrogen bonding interactions with steric and electronic modifications, dibenzobarrelene-based alpha-diimine palladium complexes with different substituents (X = OMe, H, Cl, Br, and I) have been synthesized and characterized. The steric effect of the palladium complexes was elucidated by their buried volumes, and the electronic effect of the substituents was clarified by the Hammett constants (sigma) of the substituents and H-1 NMR analysis of the Pd-bound methyl. The hydrogen bonding interactions (H center dot center dot center dot Cl and H center dot center dot center dot OMe) were confirmed by single crystal structures of chloro- and methoxy-substituted neutral and cationic palladium complexes. Contributed by the steric and electronic effects as well as the hydrogen bonding, the chloro-substituted palladium catalyst was thermally robust at temperatures as high as 100 degrees C for ethylene polymerization, while the methoxy-substituted palladium catalyst showed excellent tolerance toward high temperature and polar groups and was able to copolymerize ethylene and methyl acrylate (MA) at 80 degrees C to produce the copolymer with high MA incorporation up to 9.5 mol%.
机译：热palladium-based强劲的发展(co)聚合的乙烯和催化剂是一个极性单体高的活动持续的挑战。与立体和电子的交互修改,dibenzobarrelene-basedalpha-diimine钯配合物具有不同取代基(X =, H, Cl, Br,和我)被合成和特点。影响钯配合物的阐明埋卷,和电子阐明了取代基的影响哈米特常量(σ)的取代基h - NMR分析Pd-bound甲基。氢键相互作用(H点中心中心导中心圆点Cl和H中心导中心导中心导性经单身氯和晶体结构methoxy-substituted中性和阳离子钯配合物。和电子效应以及氢键,chloro-substituted钯催化剂在温度作为热健壮高作为乙烯100摄氏度聚合,而methoxy-substituted钯催化剂表现出优秀的宽容对高温和极性基团能够使异分子聚合乙烯和丙烯酸甲酯在80摄氏度(MA)生产共聚物高马公司9.5 mol %。

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