Synthesis and applications of functionalized polyolefins using organometallic complexes = 유기금속 촉매를 이용한 기능성 폴리올레핀의 합성 및 응용에 관한 연구

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The copolymerization of ethylene with triphenylamine (TPA)-containing $\alpha$-olefin monomer 4-(7-Octen-1-yl)-N,N-diphenylaniline (\bf{1}) using a \emph{rac}-$Et(Ind)_2ZrCl_2$ (EBIZr)/MAO catalytic system was investigated to prepare polyethylene with pendent TPA groups. Despite the presence of a large excess of TPA moieties, the polymerization reactions efficiently produce copolymers of high-molecular-weight with the comonomer incorporation up to 6.1 mol % upon varying the comonomer concentration in the feed. Inspection of the aliphatic region of the $^{13}C$ NMR spectrum and the estimated copolymerization parameters ($\emph{r_1}\approx 0$ for 1 and $\emph{r_E}\approx43$ for ethylene) reveal the presence of isolated comonomer units in the polymer chain. While UV-vis absorption measurements of the copolymers show an invariant absorption feature, PL spectra exhibit a slightly red-shifted emission with increasing content of $\bf{1}$ in the polymer chain. All the copolymers show high thermal stability ($T_{d5} > 436^\circC$) and the electrochemical stability toward oxidation is also observed. Particularly the copolymer displays hole-transporting ability for the stable green emission of $Alq_{3}$ when incorporated into the hole-transporting layer of an electroluminescence device. Single-site group 4 metallocene catalytic systems have enabled us to produce polyolefins with the tailored polymer architecture in terms of molecular weight, functionalities, and degree of functionalization, which in turn may lead to intriguing properties. Particularly, polyolefins bearing triarylamine (TAA) functionality could be of great interest in display applications like OLEDs since they can possess hole-transporting properties. In this regard, we recently reported that polyethylene bearing triphenylamine group can act as hole-transporting layer materials in OLEDs. As part of our continuous contributions to this area, we have investigated the effects of catalyst structure and tria...
Do, Young-Kyuresearcher도영규researcher
한국과학기술원 : 화학과,
Issue Date
455478/325007  / 020075066

학위논문(박사) - 한국과학기술원 : 화학과, 2010.08, [ xv, 198 p. ]


triaryborane; triarylamine; functionalized polyolefin; organometallic complexes; polymerization; 중합; 트리아릴보레인; 트리아릴아민; 기능성 폴리올레핀; 유기금속촉매

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