Synthesis of new homogeneous olefin polymerization catalysts신규 올레핀 중합용 균일계 촉매에 관한 연구

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dc.contributor.advisorDo, Young-Kyu-
dc.contributor.advisor도영규-
dc.contributor.authorHan, Yong-Gyu-
dc.contributor.author한용규-
dc.date.accessioned2011-12-13T04:30:08Z-
dc.date.available2011-12-13T04:30:08Z-
dc.date.issued2004-
dc.identifier.urihttp://library.kaist.ac.kr/search/detail/view.do?bibCtrlNo=240585&flag=dissertation-
dc.identifier.urihttp://hdl.handle.net/10203/31634-
dc.description학위논문(박사) - 한국과학기술원 : 화학과, 2004.8, [ ix, 146 p. ]-
dc.description.abstractNine thermally stable complexes $(η^5-Cp^*)[η^5-(C_5H_4)CMe_2CB_{10}H_{10}CR]MCl_2$ (R = H; a and Me; b) (M = Ti; 1, Zr; 2 and Hf; 3) and $(η^5-Cp^*)[η^5; η^1-(C_5H_4)CMe_2(CB_{10}H_{10}C)]MCl$ (M = Ti; 4, Zr; 5 and Hf; 6) have been prepared via metathesis reactions of $Cp^*MCl_3 (M = Ti, Zr and Hf, Cp^* = pentamethylcyclopentadienyl)$ with monolithium salts of $(C_5H_5)CMe_2(CB_{10}H_{10}CR)$ (R = H; a and Me; b) and with dilithium salt of $(C_5H_5)CMe_2(CB_{10}H_{10}CH)$, respectively. These compounds have been fully characterized by various spectroscopic methods and elemental analyses. All of the compounds except $(η^5-Cp^*)[η^5-(C_5H_4)CMe_2CB_{10}H_{10}CMe]HfCl_2$ were additionally characterized by a single crystal X-ray diffraction study, establishing their monomeric bent metallocene structural feature with carborane acting as a substituent or an ancillary ligand. The titanium and zirconium complexes produce high-density polyethylenes with the activity range of about $10^3-10^4$ g PE/(mol of M?bar?h) in the presence of MMAO cocatalyst. Reactions of the dilithium salt of aminosilylene-bridged ligands with $(Me_2N)_2ZrCl_2(THF)_2$ followed by the treatment of TMSCl are found to be the efficient method to synthesize aminosilylene-bridged ansa-zirconocenes, $R_2N(Me)Si(η^5-C_5H_4)_2ZrCl_2$ (R = Me (1), Et (2)), $R_2N(Me)Si(η^5-C_5H_4)(η^5-C_5Me_4)ZrCl_2$ (X = Me (3), Et (4)). These complexes were completely characterized and the complex 3 was also characterized by X-ray crystallography. The complex 3 and its prototype complex, $Me_2Si(η^5-C_5H_4)(η^5-C_5Me_4)ZrCl_2$ (9) have very similar steric environment around the metal center comparing their geometrical parameters. Even the similar steric environment, the aminosilylene-brigded ansa-zirconocenes generate branched polyethylenes with broad molecular weight distribution caused by the interaction the amine groups introduced and methylalumoxane (MAO) in ethylene homopolymerization. The branched polyethylene can...eng
dc.languageeng-
dc.publisher한국과학기술원-
dc.subject산-염기 상호작용-
dc.subject오르토카보레인-
dc.subject분자량 분포-
dc.subject폴리에틸렌-
dc.subject이종원소-
dc.subject메탈로센-
dc.subject폴리스티렌-
dc.subjectPOLYSTYRENE-
dc.subjectACID-BASE INTERACTION-
dc.subjectORTHOCARBORANE-
dc.subjectMOLECULAR WEIGHT DISTRIBUTION-
dc.subjectPOLYETHYLENE-
dc.subjectHETEROATOM-
dc.subjectMETALLOCENE-
dc.titleSynthesis of new homogeneous olefin polymerization catalysts-
dc.title.alternative신규 올레핀 중합용 균일계 촉매에 관한 연구-
dc.typeThesis(Ph.D)-
dc.identifier.CNRN240585/325007 -
dc.description.department한국과학기술원 : 화학과, -
dc.identifier.uid000995831-
dc.contributor.localauthorDo, Young-Kyu-
dc.contributor.localauthor도영규-
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