Borane-catalyzed hydrosilylation for polymer synthesis and heterogeneous catalysis = 붕소 촉매 기반의 수소규소화 반응을 이용한 고분자 합성과 불균일 촉매 반응 연구

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1. Metal-Free Hydrosilylation Polymerization by Borane Catalyst A novel polymerization strategy utilizing metal-free hydrosilylation of dienes with disilanes was developed by using $B(C_6F_5)_3$ catalyst to replace precious transition metal-based systems. The highly reactive $B(C_6F_5)_3$ catalyst enabled a step-growth polymerization with high degrees of polymerization under the easy-to-handle and mild conditions. Diverse polycarbosilanes with a broad range of structures and properties were obtained by various combinations of dienes and disilanes. 2. Borane-Catalyzed Hydrosilylative Post-Modification of Polymers We explored the $B(C_6F_5)_3$-catalyzed deoxygenation reaction of oxygen functionalized polymer. The olefin-containing block copolymer was prepared by deoxygenation reaction of the acrylate block copolymers synthesized by reversible addition-fragmentation chain transfer (RAFT) polymerization. This novel post-modification method provides a new way to prepare olefin copolymer with highly regulated structure and unprecedented combination which have not been synthesized by conventional olefin polymerization methods. 3. Heterogeneous B(C6F5)3 Catalyst for Hydrosilylative Reduction We developed borane-immobilized carbon nanotubes as the catalyst for hydrosilylative reduction. The heterogeneous borane catalysts are readily prepared via $\pi-\pi$ interactions between $B(C_6F_5)_3$ and the CNT surface. The substrate scope is broad to include carbonyls, acetals, and epoxides with excellent chemoselectivity under mild conditions. Preliminary kinetic studies reveal that the turnover frequency is highly sensitive on the steric bulkiness of both substrates and silanes rather than the electronic effects probably due to the sterically demanding environment surrounding the molecular borane anchored on the surface of carbon nanotubes.
Advisors
Chang, Sukbokresearcher장석복researcher
Description
한국과학기술원 :화학과,
Publisher
한국과학기술원
Issue Date
2017
Identifier
325007
Language
eng
Description

학위논문(박사) - 한국과학기술원 : 화학과, 2017.8,[iv, 73 p. :]

Keywords

borane catalyst▼ahydrosilylation▼apolycarbosilanes▼adeoxygenation▼apost-modification▼aheterogeneous borane catalyst▼acarbon nanotube▼a$\pi$-stacking interactions▼achemoselectivity▼apolyolefin▼aPS-b-PP-b-PS; 붕소 촉매▼a수소규소화반응▼a탄소규소 고분자▼a탈작용기화반응▼a고분자개질▼a불균일 붕소 촉매▼a비전이금속 촉매법▼a고분자 중합▼a폴리올레핀▼a폴리(스티렌-프로필렌-스티렌)▼a카본나노튜브▼a파이전자 상호작용▼a화학적 선택성

URI
http://hdl.handle.net/10203/265502
Link
http://library.kaist.ac.kr/search/detail/view.do?bibCtrlNo=866995&flag=dissertation
Appears in Collection
CH-Theses_Ph.D.(박사논문)
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