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A Catalytic Hydrogel System Reinforced by Palladium Encapsulated Metal-Organic Framework for Suzuki-Miyaura Coupling Reaction : 스즈키-미야우라 반응을 위한 팔라듐이 도입된 금속-유기 구조체로 강화한 하이드로젤 촉매
DC Field | Value | Language |
---|---|---|
dc.contributor.advisor | 장지영 | - |
dc.contributor.author | 조성인 | - |
dc.date.accessioned | 2018-05-29T03:23:39Z | - |
dc.date.available | 2018-05-29T03:23:39Z | - |
dc.date.issued | 2018-02 | - |
dc.identifier.other | 000000149775 | - |
dc.identifier.uri | https://hdl.handle.net/10371/141470 | - |
dc.description | 학위논문 (석사)-- 서울대학교 대학원 : 공과대학 재료공학부, 2018. 2. 장지영. | - |
dc.description.abstract | 환경오염 문제가 점점 대두되면서 휘발성 유기용매의 사용을 감소시킬 수 있는 수용액에서의 화학반응이 주목을 받고 있다. 본 연구에서는 물을 용매로 하는 스즈키-미야우라 반응에 적합한 하이드로젤 촉매를 제조하였다. 팔라듐 나노입자를 도입한 금속-유기 구조체(MOF)를 개질한 후 하이드로젤 제조에 이용하여 기계적 특성과 촉매 활성이 우수한 촉매 시스템을 얻었다. MOF로는 2-aminoterephthalic acid와 zirconium(IV) chloride로부터 합성한 UiO-66-NH2를 이용하였다. 수소 기체를 이용하여 팔라듐 나노입자를 UiO-66-NH2 안에서 생성하고 비닐기를 UiO-66-NH2 에 도입하였다. 비닐기가 도입된 MOF와 아크릴아마이드의 라디칼 중합반응을 소량의 가교제 존재 하에 수행하여 하이드로젤 촉매를 제조하였다. 하이드로젤 촉매의 촉매 활성 및 재사용 가능성을 phenylboronic acid와 iodobenzene의 스즈키-미야우라 반응을 물-에탄올 용매에서 수행하여 조사하였다. | - |
dc.description.abstract | As environmental concerns increase, reactions in aqueous media are moving into the spotlight of synthetic chemistry where the usage of volatile organic solvents is reduced. We developed a catalytic hydrogel system for Suzuki-Miyaura coupling reaction in an aqueous medium. The hydrogel system contained palladium nanoparticle (PdNP) encapsulated metal-organic frameworks (MOFs) as catalytically active species and as reinforcement. The MOF (UiO-66-NH2) was prepared from 2-aminoterephthalic acid and zirconium(IV) chloride. High surface area, chemical modifiability, and numerous hydrogen bonding sites of UiO-66-NH2 made it a good candidate for catalytic cage, chemical crosslinker, and physical filler, respectively. PdNPs were encapsulated inside of UiO-66-NH2 by in situ hydrogen reduction and vinyl moieties for chemical crosslinking were introduced to UiO-66-NH2 by postsynthetic modification. Palladium content and vinyl modification ratio were 2.79 and 96.1 %, respectively. No damage on the crystal structure of UiO-66-NH2 was confirmed by nitrogen adsorption/desorption measurements and X-ray diffraction patterns. A catalytic hydrogel was prepared by free radical polymerization of acrylamide and the vinyl modified, PdNP encapsulated MOF in the presence of a small amount of a chemical cross-linker. The MOF reinforced hydrogel showed higher modulus and elongation by 105 and 25.8 %, respectively than the acrylamide hydrogel without the MOF. The catalytic activity and recyclability of the hydrogel were examined for the Suzuki-Miyaura coupling reaction of phenylboronic acid and iodobenzene. | - |
dc.description.tableofcontents | 1. Introduction 1
2. Experimental 11 2.1. Materials 11 2.2. Synthesis of UiO-66-NH2 11 2.3. Synthesis of Pd@UiO-66-NH2 12 2.4. Postsynthetic modification of Pd@UiO-66-NH2 13 2.5. Fabrication of catalytic hydrogel system 13 2.6. Suzuki-Miyaura coupling reaction 14 2.7. Characterization 14 2.7.1. Nuclear magnetic resonance spectroscopy 14 2.7.2. N2 adsorption/desorption measurements 15 2.7.3. X-ray diffraction measurements 15 2.7.4. Scanning electron microscopy 15 2.7.5. Transmission electron microscopy 16 2.7.6. Tensile test 16 3. Result and Discussion 17 3.1. Synthesis of UiO-66-NH2 and Pd@UiO-66-NH2 17 3.2. Characterization of the MOF 21 3.3. Postsynthetic modification of the MOF 27 3.4. Fabrication of the catalytic hydrogel system 31 3.5. Suzuki-Miyaura coupling reaction 36 4. Conclusion 40 5. References 41 | - |
dc.format | application/pdf | - |
dc.format.extent | 2540621 bytes | - |
dc.format.medium | application/pdf | - |
dc.language.iso | en | - |
dc.publisher | 서울대학교 대학원 | - |
dc.subject | hydrogel catalyst | - |
dc.subject | heterogeneous catalyst | - |
dc.subject | palladium nanoparticles metal-organic framework | - |
dc.subject | Suzuki-Miyaura reaction | - |
dc.subject | aqueous reaction | - |
dc.subject.ddc | 620.1 | - |
dc.title | A Catalytic Hydrogel System Reinforced by Palladium Encapsulated Metal-Organic Framework for Suzuki-Miyaura Coupling Reaction | - |
dc.title.alternative | 스즈키-미야우라 반응을 위한 팔라듐이 도입된 금속-유기 구조체로 강화한 하이드로젤 촉매 | - |
dc.type | Thesis | - |
dc.contributor.AlternativeAuthor | Seongin Jo | - |
dc.description.degree | Master | - |
dc.contributor.affiliation | 공과대학 재료공학부 | - |
dc.date.awarded | 2018-02 | - |
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