Heterobimetallic Lewis Acid Catalyst Development for Polyesterification and Depolymerization
Heterobimetallic Lewis Acid Catalyst Development for Polyesterification and Depolymerization
상세정보
- 자료유형
- 학위논문 서양
- 최종처리일시
- 20250211152817
- ISBN
- 9798384011873
- DDC
- 540
- 저자명
- Jansen, Jacob H.
- 서명/저자
- Heterobimetallic Lewis Acid Catalyst Development for Polyesterification and Depolymerization
- 발행사항
- [Sl] : The University of Wisconsin - Madison, 2024
- 발행사항
- Ann Arbor : ProQuest Dissertations & Theses, 2024
- 형태사항
- 146 p
- 주기사항
- Source: Dissertations Abstracts International, Volume: 86-02, Section: B.
- 주기사항
- Advisor: Hermans, Ive.
- 학위논문주기
- Thesis (Ph.D.)--The University of Wisconsin - Madison, 2024.
- 초록/해제
- 요약Polyesters made through the use of a homogeneous catalyst are integral to many areas of life and the chemical or materials industries. Titanate catalysts such as titanium tetrabutoxide (TBT) have long been known to be effective polyesterification catalysts. However, their use on an industrial scale has been hindered by their sensitivity to moisture. Previously, this challenge has been addressed by using mixtures of titanate catalysts with tin-based catalysts such as stannous octoate (SnOct), showing a synergistic effect for hydrolytic stability. The structure of this mixed metal catalyst has been defined for the first time since its discovery as a heterobimetallic dimer using a suite of nuclear magnetic spectroscopy (NMR) techniques and mass spectrometry. Unfortunately, due to toxicity concerns around tin catalysts, this efficient catalyst mixture is not a long-term viable solution. To address this issue, a mixed metal catalyst of TBT and bismuth neodecanoate (BiNeo) is first reported on and possesses little toxicity concerns while have as good of or better stability or reactivity as mixtures of titanium and tin. A key set of discoveries allowed for the understanding that mixed metal catalysts possess greater stability but not necessarily greater activity.The mixed metal catalysts were studied for the strength of their Lewis acidity and for any interactions arising from proximal metal centers. A series of different measurements of the effective Lewis acidity gave varied results but agreed with respect to the metals being generally isolated active sites for reactant binding. Finally, the novel mixed metal Lewis acid catalysts were tested in the glycolysis of polyethylene terephthalate waste plastic. The mixed metal catalysts outperformed the unmixed precursors but did not outperform an industrial catalyst under most reaction conditions.
- 일반주제명
- Chemistry
- 일반주제명
- Inorganic chemistry
- 일반주제명
- Organic chemistry
- 키워드
- Depolymerization
- 기타저자
- The University of Wisconsin - Madison Chemistry
- 기본자료저록
- Dissertations Abstracts International. 86-02B.
- 전자적 위치 및 접속
- 로그인 후 원문을 볼 수 있습니다.
MARC
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■040 ▼aMiAaPQ▼cMiAaPQ
■0820 ▼a540
■1001 ▼aJansen, Jacob H.
■24510▼aHeterobimetallic Lewis Acid Catalyst Development for Polyesterification and Depolymerization
■260 ▼a[Sl]▼bThe University of Wisconsin - Madison▼c2024
■260 1▼aAnn Arbor▼bProQuest Dissertations & Theses▼c2024
■300 ▼a146 p
■500 ▼aSource: Dissertations Abstracts International, Volume: 86-02, Section: B.
■500 ▼aAdvisor: Hermans, Ive.
■5021 ▼aThesis (Ph.D.)--The University of Wisconsin - Madison, 2024.
■520 ▼aPolyesters made through the use of a homogeneous catalyst are integral to many areas of life and the chemical or materials industries. Titanate catalysts such as titanium tetrabutoxide (TBT) have long been known to be effective polyesterification catalysts. However, their use on an industrial scale has been hindered by their sensitivity to moisture. Previously, this challenge has been addressed by using mixtures of titanate catalysts with tin-based catalysts such as stannous octoate (SnOct), showing a synergistic effect for hydrolytic stability. The structure of this mixed metal catalyst has been defined for the first time since its discovery as a heterobimetallic dimer using a suite of nuclear magnetic spectroscopy (NMR) techniques and mass spectrometry. Unfortunately, due to toxicity concerns around tin catalysts, this efficient catalyst mixture is not a long-term viable solution. To address this issue, a mixed metal catalyst of TBT and bismuth neodecanoate (BiNeo) is first reported on and possesses little toxicity concerns while have as good of or better stability or reactivity as mixtures of titanium and tin. A key set of discoveries allowed for the understanding that mixed metal catalysts possess greater stability but not necessarily greater activity.The mixed metal catalysts were studied for the strength of their Lewis acidity and for any interactions arising from proximal metal centers. A series of different measurements of the effective Lewis acidity gave varied results but agreed with respect to the metals being generally isolated active sites for reactant binding. Finally, the novel mixed metal Lewis acid catalysts were tested in the glycolysis of polyethylene terephthalate waste plastic. The mixed metal catalysts outperformed the unmixed precursors but did not outperform an industrial catalyst under most reaction conditions.
■590 ▼aSchool code: 0262.
■650 4▼aChemistry
■650 4▼aInorganic chemistry
■650 4▼aOrganic chemistry
■653 ▼aHeterobimetallic Lewis Acid
■653 ▼aCatalyst Development
■653 ▼aPolyesterification
■653 ▼aDepolymerization
■690 ▼a0485
■690 ▼a0488
■690 ▼a0490
■71020▼aThe University of Wisconsin - Madison▼bChemistry.
■7730 ▼tDissertations Abstracts International▼g86-02B.
■790 ▼a0262
■791 ▼aPh.D.
■792 ▼a2024
■793 ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17163985▼nKERIS▼z이 자료의 원문은 한국교육학술정보원에서 제공합니다.
