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Development of Artificial Metalloenzymes for Application in Synthetic Chemistry
Development of Artificial Metalloenzymes for Application in Synthetic Chemistry
상세정보
- 자료유형
- 학위논문 서양
- 최종처리일시
- 20260202105112
- ISBN
- 9798297601635
- DDC
- 547
- 서명/저자
- Development of Artificial Metalloenzymes for Application in Synthetic Chemistry
- 발행사항
- [Sl] : University of California, Berkeley, 2025
- 발행사항
- Ann Arbor : ProQuest Dissertations & Theses, 2025
- 형태사항
- 192 p
- 주기사항
- Source: Dissertations Abstracts International, Volume: 87-04, Section: B.
- 주기사항
- Advisor: Hartwig, John F.
- 학위논문주기
- Thesis (Ph.D.)--University of California, Berkeley, 2025.
- 초록/해제
- 요약The following dissertation discusses the development and emerging applications of computationally designed enzymes for catalysis and the development of a ruthenium complex for selective and mild aliphatic C(sp3)-H bond oxidation.Chapter 1 provides an overview of reactions catalyzed by metalloenzymes with a focus on new-to-nature reactions. This section highlights the growing potential of biocatalysis through contemporary and historical examples of industrial biocatalytic processes. Methods for the generation of artificial metalloenzymes and examples of functional de novo designed metalloenzymes are discussed.Chapter 2 focuses on the development of a de novo designed protein for C-H bond oxidation. The application of some of the most common natural oxidases is challenging because of complicated reaction mechanisms, the need for partner enzymes or proteins, and limited stability of relevant enzymes under the reaction conditions. This chapter demonstrates the potential benefits of combining synthetic small molecule catalysts with hyper-stable protein hosts. The combination of these two systems enables their characterization in parallel and therefore, more rapid characterization of the system.Chapter 3 describes the development of a small molecule catalyst for C-H bond oxidation. Many of the reported metal complexes that catalyze undirected C-H bond oxidation suffer from limited stability under the reaction conditions. This section discusses the generation, characterization, and reactivity of a ruthenium complex with a tetradentate pyridine-based ligand. The ruthenium complex is shown to catalyze the oxidation of unactivated tertiary C-H bonds with high turnover numbers, at low substrate concentration, and after prolonged exposure to the terminal oxidant.
- 일반주제명
- Organic chemistry
- 일반주제명
- Chemistry
- 일반주제명
- Analytical chemistry
- 키워드
- Aqueous
- 키워드
- Biocatalysis
- 키워드
- Oxidation
- 기타저자
- University of California, Berkeley Chemistry
- 기본자료저록
- Dissertations Abstracts International. 87-04B.
- 전자적 위치 및 접속
- 로그인 후 원문을 볼 수 있습니다.
MARC
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■006m o d
■007cr#unu||||||||
■020 ▼a9798297601635
■035 ▼a(MiAaPQ)AAI32237079
■040 ▼aMiAaPQ▼cMiAaPQ
■0820 ▼a547
■1001 ▼aJoyner, Isaac August DeLong.
■24510▼aDevelopment of Artificial Metalloenzymes for Application in Synthetic Chemistry
■260 ▼a[Sl]▼bUniversity of California, Berkeley▼c2025
■260 1▼aAnn Arbor▼bProQuest Dissertations & Theses▼c2025
■300 ▼a192 p
■500 ▼aSource: Dissertations Abstracts International, Volume: 87-04, Section: B.
■500 ▼aAdvisor: Hartwig, John F.
■5021 ▼aThesis (Ph.D.)--University of California, Berkeley, 2025.
■520 ▼aThe following dissertation discusses the development and emerging applications of computationally designed enzymes for catalysis and the development of a ruthenium complex for selective and mild aliphatic C(sp3)-H bond oxidation.Chapter 1 provides an overview of reactions catalyzed by metalloenzymes with a focus on new-to-nature reactions. This section highlights the growing potential of biocatalysis through contemporary and historical examples of industrial biocatalytic processes. Methods for the generation of artificial metalloenzymes and examples of functional de novo designed metalloenzymes are discussed.Chapter 2 focuses on the development of a de novo designed protein for C-H bond oxidation. The application of some of the most common natural oxidases is challenging because of complicated reaction mechanisms, the need for partner enzymes or proteins, and limited stability of relevant enzymes under the reaction conditions. This chapter demonstrates the potential benefits of combining synthetic small molecule catalysts with hyper-stable protein hosts. The combination of these two systems enables their characterization in parallel and therefore, more rapid characterization of the system.Chapter 3 describes the development of a small molecule catalyst for C-H bond oxidation. Many of the reported metal complexes that catalyze undirected C-H bond oxidation suffer from limited stability under the reaction conditions. This section discusses the generation, characterization, and reactivity of a ruthenium complex with a tetradentate pyridine-based ligand. The ruthenium complex is shown to catalyze the oxidation of unactivated tertiary C-H bonds with high turnover numbers, at low substrate concentration, and after prolonged exposure to the terminal oxidant.
■590 ▼aSchool code: 0028.
■650 4▼aOrganic chemistry
■650 4▼aChemistry
■650 4▼aAnalytical chemistry
■653 ▼aAqueous
■653 ▼aBiocatalysis
■653 ▼aOxidation
■653 ▼aRuthenium complex
■690 ▼a0490
■690 ▼a0486
■690 ▼a0485
■71020▼aUniversity of California, Berkeley▼bChemistry.
■7730 ▼tDissertations Abstracts International▼g87-04B.
■790 ▼a0028
■791 ▼aPh.D.
■792 ▼a2025
■793 ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17359384▼nKERIS▼z이 자료의 원문은 한국교육학술정보원에서 제공합니다.
