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Development of Artificial Metalloenzymes for Application in Synthetic Chemistry
Development of Artificial Metalloenzymes for Application in Synthetic Chemistry
Development of Artificial Metalloenzymes for Application in Synthetic Chemistry

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자료유형  
 학위논문 서양
최종처리일시  
20260202105112
ISBN  
9798297601635
DDC  
547
저자명  
Joyner, Isaac August DeLong.
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
키워드  
Ruthenium complex
기타저자  
University of California, Berkeley Chemistry
기본자료저록  
Dissertations Abstracts International. 87-04B.
전자적 위치 및 접속  
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■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.

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