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Catalyst Selectivity and Motion Imaged by Single-Molecule Spectroscopy and Curriculum Development for Undergraduate Argument-Driven Inquiry Laboratories
Catalyst Selectivity and Motion Imaged by Single-Molecule Spectroscopy and Curriculum Development for Undergraduate Argument-Driven Inquiry Laboratories
상세정보
- 자료유형
- 학위논문 서양
- 최종처리일시
- 20250211152041
- ISBN
- 9798384498346
- DDC
- 540
- 서명/저자
- Catalyst Selectivity and Motion Imaged by Single-Molecule Spectroscopy and Curriculum Development for Undergraduate Argument-Driven Inquiry Laboratories
- 발행사항
- [Sl] : University of California, Irvine, 2024
- 발행사항
- Ann Arbor : ProQuest Dissertations & Theses, 2024
- 형태사항
- 404 p
- 주기사항
- Source: Dissertations Abstracts International, Volume: 86-04, Section: B.
- 주기사항
- Advisor: Patterson, Joe.
- 학위논문주기
- Thesis (Ph.D.)--University of California, Irvine, 2024.
- 초록/해제
- 요약This dissertation is composed of two main parts. The first half, Chapter 1 through Chapter 3, discusses my efforts to investigate the selectivity and motion of individual molecular catalysts in polymer networks through the use of single-molecule fluorescence microscopy. The second half, Chapter 4 through Chapter 6, discusses my chemical education research for the transition of existing curriculum to Argument-Driven Inquiry.Chapter 1 focuses on the introduction of single-molecule fluorescence microscopy, specifically towards innovation and elucidation of catalyst dynamics, which is relevant to the first half of this dissertation. Super resolution fluorescence microscopy provides a powerful tool to investigate mechanistic questions and reaction dynamics that would otherwise be resolution- or diffraction-limited, providing insight at the nanometer level. An overview of recent applications of single-molecule and sub ensemble fluorescence microscopy to synthetic applications and catalytic motion-tracking is included herein, providing context for the scholarship in this dissertation.Chapter 2 discusses, for the first time, the selectivity of individual molecular catalysts for two different reactions is imaged in real time at the single-catalyst level. This imaging is achieved through fluorescence microscopy paired with spectral probes that produce a "snapshot" of the instantaneous chemoselectivity of a single catalyst for either a single-chain-elongation or a single-chain-termination event during ruthenium-catalyzed polymerization. Super resolution imaging of multiple selectivity events, each at a different single-molecular ruthenium catalyst, indicates that catalyst selectivity may be unexpectedly spatial- and time-variable.In Chapter 3, the motion of single molecular ruthenium catalysts during and after single turnover events of ring-opening metathesis polymerization is imaged through single-molecule super resolution tracking with positional accuracy of ±32 nm. This tracking is achieved through real-time incorporation of spectrally tagged monomer units into active polymer chains ends during living polymerization; thus, by design, only active-catalyst motion is detected and imaged, without convolution by inactive catalysts. The catalysts show diverse individualistic diffusive behaviors with respect to time that persist for up to 20 s. Such differential motion indicates widely different local catalyst microenvironments during catalytic turnover. These mobility differences are uniquely observable through single-catalyst microscopy and are not measurable through traditional ensemble analytical techniques for characterizing the behavior of molecular catalysts, such as NMR spectroscopy.Traditional laboratory classes are often administered through "cookbook" style curriculum that does not accurately reflect the scientific inquiry and debate. To reflect this more realistic picture of the scientific process, the traditional curriculum of confirmation labs for the lower division undergraduate labs at University of California, Irvine has been adapted to Argument-Driven Inquiry, a guided inquiry curriculum that allows for debate and revision. Chapter 4 introduces a literature overview of the process of Argument-Driven Inquiry and its use as an alternative style of laboratory curriculum in other institutions.Chapter 5 describes the creation of a second quarter of a two-quarter sequence of argument-driven-inquiry general chemistry laboratories. The course contains four projects investigating the chemistry of spices (vanilla, cinnamon, spearmint, and cloves) and incorporates a structured review and hands-on applications of fundamental concepts necessary to transition between general and organic chemistry (colligative properties, TLC, synthesis, characterization tests, and unknown determination). The inquiry-based curriculum was designed to give students increasing responsibility and freedom to develop experimental design skills. Specifications grading is used to increase concept iteration and encourage teamwork amongst students. Survey results for student learning style, feelings about chemistry, and perception of the course format are compared for first and second quarter courses. Changes in survey responses show higher average positive responses in many categories for the second quarter course.Chapter 6 outlines the ongoing effort to design a series of Organic Chemistry experiments to be used in an ADI course, with a focus on designing intentional variation to lead to robust argumentation. These experiments were evaluated by a group of undergraduate beta-testers, who performed the full course as students, including the argumentation sessions. These designed experiments are discussed and analyzed based on student feedback. The argumentation sessions were analyzed by the Assessment of Student Argumentation in the Classroom protocol to quantify the level of discourse achieved by the students. Both results are evaluated to determine the efficacy of the designed curriculum. Future directions and continuing work on the curriculum are outlined.
- 일반주제명
- Chemistry
- 일반주제명
- Organic chemistry
- 일반주제명
- Molecular chemistry
- 기타저자
- University of California, Irvine Chemistry
- 기본자료저록
- Dissertations Abstracts International. 86-04B.
- 전자적 위치 및 접속
- 로그인 후 원문을 볼 수 있습니다.
MARC
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■020 ▼a9798384498346
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■040 ▼aMiAaPQ▼cMiAaPQ
■0820 ▼a540
■1001 ▼aSaluga, Shannon J.
■24510▼aCatalyst Selectivity and Motion Imaged by Single-Molecule Spectroscopy and Curriculum Development for Undergraduate Argument-Driven Inquiry Laboratories
■260 ▼a[Sl]▼bUniversity of California, Irvine▼c2024
■260 1▼aAnn Arbor▼bProQuest Dissertations & Theses▼c2024
■300 ▼a404 p
■500 ▼aSource: Dissertations Abstracts International, Volume: 86-04, Section: B.
■500 ▼aAdvisor: Patterson, Joe.
■5021 ▼aThesis (Ph.D.)--University of California, Irvine, 2024.
■520 ▼aThis dissertation is composed of two main parts. The first half, Chapter 1 through Chapter 3, discusses my efforts to investigate the selectivity and motion of individual molecular catalysts in polymer networks through the use of single-molecule fluorescence microscopy. The second half, Chapter 4 through Chapter 6, discusses my chemical education research for the transition of existing curriculum to Argument-Driven Inquiry.Chapter 1 focuses on the introduction of single-molecule fluorescence microscopy, specifically towards innovation and elucidation of catalyst dynamics, which is relevant to the first half of this dissertation. Super resolution fluorescence microscopy provides a powerful tool to investigate mechanistic questions and reaction dynamics that would otherwise be resolution- or diffraction-limited, providing insight at the nanometer level. An overview of recent applications of single-molecule and sub ensemble fluorescence microscopy to synthetic applications and catalytic motion-tracking is included herein, providing context for the scholarship in this dissertation.Chapter 2 discusses, for the first time, the selectivity of individual molecular catalysts for two different reactions is imaged in real time at the single-catalyst level. This imaging is achieved through fluorescence microscopy paired with spectral probes that produce a "snapshot" of the instantaneous chemoselectivity of a single catalyst for either a single-chain-elongation or a single-chain-termination event during ruthenium-catalyzed polymerization. Super resolution imaging of multiple selectivity events, each at a different single-molecular ruthenium catalyst, indicates that catalyst selectivity may be unexpectedly spatial- and time-variable.In Chapter 3, the motion of single molecular ruthenium catalysts during and after single turnover events of ring-opening metathesis polymerization is imaged through single-molecule super resolution tracking with positional accuracy of ±32 nm. This tracking is achieved through real-time incorporation of spectrally tagged monomer units into active polymer chains ends during living polymerization; thus, by design, only active-catalyst motion is detected and imaged, without convolution by inactive catalysts. The catalysts show diverse individualistic diffusive behaviors with respect to time that persist for up to 20 s. Such differential motion indicates widely different local catalyst microenvironments during catalytic turnover. These mobility differences are uniquely observable through single-catalyst microscopy and are not measurable through traditional ensemble analytical techniques for characterizing the behavior of molecular catalysts, such as NMR spectroscopy.Traditional laboratory classes are often administered through "cookbook" style curriculum that does not accurately reflect the scientific inquiry and debate. To reflect this more realistic picture of the scientific process, the traditional curriculum of confirmation labs for the lower division undergraduate labs at University of California, Irvine has been adapted to Argument-Driven Inquiry, a guided inquiry curriculum that allows for debate and revision. Chapter 4 introduces a literature overview of the process of Argument-Driven Inquiry and its use as an alternative style of laboratory curriculum in other institutions.Chapter 5 describes the creation of a second quarter of a two-quarter sequence of argument-driven-inquiry general chemistry laboratories. The course contains four projects investigating the chemistry of spices (vanilla, cinnamon, spearmint, and cloves) and incorporates a structured review and hands-on applications of fundamental concepts necessary to transition between general and organic chemistry (colligative properties, TLC, synthesis, characterization tests, and unknown determination). The inquiry-based curriculum was designed to give students increasing responsibility and freedom to develop experimental design skills. Specifications grading is used to increase concept iteration and encourage teamwork amongst students. Survey results for student learning style, feelings about chemistry, and perception of the course format are compared for first and second quarter courses. Changes in survey responses show higher average positive responses in many categories for the second quarter course.Chapter 6 outlines the ongoing effort to design a series of Organic Chemistry experiments to be used in an ADI course, with a focus on designing intentional variation to lead to robust argumentation. These experiments were evaluated by a group of undergraduate beta-testers, who performed the full course as students, including the argumentation sessions. These designed experiments are discussed and analyzed based on student feedback. The argumentation sessions were analyzed by the Assessment of Student Argumentation in the Classroom protocol to quantify the level of discourse achieved by the students. Both results are evaluated to determine the efficacy of the designed curriculum. Future directions and continuing work on the curriculum are outlined.
■590 ▼aSchool code: 0030.
■650 4▼aChemistry
■650 4▼aOrganic chemistry
■650 4▼aMolecular chemistry
■653 ▼aArgument-driven inquiry
■653 ▼aChemical education
■653 ▼aCurriculum development
■653 ▼aMolecular catalysis
■653 ▼aSingle-molecule spectroscopy
■690 ▼a0485
■690 ▼a0431
■690 ▼a0490
■71020▼aUniversity of California, Irvine▼bChemistry.
■7730 ▼tDissertations Abstracts International▼g86-04B.
■790 ▼a0030
■791 ▼aPh.D.
■792 ▼a2024
■793 ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17162683▼nKERIS▼z이 자료의 원문은 한국교육학술정보원에서 제공합니다.
