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Operando Microscopy for Mechanistic Insights Into Cocatalyst Modified Semiconductor Photo(electro)catalysis
Operando Microscopy for Mechanistic Insights Into Cocatalyst Modified Semiconductor Photo(electro)catalysis
상세정보
- 자료유형
- 학위논문 서양
- 최종처리일시
- 20260202103058
- ISBN
- 9798283140810
- DDC
- 540
- 저자명
- Zhao, Zhiheng.
- 서명/저자
- Operando Microscopy for Mechanistic Insights Into Cocatalyst Modified Semiconductor Photo(electro)catalysis
- 발행사항
- [Sl] : Cornell University, 2025
- 발행사항
- Ann Arbor : ProQuest Dissertations & Theses, 2025
- 형태사항
- 431 p
- 주기사항
- Source: Dissertations Abstracts International, Volume: 86-12, Section: B.
- 주기사항
- Advisor: Chen, Peng.
- 학위논문주기
- Thesis (Ph.D.)--Cornell University, 2025.
- 초록/해제
- 요약This dissertation presents studies on semiconductor photoelectrochemical systems, with 2 chapters detailing my major contributions and 3 appendices covering collaborative efforts with my minor contributions. Chapter 1 investigates how single cocatalyst particle depositions influence local and remote charge dynamics on particulate BiVO4 photoanodes. I led the experimental design, synthesis, single-molecule fluorescence imaging, and analysis. Results show that single cocatalyst particles enhance local catalytic activity, while remote suppression occurs for cocatalyst CoOx deposition on basal facets. Operando single-molecule imaging reveals synergistic effects for cocatalyst CoOx and anti-synergistic effects for cocatalyst Pt/PtOx, contributing to improved photocatalyst performance. This chapter comes from a completed first-authored manuscript.Chapter 2 explores overall water splitting on InGaN/GaN nanowires with integrated cocatalysts. I applied operando fluorescence microscopy to map electron- and hole-induced reactions by tracking resazurin reduction and amplex red oxidation. Imaging revealed reaction "hotspots" where electrons and holes converge at shared HER and OER cocatalyst sites, validating critical design principles for optimized nanowires. This chapter comes from a completed manuscript on which I am a co-first author.Appendix 1 examines long-range micropollutant adsorption on metal-promoted photocatalysts (Nature Catal. 2024, 7, 912-920). Appendix 2 investigates nanoscale cooperative adsorption for materials control (Nature Commun. 2021, 12, 4287). Appendix 3 uncovers energy conversion pathways in biohybrids using single-cell multimodal imaging (Nature Chem. 2023, 15, 1400-1407). This dissertation demonstrates the potential of operando single-molecule and single-particle microscopy for elucidating cocatalyst-induced mechanisms, advancing both photo(electro)chemical and biohybrid catalytic system design.
- 일반주제명
- Chemistry
- 일반주제명
- Physical chemistry
- 일반주제명
- Condensed matter physics
- 일반주제명
- Nanoscience
- 키워드
- Cocatalyst
- 기타저자
- Cornell University Chemistry and Chemical Biology
- 기본자료저록
- Dissertations Abstracts International. 86-12B.
- 전자적 위치 및 접속
- 로그인 후 원문을 볼 수 있습니다.
MARC
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■00520260202103058
■006m o d
■007cr#unu||||||||
■020 ▼a9798283140810
■035 ▼a(MiAaPQ)AAI31933174
■040 ▼aMiAaPQ▼cMiAaPQ
■0820 ▼a540
■1001 ▼aZhao, Zhiheng.▼0(orcid)0009-0006-1312-7010
■24510▼aOperando Microscopy for Mechanistic Insights Into Cocatalyst Modified Semiconductor Photo(electro)catalysis
■260 ▼a[Sl]▼bCornell University▼c2025
■260 1▼aAnn Arbor▼bProQuest Dissertations & Theses▼c2025
■300 ▼a431 p
■500 ▼aSource: Dissertations Abstracts International, Volume: 86-12, Section: B.
■500 ▼aAdvisor: Chen, Peng.
■5021 ▼aThesis (Ph.D.)--Cornell University, 2025.
■520 ▼aThis dissertation presents studies on semiconductor photoelectrochemical systems, with 2 chapters detailing my major contributions and 3 appendices covering collaborative efforts with my minor contributions. Chapter 1 investigates how single cocatalyst particle depositions influence local and remote charge dynamics on particulate BiVO4 photoanodes. I led the experimental design, synthesis, single-molecule fluorescence imaging, and analysis. Results show that single cocatalyst particles enhance local catalytic activity, while remote suppression occurs for cocatalyst CoOx deposition on basal facets. Operando single-molecule imaging reveals synergistic effects for cocatalyst CoOx and anti-synergistic effects for cocatalyst Pt/PtOx, contributing to improved photocatalyst performance. This chapter comes from a completed first-authored manuscript.Chapter 2 explores overall water splitting on InGaN/GaN nanowires with integrated cocatalysts. I applied operando fluorescence microscopy to map electron- and hole-induced reactions by tracking resazurin reduction and amplex red oxidation. Imaging revealed reaction "hotspots" where electrons and holes converge at shared HER and OER cocatalyst sites, validating critical design principles for optimized nanowires. This chapter comes from a completed manuscript on which I am a co-first author.Appendix 1 examines long-range micropollutant adsorption on metal-promoted photocatalysts (Nature Catal. 2024, 7, 912-920). Appendix 2 investigates nanoscale cooperative adsorption for materials control (Nature Commun. 2021, 12, 4287). Appendix 3 uncovers energy conversion pathways in biohybrids using single-cell multimodal imaging (Nature Chem. 2023, 15, 1400-1407). This dissertation demonstrates the potential of operando single-molecule and single-particle microscopy for elucidating cocatalyst-induced mechanisms, advancing both photo(electro)chemical and biohybrid catalytic system design.
■590 ▼aSchool code: 0058.
■650 4▼aChemistry
■650 4▼aPhysical chemistry
■650 4▼aCondensed matter physics
■650 4▼aNanoscience
■653 ▼aSemiconductor photoelectrochemical systems
■653 ▼aCocatalyst
■653 ▼aMetal-promoted photocatalysts
■653 ▼aSingle-particle microscopy
■653 ▼aBiohybrid catalytic system design
■690 ▼a0485
■690 ▼a0494
■690 ▼a0565
■690 ▼a0611
■71020▼aCornell University▼bChemistry and Chemical Biology.
■7730 ▼tDissertations Abstracts International▼g86-12B.
■790 ▼a0058
■791 ▼aPh.D.
■792 ▼a2025
■793 ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17356899▼nKERIS▼z이 자료의 원문은 한국교육학술정보원에서 제공합니다.
