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Charge Transfer at the Molecular-Semiconductor Interface of Photoelectrocatalytic Water Splitting Systems
Charge Transfer at the Molecular-Semiconductor Interface of Photoelectrocatalytic Water Splitting Systems
상세정보
- 자료유형
- 학위논문 서양
- 최종처리일시
- 20250211151950
- ISBN
- 9798384022725
- DDC
- 540
- 저자명
- Xiao, Langqiu.
- 서명/저자
- Charge Transfer at the Molecular-Semiconductor Interface of Photoelectrocatalytic Water Splitting Systems
- 발행사항
- [Sl] : University of Pennsylvania, 2024
- 발행사항
- Ann Arbor : ProQuest Dissertations & Theses, 2024
- 형태사항
- 167 p
- 주기사항
- Source: Dissertations Abstracts International, Volume: 86-02, Section: B.
- 주기사항
- Advisor: Mallouk, Thomas E.
- 학위논문주기
- Thesis (Ph.D.)--University of Pennsylvania, 2024.
- 초록/해제
- 요약Solar fuels that are produced by using abundant molecules (carbon dioxide and water) and sunlight have provided a promising sustainable solution for future energy production. Water-splitting dye-sensitized solar cells utilize semiconductor substrates with high surface areas to incorporate molecular sensitizers and catalysts. The charge transfer processes at the molecule-semiconductor interfaces are crucial to the overall efficiency and performance of these devices. In this dissertation, the interface of molecular sensitizers and the semiconductor electrodes was investigated.In Chapter 1, historical milestones and recent progress in the development of water-splitting dye-sensitized photoelectrochemical cells are summarized. In Chapter 2, the process of interfacial charge transfer at dye-sensitized TiO2 nanowire array electrodes in aqueous electrolytes was studied. This project illustrates the impact of the semiconductor morphology on the charge transport dynamics and recombination rates. In Chapter 3, the solvent effect on interfacial electron injection was studied for dye-sensitized mesoporous TiO2 and SnO2/TiO2 core/shell structures. It was found that changing the dielectric constant of the electrolyte by mixing aqueous and nonaqueous solutions can tune the electron injection efficiency. An injection-induced electric field was found to be present in electrolytes with low ion concentrations and low dielectric constants. This field causes trapping of conduction band electrons at the SnO2/TiO2 interface, resulting in lower overall quantum yields for charge collection. Chapter 4 studied the impact of sensitizer structure and nuclearity on the stability and electron injection efficiency. The study presents the strategy of dimerizing Ru(II) sensitizers that contain various anchoring groups. It was found that dimers with carboxylic acid groups exhibited enhanced stability and the highest injection efficiency.By studying the impact of the morphology of the semiconductor, the solvent, and sensitizer functional groups on the interfacial charge transfer dynamics, we gain insight into the fundamentals of the molecule-semiconductor system. The understanding that is developed not only offers guidance on the future design of better performing photo(electro)catalytic systems for solar fuel production, but also provides useful insights for other photochemical systems that contain a molecule-semiconductor junction.
- 일반주제명
- Chemistry
- 일반주제명
- Physical chemistry
- 일반주제명
- Energy
- 일반주제명
- Engineering
- 키워드
- Charge transfer
- 키워드
- Solar energy
- 키워드
- Water splitting
- 키워드
- `
- 기타저자
- University of Pennsylvania Chemistry
- 기본자료저록
- Dissertations Abstracts International. 86-02B.
- 전자적 위치 및 접속
- 로그인 후 원문을 볼 수 있습니다.
MARC
008250123s2024 us c eng d■001000017162248
■00520250211151950
■006m o d
■007cr#unu||||||||
■020 ▼a9798384022725
■035 ▼a(MiAaPQ)AAI31328286
■040 ▼aMiAaPQ▼cMiAaPQ
■0820 ▼a540
■1001 ▼aXiao, Langqiu.
■24510▼aCharge Transfer at the Molecular-Semiconductor Interface of Photoelectrocatalytic Water Splitting Systems
■260 ▼a[Sl]▼bUniversity of Pennsylvania▼c2024
■260 1▼aAnn Arbor▼bProQuest Dissertations & Theses▼c2024
■300 ▼a167 p
■500 ▼aSource: Dissertations Abstracts International, Volume: 86-02, Section: B.
■500 ▼aAdvisor: Mallouk, Thomas E.
■5021 ▼aThesis (Ph.D.)--University of Pennsylvania, 2024.
■520 ▼aSolar fuels that are produced by using abundant molecules (carbon dioxide and water) and sunlight have provided a promising sustainable solution for future energy production. Water-splitting dye-sensitized solar cells utilize semiconductor substrates with high surface areas to incorporate molecular sensitizers and catalysts. The charge transfer processes at the molecule-semiconductor interfaces are crucial to the overall efficiency and performance of these devices. In this dissertation, the interface of molecular sensitizers and the semiconductor electrodes was investigated.In Chapter 1, historical milestones and recent progress in the development of water-splitting dye-sensitized photoelectrochemical cells are summarized. In Chapter 2, the process of interfacial charge transfer at dye-sensitized TiO2 nanowire array electrodes in aqueous electrolytes was studied. This project illustrates the impact of the semiconductor morphology on the charge transport dynamics and recombination rates. In Chapter 3, the solvent effect on interfacial electron injection was studied for dye-sensitized mesoporous TiO2 and SnO2/TiO2 core/shell structures. It was found that changing the dielectric constant of the electrolyte by mixing aqueous and nonaqueous solutions can tune the electron injection efficiency. An injection-induced electric field was found to be present in electrolytes with low ion concentrations and low dielectric constants. This field causes trapping of conduction band electrons at the SnO2/TiO2 interface, resulting in lower overall quantum yields for charge collection. Chapter 4 studied the impact of sensitizer structure and nuclearity on the stability and electron injection efficiency. The study presents the strategy of dimerizing Ru(II) sensitizers that contain various anchoring groups. It was found that dimers with carboxylic acid groups exhibited enhanced stability and the highest injection efficiency.By studying the impact of the morphology of the semiconductor, the solvent, and sensitizer functional groups on the interfacial charge transfer dynamics, we gain insight into the fundamentals of the molecule-semiconductor system. The understanding that is developed not only offers guidance on the future design of better performing photo(electro)catalytic systems for solar fuel production, but also provides useful insights for other photochemical systems that contain a molecule-semiconductor junction.
■590 ▼aSchool code: 0175.
■650 4▼aChemistry
■650 4▼aPhysical chemistry
■650 4▼aEnergy
■650 4▼aEngineering
■653 ▼aArtificial photosynthesis
■653 ▼aCharge transfer
■653 ▼aMolecular-semiconductor interface
■653 ▼aPhotoelectrochemical cells
■653 ▼aSolar energy
■653 ▼aWater splitting
■653 ▼a`
■690 ▼a0485
■690 ▼a0494
■690 ▼a0791
■690 ▼a0537
■71020▼aUniversity of Pennsylvania▼bChemistry.
■7730 ▼tDissertations Abstracts International▼g86-02B.
■790 ▼a0175
■791 ▼aPh.D.
■792 ▼a2024
■793 ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17162248▼nKERIS▼z이 자료의 원문은 한국교육학술정보원에서 제공합니다.
