자료유형  

 학위논문

Control Number  

0017162248

International Standard Book Number  

9798384022725

Dewey Decimal Classification Number  

540

Main Entry-Personal Name  

Xiao, Langqiu.

Publication, Distribution, etc. (Imprint  

[S.l.] : University of Pennsylvania., 2024

Publication, Distribution, etc. (Imprint  

Ann Arbor : ProQuest Dissertations & Theses, 2024

Physical Description  

167 p.

General Note  

Source: Dissertations Abstracts International, Volume: 86-02, Section: B.

General Note  

Advisor: Mallouk, Thomas E.

Dissertation Note  

Thesis (Ph.D.)--University of Pennsylvania, 2024.

Summary, Etc.  

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.

Subject Added Entry-Topical Term  

Chemistry.

Subject Added Entry-Topical Term  

Physical chemistry.

Subject Added Entry-Topical Term  

Energy.

Subject Added Entry-Topical Term  

Engineering.

Index Term-Uncontrolled  

Artificial photosynthesis

Index Term-Uncontrolled  

Charge transfer

Index Term-Uncontrolled  

Molecular-semiconductor interface

Index Term-Uncontrolled  

Photoelectrochemical cells

Index Term-Uncontrolled  

Solar energy

Index Term-Uncontrolled  

Water splitting

Index Term-Uncontrolled  

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Added Entry-Corporate Name  

University of Pennsylvania Chemistry

Host Item Entry  

Dissertations Abstracts International. 86-02B.

Electronic Location and Access  

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Control Number  

joongbu:653740