國立高雄大學圖資館 |

Language: English

Back

Charge Transfer at the Molecular-Semiconductor Interface of Photoelectrocatalytic Water Splitting Systems /

Record Type:	Electronic resources : Monograph/item
Title/Author:	Charge Transfer at the Molecular-Semiconductor Interface of Photoelectrocatalytic Water Splitting Systems /Langqiu Xiao.
Author:	Xiao, Langqiu,
Description:	1 electronic resource (167 pages)
Notes:	Source: Dissertations Abstracts International, Volume: 86-02, Section: B.
Notes:	Advisors: Mallouk, Thomas E. Committee members: Schelter, Eric J.; Kagan, Cherie R.; Pikul, James H.
Contained By:	Dissertations Abstracts International86-02B.
Subject:	Chemistry.
Online resource:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=31328286
ISBN:	9798384022725

Charge Transfer at the Molecular-Semiconductor Interface of Photoelectrocatalytic Water Splitting Systems /
Xiao, Langqiu,

Charge Transfer at the Molecular-Semiconductor Interface of Photoelectrocatalytic Water Splitting Systems /Langqiu Xiao. - 1 electronic resource (167 pages)

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

Solar 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.

English

ISBN: 9798384022725Subjects--Topical Terms:

188628
Chemistry.
Subjects--Index Terms:

Artificial photosynthesis

Charge Transfer at the Molecular-Semiconductor Interface of Photoelectrocatalytic Water Splitting Systems /
LDR:04063nmm a22004693i 4500 001 676336
005 20250420214345.5
006 m o d
007 cr|nu||||||||
008 250901s2024 miu||||||m |||||||eng d
020 $a 9798384022725
035 $a (MiAaPQD)AAI31328286
035 $a AAI31328286
040 $a MiAaPQD $b eng $c MiAaPQD $e rda
100 1 $a Xiao, Langqiu, $e author. $3 990116
245 1 0 $a Charge Transfer at the Molecular-Semiconductor Interface of Photoelectrocatalytic Water Splitting Systems / $c Langqiu Xiao.
264 1 $a Ann Arbor : $b ProQuest Dissertations & Theses, $c 2024
300 $a 1 electronic resource (167 pages)
336 $a text $b txt $2 rdacontent
337 $a computer $b c $2 rdamedia
338 $a online resource $b cr $2 rdacarrier
500 $a Source: Dissertations Abstracts International, Volume: 86-02, Section: B.
500 $a Advisors: Mallouk, Thomas E. Committee members: Schelter, Eric J.; Kagan, Cherie R.; Pikul, James H.
502 $b Ph.D. $c University of Pennsylvania $d 2024.
520 $a Solar 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.
546 $a English
590 $a School code: 0175
650 4 $a Chemistry. $3 188628
650 4 $a Physical chemistry. $3 708580
650 4 $a Energy. $3 212397
650 4 $a Engineering. $3 210888
653 $a Artificial photosynthesis
653 $a Charge transfer
653 $a Molecular-semiconductor interface
653 $a Photoelectrochemical cells
653 $a Solar energy
653 $a Water splitting
653 $a `
690 $a 0485
690 $a 0494
690 $a 0791
690 $a 0537
710 2 $a University of Pennsylvania. $b Chemistry. $3 730347
720 1 $a Mallouk, Thomas E. $e degree supervisor.
773 0 $t Dissertations Abstracts International $g 86-02B.
790 $a 0175
791 $a Ph.D.
792 $a 2024
856 4 0 $u http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=31328286