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Mechanisms of interfacial electron-t...

Rowley, John G.

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Mechanisms of interfacial electron-transfer within high-surface-area metal-oxide thin films.

紀錄類型:	書目-電子資源 : Monograph/item
正題名/作者:	Mechanisms of interfacial electron-transfer within high-surface-area metal-oxide thin films./
作者:	Rowley, John G.
出版者:	Ann Arbor : ProQuest Dissertations & Theses, : 2011,
面頁冊數:	133 p.
附註:	Source: Dissertation Abstracts International, Volume: 73-01, Section: B, page: 3170.
Contained By:	Dissertation Abstracts International73-01B.
標題:	Inorganic chemistry. -
電子資源:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3483372
ISBN:	9781124992471

Mechanisms of interfacial electron-transfer within high-surface-area metal-oxide thin films.
Rowley, John G.

Mechanisms of interfacial electron-transfer within high-surface-area metal-oxide thin films. - Ann Arbor : ProQuest Dissertations & Theses, 2011 - 133 p.

Source: Dissertation Abstracts International, Volume: 73-01, Section: B, page: 3170.

Thesis (Ph.D.)--The Johns Hopkins University, 2011.

The direct conversion of solar photon energy into electrical power is achieved with photovoltaic technology, yet existing technology is too inefficient or expensive to implement on a global scale. Dye sensitized solar cells (DSSCs) based on earth abundant low cost materials could overcome the barriers for world-wide implantation of photovoltaic technology. Historically the most efficient regenerative DSSCs utilize iodide based redox mediators in nitrile solvents. Despite the dominance of iodide redox mediator in DSSCs, the chemical attribute(s) that make iodide based electrolytes superior to other electrolyte is yet unproven. Discovering the chemical cause of iodide's superiority as a redox mediator was and important aspect of this thesis research.

ISBN: 9781124992471Subjects--Topical Terms:

3173556
Inorganic chemistry.

Mechanisms of interfacial electron-transfer within high-surface-area metal-oxide thin films.
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245 1 0 $a Mechanisms of interfacial electron-transfer within high-surface-area metal-oxide thin films.
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300 $a 133 p.
500 $a Source: Dissertation Abstracts International, Volume: 73-01, Section: B, page: 3170.
500 $a Adviser: Gerald J. Meyer.
502 $a Thesis (Ph.D.)--The Johns Hopkins University, 2011.
520 $a The direct conversion of solar photon energy into electrical power is achieved with photovoltaic technology, yet existing technology is too inefficient or expensive to implement on a global scale. Dye sensitized solar cells (DSSCs) based on earth abundant low cost materials could overcome the barriers for world-wide implantation of photovoltaic technology. Historically the most efficient regenerative DSSCs utilize iodide based redox mediators in nitrile solvents. Despite the dominance of iodide redox mediator in DSSCs, the chemical attribute(s) that make iodide based electrolytes superior to other electrolyte is yet unproven. Discovering the chemical cause of iodide's superiority as a redox mediator was and important aspect of this thesis research.
520 $a In Chapter 2 the photoinitated formation and cleavage of I-I bonds is demonstrated at an un-sensitized potentiostatically controlled mesoporous nanocrystalline (anatase) TiO2 thin film. After pulsed laser excitation of a TiO2 thin film, I2·- was observed that disproportionated to yield I3- and I-, but did not react with TiO2. In contrast evidence for a quasi-Fermi level dependent reaction between TiO2(e -) and I3- was observed.
520 $a In agreement with the findings at un-sensitized TiO2 in Chapter 2, the results presented in Chapter 3 demonstrate that after pulsed laser excitation of an operational DSSC: I2·- is observed, I2·-does not react with TiO 2, and that charge recombination between I3- and TiO2(e-) is operative. In addition to absorption changes attributed to iodide redox chemistry, evidence for a transient electric field induced Stark effect was observed in the operational DSSC. Absorption changes reporting on the electric field at the TiO2 surface were simultaneously quantified at specific power conditions fo the operational DSSC.
520 $a Chapter 4 explores alternative redox mediators to the iodide/triiodide couple. The photophysical studies presented herein provide key mechanistic details on kinetic processes pertinent to operational DSSCs. Specifically, electron transfer to and from iodide species found in an operational DSSC were quantified. Taken together this research advances the body of knowledge quantifying the chemical properties that make iodide based electrolytes a superior redox mediator in dye sensitized solar cells.
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