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Making Molecules for Light-Driven Wa...

Norris, Michael R.

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Making Molecules for Light-Driven Water Splitting.

紀錄類型:	書目-語言資料,印刷品 : Monograph/item
正題名/作者:	Making Molecules for Light-Driven Water Splitting./
作者:	Norris, Michael R.
面頁冊數:	284 p.
附註:	Source: Dissertation Abstracts International, Volume: 75-01(E), Section: B.
Contained By:	Dissertation Abstracts International75-01B(E).
標題:	Chemistry, Molecular. -
電子資源:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3594192
ISBN:	9781303378669

Making Molecules for Light-Driven Water Splitting.
Norris, Michael R.

Making Molecules for Light-Driven Water Splitting. - 284 p.

Source: Dissertation Abstracts International, Volume: 75-01(E), Section: B.

Thesis (Ph.D.)--The University of North Carolina at Chapel Hill, 2013.

To meet growing global energy demand, methods to transform solar energy into chemical fuels are necessary. Photosynthesis provides a blueprint: using electrons from the photo-driven oxidation of water to generate reductive equivalents, which ultimately convert CO2 to carbohydrates. Key to any artificial photosynthetic device that attempts to mimic this process is the light-driven water oxidation reaction, 2H2O + 4hnu → O2 + 4e-. Incorporation of a chromophoric material for absorption of light and a catalyst for water oxidation are therefore required.

ISBN: 9781303378669Subjects--Topical Terms:

1676084
Chemistry, Molecular.

Making Molecules for Light-Driven Water Splitting.
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245 1 0 $a Making Molecules for Light-Driven Water Splitting.
300 $a 284 p.
500 $a Source: Dissertation Abstracts International, Volume: 75-01(E), Section: B.
500 $a Advisers: Thomas J. Meyer; Joseph L. Templeton.
502 $a Thesis (Ph.D.)--The University of North Carolina at Chapel Hill, 2013.
520 $a To meet growing global energy demand, methods to transform solar energy into chemical fuels are necessary. Photosynthesis provides a blueprint: using electrons from the photo-driven oxidation of water to generate reductive equivalents, which ultimately convert CO2 to carbohydrates. Key to any artificial photosynthetic device that attempts to mimic this process is the light-driven water oxidation reaction, 2H2O + 4hnu → O2 + 4e-. Incorporation of a chromophoric material for absorption of light and a catalyst for water oxidation are therefore required.
520 $a Several monomeric, single-site Ru polypryidyl catalysts have been investigated for this transformation. Electrochemical or CeIV oxidation results in homogeneous catalytic water oxidation. Catalytic rates and onset potentials were found to be highly tunable based on the ligand environment. Water oxidation catalysts built with first-row transition metals were also investigated. Electrochemical studies of these complexes indicated complexes of Fe and Cu were catalysts for water oxidation at elevated pH.
520 $a In addition to water oxidation catalysts, chromophore/redox mediator (CRM) complexes are necessary for light-driven water oxidation. A series of nine Ru polypyridyl complexes as well as four organic derivatives of perylene diimide (PDI) were synthesized, and their electrochemical and photophysical properties were investigated for possible use in an artificial photosynthetic device. Control of conjugation and heteroatoms in the polypyridyl ligands led to highly tunable redox potentials, UV/vis absorptions, and emission energies for the Ru complexes, while the PDI derivatives were found to undergo rapid charge separation upon excitation.
520 $a For artificial photosynthetic devices to operate in aqueous media, it is necessary to form stable anchors to metal oxide surfaces. New synthetic procedures for making phosphonic acid-derivatized bipyridine ligands and their Ru polypyridyl complexes were devised, and these routes allow easy access to important ligands and to complexes that can bind to metal oxide surfaces.
520 $a Finally, CRM complexes and catalysts were combined in a molecular Ru-choromphore-Ru-catalyst assembly. Solution studies led to the discovery of a redox mediator effect in water oxidation driven by CeIV. Detailed electrochemical and photophysical studies of the assembly anchored to metal oxide surfaces were performed, and the assembly was shown to be the first molecular chromophore-catalyst assembly capable of light-driven water oxidation.
590 $a School code: 0153.
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650 4 $a Chemistry, Inorganic. $3 517253
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710 2 $a The University of North Carolina at Chapel Hill. $b Chemistry. $3 1021872
773 0 $t Dissertation Abstracts International $g 75-01B(E).
790 $a 0153
791 $a Ph.D.
792 $a 2013
793 $a English
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