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Models of the Oxygen-Evolving Comple...

Kanady, Jacob Steven.

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Models of the Oxygen-Evolving Complex of Photosystem II.

紀錄類型:	書目-電子資源 : Monograph/item
正題名/作者:	Models of the Oxygen-Evolving Complex of Photosystem II./
作者:	Kanady, Jacob Steven.
面頁冊數:	289 p.
附註:	Source: Dissertation Abstracts International, Volume: 76-02(E), Section: B.
Contained By:	Dissertation Abstracts International76-02B(E).
標題:	Inorganic chemistry. -
電子資源:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3637038
ISBN:	9781321194074

Models of the Oxygen-Evolving Complex of Photosystem II.
Kanady, Jacob Steven.

Models of the Oxygen-Evolving Complex of Photosystem II. - 289 p.

Source: Dissertation Abstracts International, Volume: 76-02(E), Section: B.

Thesis (Ph.D.)--California Institute of Technology, 2015.

In the five chapters that follow, I delineate my efforts over the last five years to synthesize structurally and chemically relevant models of the Oxygen Evolving Complex (OEC) of Photosystem II. The OEC is nature's only water oxidation catalyst, in that it forms the dioxygen in our atmosphere necessary for oxygenic life. Therefore understanding its structure and function is of deep fundamental interest and could provide design elements for artificial photosynthesis and manmade water oxidation catalysts. Synthetic endeavors towards OEC mimics have been an active area of research since the mid 1970s and have mutually evolved alongside biochemical and spectroscopic studies, affording ever-refined proposals for the structure of the OEC and the mechanism of water oxidation. This research has culminated in the most recent proposal: a low symmetry Mn4CaO5 cluster with a distorted Mn3CaO4 cubane bridged to a fourth, dangling Mn. To give context for how my graduate work fits into this rich history of OEC research, Chapter 1 provides a historical timeline of proposals for OEC structure, emphasizing the role that synthetic Mn and MnCa clusters have played, and ending with our Mn3CaO4 heterometallic cubane complexes.

ISBN: 9781321194074Subjects--Topical Terms:

3173556
Inorganic chemistry.

Models of the Oxygen-Evolving Complex of Photosystem II.
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245 1 0 $a Models of the Oxygen-Evolving Complex of Photosystem II.
300 $a 289 p.
500 $a Source: Dissertation Abstracts International, Volume: 76-02(E), Section: B.
500 $a Adviser: Theodor Agapie.
502 $a Thesis (Ph.D.)--California Institute of Technology, 2015.
520 $a In the five chapters that follow, I delineate my efforts over the last five years to synthesize structurally and chemically relevant models of the Oxygen Evolving Complex (OEC) of Photosystem II. The OEC is nature's only water oxidation catalyst, in that it forms the dioxygen in our atmosphere necessary for oxygenic life. Therefore understanding its structure and function is of deep fundamental interest and could provide design elements for artificial photosynthesis and manmade water oxidation catalysts. Synthetic endeavors towards OEC mimics have been an active area of research since the mid 1970s and have mutually evolved alongside biochemical and spectroscopic studies, affording ever-refined proposals for the structure of the OEC and the mechanism of water oxidation. This research has culminated in the most recent proposal: a low symmetry Mn4CaO5 cluster with a distorted Mn3CaO4 cubane bridged to a fourth, dangling Mn. To give context for how my graduate work fits into this rich history of OEC research, Chapter 1 provides a historical timeline of proposals for OEC structure, emphasizing the role that synthetic Mn and MnCa clusters have played, and ending with our Mn3CaO4 heterometallic cubane complexes.
520 $a In Chapter 2, the triarylbenzene ligand framework used throughout my work is introduced, and trinuclear clusters of Mn, Co, and Ni are discussed. The ligand scaffold consistently coordinates three metals in close proximity while leaving coordination sites open for further modification through ancillary ligand binding. The ligands coordinated could be varied, with a range of carboxylates and some less coordinating anions studied. These complexes' structures, magnetic behavior, and redox properties are discussed.
520 $a Chapter 3 explores the redox chemistry of the trimanganese system more thoroughly in the presence of a fourth Mn equivalent, finding a range of oxidation states and oxide incorporation dependent on oxidant, solvent, and Mn salt. Oxidation states from MnII4 to MnIIIMn IV3 were observed, with 1-4 O2- ligands incorporated, modeling the photoactivation of the OEC. These complexes were studied by X-ray diffraction, EPR, XAS, magnetometry, and CV.
520 $a As Ca2+ is a necessary component of the OEC, Chapter 4 discusses synthetic strategies for making highly structurally accurate models of the OEC containing both Mn and Ca in the Mn3CaO4 cubane + dangling Mn geometry. Structural and electrochemical characterization of the first Mn3CaO4 heterometallic cubane complex---and comparison to an all-Mn Mn4O4 analog---suggests a role for Ca2+ in the OEC. Modification of the Mn3CaO 4 system by ligand substitution affords low symmetry Mn3CaO 4 complexes that are the most accurate models of the OEC to date.
520 $a Finally, in Chapter 5 the reactivity of the Mn3MO4 cubane complexes toward O-atom transfer is discussed. The metal M strongly affects the reactivity. The mechanisms of O-atom transfer and water incorporation from and into Mn4O4 and Mn4O3 clusters, respectively, are studied through computation and 18O-labeling studies. The micro3-oxos of the Mn4O4 system prove fluxional, lending support for proposals of O2- fluxionality within the OEC.
590 $a School code: 0037.
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650 4 $a Biochemistry. $3 518028
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