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Preparation and properties of high-v...

Bhaduri, Sumit.

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Preparation and properties of high-valent manganese carboxylate clusters: Single-molecule magnetism properties and models for water oxidation.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Preparation and properties of high-valent manganese carboxylate clusters: Single-molecule magnetism properties and models for water oxidation./
Author:	Bhaduri, Sumit.
Description:	324 p.
Notes:	Source: Dissertation Abstracts International, Volume: 63-12, Section: B, page: 5833.
Contained By:	Dissertation Abstracts International63-12B.
Subject:	Chemistry, Inorganic. -
Online resource:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3075932
ISBN:	0493963758

Preparation and properties of high-valent manganese carboxylate clusters: Single-molecule magnetism properties and models for water oxidation.
Bhaduri, Sumit.

Preparation and properties of high-valent manganese carboxylate clusters: Single-molecule magnetism properties and models for water oxidation. - 324 p.

Source: Dissertation Abstracts International, Volume: 63-12, Section: B, page: 5833.

Thesis (Ph.D.)--Indiana University, 2002.

A lot of effort has been devoted in the past to the development of preparative methods to polynuclear, oxide-bridged Mn carboxylate clusters with relevance to areas as diverse as magnetic materials and bioinorganic chemistry. The former area involves the ability of single molecules to retain, below a critical temperature, the orientation of their individual magnetic moments, resulting in the observation of bulk magnetization in the absence of a magnetic field without long range interaction of the spin centers. Such molecules are termed single-molecule magnets (SMMs). In the latter area, a tetranuclear Mn-oxo aggregate referred to as the Water Oxidation Complex (WOC) is known to catalyze the photosynthetic transformation of water to dioxygen near the Photosystem II reaction site.

ISBN: 0493963758Subjects--Topical Terms:

517253
Chemistry, Inorganic.

Preparation and properties of high-valent manganese carboxylate clusters: Single-molecule magnetism properties and models for water oxidation.
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100 1 $a Bhaduri, Sumit. $3 1933001
245 1 0 $a Preparation and properties of high-valent manganese carboxylate clusters: Single-molecule magnetism properties and models for water oxidation.
300 $a 324 p.
500 $a Source: Dissertation Abstracts International, Volume: 63-12, Section: B, page: 5833.
500 $a Chair: George Christou.
502 $a Thesis (Ph.D.)--Indiana University, 2002.
520 $a A lot of effort has been devoted in the past to the development of preparative methods to polynuclear, oxide-bridged Mn carboxylate clusters with relevance to areas as diverse as magnetic materials and bioinorganic chemistry. The former area involves the ability of single molecules to retain, below a critical temperature, the orientation of their individual magnetic moments, resulting in the observation of bulk magnetization in the absence of a magnetic field without long range interaction of the spin centers. Such molecules are termed single-molecule magnets (SMMs). In the latter area, a tetranuclear Mn-oxo aggregate referred to as the Water Oxidation Complex (WOC) is known to catalyze the photosynthetic transformation of water to dioxygen near the Photosystem II reaction site.
520 $a In this work, different synthetic methods have been developed to prepare a variety of tetranuclear clusters that provide new members of the SMM family of complexes. The products have been characterized by X-ray crystallography, 1H-NMR spectroscopy, magnetic susceptibility studies, EPR spectroscopy and electrochemistry. Addition of mineral acids (HX; X = Cl- , Br-, F-, NO3 -) to [Mn4O2(O2CEt)6(dbm) 2] results in disproportionation leading to high yields of [Mn 4O3X(O2CEt)3(dbm)3] complexes containing the [Mn4(mu3-O)3(mu3-X)] core (dbm- is the anion of dibenzoylmethane). Chemical oxidation of [Mn4O2(O2CEt)6(dbm)2] with permanganate leads to [Mn4O3(O2CEt )4(dbm)3]. The latter crystallizes as a 1:1 mixture of two isomers comprising the [mu3:eta1] and [mu 3:eta2] forms of the triply bridging propionate group. The reaction of [Mn4O3(O2CR) 4(dbm)3] (R = Me, Et) with trimethylsilyl acetamide results in the formation of [Mn4O3(OSiMe3)(O 2CR)3(dbm)3] (R = Me, Et). These complexes possess crystallographic C3 symmetry, and thus represent the first axially symmetric cubane complexes with dbm- ligands. The crystal structure of these complexes indicates the presence of solvent molecules of crystallization.
520 $a In the area of bioinorganic chemistry, a series of complexes possessing the previously unknown [Mn3O4]4+ core have been synthesized and isolated for the first time. These complexes are [Mn3O4(O2CMe)4(bpy)2] (bpy = 2,2'-bipyridine) and [Mn3O4(O 2CR)2Cl2(bpy)2] (R = Me, Et). The incorporation of Cl- in the latter series of complexes is a significant development as this ion is a cofactor of the WOC. (Abstract shortened by UMI.)
590 $a School code: 0093.
650 4 $a Chemistry, Inorganic. $3 517253
690 $a 0488
710 2 0 $a Indiana University. $3 960096
773 0 $t Dissertation Abstracts International $g 63-12B.
790 1 0 $a Christou, George, $e advisor
790 $a 0093
791 $a Ph.D.
792 $a 2002
856 4 0 $u http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3075932