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Synthesis and properties of high-spi...

Aromi, Guillem.

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Synthesis and properties of high-spin manganese clusters.

紀錄類型:	書目-電子資源 : Monograph/item
正題名/作者:	Synthesis and properties of high-spin manganese clusters./
作者:	Aromi, Guillem.
面頁冊數:	363 p.
附註:	Source: Dissertation Abstracts International, Volume: 61-02, Section: B, page: 0848.
Contained By:	Dissertation Abstracts International61-02B.
標題:	Chemistry, Inorganic. -
電子資源:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=9962757
ISBN:	0599668571

Synthesis and properties of high-spin manganese clusters.
Aromi, Guillem.

Synthesis and properties of high-spin manganese clusters. - 363 p.

Source: Dissertation Abstracts International, Volume: 61-02, Section: B, page: 0848.

Thesis (Ph.D.)--Indiana University, 2000.

Many crucial enzymes in Nature require manganese for proper functioning. Photosystem II (PSII), which catalyzes the formation of atmospheric oxygen from water, is perhaps the most important example. This reaction takes place at the water oxidation complex (WOC), which is a tetranuclear manganese oxo-aggregate whose exact structure is not known to date. Manganese plays also a privileged role in the rapidly evolving field of molecule-based magnetic materials owing to its tendency to form molecular aggregates with high-spin ground states. This work focuses on the preparation of new tetranuclear manganese clusters as potential models for the WOC, and the study of the interaction of these complexes with small species important to the enzyme. Synthesis of novel multinuclear manganese aggregates has also been sought because of their interesting magnetic properties.

ISBN: 0599668571Subjects--Topical Terms:

517253
Chemistry, Inorganic.

Synthesis and properties of high-spin manganese clusters.
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500 $a Source: Dissertation Abstracts International, Volume: 61-02, Section: B, page: 0848.
500 $a Adviser: George Christou.
502 $a Thesis (Ph.D.)--Indiana University, 2000.
520 $a Many crucial enzymes in Nature require manganese for proper functioning. Photosystem II (PSII), which catalyzes the formation of atmospheric oxygen from water, is perhaps the most important example. This reaction takes place at the water oxidation complex (WOC), which is a tetranuclear manganese oxo-aggregate whose exact structure is not known to date. Manganese plays also a privileged role in the rapidly evolving field of molecule-based magnetic materials owing to its tendency to form molecular aggregates with high-spin ground states. This work focuses on the preparation of new tetranuclear manganese clusters as potential models for the WOC, and the study of the interaction of these complexes with small species important to the enzyme. Synthesis of novel multinuclear manganese aggregates has also been sought because of their interesting magnetic properties.
520 $a A new methodology for the preparation of distorted cubane complexes with a [Mn4O3X]6+ core has been developed. In this route, the acidolysis of [Mn4O3(OAc)4(dbm) 3] or [Mn4O2(O2CEt)6(dbm) 2] with mineral acids of the type HX has led to the formation of the tetranuclear complexes with X--=F--, Cl--, Br-- and NO3 --. Of these, the nitrate-bound complex is a new compound and displays an unprecedented eta1:mu3-- NO3-- binding mode.
520 $a The reactivity of [Mn4O3(OAc)4(R 2dbm)3] (R=H, Me) with alcohols has been explored and this effort has led to the preparation of the array of new complexes [Mn4 O3(OR')(OAc)3(R2dbm) 3] (R'=Me, Et). The mu3-OR ' ligands in these complexes act as good leaving groups in metathesis reactions via protonation by weak acids. Thus, the incorporation of phenoxide ligands (as models for a tyrosine residue) into the manganese cluster has been achieved with the isolation of a family of compounds with the [Mn 4(mu3-O)3(mu3-OR)]6+ (R=Ph, C6H4-p-Me) core. This group of molecules has also very similar properties to the related clusters previously studied except for a very distinct electrochemical behavior, presumably caused by the redox activity of the phenoxide ligands. In a similar manner, hydrolysis of [Mn4O3(OMe)(OAc)3(dbm)3] has given rise to the new complex [Mn4O3(OH)(OAc)3 (dbm)3] in a transformation that models the activation of water by the enzyme via deprotonation and incorporation into a manganese cluster.
520 $a In related work, the new class of hexanuclear manganese complexes with formula [Mn6O4X4(R2dbm)6 ] (X--=Cl--, Br-- ; R=Me, Et) has been accessed from the slow hydrolysis of the corresponding five-coordinate mononuclear species [MnX(R2dbm)2]. The new clusters are highly symmetric (Td) and display an ST=12 spin ground state.
590 $a School code: 0093.
650 4 $a Chemistry, Inorganic. $3 517253
650 4 $a Chemistry, Biochemistry. $3 1017722
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710 2 0 $a Indiana University. $3 960096
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