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Macrocyclic amides as platforms for ...

Korendovych, Ivan Victorovych.

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Macrocyclic amides as platforms for oxygen activation and anion recognition.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Macrocyclic amides as platforms for oxygen activation and anion recognition./
Author:	Korendovych, Ivan Victorovych.
Description:	525 p.
Notes:	Source: Dissertation Abstracts International, Volume: 67-08, Section: B, page: 4417.
Contained By:	Dissertation Abstracts International67-08B.
Subject:	Inorganic chemistry. -
Online resource:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3232132
ISBN:	9780542848247

Macrocyclic amides as platforms for oxygen activation and anion recognition.
Korendovych, Ivan Victorovych.

Macrocyclic amides as platforms for oxygen activation and anion recognition. - 525 p.

Source: Dissertation Abstracts International, Volume: 67-08, Section: B, page: 4417.

Thesis (Ph.D.)--Tufts University, 2006.

A new, stable iron(III) complex with a pentadentate amide-containing macrocyclic ligand H2pydioneN5 was prepared and fully characterized. The coordination of deprotonated amide groups resulted in stabilization of a high oxidation state of iron. In contrast to the majority of the iron complexes with polydentate amide ligands, the pentagonal-bipyramidal geometry of the macrocyclic complex affords a high-spin configuration of the metal ion. Iron-57 Mossbauer spectroscopy and ac and dc magnetization studies indicate slow paramagnetic relaxation and a crossover to long range antiferromagnetic order at T < &sim;3.2 K.

ISBN: 9780542848247Subjects--Topical Terms:

3173556
Inorganic chemistry.

Macrocyclic amides as platforms for oxygen activation and anion recognition.
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020 $a 9780542848247
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100 1 $a Korendovych, Ivan Victorovych. $3 3178766
245 1 0 $a Macrocyclic amides as platforms for oxygen activation and anion recognition.
300 $a 525 p.
500 $a Source: Dissertation Abstracts International, Volume: 67-08, Section: B, page: 4417.
500 $a Adviser: Elena V. Rybak-Akimova.
502 $a Thesis (Ph.D.)--Tufts University, 2006.
520 $a A new, stable iron(III) complex with a pentadentate amide-containing macrocyclic ligand H2pydioneN5 was prepared and fully characterized. The coordination of deprotonated amide groups resulted in stabilization of a high oxidation state of iron. In contrast to the majority of the iron complexes with polydentate amide ligands, the pentagonal-bipyramidal geometry of the macrocyclic complex affords a high-spin configuration of the metal ion. Iron-57 Mossbauer spectroscopy and ac and dc magnetization studies indicate slow paramagnetic relaxation and a crossover to long range antiferromagnetic order at T < &sim;3.2 K.
520 $a Iron(II) complexes of H2pydioneN5 and H2pyCldioneN 5 were also fully characterized. Complexes with one and two deprotonated amide groups can both be obtained. Detailed kinetic studies of oxygenation of the iron(II) complexes showed that the deprotonation state of the complex has a profound effect on the reactivity. Oxygenation of Fe(pydioneN5 ) in aprotic solvents proceeds via a iron(III) superoxo and diiron(III) peroxo species (that can be stabilized by 1-methylimidazole) yielding iron(III) mu-oxo dimers. The presence of an accessible proton in Fe(HpydioneN5)(Cl) proves sufficient to alter the oxygenation pathway. The new amidopyridine macrocycles can be considered as new members of the "expanded porphyrin analog" family providing control over the spin state and availability of protons as well as allowing for easy synthetic modifications, paving the way to new versatile metal complexes.
520 $a We have also synthesized a diiron(II) complex with a novel aqua-hydroxo bridging motif, [Fe2(mu-H2O)(mu-OH)(TPA)2](OTf) 3. This is a new member of the diiron diamond core family. The drastic difference of ca. 1 V in redox potential between complex [Fe2(mu-H2O)(mu-OH)(TPA)2](OTf) 3 and its bis-hydroxo bridged analog Fe2(OH)2(TPA) 3+ is accompanied by only moderate difference in dioxygen reactivity which is consistent with the inner-sphere mechanism of iron(II)-dioxygen association rather than the outer-sphere electron transfer.
520 $a Binding of inorganic anions as well as carboxylic acids and tetraalkylammonium carboxylates by macrocyclic compounds of different size was studied by NMR in d6-DMSO. It has been shown that for successful recognition of fluoride at least a 15-membered ring is necessary. The 30-membered macrocycle 4 has been shown to selectively bind dicarboxylic acid based on size and shape complimentarity. Macrocycle 4m showed selectivity toward alpha-ketocarboxylic acids.
590 $a School code: 0234.
650 4 $a Inorganic chemistry. $3 3173556
650 4 $a Organic chemistry. $3 523952
650 4 $a Biochemistry. $3 518028
690 $a 0488
690 $a 0490
690 $a 0487
710 2 $a Tufts University. $3 1017847
773 0 $t Dissertation Abstracts International $g 67-08B.
790 $a 0234
791 $a Ph.D.
792 $a 2006
793 $a English
856 4 0 $u http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3232132