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Oxidative Studies in Decontamination and Water Oxidation Catalysis.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Oxidative Studies in Decontamination and Water Oxidation Catalysis./
Author:	Sullivan, Kevin P.
Published:	Ann Arbor : ProQuest Dissertations & Theses, : 2019,
Description:	201 p.
Notes:	Source: Dissertations Abstracts International, Volume: 81-08, Section: B.
Contained By:	Dissertations Abstracts International81-08B.
Subject:	Polymer chemistry. -
Online resource:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=27659860
ISBN:	9781392532263

Oxidative Studies in Decontamination and Water Oxidation Catalysis.
Sullivan, Kevin P.

Oxidative Studies in Decontamination and Water Oxidation Catalysis. - Ann Arbor : ProQuest Dissertations & Theses, 2019 - 201 p.

Source: Dissertations Abstracts International, Volume: 81-08, Section: B.

Thesis (Ph.D.)--Emory University, 2019.

This item is not available from ProQuest Dissertations & Theses.

Oxidation reactions are ubiquitous throughout our society. The development of oxidation catalysts has propelled the advancement of civilization and allowed for significant advancements in science and technology. However, the Earth is currently entering a period in which human activities are causing substantial damage both through chemical pollution and global warming resulting from production of greenhouse gasses. This work addresses issues related to both these concerns, by outlining efforts towards the development of oxidation catalysts in three systems relevant to mitigating the impacts of toxic or polluting chemicals. In the first, synthesis and characterization of a new class of organic/inorganic hybrid polymers composed of covalently-bound 1,3,5-benzenetricarboxamide linkers and anionic polyoxovanadate clusters with varying counter-cations is described. These materials form gels within seconds upon contact with polar aprotic organic liquids and catalyze the degradation of odorants and toxic molecules under mild conditions including aerobic oxidation of thiols, hydrogen peroxide-catalyzed oxidation of sulfides, and hydrolysis of organophosphate chemical warfare agent analogues. The second project describes efforts towards the development of rapid aerobic oxidation catalysts for sulfoxidation reactions. Systems involving tetrabutylammonium tribromide and tetrabutylammonium nitrate are studied and optimized for catalyzing the aerobic oxidation of the mustard gas analogue 2-chloroethyl ethyl sulfide. The addition of Cu(II) to this system results in significant rate enhancements, as well as provides a detection capability by changing color in the presence of sulfides, followed by recovery of the original color when the sulfoxidation is complete. Finally, the third project described in this work details stability studies conducted on the water oxidation catalyst Na10[Co4(H2O)2(VW9O34)2] • 26 H2O. This polyoxometalate has been the subject of an ongoing debate regarding its stability under water oxidation catalysis conditions. Solution studies are examined clarifying the stability limitations in this system through 51V NMR resonance experiments on the polyoxometalate. The study demonstrates that the observed catalytic activity cannot be explained simply by Co(II)aq, but arises from multiple active water oxidation catalyst species in solution.

ISBN: 9781392532263Subjects--Topical Terms:

3173488
Polymer chemistry.
Subjects--Index Terms:

Kinetics

Oxidative Studies in Decontamination and Water Oxidation Catalysis.
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245 1 0 $a Oxidative Studies in Decontamination and Water Oxidation Catalysis.
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300 $a 201 p.
500 $a Source: Dissertations Abstracts International, Volume: 81-08, Section: B.
500 $a Advisor: Hill, Craig L.
502 $a Thesis (Ph.D.)--Emory University, 2019.
506 $a This item is not available from ProQuest Dissertations & Theses.
506 $a This item must not be sold to any third party vendors.
520 $a Oxidation reactions are ubiquitous throughout our society. The development of oxidation catalysts has propelled the advancement of civilization and allowed for significant advancements in science and technology. However, the Earth is currently entering a period in which human activities are causing substantial damage both through chemical pollution and global warming resulting from production of greenhouse gasses. This work addresses issues related to both these concerns, by outlining efforts towards the development of oxidation catalysts in three systems relevant to mitigating the impacts of toxic or polluting chemicals. In the first, synthesis and characterization of a new class of organic/inorganic hybrid polymers composed of covalently-bound 1,3,5-benzenetricarboxamide linkers and anionic polyoxovanadate clusters with varying counter-cations is described. These materials form gels within seconds upon contact with polar aprotic organic liquids and catalyze the degradation of odorants and toxic molecules under mild conditions including aerobic oxidation of thiols, hydrogen peroxide-catalyzed oxidation of sulfides, and hydrolysis of organophosphate chemical warfare agent analogues. The second project describes efforts towards the development of rapid aerobic oxidation catalysts for sulfoxidation reactions. Systems involving tetrabutylammonium tribromide and tetrabutylammonium nitrate are studied and optimized for catalyzing the aerobic oxidation of the mustard gas analogue 2-chloroethyl ethyl sulfide. The addition of Cu(II) to this system results in significant rate enhancements, as well as provides a detection capability by changing color in the presence of sulfides, followed by recovery of the original color when the sulfoxidation is complete. Finally, the third project described in this work details stability studies conducted on the water oxidation catalyst Na10[Co4(H2O)2(VW9O34)2] • 26 H2O. This polyoxometalate has been the subject of an ongoing debate regarding its stability under water oxidation catalysis conditions. Solution studies are examined clarifying the stability limitations in this system through 51V NMR resonance experiments on the polyoxometalate. The study demonstrates that the observed catalytic activity cannot be explained simply by Co(II)aq, but arises from multiple active water oxidation catalyst species in solution.
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650 4 $a Inorganic chemistry. $3 3173556
650 4 $a Analytical chemistry. $3 3168300
653 $a Kinetics
653 $a Polymers
653 $a Decontamination
653 $a Catalysis
653 $a Polyoxometalate
653 $a Water oxidation
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