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Reactivity Studies of Group Six and ...

Navarro, David Matthew,

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Reactivity Studies of Group Six and Ten Transition Metal Complexes Containing Redox-Active Ligands /

Record Type:	Electronic resources : Monograph/item
Title/Author:	Reactivity Studies of Group Six and Ten Transition Metal Complexes Containing Redox-Active Ligands // David Matthew Navarro.
Author:	Navarro, David Matthew,
Description:	1 electronic resource (626 pages)
Notes:	Source: Dissertations Abstracts International, Volume: 86-08, Section: B.
Contained By:	Dissertations Abstracts International86-08B.
Subject:	Chemistry. -
Online resource:	https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=31633036
ISBN:	9798302853837

Reactivity Studies of Group Six and Ten Transition Metal Complexes Containing Redox-Active Ligands /
Navarro, David Matthew,

Reactivity Studies of Group Six and Ten Transition Metal Complexes Containing Redox-Active Ligands /David Matthew Navarro. - 1 electronic resource (626 pages)

Source: Dissertations Abstracts International, Volume: 86-08, Section: B.

This dissertation focuses on understanding the propensity of group 6 and 10 transition metal complexes with multiple redox and proton non-innocent ligands to serve as proton and electron transfer agents.Chapter 2 presents data from the study of (RapH)Pt(•bpytBu), which was of interest as a potential hydride donor. It was found that hydrogen generation was favorable, and the complex favored a one-electron hydrogen evolution pathway due to the mismatch reduction potentials of the ligands. The chapter also studies the effects that changing the para-subtituent on the phenyl group of the amidophenolate ligand has on the thermodynamics of the system.Chapter 3, a novel platinum complex (Hisq•)Pt(sq•) with two redox-active ligands of similar redox properties was generated to circumvent this issue. This complex did favor two electron reactivity as it was tested for its ability to transfer hydrides. It acted as a hydride donor in the reaction of the platinum complex (HapH)Pt(cat)- and trityl cation. The neutral species (Hisq•)Pt(sq•) was reacted with isopropanol and sodium formate and the oxidation of isopropanol was catalytic. The redox processes centered on the catecholate ligand made the complex a better hydride acceptor than donor.Chapter 4 investigates nickel complexes containing bis-amidophenolate ligands to generate complexes that favor hydride donation. [K][(Rap)Ni(RapH)] was reactive towards carbon dioxide but did proceed through a hydride pathway. This was further confirmed as [K2][Ni(Rap)2] also reacted with carbon dioxide to generate carbonate. The study also focuses on the para-substituent of the phenyl groups of the amidophenolate ligand and how modifications to the groups can change the thermodynamics of the complex.Chapter 5 investigates the reactivity of new tungsten complexes containing two amidophenolate ligands. Salt metathesis is performed with W(Hap)2(Cl)2 to generate a slew of different tungsten complexes. The reaction of the complex with phenyl lithium leads to the generation of biphenyl, but the complex does not proceed through a reductive elimination path. This mechanism is studied through the use of different tungsten complexes and substates.

English

ISBN: 9798302853837Subjects--Topical Terms:

516420
Chemistry.
Subjects--Index Terms:

Metal complexes

Reactivity Studies of Group Six and Ten Transition Metal Complexes Containing Redox-Active Ligands /
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520 $a This dissertation focuses on understanding the propensity of group 6 and 10 transition metal complexes with multiple redox and proton non-innocent ligands to serve as proton and electron transfer agents.Chapter 2 presents data from the study of (RapH)Pt(•bpytBu), which was of interest as a potential hydride donor. It was found that hydrogen generation was favorable, and the complex favored a one-electron hydrogen evolution pathway due to the mismatch reduction potentials of the ligands. The chapter also studies the effects that changing the para-subtituent on the phenyl group of the amidophenolate ligand has on the thermodynamics of the system.Chapter 3, a novel platinum complex (Hisq•)Pt(sq•) with two redox-active ligands of similar redox properties was generated to circumvent this issue. This complex did favor two electron reactivity as it was tested for its ability to transfer hydrides. It acted as a hydride donor in the reaction of the platinum complex (HapH)Pt(cat)- and trityl cation. The neutral species (Hisq•)Pt(sq•) was reacted with isopropanol and sodium formate and the oxidation of isopropanol was catalytic. The redox processes centered on the catecholate ligand made the complex a better hydride acceptor than donor.Chapter 4 investigates nickel complexes containing bis-amidophenolate ligands to generate complexes that favor hydride donation. [K][(Rap)Ni(RapH)] was reactive towards carbon dioxide but did proceed through a hydride pathway. This was further confirmed as [K2][Ni(Rap)2] also reacted with carbon dioxide to generate carbonate. The study also focuses on the para-substituent of the phenyl groups of the amidophenolate ligand and how modifications to the groups can change the thermodynamics of the complex.Chapter 5 investigates the reactivity of new tungsten complexes containing two amidophenolate ligands. Salt metathesis is performed with W(Hap)2(Cl)2 to generate a slew of different tungsten complexes. The reaction of the complex with phenyl lithium leads to the generation of biphenyl, but the complex does not proceed through a reductive elimination path. This mechanism is studied through the use of different tungsten complexes and substates.
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