Invesitgation of Nickel(II)-oximate Complexes that React with Molecular Oxygen PDF Download
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Languages : en
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Ni(II) complexes containing amidates and thiolates have been shown to react with O2 via irreversible ligand oxidation. We have constructed a series of Ni(II) complexes based on a tripodal amine bis(oxime) ligand framework. These complexes display oxygen reactivity upon deprotonation of the oximes without requiring irreversible ligand oxidation. This project investigated the reaction involving one of the complexes in the library, [Ni(TRISOXH3)(NO3)(H2O)](NO3)ʺ (H2O), where TRISOXH3 = (tris(1-propan-2-onyl oxime)amine). It was discovered that the reaction of this complex with molecular oxygen is contingent upon the presence of a source of hydrogen atoms. This two-hydrogen atom donor acts as a substrate. Several primary alcohols, including the relatively inert methanol, and amines were catalytically oxidized by this reaction. Spectroscopic analysis using a variety of techniques has demonstrated that reversible oxidation occurs on the oximate nitrogen to form an iminoxyl radical. Many of the other complexes in the series were also investigated to examine their electronic structure, their electrochemical properties, and their ability to oxidize methanol.
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Languages : en
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Ni(II) complexes containing amidates and thiolates have been shown to react with O2 via irreversible ligand oxidation. We have constructed a series of Ni(II) complexes based on a tripodal amine bis(oxime) ligand framework. These complexes display oxygen reactivity upon deprotonation of the oximes without requiring irreversible ligand oxidation. This project investigated the reaction involving one of the complexes in the library, [Ni(TRISOXH3)(NO3)(H2O)](NO3)ʺ (H2O), where TRISOXH3 = (tris(1-propan-2-onyl oxime)amine). It was discovered that the reaction of this complex with molecular oxygen is contingent upon the presence of a source of hydrogen atoms. This two-hydrogen atom donor acts as a substrate. Several primary alcohols, including the relatively inert methanol, and amines were catalytically oxidized by this reaction. Spectroscopic analysis using a variety of techniques has demonstrated that reversible oxidation occurs on the oximate nitrogen to form an iminoxyl radical. Many of the other complexes in the series were also investigated to examine their electronic structure, their electrochemical properties, and their ability to oxidize methanol.
Author: Ronelito Josue Perez
Publisher:
ISBN:
Category : Complex compounds
Languages : en
Pages : 130
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Author: Margo Nicole Montgomery
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Category :
Languages : en
Pages : 288
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This research presents an investigation of synthetic model complexes with relevance to the active site of Ni(II) acireductone dioxygenase (Ni-ARD) and Ni(II) superoxide dismutase (Ni-SOD). Acireductone dioxygenases (ARDs) are a unique set of enzymes found in the methionine salvage pathway that catalyze the oxidation reaction of acireductone (1, 2-dihydroxy-3-oxo-5-(methylthio)pent-1-ene). These enzymes share a common polypeptide sequence but bind different metal ions, Ni 2+ or Fe2+, at the active site. The Ni-ARD enzyme is responsible for the off pathway shunt in the pathway. Using the tridentate nitrogen donor ligands hydrotris(3,5-dimethyl-1-pyrazolyl)borate (Tp*) and the newly developed tris(1, 2-dimethyl-4-imadozyl)carbinol, (4-TIC Me, Me) several reactions involving the acireductone analog 2-hydroxy-1, 3-diphenylpropan-1, 3-dione and O2 were investigated for similarities to the Ni-ARD active site. Superoxide dismutases (SODs) play a key role in protecting cells against oxidative damage by regulating the cellular concentration of the superoxide radical (O2.- ) which is an unwanted byproduct of cellular metabolism. This process is accomplished by converting the superoxide radicals to hydrogen peroxide and molecular oxygen. Several small-molecule complexes were synthesized and characterized in an effort to model the reduced state of the Ni-SOD using the Tp* ligand. The structures for these complexes have been determined using X-Ray Crystallography.
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Category :
Languages : en
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Author:
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Category : Nuclear energy
Languages : en
Pages : 1132
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Author: Denver Heitger
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Category :
Languages : en
Pages :
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Metal complexes that can activate natural oxidants like H2O2 and O2 have become a key research topic in many labs in hope of mimicking nature, by generating a bioinspired complex that can perform unique chemistry through green processes. To prepare the perfect catalyst, this has lead scientists to explore numerous avenues, including the use of both natural and artificial oxidants, to tease apart the reaction pathway taking place. A ligand system dear to the Lucas Lab (13-DOB) has been metalated with nickel, a cheap and earth abundant transition metal. Our bioinspired metal-(di)oxygen adducts can be formed from H2O2, O2, mCPBA, and PhIO.
Author: Chemical Society (Great Britain)
Publisher:
ISBN:
Category : Chemistry
Languages : en
Pages : 1020
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Author: Kenneth D. Karlin
Publisher: John Wiley & Sons
ISBN: 1118870166
Category : Science
Languages : en
Pages : 594
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This series provides inorganic chemists and materials scientists with a forum for critical, authoritative evaluations of advances in every area of the discipline. Volume 59 continues to report recent advances with a significant, up-to-date selection of contributions by internationally-recognized researchers. The chapters of this volume are devoted to the following topics: • Iron Catalysis in Synthetic Chemistry • A New Paradigm for Photodynamic Therapy Drug Design: Multifunctional, Supramolecular DNA Photomodification Agents Featuring Ru(II)/Os(II) Light Absorbers Coupled to Pt(II) or Rh(III) Bioactive Sites • Selective Binding of Zn2+ Complexes to Non-Canonical Thymine or Uracil in DNA or RNA. • Progress Toward the Electrocatalytic Production of Liquid Fuels from Carbon Dioxide • Monomeric Dinitrosyl Iron Complexes: Synthesis and Reactivity • Interactions of Nitrosoalkanes/arenes, Nitrosamines, Nitrosothiols, and Alkyl Nitrites with Metals • Aminopyridine Iron and Manganese Complexes as Molecular Catalysts for Challenging Oxidative Transformations
Author:
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Category : Aeronautics
Languages : en
Pages : 1282
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Lists citations with abstracts for aerospace related reports obtained from world wide sources and announces documents that have recently been entered into the NASA Scientific and Technical Information Database.
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Category : Nuclear energy
Languages : en
Pages : 506
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