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Development Of Nickelii Complexes Of Oxime Containing Ligands For The Activation Of Dioxygen
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Book Synopsis Development of Nickel(II) Complexes of Oxime Containing Ligands for the Activation of Dioxygen by : Michael Joseph Goldcamp
Download or read book Development of Nickel(II) Complexes of Oxime Containing Ligands for the Activation of Dioxygen written by Michael Joseph Goldcamp and published by . This book was released on 2002 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: Ligands containing two oxime donor groups with a variable third group in a tripodal amine motif have been designed and synthesized. Their Ni(II) complexes, and some Zn(II), Cu(II), and Fe(III) complexes, have been structurally and spectroscopically characterized. Deprotonation of the oxime groups gives Ni(II)--Polyoximate complexes that form bis(N-O) oximate bridged dimers with significantly low oxidation potentials for Ni(II). These Ni(II)-polyoximate complexes react with dioxygen, consuming multiple equivalents. This is unusual chemistry for Ni(II), especially in the absence of ligand oxidation. The Ni(II) / O 2 reaction system promotes oxidation of triphenyl phosphine, with oxygen atom transfer, benzyl alcohol, and 3,5-di-tert-butylcatechol. Reaction of the Ni(II)-polyoximate complexes with o-quinones causes the formation of high-valent nickel complexes of the reduced dioxolenes, semiquinones and catecholates.
Book Synopsis Invesitgation of Nickel(II)-oximate Complexes that React with Molecular Oxygen by :
Download or read book Invesitgation of Nickel(II)-oximate Complexes that React with Molecular Oxygen written by and published by . This book was released on 2004 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: 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)สบ (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.
Book Synopsis American Doctoral Dissertations by :
Download or read book American Doctoral Dissertations written by and published by . This book was released on 2002 with total page 776 pages. Available in PDF, EPUB and Kindle. Book excerpt:
Book Synopsis Novel Dinucleating Poly(oxime) Amine Ligands and Their Nickel and Zinc Complexes by : Elizabeth Ann Deters
Download or read book Novel Dinucleating Poly(oxime) Amine Ligands and Their Nickel and Zinc Complexes written by Elizabeth Ann Deters and published by . This book was released on 2007 with total page 120 pages. Available in PDF, EPUB and Kindle. Book excerpt: A series of mononuclear poly(oxime) amine nickel(II) complexes has been shown to catalyze the oxidation of various substances. To further this work, a series of novel dinucleating ploy(oxime) amine ligands and their nickel complexes were synthesized. During this synthesis, a novel anion dependence on the nuclearity of the complex was discovered and investigated for two of the ligands. All of the dinuclear complexes were shown to catalyze the oxidation of various substances, including methanol, benzyl alcohol, and benzylamine. In addition to the oxygen reactivity, zinc complexes of the poly(oxime) amine ligands were shown to have hydrolysis reactivity. These complexes successfully catalyzed the hydrolysis of p-nitrophenyl acetate. Some preliminary kinetic data for the reaction was also obtained.
Book Synopsis Dissertation Abstracts International by :
Download or read book Dissertation Abstracts International written by and published by . This book was released on 2006 with total page 854 pages. Available in PDF, EPUB and Kindle. Book excerpt:
Book Synopsis Dioxygen Activation with Bis(arylimino)pyridine Radical Anion Complexes of Nickel by : Antonio David Manuel
Download or read book Dioxygen Activation with Bis(arylimino)pyridine Radical Anion Complexes of Nickel written by Antonio David Manuel and published by . This book was released on 2014 with total page 111 pages. Available in PDF, EPUB and Kindle. Book excerpt: The half-life of the reaction was not affected by deuterium labeling of the acetimino methyl groups but was affected by different substituents in the 4-position of the phenyl groups of the ligand. The reactions caused intraligand C-C bond cleavage with formation of a new C=O double bond, resulting in the complexes [Ni{6-(ArN=CMe)C5H3N-2-C(O)NAr}Cl] (where Ar = 4-X-2,6-iPr2C6H2 and X = H, Cl, or Br) and [Ni{6-(ArN=CCD3)C5H3N-2-C(O)NAr}Cl](where Ar = 2,6-iPr2C6H3). The structures of the complexes [Ni{6-(ArN=CR)C5H3N-2-C(O)NAr}Cl] (where Ar = 2,6-iPr2C6H3 and R = CH3 or CD3) were determined by X-ray crystallography. For all four complexes, the carboxamidato group was identified by a strong band in the infrared spectra assignable to the CO stretching vibration. Furthermore, the new carboxamidato ligands were removed from the metal center and isolated in their neutral form as 6-(ArN=CMe)C5H3N-2-C(O)NHAr (where Ar = 4-X-2,6-iPr2C6H2 and X = H, Cl, or Br) and 6-(ArN=CCD3)C5H3N-2-C(O)NHAr(where Ar = 2,6-iPr2C6H3). Taken together, these results indicate that the activation of dioxygen occurs at the ligand and without an overall oxidation state change at the Ni center. The observed ligand-centered oxygenation in these reactions contrasts with the prevailing metal-centered chemistry of redox-active bis(arylimino)pyridine complexes and demonstrates that they can be directly involved in the activation and conversion of a small molecule.
Book Synopsis Dioxygen Activation by Thiolate Ligated Complexes with Tunable Pi-acceptor N-heterocyclic Ligands by : Chaau Yan Poon
Download or read book Dioxygen Activation by Thiolate Ligated Complexes with Tunable Pi-acceptor N-heterocyclic Ligands written by Chaau Yan Poon and published by . This book was released on 2021 with total page 227 pages. Available in PDF, EPUB and Kindle. Book excerpt: Dioxygen reduction and water oxidation are critical processes for aerobic life. Developing a better understanding of O-O bond activation and formation mechanisms mediated by metalloenzymes involving first-row transition metals such as Fe and Mn, would provide valuable insights for catalyst and drug development. While synthetic iron and copper oxo species generated from O2 have been extensively studied, the process of manganese dioxygen activation and its intermediates is comparatively unexplored. This dissertation focuses on the synthesis, characterization, and dioxygen reactivity of structurally analogous Mn- and Fe-thiolate complexes with tunable N-heterocyclic amine ligands. Chapter one provides an introduction to oxygen-evolving and oxygen-dependent metalloenzymes containing Mn and Fe metallocofactors. Chapter two highlights how metal ion Lewis acidity and steric properties influence the kinetics and thermodynamics of O2 activation by a series of structurally analogous Mn-thiolate complexes. A total of four high-valent Mn-oxo intermediates were observed along the O2 activation pathway, including MnIIIMnIV(m-oxo)(m-OH) intermediates. Chapter three covers the hydrogen atom transfer activity by the MnIIIMnIV(mu-oxo)(mu-OH) intermediate characterized in chapter two. Chapter four focuses on the synthesis, characterization, and preliminary O2 reactivity of Fe-thiolate complexes that possess a tunable N-heterocyclic amine, wherein a less Lewis acidic FeII species within the structurally analogous series led to the observation of a new O2 activation intermediate. Chapter five discusses the comparison between the structures and reactivities of alkoxide- and thiolate-ligated Mn alkylperoxo species with otherwise identical ligand frameworks, which demonstrates key insight into how the primary coordination sphere of active sites could alter their reactivity.
Book Synopsis Nickel (II) Complexes with Four Oxygen and Sulfur Containing Ligands by : Frederick W. Nieske
Download or read book Nickel (II) Complexes with Four Oxygen and Sulfur Containing Ligands written by Frederick W. Nieske and published by . This book was released on 1971 with total page 110 pages. Available in PDF, EPUB and Kindle. Book excerpt:
Book Synopsis Macrocycle Ligand Modifications in the Pursuit of Nickel-oxygen Complexes by : Joliene Renee Trujillo
Download or read book Macrocycle Ligand Modifications in the Pursuit of Nickel-oxygen Complexes written by Joliene Renee Trujillo and published by . This book was released on 2010 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: The utility of small molecules lies in the ability to alter the structure of the molecule and examine the spectroscopic characteristics as well as the reactivity of the complex. Small molecules are often used to probe mechanistic questions on much more complicated systems, such as enzymes. In 1996 a new form of superoxide dismutase was discovered which had nickel in the active site of the enzyme. This discovery sparked renewed interest in nickel-oxygen chemistry. Small molecules were used to probe different nickel-oxygen structure types and their spectroscopic characteristics, though complete understanding of the implications when altering the small molecules has yet to develop. This thesis addresses macrocycle ligand modifications, the varying ways of synthesizing nickel-oxygen complexes, and the reactivity of the nickel-oxygen adducts with exogenous substrates. The work presented herein, describes the synthesis and characterization of [Ni(tmcyclen)(CO)](OTf). Subsequent oxygen activation by [Ni(tmcyclen)(CO)](OTf) lead to the formation of "side-on" nickel(III) peroxo complex as determined by electronic absorption spectroscopy, electron paramagnetic resonance spectroscopy, and mass spectroscopy. Alternatively, the complex can be synthesized from nickel(II) and reduced oxygen reagents, H2O2 or KO2. Reactivity studies of the [Ni(tmcyclen)(O2)](OTf) with phosphines, sulfides, olefins, activated CH bonds, and substituted phenols were investigated. The reactivity studies completed on the "side-on" nickel(III)-peroxo complex shed light on the electronic characteristics of the complex. This thesis represents the first time a "side-on" nickel(III)-peroxo complex is synthesized from monovalent nickel and dioxygen.
Download or read book Index Medicus written by and published by . This book was released on 2003 with total page 2102 pages. Available in PDF, EPUB and Kindle. Book excerpt: Vols. for 1963- include as pt. 2 of the Jan. issue: Medical subject headings.
Download or read book Chemical Abstracts written by and published by . This book was released on 2002 with total page 2626 pages. Available in PDF, EPUB and Kindle. Book excerpt:
Book Synopsis Directory of Graduate Research by : American Chemical Society. Committee on Professional Training
Download or read book Directory of Graduate Research written by American Chemical Society. Committee on Professional Training and published by . This book was released on 2005 with total page 1932 pages. Available in PDF, EPUB and Kindle. Book excerpt: Faculties, publications and doctoral theses in departments or divisions of chemistry, chemical engineering, biochemistry and pharmaceutical and/or medicinal chemistry at universities in the United States and Canada.
Download or read book Indian Science Abstracts written by and published by . This book was released on 2002-11 with total page 876 pages. Available in PDF, EPUB and Kindle. Book excerpt:
Download or read book Energy Research Abstracts written by and published by . This book was released on 1988 with total page 784 pages. Available in PDF, EPUB and Kindle. Book excerpt:
Book Synopsis Nickel Catalysis in Organic Synthesis by : Sensuke Ogoshi
Download or read book Nickel Catalysis in Organic Synthesis written by Sensuke Ogoshi and published by John Wiley & Sons. This book was released on 2020-03-09 with total page 348 pages. Available in PDF, EPUB and Kindle. Book excerpt: A comprehensive reference to nickel chemistry for every scientist working with organometallic catalysts Written by one of the world?s leading reseachers in the field, Nickel Catalysis in Organic Synthesis presents a comprehensive review of the high potential of modern nickel catalysis and its application in synthesis. Structured in a clear and assessible manner, the book offers a collection of various reaction types, such as cross-coupling reactions, reactions for the activation of unreactive bonds, carbon dioxide fixation, and many more. Nickel has been recognized as one of the most interesting transition metals for homogeneous catalysis. This book offers an overview to the recently developed new ligands, new reaction conditions, and new apparatus to control the reactivity of nickel catalysts, allowing scientists to apply nickel catalysts to a variety of bond-forming reactions. A must-read for anyone working with organometallic compounds and their application in organic synthesis, this important guide: -Reviews the numerous applications of nickel catalysis in synthesis -Explores the use of nickel as a relatively cheap and earth-abundant metal -Examines the versatility of nickel catalysis in reactions like cross-coupling reactions and CH activations -Offers a resource for academics and industry professionals Written for catalytic chemists, organic chemists, inorganic chemists, structural chemists, and chemists in industry, Nickel Catalysis in Organic Synthesis provides a much-needed overview of the most recent developments in modern nickel catalysis and its application in synthesis.
Book Synopsis Index to Theses with Abstracts Accepted for Higher Degrees by the Universities of Great Britain and Ireland and the Council for National Academic Awards by :
Download or read book Index to Theses with Abstracts Accepted for Higher Degrees by the Universities of Great Britain and Ireland and the Council for National Academic Awards written by and published by . This book was released on 2001 with total page 372 pages. Available in PDF, EPUB and Kindle. Book excerpt: Theses on any subject submitted by the academic libraries in the UK and Ireland.
Book Synopsis Molybdenum and Tungsten Enzymes by : Russ Hille
Download or read book Molybdenum and Tungsten Enzymes written by Russ Hille and published by Royal Society of Chemistry. This book was released on 2016-10-10 with total page 341 pages. Available in PDF, EPUB and Kindle. Book excerpt: There has been enormous progress in our understanding of molybdenum and tungsten enzymes and relevant inorganic complexes of molybdenum and tungsten over the past twenty years. This set of three books provides a timely and comprehensive overview of the field and documents the latest research. Building on the first and second volumes that focussed on biochemistry and bioinorganic chemistry aspects, the third volume focusses on spectroscopic and computational methods that have been applied to both enzymes and model compounds. A particular emphasis is placed on how these important studies have been used to reveal critical components of enzyme mechanisms. This text will be a valuable reference to workers both inside and outside the field, including graduate students and young investigators interested in developing new research programs in this area.
