Molybdenum and Tungsten Complexes of Dinitrogen, CO, and Isocyanides that Contain Aryl-substituted Triamidoamine Ligands PDF Download
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Author: George Emil Greco
Publisher:
ISBN:
Category :
Languages : en
Pages : 498
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Author: George Emil Greco
Publisher:
ISBN:
Category :
Languages : en
Pages : 498
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Author: Jia Min Chin
Publisher:
ISBN:
Category :
Languages : en
Pages : 188
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A series of monopyrroletriamine ligands [Arpyr(Ar')2]H3 of the form ArC4H2NHCH2N(CH2CH2NHAr')2 (Ar = 2,4,6-mesityl (Mes), 2,4,6-triisopropylphenyl (TRIP); Ar' = C6F5, 2-tolyl (o-tol), naphthyl, 3,5-(2,4,6-triisopropylphenyl)phenyl (HIPT), 3,5- dimethylphenyl, 3,5-di-tert-butylphenyl were synthesized. [Mespyr(C6F5)2]MoCl, ([Mespyr(C6F5)2]Mo = MesitylC4H2NCH2N(CH2CH2NC6F5)2) was prepared by reaction of [Mespyr(C6F5)2]H3 with MoCl4(THF)2 and base and [Mespyr(3,5-t-Bu)2]MoCl and [Mespyr(3,5- Me)2]MoCl (3,5-t-Bu=3,5-di-tert-butylphenyl, Me = 3,5-dimethylphenyl) were synthesized likewise. All three monochlorides are paramagnetic. [Mespyr(C6F5)2]MoNMe2, [[Mespyr(otol) 2]MoNMe2, [Mespyr(3,5-t-Bu)2]MoNMe2, [Mespyr(3,5-Me)2]MoNMe2 were synthesized by reaction of the ligands with Mo(NMe2)4. The resulting compounds are diamagnetic and range in color from teal blue to emerald green. These low spin monodimethylamide complexes exist in rapid equilibria with their high spin forms. [Mespyr(C6F5)2]MoN and [Mespyr(3,5-t-Bu)2]MoN were synthesized by reaction of their respective monochlorides with NaN3 and are yellow diamagnetic species. Reaction of [Mespyr(3,5-t-Bu)2]MoN with Et3OBF4 leads to {[Mespyr(3,5- t-Bu)2]MoNEt}BF4, also a diamagnetic yellow species. [Mespyr(C6F5)2]MoOTf is synthesized by the reaction of [Mespyr(C6F5)2]MoCl with AgOTf. Reduction of [Mespyr(3,5-t-Bu)2]MoCl with Na under N2 led to [Mespyr(3,5-t-Bu)2]MoNNNa(THF)x, several species with varying numbers of THF coordination, x. A single species can be obtained when [Mespyr(3,5-t- Bu)2]MoNNNa(THF)x is reacted with either NBu4Cl or 15-crown-5 ether to yield purple green 4 {[Mespyr(3,5-t-Bu)2]MoNN}NBu4 or [Mespyr(3,5-t-Bu)2]MoNNNa(15-c-5). All the diazenide species are diamagnetic. Oxidation of the diazenide with AgOTf yields [Mespyr(3,5-t- Bu)2]Mo(N2). [Mespyr(3,5-t-Bu)2]Mo(CO) is synthesized by exposure of [Mespyr(3,5-t- Bu)2]Mo(N2) to CO. Reaction of [Mespyr(3,5-t-Bu)2]MoCl with NaBPh4 and NH3 yields {[Mespyr(3,5-t-Bu)2]Mo(NH3)}BPh4. Catalytic runs employing [Mespyr(3,5-t-Bu)2]MoN as the catalyst yielded one equivalent of NH3. A triamidoamine ligand [(HIPTNCH2CH2CH2)3N]3- was synthesized and metalated with MoCl4(THF)2 to produce [(HIPTNCH2CH2CH2)3N]MoCl ([HIPTtrpn]MoCl). Reduction of [HIPTtrpn]MoCl by KC8 under an atmosphere of dinitrogen leads to the green species [HIPTtrpn]MoNNK which can be oxidized by ZnCl2(dioxane) to produce [HIPTtrpn]Mo(N2). Other complexes synthesized include {[HIPTtrpn]Mo(NH3)}+ salts and [HIPTtrpn]Mo(CO). Xray studies were carried out on [HIPTtrpn]MoN and {[HIPTtrpn]Mo(NH3)}BAr'4. This system is not catalytic for the reduction of dinitrogen to ammonia and studies were carried out to elucidate the reasons. Oxidation studies were carried out on [HIPTN3N]Mo(N2) and [HIPTN3N]W(N2) ([HIPTN3N] = [(HIPTNCH2CH2)3N]3- ). The rate of conversion of [HIPTN3N]Mo(NH3) to [HIPTN3N]Mo(N2) was studied and found to be increased in the presence of BPh3. [HIPTN3N]Mo(N2) conversion to [HIPTN3N]Mo(CO) was found to be dependent on CO pressure. Protonation studies of [HIPTN3N]Mo(N2) were also carried out. Studies of [HIPTN3N]MoNNH decomposition showed that decomposition is not base-catalyzed. [HIPTN3N]W(CO) was synthesized by exposure of [HIPTN3N]W(N2) to CO. It is a green, paramagnetic compound and its use as a standard (for determining relative concentrations of other compounds in the IR sample) in IR spectroscopic studies appears to be promising. [HIPTN3N]MoCNH2 was synthesized by addition of acid and reducing agent to [HIPTN3N]MoCN and is a yellow, diamagnetic compound. Two triamidophosphine ligands, triHIPTamine and tri-n-Buamine were synthesized. Metalation of Zr(NMe2)4 with these ligands leads to formation of pn3HIPTZrNMe2 and pn3-n- BuZrNMe2, both diamagnetic, pale yellow complexes.
Author: Myra Brigid O'Donoghue
Publisher:
ISBN:
Category :
Languages : en
Pages : 356
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ISBN:
Category : Dissertations, Academic
Languages : en
Pages : 680
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ISBN:
Category : Dissertation abstracts
Languages : en
Pages : 816
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Author: Cole Seager
Publisher:
ISBN:
Category : Ligands
Languages : en
Pages : 58
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"A series of known and new seven coordinate molybdenum and tungsten complexes of tris(pyrazolyl)methane (Tpm) and substituted Tpm, [TpmM(CO)3X]+, have been synthesized. Depending on the identity of X, (bromo, iodo, hydrido) and the substitution of the Tpm ligand, substantial chemical shift differences are observed for the hydrogen on the central carbon of the Tpm ligand. Factors impacting the chemical shift of the hydrogen on the central carbon of the Tpm ligand, such as the electron donating ability of the Tpm ligand and the electronegativity of the additional ligand on the metal, will be discussed"--Unnumbered leaf 1.
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Category :
Languages : en
Pages :
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The aim of this work was to examine in closer detail the reduction of dinitrogen coordinated to molybdenum and tungsten and in particular the reactivity of hydrazido(2-) complexes. A brief introduction to nitrogen fixation is presented in Chapter 1 and chemical models of biological nitrogen fixation are discussed. The influence of ligand environment on the further reactions of hydrazido(2-) complexes is the subject of Chapter 2 whilst Chapter 3 describes the isolation of novel hydrido-, hydrazido(2-) complexes of tungsten and the X-ray structure of [WCl3(NNH2) - (PMe2Ph)2] Recent applications of 15 N nuclear magnetic resonance spectroscopy in coordination chemistry are reviewed in Chapter 4 introducing results of spectroscopic studies of 15N-labelled dinitrogen and hydrazido(2-) complexes. Attempts to prepare novel hydrazido(2-) complexes of tungsten are described in Chapter 5. A discussion of the results presented in Chapter's 2-5 is given in Chapter 6.
Author: H. M. Ali
Publisher:
ISBN:
Category :
Languages : en
Pages :
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Author: John K. Gibson
Publisher: John Wiley & Sons
ISBN: 1119115523
Category : Science
Languages : en
Pages : 534
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A review of contemporary actinide research that focuses on new advances in experiment and theory, and the interplay between these two realms Experimental and Theoretical Approaches to Actinide Chemistry offers a comprehensive review of the key aspects of actinide research. Written by noted experts in the field, the text includes information on new advances in experiment and theory and reveals the interplay between these two realms. The authors offer a multidisciplinary and multimodal approach to the nature of actinide chemistry, and explore the interplay between multiple experiments and theory, as well as between basic and applied actinide chemistry. The text covers the basic science used in contemporary studies of the actinide systems, from basic synthesis to state-of-the-art spectroscopic and computational techniques. The authors provide contemporary overviews of each topic area presented and describe the current and anticipated experimental approaches for the field, as well as the current and future computational chemistry and materials techniques. In addition, the authors explore the combination of experiment and theory. This important resource: Provides an essential resource the reviews the key aspects of contemporary actinide research Includes information on new advances in experiment and theory, and the interplay between the two Covers the basic science used in contemporary studies of the actinide systems, from basic synthesis to state-of-the-art spectroscopic and computational techniques Focuses on the interplay between multiple experiments and theory, as well as between basic and applied actinide chemistry Written for academics, students, professionals and researchers, this vital text contains a thorough review of the key aspects of actinide research and explores the most recent advances in experiment and theory.
Author: Yoshiaki Nishibayashi
Publisher: John Wiley & Sons
ISBN: 352734425X
Category : Science
Languages : en
Pages : 496
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Book Description
A comprehensive book that explores nitrogen fixation by using transition metal-dinitrogen complexes Nitrogen fixation is one of the most prominent fields of research in chemistry. This book puts the focus on the development of catalytic ammonia formation from nitrogen gas under ambient reaction conditions that has been recently repowered by some research groups. With contributions from noted experts in the field, Transition Metal-Dinitrogen Complexes offers an important guide and comprehensive resource to the most recent research and developments on the topic of nitrogen fixation by using transition metal-dinitrogen. The book is filled with the information needed to understand the synthesis of transition metal-dinitrogen complexes and their reactivity. This important book: -Offers a resource for understanding nitrogen fixation chemistry that is essential for explosives, pharmaceuticals, dyes, and all forms of life -Includes the information needed for anyone interested in the field of nitrogen fixation by using transition metal-dinitrogen complexes -Contains state-of-the-art research on synthesis of transition metal-dinitrogen complexes and their reactivity in nitrogen fixation -Incorporates contributions from well-known specialists and experts with an editor who is an innovator in the field of dinitrogen chemistry Written for chemists and scientists with an interest in nitrogen fixation, Transition Metal-Dinitrogen Complexes is a must-have resource to the burgeoning field of nitrogen fixation by using transition metal-dinitrogen complexes.
