Ammonia And Hydrazine Transition Metal Catalyzed Hydroamination And Metal Free Catalyzed Functionalization
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Ammonia And Hydrazine Transition Metal Catalyzed Hydroamination And Metal Free Catalyzed Functionalization
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Author :
language : en
Publisher:
Release Date : 2012
Ammonia And Hydrazine Transition Metal Catalyzed Hydroamination And Metal Free Catalyzed Functionalization written by and has been published by this book supported file pdf, txt, epub, kindle and other format this book has been release on 2012 with categories.
The efficient and selective preparation of organic molecules is critical for mankind. For the future, it is of paramount importance to find catalysts able to transform abundant and cheap feedstocks into useful compounds. Acyclic and heterocyclic nitrogen-containing derivatives are common components of naturally occurring compounds, agrochemicals, cosmetics, and pharmaceuticals; they are also useful intermediates in a number of industrial processes. One of the most widely used synthetic strategies, allowing the formation of an N-C bond, is the addition of an N-H bond across a carbon-carbon multiple bond, the so-called hydroamination reaction. This chemical transformation fulfills the principle of "green chemistry" since it ideally occurs with 100% atom economy. Various catalysts have been found to promote this reaction, although many limitations remain; one of the most prominent is the lack of methods that permit the use of NH3 and NH2NH2 as the amine partners. In fact, ammonia and hydrazine have rarely succumbed to homogeneous catalytic transformations. Considering the low cost and abundance of ammonia (136 million metric tons produced in 2011) and hydrazine, catalysts able to improve the reactivity and selectivity of the NH3- and NH2NH2-hydroamination reaction, and more broadly speaking the functionalization of these chemicals, are highly desirable. In the last funded period, we discovered the first homogeneous catalysts able to promote the hydroamination of alkynes and allenes with ammonia and the parent hydrazine. The key feature of our catalytic systems is that the formation of catalytically inactive Werner complexes is reversible, in marked contrast to most of the known ammonia and hydrazine transition metal complexes. This is due to the peculiar electronic properties of our neutral ancillary ligands, especially their strong donating capabilities. However, our catalysts currently require high temperatures and long reaction times. To address this issue, we have developed several new families of carbon- and boron-based ligands, which are even better donors. The corresponding metal complexes (particularly gold, rhodium, iridium, and ruthenium) of all these species will be tested in the Markovnikov and anti-Markovnikov hydroamination of alkynes, allenes, and also alkenes with ammonia and hydrazine. We will also develop metal-free catalytic processes for the functionalization of ammonia and hydrazine. By possessing both a lone pair of electrons and an accessible vacant orbital, singlet carbenes resemble and can mimic the chemical behavior of transition metals. Our preliminary results demonstrate that specially designed carbenes can split the N-H bond of ammonia by an initial nucleophilic activation that prevents the formation of Lewis acid-base adducts, which is the major hurdle for the transition metal catalyzed functionalization of NH3. The use of purely organic compounds as catalysts will eliminate the major drawbacks of transition-metal-catalysis technology, which are the excessive cost of metal complexes (metal + ligands) and in many cases the toxicity of the metal.
Catalytic Hydrogenation Of Metal Nitrides To Generate Ammonia Using Transition Metal Hydrides
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Author : Sangmin Kim
language : en
Publisher:
Release Date : 2021
Catalytic Hydrogenation Of Metal Nitrides To Generate Ammonia Using Transition Metal Hydrides written by Sangmin Kim and has been published by this book supported file pdf, txt, epub, kindle and other format this book has been release on 2021 with categories.
Ammonia (NH3) is one of the most crucial chemical compounds in human civilization due to its wide range of applications and demonstrated ability to transform global food production. The traditional, but still contemporary method for the synthesis of ammonia on industrial scale is the Haber-Bosch process, but high temperature and pressure conditions (> 300 atm, > 300 °C) result 1-2% of the global energy consumption and 7% of the global CO2 emissions solely to produce ammonia. The nitrogenase family of enzymes converts dinitrogen to ammonia under mild reaction conditions by proton-coupled electron transfer (PCET). By utilizing this concept, chemists have achieved the catalytic ammonia formation from N2 and H2 under mild reaction conditions using well-defined transition metal catalysts. However, all these examples used stoichiometric amounts of acids and reductants as the source of hydrogen, which incurs a tremendous chemical overpotential and stochiometric waste. Consequently, these problems raise this question. Can we develop a system to convert dinitrogen into ammonia with well-defined metal complexes 1) using dihydrogen as the terminal reductant just like the Haber-Bosch process, 2) under milder reaction conditions by PCET just like nitrogenase?To develop the corresponding system, metal hydrides that can undergo PCET or HAT (hydrogen atom transfer) using H2 as the terminal reductant were explored along with photoactivated metal hydrides to energetically access weak N-H bonds in the N2-derived complexes to make ammonia. In this thesis, four major research projects were discussed: 1) evaluation of the strategy using the rhodium hydride catalysts, identification of undesired side reactions and utilizing the side reaction for an application to catalytic hydrogenation of N-heteroarenes, 2) development of a thermally stable rhodium hydride catalyst to generate ammonia from an NH3-derived manganese nitride using H2, 3) development of a thermally- and photochemically stable ruthenium hydride HAT catalyst, and 4) photodriven ammonia formation from an N2-derived molybdenum nitride using iridium hydride catalysts and H2 as the terminal reductant and completion of the synthetic cycle for N2 hydrogenation.
Artificial Metalloenzymes And Metallodnazymes In Catalysis
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Author : Montserrat Diéguez
language : en
Publisher: John Wiley & Sons
Release Date : 2018-02-21
Artificial Metalloenzymes And Metallodnazymes In Catalysis written by Montserrat Diéguez and has been published by John Wiley & Sons this book supported file pdf, txt, epub, kindle and other format this book has been release on 2018-02-21 with Technology & Engineering categories.
An important reference for researchers in the field of metal-enzyme hybrid catalysis Artificial Metalloenzymes and MetalloDNAzymes in Catalysis offers a comprehensive review of the most current strategies, developed over recent decades, for the design, synthesis, and optimization of these hybrid catalysts as well as material about their application. The contributors—noted experts in the field—present information on the preparation, characterization, and optimization of artificial metalloenzymes in a timely and authoritative manner. The authors present a thorough examination of this interesting new platform for catalysis that combines the excellent selective recognition/binding properties of enzymes with transition metal catalysts. The text includes information on the various applications of metal-enzyme hybrid catalysts for novel reactions, offers insights into the latest advances in the field, and contains an informative perspective on the future: Explores the development of artificial metalloenzymes, the modern and strongly evolving research field on the verge of industrial application Contains a comprehensive reference to the research area of metal-enzyme hybrid catalysis that has experienced tremendous growth in recent years Includes contributions from leading researchers in the field Shows how this new catalysis combines the selective recognition/binding properties of enzymes with transition metal catalysts Written for catalytic chemists, bioinorganic chemists, biochemists, and organic chemists, Artificial Metalloenzymes and MetalloDNAzymes in Catalysis offers a unique reference to the fundamentals, concepts, applications, and the most recent developments for more efficient and sustainable synthesis.
Organotransition Metal Chemistry From Bonding To Catalysis
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Author : John F. Hartwig
language : en
Publisher:
Release Date : 2010-02-10
Organotransition Metal Chemistry From Bonding To Catalysis written by John F. Hartwig and has been published by this book supported file pdf, txt, epub, kindle and other format this book has been release on 2010-02-10 with Science categories.
Based on Collman et al.'s best-selling classic book, Principles and Applications of Organotransition Metal Chemistry, Hartwig's text consists of new or thoroughly updated and restructured chapters and provides an in-depth view into mechanism, reaction scope, and applications. It covers the most important developments in the field over the last twenty years with great clarity with a selective, but thorough and authoritative coverage of the fundamentals of organometallic chemistry, the elementary reactions of these complexes, and many catalytic processes occurring through organometallic intermediates, making this the Organotransition Metal Chemistry text for a new generation of scientists.
Ligand Design In Metal Chemistry
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Author : Mark Stradiotto
language : en
Publisher: John Wiley & Sons
Release Date : 2016-09-01
Ligand Design In Metal Chemistry written by Mark Stradiotto and has been published by John Wiley & Sons this book supported file pdf, txt, epub, kindle and other format this book has been release on 2016-09-01 with Science categories.
The design of ancillary ligands used to modify the structural and reactivity properties of metal complexes has evolved into a rapidly expanding sub-discipline in inorganic and organometallic chemistry. Ancillary ligand design has figured directly in the discovery of new bonding motifs and stoichiometric reactivity, as well as in the development of new catalytic protocols that have had widespread positive impact on chemical synthesis on benchtop and industrial scales. Ligand Design in Metal Chemistry presents a collection of cutting-edge contributions from leaders in the field of ligand design, encompassing a broad spectrum of ancillary ligand classes and reactivity applications. Topics covered include: Key concepts in ligand design Redox non-innocent ligands Ligands for selective alkene metathesis Ligands in cross-coupling Ligand design in polymerization Ligand design in modern lanthanide chemistry Cooperative metal-ligand reactivity P,N Ligands for enantioselective hydrogenation Spiro-cyclic ligands in asymmetric catalysis This book will be a valuable reference for academic researchers and industry practitioners working in the field of ligand design, as well as those who work in the many areas in which the impact of ancillary ligand design has proven significant, for example synthetic organic chemistry, catalysis, medicinal chemistry, polymer science and materials chemistry.
Hydrogen Transfer Reactions
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Author : Gabriela Guillena
language : en
Publisher: Springer
Release Date : 2016-09-27
Hydrogen Transfer Reactions written by Gabriela Guillena and has been published by Springer this book supported file pdf, txt, epub, kindle and other format this book has been release on 2016-09-27 with Science categories.
The series Topics in Current Chemistry Collections presents critical reviews from the journal Topics in Current Chemistry organized in topical volumes. The scope of coverage is all areas of chemical science including the interfaces with related disciplines such as biology, medicine and materials science. The goal of each thematic volume is to give the non-specialist reader, whether in academia or industry, a comprehensive insight into an area where new research is emerging which is of interest to a larger scientific audience. Each review within the volume critically surveys one aspect of that topic and places it within the context of the volume as a whole. The most significant developments of the last 5 to 10 years are presented using selected examples to illustrate the principles discussed. The coverage is not intended to be an exhaustive summary of the field or include large quantities of data, but should rather be conceptual, concentrating on the methodological thinking that will allow the non-specialist reader to understand the information presented. Contributions also offer an outlook on potential future developments in the field.
Frustrated Lewis Pairs
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Author : J. Chris Slootweg
language : en
Publisher: Springer
Release Date : 2021-11-23
Frustrated Lewis Pairs written by J. Chris Slootweg and has been published by Springer this book supported file pdf, txt, epub, kindle and other format this book has been release on 2021-11-23 with Science categories.
This volume highlights the latest research in frustrated Lewis pair (FLP) chemistry and its applications. The contributions present the recent developments of the use of FLPs in asymmetric catalysis, polymer synthesis, homogeneous and heterogeneous catalysis, as well as demonstrating their use as a pedagogical tool. The book will be of interest to researchers in academia and industry alike.
Modern Amination Methods
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Author : Alfredo Ricci
language : en
Publisher: John Wiley & Sons
Release Date : 2008-07-11
Modern Amination Methods written by Alfredo Ricci and has been published by John Wiley & Sons this book supported file pdf, txt, epub, kindle and other format this book has been release on 2008-07-11 with Science categories.
Organic compounds containing amino groups are at the center of modern organic chemistry, and are widely used in the pharmaceutical industry, crop protection, natural product chemistry, and in advanced materials. Modern methods for the introduction of the amino group are therefore of major importance to synthetic chemists and product developers. Over the last decade, many methods have been developed to generate new C-N bonds. At the same time, the pharmaceutical and chemical industry was rapidly moving away from the development of racemic compounds to the direct synthesis of enantiomerically pure materials. The articles of this book, written by internationally recognized experts, thus focus on asymmetric synthesis. The most recent catalytic amination methods have particularly revolutionized the chemistry of amino compounds - and you find them all in this first comprehensive overview.
Click Triazoles
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Author : Janez Košmrlj
language : en
Publisher: Springer
Release Date : 2014-06-11
Click Triazoles written by Janez Košmrlj and has been published by Springer this book supported file pdf, txt, epub, kindle and other format this book has been release on 2014-06-11 with Science categories.
B. R. Buckley and H. Heaney: Mechanistic Investigations of Copper(I)- Catalyzed Alkyne–Azide Cycloaddition Reactions.- J. D. Crowley and D. A. McMorran: “Click-Triazole” Coordination Chemistry: Exploiting 1,4-Disubstituted-1,2,3-Triazoles as Ligands.- S. Lee and A. H. Flood: Binding Anions in Rigid and Reconfigurable Triazole Receptors.- M. Watkinson: Click Triazoles as Chemosensors.- H.-F. Chow, C.-M. Lo and Y. Chen: Triazole-Based Polymer Gels.- T. Zheng, S. H. Rouhanifard, A. S. Jalloh, P. Wu: Click Triazoles for Bioconjugation.- S. Mignani, Y. Zhou, T. Lecourt and L. Micouin: Recent Developments in the Synthesis 1,4,5-Trisubstituted Triazoles.
Nitrogenation Strategy For The Synthesis Of N Containing Compounds
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Author : Ning Jiao
language : en
Publisher: Springer
Release Date : 2016-11-15
Nitrogenation Strategy For The Synthesis Of N Containing Compounds written by Ning Jiao and has been published by Springer this book supported file pdf, txt, epub, kindle and other format this book has been release on 2016-11-15 with Science categories.
This book focuses on direct nitrogenation strategies to incorporate one or more N-atoms into simple substrates especially hydrocarbons via C–H and/or C–C bond cleavage, which is a green and sustainable way to synthesize nitrogen-containing compounds. The book consists of seven chapters demonstrating interesting advances in the preparation of amines, amides, nitriles, carbamides, azides, and N-heterocyclic compounds and illustrating the mechanisms of these novel transformations. It offers an accessible introduction to nitrogenation reactions for chemists involved in N-compound synthesis and those interested in discovering new reagents and reactions. Ning Jiao is a Professor of Chemistry at Peking University, China.