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Author: Feng Niu Publisher: ISBN: Category : Languages : en Pages : 0
Book Description
Amines are very important intermediates for chemical industry and life science, which can be synthesized through different traditional routes. Metals based catalytic amination of alcohols via the so-called “hydrogen borrowing” mechanism is a relative efficient and environmental benign way for synthesis of different primary amines. However, there are still some challenges exist, such as high cost of noble metals, low selectivity of primary amine products, and poor stability and recyclability for industrial applications. To solve these problems, different strategies have been applied in this thesis. Carbon deposition produced by catalyst pre-treatment with alcohols under the optimized conditions has been employed for major enhancement of the selectivity of alcohol amination to primary amines (from 30-50 to 80-90%), which arises from steric hindrance in hydrogenation of bulky secondary imines as intermediate products over partially carbon-decorated cobalt nanoparticles. An efficient approach to protect cobalt catalyst from catalytic deactivation by liquid bismuth promotion with different loading content was disclosed for selectively amination of 1-octanol. The N-alkylation of amines by alcohols over a cheap and efficient heterogeneous catalyst-titanium hydroxide was also proposed. The catalyst with mild Brönsted acidity provides the selectivity higher than 90% to secondary amines for functionalized aromatic and aliphatic alcohols and amines at high catalytic activity and stability.
Author: Feng Niu Publisher: ISBN: Category : Languages : en Pages : 0
Book Description
Amines are very important intermediates for chemical industry and life science, which can be synthesized through different traditional routes. Metals based catalytic amination of alcohols via the so-called “hydrogen borrowing” mechanism is a relative efficient and environmental benign way for synthesis of different primary amines. However, there are still some challenges exist, such as high cost of noble metals, low selectivity of primary amine products, and poor stability and recyclability for industrial applications. To solve these problems, different strategies have been applied in this thesis. Carbon deposition produced by catalyst pre-treatment with alcohols under the optimized conditions has been employed for major enhancement of the selectivity of alcohol amination to primary amines (from 30-50 to 80-90%), which arises from steric hindrance in hydrogenation of bulky secondary imines as intermediate products over partially carbon-decorated cobalt nanoparticles. An efficient approach to protect cobalt catalyst from catalytic deactivation by liquid bismuth promotion with different loading content was disclosed for selectively amination of 1-octanol. The N-alkylation of amines by alcohols over a cheap and efficient heterogeneous catalyst-titanium hydroxide was also proposed. The catalyst with mild Brönsted acidity provides the selectivity higher than 90% to secondary amines for functionalized aromatic and aliphatic alcohols and amines at high catalytic activity and stability.
Author: Feng Shi Publisher: Academic Press ISBN: 0128122854 Category : Technology & Engineering Languages : en Pages : 208
Book Description
Catalytic Amination for N-Alkyl Amine Synthesis provides a useful survey of this key type of reaction for chemistry researchers in academia and industry. Beginning with an introduction to amination and the development of the field, the book focuses on useful and high potential methods, such as the catalytic amination of alcohol with homogeneous and heterogeneous catalysts, the coupling reaction of olefin and amine, and the reductive amination of carbon dioxide with different reducing agents. The work also discusses two key examples of one-pot synthesis, the oxidative amination of alkane and amine and synthesis of N-alkyl amine with nitrobenzene and nitrile as starting materials. Valuable for chemists, materials scientists, chemical engineers and others, the book offers a unique overview of this growing area and its future possibilities. Describes the catalytic amination of alcohol with homogeneous and heterogeneous catalysts Discusses the one-pot oxidative amination of alkane and amine Explores the application of ammonia as the N-source in amination reaction to avoid primary or secondary amine synthesis
Author: Alexandre Dumon Publisher: ISBN: Category : Languages : en Pages : 0
Book Description
Polyamines are important industrial intermediates. Their production however relies on petroleum, external hydrogen input and toxic products (HCN, HCl). It becomes therefore important to change the feedstock. In that optic, we aim here at aminate biosourced alcohols.We have performed a DFT study in order to understand alcohols amination key steps, to master its principle and outcomes.In particular, we showed that the chemical environment was playing an important role during that reaction : experimentally, Nickel (Ni) is more active than Palladium (Pd). However bare surfaces models were not predicting that fact. Taking a 1/9-monolayer ammonia coverage into account allowed to retrieve the correct reactivity.We studied the effects of the chemical environment on levulinic acid hydrogenation by formic acid, and on isosorbide isomerization. We showed that it was playing a key role on intermediates stability, modifying the catalysts activity.
Author: Michael James Boyd Publisher: ISBN: Category : Alcohol Languages : en Pages : 107
Book Description
As the production of natural gas and agricultural biomass/energy crops increases, new efficient and sustainable technologies will be required to convert these feedstock molecules into the same fuels and chemical we get from conventional petroleum today. Electrochemistry is a possible tool for the conversion of these species that can be coupled to renewable electricity. The discovery and development of selective and active electrocatalysts is one of the primary challenges in utilizing natural gas and biomass resources. But first there is a lack of fundamental understanding in (1) the reaction mechanism and (2) how operating conditions such as potential, electrolyte pH, mass transport, and time affect the the activity and selectivity of catalysts. To this end platinum was used as a model system to study electrochemical methane oxidation at room temperature and pressure. The experimental results on platinum combined with density functional theory calculations show that methane is first thermally activated at Pt (211) like step sites, then the resulting methyl intermediate is electrochemically oxidized to CO* which is in equilibrium with the final product CO2. The equilibrium can be shifted to favor complete oxidation by adjusting the applied electrochemical potential, specifically at potentials below 0.5 V vs. RHE CO* is the most thermodynamically stable species along the reaction pathway whereas above 0.5 V vs. RHE CO2 is now the most stable species. Important to note however is that since the kinetics for methane activation are very slow (barrier of ~0.95 eV) the platinum surface must be free of other adsorbed species, namely protons or hydroxides. Based on reaction mechanism for electrochemical methane oxidation on platinum it is unlikely that partial oxidation of methane on metallic electrodes well occur. For this reason we probed the activity of several transition metal oxide materials with the hope that they may be active for methane oxidation. Unfortunately our initial results suggest no significant methane oxidation occurs on these materials. In the case of biomass oxidation 1st row transition metal oxides have recently been shown to be quite selective in the conversion of alcohols to their corresponding carboxylic acids. Benzyl alcohol was used as a model molecule to study the reaction mechanism for alcohol oxidation on Ni(OH)2 electrodes as a function of potential and electrolyte pH. It was found that the active phase for alcohol oxidation is the metal oxy-hydroxide. The activity and selectivity were found to be heavily dependent on the electrolyte pH. Under strong alkaline conditions (> pH 13) high current densities and complete oxidation of benzyl alcohol to benzoate was favored whereas at more moderately alkaline conditions low current densities and partial oxidation to benzaldehyde was favored. Based on these results we hypothesize that a significant concentration of OH- in solution is required to activated the intermediate product benzaldehyde. The activity of several novel Ni materials was also probed for benzyl alcohol oxidation. Ni-doped nitrided carbons which have single atom nickel active sites were found to be selective for partial oxidation, however further optimization of the catalyst synthesis is required to increase the activity to compete with the bulk Ni(OH)2 electrodes. In conclusion, this dissertation presents a variety of experimental work focused on identifying the reaction mechanism for several oxidation reactions and provides key understanding that can be used towards the development of new electrocatalysts for the oxidation of hydrocarbons and alcohols.
Author: Zhen-Xing Liang Publisher: Royal Society of Chemistry ISBN: 184973478X Category : Science Languages : en Pages : 265
Book Description
Energy and environment issues are of paramount importance to achieve the sustainable development of our society. Alcohol-fuelled direct oxidation fuel cells (DOFCs), as a clean and highly-efficient energy harvesting engine, have attracted intensive research activity over recent decades. Electrocatalysts are the material at the very heart of the cell that determines the performance of DOFCs. The rapid advances in electrocatalysts, particularly nano-sized ones, have left current information only available in scattered journals. To be truly useful to both present and future researchers, a new book is needed to present an insightful review of the reaction nature of this research and to systematically summarize recent advances in nanocatalysts, and convey a more global perspective. Catalysts for Alcohol-fuelled Direct Oxidation Fuel Cells will present a state-of-the-art review on recent advances in nanocatalysts and electrocatalysis in DOFCs, including both proton and hydroxide ion exchange membrane fuel cells. The main topics covered include a molecular-level understanding of electrocatalysis, the design principles of electrocatalysts, recent advances in nanocatalysts and future perspectives for DOFCs. The book presents a cutting-edge collection on nanocatalysts for alcohol-fuelled direct oxidation fuel cells and brings together the most authoritative researchers in the field from both industry and academia, filling the gap between both sides. Finally, the book will provide an insightful review on electrocatalysis at the molecular- level, which will be useful for postgraduate students and junior researchers in this field. It will be an essential resource for postgraduates, researchers and policy-makers globally in academia, industry, and government institutions.
Author: Philip L. Fuchs Publisher: John Wiley & Sons ISBN: 1118704843 Category : Science Languages : en Pages : 2037
Book Description
The Handbook is part of the Handbook of Reagents for Organic Chemistry series, aiming at collecting articles on a particular theme that individual researchers in academia or industry can use on a daily basis. The Handbook starts with a section discussing the most important aspects of heteroarene functionalization. The introduction is followed by the alphabetical listing of the most relevant reagents drawn from the EROS database. The Editor, André Charette from the University of Montreal, has selected 120 reagent descriptions, many of them updated with heteroarene-specific reactions for this Handbook. Following the standard format for EROS, each article contains an overview of the synthesis and physical properties of the reagents or catalyst, conditions for its storage, and purification methods. Given the importance of heteroarenes in biology and especially in medicinal chemistry, a Handbook that focuses exclusively on heteroarene functionalization has been long overdue. This Handbook will have a broad appeal to many individuals engaged in the area of medicinal chemistry, fine chemical synthesis and industrial-scale chemistry. Key features: Builds on the success of the previously published Handbooks of Reagents for Organic Synthesis Compares the numerous new C-H functionalization reactions that have been developed in the past decade Heteroarene functionalization is widely used in the development of pharmaceuticals and other bioactive compounds Contains listings of secondary reagents for which more information is available in the online edition
Author: Anthony J. Burke Publisher: John Wiley & Sons ISBN: 3527807268 Category : Science Languages : en Pages : 603
Book Description
Presents the most effective catalytic reactions in use today, with a special focus on process intensification, sustainability, waste reduction, and innovative methods This book demonstrates the importance of efficient catalytic transformations for producing pharmaceutically active molecules. It presents the key catalytic reactions and the most efficient catalytic processes, including their significant advantages over compared previous methods. It also places a strong emphasis on asymmetric catalytic reactions, process intensification (PI), sustainability and waste mitigation, continuous manufacturing processes as enshrined by continuous flow catalysis, and supported catalysis. Active Pharmaceutical Ingredients in Synthesis: Catalytic Processes in Research and Development offers chapters covering: Catalysis and Prerequisites for the Modern Pharmaceutial Industry Landscape; Catalytic Process Design - The Industrial Perspective; Hydrogenation, Hydroformylation and Other Reductions; Oxidation; ; Catalytic Addition Reactions; Catalytic Cross-Coupling Reactions; Catalytic Metathesis Reactions; Catalytic Cycloaddition Reactions: Coming Full-Circle; Catalytic Cyclopropanation Reactions; Catalytic C-H insertion Reactions; Phase Transfer Catalysis; and Biocatalysis. -Provides the reader with an updated clear view of the current state of the challenging field of catalysis for API production -Focuses on the application of catalytic methods for the synthesis of known APIs -Presents every key reaction, including Diels-Alder, CH Insertions, Metal-catalytic coupling-reactions, and many more -Includes recent patent literature for completeness Covering a topic of great interest for synthetic chemists and R&D researchers in the pharmaceutical industry, Active Pharmaceutical Ingredients in Synthesis: Catalytic Processes in Research and Development is a must-read for every synthetic chemist working with APIs.
Author: Feng Niu
Author: Feng Niu
Author: Feng Shi
Author: Alexandre Dumon
Author: Jason Scott
Author: Gerrit Wienhöfer
Author: Michael James Boyd
Author: Zhen-Xing Liang
Author: Philip L. Fuchs
Author: Anthony J. Burke
Author: Alexandru Gheorghe