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Surface organometallic chemistry is a new field bringing together researchers from organometallic, inorganic, and surface chemistry and catalysis. Topics ranging from reaction mechanisms to catalyst preparation are considered from a molecular basis, according to which the "active site" on a catalyst surface has a supra-molecular character. This. the first book on the subject, is the outcome of a NATO Workshop held in Le Rouret. France, in May. 1986. It is our hope that the following chapters and the concluding summary of recommendations for research may help to provide a definition of surface organometallic chemistry. Besides catalysis. the central theme of the Workshop, four main topics are considered: 1) Reactions of organometallics with surfaces of metal oxides, metals. and zeolites; 2) Molecular models of surfaces, metal oxides, and metals; 3) Molecular approaches to the mechanisms of surface reactions; 4) Synthesis and modification of zeolites and related microporous solids. Most surface organometallic chemistry has been carried out on amorphous high-surf ace-area metal oxides such as silica. alumina. magnesia, and titania. The first chapter. contributed by KNOZINGER. gives a short summary of the structure and reactivity of metal oxide surfaces. Most of our understanding of these surfaces is based on acid base and redox chemistry; this chemistry has developed from X-ray and spectroscopic data, and much has been inferred from the structures and reactivities of adsorbed organic probe molecules. There are major opportunities for extending this understanding by use of well-defined (single crystal) oxide surfaces and organometallic probe molecules.
With contributions by numerous experts
Covering everything from the basics to recent applications, this monograph represents an advanced overview of the field. Edited by internationally acclaimed experts respected throughout the community, the book is clearly divided into sections on fundamental and applied surface organometallic chemistry. Backed by numerous examples from the recent literature, this is a key reference for all chemists.
The literature contains tens of thousands of publications and patents devoted to the synthesis, characterization and processing of polymers. Despite the fact that there are more than one hundred elements, the majority of these publications and patents concern polymers with carbon backbones. Furthermore, the limited (by comparison) number of publications on polymers that contain elements other than carbon in their backbones are typically devoted to polymers based on silicon, especially those with Si-O bonds. This disparity is partially a consequence of the dearth of low cost organometallic feedstock chemicals potentially useful for polymer synthesis. It also derives from the lack of general synthetic techniques for the preparation of organometallic polymers. That is, by comparison with the numerous synthetic strategies available for the preparation of organic polymers, there are few such strategies available for synthesizing tractable, organometallic polymers. In recent years, commerical and military performance requirements have begun to challenge the performance limits of organic polymers. As such, researchers have turned to organometallic polymers as a possible means of exceeding these limits for a wide range of applications that include: (1) microelectronics processing (e.g. photoresists) [1]; (2) light weight batteries (conductors and semi-conductors) [2]; (3) non-linear optical devices [3] and, (4) high temperature structural materials (e.g. ceramic fiber processing) [4,5].
The book is a multi-author survey (in 15 chapters) of the current state of knowledge and recent developments in our understanding of oxide surfaces. The author list includes most of the acknowledged world experts in this field. The material covered includes fundamental theory and experimental studies of the geometrical, vibrational and electronic structure of such surfaces, but with a special emphasis on the chemical properties and associated reactivity. The main focus is on metal oxides but coverage extends from 'simple' rocksalt materials such as MgO through to complex transition metal oxides with different valencies.
It is widely recognized that an understanding of the physical and chemical properties of clusters will give a great deal of important information relevant to surface and bulk properties of condensed matter. This relevance of clusters for condensed matter is one of the major motivations for the study of atomic and molecular clusters. The changes of properties with cluster size, from small clusters containing only a few atoms to large clusters containing tens of thousands of atoms, provides a unique way to understand and to control the development of bulk properties as separated units are brought together to form an extended system. Another important use of clusters is as theoretical models of surfaces and bulk materials. The electronic wavefunctions for these cluster models have special advantages for understanding, in particular, the local properties of condensed matter. The cluster wavefunctions, obtained with molecular orbital theory, make it possible to relate chemical concepts developed to describe chemical bonds in molecules to the very closely related chemical bonding at the surface and in the bulk of condensed matter. The applications of clusters to phenomena in condensed matter is a cross-disciplinary activity which requires the interaction and collaboration of researchers in traditionally separate areas. For example, it is necessary to bring together workers whose background and expertise is molecular chemistry with those whose background is solid state physics. It is also necessary to bring together experimentalists and theoreticians.
The features of this book which will be of special interest to academic organic chemists are the introduction (Chapter 1), which presents a short course on the concepts and language of heterogeneous catalysis, covers organic reaction mechanisms of hydrogenation (Chapter 2), hydrogenolysis (Chapter 4), and oxidation (Chapter 6), a presents problems and solutions specific for running heterogeneous catalytic organic reactions in solution. These materials can supplement advanced chemistry courses. Most synthetic organic chemists use a variety of "protecting groups" which they attach to functional groups (reactive groups of atoms) while some reaction is being conducted on another part of the molecule. These protecting groups prevent reactions of the functional groups during other reactions and are removed later by a heterogeneous catalytic method called hydrogenolysis. One unique feature of this book, not found in other books on catalysis, is an exhaustive chapter (Chapter 4) on hydrogenolysis, which is dredged from the recent synthetic literature published by modern organic chemists. Academic organic chemists should find this chapter extremely useful and may wish to adopt the book as a supplement for advanced organic chemistry courses designed for seniors and for graduate students. It will also be useful for professors and their research groups engaged in synthetic organic chemistry. Many academic organic chemists are not aware of recent advances in heterogeneous enantioselective catalysis (Chapter 3) or in selective low temperature, liquid phase heterogeneous catalytic oxidations by hydrogen peroxide (Chapter 6). These specialty topics are timely and may be new to academic organic chemists and can be used to supplement their advanced courses. Several features of this book will also be of special interest to industrial chemists who are unfamiliar with heterogeneous catalysis. Many good organic chemists are hire by industry. They synthesize a new compound using standard organic synthetic techniques but are informed by their supervisor that they must convert some of their synthetic steps into heterogeneous catalytic steps. They may not have been exposed to heterogeneous catalysis and have few places to turn. This book offers them a crash course in heterogeneous catalysis as well as many examples of reactions and conditions with which they can start their search. Those industrial organic chemists already familiar with heterogeneous catalysis will find this book useful as a reference to many examples in the recent literature. They will find recent surface science discoveries correlated with heterogeneous catalysis or organic reactions and mechanistic suggestions designed to stimulate innovative nontraditional thinking about organic reactions on surfaces. - Written by organic chemists for organic chemists - Introduces heterogeneous catalysis concepts and language - Presents a comprehensive compilation of protecting group removal procedures - Covers liquid-phase hydrogenations, hydrogenolysis, and oxidations - Addresses heterogeneous methods for producing pure enantiomers of chiral products - Examines the emerging field of heterogenized homogeneous catalysts - Mixes practical applications with mechanistic interpretations
The analogy between the chemistry of molecular transition metal clusters and the processes of chemisorption and catalysis at metal surfaces (the Cluster Surface analogy) has for a number of years provided an interplay between experimental and theoretical inorganic and physical chemists. This collaborative approach has born fruit in the use of well defined modes of metal-ligand bonding in discrete molecular clusters, models for metal-ligand binding on surfaces. Some of the key topics discussed in The Synergy between Dynamics and Reactivity at Clusters and Surfaces are: (1) Mechanisms of the fluxional behaviour in clusters in the liquid phase and the connections with diffusion processes on extended surfaces. The role of metal-metal bond breaking in diffusion. (2) Analogies in the structure of chemisorbed species and related ligands on metallic clusters. (3) Analogies between benzene surface chemistry on extended metal surfaces and on metal surfaces in molecular cluster compounds with particular reference to structural distortions. (4) The role of mobile precursors for dissociation of chemisorption on extended metals and on clusters. Are there analogies in the ligand attachment during cluster compound synthesis? (5) The role of defect sites on metal surfaces in catalyzing chemical reactions and the connection to the special bonding properties of sites on metal clusters having lowest metal-metal coordination. (6) The size of metal clusters needed to mimic surface phenomena on bulk metal surfaces. Different sites needed for different phenomena.
When one considers the overall representation of frontier orbital filling of hexacoordinate (Oh) and tetracoordinate (Td) inorganic and organo metallic complexes, it clearly appears that out of 26 cases covering both high spin and low spin situations, 21 represent paramagnetic species (K. Purcell, J. Kotz, "Inorganic Chemistry", Saunders, 1977, p561). This would suggest that, if there is a part in chemistry to illustrate the reactivity of radical species, this part certainly is inorganic organometallic chemistry. In contrast with these expectations, and whereas the standard Organic Chemistry textbook (J. March ,"Advanced Organic Chemistry", J. Wiley, N. Y. , 1985) has a specific chapter devoted to free radical reactivity, neither the inorganic standard (FA Cotton, G. Wilkinson, "Advanced Inorganic Chemistry", Wiley, 1988), nor the Organometallic one (J. P. Collman, L. S. Hegedus, J. R. Norton, R. G. Finke, "Principles and Applications of Organotransition Metal Chemistry", University Science Books Mill Valley C. A. , 1987) possess such a specific chapter. The balance is partly restored because the two last cited books have a more comprehensive treatment of electron transfer phenomena. These comparisons show unambiguously that the importance of paramagnetic species in chemical reactivity still lacks a consistent treatment transcending the artificial barriers between branches of Chemistry. This book, which brings together experimental facts and concepts originating from organometallic and organic reactivities, is a step in the direction of bridging this gap. The unifying thread which connects the 35 chapters throughout this book is Activation/Selectivity and Catalysis by means of radical chemistry.
The recession in the traditional heavy industries along with the development of advanced technologies in all the industrial countries has meant that the impact of heterogeneous catalysis in the synthesis of fine chemicals is becoming increasingly noticeable. The second International Symposium on Heterogeneous Catalysis and Fine Chemicals is to be seen in this perspective. Organised by the Laboratory of Catalysis in Organic Chemistry of the University of Poitiers within the framework of the International Symposia of the `Centre National de la Recherche Scientifique' (CNRS), the symposium provided an opportunity for contact between academic researchers and manufacturers, users (or potential users) of solid catalysts for fine chemical synthesis. The book gives an overall view of the problems encountered by academic and industrial researchers. A large variety of reactions are described, the emphasis being on selectivity: chemo-, regio-, stereoselectivity (even enantioselectivity) and on the change of these selectivities as a function of the characteristics of the surface sites (nature, distribution, etc.).The three themes of the symposium, hydrogenation, oxidation and acid-base catalysis were introduced in four plenary lectures and two invited communications, maintaining a balance between the industrial and the academic points of view. Some 60 research papers selected by the Scientific Committee were presented. All are reproduced in full in this proceedings volume.