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This book deals with adsorption and catalysis on the surface of transition elements and their compounds, many of which are in teresting because of their particular electronic structure. The authors have worked through a vast body of experimental evi dence on the structure and properties of surfaces of transition metals and relevant oxides. Consideration is given mostly to simple (as opposed to mixed) oxides of transition elements, to common metals and to the adsorption of simple gases. A great deal of attention is paid to the nature of active surface sites responsible for chemisorption and catalytic transformations. The description relies mainly on the simplified ligand-field theory, which, however, proves quite satisfactory for predicting the adsorptive and catalytic activity of species. In many cases simple systems were explored with the aid of novel techniques, and it is only for such systems that the mechanism of the ele mentary act of adsorption and catalysis can be given adequate treatment. The present monograph has emerged from our earlier work in Russian, which appeared in the Khimiya Publishing House (Mos cow) in 1981. This English edition has, however, been revised completely to broaden its scope and to include more recent a chievements. For fruitful discussions the authors are grateful to A.A.
In this book the author presents an up-to-date summary of existing information on the structure, electronic properties, chemistry and catalytic properties of transition metal oxides. The subjects covered in the book can be divided into three sections. The first (chapters 1 to 3) covers the structural, physical, magnetic, and electronic properties of transition metal oxides. Although the emphasis is on surface properties, relevant bulk properties are also discussed. The second section (chapters 4 to 7) covers surface chemical properties. It includes topics that describe the importance of surface coordinative unsaturation in adsorption, the formation of surface acidity and the role of acidity in determining surface chemical properties, the nature and reactivities of adsorbed oxygen, and the surface chemistry in the reduction of oxides. The third section (chapters 8 to 14) is on the catalytic properties. Various catalytic reactions including decomposition, hydrogenation, isomerization, metathesis, selective oxidation, and reactions involving carbon oxides are discussed. Emphasis is placed more on reaction mechanisms and the role of catalysts than on kinetics and processes. Chapters on the preparation of oxide catalysts and on photo-assisted processes are also included. Whenever appropriate, relationships between various topics are indicated. Written for surface physicists, chemists, and catalytic engineers, the book will serve as a useful source of information for investigators and as a comprehensive overview of the subject for graduate students.
Author : S. David Jackson Publisher : John Wiley & Sons Page : 916 pages File Size : 27,87 MB Release : 2008-11-24 Category : Science ISBN : 9783527318155
With its two-volume structure, this handbook and ready reference allows for comprehensive coverage of both characterization and applications, while uniform editing throughout ensures that the structure remains consistent. The result is an up-to-date review of metal oxides in catalysis. The first volume covers a range of techniques that are used to characterize oxides, with each chapter written by an expert in the field. Volume 2 goes on to cover the use of metal oxides in catalytic reactions. For all chemists and engineers working in the field of heterogeneous catalysis.
The chemistry of metals has traditionally been more understood than that of its oxides. As catalytic applications continue to grow in a variety of disciplines, Metal Oxides: Chemistry and Applications offers a timely account of transition-metal oxides (TMO), one of the most important classes of metal oxides, in the context of catalysis. The
Heterogeneous catalysis provides the backbone of the world's chemical and oil industries. The innate complexity of practical catalytic systems suggests that useful progress should be achievable by investigating key aspects of catalysis by experimental studies on idealised model systems. Thin films and supported clusters are two promising types of model system that can be used for this purpose, since they mimic important aspects of the properties of practical dispersed catalysts. Similarly, appropriate theoretical studies of chemisorption and surface reaction clusters or extended slab systems can provide valuable information on the factors that underlie bonding and catalytic activity. This volume describes such experimental and theoretical approaches to the surface chemistry and catalytic behaviour of metals, metal oxides and metal/metal oxide systems. An introduction to the principles and main themes of heterogeneous catalysis is followed by detailed accounts of the application of modern experimental and theoretical techniques to fundamental problems. The application of advanced experimental methods is complemented by a full description of theoretical procedures, including Hartree-Fock, density functional and similar techniques. The relative merits of the various approaches are considered and directions for future progress are indicated.
The Symposium was held to honour the memory of the late Dr. A.J. Tench who made numerous important contributions to our knowledge of the structure, reactivity and adsorption properties of oxide surfaces. This volume contains an up-to-date picture of adsorption and catalysis on oxide surfaces, not in the form of a comprehensive review but in its living aspects of work in progress. It describes detailed studies on the determination of the coordination surface ions, particularly oxide ions, by photoluminescence and reflectance spectroscopy, on the identification of adsorbed species by magnetic optical or surface techniques and on catalysis, with emphasis on new concepts such as catalysis involving excited states or structure sensitive reactions.Professionals working in the industrial and academic laboratories will find the book particularly useful as it provides a state-of-the-art account of our understanding of the structure and adsorption characteristics of oxide surfaces. Contained in the book are first class research papers by leading exponents in this field. A very important issue is that the book highlights for the first time the importance of excited states and structure sensitivity in determining the behaviour of oxide surfaces.
Heterogeneous catalysis is a fascinating and complex subject of utmost importance in the present day. Its immense technological and economical importance and the inherent complexity of the catalytic phenomena have stimulated theoretical and experimental studies by a broad spectrum of scientists, including chemists, physicists, chemical engineers, and material scientists. Computational and theoretical techniques are now having a major impact in this field. This book aims to illustrate and discuss the subject of heterogeneous catalysis and to show the current capabilities of the theoretical and computational methods for studying the various steps (diffusion, adsorption, chemical reaction) of heterogeneous catalytic process involving zeolites, metal oxides, and transition metal surfaces. The book covers: the use of techniques of computational chemistry to simulate zeolites, metallic and bimetallic surfaces, and oxide-supported metals; the impact of simulation methods on the understanding of the diffusion and adsorption of molecules and cations within the pores of zeolites, and also on the adsorption of molecules on metal and metal-oxide surfaces; and the applications of quantum-mechanical methods to the study of the reaction mechanism and pathways of the adsorbed molecules. This book is recommended primarily to scientists and graduate students conducting research in the fields of heterogeneous catalysis and surface science. It will also be valuable to advanced undergraduate students wishing to become acquainted with the latest developments in these exciting fields of research, and to experimentalists seeking theoretical support for interpreting their results.
Heterogeneous catalysts consisting of transition metal nanoparticles dispersed on high surface area oxide supports are ubiquitous in industrial-scale chemistry and alternative energy technology. Despite their importance, our fundamental understanding of the physical and chemical properties that make these systems catalytically effective is still incomplete. This dissertation details the use of surface-sensitive ultrahigh vacuum (UHV) techniques to study model catalysts consisting of late transition metals that are vapor-deposited onto single-crystal oxide films in order to understand how their fundamental physical and chemical properties affect their catalytic properties, such as activity, selectivity, and resistance to deactivation. Specifically, the binding energies of metal atoms and nanoparticles - and the adhesion energy of metal nanoparticles and films - are measured as a function of the size and type of nanoparticle, and the surface or site that they are adsorbed on. The key technique utilized in this study is single-crystal adsorption calorimetry (SCAC), which uses a highly sensitive detector to directly measure the heats of adsorption of metal vapor adsorbing onto oxide thin films. These calorimetric data are combined with surface-sensitive spectroscopic techniques to characterize the oxide surface, and to model the size of the nanoparticles a function of total metal coverage. This approach allows the heat data to be correlated with the surface structure, composition, particle size, or electronic character of the system. Several improvements to the instrument are discussed that allow for the study of metals with very low vapor pressures (high heats of vaporization), specifically Au, which is the focus of this work. This new instrument can also be operated at temperatures as low as 100 K, which is used to study metal atom adsorption under conditions where adatom diffusion is slower, which increases the particle density (reducing the size of particles formed) and increasing the likelihood that nucleation occurs at less favorable sites. Au adsorption is discussed here on three difference surfaces with increasing complexity: Pt(111), MgO(100), and CeO2-x(111). These results are compared to Cu adsorption on Pt(111) and CeO2-x(111) (also presented in this work), and to Cu adsorption on MgO(100) as well as Ag adsorption on MgO(100) and CeO2-x(111) (from previous work done by this research group). The first ever experimental measurements of gold adsorption onto an oxide surface as a function of particle size are presented, and the adsorption energy of both a single Au atom and a single Cu atom was measured on CeO1.95(111). This represents the first experimental measurements of any metal atom adsorption onto any oxide surface. The effect of defects on Au and Cu adsorption, such as step edges and electron-rich oxygen vacancies is discussed in detail. These defects are either introduced in film preparation (in the case of oxygen vacancies on CeO2-x(111)), or are inherently present in thin film preparations (morphological defects). The metals studied here, like most late transition metals, adsorb more strongly on morphological defects such as steps, while only Au and Ag bind more strongly to oxygen vacancies on CeO2-x(111) (Cu does not). Additionally, Au was found to nucleate significantly more strongly than Ag and Cu on morphological defects of MgO(100), and to form 2D islands on MgO(100) within the first 0.4 monolayers (ML) coverage. This work presents the first ever measurement of the heat of adsorption (and thus the chemical potential) of metal atoms in metal nanoparticles as a function of their 2D island diameter. A similar interpretation is used to present the chemical potential of Cu atoms in Cu nanoparticles as a function of their 3D particle dimeter on CeO2-x(111). The work contained in this dissertation has added critically important thermodynamic and structural data to the library of research in the catalysis and surface science communities, and has addressed some of the most relevant materials that could not be studied with previous generations of SCAC instruments. These model catalyst systems are of substantial fundamental and practice interest due to their immediate use in industrial catalysis, and combining these newest results with existing data (both from our group and from the literature) has allowed us to propose a new trend for metal-oxide adhesion. These investigations, and specifically this trend, will aid in the global effort to expedite the future design and testing process of new catalytic materials through improved understanding of their fundamental properties.