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Gold has traditionally been regarded as inactive as a catalytic metal. However, the advent of nanoparticulate gold on high surface area oxide supports has demonstrated its high catalytic activity in many chemical reactions. Gold is active as a heterogeneous catalyst in both gas and liquid phases, and complexes catalyse reactions homogeneously in solution. Many of the reactions being studied will lead to new application areas for catalysis by gold in pollution control, chemical processing, sensors and fuel cell technology. This book describes the properties of gold, the methods for preparing gold catalysts and ways to characterise and use them effectively in reactions. The reaction mechanisms and reasons for the high activities are discussed and the applications for gold catalysis considered./a
This book is devoted to the emerging field of techniques for visualizing atomic-scale properties of active catalysts under actual working conditions, i.e. high gas pressures and high temperatures. It explains how to understand these observations in terms of the surface structures and dynamics and their detailed interplay with the gas phase. This provides an important new link between fundamental surface physics and chemistry, and applied catalysis. The book explains the motivation and the necessity of operando studies, and positions these with respect to the more traditional low-pressure investigations on the one hand and the reality of industrial catalysis on the other. The last decade has witnessed a rapid development of new experimental and theoretical tools for operando studies of heterogeneous catalysis. The book has a strong emphasis on the new techniques and illustrates how the challenges introduced by the harsh, operando conditions are faced for each of these new tools. Therefore, one can also read this book as a collection of recipes for the development of operando instruments. At present, the number of scientific results obtained under operando conditions is still limited and mostly focused on a simple test reaction, the catalytic oxidation of CO. This reaction thus forms a natural binding element between the chapters, linking the demonstrations of new techniques, and also connecting the theoretical and experimental studies. Some first results on other reactions are also presented. If there is one thing that can be concluded already in this early stage, it is that the catalytic conditions themselves can have dramatic effects on the structure and composition of the surfaces of catalysts, which, in turn can greatly affect the mechanisms, the activity, and the selectivity of the chemical reactions that they catalyze.
As in the study of transition metal complexes in solution, molecular spectroscopic methods - principally the infrared, ultraviolet/visible and electron spin resonance spectroscopies - have played key roles in establishing the concepts of coordination chemistry occurring at the surfaces of solids. This book describes the development of the principals of coordination chemistry of oxide surfaces using analyses of data obtained by these methods. The nature, properties, concentration of the surface adsorption centers and their influence on the character of interaction with different molecules are investigated. The book commences with an account of the basic theoretical principles and experimental techniques of the various spectroscopy methods, with special attention devoted to in situ measurements where the oxide or catalyst sample is in contact with the adsorbate or the reactant. A detailed account is presented of the methods for characterizing the oxidation state and degree of coordination of surface cations and oxygen anions by the adsorption of probe molecules. The complexation of many inorganic, organometallic and organic molecules with different oxide systems is critically examined, and a classification of formed surface compounds, based on the interaction with definite type of adsorption centers, is given. Possible mechanisms of numerous catalytic reactions, including the transformation of organic molecules over acidic catalysts via the carboionic mechanism, are discussed using the spectroscopic identifications of reaction intermediates. A comprehensive analysis of the literature on the interpretation of the spectra of surface compounds on oxides is presented. This highly illustrated and extensively referenced volume is intended for specialists working in the fields of surface physical chemistry, surface and materials sciences, and adsorption phenomena and is essential reading for those involved in the heterogeneous catalysis by transition metal-oxides.