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The subject of this research project was to investigate the catalytic properties of a new class of materials, transition metal carbides and nitrides, for treatment of coal liquid and petroleum feedstocks. The main objectives were: (1) preparation of catalysts in unsupported and supported form; (2) characterization of the materials; (3) evaluation of their catalytic properties in HDS and HDN; (4) measurement of the surface properties; and (5) observation of adsorbed species. All of the objectives were substantially carried out and the results will be described in detail below. The catalysts were transition metal carbides and nitrides spanning Groups 4--6 in the Periodic Table. They were chosen for study because initial work had shown they were promising materials for hydrotreating. The basic strategy was first to prepare the materials in unsupported form to identify the most promising catalyst, and then to synthesize a supported form of the material. Already work had been carried out on the synthesis of the Group VI compounds Mo2C, Mo2N, and WC, and new methods were developed for the Group V compounds VC and NbC. All the catalysts were then evaluated in a hydrotreating test at realistic conditions. It was found that the most active catalyst was Mo2C, and further investigations of the material were carried out in supported form. A new technique was employed for the study of the bulk and surface properties of the catalysts, near edge x-ray absorption spectroscopy (NEXAFS), that fingerprinted the electronic structure of the materials. Finally, two new research direction were explored. Bimetallic alloys formed between two transition metals were prepared, resulting in catalysts having even higher activity than Mo2C. The performance of the catalysts in hydrodechloration was also investigated.
Our project deals with the investigation of a new class of catalysts for processing coal liquids. The catalysts are supported carbides and nitrides of transition metals. These compounds are unique because they have properties similar to those of the precious metals, but are resistant to sulfur. Because they have high hydrogenation activity in the presence of sulfur, they are ideal for coal processing. For our initial work we have decided to start with unsupported carbides and nitrides in order to identify the best possible composition for work with supported catalysts. The research includes synthesis, characterization, and testing of the compounds.
Coal is more abundant than petroleum and natural gas. Further, coal is not localized but can be used by many more countries than petroleum. Therefore, if we can establish coal utilization technology, coal will bring about a great contribution to human life and society. On the other hand, shortage of petroleum and natural gas are anticipated in the second half of the 21st century. To compensate, the use of coal is expected to gradually increase during the 21st century. In the future, the development of the coal utilization technology will become more and more important to insure the supply of liquid fuels for transportation and carbon sources for the manufacture of chemicals and plastic materials.In order to develop such technologies, the elucidation of the structure of coal is a fundamental area of study. Further, more efficient coal utilization technology must be established to meet environmental legislation. One of the key technologies for this purpose is catalysis. This volume provides detail of the basic and practical aspects of the science and technology of coal utilization with and without catalysts. The actual structure of coal, the chemistry included in the reactivity of coal, the methods to elucidate the structure of coal and re-action mechanisms of coal conversion, the most important catalyst for converting coal to liquid and gas, the role of the catalysts in coal conversion, the problems in the process engineering, and how to meet environmental regulations are discussed in detail. The recent progress in studies on the structure and reactivity of coal made over the last century is summarized and reviewed with emphasis on both fundamental and applied aspects of the science and technology for coal processing in the presence and absence of catalysts. * This book highlights the issues faced in trying to discover more efficient coal utilization technology.* Provides detailed discussion on how to meet environmental regulations and legislation. * Fills the gap between both the scientific and practical sides of coal utilization with and without catalysts.
The main objective of this project was to study transition metal carbides and nitrides as catalysts for hydroprocessing. In particular, the goals were to study the solid-state transformations that occur during synthesis of the compounds using a temperature-programmed method, and to investigate the catalytic properties of the materials for the upgrading of model coal liquids at realistic process conditions.
Catalysis in Coal Conversion tells of the advances in catalysis and related fields in order to suggest decisive contributions towards finding solutions for the catalytic problems of coal conversion. The book also details the preparation, mode of action, and behavior of various catalysts. The book is divided into three major parts, the first of which discusses the advances of catalysis during the last two decades including the bimetallic catalysts. Other areas of interest covered in the first part include characterization and preparation of catalysts; poisoning and regeneration; and reaction mechanisms. Part II summarizes the developments of related disciplines such as reactor engineering, inorganic and organometallic chemistry, materials science, and surface science. The last part serves as a review of the nature of the different coal liquefaction processes and their products. This book is of value to chemists and chemical engineers involved in coal conversion or fuel processing researches. Chemistry teachers and students can also use this book for examples of practical applications in industrial catalysis.
Work involving the synthesis of monometallic transition metal carbides supported on alumina is described. The catalysts have excellent initial activity in the hydrodechlorination of CCl2F2 (CFC 12), but deactivate with time by the deposition of carbon. Initial work on the preparation of unsupported bimetallic oxynitrides is also described.