The Activation And Conversion Of Small Molecular CO₂ And CH₄

The conversions of carbon dioxide and methane are important and new regions in C₁ chemistry, the activations of these two stablest chemical substances are also the challengingest theoretic tasks in chemistry field. It's lucky for me to participate in two tasks correlative to the research of these two moleculars in the period of studying for my doctor's degree. My Ph. D. dissertation is made up of two parts: Part â…  . Supercritical carbon dioxide hydrogenation to formic acid using functionalized silica supported ruthenium catalyst. Part â…¡ . Methane dehydro-aromatization using HZSM-5 supported molybdenum catalyst under O₂-free condition. The first part is the main research work of my studying period.Part â…  . Supercritical carbon dioxide hydrogenation to formic acid using organic functionalized silica supported ruthenium catalystThe synthesis of formic acid from carbon dioxide hydrogenation is not only an atom economic reaction, but also according with the developing trend of green chemistry. If carbon dioxide is in supercritical condition, it will increase the solubility of hydrogen in it. On the other hand, to overcome the disadvantage of difficult separation and recovery when using homogeneous catalyst effective to this reaction, we combine the immobilization of homogeneous catalyst bearing high activity and high selectivity with the technique of applying supercritical fluid. We developed ruthenium complexes supported on functionalized silica with mechanically, chemically and thermally stability, obtained higher activity than homogeneous counterparts. Simultaneously, the immobilized catalyst exhibited good recoverability and reusability. We also applied the techniques of element analysis, BET, FT-IR, ICP-AES, UV-VIS, XPS and quantum chemistry theoretic calculation to characterize...