Assembly Synthesis And Catalytic Behavior Of Simulated-Enzyme Activated Materials

The thesis is concerned with the preparation and biomimetic catalysis of simulated enzymes. The new molecular designing model of mono-oxygenase cytochrome P450, the pillared layered simulated structure, was put forward to the investigation of simulated enzymes. Layered host materials with the rigidity of layer skeleton and expandable interlayer structure was used for the intercalation of active species. The technique of molecular assembly synthesis was applied to develop the front investigation of simulated enzymes.With the help of the innovative molecular designing model and molecular assembly technique, the intercalation of porphyrins and phthalocyanines into the interlayer structure of host materials was investigated. The pillared layered structure of simulated enzyme materials can yield the better orientation of the porphyrins and phthalocyanines and the better tuning of the microenvironment around the activate species. The catalysis occurs when reactants go through the pillared layered structure of simulated enzyme materials to come into contact with the active canters. The pillared layered structure of simulated enzyme materials make reactants easier to access to the active centers than the tunnel of the coordination compounds-encapsulated simulated zeolite materials with fixed three dimensional structure.In order to get rid of the difficulties in the in-situ synthesis of larger cyclic coordination compounds and to succeed in the assembly synthesis of a serial of metalloporphyrins and metallophthalocyanines, we used X-ray diffraction and infrared spectrum techniques to fine-tune the in-situ reaction conditions of assembly synthesis and speed up the progress in our research work very much. A variety of modern physical chemical techniques, such as FTIR spectra, solid state UV-Vis spectra, X-ray diffraction spectra, solid state ³¹P NMR spectra, EPR spectra, scanning electronic microscope and so on, were used for the investigation...