Synthesis And Characterization Of Binuclear Complexes And Their Catalytic Activitity Research

Biocatalysts -enzymes are well known for their ability to carry out chemical reactions with high selectivity and high efficiency under ambient conditions. Chemists have long been engaged in studying on the correlation between the structure and function of enzymes, and in prospecting their use in organic synthesis and industrial product Though a lot of research we found the most important thing is to study the coordinate environment of metal in the active site of enzyme, minimize the correspond catalytic systems purposely. In order to simulate the immediate coordination environment of the metallobiosite, the coordination chemists use synthetic analogues derived from small molecular compounds which have more plasticity and simple structure than that of metallobiosite so a lot of low-molecular-weight coordination compounds were prepared . it is of both academic and industrial important.Continuing interest in the design and synthesis of various types of binuclear complexes is mainly due to their potential application as models for binuclear metallobiosites such as methane monooxygenase, tyrosinase, haemocyanin et al. In this paper we describle some of our work aimed at mimicking the methane monooxygenase, tyrosinase and haemocyanin. Three diiron complexes and one binuclear copper were synthesized and well characterized by element analysis, molecular conductivity, IR, Uv-vis, 1H NMR, Electron Paramagnetic Resonance and cyclic voltammetric. The results show that the complexes all have asymmetry chiral structure and their coordination environment are similar to the correspond enzymes. Their catalytic properties in olefin epoxidation were investigated with iodosylbenzene as a terminal oxidant under mild condition.The first chapter concerns the research progress of Methane monooxygenase (MMO) introducing the MMO's resource, existent form, component and catalytic mechanism then haemocyanin and tyrosinase were introduced in the aspects of their structure and functional mechanism. Lastly we reviewed the chemical mimic of the enzyme from structure mimic to functional mimic and its catalytic properties research.Methane monooxygenase which catalyzes the conversion of methane to methanol under mild conditions remains a very interesting theoretical problem and also has important particular implications. In the second part, preparations and characterizations of three different bridged complexes models of MMO are reported .The ligand is obtained by Reimer-Tiemann reaction, Chloromethylation, N-alkation, hydroxylation, reduction reactions. In the synthetic procedure of complexes, we gained three different bridged complexes by changing carboxylate bridges. The structure of the complexesclosely resemble with other MMO-like systems. The compounds have not been reported in the literature.The chemistry of macrocyclic binuclear complexes has been stimulated by a desire to mimic the active sites of some metalloenzymes to search appropriate systems for binding and activating small molecular, and to investigate the mutual influence of two metal centres on the electric, magnetic and redox properties of such systems. So the search for marocycle ligands mimicking the environment of the metals in haemocyanin tyrosinase has resulted in a tremendous upsurge. In the third chapter, the new type of binuclear copper complex was synthesized from dinucleating ligand (2,6-difbrmyl-4-methyl phenol) by reaction with diamine and L-amino acid, Compared with the reported complexes, the complexes is asymmetrical and chiral, the structure is similar to the active sites of haemocyanin , tyrosinase .In the last chapter the complexes' catalytic activities of transferring oxygen atom from PhIO to olefins were tested. The results show that they all have good catalytic properties and are friendly to the environment.