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Synthesis And Characterization Of New Asymmertrical Methane Momooxygenase-like Model Complexes Chen Mo

Posted on:2003-04-29Degree:MasterType:Thesis
Country:ChinaCandidate:M ChenFull Text:PDF
GTID:2121360062980674Subject:Organic Chemistry
Abstract/Summary:PDF Full Text Request
Methane Momooxygenase(MMO) can selectively catalyze some organic molecules (for instance, n-alkanes, n-alkenes, alcohols, phenols, halohydrocarbon, ethers, alicyclic, aromatic and heterocyclic compounds, etc.) into corresponding oxygen-containing products under moderate conditions, which affords an excellent model for new biomimetic catalysts. According to the structure of MMO's active site, new enzyme-like catalysts with high efficiency are developed. At the same time, it is important for understanding MMO's complexes structure , analytical properties, even vital phenomenon that people design and synthesize the similar model complexes with low molecular weight for enzyme's active site. The structure and functional mimic of MMO with binuclear and their model complexes have been an active frontier and a challenge in bionomy and chemistry. This study enriches biology, bionics, chemistry, enzymatic chemistry, coordination chemistry and relame fields.The first section is a review in which the research progress on MMO has been introduced in five aspects such as resource, existent form, component, structure, and function of MMO all over the world, There are two forms of MMO. One is the pMMO. and the other is sMMO. The later consists three components such as MMOH. MMOB. and MMOR. MMOH is the most important component, which consists of three subunits a, p, and y. The active site, located at the a-subunit, contains a carboxylate-bridged diiron core where the activition of O2 and hydroxylation of C-H bond take place. Secondly, we briefly recite investigative significance, history and current situation of chemistry simulation and model complexes' catalysis function study. The mimic of MMO can be divided into structure and functional mimic. The mimics of the active intermediate, such as P and Q. during the catalytic process. In this part, many creative research works have been carried out by experiment teams leaded by S. J. Lippard, L.Que Jr.. etc.The binuclear model complexes designed and synthesized as model compoundsof MMO in our article own different coordinate circumstance and chiral, which have not been reported. They closely resemble MMO in the aspects of structure compared with other Methane Momooxygenase-like systems. It is important for understanding MMO and its asymmetrical catalyst and different function of asymmetrical diiron core during activating and transferring of oxygen. All compounds were characterized by elementary analysis, mass spectra, infrared spectra, ultraviolet-visible spectra, and nuclear magnetic resonance spectra. The results indicate that the structure of aim compound is coincident with expectation. In addition, conditions of the reactions involved in synthetic route, such as alkylation of 4-hydroxy-benzaldehyde, chloromethylation, substitution reaction, hydrolyzation, formation and reduction of Schiffs base, as well as the formation of complexes (including reaction time, temperature, ratio of reactants, selectivity of solvent, purification of product) have been investigated.
Keywords/Search Tags:Methane Momooxygenase, diiron complex, chiral biomimetic, catalvsis
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