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Tungsten structure factor activity Biomimetic Synthesis and Characterization

Author: WeiChunXia
Tutor: LuXiaoMing
School: Capital Normal University
Course: Physical and chemical
Keywords: Transferase activity of tungsten oxide structure factor biomimetic complexes Crystal structure EPR IR NMR TEM SEM
CLC: O629.8
Type: Master's thesis
Year: 2007
Downloads: 35
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Abstract


Tungsten is a biologically active trace elements of life, tungsten oxide in biological systems COMT of nitrogen, sulfur and carbon in the natural cycle plays an important catalytic role. With tungsten enzymes in vivo effect gradually get attention, and its simulation capabilities tungsten complexes in exploring the physiological activity of the enzyme and catalytic mechanism of the outstanding contributions made to make tungsten oxide transferase activity biomimetic synthesis of structure factors, physiological Catalytic Mechanism of activity and become a research hotspot. Tungsten enzymes by X-ray crystal structure analysis study showed that the activity of the metal tungsten and the structure factor S on dithiol alkenyl ligand atoms are formed. Polyhydric phenol due to its anti-tumor and anti-viral activity, and its derivatives has been a research focus. Polyhydric phenol as an antioxidant, can affect the bioavailability of the metal body, in addition to metal - catechol complexes present interesting electronic effects. This electronic effect and multivalent metal charge distribution on the ligand, is due to the frontier orbitals and quinine metal rail delicate balance exists between the energy generated, the organism is considered to ion transport and catechol / Kui Ning enzymes and model biological molecules. In this paper, catechol ligands synthesized a series of tungsten oxygen transfer complexes biomimetic active center of the enzyme, and characterized by IR, 1 HNMR spectroscopy and EPR such characterization and crystal structure determination, main contents are as follows: 1. Containing an ortho-substituted catechol ligands in methanol and acetonitrile mixed solvent (n-Bu 4 N) 4 [W 10 O 32 ] response, respectively, to the system 1,3 - propanediamine, 1,2 - propylene diamine and ethylene diamine, have different shapes showed chiral octahedral type mononuclear tungsten complexes, (NH 3 CH 2 CH 2 CH 2 NH 2 ) 2 [WO 2 (C 6 H 4 O 2 ) 2 ] (1), [(NH 3 CH 2 CH (NH 2 ) CH 3 ) 2 [WO 2 (C 6 H 4 O 2 < / sub>) 2 )] (2) and (NH 3 CH 2 CH 2 NH 2 ) 3 [W Ⅴ O 2 (C 6 H 4 O 2 ) 2 ] (3). (A) EPR: Although the central ion of valence different, EPR signals are different, but the same structure as the ligand. W Ⅴ compounds due to d 1 with EPR electron configuration and activity, and milk zeaxanthin oxidase EPR showed similarity between tungsten enzyme active center during oxygen transfer electron transfer, ligand field unchanged. (B) NMR: NMR study of the use of complexes 2 interaction with ATP and found that chiral characteristics 1,2 - propanediamine and catechol benzene 1 H chemical shift ATE mixed with large differences were shown before and after analysis reveals that: complexes of metal ions in the D 2 O Most are W (Ⅴ) valence state exists, but with the ATP coexistence into W (Ⅵ), and with the understanding from the ligand occurs. 2. Catechol as ligands in methanol mixed solvent of acetonitrile and NaWO 4 · 2H 2 O reaction, respectively, added to the system 1,3 - propanediamine , 1,2 - propylene diamine, ethylene diamine, get three structures distinct product, (NH 3 CH 2 CH 2 CH 2 NH 3 ) 2 {Na 2 [(C 6 H < sub> 4 O 2 ) 2 ] (C 6 H 4 O 2 H) 2 } (4) [NH 3 CH 2 CH (NH 2 ) CH 3 ] {WO 2 (C 6 H 4 O 2 ) 2 Na [NH 2 CH 2 CH (NH 2 ) CH 3 ]} < sub> n (5), (NH 2 CH 2 CH 2 NH 2 ) < sub> 2 {Na 2 [μ 2 - (C 6 H 6 O 2 ) 2 ] (C 6 H 4 OOH) 2 } (6). (A) X diffraction: complexes (6) as a separate two sodium metal clusters, and (5) for the one-dimensional chain structure. (B) NMR: complexes (6) Solid and heavy water 13 C NMR comparison shows that bridging ligand μ 2 - (C 6 H 6 O 2 ) and end-ligand (C 6 H 4 OOH) - in solution rapid exchange occurs.

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