| 摘要: | 本論文合成一系列兒茶酚1,2-雙加氧酶之功能性模型鐵(III)錯合物錯合物且性質由X-ray單晶繞射儀、UV-Vis光譜、元素分析儀及電化學方法來分析。
酵素-受質型錯合物及配位基:
(1) [Fe(L1)(C6Br4O2)]
(2) [Fe(L1)(C6Cl4O2)]
(3) [Fe(L2)(C6Cl4O2)]
(4) [Fe(L3)(C6Cl4O2)]
(5) [Fe(L4)(C6Cl4O2)]
L1: 2-{[2-(2-diethylamino-ethylamino)-ethylimino]-methyl}-phenol
L2: 2-{[2-(2-diethylamino-ethylamino)-ethylimino]-methyl}-5-bromo-phenol
L3: 2-{[2-(2-diethylamino-ethylamino)-ethylimino]-methyl}-4,6-methoxy-phenol
L4: 2-{[2-(2-diethylamino-ethylamino)-ethylimino]-methyl}-3-methoxy-phenol
加入四種不同的兒茶酚陰離子tetrabromocatechol(TBC), tetrachlorocatechol(TCC), catechol(HC),和3,5-di-tert-butylcatechol(3,5-DTBC)與[Fe(L1~4)Cl2]反應，可藉由電子吸收光譜發現兩個新生成兒茶酚到鐵(III)的電子轉移，根據吸收位置與路易士酸性的關係可發現，路易士酸性越強的錯合物[Fe(L2) 3,5-DTBC]有較佳的兒茶酚1,2-雙加氧霉的催化反應性。
A seiries of iron(III) complexes as funtionl model compounds for catechol 1,2-dioxygenases (intradiol cleavage) were synthesized and characterized by X-ray
single crystal diffraction, UV-Vis spectroscopy, element analyzer, and electronchemical analysises.Enzyme-substrate complexes and ligands:
(1) [Fe(L1)(C6Br4O2)]
(2) [Fe(L1)(C6Cl4O2)]
(3) [Fe(L2)(C6Cl4O2)]
(4) [Fe(L3)(C6Cl4O2)]
(5) [Fe(L4)(C6Cl4O2)]
L1: 2-{[2-(2-diethylamino-ethylamino)-ethylimino]-methyl}-phenol
L2: 2-{[2-(2-diethylamino-ethylamino)-ethylimino]-methyl}-5-bromo-phenol
L3: 2-{[2-(2-diethylamino-ethylamino)-ethylimino]-methyl}-4,6-methoxy-phenol
L4: 2-{[2-(2-diethylamino-ethylamino)-ethylimino]-methyl}-3-methoxy-phenol
Catechol 1,2-dioxygenase reactivity has been performed by electronic spectrum in methanol/acetonitrile solutions. The solutions are contained [Fe(L1~4)Cl2] with catecholate anions of tetrabromocatechol(TBC), tetrachlorocatechol(TCC),catechol(HC), and 3,5-di-tert-butylcatechol(3,5-DTBC). The results show that the high lewis acidity iron(III) complexes [Fe(L2) 3,5-DTBC] exhibits the higher catechol 1,2-dioxygenase reactivity. |
