高等学校化学学报 ›› 2005, Vol. 26 ›› Issue (1): 78.

• 研究简报 • 上一篇    下一篇

Schiff碱双核配合物的磁性及模拟甲烷单加氧酶催化性能的研究

陈新斌1, 廖代正2, 孙咏芬1, 胡新娟1, 杨艳1, 朱申杰2   

  1. 1. 上海师范大学生命与环境科学学院,上海 200234;
    2. 南开大学化学系,天津 300071
  • 收稿日期:2003-12-11 出版日期:2005-01-10 发布日期:2005-01-10
  • 通讯作者: 陈新斌(1961年出生),男,博士,副教授,主要从事仿生催化研究.E-mail:xbchen@shtu.edu.cn E-mail:xbchen@shtu.edu.cn
  • 基金资助:

    国家自然科学基金(批准号:29472055);上海市高等学校科学技术发展基金(批准号:03DZ14)资助

Magnetic and Biomimetic Catalytic Properties of New Schiff Base Dinuclear Complexes as Model Compounds of Methane Monooxygenase

CHEN Xin-Bin1, LIAO Dai-Zheng2, SUN Yong-Fen HU Xin-Juan1, YANG Yan1, ZHU Shen-Jie1   

  1. 1. College of Biotechnology and Environment Science, Shanghai Normal University, Shanghai 200234, China;
    2. Department of Chemistry, Nankai University, Tianjin 300071, China
  • Received:2003-12-11 Online:2005-01-10 Published:2005-01-10

关键词: Schiff碱, 双核配合物, 磁交换作用, 拟酶催化, 协同作用

Abstract: This paper reports the biomimetic catalytic properties of new Schiff base mononuclear complexes MH2LM = Mn(Ⅱ), Fe(Ⅲ)Cl, Cr(Ⅲ)Cl, Cu(Ⅱ), Co(Ⅱ), Ni(Ⅱ), Zn(Ⅱ); L=bis[ N,N'-ethylene-2,2'-(phenylmethylene)bis(3,4-dimethylpyrrole-5-aldimino)] and dinuclear complexes MnML[M=Mn(Ⅱ), Fe(Ⅲ)Cl, Cr(Ⅲ)Cl, Cu(Ⅱ), Co(Ⅱ), Ni(Ⅱ), Zn(Ⅱ)] for studying the monooxygenation of cyclohexane with PhIO and magnetic properties of the dinuclear complexes. The investigation of the magnetic properties(4—300 K) of the dinuclear complexes revealed that their antiferromagnetic spin exchange with J varied from -10.49 to -0.482 cm -1 except MnZnL, and antiferromagnetic spin exchange decreased in the order: Mn(Ⅱ)-Cu(Ⅱ)>Mn(Ⅱ)-Ni(Ⅱ)>Mn(Ⅱ)-Mn(Ⅱ)>Mn(Ⅱ)-Fe(Ⅲ)>Mn(Ⅱ)-Co(Ⅱ)>Mn(Ⅱ)-Cr(Ⅲ). The yield determination of monooxygenation of cyclohexane indicated that the catalytic reactivity of the dinuclear complex was better than that of the corresponding mononuclear complex, so we supposed that there was some cooperative action between the two metals in these dinuclear complexes. It was found that the cooperation lay in the decreasing order: Mn-Fe>Mn-Cr>Mn-Cu>Mn-Mn>Mn-Co>Mn-Ni>Mn-Zn. It seems that this cooperation increased with the increase of the number of unpaired d electrons and the magnetic exchange between the two metals in these dinuclear complexes.

Key words: Schiff base, Dinuclear complexes, Magnetic exchange, Biomimetic catalysis, Synergetic function

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