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三脚式tris-tacn和tris-dpa平台用于组装酸盐模板三金属中心

Rui Cao¹, Peter Müller, Stephen J Lippard

¹Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA.

Journal of the American Chemical Society

|November 25, 2010

概括

研究人员开发了新的三脚连接体,以创建模仿生物三金属中心参与酸盐代谢的金属集群. 这些新型集群在催化酸盐水解反应方面表现有前途.

科学领域:

协调化学协调化学
生物有机化学生物有机化学
超分子化学超分子化学

背景情况:

生物系统利用三金属中心进行酸盐代谢.
设计合成类似物来模仿这些活性位点对于理解它们的功能至关重要.
多牙三脚连接体为构建复杂金属组件提供了多功能平台.

研究的目的:

为组装高核度金属集群设计新的多牙三脚联体.
为了合成和结构性地描述离散的三甲酸盐/酸盐单位.
创建生物相关酸盐代谢三金属中心的合成模型.

主要方法:

合成了两种新型三脚体连接体:N(CH2-m-C6H4-CH2tacn) 3 (L1) 和N(CH2-o-C6H4-CH2N(CH2py) 2) 3 (L2). 这两种新型三脚体连接体是:N(CH2-m-C6H4-CH2tacn) 3 (L1) 和N(CH2-o-C6H4-CH2N(CH2py) 2) 3 (L2).
使用这些连接物与酸盐或酸盐组合金属集群.
四种合成化合物的结构特征: [CuIICl3HPO4L1]PF6 (1), [CuIICl3HAsO4L1]PF6 (2), Na2MnIII6MnII2H2O2HPO4和 [CoII3H2PO4]Cl2MeCNL2PF6 (4).
对4-尼托芬酸的水解进行催化研究.

主要成果:

成功合成并对四种离散的三金属酸盐/酸盐化合物进行结构性表征.
证明三脚体连接体平台能够组装{M3{EO4}}单元的能力.
在酸盐代谢蛋白中的三金属活性位点的结构模仿.
三铜复合体1在酸盐水解中表现出较高的催化效率,与单铜类型相比.

结论:

这种新型的三脚体连接体平台有效地构建{M3{EO4}}单元.
这些合成集群为生物三金属活性站点提供了有价值的结构模型.
开发的铜复合体显示了酸水解中催化应用的潜力.

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