Selective assembly and disassembly of a water-soluble Fe10L15 prism.
Selective assembly and disassembly of a water-soluble Fe10L15 prism.
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DOI：
10.1002/anie.201209694
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发表时间：
2013-04
影响因子：
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通讯作者：
S. Zarra;J. Clegg;J. Nitschke
中科院分区：
文献类型：
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作者：
S. Zarra;J. Clegg;J. Nitschke
Significant attention has been recently given to the synthesis of new metal–organic architectures, which have found applications in molecular recognition, reactivity modulation, and catalysis.[1] The assembly of structures such as tetrahedra [2] and cubes [3] is increasingly practical for metal–organic chemists. However, more complex architectures remain elusive.[4] Others [5] and our group [6] have prepared a variety of metal–organic capsules through subcomponent self-assembly. Tetrahedra [7] and more complex prismatic structures,[7b, 8] displaying facial (fac) and meridional (mer) coordination of ligands to octahedral metal centers, have been made by us through the assembly of various metal ions with linear dialdehydes and monoamines. However, so far the complementary diamine–monoaldehyde motif has afforded only tetrahedra.[9] A new diamine ligand, 2, 2’-bis (hydroxymethyl) benzidine (1), designed with the aim of preparing a cationic watersoluble tetrahedron, has displayed a versatile solubility, which allowed the exploration of self-assembly in various reaction media. This has enabled us to find experimental conditions that would favor mer over fac stereochemistry at the metal centers, thus increasing the structural complexity of the final assembly.[7b, 8a]Herein we report the preparation of an FeII 4L6 tetrahedron, 2, as well as a water-soluble FeII 10L15 prism, 3, from the same starting materials. Either 2 or 3 could be obtained by changing the reaction medium, and 4-methoxyaniline was observed to react selectively with 3 in the presence of 2, thereby resulting in the complete disassembly of 3 to give mononuclear complex 4 and free 1 and 2 in solution. The reaction of 2, 2’-bis (hydroxymethyl) benzidine (1)(6equiv) and 2-formylpyridine (12equiv) in presence of
