Post-Assembly Covalent Di- and Tetracapping of a Dinuclear [Fe2L3]4+ Triple Helicate and Two [Fe4L6]8+ Tetrahedra Using Sequential Reductive Aminations

被引:23
作者
Glasson, Christopher R. K. [1 ]
Meehan, George V. [1 ]
Davies, Murray [1 ]
Motti, Cherie A. [2 ]
Clegg, Jack K. [3 ]
Lindoy, Leonard F. [1 ,4 ]
机构
[1] James Cook Univ, Coll Sci Technol & Engn, Townsville, Qld 4811, Australia
[2] Australian Inst Marine Sci, Townsville, Qld 4810, Australia
[3] Univ Queensland, Sch Chem & Mol Biosci, St Lucia, Qld 4072, Australia
[4] Univ Sydney, Sch Chem, Sydney, NSW 2006, Australia
基金
澳大利亚研究理事会;
关键词
SPIN-CROSSOVER; COMPLEXES; IRON(II); SIZE; NICKEL(II); CATENANES;
D O I
10.1021/acs.inorgchem.5b00940
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
The use of a highly efficient reductive amination procedure for the postsynthetic end-capping of metal-templated helicate and tetrahedral supramolecular structures bearing terminal aldehyde groups is reported. Metal template formation of a [Fe2L3](4+) dinudear helicate and two [Fe4L6](8+) tetrahedra (where L is a linear ligand incorporating two bipyridine domains separated by one or two 1,4-(2,5-dimethoxyaryl) linkers and terminated by salicylaldehyde functions is described. Postassembly reaction of each of these "open" di- and tetranudear species with excess ammonium acetate (as a source of ammonia) and sodium cyanoborohydride results in a remarkable reaction sequence whereby the three aldehyde groups terminating each end of the helicate, or each of the four vertices of the respective tetrahedra, react with ammonia then undergo successive reductive amination to yield corresponding fully tertiary-amine capped cryptate and tetrahedral covalent cages.
引用
收藏
页码:6986 / 6992
页数:7
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