Metal-ligand Lability and Ligand Mobility Enables Framework Transformation via Ligand Release in a Family of Crystalline 2D Coordination Polymers

金属-配体不稳定性及配体流动性使得一类二维晶体配位聚合物能够通过配体释放实现框架转变

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Abstract

A family of seven silver(I)-perfluorocarboxylate-quinoxaline coordination polymers, [Ag(4) (O(2) CR(F) )(4) (quin)(4) ] 1-5 (R(F) =(CF(2) )(n-1) CF(3) )(4) , n=1 to 5); [Ag(4) (O(2) C(CF(2) )(2) CO(2) )(2) (quin)(4) ] 6; [Ag(4) (O(2) CC(6) F(5) )(4) (quin)(4) ] 7 (quin=quinoxaline), denoted by composition as 4 : 4 : 4 phases, was synthesised from reaction of the corresponding silver(I) perfluorocarboxylate with excess quinoxaline. Compounds 1-7 adopt a common 2D layered structure in which 1D silver-perfluorcarboxylate chains are crosslinked by ditopic quinoxaline ligands. Solid-state reaction upon heating, involving loss of one equivalent of quinoxaline, yielding new crystalline 4 : 4 : 3 phases [Ag(4) (O(2) C(CF(2) )(n-1) CF(3) )(4) (quin)(3) ](n) (8-10, n=1 to 3), was followed in situ by PXRD and TGA studies. Crystal structures were confirmed by direct syntheses and structure determination. The solid-state reaction converting 4 : 4 : 4 to 4 : 4 : 3 phase materials involves cleavage and formation of Ag-N and Ag-O bonds to enable the structural rearrangement. One of the 4 : 4 : 3 phase coordination polymers (10) shows the remarkably high dielectric constant in the low electric field frequency range.

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