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Issue 40, 2015

Coordination polymers from a highly flexible alkyldiamine-derived ligand: structure, magnetism and gas adsorption studies

Author affiliations

Abstract

The synthesis and structural, magnetic and gas adsorption properties of a series of coordination polymer materials prepared from a new, highly flexible and internally functional tetrakis-carboxybenzyl ligand H4L derived from 1,2-diaminoethane have been examined. The compound poly-[Ni3(HL)2(OH2)4]·2DMF·2H2O 1, a two-dimensional coordination polymer, contains aqua- and carboxylato-bridged trinuclear NiII clusters, the magnetic behaviour of which can be well described through experimental fitting and ab initio modelling to a ferromagnetically coupled trimer with a positive axial zero-field splitting parameter D. Compound poly-[Zn2L]·2DMF·3H2O 2, a three-dimensional coordination polymer displaying frl topology, contains large and well-defined solvent channels, which are shown to collapse on solvent exchange or drying. Compound poly-[Zn2(L)(DMSO)4]·3DMSO·3H2O 3, a highly solvated two-dimensional coordination polymer, displayed poor stability characteristics, however a structurally related material poly-[Zn2(L)(bpe)(DMSO)2]·DMSO·3H2O 4 was prepared under similar synthetic conditions by including the 1,2-bis(4-pyridyl)ethylene bpe co-ligand. Compound 4, containing small one-dimensional solvent channels, shows excellent structural resilience to solvent exchange and evacuation, and the evacuated material displays selective adsorption of CO2 over N2 at 273 K in the pressure range 0–1 atm. Each of the coordination polymers displays subtle differences in the conformation and binding mode of the ligand species, with switching between two distinct conformers (X-shaped and H-shaped), as well as a variable protonation state of the central core, with significant effects on the resulting network structures and physical properties of the materials.

Graphical abstract: Coordination polymers from a highly flexible alkyldiamine-derived ligand: structure, magnetism and gas adsorption studies

Supplementary files

Article information


Submitted
18 Jun 2015
Accepted
16 Jul 2015
First published
17 Jul 2015

Dalton Trans., 2015,44, 17494-17507
Article type
Paper

Coordination polymers from a highly flexible alkyldiamine-derived ligand: structure, magnetism and gas adsorption studies

C. S. Hawes, N. F. Chilton, B. Moubaraki, G. P. Knowles, A. L. Chaffee, K. S. Murray, S. R. Batten and D. R. Turner, Dalton Trans., 2015, 44, 17494 DOI: 10.1039/C5DT02323H

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