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Directed Assembly of acac-Based Complexes by Deliberately Fine-Tuning Electrostatic Molecular-Recognition Events
journal contribution
posted on 2016-11-18, 14:34 authored by Boris-Marko Kukovec, Magdalena Malik, Ivan Kodrin, Christer B. Aakeröy, Marijana ĐakovićA protocol for supramolecular synthesis
of one-dimensional (1-D)
chains comprising octahedral metal-complexes linked by predictable
hydrogen bonds has been established. The synthetic process was refined
by adjusting the reactants in an iterative manner to shift the magnitude
of the electrostatic potential surfaces of competing hydrogen-bond
acceptor sites thereby avoiding the formation of unwanted products.
The synthetic space for this study was provided by a combination of
reactants: Co(II)/Ni(II) cations and acac-based anions (dibenzoylmethanato,
dbm/hexafluoracetylacetonato, hfac) combined with a series of pyridine-oxime
ligands (4-pyridinealdoxime, 4-Hoxpy; methyl 4-pyridyl ketoxime, 4-Meoxpy;
3-pyridinealdoxime, 3-Hoxpy; methyl 3-pyridyl ketoxime, 3-Meoxpy).
The initial self-assembly process did not produce the desired 1-D
chains held together by oxime···oxime hydrogen bonds;
however, through deliberate fine-tuning of the reactants, a robust
synthetic protocol for the reproducible synthesis of the correct supramolecular
products was obtained. The successful synthetic protocol was arrived
at in much the same way as organic synthesis is systematically altered
and refined in response to product yields.
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3- pyridinealdoximehydrogen-bond acceptor sitesreactantsacac-Based Complexes4- Hoxpy4- Meoxpyiterative manneracac-based anionsself-assembly processsupramolecular productsproduct yieldsMolecular-Recognition Eventshydrogen bondsmethyl 4- pyridyl ketoxime3- Hoxpy3- Meoxpyoctahedral metal-complexessupramolecular synthesismethyl 3- pyridyl ketoxime1- D chains
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