6533b81ffe1ef96bd1278fcb
RESEARCH PRODUCT
Self-assembly of catalytically-active supramolecular coordination compounds within metal-organic frameworks
Richard E. P. WinpennyAntonio Leyva-pérezEmilio PardoDonatella ArmentanoLucas H. G. KalinkeJesús Ferrando-soriaAntonio FernandezMarta MonRosa AdamRossella GrecoJ. Alejandro Vidal-moyaAntonio Doménech-carbósubject
Mechanistic characterizationMetalationCavitySupramolecular chemistryQuímica organometàl·licaNanoreactor010402 general chemistry7. Clean energy01 natural sciencesBiochemistryCatalysisCoordination complexSupramolecular assemblyClustersQUIMICA ORGANICAColloid and Surface ChemistryOxidationPolyhedraConstructionchemistry.chemical_classificationChemistryCagesGeneral ChemistryCombinatorial chemistry0104 chemical sciencesEfficientAlkynesMetal-organic frameworkCatalystSelf-assemblySupramolecular catalysisdescription
[EN] Supramolecular coordination compounds (SCCs) represent the power of coordination chemistry methodologies to self-assemble discrete architectures with targeted properties. SCCs are generally synthesized in solution, with isolated fully coordinated metal atoms as structural nodes, thus severely limited as metal-based catalysts. Metal-organic frameworks (MOFs) show unique features to act as chemical nanoreactors for the in situ synthesis and stabilization of otherwise not accessible functional species. Here, we present the self-assembly of Pd-II SCCs within the confined space of a pre-formed MOF (SCCs@MOF) and its post-assembly metalation to give a Pd-II-Au-III supra molecular assembly, crystallography underpinned. These SCCs@MOFs catalyze the coupling of boronic acids and/or alkynes, representative multi-site metal-catalyzed reactions in which traditional SCCs tend to decompose, and retain their structural integrity as a consequence of the synergetic hybridization between SCCs and MOFs. These results open new avenues in both the synthesis of novel SCCs and their use in heterogeneous metal-based supramolecular catalysis.
year | journal | country | edition | language |
---|---|---|---|---|
2019-06-13 |