NDLI: Heterometallic Modular Metal–Organic 3D Frameworks Assembled via New Tris-β-Diketonate Metalloligands: Nanoporous Materials for Anion Exchange and Scaffolding of Selected Anionic Guests

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Heterometallic Modular Metal–Organic 3D Frameworks Assembled via New Tris-β-Diketonate Metalloligands: Nanoporous Materials for Anion Exchange and Scaffolding of Selected Anionic Guests

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Heterometallic Modular Metal–Organic 3D Frameworks Assembled via New Tris-β-Diketonate Metalloligands: Nanoporous Materials for Anion Exchange and Scaffolding of Selected Anionic Guests

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	Carlucci, Lucia Maggini, Simona Ciani, Gianfranco Proserpio, Davide M. Visconti, Marco
Description	Author Affiliation: Carlucci L ( Dipartimento di Chimica Strutturale e Stereochimica Inorganica, Università degli Studi di Milano, Via Venezian 21, 20133 Milano, Italy. lucia.carlucci@unimi.it)
Abstract	The modular engineering of heterometallic nanoporous metal–organic frameworks (MOFs) based on novel tris-chelate metalloligands, prepared using the functionalised β-diketone 1,3-bis(4′-cyanophenyl)-1,3-propanedione (HL), is described. The complexes $[M^{III}L_{3}]$ $(M=Fe^{3+},$ $Co^{3+})$ and $[M^{II}L_{3}](NEt_{4})$ $(M=Mn^{2+},$ $Co^{2+},$ $Zn^{2+},$ $Cd^{2+})$ have been synthesised and characterised, all of which exhibit a distorted octahedral chiral structure. The presence of six exo-oriented cyano donor groups on each complex makes it a suitable building block for networking through interactions with external metal ions. We have prepared two families of MOFs by reacting the metalloligands $[M^{III}L_{3}]$ and $[M^{II}L_{3}]^{−}$ with many silver salts AgX $(X=NO_{3}^{−},$ $BF_{4}^{−},$ $PF_{6}^{−},$ $AsF_{6}^{−},$ $SbF_{6}^{−},$ $CF_{3}SO_{3}^{−},$ tosylate), specifically the $[M^{III}L_{3}Ag_{3}]X_{3}⋅Solv$ and $[M^{II}L_{3}Ag_{3}]X_{2}⋅Solv$ network species. Very interestingly, all of these network species exhibit the same type of 3D structure and crystallise in the same trigonal space group with similar cell parameters, in spite of the different metal ions, ionic charges and $X^{−}$ counteranions of the silver salts. We have also succeeded in synthesising trimetallic species such as $[Zn_{x}Fe_{y}L_{3}Ag_{3}](ClO_{4})_{(2x+3y)}⋅Solv$ and $[Zn_{x}Cd_{y}L_{3}Ag_{3}](ClO_{4})_{2}⋅Solv$ (with x+y=1). All of the frameworks can be described as sixfold interpenetrated pcu nets, considering the $Ag^{+}$ ions as simple digonal spacers. Each individual net is homochiral, containing only Δ or Λ nodes; the whole array contains three nets of type Δ and three nets of type Λ. Otherwise, taking into account the presence of weak AgC σ bonds involving the central carbon atoms of the β-diketonate ligands of adjacent nets, the six interpenetrating pcu networks are joined into a unique non-interpenetrated six-connected frame with the rare acs topology. The networks contain large parallel channels of approximate hexagonal-shaped sections that represent 37–48 % of the cell volume and include the anions and many guest solvent molecules. The guest solvent molecules can be reversibly removed by thermal activation with retention of the framework structure, which proved to be stable up to about 270 °C, as confirmed by TGA and powder XRD monitoring. The anions could be easily exchanged in single-crystal to single-crystal processes, thereby allowing the insertion of selected anions into the framework channels.
ISSN	09476539
e-ISSN	15213765
Journal	Chemistry - A European Journal
Issue Number	41
Volume Number	16
Language	English
Publisher	Wiley-VCH;ChemPubSoc Europe
Publisher Date	2010-11-02
Publisher Place	Germany
Access Restriction	Open
Subject Keyword	Chemistry
Content Type	Text
Resource Type	Article
Subject	Organic Chemistry Catalysis

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