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New Lanthanide Metalloligands and Their Use for the Assembly of Ln–Ag Bimetallic Coordination Frameworks: Stepwise Modular Synthesis, Structural Characterization, and Optical Properties

  • Marco Visconti
    Marco Visconti
    Dipartimento di Chimica, Università degli Studi di Milano, via Golgi 19, 20133 Milano, Italy
  • Simona Maggini
    Simona Maggini
    Dipartimento di Chimica, Università degli Studi di Milano, via Golgi 19, 20133 Milano, Italy
  • Gianfranco Ciani
    Gianfranco Ciani
    Dipartimento di Chimica, Università degli Studi di Milano, via Golgi 19, 20133 Milano, Italy
  • Pierluigi Mercandelli
    Pierluigi Mercandelli
    Dipartimento di Chimica, Università degli Studi di Milano, via Golgi 19, 20133 Milano, Italy
  • Benedetta Del Secco
    Benedetta Del Secco
    Dipartimento di Chimica “Giacomo Ciamician”, Università degli Studi di Bologna, via Selmi 2, 40126 Bologna, Italy
  • Luca Prodi
    Luca Prodi
    Dipartimento di Chimica “Giacomo Ciamician”, Università degli Studi di Bologna, via Selmi 2, 40126 Bologna, Italy
    More by Luca Prodi
  • Massimo Sgarzi
    Massimo Sgarzi
    Dipartimento di Chimica “Giacomo Ciamician”, Università degli Studi di Bologna, via Selmi 2, 40126 Bologna, Italy
  • Nelsi Zaccheroni
    Nelsi Zaccheroni
    Dipartimento di Chimica “Giacomo Ciamician”, Università degli Studi di Bologna, via Selmi 2, 40126 Bologna, Italy
  • , and 
  • Lucia Carlucci*
    Lucia Carlucci
    Dipartimento di Chimica, Università degli Studi di Milano, via Golgi 19, 20133 Milano, Italy
    *E-mail: [email protected]
Cite this: Cryst. Growth Des. 2019, 19, 9, 5376–5389
Publication Date (Web):July 25, 2019
https://doi.org/10.1021/acs.cgd.9b00894
Copyright © 2019 American Chemical Society

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    Abstract

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    Stepwise self-assembly processes using new lanthanide metalloligands (Ln–MLs) and silver salts have been successfully applied to isolate 4f–4d heterometallic coordination networks of four different structural types. In particular, the new lanthanide tetrakis–chelate complexes NEt4[Ln(L1)4] [HL1 = 1,3-bis(4′-cyanophenyl)-1,3-propanedione; Ln = Eu (1a), La (1b), Nd (1c), Tb (1d)] and NEt4[Ln(L2)4] (HL2 = 1,3-bis(4′-pyridyl)-1,3-propanedione; Ln = Eu (1e), Nd (1f)] have been synthesized, characterized, and reacted with different silver salts. The use of NEt4[Ln(L1)4] allowed then to isolate and characterize i) neutral one-dimensional ladder-like species of formula [Ln(L1)4Ag] [Ln = Eu (2a), La(2b), Nd(2c), Tb(2d)] and ii) their supramolecular isomers [Ln(L1)4Ag] [Ln = Eu (3a), La (3b), Nd (3c), Tb (3d)] showing a very unstable 2D network structure, iii) the cationic 2D species [Ln(L1)4Ag2]X [Ln = Eu, X = PF6, CF3SO3, ClO4 (4a4c); Ln = Tb, Nd, La X = PF6 (4d4f)], and, only for lanthanum, iv) a fourth 2D species of formula [La(L1)4(H2O)Ag] (5) and sql topology. Of the eight nitrile groups on the MLs potentially coordinating, only a partial number is used for networking with Ag(I), that is, only two in families 2 and 3 and four in family 4 and in network 5. Finally, the four structural types are rationalized in terms of a new “pincer-like” secondary building unit (SBU) consisting of a silver cation coordinating two central carbon atoms (γ carbon) of two different diketonate ligands on the same ML. Therefore, it is shown that compounds 5, 4, and 23 contain, respectively, none, one, or two of such pincer-like SBUs. The luminescence properties of the Ln–MLs and some of their polymeric species have been also investigated in solution and in the solid state.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.cgd.9b00894.

    • TGA plots; X-ray powder diffraction patterns; representations of molecular and crystal structures; absorption and emission spectra; tables of crystallographic data (PDF)

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    CCDC 19107711910779 contain the supplementary crystallographic data for this paper. These data can be obtained free of charge via www.ccdc.cam.ac.uk/data_request/cif, or by emailing [email protected], or by contacting The Cambridge Crystallographic Data Centre, 12 Union Road, Cambridge CB2 1EZ, UK; fax: +44 1223 336033.

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