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Hierarchical Self-Assembly of Polyoxometalate-Based Hybrids Driven by Metal Coordination and Electrostatic Interactions: From Discrete Supramolecular Species to Dense Monodisperse Nanoparticles

  • Identification data

    Identifier: imarina:5129726
    Authors:
    Izzet, GuillaumeAbecassis, BenjaminBrouri, DalilPiot, MadeleineMatt, BenjaminSerapian, Stefano ArtinBo, CariesProust, Anna
    Abstract:
    The metal-driven self-assembly processes of a covalent polyoxometalate (POM)-based hybrid bearing remote terpyridine binding sites have been investigated. In a strongly dissociating solvent, a discrete metallomacrocycle, described as a molecular triangle, is formed and characterized by 2D diffusion NMR spectroscopy (DOSY), small-angle X-ray scattering (SAXS), and molecular modeling. In a less dissociating solvent, the primary supramolecular structure, combining negatively charged POMs and cationic metal linkers, further self-assemble through intermolecular electrostatic interactions in a reversible process. The resulting hierarchical assemblies are dense monodisperse nanoparticles composed of ca. 50 POMs that were characterized by SAXS and transmission electron microscopy (TEM). This multiscale organized system directed by metal coordination and electrostatic interactions constitutes a promising step for the future design of POM self-assemblies with controllable structure-directing factors.
  • Others:

    Author, as appears in the article.: Izzet, Guillaume; Abecassis, Benjamin; Brouri, Dalil; Piot, Madeleine; Matt, Benjamin; Serapian, Stefano Artin; Bo, Caries; Proust, Anna;
    Department: Química Física i Inorgànica
    URV's Author/s: Bo Jané, Carles
    Keywords: Systems Scattering Program Metal nanoparticles Macroions Integration scheme Energy Electrostatics Complexes Biological macromolecules Binding sites Approximation Aggregation
    Abstract: The metal-driven self-assembly processes of a covalent polyoxometalate (POM)-based hybrid bearing remote terpyridine binding sites have been investigated. In a strongly dissociating solvent, a discrete metallomacrocycle, described as a molecular triangle, is formed and characterized by 2D diffusion NMR spectroscopy (DOSY), small-angle X-ray scattering (SAXS), and molecular modeling. In a less dissociating solvent, the primary supramolecular structure, combining negatively charged POMs and cationic metal linkers, further self-assemble through intermolecular electrostatic interactions in a reversible process. The resulting hierarchical assemblies are dense monodisperse nanoparticles composed of ca. 50 POMs that were characterized by SAXS and transmission electron microscopy (TEM). This multiscale organized system directed by metal coordination and electrostatic interactions constitutes a promising step for the future design of POM self-assemblies with controllable structure-directing factors.
    Thematic Areas: Química Materiais Interdisciplinar General chemistry Farmacia Engenharias iv Engenharias iii Engenharias ii Colloid and surface chemistry Ciências biológicas ii Ciências biológicas i Ciências agrárias i Ciência de alimentos Chemistry, multidisciplinary Chemistry (miscellaneous) Chemistry (all) Chemistry Catalysis Biochemistry Astronomia / física
    licence for use: https://creativecommons.org/licenses/by/3.0/es/
    Author's mail: carles.bo@urv.cat
    Author identifier: 0000-0001-9581-2922
    Record's date: 2024-09-07
    Papper version: info:eu-repo/semantics/acceptedVersion
    Link to the original source: https://pubs.acs.org/doi/10.1021/jacs.6b00972
    Licence document URL: https://repositori.urv.cat/ca/proteccio-de-dades/
    Papper original source: Journal Of The American Chemical Society. 138 (15): 5093-5099
    APA: Izzet, Guillaume; Abecassis, Benjamin; Brouri, Dalil; Piot, Madeleine; Matt, Benjamin; Serapian, Stefano Artin; Bo, Caries; Proust, Anna; (2016). Hierarchical Self-Assembly of Polyoxometalate-Based Hybrids Driven by Metal Coordination and Electrostatic Interactions: From Discrete Supramolecular Species to Dense Monodisperse Nanoparticles. Journal Of The American Chemical Society, 138(15), 5093-5099. DOI: 10.1021/jacs.6b00972
    Article's DOI: 10.1021/jacs.6b00972
    Entity: Universitat Rovira i Virgili
    Journal publication year: 2016
    Publication Type: Journal Publications
  • Keywords:

    Biochemistry,Catalysis,Chemistry,Chemistry (Miscellaneous),Chemistry, Multidisciplinary,Colloid and Surface Chemistry
    Systems
    Scattering
    Program
    Metal nanoparticles
    Macroions
    Integration scheme
    Energy
    Electrostatics
    Complexes
    Biological macromolecules
    Binding sites
    Approximation
    Aggregation
    Química
    Materiais
    Interdisciplinar
    General chemistry
    Farmacia
    Engenharias iv
    Engenharias iii
    Engenharias ii
    Colloid and surface chemistry
    Ciências biológicas ii
    Ciências biológicas i
    Ciências agrárias i
    Ciência de alimentos
    Chemistry, multidisciplinary
    Chemistry (miscellaneous)
    Chemistry (all)
    Chemistry
    Catalysis
    Biochemistry
    Astronomia / física
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