SCIENTIFIC HIGHLIGHTS

Unraveling the surface of nanoparticles: From aggregates to patchy Rare Earth Fluoride (ReF3) Nanoparticles

LnF3 nanocrystals are synthesized and their different behavior is studied by a combination of experimental and all-atomic molecular dynamics simulations. We show here that the deep knowledge of the surface is a powerful tool to control the final size, shape and behavior of the nanoparticles
Surface chemistry serves a fundamental role as the bridge between nanocrystal design and their final applications. In the study LnF3 nanocrystals are synthesized using co-precipitation method with citrate stabilization, as commonly is used to allow the fast, easy and reproducible synthesis of several nanoscaled structures in water. General trends related to the behavior of LnF3 nanocrystals are highlighted due to their broad range of application in several fields (e.g. medical applications). The same demeanor for all lanthanide (III) cations is expected due to the internal role of their f-orbitals. However we found that the use of different lanthanide elements is crucial in the final size, shape, assembly and crystalline structure. Fifteen Rare Earth elements (plus Y) were studied and the mechanism for the formation of the aggregates or patches and the properties of the obtained nanocrystals are characterized by a combination of experimental techniques and all-atomic molecular dynamics simulations. The crystallographic phase is tuned by changing the pH of the reaction. General trends are unraveled for each lanthanide, giving a classification where the metal-cation size is the pivotal key. Therefore, a different crystal structure and surface chemistry distributions are obtained, depending on the used lanthanide, pH and its final NCs shape. Nowadays, the accurate control of the interface between NC surface and stabilizers become in a hard and tedious work to enhance the intricate bridge, arriving to a future deep range of applications.   Further studies towards an accurate and selective control over surface serves a fundamental role as the bridge between nanocrystal design and their final applications.

Authors:

  • Jordi Martínez-Esaín,1,2 Teresa Puig,2 Xavier Obradors,2 Josep Ros,1 Ramón Yáñez,1 Jordi Faraudo2,*and Susagna Ricart2,*

    Affiliation:
    1 Departament de Química, Universitat Autònoma de Barcelona, Spain.
    2 Institut de Ciència de Materials de Barcelona, ICMAB-CSIC, Spain.

  • Figure:
    The study not only reveals the dependence of the crystalline structure with used metal and pH, but also the achievement of assembled particles depending on the final shape of nanocrystals.


  • Publication:
    Tunable Self-Assembly of YF3 Nanoparticles by Citrate-Mediated Ionic Bridges
    Journal of the American Chemical Society 140, 6, 2127-2134 (2018)
    DOI: 10.1021/jacs.7b09821

  • Faceted-Charge Patchy LnF(3) Nanocrystals with a Selective Solvent Interaction
    Angewandte Chemie-International Edition 130, 14963-14967 (2018)
    DOI: 10.1002/ange.201806273

  • Tailoring the Synthesis of LnF(3) (Ln = La-Lu and Y) Nanocrystals via Mechanistic Study of the Coprecipitation Method
    Langmuir 34, 22, 6443-6453 (2018)
    DOI: 10.1021/acs.langmuir.7b03454 

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