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  • De Feyter, Steven  (2)
  • Feng, Xinliang  (2)
  • Mertens, Stijn F. L.  (2)
  • 2015-2019  (2)
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  • 2015-2019  (2)
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  • 1
    Online Resource
    Online Resource
    Reversible Anion‐Driven Switching of an Organic 2D Crystal at a Solid–Liquid Interface
    Wiley ; 2017
    In:  Small Vol. 13, No. 46 ( 2017-12)
    Details
    In: Small, Wiley, Vol. 13, No. 46 ( 2017-12)
    Abstract: Ionic self‐assembly of charged molecular building blocks relies on the interplay between long‐range electrostatic forces and short‐range, often cooperative, supramolecular interactions, yet has been seldom studied in two dimensions at the solid–liquid interface. Here, we demonstrate anion‐driven switching of two‐dimensional (2D) crystal structure at the Au(111)/octanoic acid interface. Using scanning tunneling microscopy (STM), three organic salts with identical polyaromatic cation (PQPC 6 + ) but different anions (perchlorate, anthraquinonedisulfonate, benzenesulfonate) are shown to form distinct, highly ordered self‐assembled structures. Reversible switching of the supramolecular arrangement is demonstrated by in situ exchange of the anion on the pre‐formed adlayer, by changing the concentration ratio between the incoming and outgoing anion. Density functional theory (DFT) calculations reveal that perchlorate is highly mobile in the adlayer, and corroborate why this anion is only resolved transiently in STM. Surprisingly, the templating effect of the anion persists even where it does not become part of the adlayer 2D fabric, which we ascribe to differences in stabilization of cation conformations by the anion. Our results provide important insight into the structuring of mixed anion–cation adlayers. This is essential in the design of tectons for ionic self‐assembled superstructures and biomimetic adaptive materials and valuable also to understand adsorbate–adsorbate interactions in heterogeneous catalysis.
    Type of Medium: Online Resource
    ISSN: 1613-6810 , 1613-6829
    URL: Issue
    URL: Article
    DOI: 10.1002/smll.v13.46
    DOI: 10.1002/smll.201702379
    Language: English
    Publisher: Wiley
    Publication Date: 2017
    detail.hit.zdb_id: 2168935-0
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  • 2
    Online Resource
    Online Resource
    From Breathing Pores to Three-Dimensional Ionic Self-Assembly Under Electrochemical Control
    The Electrochemical Society ; 2015
    In:  ECS Meeting Abstracts Vol. MA2015-01, No. 11 ( 2015-04-29), p. 1030-1030
    Details
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2015-01, No. 11 ( 2015-04-29), p. 1030-1030
    Abstract: Molecular self-assembly at the solid–liquid interface is highly developed, yet still faces several challenges, in particular related to reaching into the third dimension. Here, we demonstrate the spontaneous and reversible transition between two- and three-dimensional self-assembly of a charged polyaromatic molecule at the solid–liquid interface under electrochemical conditions, using in situ scanning tunnelling microscopy. By tuning the interfacial potential, we can selectively organise our target molecules in an open porous pattern, stretch these pores to accommodate another molecule and form an auto-host–guest structure, or stack the building blocks in a stratified bilayer. Using a simple electrostatic model, we rationalise which charge density is required to enable bilayer formation, and conversely, which molecular size/charge ratio is necessary in the design of new building blocks. Our findings could form the basis of electrochemically controlled dynamic host–guest systems and 3D structures such as artificial receptors. References [1] K. Cui, K.S. Mali, O. Ivasenko, D. Wu, X. Feng, M. Walter, K. Müllen, S. De Feyter, S.F.L. Mertens, Angew. Chem., Int. Ed. 53, 12951 (2014). [2] K. Cui, O. Ivasenko, K. S. Mali, D. Wu, X. Feng, K. Müllen, S. De Feyter, S. F. L. Mertens, Chem. Commun. 50, 10376 (2014). Figure 1
    Type of Medium: Online Resource
    ISSN: 2151-2043
    URL: Article
    DOI: 10.1149/MA2015-01/11/1030
    Language: Unknown
    Publisher: The Electrochemical Society
    Publication Date: 2015
    detail.hit.zdb_id: 2438749-6
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