NDLI: Reversible Binding of Solvent to Naked $Pb^{II}$ Centers in Unusual Homoleptic Alkynyl-Based $Pt_{2}Pb_{2}$ Clusters

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Reversible Binding of Solvent to Naked $Pb^{II}$ Centers in Unusual Homoleptic Alkynyl-Based $Pt_{2}Pb_{2}$ Clusters

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	Lalinde, Elena Sánchez, Sergio Fernández, Julio Berenguer, Jesús R. Gil, Belén
Description	Author Affiliation: Berenguer JR ( Departamento de Química, Centro de Investigación en Síntesis Química, Universidad de La Rioja, 26006, Logroño (Spain).)
Abstract	We report a series of luminescent sandwich-type clusters $[Pt_{2}Pb_{2}(C≡CR)_{8}]$ (R=Tol, 1; $C_{6}H_{4}OMe-3,$ 2; $C_{6}H_{4}OMe-4,$ 3) with a dynamic $Pt_{2}Pb_{2}$ metallic core, which is key to their intriguing stimuli-responsive photophysical properties. The solvent-free solids 1–3 display an orange emission ascribed to charge transfer from Pt–alkynyl fragments to a delocalized orbital with mixed $Pt_{2}Pb_{2}/C≡CR$ nature, with a predominant lead contribution and Pb⋅⋅⋅Pb bonding character $(^{3}MLCCT/^{3}IL).$ They exhibit mechanical, color, and luminescence changes that are reversible and perceivable with the naked eye, which are attributed to small inter- and intramolecular structural modifications induced by gentle grinding. Interestingly, 1 and 2 also exhibit remarkable and fast reversible vapochromic responses to donor solvent vapors (acetone, THFMe-2: yellow; NCMe: green, vs. dry solids: orange). The structures of $1(acetone)_{2}⋅2(Me_{2}CO),$ $2(acetone)_{3},$ and $2(THFMe-2)_{2}$ allow the vapochromic responses to be ascribed to the fast creation/disruption of solvate clusters $[Pt_{2}Pb_{2}(C≡CR)_{8}S_{x}]$ (x≥2), with concomitant electronic and geometrical modifications within the $Pt_{2}Pb_{2}$ core, which are easily accessible through a slight change in the stereochemical activity of the lone pair. The binding of one (or two) solvent molecules to $Pb^{2+}$ increases the Pb⋅⋅⋅Pb separation in the metallic core, causing a destabilization of the target orbital and larger energy gaps of the transitions. All the solvates exhibit remarkable rigidochromism upon a decrease in temperature, which is also associated with the gradual increase in the transannular Pb⋅⋅⋅Pb separation, as revealed by X-ray crystallography of $1(acetone)_{2}$ at different temperatures. Investigation of the crystal lattice of $1⋅CH_{2}Cl_{2}$ and $3⋅2 CH_{2}Cl_{2}$ further suggests that the lack of vapor stimuli response of complex 3 could be attributed to the presence of competitive additional secondary intermolecular Pb⋅⋅⋅O(OMe) contacts, which give rise to a more compact network built up from extended chains of clusters.
ISSN	09476539
e-ISSN	15213765
Journal	Chemistry - A European Journal
Issue Number	9
Volume Number	20
Language	English
Publisher	Wiley-VCH;ChemPubSoc Europe
Publisher Date	2014-02-24
Publisher Place	Germany
Access Restriction	Open
Subject Keyword	Chemistry
Content Type	Text
Resource Type	Article
Subject	Organic Chemistry Catalysis

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