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Issue 45, 2013
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Metal array fabrication based on ultrasound-induced self-assembly of metalated dipeptides

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Abstract

Pd- and Pt-bound bis-metalated peptides were synthesised by the condensation of Pd- or Pt-aldimine-complex-bound glutamic acids to afford the four possible metal isomers of bis-Pd and bis-Pt-homometalated dipeptides and PdPt- and PtPd-heterometalated dipeptides without metal disproportionation. Ultrasound-induced self-assembly of these bis-metalated peptides proceeded effectively to afford supramolecular gels that displayed well-ordered metal arrays. The formation of parallel β-sheet type aggregates through interpeptide amideamide hydrogen bonding was confirmed by IR, scanning electron microscopy (SEM), and synchrotron X-ray diffraction analyses (WAXS and SAXS). The mechanism of the ultrasound-induced self-assembly of the metalated dipeptides was elucidated via kinetic and association experiments by 1H NMR, in which ultrasound-triggered dissociation of intramolecular hydrogen bonds between the chloride ligands of the Pd- and Pt-complexes and amides initially occurred. This was followed by the formation of intermolecular amideamide hydrogen bonds, which afforded the corresponding oligomeric peptide self-assembly as the nucleus for supramolecular aggregation. The observed first-order relationship of the gelation rate versus the sonication frequency suggested that the microcavitation generated under sonication conditions acted as a crucial trigger and provided a reaction field for efficient self-assembly.

Graphical abstract: Metal array fabrication based on ultrasound-induced self-assembly of metalated dipeptides

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Publication details

The article was received on 25 Jun 2013, accepted on 22 Jul 2013 and first published on 25 Jul 2013


Article type: Paper
DOI: 10.1039/C3DT51696B
Citation: Dalton Trans., 2013,42, 15953-15966
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    Metal array fabrication based on ultrasound-induced self-assembly of metalated dipeptides

    K. Isozaki, Y. Haga, K. Ogata, T. Naota and H. Takaya, Dalton Trans., 2013, 42, 15953
    DOI: 10.1039/C3DT51696B

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