期刊
DALTON TRANSACTIONS
卷 42, 期 45, 页码 15953-15966出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c3dt51696b
关键词
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资金
- Ministry of Education, Culture, Sports, Science and Technology (MEXT) [22550099, 24108719]
- PREST program from Japan Science and Technology Agency (JST) [07051361]
- Global COE program International Center for Integrated Research and Advanced Education in Materials Science
- Grants-in-Aid for Scientific Research [22550099, 24108719, 25620059] Funding Source: KAKEN
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 supra-molecular gels that displayed well-ordered metal arrays. The formation of parallel beta-sheet type aggregates through interpeptide amide-amide 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 H-1 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 amide-amide 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.
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