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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Metal array fabrication based on ultrasound-induced self-assembly of metalated dipeptides
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Metal array fabrication based on ultrasound-induced self-assembly of metalated dipeptides

机译：基于超声诱导的金属化二肽自组装的金属阵列制备

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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 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 ~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 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.
机译：通过与Pd或Pt-丙二胺复合物结合的谷氨酸的缩合合成Pd和Pt结合的双金属化肽，以提供bis-Pd和bis-Pt均金属化二肽的四种可能的金属异构体以及PdPt-和没有金属歧化的PtPd杂金属化二肽。超声诱导的这些双金属化肽的自组装有效地进行，以提供显示出有序金属阵列的超分子凝胶。通过IR，扫描电子显微镜（SEM）和同步加速器X射线衍射分析（WAXS和SAXS）证实了通过肽间酰胺-酰胺氢键形成的平行β-折叠型聚集体的形成。通过1H NMR的动力学和缔合实验阐明了超声诱导的金属化二肽自组装的机理，其中超声触发了Pd和Pt配合物的氯化物配体与酰胺之间的分子内氢键的解离。最初发生。随后形成分子间酰胺-酰胺氢键，从而提供相应的寡聚肽自组装作为超分子聚集的核。观察到的胶凝速率与超声处理频率的一阶关系表明，在超声处理条件下产生的微空化作用是关键的触发因素，并为有效的自组装提供了反应场。

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