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      Chiral ceramic nanoparticles and peptide catalysis

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      Author(s)
      Jiang S.
      Chekini, M.
      Qu, Z.-B.
      Wang Y.
      Yeltik A.
      Liu, Y.
      Kotlyar, A.
      Zhang, T.
      Li, B.
      Demir, Hilmi Volkan
      Kotov, N. A.
      Date
      2017
      Source Title
      Journal of the American Chemical Society
      Print ISSN
      0002-7863
      Publisher
      American Chemical Society
      Volume
      139
      Issue
      39
      Pages
      13701 - 13712
      Language
      English
      Type
      Article
      Item Usage Stats
      241
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      522
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      Abstract
      The chirality of nanoparticles (NPs) and their assemblies has been investigated predominantly for noble metals and II-VI semiconductors. However, ceramic NPs represent the majority of nanoscale materials in nature. The robustness and other innate properties of ceramics offer technological opportunities in catalysis, biomedical sciences, and optics. Here we report the preparation of chiral ceramic NPs, as represented by tungsten oxide hydrate, WO3-x·H2O, dispersed in ethanol. The chirality of the metal oxide core, with an average size of ca. 1.6 nm, is imparted by proline (Pro) and aspartic acid (Asp) ligands via bio-to-nano chirality transfer. The amino acids are attached to the NP surface through C-O-W linkages formed from dissociated carboxyl groups and through amino groups weakly coordinated to the NP surface. Surprisingly, the dominant circular dichroism bands for NPs coated by Pro and Asp are different despite the similarity in the geometry of the NPs; they are positioned at 400-700 nm and 500-1100 nm for Pro- and Asp-modified NPs, respectively. The differences in the spectral positions of the main chiroptical band for the two types of NPs are associated with the molecular binding of the two amino acids to the NP surface; Asp has one additional C-O-W linkage compared to Pro, resulting in stronger distortion of the inorganic crystal lattice and greater intensity of CD bands associated with the chirality of the inorganic core. The chirality of WO3-x·H2O atomic structure is confirmed by atomistic molecular dynamics simulations. The proximity of the amino acids to the mineral surface is associated with the catalytic abilities of WO3-x·H2O NPs. We found that NPs facilitate formation of peptide bonds, leading to Asp-Asp and Asp-Pro dipeptides. The chiroptical activity, chemical reactivity, and biocompatibility of tungsten oxide create a unique combination of properties relevant to chiral optics, chemical technologies, and biomedicine.
      Keywords
      Amino acids
      Biocompatibility
      Catalysis
      Ceramic materials
      Chirality
      Crystal atomic structure
      Dichroism
      Metal nanoparticles
      Metals
      Molecular dynamics
      Nanoparticles
      Oxides
      Peptides
      Polymethyl methacrylates
      Tungsten
      Tungsten compounds
      Atomistic molecular dynamics simulations
      Biomedical science
      Ceramic nanoparticles
      Chemical technologies
      Chirality transfer
      Nano-scale materials
      Nanoparticle (NPs)
      Technological opportunity
      Stereochemistry
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      http://hdl.handle.net/11693/37273
      Published Version (Please cite this version)
      http://dx.doi.org/10.1021/jacs.7b01445
      Collections
      • Department of Electrical and Electronics Engineering 4012
      • Department of Physics 2551
      • Institute of Materials Science and Nanotechnology (UNAM) 2260
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