Browsing by Subject "Self-assembling peptides"
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Item Open Access Catalytic supramolecular self-assembled peptide nanostructures for ester hydrolysis(Royal Society of Chemistry, 2016) Gulseren, G.; Khalily, M. A.; Tekinay, A. B.; Güler, Mustafa O.Essential amino acids in catalytic sites of native enzymes are important in nature inspired catalyst designs. Active sites of enzymes contain the coordinated assembly of multiple amino acids, and catalytic action is generated by the dynamic interactions among multiple residues. However, catalysis studies are limited by the complex and dynamic structure of the enzyme; and it is difficult to exclusively attribute a given function to a specific residue. Minimalistic approaches involving artificial catalytic sites are promising for the investigation of the enzyme function in the absence of non-essential protein components, and self-assembling peptide nanostructures are especially advantageous in this context. Here we demonstrate the design and characterization of an enzyme-mimetic catalytic nanosystem presenting essential residues (Ser, His, Asp). The function of each residue and its combinations on the nanostructures in hydrolysis reaction was studied. The catalytic self-assembled nanostructures were used for efficient ester hydrolysis such as a model substrate (pNPA) and a natural substrate (acetylcholine) highlighting the key role of self-assembly in catalytic domain formation to test the efficiency of the de novo designed catalyst as a catalytic triad model.Item Open Access Design and synthesis of self-assembling peptides for fabrication of functional nanomaterials(Bilkent University, 2016-12) Khalily, Mohammad ArefSelf-assembling peptides are a class of supramolecular polymers, which exploit noncovalent interactions such as hydrogen bonding, hydrophobic, electrostatic, charge-transfer complex, π-π, and van der Waals interactions to generate well-defined supramolecular nanostructures including nanospheres, nanosheets, nanotubes, and nanofibers. These versatile peptide-based supramolecular nanomaterials have been utilized in variety of applications including catalysis, sensing, light harvesting, optoelectronic, bioelectronic and tissue engineering. In this thesis, use of supramolecular peptide nanofibers formed by specially designed short peptide sequences that can form sheet-like hydrogen bonded structures for controlled synthesis of nanometer scale functional materials were explored. Specifically, n-type and p-type β-sheet forming short peptide sequences were synthesized, which assemble separately into well-ordered nanofibers in aqueous media. These p-type and n-type nanofibers coassemble via hydrogen bonding and electrostatic interactions to generate highly uniform supramolecular n/p-coassembled 1D nanowires. This smart molecular design ensures alternating arrangement of D and A chromophores within n/p-coassembled supramolecular nanowires. Supramolecular n/p- coassembled nanowires were found to be formed by alternating A-D-A unit cells having an association constant of (KA) of 5 x 105 M-1. Moreover, I designed and synthesized β-sheet forming peptide nanofibers to fabricate different metal and metal oxide nanostructures in highly controlled manner using wet chemistry and atomic layer deposition techniques. These hybrid organic-inorganic nanostructures were employed in model Suzuki coupling, alkyne-azide cycloaddition and hydrolysis of ammonia borane reactions.Item Open Access Hierarchical self-assembly of histidine-functionalized peptide amphiphiles into supramolecular chiral nanostructures(American Chemical Society, 2017) Koc, M. H.; Ciftci, G. C.; Baday, S.; Castelletto, V.; Hamley, I. W.; Güler, Mustafa O.Controlling the hierarchical organization of self-assembling peptide amphiphiles into supramolecular nanostructures opens up the possibility of developing biocompatible functional supramolecular materials for various applications. In this study, we show that the hierarchical self-assembly of histidine- (His-) functionalized PAs containing d- or l-amino acids can be controlled by both solution pH and molecular chirality of the building blocks. An increase in solution pH resulted in the structural transition of the His-functionalized chiral PA assemblies from nanosheets to completely closed nanotubes through an enhanced hydrogen-bonding capacity and π-π stacking of imidazole ring. The effects of the stereochemistry and amino acid sequence of the PA backbone on the supramolecular organization were also analyzed by CD, TEM, SAXS, and molecular dynamics simulations. In addition, an investigation of chiral mixtures revealed the differences between the hydrogen-bonding capacities and noncovalent interactions of PAs with d- and l-amino acids.Item Open Access Nanoengineering hybrid supramolecular multilayered biomaterials using polysaccharides and self-assembling peptide amphiphiles(Wiley-VCH Verlag, 2017) Borges, J.; Sousa, M. P.; Cinar, G.; Caridade, S. G.; Güler, Mustafa O.; Mano, J. F.Developing complex supramolecular biomaterials through highly dynamic and reversible noncovalent interactions has attracted great attention from the scientific community aiming key biomedical and biotechnological applications, including tissue engineering, regenerative medicine, or drug delivery. In this study, the authors report the fabrication of hybrid supramolecular multilayered biomaterials, comprising high-molecular-weight biopolymers and oppositely charged low-molecular-weight peptide amphiphiles (PAs), through combination of self-assembly and electrostatically driven layer-by-layer (LbL) assembly approach. Alginate, an anionic polysaccharide, is used to trigger the self-assembling capability of positively charged PA and formation of 1D nanofiber networks. The LbL technology is further used to fabricate supramolecular multilayered biomaterials by repeating the alternate deposition of both molecules. The fabrication process is monitored by quartz crystal microbalance, revealing that both materials can be successfully combined to conceive stable supramolecular systems. The morphological properties of the systems are studied by advanced microscopy techniques, revealing the nanostructured dimensions and 1D nanofibrous network of the assembly formed by the two molecules. Enhanced C2C12 cell adhesion, proliferation, and differentiation are observed on nanostructures having PA as outermost layer. Such supramolecular biomaterials demonstrate to be innovative matrices for cell culture and hold great potential to be used in the near future as promising biomimetic supramolecular nanoplatforms for practical applications.