0000000000117493
AUTHOR
Ronja Otter
showing 8 related works from this author
Probing the Folding of Peptide–Polymer Conjugates Using the π-Dimerization of Viologen End-Groups
2020
The synthesis of a foldable viologen-functionalized peptide–polymer conjugate is presented. The ABA-type triblock conjugate with a PEG polymer was capped with a FHFHF pentapeptide sequence and further modified with a viologen building block at both chain ends. The pH-responsive peptide domains fold into an intermediate structure inducing close proximity of the viologen units, which upon a reduction step form π-dimers of the radical cation. Overall the intramolecular folding and intermolecular self-assembly process leads to the formation of supramolecular nanorods. Mixing of viologen-peptide–polymer conjugates with unfunctionalized conjugates leads to crosslinking of the nanorods and hydroge…
Secondary Structure-Driven Hydrogelation Using Foldable Telechelic Polymer-Peptide Conjugates.
2018
The synthesis of ABA and ABA' triblock polyethylene glycol-and polysarcosine-peptide conjugates is reported. The A/A' peptides are based on phenylalanine(F)-histidine(H) pentapeptide sequences FHFHF, which promote pH-switchable β-sheet self-assembly into nanorods in water. Only parallel β-sheet-driven folding and intermolecular assembly using ABA triblock polymer-peptide conjugates leads to interstrand cross-linking and hydrogelation, highlighting the impact of supramolecular interactions-directed structure formation at the nano- and mesoscopic level.
Folding induced supramolecular assembly into pH-responsive nanorods with a protein repellent shell
2018
We report the synthesis of ABA' triblock peptide-polysarcosine-peptide conjugates featuring two complementary phenylalanine-histidine pentapeptide strands A/A'. These sequences encode for antiparallel beta-sheet formation into folded conjugates, which promote the self-assembly into polysarcosine-shielded core-shell nanorods. These do not cause aggregation of serum proteins in human blood plasma underlining an enhanced stability.
Evaluation of Charge‐Regulated Supramolecular Copolymerization to Tune the Time Scale for Oxidative Disassembly of β‐Sheet Comonomers
2019
A multistimuli-responsive supramolecular copolymerization is reported. The copolymerization is driven by hydrogen bond encoded β-sheet-based charge co-assembly into 1D nanorods in water, using glutamic acid or lysine residues in either of the peptide comonomers. The incorporation of methionine as hydrophobic amino acid supports β-sheet formation, but oxidation of the thioether side-chain to a sulfoxide functional group destabilizes the β-sheet ordered domains and induces disassembly of the supramolecular polymers. Using H2 O2 as reactive oxygen species, the time scale and kinetics of the oxidative disassembly are probed. Compared to the charge neutral homopolymers, it is found that the oxid…
Kinetically Controlled Stepwise Self-Assembly of AuI-Metallopeptides in Water
2018
The combination of attractive supramolecular interactions of a hydrophobic AuI-metallopeptide with the shielding effect of flexible oligoethylene glycol chains provides access to a stepwise self-assembly of a AuI-metalloamphiphile in water. Kinetic control of the supramolecular polymer morphology is achieved using a temperature-dependent assembly protocol, which yields low dispersity supramolecular polymers (metastable state I) or helical bundled nanorods (state II).
Supramolecular assembly of functional peptide-polymer conjugates.
2019
The following review gives an overview about synthetic peptide-polymer conjugates as macromolecular building blocks and their self-assembly into a variety of supramolecular architectures, from supramolecular polymer chains, to anisotropic 1D arrays, 2D layers, and more complex 3D networks. A selection of recent literature examples using linear, coiled-coil and cyclic peptide motifs is provided. The reversible nature of the unimer-to-supramolecular polymer transition provides unique opportunities to investigate mechanistic aspects of the supramolecular assembly, with respect to the thermodynamic or kinetic parameters and furthermore provides exciting opportunities for non-equilibrium assembl…
Tuning the life-time of supramolecular hydrogels using ROS-responsive telechelic peptide-polymer conjugates
2019
Abstract The synthesis of multi-stimuli responsive peptide-poly(ethylene glycol) ABA-type conjugates is reported. The β-sheet encoded intramolecular folding and intermolecular self-assembly into 1D nanorods is based on a phenylalanine(F)-methionine(M)-histidine(H) FMHMHF hexapeptide sequence, and the supramolecular nanorods are stabilised by a shielding corona of hydrophilic PEG polymers. Interstrand crosslinking leads to the formation of physical networks and hydrogels at physiological pH and at room temperature. The thioether functional groups integrate oxidation responsive properties in the supramolecular polymer assemblies. We show that the glucose fuelled and glucose oxidase catalysed …
A clickable NHC–Au(i)-complex for the preparation of stimulus-responsive metallopeptide amphiphiles
2018
We report the synthesis of an alkyne functionalised NHC-Au(i)-complex which is conjugated with amphiphilic oligopeptides using a copper(i) catalysed cycloaddition. The resulting Au(i)-metalloamphiphiles are shown to self-assemble into charge-regulated stimulus-responsive supramolecular polymers in water via a weakly cooperative polymerisation mechanism.